Title of Invention

INTERMEDIATE FILM FOR LAMINATED GLASS AND LAMINATED GLASS

Abstract The present invention provides an interlayer for laminated glass which comprises at least one layer composed of an opaque ethylene-vinyl acetate copolymer resin composition or opaque polyvinyl acetal resin composition, and also provides the laminated glass using such interlayers. The interlayer for laminated glass and the laminated glass according to the present invention can offer excellent privacy protection.
Full Text

DESCRIPTION
TECHNICAL FIELD
The present invention relates to an interlayer for
laminated glass and also to laminated glass, both of which
allow light to pass but cannot permit the persons or
objects existing behind them to be visually identified.
BACKGROUND ART
There have heretofore been known opaque laminated
glass, which is produced by bonding at least two
transparent glass sheets with an interlayer having such an
opacifier as calcium carbonate or silica dispersed in a
thermoplastic resin. Such opaque laminated glass can
transmit light, but cannot permit the persons or objects
existing behind them to be visually identified. Therefore,
the opaque laminated glass has been used in the locations
where privacy protection is required to be secured,—such as
lighting windows, bathroom doors and panels or wainscots
for balconies (for example, refer to Japanese Patent
Publication (examined) No. 2-56295).
However, such conventional opaque laminated glass
using an opacifier causes the problem that uneven coloring
is likely to occur due to agglomeration or poor dispersion
of particles of the opacifier. In addition, there is also
created the problem that the particles of the opacifier,
which are present at an interface between each glass sheet
and the interlayer, impair adhesion at the interface so
that fine air bubbles are likely to be formed.

In order to solve such problems, there has been proposed
an interlayer for opaque laminated glass consisting of (a) a
polyvinyl acetal resin produced by acetalization of a polyvinyl
alcohol having a degree of saponification of not less than 96
mol% with an aldehyde having 1 to 10 carbon atoms, (b) a polyvinyl
acetal resin produced by acetalization of a polyvinyl alcohol
having a degree of saponification of less than 96 mol% with an
aldehyde having 1 to 10 carbon atoms and (c) a plasticizer
(Japanese Patent Laid-open No. 6-263489).
However, opaque laminated glass described in Japanese Patent
Laid-Open No. 6-263489 does not yet have a lowered visible-light
transmittance suited for privacy protection, and also undergoes
decreases in its transmittances for other rays or light, or
impairs the proper, fundamental characteristics required of
laminated glass, when an attempt is made to get its visible light
transmittance decreased to a lowered level suited for privacy
protection, thus being not necessarily satisfactory.
Also, the laminated glass, as produced by bonding, for
example, an interlayer composed of a polyvinyl butyral rein
plasticized with a plasticizer, etc. between at least two
transparent glass sheets has been widely used as windowpanes
in automobiles and buildings , etc. Furthermore, such laminated
glass offers the advantage that utilization of interlayers
colored with a variety of coloring agents can facilitate the
resultanttinted laminated glass to control or regulate the inner
quantity of light.
Laminated glass using this type of interlayers has the
fundamental characteristics required of the laminated glass,
such as good weatherability, satisfactory adhesion between the

interlayer and glass sheet, reasonable resistance to penetration
or piercement by objects when subjected to external impacts,
and adequate resistance to shattering or shatter-proof ness when
broken by external impacts, although the laminated glass
encounters the problem of inferior sound-insulating property.
Particularly, such laminated glass shows a reduced sound
transmission loss owing to the coincidence effect in the range
of middle to high frequencies of about 2,000 to 5,000 Hz, and
suffers from deterioration in sound-insulating property,
wherein the term "coincidence effect" is understood to refer
to the phenomenon in which when a soundwave enters a glass sheet,
a transverse wave is propagated on the surface of the glass sheet
due to the rigidity and inertia of the glass sheet and becomes
resonant with the incident sound wave, thereby causing sound
transmission. The coincidence effect is shifted to a higher
frequency region according as the surface density of the
laminated glass is smaller, that is, the thickness of the glass
sheet diminishes.
In accordance with an increasingly growing demand for
improved sound-insulating property, in recent years, there is
required the laminated glass which can exhibit excellent
sound-insulating property in addition to the fundamental
characteristics as described above. Referring to an interlayer
for improved sound-insulating laminated glass and such
sound-insulating laminated glass, for example, Japanese Patent
No. 2703471 discloses laminated glass using an interlayer for
sound-insulating laminated glass of which interlayer comprises
not less than at least two different plasticized polyvinyl acetal
resin films being laminated.

In order to enhance the sound-insulating property of
laminated glass, however, there has been strongly demanded an
interlayer for laminated glass which can attain the enhanced
sound-insulating property as compared with the conventional ones.
In addition, the conventional sound-insulating
polyvinylacetal resin interlayers, with their increased
contents of plasticizers, have caused the problem that blocking
is likely to occur during storage or handling, and such
sound-insulating polyvinyl acetal resin film has therefore been
laminated on both sides with the polyvinyl acetal resin films
with a reduced content of a plasticizer to form the three-layered
film, thereby preventing the interlayer from causing blocking.
The laminated glass using the conventional sound-insulating
interlayers, although it has successfully prevented
deterioration in the sound-insulating property as caused by the
above-described coincidence effect and has exhibited excellent
sound-insulating property, has confronted the problem that its
sound-insulating property gets impaired in cases where it is
exposed to temperature rises causedby irradiation with sunlight,
etc.
SUMMARY OF THE INVENTION
PROBLEMS TO BE SOLVED BY THE INVENTION
With a specific view to solving the above-described problems,
the present invention has been completed, and an object of the
present invention is to provide the interlayer for laminated
glass and the laminated glass, both of which can offer excellent
performance in privacy protection.
The preferred first invention of the present invention has

also been completed in consideration of the above-described
problems, and has as its object to provide the interlayer for
laminated glass, and the laminated glass, both of which can
exhibit excellent privacy protection.
The preferred second invention of the present invention
has also been accomplished in light of the above-described
problems, and has as its object to provide an interlayer for
laminated glass, and laminated glass, which exhibit improved
privacy protection and sound-insulating property, is reduced
in self-adhesiveness and less likely to cause blocking, and can
shield the sunlight.
The preferred third invention of the present invention has
also been completed in consideration of the above-described
problems, and has as its object to provide an interlayer for
laminated glass and laminated glass, which exhibits excellent
privacy protection and sound-insulating property, and also
shield the sunlight.
The preferred fourth invention of the present invention
has been made too in view of the above-described problems, and
has as its object to provide an interlayer for laminated glass
and laminated glass, which can prevent deterioration in the
sound-insulating property associated with the temperature rises
caused by irradiation with the sunlight, and also exhibit
excellent performance in privacy protection and light shielding
property.
THE MEANS TO SOLVE THE PROBLEMS
The present inventors conducted extensive research to
achieve the above objects , and as a result found that an interlayer

for laminated glass, which comprises at least one layer composed
of an opaque ethylene-vinyl acetate copolymer resin composition
or opaque polyvinyl acetal resin composition, can offer excellent
privacy protection, thus leading to completion of the present
invention. This was followed by further extensive
investigation, resulting in completion of the below-described
first, second, third, and fourth inventions of the present
invention.
(The means to solve the problems of the first invention)
The present inventors conducted extensive investigation
to achieve the above-described objects, and as a result found
that use of an interlayer for laminated glass composed of an
opaque ethylene-vinyl acetate copolymer (EVA) resin composition
containing fine-particle inorganic powder and heat-ray
shielding fine particles makes it possible to produce a laminated
glass which shows a lowered visible light transmittance suited
for privacy protection and also dose not create the problems
of occurrence of uneven coloring due to agglomeration or poor
dispersion of fine-particle inorganic powder (especially, an
opacif ier) and formation of fine air bubbles due to deterioration
of adhesion at the interface between a glass sheet and an
interlayer brought about by fine-particle inorganic powder
(especially an opacifier) present at the interface, thereby
permitting the problems of the prior art to be solved at once,
and these findings were followed by further extensive
investigation, leading to completion of the first invention of
the present invention.
Namely, the first invention of the present invention relates
to:

(1-1) An interlayer for laminated glass, characterized in
that said interlayer is composed of an opaque ethylene-vinyl
acetate copolymer resin composition containing fine-particle
inorganic powder and heat-ray shielding fine particles,
(1-2) The interlayer for laminated glass according to the
above (1-1), wherein the fine-particle inorganic powder is
calcium carbonate or silica,
(1-3) The interlayer for laminated glass according to the
above (1-1) or (1-2), wherein the heat-ray shielding fine
particles are tin-doped indium oxide, and
(1 - 4) Laminated glass, characterized in that said laminated
glass comprises the interlayer for laminated glass according
to any one of the above (1-1) to (1-3) being bonded between at
least two glass sheets.
(The means to solve the problems of the second invention)
The above-described object of the second invention can be
accomplished by the inventions to be described below under (2-1')
to (2-3).
(2-1) An interlayer for laminated glass, characterized in
that said interlayer is composed of an opaque and
sound-insulating polyvinyl acetal resin composition containing
fine-particle inorganic powder,
(2-2) An interlayer for laminated glass, characterized in
that the opaque and sound-insulating polyvinyl acetal resin
composition further contains heat-ray shielding fine particles,
and
(2-3) Laminated glass, characterized in that said laminated
glass comprises at least two transparent glass sheets, wherein
the interlayer for laminated glass according to the above (2-1)

or (2-2) is bonded between them.
(The means to solve the problem of the third invention)
The above-described object of the third invention can be
accomplished by the inventions to be described below under (3-1)
to (3-3).
(3-1) An interlayer for laminated glass, characterized in
that said interlayer comprises at least two layers of (A) an
opaque and sound-insulating polyvinyl acetal resin layer
containing fine-particle inorganic powder and (B) a transparent
polyvinyl acetal resin layer being laminated together,
(3-2) The interlayer for laminated glass according to the
above (3-1), characterized in that at least either one of (A)
the opaque and sound-insulating polyvinyl acetal resin layer
and (B) the transparent polyvinyl acetal resin layer contains
heat-ray shielding fine particles, and
(3-3) Laminated glass, characterized in that said laminated
glass comprises at least two transparent glass sheets, wherein
the interlayer for laminated glass according to the above (3-1)
or (3-2) is bonded between them.
(The means to solve the problems of the fourth invention)
The object of the fourth invention can be accomplished by
the inventions to be described below under the items (4-1) to
(4-8).
(4-1) An interlayer for laminated glass, characterized in
that said interlayer comprises a sound-insulating polyvinyl
acetal resin layer being laminated to an opaque polyvinyl acetal
resin layer.
(4-2) The interlayer for laminated glass according to the
above (4-1) , characterized in that the opaque polyvinyl acetal

resin layer consists, of a tinted layer being colored with
inorganic fine particles,
(4-3) The interlayer for laminated glass according to the
above (4-1) or (4-2), characterized in that the opaque polyvinyl
acetal resin layer consists of a tinted layer being colored with
achromatic inorganic fine particles.
(4-4) The interlayer for laminated glass according to any
one of the above (4-1) to (4-3), characterized in that the
sound-insulating polyvinyl acetal resin layer is chromatically
or achromatically colored and is transparent or opaque.
(4-5) The interlayer for laminated glass according to any
one of the above (4-1) to (4-4), characterized in that at least
either one of the sound-insulating polyvinyl acetal resin layer
and the opaque polyvinyl acetal resin layer contains heat-ray
shielding fine particles.
(4-6) The interlayer for laminated glass according to any
one of the above (4-1) to (4-5), characterized in that the
sound-insulating polyvinyl acetal resin layer and the opaque
polyvinyl acetal resin layer are laminated together through a
transparent polyvinyl acetal layer interposed.
(4 - 7) Laminated glass , characterized in that said laminated
glass comprises at least two transparent glass sheets, wherein
the interlayer for laminated glass according to any one of the
above (4-1) to (4-6) being bonded between them.
(4-8) The laminated glass according to the above (4-7),
characterized in that said laminated glass has a haze value of
not less than 20%.
Namely, the present invention relates to:
(1) An interlayer for laminated glass, which comprises at

least one layer composed of an opaque ethylene-vinyl acetate
copolymer resin composition or an opaque polyvinyl acetal resin
composition,
(2) An interlayer for laminated glass, which is composed
of an opaque ethylene-vinyl acetate copolymer resin composition
containing fine-particle inorganic powder and heat-ray
shielding fine particles,
(3) The interlayer for laminated glass according to the
above (2) , wherein the fine-particle inorganic powder is calcium
carbonate or silica,
(4) The interlayer for laminated glass according to the
above (2) or (3) , wherein the heat-ray shielding fine particles
are tin-doped indium oxide,
(5) An interlayer for laminated glass, characterized in
that said interlayer is composed of an opaque and
sound-insulating polyvinyl acetal resin composition containing
fine-particle inorganic powder,
(6) The interlayer for laminated glass according to the
above (5) , characterized in that the opaque and sound-insulating
polyvinyl acetal resin composition further contains heat-ray
shielding fine particles,
(7) An interlayer for laminated glass, characterized in
that said interlayer comprises at least two kinds of layers of
(A) an opaque and sound-insulating polyvinyl acetal resin layer
containing fine-particle inorganic powder and (B) a
transparent polyvinyl acetal resin layer, the layers being
laminated together,
(8) The interlayer for laminated glass according to the
above (7), characterized in that at least either one of (A) an

opaque and sound-insulating polyvinyl acetal resin layer and
(B) a transparent polyvinyl acetal resin layer contains heat-ray
shielding fine particles,
(9) An interlayer for laminated glass, characterized in
that said interlayer comprises a sound-insulating polyvinyl
acetal resin layer and an opaque polyvinyl acetal resin layer
being laminated together,
(10) The interlayer for laminated glass according to the
above (9), wherein the opaque polyvinyl acetal resin layer is
a tinted layer colored with inorganic fine particles,
(11) The interlayer for laminated glass according to the
above (9) or (10), wherein the opaque polyvinyl acetal resin
layer is a tinted layer colored with achromatic inorganic fine
particles,
(12) The interlayer for laminated glass according to any
one of the above (9) to (11), characterized in that the
sound-insulating polyvinyl acetal resin layer is chromatically
or achromatically colored and is transparent or opaque,
(13) The interlayer for laminated glass according to any
one of the above (9) to (12), characterized in that at least
either one of the sound-insulating polyvinyl acetal resin layer
and opaque polyvinyl acetal resin layer contains heat-ray
shielding fine particles,
(14) The interlayer for laminated glass according to any
one of the above (9) to (13), wherein the interlayer comprises
the sound-insulating polyvinyl acetal resin layer and the opaque
polyvinyl acetal resin layer being laminated together through
a transparent polyvinyl acetal layer interposed;
(15) A laminated glass , characterized in that the interlayer

for laminated glass according to any one of the above (1) to
(14) is bonded between at least two glass sheets, and
(16) The laminated glass according to the above (15),
characterized in that the laminated glass has a haze value of
not less than 20%.
EFFECTS OF THE INVENTION
The interlayer for laminated glass and the laminated glass
comprising said interlayer can exhibit excellent performance
in privacy protection.
(Effect of the First Invention)
Laminated glass which comprises the interlayer for laminated
glass according to the first invention can exhibit excellent
performance in privacy protection, while it particularly
exhibits a low visible light transmittance suited for privacy
protection, namely a visible-light transmittance as low as not
more than 2.5 %, and also shows excellent heat-shielding
property.
The laminated glass according to the first invention not
only exhibits a low visible light transmittance suited for
privacy protection, but also eliminates the problem of occurrence
of uneven coloring caused by agglomeration or poor dispersion
of fine-particle inorganic powder (especially the opacifier),
while at the same time, it can produce the effect of preventing
the problem of formation of fine air bubbles caused by a decrease
in interfacial adhesion brought about by the fine-particle
inorganic powder being present at the interface between the glass
sheet and interlayer.
On account of these, the laminated glass according to the

first invention is suitably usable in the application fields
where the privacy protection is particularly required to be
ensured, among the roof and side-window panes of automobiles
or panes for buildings, etc.
(Effect of the Second Invention)
The interlayer for laminated glass according to the second
invention is composed of an opaque and sound-insulating polyvinyl
acetal resin composition, and, with the fine-particle inorganic
powder formulated therein, can achieve the enhanced
sound-insulating property. Because the sound-insulating
polyvinyl acetal resin composition is opaque, furthermore,
the interlayer can yield the laminated glass with additionally
excellent light-shielding property.
Moreover, the resin composition contains fine-particle
inorganic powder formulated therein, resulting in production
of the interlayer for laminated glass with decreased
self-adhesiveness in spite of its greater content of plasticizer.
The interlayer for laminated glass according to the second
invention, when colored with achromatic inorganic powder, can
produce the effect of development of much more subdued color
tone.
Because the laminated glass according to the second
invention is composed of the opaque and sound-insulating
polyvinyl acetal resin composition having fine-particle
inorganic powder formulated therein, the laminated glass
produced with use of said interlayer is suitably usable in the
application fields where the light-shielding property is
particularly required, among the roof and side-window panes of
automobiles except windshields, or panes for buildings, and the

like. In particular, the laminated glass produced by use of
the white-colored interlayer for laminated glass allows the
visible light to transmit but cannot permit the persons or objects
existing behind it to be visually identified, and consequently
is suitably utilizable in the locations where privacy protection
is particularly required to be ensured, such as lighting windows ,
bathroom doors, and panels or wainscots for balconies.
(Effect of the Third Invention)
The interlayer for laminated glass according to the third
invention comprises an opaque polyvinylacetal resin layer (A)
and a transparent polyvinyl acetal resin layer (B) being
laminated together, and can produce enhanced sound-insulating
effect owing to the fine-particle inorganic powder formulated
therein.
The difference in viscoelastic property between the
sound-insulating polyvinyl acetal rein layer (A) and the
transparent polyvinyl acetal resin layer (B) can permit sound
energy to be effectively converted and absorbed into heat energy
on account of the internal friction effect between the two resin
layers, and the sound-insulating property can be prevented from
deterioration caused by the coincidence effect at the middle
to high frequencies of about 2,000 to 5,000 Hz.
The interlayer, in which the sound-insulating polyvinyl
acetal resin layer is opaque, can provide the laminated glass
with excellent light-shielding property.
The interlayer for laminated glass according to the third
invention , when colored with achromatic inorganic fine particles ,
can produce the effect of development of much more subdued color
tone.

Since the interlayer for laminated glass is composed of
the sound-insulating polyvinyl acetal resin layer containing
fine-particle inorganic powder, the laminated glass produced
with use of said interlayer is suitably usable in the application
fields where the light-shielding property is particularly
required, among the roof and side-window panes of automobiles
except windshields, or panes for buildings. In particular, the
laminated glass produced by use of the white-colored interlayer
for laminated glass allows the transmittance of visible light
but cannot permit the persons or objects existing behind it to
be visually identified, and consequently is suitably utilizable
in the locations where privacy protection is particularly
required to be ensured, such as lighting windows, bathroom doors,
and panels or wainscots for balconies.
(Effect of the Fourth Invention)
Since the interlayer for laminated glass according to the
fourth invention comprises the above-described
sound-insulating polyvinyl acetal resin layer and opaque
polyvinylacetal resin layer being laminated together, and
shows excellent light-shielding property, the laminated glass
produced by use of the interlayer can cut off through absorption
or reflectance the infrared radiation (heat-ray) with
particularly great thermal effect among the rays of light
entering through the laminated glass originating from sunlight,
etc., while it suppresses temperature rises in the
sound-insulating polyvinyl acetal resin layer and also
temperature rises in the inside of automobiles and rooms of
buildings, and this can securedly prevent temperature rises in
the sound-insulating interlayer for laminated glass and

therefore the deterioration in sound-insulating property, as
well.
The interlayer for laminated glass according to the fourth
invention, which utilizes the tinted layer colored with
inorganic fine particles, exhibits excellent weatherability and
is resistant to deterioration in terms of such optical
characteristics as Haze value, physical strength of the
interlayer, etc.
The interlayer for laminated glass according to the fourth
invention, which utilizes the tinted layer colored with
achromatic inorganic fine particles, can produce the effect of
development of much more subdued color tone.
Because the interlayer for laminated glass according to
the fourth invention comprises the opaque polyvinyl acetal resin
layer being laminated, the laminated glass produced by use of
such interlayer is suitably usable in the application fields
where the light-shielding property is particularly required,
among the roof and side-window panes of automobiles except
windshields, or panes for buildings. In particular, the
laminated glass produced by use of the white-colored interlayer
for laminated glass allows the transmittance of visible light
but cannot permit the persons or objects existing behind it to
be visually identified, and consequently is suitably utilizable
in the locations where privacy protection is particularly
required to be ensured, such as lighting windows , bathroom doors,
and panels or wainscots for balconies.
In cases where the laminated glass according to the fourth
invention is used for automobiles and buildings in the places
or spots in contact with the outdoor environment, the interlayer

for laminated glass according to the fourth invention desirably
has the laminate construction in which the above-mentioned opaque
polyvinyl acetal resin layer is so arranged as to be on the outdoor
side.
When the interlayer for laminated glass according to the
fourth invention comprises the conventionally known
sound-insulating polyvinyl acetal resin layer, especially two
kinds of plasticized polyvinyl acetal resin layers being
laminated as a sound-insulating polyvinyl acetal resin layer,
the internal friction effect between two of the respective resin
layers having different viscoelastic properties can permit sound
energy to be effectively converted and absorbed into heat energy,
and the sound-insulating property can be prevented from
deterioration caused by the coincidence effect at the middle
to high frequencies of about 2,000 to 5,000 Hz.
BEST MODE FOR CARRYING OUT THE INVENTION
The interlayer for laminated glass of the present invention
is characterized in that said interlayer comprises at least one
layer composed of an opaque EVA resin composition or an opaque
polyvinyl acetal resin composition.
(Opaque EVA Resin Composition)
The opaque EVA resin composition to be used in the present
invention can be produced by mixing and dispersing an appropriate
amount of fine-particle inorganic powder in an EVA resin.
The EVA resin is a non-crosslinked ethylene-vinyl acetate
copolymer resin or a high-temperature crosslinked ethylene-
vinyl acetate copolymer resin. As the EVA resin, use can be
made of modified ethylene-vinyl acetate resins, such as

saponified ethylene-vinyl acetate copolymers. To produce a
variety of such EVA resins as mentioned above, there can be adopted
the conventionally known methods.
The ethylene-vinyl acetate copolymers (EVA) show a
vinyl-acetate content of 20 to 40wt% as measured in accordance
with JISK6730 "Testing Methods for Ethylene/Vinyl Acetate Resin
Materials " . When the vinyl acetate content is less than 20 wt%,
the resultant interlayer is so hard that its adhesion to a glass
sheet is impaired, while the laminated glass produced exhibits
deteriorated penetration resistance. When the vinyl-acetate
content exceeds 40 wt%, on the other hand, the resultant
interlayer has poor breaking strength so that the laminated glass
produced shows inferior impact resistance.
As examples of the fine-particle inorganic powder to be
used for producing the EVA resin composition, there may be
mentioned calcium carbonate, alumina, kaolin clay, calcium
silicate, magnesium oxide, magnesium hydroxide, aluminum
hydroxide, magnesium carbonate, talc, feldspar powder, mica,
baryte. barium carbonate, titanium oxide, silica, and glass beads .
Such fine-particle inorganic powder may be used singly or as
mixtures of two or more thereof. It is to be noted that the
above-mentioned fine-particle inorganic powder is preferably
opacifiers, more preferably calcium carbonate or silica, most
preferably calcium carbonate.
The fine-particle inorganic powder to be used for producing
the EVA resin compositions preferably have an average particle
size in the range of 0.1 to 100 µm, more preferably in the range
of 0.1 to 50 µm. The average particle sizes of the fine-particle
inorganic powder can be measured by the dynamic light scattering

inmethod usg a light scattering instrument (e.g. , "DLS-6000AL"
manufactured by Otsuka Electronics Co., Ltd. ) and an Ar laser
as a light source. The above-mentioned fine-particle inorganic
powder is generally used at ratios in the range of 0.3 to 30
parts by weight, preferably in the range of 0.5 to 20 parts by
weight, per 100 parts by weight of the EVA resin, so that the
opaque EVA resin compositions may be produced.
(Opaque Polyvinyl Acetal Resin Composition)
The above-mentioned opaque polyvinyl acetal resin
composition can be usually produced by mixing and dispersing
an appropriate amount of each of a plasticizer and fine-particle
inorganic powder in a polyvinyl acetal resin. The opaque
polyvinyl acetal resin composition may be, but is not
specifically limited to, any one obtained by mixing and
dispersing an appropriate amount of fine-particle inorganic
powder in a polyvinyl acetal resin composition containing for
example not less than 45 parts by weight of a plasticizer per
100 parts by weight of a known polyvinyl acetal resin as used
conventionally for an interlayer for sound-insulating laminated
glass. Namely, the opaque polyvinyl acetal resin composition
may be any polyvinyl acetal resin compositions containing
fine-particle inorganic powder and not less than 45 parts by
weight of a plasticizer per 100 parts by weight of a polyvinyl
acetal resin.
The plasticizer to be used for producing the polyvinyl acetal
resin composition is not particularly limited, and
conventionally known plasticizers generally used for producing
this type of interlayers can be used. Preferred examples of
such plasticizers include triethylene

glycol-di-2-ethylbutyrate (3GH), triethylene glycol-di-2-
ethylhexanoate (3GO) , triethylene glycol-di-n-heptanoate (3G7),
tetraethyleneglycol-di-2-ethylhexanoate (4G0), tetraethylene
glycol-di-n-heptanoate (4G7), and oligoethylene glycol-di-2-
ethylhexanoate (NGO), etc. Such plasticizers are generally
used at ratios in the range of 25 to 70 parts by weight per 100
parts by weight of the polyvinyl acetal resin.
The fine-particle inorganic powder to be used for producing
the above-mentioned opaque polyvinyl acetal resin composition
may be the same as those described above for producing the opaque
EVA resin compositions.
The fine-particle inorganic powder is generally used at
ratios in the range of 0.3 to 30 parts by weight, preferably
in the range of 0.5 to 20 parts by weight, per 100 parts by weight
of the polyvinyl acetal resin so that the opaque polyvinylacetal
resin film may be produced.
Particularly, the above-mentioned opaque polyvinyl acetal
resin composition is easy to be obtained in the subdued color
tone, since most of the above-mentioned fine-particle inorganic
powder is achromatic (white, light gray, gray, blackish gray,
black).
(Optional components)
The above-mentioned opaque EVA resin composition or opaque
polyvinyl acetal resin composition may further be admixed with
light shielding agents, a variety of coloring agents (e.g.,
pigments or dyes), etc., as the case may be.
Examples of the light shielding agents include carbon black,
red iron oxide, and the like. As the coloring agents, pigments
are preferably used, and examples of such pigments include a

dark red-brown mixed pigment produced by mixing four pigments,
i. e. a black pigment of carbon black, a red pigment of C. I. Pigment
red, a blue pigment of C.I.Pigment blue, and a yellow pigment
of C.I.Pigment yellow.
Furthermore, the above-mentioned opaque EVA resin
composition or the opaque polyvinyl acetal resin composition
may be incorporated with various additives generally used for
producing this type of interlayers, such as UV absorbers,
antioxidants, adhesion regulating agents, plasticizers, and the
like, as the case may be.
Preferred examples of the UV absorber include
2-(2'-hydroxy-5'-methylphenyl)benzotriazole (e.g., "TINUVIN
P" manufactured by CIBA-GEIGY Co.), 2- (2' -hydroxy-3 ', 5 ' -di-t-
methylphenyl)benzotriazole (e.g., "TINUVIN 320" manufactured
by CIBA-GEIGY Co.), 2-(2'-hydroxy-3'-t-butyl-5'-methyl-
phenyl)-5-chlorobenzotriazole (e.g., "TINUVIN 326"
manufactured by CIBA-GEIGY Co.), and 2-(2'-hydroxy-
s' , 5 ' -di-amylphenyl) -benzotriazole (e.g., "TINUVIN 328"
manufactured by CIBA-GEIGY Co.) . Alternatively, hindered amine
light stabilizers such as "ADEKA STAB LA-57" manufactured by
Adeka Argus Co.) is also preferable.
Preferred examples of the antioxidant include t-butyl
hydroxy toluene (e.g. , "Sumilizer BHT" manufactured by Sumitomo
Chemical Co.) and tetrakis-[methylene-3-(3',5'-di-t-butyl-4'-
hydroxyphenyl)propionate]methane (e.g., "IRGANOX 1010"
manufactured by CIBA-GEIGY Co.).
Preferred examples of the adhesion regulating agent include
alkali metal salts or alkaline earth metal salts of organic or
inorganic acids.

Examples of the plasticizer to be used for the
above-mentioned EVA resin composition include, for example,
phthalic acid esters such as dioctyl phthalate (DOP), dibutyl
phthalate (DBP) and diisodecyl phthalate (DIDP); adipic acid
esters such as di-2-ethylhexyl adipate (DOA) and diisodecyl
adipate (DIDA); sebacic acid esters such as dibutyl sebacate
(DBS) and di-2-ethylhexyl sebacate (DOS); phosphoric acid esters
such as tricresyl phosphate (TCP) and trioctyl phosphate (TOP) ;
and epoxidized soybean oil.
The interlayer for laminated glass of the present invention
is not particularly limited, as long as it is composed of the
above-mentioned opaque EVA resin composition or opaque polyvinyl
acetal resin composition, and may comprise a single layer or
multiple layers . In the case of the multiple layers, for example,
a layer composed of the above-mentioned opaque EVA resin
composition or polyvinyl acetal resin composition may
furthermore be laminated with a plural number of layers composed
of EVA resin compositions or polyvinyl acetal resin compositions
each having the same or different composition and miscellaneous
opaque resin compositions, or may be laminated with layers
composed of, for example, transparent resin compositions or
sound-insulating resin compositions.
Taking into consideration the minimum magnitudes of
penetration resistance and weatherability required of the
laminated glass, the interlayer for laminated glass according
to the present invention preferably shows a total film thickness
in the range of 0.3 to 1.6 mm for practical reasons, as is the
same with the conventional transparent interlayers for laminated
glass.

The interlayer for laminated glass composed of the
above-mentioned opaque EVA resin composition or the opaque
polyvinyl acetal resin composition can be produced by kneading
(I) the above-mentioned EVA resin and the above-mentioned
fine-particle inorganic powder, as well as a variety of
additives to be added if required, or (II) the above-mentioned
polyvinyl acetal resin composition, the above-mentioned
plasticizer and the above-mentioned fine-particle inorganic
powder, as well as a variety of additives to be added if required,
with an extruder, a plastograph, a kneader, a banbury mixer,
or a calender roll, etc., followed by film-forming into the sheet
form by the conventional film forming processes, such as the
extrusion, calendering and press processes.
The laminated glass of the present invention can be produced
using the same process as used for producing the conventional
laminated glass. For example, the laminated glass can be
manufactured , by sandwitching the above-described interlayer
for laminated glass between at least two transparent glass sheets ,
passing them through pressure rolls or placing them in a rubber
bag, followed by vacuum suction, to give a laminated body through
the preliminary bonding of the interlayer with the glass sheets
at about 70 to 110°C, while removing the air remaining between
the glass sheet and the interlayer and placing the deaerated
laminated body in an autoclave or subjecting it to pressing to
carry out the final bonding at about 120 to 150°C under applied
pressure of about 1 to 1.5 MPa.
It is to be noted that the transparent glass sheets to be
used in the present invention are not particularly limited, and
that any transparent glass sheets generally used can be used.

Examples of such transparent glass sheets include various kinds
of inorganic glass sheets such as float plate glass sheets,
heat-absorbing glass sheets, polished glass sheets, template
glass sheets, wire plate glass sheets, and line plate glass
sheets, and organic glass sheets such as polycarbonate sheets
and polymethyl methacrylate sheets. These glass sheets may be
used singly or in combination of two or more thereof. Among
them, heat-absorbing glass sheets are preferably used. It is
to be noted that the thickness of such glass sheets is not
particularly 1 imited and can be appropriately selected according
to their intended use, although it is desirably in the range
of 1 to 3 mm.
The thus obtained laminated glass of the present invention
has a low visible light transmittance suitable for privacy
protection.
(The First Invention)
To be described below is the first invention as a preferred
embodiment of the present invention.
An interlayer for laminated glass of the first invention
is characterized in that said interlayer is composed of an opaque
EVA resin composition containing fine -particle inorganic powder
and heat-ray shielding fine particles.
In the first invention, such an opaque EVA resin composition
can be obtained by mixing and dispersing an appropriate amount
of each of the above-mentioned fine-particle inorganic powder
and heat-ray shielding fine particles in the above-described
EVA resin. Examples of the fine-particle inorganic powder to
be used in the first invention include calcium carbonate, alumina,
kaolin clay, calcium silicate, magnesium oxide, magnesium

hydroxide, aluminum hydroxide, magnesium carbonate, talc,
feldspar powder, mica, baryte, barium carbonate, titanium oxide,
silica, and glass beads, etc. These may be used singly or as
mixtures of two or more thereof. It is to be noted that the
above-mentioned fine-particle inorganic powder is preferably
opacifiers, more preferably calcium carbonate or silica, most
preferably calcium carbonate.
Examples of the heat-ray shielding fine particles to be
used in the first invention include tin-doped indium oxide (ITO) ,
antimony-doped tin oxide (ATO), aluminum-doped zinc oxide (AZO) ,
indium-doped zinc oxide (IZO), tin-doped zinc oxide,
silicon-doped zinc oxide, zinc antimonate, lanthanum hexaboride,
cerium hexaboride, fine gold powder, fine silver powder, fine
platinum powder, and fine aluminum powder. Among them, ITO is
preferable.
The average particle sizes of the fine-particle inorganic
powder and the heat-ray shielding fine particles to be used in
the first invention are preferably in the range of 0.1 to 100
µm, more preferably in the range of 0.1 to 50 µm. These average
particle sizes can be measured by the dynamic light scattering
method using a light scattering instrument (e.g. , "DLS-6000AL"
manufactured by Otsuka Electronics) and an Ar laser as a light
source. The above-mentioned fine-particle inorganic powder is
generally used at ratios in the range of 0.3 to 30 parts by weight,
preferably in the range of 0.5 to 20 parts by weight, per 100
parts by weight of the EVA resin so that the opaque EVA resin
composition may be produced. The above-mentioned heat-ray
shielding fine particles are usually used at ratios in the range
of 0.001 to 30 parts by weight, preferably in the range of 0.001

to 10 parts by weight, more preferably in the range of 0.005
to 5 parts by weight, per 100 parts by weight of the EVA resin.
It is to be noted that when the fine-particle inorganic
powder to be used in the first invention is calcium carbonate,
the average particle size of said inorganic powder is preferably
in the range of 0.5 to 10 µm, and the calcium carbonate content
in the interlayer for laminated glass preferably is in such a
range as may satisfy the following equation (1), more preferably
the following equation (2).
Equation (1):
Calcium carbonate content in the interlayer (wt%) x
thickness of the interlayer (mm) = 1.0 to 3.0,
Equation (2):
Calcium carbonate content in the interlayer (wt%) x
thickness of the interlayer (mm) = 1.5 to 2.5
Particularly, the above-mentioned opaque EVA resin
composition is easy to be obtained in the subdued color tone,
since most of the fine-particle inorganic powder is achromatic
(white, light gray, gray, blackish gray, black).
The above-mentioned opaque EVA resin composition may further
be incorporated with light shielding agents, coloring agents
(e.g., pigments or dyes), etc., as the case may be.
Furthermore, the above-mentioned opaque EVA resin
composition may be incorporated with a variety of additives
generally used for producing this type of interlayers, such as
UV absorbers, antioxidants, adhesion regulating agents, and
plasticizers, as the case may be.
The interlayer for laminated glass according to the first
invention of the present invention is not particularly limited.

only if it is composed of the above-mentioned opaque EVA resin
composition, and may comprise a single layer or multiple layers .
In the case of multiple layers, for example, a layer composed
of the above-mentioned opaque EVA resin composition may be
laminated with a plural number of layers composed of EVA resin
compositions or miscellaneous opaque resin compositions each
having a different composition, or layers comprising transparent
resin compositions or sound-insulating resin compositions.
Taking into consideration the minimum levels or magnitudes
of penetration resistance and weatherability required of the
laminated glass, the interlayer for laminated glass according
to the present invention preferably shows a total film thickness
in the range of 0.3 to 1.6 mm for practical reasons, as is the
same with the conventional transparent interlayers for laminated
glass.
The interlayer for laminated glass composed of the
above-mentioned opaque EVA resin composition or opaque polyvinyl
acetal resin composition can be produced by kneading the
above-mentioned EVA resin, the above-mentioned fine-particle
inorganic powder, and various additives to be added as the case
maybe, with an extruder, a plastograph, a kneader, a banbury
mixer, or a calender roll, followed by film-forming into the
sheet form by the conventional film forming process, such as
the extrusion, calendering and press processes.
The laminated glass of the first invention can be produced
using the same process as used for producing the conventional
laminated glass. For example, the laminated glass can be
manufactured by sandwitching the above-de scribed interlayer for
laminated glass between at least two transparent glass sheets.

passing them through pressure rolls or placing them in a rubber
bag, followed by vacuum suction, to give a laminated body through
the preliminary bonding of the interlayer with the glass sheets
at about 70 to 110°C, while removing the air remaining between
the glass sheet and the interlayer, and placing the deaerated
laminated body in an autoclave or subjecting the same to pressing
to carrying out the final bonding at about 120 to 150°C under
applied pressure of about 1 to 1.5 MPa.
It is to be noted that the transparent glass sheets to be
used in the present invention are not particularly limited, and
that any transparent glass sheets generally used can be used.
Examples of such transparent glass sheets include various kinds
of inorganic glass sheets such as float plate glass sheets,
heat-absorbing glass sheets, polished glass sheets, template
glass sheets, wire plate glass sheets, and line plate glass
sheets, and organic glass sheets such as polycarbonate plates
or sheets and polymethyl methacrylate plates or sheets. These
glass sheets may be used singly or in combination of two or more
thereof. Among them, heat-absorbing glass sheets are
preferably used. It is to be noted that the thickness of glass
sheets is not particularly limited and can be appropriately
selected according to their intended use, although it is
desirably in the range of 1 to 3 mm per glass sheet.
The thus produced laminated glass of the first invention
has a low visible light transmittance suited for privacy
protection, namely a visible light transmittance of not more
than 2.5 %, and furthermore not more than 2 %. Additionally,
the laminated glass do neither encounter the problem of uneven
coloring caused by agglomeration or poor dispersion of

fine-particle inorganic powder (especially opacifier) nor
create the problem of formation of fine air bubbles caused by-
deteriorated interface adhesion due to the fine-particle
inorganic powder (especially opacifier) present at the interface
between the glass sheet and the interlayer.
(The Second Invention)
To be described below is the second invention as a preferred
embodiment of the present invention.
The interlayer for laminated glass according to the second
invention is characterized in that said interlayer is composed
of an opaque and sound-insulating polyvinyl acetal resin
composition containing fine-particle inorganic powder.
The interlayer for laminated glass according to the second
invention is characterized in that the opaque and
sound-insulating polyvinyl acetal resin composition further
contains heat-ray shielding fine particles.
In the second invention, such opaque and sound-insulating
polyvinyl acetal resin composition can be produced by mixing
and dispersing an appropriate amount of each of a plasticizer
and fine-particle inorganic powder in a polyvinyl acetal resin.
The polyvinyl acetal resin composition is not limited
particularly, and an appropriate amount of fine-particle
inorganic powder may be dispersed through mixing in a known
sound-insulating polyvinyl acetal resin composition being
conventionally used as an interlayer for sound-insulating
laminated glass, for example, a polyvinyl acetal resin
composition containing not less than 45 parts by weight of a
plasticizer per 100 parts by weight of polyvinyl acetal resin.
Namely, the opaque and sound-insulating polyvinyl acetal resin

composition may be a polyvinyl acetal resin composition
containing fine-particle inorganic powder and not less than 45
parts by weight of a plasticizer per 100 parts by weight of
polyvinyl acetal resin.
It is to be noted that the interlayer for laminated glass
according to the second invention may be laminated with a plural
number of layers of an opaque and sound-insulating polyvinyl
acetal resin composition having a different composition. In
this case, sound energy is effectively converted and absorbed
into heat energy due to the internal friction effect between
the two resin layers having different viscoelastic properties,
and particularly, the sound-insulating property can be prevented
from deterioration caused by the coincidence effect at the middle
to high frequencies of about 2,000 to 5,000 Hz.
The opaque and sound-insulating polyvinyl acetal resin
composition according to the second invention may further be
admixed with heat-ray shielding fine particles, as the case may
be.
The laminated glass having transparent glass sheets bonded
to both sides of the thus obtained interlayer for laminated glass
preferably shows a haze value of not less than 20%, particularly
preferably not less than 50%, more preferably not less than 60%.
When the haze value of the laminated glass is less than 20%,
scattering of visible light diminishes, thereby impairing the
light shielding property of the laminated glass.
Examples of the fine-particle inorganic powder to be used
in the second invention include calcium carbonate, alumina,
kaolin clay, calcium silicate, magnesium oxide, magnesium
hydroxide, aluminum hydroxide, magnesium carbonate, talc.

feldspar powder, mica, baryte, barium carbonate, titanium oxide,
silica, and glass beads, and thesemay be usedsinglyor as mixtures
thereof.
Examples of the heat-ray shielding fine particles to be
used in the second invention include tin-doped indium oxide (ITO) ,
antimony-doped tin oxide (ATO), aluminum-doped zinc oxide
(AZO), indium-doped zinc oxide (IZO), tin-doped zinc oxide,
silicon-doped zinc oxide, zinc antimonate, lanthanumhexaboride,
cerium hexaboride, fine gold powder, fine silver powder, fine
platinum powder, and fine aluminum powder.
The average particle size of the fine-particle inorganic
powder or the heat-ray shielding fine particles to be used in
the second invention are preferably in the range of 1 to 100
µm, more preferably in the range of 1 to 50 µm. These average
particle sizes can be measured by the dynamic light scattering
method using a light scattering instrument (e.g. , "DLS-6000AL"
manufactured by Otsuka Electronics) and an Ar laser as a light
source. The fine-particle inorganic powder is generally used
at ratios in the range of 0.3 to 30 parts by weight, preferably
in the range of 0.5 to 20 parts by weight, per 100 parts by weight
of the polyvinyl acetal resin, so that the opaque polyvinyl acetal
resin film may be produced. The heat-ray shielding fine
particles are usually used at ratios in the range of 0.001 to
30 parts by weight, preferably in the range of 0.001 to 10 parts
by weight, more preferably in the range of 0.005 to 5 parts by
weight, per 100 parts by weight of the polyvinyl acetal resin.
Particularly, the opaque and sound-insulating polyvinyl
acetal resin composition to be used in the second invention is
easy to be obtained in the subdued color tone, since many of

the fine-particle inorganic powder is achromatic (white, light
gray, gray, blackish gray, black).
Taking into consideration the minimum levels or magnitudes
of penetration resistance and weatherability required of the
laminated glass, the interlayer for laminated glass according
to the second invention preferably shows a total film thickness
in the range of 0.3 to 1.6 mm for practical reasons, as is the
same with the conventional transparent interlayers for laminated
glass.
The opaque and sound-insulating polyvinyl acetal resin
composition can be produced by kneading the above-mentioned
polyvinyl acetal resin, the above-mentioned plasticizer and a
variety of additives to be added, as the case may be, with an
extruder, a plastograph, akneader, a banbury mixer or a calender
roll, followed by film-forming by the conventional film forming
process, such as the extrusion, calendering and press processes.
The laminated glass of the second invention can be produced
using the same process as used for producing the conventional
laminated glass, for example, by sandwitching the
above-de scribed interlayer for laminated glass between at least
two transparent glass sheets, passing them through pressure
rolls or placing them in a rubber bag, followed by vacuum suction
to give a laminated body through the preliminary bonding of the
interlayer with the glass sheets at about 70 to 110°C, while
removing the air remaining between each glass sheet and the
interlayer, and placing the deaerated laminated body in an
autoclave or subjecting the same to pressing to carry out the
final bonding at about 120 to 150°C under applied pressure of
about 1 to 1.5 MPa.

It is to be noted that the transparent glass sheets to be
used in the second invention are not particularly limited, and
that any transparent glass sheets generally used can be used.
Examples of such transparent glass sheets include various kinds
of inorganic glass sheets such as float plate glass sheets,
heat-absorbing glass sheets, polished glass sheets, template
glass sheets, wire plate glass sheets, and line plate glass sheets,
and various organic glass plates or sheets such as polycarbonate
plates and polymethyl methacrylate plates. These glass sheets
may be used singly or in combination of two or more thereof.
Among them, heat-absorbing glass sheets are preferably used.
It is to be noted that the thickness of each glass sheet to be
used in the second invention is not particularly limited and
can be appropriately selected according to their intended use,
although it is desirably in the range of 1 to 3 mm.
(The Third Invention)
The interlayer for laminated glass according to the third
invention is characterized in that said interlayer comprises
a laminate structure of at least two layers consisting of an
opaque and sound-insulating polyvinyl acetal resin layer(A)
containing fine-particle inorganic powder and a transparent
polyvinyl acetal resin layer (B).
In the third invention, a polyvinyl acetal resin to be used
for the opaque and sound-insulating polyvinyl acetal resin layer
(A) is not particularly limited, and although use can be made
of any polyvinyl acetal resins used for producing a known
sound-insulating polyvinyl acetal resin films conventionally
used as an interlayer for sound-insulating laminated glass,
particularly, the polyvinyl acetal resin, which is used for a

sound-insulating polyvinyl acetal resin layer, as described in
Japanese Patent No. 2703471, is preferably used.
Namely, use is preferably made of polyvinyl acetal resins
(a) with a vinyl acetate content (residual acetyl groups) of
8 to 30 mol% obtained by acetalization of a polyvinyl alcohol
with an aldehyde having 4 to 6 carbon atoms.
The opaque and sound- insulating polyvinyl acetal resin layer
(A) to be used in the third invention may be composed of an opaque
and sound-insulating polyvinyl acetal resin composition, which
polyvinyl acetal resin composition may be any polyvinyl acetal
resin compositions containing fine-particle inorganic powder
and 45 parts by weight or more of a plasticizer per 100 parts
by weight of a polyvinyl acetal resin.
The opaque and sound-insulating polyvinyl acetal resin layer
(A) to be used in the third invention can be produced by furthermore
mixing and dispersing at least an appropriate amount of
fine-particle inorganic powder in the resin composition
containing the polyvinyl acetal resin as described above and
a plasticizer. In addition to the plasticizer and the
fine-particle inorganic powder, heat-ray shielding fine
particles, light shielding agents, UV absorbers, dyes, pigments,
etc. may be added, as the case may be.
It is to be noted that the resin layer (A) may be formed
by the lamination of a plural number of thin films . For example,
use of the laminate, which comprises the interlayer for laminated
glass according to the third invention being laminated with
layers of the known sound-insulating polyvinyl acetal resin,
especially two kinds of plasticized polyvinyl acetal resins,
being used as a sound-insulating polyvinyl acetal resin layer.

can allow the sound energy to be effectively converted and
absorbed into the heat energy due to the internal friction effect
produced between resin layers having different viscoelastic
properties, and particularly permits the sound-insulating
property to be prevented from deterioration due to the
coincidence effect in the middle to high sound region at 2,000
to 5,000 Hz.
In the third invention, an opaque polyvinyl acetal resin
layer may be produced by mixing and dispersing an appropriate
amount each of a plasticizer and fine-particle inorganic powder
in a sound-insulating polyvinyl acetal resin. The polyvinyl
acetal resin layer (A) may be composed of any opaque polyvinyl
acetal resins being further admixed with heat-ray shielding fine
particles , light shielding agents , a variety of dyes and pigments ,
etc.
In the third invention, a laminate construction consisting
of at least two layers of an opaque and sound-insulating polyvinyl
acetal resin layer (A) and a transparent polyvinyl acetal resin
layer (B) is utilized as an interlayer for laminated glass.
The construction of the transparent polyvinyl acetal resin
layer (B) is not particularly limited, and is exemplified by
a polyvinyl acetal resin layer composed of a resin composition
having an appropriate amount of a plasticizer dispersed through
mixing in a known polyvinyl acetal resin conventionally used
as an interlayer for laminated glass. Particularly, use is
desirably made of a transparent polyvinyl acetal resin layer
(B) composed of a polyvinyl acetal resin (b) with a vinyl acetate
content (residual acetyl groups ) of not more than 14 mol% produced
by acetalization of a polyvinyl alcohol with an aldehyde having

3 to 4 carbon atoms and a plasticizer. The resin composition
constituting the polyvinyl acetal resin layer (B) may be
furthermore admixed with heat-ray shielding fine particles, a
variety of dyes and pigments, etc., as the case may be.
The interlayer for laminated glass of the third invention
comprises the resin layer (A) and resin layer (B) as the essential
components, whereby a layer (C) of a resin other than polyvinyl
acetal resins may be laminated therebetween, as the case may
be. Examples of such resin layer (C) include layers of resins,
such as polyester, polyurethane and ethylene vinyl acetate
resins.
The order of stacking these resin layers (A), (B) and (C)
which constitute the interlayer for laminated glass according
to the third invention is not particularly limited, but these
resin layers are preferably stacked in such a manner that the
resin layer" (A) may constitute an intermediate layer, while at
least one resin layer (B) may make up the outermost surface layer,
whereby use can be made of any arbitrary constructions, such
as(B)/(A)/(B), (B)/(A), (B) /(C)/(A)/(B), (B)/(C)/(A)/(C)/(B),
and the like. From the viewpoint of secured ease of handling,
preferred is the interlayer for laminated glass having the
construction in which the resin layer (B) makes up the outermost
layer.
The laminated glass produced by bonding transparent glass
sheets to both sides of the thus obtained interlayer for laminated
glass desirably shows a haze value of not less than 20%,
particularly preferably not less than 50% , more preferably not
less than 60%. When the haze value of the laminated glass falls
beneath 20%, scattering of visible light diminishes, thereby

impairing the light shielding property of the laminated glass.
Examples of the fine-particle inorganic powder to be used
in the third invention include calcium carbonate, alumina, kaolin
clay, calcium silicate, magnesium oxide, magnesium hydroxide,
aluminum hydroxide, magnesium carbonate, talc, feldspar powder,
mica, baryta-, barium carbonate, titanium oxide, silica, and
glass beads. These fine-particle inorganic powder may be used
singly or in combination of two or more of them.
Examples of the heat-ray shielding fine particles to be
used in the third invention include tin-doped indium oxide (ITO),
antimony-doped tin oxide (ATO), aluminum-doped zinc oxide (AZO),
indium-doped zinc oxide (IZO), tin-doped zinc oxide,
silicon-doped zinc oxide, zinc antimonate, lanthanumhexaboride,
cerium hexaboride, fine gold powder, fine silver powder, fine
platinum powder, and fine aluminum powder. Examples of the light
shielding agents include carbon black and red iron oxide.
Examples of the pigments include dark red-brown pigments obtained
by mixing four pigments, namely carbon black of a black pigment,
a red pigment (C.I.Pigment red), a blue pigment (C.I.Pigment
blue) and a yellow pigment (C.I.Pigment yellow).
The average particle size of the fine-particle inorganic
powder to be used in the third invention is preferably in the
range of 1 to 100 \xm, more preferably in the range of 1 to 50
µm. Such average particle size can be measured by the dynamic
light scatteringmethodusing a light scattering instrument (e.g. ,
"DLS-6000AL" manufactured by Otsuka Electronics) and an Ar laser
as a light source. The amount of the fine-particle inorganic
powder is generally used at ratios in the range of 0.3 to 30
parts by weight, preferably in the range of 0.5 to 20 parts by

weight, per 100 parts by weight of the polyvinyl acetal resin,
so that the transparent polyvinyl acetal resin film may be
produced. The heat-ray shielding fine particles are usually
used at ratios in the range of 0.001 to 30 parts by weight,
preferably in the range of 0.001 to 10 parts by weight, more
preferably in the range of 0.005 to 5 parts by weight, per 100
parts by weight of the polyvinyl acetal resin.
Particularly, the above-described opaque and
sound-insulating polyvinyl acetal resin layer is easy to be
produced in the subdued color tone, since most of the
fine-particle inorganic powder is achromatic (white, light gray,
gray, blackish gray, black).
Taking into consideration the minimum levels or magnitudes
of penetration resistance and weatherability required of the
laminated glass, in general, the interlayer for laminated glass
according to the third invention preferably shows a total film
thickness in the range of 0.3 to 1.6 mm for practical reasons,
as is the same with the conventional transparent interlayers
for laminated glass.
The above-described sound-insulating polyvinyl acetal
resin layer can be produced by kneading the above-described
polyvinyl acetal resin, the above-mentioned plasticizer, and
a variety of additives to be added, as the case may be, with
an extruder, a plastograph, a kneader, a banbury mixer or a
calender roll, followed by film-forming into the sheet form by
the conventional film forming process such as the extrusion,
calendering and press processes.
The opaque and sound-insulating polyvinyl acetal resin layer
can be produced by kneading the above-described polyvinyl acetal

resin, the above-mentioned fine -particle inorganic powder, the
above-mentioned plasticizer, and the above-described opacif ier,
as well as heat-ray shielding fine particles, inorganic fine
particles such as various pigments and a variety of additives
to be added, as the case may be, with an extruder, a plastograph,
a kneader, a banbury mixer, or a calender roll, followed by film
forming into the sheet form by the conventional film forming
process such as the extrusion, calendaring and press processes .
The interlayer for laminated glass according to the third
invention can be produced by stacking the opaque and
sound-insulating polyvinyl acetal resin layer and the
transparent polyvinyl acetal resin layer as individually formed
separately in the above-described, and applying heat and pressure
to integrate the layer assembly into one structural member. Also,
the interlayer may be produced by film-forming through the
multiple-layer extrusion process into one structural member a
film-forming resin composition for forming the above-described
opaque and sound insulting polyvinyl acetal resin layer, a
film-forming resin composition for forming a transparent
polyvinyl acetal resin layer, and optionally a resin composition
for forming a transparent polyvinyl acetal resin layer. As an
alternative production process, the interlayer may be produced
concurrently with the production of the laminated glass by
stacking the opaque and sound-insulating polyvinyl acetal resin
layer, the transparent polyvinyl acetal resin layer, and a
transparent polyvinyl acetal resin layer, if necessary, between
two glass sheets, followed by heating and compressing to be
integrated into one structural member.
The laminated glass of the third invention can be produced

using the same method as used for producing conventional
laminated glass. For example, the laminated glass is produced
by sandwitching the above-described interlayer for laminated
glass between at least two transparent glass sheets, then passing
them through pressure rolls or placing them in a rubber bag,
followed by vacuum suction to give a laminated body through the
preliminary bonding of the interlayer with the glass sheets at
about 70 to 110°C, while removing air remaining between the glass
sheets and the interlayer, and placing the deaerated laminated
body in an autoclave or subjecting the same to pressing to carry-
out the final bonding at about 120 to 150°C under an applied
pressure of about 1 to 1.5 MPa.
It is to be noted that the transparent glass sheets are
not particularly limited, and transparent glass sheets generally
used can be used. Examples of such transparent glass sheets
include various kinds of inorganic glass sheets, such as float
plate glass sheets, heat-absorbing glass sheets, polished plate
glass sheets, template glass sheets, wire plate glass sheets
and line plate glass sheets, and various organic glass plates
or sheets, such as polycarbonate plates or sheets and polymethyl
methacrylate plates or sheets. These glass sheets may be used
singly or in combination of two or more thereof. Among them,
heat-absorbing glass sheets are preferably used. It is to be
noted that the thickness of such glass sheets is not particularly
limited and can be appropriately selected depending upon their
intended use, although it is desirably in the range of 1 to 3
mm.
(The Fourth Invention)
The interlayer for laminated glass of the fourth invention

is characterized in that said interlayer comprises a
sound-insulating polyvinyl acetal resin layer being laminated
with an opaque polyvinyl acetal resin layer.
In the fourth invention, the sound-insulating polyvinyl
acetal resin layer is not particularly limited, and there is
preferably used, for example, the known sound-insulating
polyvinyl acetal resin layers conventionally used as an
interlayer for sound-insulating laminated glass . Particularly,
use is preferably made of a sound-insulating polyvinyl acetal
resin layer as described in the above-mentioned Official Gazette
of Japanese Patent No. 2703471.
Namely, it is particularly preferable to use, as a
sound-insulating polyvinyl acetal resin layer (A) , at least one
resin layer composed of a polyvinyl acetal resin (a) with a vinyl
acetate content (residual acetyl groups) of 8 to 30 mol%, as
produced by acetalization of a polyvinyl alcohol with an
aldehyde having 4 to 6 carbon atoms, and a plasticizer.
The above-described sound-insulating polyvinyl acetal
resin layer may be composed of a sound-insulating polyvinyl
acetal resin composition, and said sound-insulating polyvinyl
acetal resin composition may be a polyvinyl acetal resin
composition which contains 45 parts by weight or more of a
plasticizer per 100 parts by weight of a polyvinyl acetal resin.
Also, in the fourth invention, the resin which constitutes
the opaque polyvinyl acetal resin layer is not particularly
limited, and there can be used the known polyvinyl acetal resins
being conventionally used as an interlayer for laminated glass .
Such resins can be admixed for dispersion with an appropriate
amount each of a plasticizer and inorganic fine particles

(coloring agent) to thereby form opaque polyvinyl acetal resin
layers. It is preferable to use opaque polyvinyl acetal resin
layers (B) composed of the above-described polyvinyl acetal
resins (b) with a vinyl acetate content (residual acetyl groups)
of not more than 14 mol%, as produced by acetalization of a
polyvinyl alcohol with an aldehyde having 3 to 4 carbon atoms,
a plasticizer, and inorganic fine particles (coloring agent)
such as opacifiers, heat-ray shielding fine particles, light
shielding agents, a variety of dyes and pigments.
When the sound-insulating polyvinyl acetal resin layer is
colored, there may be contained inorganic fine particles
(coloring agent) , such as opacifiers, heat-ray shielding fine
particles, light shielding agents, dyes and pigments.
In the fourth invention, a laminate of a sound-insulating
polyvinyl acetal resin layer (A) and an opaque polyvinyl acetal
resin layer (B) is used as the interlayer for laminated glass
and may further be laminated with a transparent polyvinyl acetal
resin layer. The composition of such transparent polyvinyl
acetal resin layer is not particularly limited and there is used
a resin layer, as obtained by mixing and dispersing an appropriate
amount of a plasticizer in a known polyvinyl acetal resin
conventionally used as an interlayer for laminated glass.
Particularly, it is preferred to use the transparent polyvinyl
acetal resin layer (C) composed of the above-described polyvinyl
acetal resin (b) and a plasticizer.
In the fourth invention, the interlayer for laminated glass
of the fourth invention can be produced by lamination of the
resin layer (A) and the resin layer (B) as essential components,
as well as a resin layer (C), if necessary, and the order of

stacking these resin layers is not particularly limited, only
if the resultant laminate has at least one layer out of the resin
layer (A) and resin layer (B) . There can be employed any arbitrary
layer-assembly constructions, such as (B)/(A)/(B), (B)/(A)/(C),
(A)/(C)/(B), (C)/(A)/(C)/(B) , andthelike. From the viewpoint
of secured ease of handling for the interlayer for laminated
glass, particularly preferred is the interlayer having the
layer-assembly construction in which the resin layer (B) or the
resin layer (C) makes up the outermost surface layer.
The haze value of the laminated glass, as produced in the
above-described manner by bonding transparent glass sheets to
both sides of the thus obtained interlayer for laminated glass,
is preferably not less than 20%, particularly preferably not
less than 50%, more preferably not less than 60% . If the haze
value of the laminated glass is less than 20%, scattering of
visible light diminishes, so that the light shielding property
of the laminated glass is impaired, thereby reducing the effect
of ameliorating the deterioration in sound-insulating property
caused by, for example, sunlight irradiation.
Examples of the above-mentioned opacif iers include calcium
carbonate, alumina, kaolin clay, calcium silicate, magnesium
oxide, magnesium hydroxide, aluminum hydroxide, magnesium
carbonate, talc, feldspar powder, mica, baryte, barium carbonate,
titanium oxide, silica, and glass beads. Examples of the
heat-ray shielding fine particles include tin-doped indium oxide
(ITO), antimony-doped tin oxide (ATO) , aluminum-doped zinc oxide
(AZO), indium-doped zinc oxide (IZO), tin-doped zinc oxide,
silicon-doped zinc oxide, zinc antimonate, lanthanumhexaboride,
cerium hexaboride, fine gold powder, fine silver powder, fine

platinum powder, and fine aluminum powder. Examples of the light
shielding agents include carbon black and red iron oxide.
Example of the pigments includes a dark red-brown pigment
obtained by mixing four pigments, i. e. , a black pigment of carbon
black, a red pigment (C.I.Pigment red), a blue pigment
(C.I. Pigment blue), and a yellow pigment (C.I. Pigment yellow) .
They can be used singly or as mixtures of two or more thereof,
and from the viewpoint of weatherability, inorganic fine
particles are considered preferable.
The average particle size of the inorganic fine particles
such as opacifiers, heat-ray shielding fine particles, light
shielding agents and pigments is preferably in the range of 1
to 100 µm, more preferably in the range of 1 to 50 µm. Their
average particle sizes can be measured by the dynamic light
scattering method using a light scattering instrument (e.g.,
"DLS-6000AL" manufactured by Otsuka Electronics) and an Ar laser
as a light source. The inorganic fine particles such as
opacifiers, light blocking agents, or pigments are generally
used at ratios in the range of 0. 3 to 30 parts by weight, preferably
in the range of 0. 5 to 20 parts by weight, per 100 parts by weight
of the polyvinyl acetal resin, so that the opaque polyvinylacetal
resin film may be produced. The heat -ray shielding fine particles
are usually used at ratios in the range of 0.001 to 30 parts
by weight, preferably in the range of 0.001 to 10 parts by weight,
more preferably in the range of 0.005 to 5 parts by weight, per
100 parts by weight of the polyvinyl acetal resin.
Particularly, the opaque polyvinyl acetal resin layer is
preferably colored with the inorganic fine particles, so that
the colored films may be formed. Preferable are the colored

films composed of the above-described opaque polyvinyl acetal
resin being colored with fine achromatic (white, light gray,
gray, blackish gray, black) inorganic particles, since they can
be produced in the subdued color tone.
Meanwhile, the various polyvinyl acetal resin layers as
described above can be incorporated with a variety of additives
used for this type of interlayers, such as UV absorbers,
antioxidants and adhesion regulating agents and the like.
Taking into consideration the minimum levels or magnitudes
of penetration resistance and weatherability required of the
laminated glass, the interlayer for laminated glass according
to the fourth invention preferably shows a total film thickness
in the range of 0.3 to 1.6 mm for practical reasons, as is the
same with the conventional transparent interlayers for laminated
glass.
The above-described sound-insulating polyvinyl acetal
resin layer can be produced by kneading the above-described
polyvinyl acetal resin and the above-mentioned plasticizer, as
well as a variety of the additives to be added, as the case may
be, with an extruder, a plastograph, a kneader, a banbury mixer
or a calender roll, followed by film-forming into the sheet form
by the conventional film forming process such as the extrusion,
calendering and press processes.
The above-described opaque polyvinyl acetal resin layer
can be produced by kneading the above-described polyvinyl
acetal resin, the above-mentioned plasticizer and the
above-mentioned opacifiers, as well as inorganic fine
particles such as heat-ray shielding fine particles, light
shielding agents and various pigments, and if necessary, a

variety of the additives to be added, with an extruder, a
plastograph, a kneader, a banbury mixer, or a calender roll,
followed by film-forming into the sheet form by the conventional
film forming process, such as the extrusion, calendering and
press processes.
The interlayer for laminated glass of the fourth invention
can be produced by stacking the sound- insulating polyvinyl acet al
resin layer and the opaque polyvinyl acetal resin layer, which
are individually film-formed separately as described above, as
well as an opaque or transparent polyvinyl acetal resin layer,
as the case may be, followed by heating and pressuring to be
integrated into one structural member. The interlayer can also
be produced by film-forming into one structural member through
multiple-layer extrusion process a film-forming resin
composition for the above-mentioned sound-insulting polyvinyl
acetal resin layer and a film-forming resin composition for the
opaque polyvinyl acetal resin layer, as well as a film-forming
resin composition for the opaque polyvinyl acetal resin layer,
as the case may be. As an alternative process, the interlayer
can be produced concurrently with the production of laminated
glass by stacking the sound-insulating polyvinyl acetal rein
layer and the opaque polyvinyl acetal resin layer, as well as
an opaque or transparent polyvinyl acetal resin layer, as the
case may be, between two glass sheets, followed by heating and
pressuring to be integrated into one structural member.
The laminated glass of the fourth invention can be produced
by the same process as the conventional one for producing
laminated glass. For example, the laminated glass is produced
by sandwitching the above-described interlayer for laminated

glass between at least two transparent glass sheets, then passing
them through pressure rolls or placing them in a rubber bag,
followed by vacuum suction to give a laminated body through
the preliminary bonding of the interlayer to the glass sheets
at about 70 to 110°C, while removing air remaining between the
glass sheets and the interlayer, and placing the deaerated
laminated body in an autoclave or subjecting the same to pressing
to carry out the final bonding at about 120 to 150°C under an
applied pressure of about 1 to 1.5 MPa.
Meanwhile, the transparent glass sheets are not particularly
limited, and transparent glass sheets generally used can be used.
Examples of such transparent glass sheets include various kinds
of inorganic glass sheets, such as float plate glass sheets,
heat-absorbing glass sheets, polished plate glass sheets,
template glass sheets, wire plate glass sheets and line plate
glass sheets, and various organic glass plates or sheets such
as polycarbonate plates and polymethyl methacrylate plates.
These glass sheets may be used singly or in combination of two
or more thereof. Among them, heat-absorbing glass sheets are
preferably used. The thickness of each glass sheet is not
particularly limited and can be appropriately selected
depending upon their intended use, but is preferably in the range
of 1 to 3 mm.
The haze value of the laminated glass as obtained in the
above manner which are included in the first to fourth inventions
is preferably not less than 20%, particularly preferably not
less than 50%, more preferably not less than 60%. When the haze
value of the laminated glass of the present invention is less
than 20%, scattering of visible light dimishes, thereby impairing

the light shielding property of the laminated glass.
EXAMPLES
The present invention will be described below in more detail
with reference to the following Examples of the present invention.
It is to be construed that the present invention is not limited
to these Examples.
(Examples of the First Invention)
(Example 1-1)
(1) Production of Interlayer A-l for Laminated Glass:
A quantity of 100 parts by weight of an ethylene-vinyl acetate
copolymer resin with a vinyl acetate content of 26 wt%
("Ultrathene 634" manufactured by Tosoh Corp.) as an EVA resin,
6 parts by weight of fine-particle calcium carbonate powder
particles (average particle size of 3 µm) as fine-particle
inorganic powder, and 0.25 part by weight of fine ITO particles
(manufactured by Mitsubishi Materials and having an average
particle size of 0.03 µm) as heat-ray shielding fine particles
were mixed, and the mixture was sufficiently melt-kneaded with
a mixing roll and press-molded at 150°C for 30 minutes with a
press-molding machine to produce an interlayer A-l for laminated
glass having an average thickness of 0.40 mm.
(2) Production of Laminated Glass
The interlayer A-l for laminated glass was sandwiched
between "two transparent float glass sheets (30 cm length x 30
cm width x 2.5 mm thickness), and they were placed in a rubber
bag, which was then deaerated under a vacuum of 2.6 kPa for 20
minutes and transferred into an oven at 90°C, while keeping it
deaerated, followed by vacuum-pressing at 90°C for 30 minutes

to carry out the preliminary bonding of the laminated body. The
preliminarily bonded laminated glass was subjected to
pressure-bonding in an air-type autoclave for 20 minutes under
the conditions of 135°C and 1.2 MPa of pressure to produce a
laminated glass.
(Example 1-2)
(1) Production of Interlayer A-2 for Laminated Glass:
An interlayer A-2 for laminated glass having an average
thickness of 0.40 mm was produced in the same manner as described
in Example 1-1 except that 6 parts by weight of the fine-particle
calcium carbonate powder used as fine-particle inorganic powder
was replaced with 5 parts by weight of fine-particle silica powder
(having an average particle size of 5 µm).
(2) Production of Laminated Glass
A laminated glass was produced in the same manner as described
in Example 1-1 except that the interlayer A-1 for laminated glass
was replaced with the interlayer A-2 for laminated glass.
(Comparative Example 1-1)
(1) Production of Interlayer B for Laminated Glass
A transparent interlayer B for laminated glass having an
average thickness of 0.40 mm was produced in the same manner
as described in Example 1-1 except that the heat-ray shielding
fine particles and the fine-particle inorganic powder were not
contained.
(2) Production of Laminated glass
A laminated glass was produced in the same manner as described
in Example 1-1 except that the interlayer A-1 for laminated glass
was replaced with the interlayer B for laminated glass.
(Evaluation)

For the laminated glasses produced individually in Examples
1-1 and 1-2 and Comparative Example 1-1, a haze value, a visible
light transmittance (Tv), a solar transmittance (Te) , and a solar
reflectance (Re) were measured using the following methods.
Further, the laminated glasses of Examples were visually
inspected for agglomeration or poor dispersion of the
fine-particle inorganic powder (especially, an opacifier),
uneven coloration of the laminated glass, and formation of fine
air bubbles at the interface between each glass sheet and the
interlayer.
The evaluation results are shown in Table 1.
(1) Measurement of Haze Value
A haze value in the rays of light at the wavelength of 340
to 1800 nm was measured with an integral turbidimeter
(manufactured by Tokyo Denshoku) in accordance with JIS K 6714
"Methacryl Resin Plate for Aircraft".
(2) Measurement of Visible Light Transmittance (Tv), Solar
Transmittance (Te), and Solar Reflectance (Re)
A visible light transmittance (Tv) at the wavelength of
380 to 780 nm, a solar transmittance (Te) at the wavelength of
300 to 2100 nm, and a solar reflectance (Re) at the wavelength
of 300 to 2100 nm were measured with a direct-recording
spectrophotometer (manufactured by Shimadzu Corp. under the
trade name of "UV-3100") in accordance with JIS Z 8722 and JIS
R 3106.


(Examples of the Second Invention)
(Example 2-1)
(1) Production of Polyvinyl Butyral Resin (a) and Interlayer
A-1 for Laminated Glass
A quantity of 191 parts by weight of a polyvinyl alcohol
having an average degree of polymerization of 1700 and a degree
of saponification of 88.1 mol% was added to 2890 parts by weight
of pure water, followed by heating for dissolution. The reaction
system, after its temperature was adjusted to 12°C, was admixed
with 201 parts by weight of a 35 wt% hydrochloric acid catalyst
and 148 parts by weight of n-butyraldehyde, and was maintained
at this temperature to allow the reaction product to precipitate.
The reaction system was maintained at 45°C for 3 hours to complete
the reaction, then washed with excessive water to wash out
unreacted n-butyraldehyde, treated with an aqueous sodium
hydroxide solution to neutralize the hydrochloric acid catalyst,

washed with excessive water and dried to give a polyvinyl butyral
resin in the form of white powder (a). The resin (a) was found
to show an average degree of butyralization of 63.8 raol% and
a vinyl acetate content of 11.9 mol%.
A quantity of 100 parts by weight of the above-mentioned
resin (a), 51 parts by weight of triethylene glycol
di-2-ethylbutyrate (3GH) as a plasticizer, 5 parts by weight
of silica powder having an average particle size of 5 pi as
fine-particle inorganic powder, 0.1 part by weight of
2- (2 ' -hydroxy-5' -methylphenyl)benzotriazole as a UV absorber,
and 0.1 part by weight of t-butylhydroxytoluene as an antioxidant
were mixed, and the mixture was sufficiently melt-kneaded with
a mixing roll and press-molded with a press-molding machine at
150°C for 30 minutes to produce an interlayer A-l for laminated
glass having an average thickness of 0.9 mm.
(2) Production of Laminated Glass
The interlayer A-l for laminated glass was sandwiched
between two transparent float glass sheets (30 cm long x 30 cm
wide x 2.5 mm thick) , and then they were placed in a rubber bag,
which was deaerated under a vacuum of 2.6 kPa for 20 minutes,
and transferred into an oven at 90°C, while keeping it deaerated,
followed by vacuum-pressing at 90°C for 30 minutes to carry out
the preliminary bonding of the laminated body. The
preliminarily bonded laminated glass was subjected to
pressure-bonding in an air-type autoclave for 20 minutes under
the conditions of 135°C of temperature and 1.2 MPa of pressure
to produce a laminated glass.
(Example 2-2)
(1) Production of Polyvinyl Butyral Resin (b) and Interlayer

B-1 for Laminated Glass
A quantity of 191 parts by weight of a polyvinyl alcohol
having an average degree of polymerization of 1700 and a degree
of saponification of 98.5 mol% was added to 2890 parts by weight
of pure water, followed by heating for dissolution, and the
reaction system, after its temperature was adjusted to 12°C,
then admixed with 201 parts by weight of a 35 wt% hydrochloric
acid catalyst and 165 parts by weight of n-butyraldehyde, and
maintained at this temperature to allow the reaction product
to precipitate. The reaction system was further maintained at
45°C for 3 hours to complete the reaction, washed with excessive
water to wash out unreacted n-butyraldehyde, treated with an
aqueous sodium hydroxide solution to neutralize the hydrochloric
acid catalyst, washed with excessive water for 2 hours, and dried
to give a polyvinyl butyral resin (b) in the form of white powder.
The resin (b) was found to show an average degree of butyralization
of 71.0 mol% and a vinyl acetate content of 1.5 mol%.
A quantity of 100 parts by weight of the resin (b), 51 parts
by weight of triethylene glycol di-2-ethylbutyrate (3GH) as a
plasticizer, 0.1 part by weight of 2-(2'-hydroxy-5'-
methylphenyl)benzotriazole as a UV absorber, 0 .1 part by weight
of t-butyl hydroxytoluene as an antioxidant, and 6.5 parts by
weight of calcium carbonate having an average particle size of
3 µm as fine-particle inorganic powder were mixed, and the mixture
was sufficiently melt-kneaded withamixing roll and press-molded
with a press-molding machine at 150°C for 30 minutes to produce
an interlayer B-l for laminated glass having an average thickness
of 0.90 mm.
(2) Production of Laminated Glass

A laminated glass was produced in the same manner as described
in Example 2-1 except that the inter layer A-1 for laminated glass
was replaced with the interlayer B-1 for laminated glass.
(Comparative Example 2-1)
Production of Interlayer B-2 for Laminated Glass
100 parts by weight of the resin (b), 51 parts by weight
of triethyleneglycoldi-2-ethylbutyrate (3GH) as aplasticizer,
0.1 part by weight of 2-(2'-hydroxy-5'-
methylphenyl)benzotriazole as a UV absorber, and 0.1 part by
weight of t-butyl hydroxy toluene as an antioxidant were mixed,
and the mixture was then sufficiently melt-kneaded with a mixing
roll and press-molded with a press-molding machine at 150°C for
30 minutes to produce a transparent interlayer B-2 for laminated
glass having an average thickness of 0. 90 mm, which did not contain
any fine-particle inorganic powder. Using the above-mentioned
interlayer B-2, laminated glass was produced in the same manner
as described in Example 2-1 having an average thickness of 0.90
mm.
(Example 2-3)
(1) Production of Interlayer for Laminated glass A-2
A quantity of 100 parts by weight of the resin (a) obtained
in Example 2-1, 51 parts by weight of triethylene glycol
di-2-ethylbutyrate (3GH) as a plasticizer, 0.5 part by weight
of fine ITO particles (manufactured by Mitsubishi Materials Co. )
as heat-ray shielding fine particles , 5 parts by weight of silica
powder having an average particle size of 5 µm as fine-particle
inorganic powder, 0.1 part by weight of 2-(2'-hydroxy-5'-
methylphenyl)-benzotriazole as a UV absorber, and 0.1 part by
weight of t-butylhydroxytoluene as an antioxidant were mixed,

and the mixture was sufficiently melt-kneaded with a mixing roll
and press-molded with a press-molding machine at 150°C for 30
minutes to produce an interlayer A-2 for laminated glass having
an average thickness of 0.9 mm.
(2) Production of Laminated Glass
A laminated glass was produced in the same manner as described
in Example 2-1 except that the interlayer A-1 for laminated glass
was replaced with the interlayer A-2 for laminated glass.
(Example 2-4)
(1) Production of Interlayer B-3 for Laminated Glass
A quantity of 100 parts by weight of the resin (b)produced
in Example 2-2, 51 parts by weight of triethylene glycol
di-2-ethylbutyrate (3GH) as a plasticizer, 1 part by weight of
fine ITO particles (manufactured by Mitsubishi Materials Co. )
as heat-ray shielding fine particles, 0.1 part by weight of
2- (2 ' -hydroxy-5 ' -methylphenyl) - benzotriazole as a UV absorber,
0.1 part by weight of t-butyl-hydroxytoluene as an antioxidant,
and 6.5 parts by weight of calcium carbonate having an average
particle size of 3 µm as fine-particle inorganic powder were
mixed, and the mixture was sufficiently melt-kneaded with a
mixing roll and press-molded with a press-molding machine at
150°C for 30 minutes to produce an interlayer B-3 for laminated
glass having an average thickness of 0.90 mm.
(2) Production of Laminated glass
A laminated glass was produced in the same manner as described
in Example 2-2 except that the interlayer B-1 for laminated glass
was replaced with the interlayer B-3 for laminated glass.
(Evaluation)
For the laminated glasses produced individually in Examples

2-1 and 2-2 and Comparative Example 2-1, a haze value and a loss
factor were measured using the following methods. For the
interlayers for laminated glass produced individually in
Examples 2-1 and 2-2 and Comparative Example 2-1, self-adhesive
strength was measured using the following method. The
evaluation results are shown in Table 2.
Further, for the laminated glasses produced individually
in Examples 2-3 and 2-4, a haze value, a loss factor and a
self-adhesive strength were measured, while a visible light
transmittance (Tv), a solar transmittance (Te), and a solar
reflectance (Re) were measured using the following methods. The
evaluation results are shown in Table 3.
(1) Measurement of Haze Value
A haze value in the rays of light at the wavelength of 340
to 1800 nm was measured with an integrating turbidimeter
(manufactured by Tokyo Denshoku Co.) in accordance with JIS K
6714 "Methacryl Resin Plate for Aircrafts".
(2) Measurement of Loss Factor
A sample (25 mm wide x 300 mm long) was cut from the laminated
glass, and subjected to vibration by use of a vibration generator
for damping test ("G21-005D" manufactured by Shinken Co.) in
a thermostat-controlled bath at 20°C, and the resulting vibration
characteristics were amplified by a mechanical impedance
amplifier ("XG-81" manufactured by RION Co.), whereby the
vibrational spectra were analyzed by an FFT spectrum analyzer
("FFT Spectrum Analyzer HP 3582A" manufactured by Yokogawa
Hewlett Packard Co.) to determine a loss factor from a peak in
the frequency range from 2 , 000 to 3 , 000 Hz . A higher loss factor
means a higher level of sound-insulating property.

(3) Measurement of Self-Adhesive Strength
Two samples (10 mm wide x 100 mm long) were cut from the
interlayer for laminated glass under the conditions of 23°C and
50%RH, and after they were positioned to overlap each other,
a roller weighing 2 kg was rolled back and forth twice over the
overlapped pieces in their lengthwise direction to make
pressure-bonding. After a double sided tape was bonded to one
side of the resultant test sample, it was fixed to a fixation
plate made of SUS via the double sided tape and subjected to
a 180° peeling test at a peeling rate of 500 mm/min to thereby
determine a peeling strength.
(4) Measurement of Visible Light Transmittance (Tv), Solar
Transmittance (Te), and Solar Reflectance (Re)
A visible light transmittance (Tv) at the wavelength of
380 to 780 nm, a solar transmittance (Te) at the wavelength of
300 to 2100 nm, and a solar reflectance (Re) at the wavelength
of 300 to 2100 nm were measured with a direct-recording
spectrophotometer ("UV-3100" manufactured by Shimadzu Corp.)
in accordance with JIS Z 8722 and JIS R 3106.


As can be seen from Table 2, the laminated glass produced
with the interlayer for laminated glass of Example 2-1 or 2-2
containing inorganic powder such as silica powder or calcium
carbonate powder has a higher loss factor than the laminated
glass produced with the interlayer for laminated glass of
Comparative Example2-1 containing no inorganic powder. These
results indicate that the laminated glasses of Examples 2-1 and
2-2 offer highly sound-insulating property.
Further, the interlayer for laminated glass containing
inorganic powder such as silica powder or calcium carbonate
powder has a lowered self-adhesive strength among the
interlayer-f ilms so that blocking is less likely to occur during
storage or handling.


(Examples of The Third Invention)
(Example 3-1)
(1) Production of Polyvinyl Butyral Resin (a) and Resin Layer
A-1
A quantity of 191 parts by weight of a polyvinyl alcohol
having an average degree of polymerization of 1700 and a degree
of saponification of 88.1 mol% was added to 2890 parts by weight
of purewater, followedby heating for dissolution . Thereaction
system, after its temperature was adjusted to 12°C, was admixed
with 201 parts by weight of a 35 wt% hydrochloric acid catalyst
and 148 parts by weight of n-butyraldehyde and maintained at
this temperature to allow the reaction product to precipitate.
Then, the reaction system was maintained at 45°C for 3 hours
to complete the reaction, washed with excessive water to wash
out unreacted n-butyraldehyde, treated with an aqueous sodium

hydroxide solution to neutralize the hydrochloric acid catalyst,
washed again with excessive water for 2 hours , and dried to give
a polyvinyl butyral resin (a) in the form of white powder. The
resin (a) was found to show an average degree of butyralization
of 63.8 mol% and a vinyl acetate content of 11.9 mol%.
A quantity of 100 parts by weight of the resin (a), 55 parts
by weight of triethylene glycol di-2-ethylbutyrate (3GH) as a
plasticizer, 8 parts by weight of silica powder having an average
particle size of 5 µm as fine-particle inorganic powder, 0.1
part by weight of 2-(2'-hydroxy-5'-methylphenyl)-
benzotriazole as a UV absorber, and 0.1 part by weight of t-butyl
hydroxytoluene as an antioxidant were mixed, and the mixture
was sufficientlymelt-kneadedwithamixingroll and press-molded
with a press-molding machine at 150°C for 30 minutes to produce
a resin layer A-1 having an average thickness of 0.2 mm.
(2) Production of Polyvinyl Butyral Resin (b) and Resin Layer
B
A quantity of 191 parts by weight of a polyvinyl alcohol
having an average degree of polymerization of 1700 and a degree
of saponification of 98.9 mol% was added to 2890 parts by weight
of pure water, followed by heating for dissolution. The reaction
system, after its temperature was adjusted to 12°C, was admixed
with 201 parts by weight of a 35 wt% hydrochloric acid catalyst
and 152 parts by weight of n-butyraldehyde, maintained at this
temperature to allow the reaction product to precipitate, then
maintained at 45°C for 3 hours to complete the reaction, washed
with excessive water to wash out unreacted n-butyraldehyde,
treated with an aqueous sodium hydroxide solution to neutralize
the hydrochloric acid catalyst, washedagain with excessive water

for 2 hours, and dried to give a polyvinyl butyral resin (b)
in the form of white powder. The resin (b) was found to have
an average degree of butyralization of 68.0 mol% and a vinyl
acetate content of .1.1 mol%.
A quantity of 100 parts by weight of the resin (b) , 40 parts
by weight of triethylene glycol di-2-ethylbutyrate (3GH) as a
plasticizer, 0.1 part by weight of 2-(2'-hydroxy-5'-
methylphenyl)benzotriazole as a UV absorber, and 0.1 part by
weight of t-butyl hydroxy toluene as an antioxidant were mixed,
and the mixture was then sufficiently melt-kneaded with a mixing
roll and press-molded at 150°C for 30 minutes with a press-molding
machine to produce a resin layer B having an average thickness
of 0.3 mm.
(3) Production of Interlayer for Laminated Glass and Laminated
Glass
The resin layers A-1 and B as used were stacked in the order
of resin layer B/resin layer A-1/resin layer B, and the stacked
resin layers were sandwiched between two transparent float glass
sheets (30 cm long x 30 cm wide x 2.5 cm thick). The stacked
assembly of the resin layers and glass sheets was placed in a
rubber bag, which was deaerated for 20 minutes under vacuum of
2.6kPa, transferred in an oven at 9 0°C, while keeping it deaerated,
and vacuum-pressed while maintaining it at 90°C for 30 minutes.
The thus preliminarily bonded laminated glass was subjected to
pressure-bonding in an air-type oven for 20 minutes under the
conditions of 135°C and 1.2 MPa of pressure to thereby carry
out the concurrent production of the interlayer and the laminate
glass sheet; namely, the interlayer for laminated glass and the
laminated glass were produced concurrently.

(Example 3-2)
(1) Production of Resin Layer A-2
A quantity of 100 parts by weight of the resin (a) , 40 parts
by weight of triethylene glycol di-2-ethylbutyrate (3GH) as a
plasticizer, 0.1 part by weight of 2- (2'-hydroxy-5'-
methylphenyl)benzotriazole as a UV absorber, 0.1 part by weight
of t-butyl hydroxytoluene as an antioxidant, and 10 parts by
weight of calcium carbonate having an average particle size of
3 \aa as fine -part icle inorganic powder were mixed, and the mixture
was sufficiently melt-kneaded with a mixing roll and press-
molded at 150°C for 30 minutes with a press-molding machine to
produce a resin layer A-2 having an average thickness of 0.20
mm.
(2) Production of Interlayer for Laminated Glass and Laminated
Glass
An interlayer for laminated glass and laminated glass were
produced concurrently in the same manner as described in Example
3-1 except that the resin layers A-l and B were used as stacked
in the order of resin layer B/resin layer A-2/resin layer B.
(Comparative Example 3-1)
(1) Production of Resin Layer A-3
A quantity of 100 parts by weight of the resin (a) , 55 parts
by weight of triethylene glycol di-2-ethylbutyrate (3GH) as a
plasticizer, 0.1 part by weight of 2-(2'-hydroxy-5'-
methylphenyl)benzotriazole as a UV absorber, and 0.1 part by
weight of t-butyl hydroxytoluene as an antioxidant were mixed,
and the mixture was sufficiently melt-kneaded with a mixing roll
and press-molded at 150°C for 30 minutes with a press-molding
machine to produce a transparent resin layer A- 3 having an average

thickness of 0.20 mm, which did not contain fine-particle
inorganic powder.
An interlayer and laminated glass were produced concurrently
in the same manner as described in Example 3-1 except that the
resin layers A-3 and B were used as stacked in the order of resin
layer B/resin layer A-3/resin layer B.
(Example 3-3)
(1) Production of Resin Layer A-4
A quantity of 100 parts by weight of the resin (a), 60 parts
by weight of triethylene glycol di-2-ethylbutyrate (3GH) as a
plasticizer, 3 parts by weight of fine ITO particles
(manufactured by Mitsubishi Materials) as heat-ray shielding
fine particles, 8 parts by weight of silica powder having an
average particle size of 5 µm as fine-particle inorganic powder,
0.1 part by weight of 2-(2'-hydroxy-5'-
methylphenyl)benzotriazole as a UV absorber, and 0.1 part by
weight of t-butyl hydroxy toluene as an antioxidant were mixed,
and the mixture was sufficiently melt-kneaded with a mixing
Rolland, press-molded with a press-molding machine at 150°C for
30 minutes to produce a resin layer A-4 having an average thickness
of 0.2 mm.
(2) Production of Interlayer for Laminated Glass and Laminated
Glass
An interlayer for laminated glass and laminated glass were
produced in the same manner as described in Example 3-1 except
that the resin layer A-1 was replaced with the resin layer A-4.
(Example 3-4)
(1) Production of Resin Layer B'
A quantity of 100 parts by weight of the resin (b) produced

in Example 3-1, 40 parts by weight of triethylene glycol
di-2-ethylbutyrate (3GH) as a plasticizer, 1 part by weight of
fine ITO particles (manufactured by Mitsubishi Materials) as
heat-ray shielding fine particles, 0.1 part by weight of
2 - (2 ' -hydroxy- 5 ' -methylphenyl) - benzotriazole as a UV absorber
and 0.1 part by weight of t-butyl hydroxy toluene as an antioxidant
were mixed, and the mixture was sufficiently melt-kneaded with
a mixing roll and press-molded with a press-molding machine at
150°C for 30 minutes to produce a resin layer B' having an average
thickness of 0.3 mm.
(2) Production of Interlayer for Laminated Glass and Laminated
Glass
An interlayer for laminated glass and a laminated glass
were produced in the same manner as described in Example 3-1
except that the resin layer B was replaced with the resin layer
B'.
(Example 3-5)
(1) Production of Resin Layer A-5
A quantity of 100 parts by weight of the resin (a) produced
in Example 3-1, 60 parts by weight of triethylene glycol
di-2-ethylbutyrate (3GH) as a plasticizer, 5 parts by weight
of fine ITO particles (manufactured by Mitsubishi Materials Co. )
as heat-ray shielding fine particles, 0.1 part by weight of
2-(2'-hydroxy-5'-methylphenyl)benzotriazole as a UV absorber,
0.1 part by weight of t-butyl-hydroxytoluene as an antioxidant,
and 10 parts by weight of calcium carbonate powder having an
average particle size of 3 µm as fine-particle inorganic powder
were mixed, and the mixture was sufficiently melt-kneaded with
a mixing roll and, press-molded with a press-molding machine

at 150°C for 30 minutes to produce a resin layer A-5 having an
average thickness of 0.20 mm.
(2) Production of Interlayer for Laminated Glass and Laminated
Glass
An interlayer for laminated glass and a laminated glass
were produced in the same manner as described in Example 3-2
except that the resin layer A-2 was replaced with the resin layer
A-5.
(Example 3-6)
An interlayer for laminated glass and a laminated glass
were produced in the same manner as described in Example 3-2
except that the resin layer B was replaced with the resin layer
B' obtained in Example 3-4.
(Evaluation)
For the laminated glasses produced individually in Examples
3-1 and 3-2 and Comparative Example 3-1, a haze value and a loss
factor were measured using the following methods. The
evaluation results are shown in Table 4.
For the laminated glasses produced individually in Examples
3-3 to 3-6, a haze value, a loss factor, a visible light
transmittance (Tv), a solar transmittance (Te), and a solar
reflectance (Re) were measured using the following methods. The
evaluation results are shown in Table 5.
(1) Measurement of Haze Value
A haze value against the rays of light at the wavelengths
of 340 to 1800 nm was measured with an integrating turbidimeter
(manufactured by Tokyo Denshoku) in accordance with JIS K 6714
"Methacryl Resin Plate for Aircrafts".
(2) Measurement of Loss Factor

A sample (25 mm wide x 300 mm long) was cut from the laminated
glass, and subjected to vibration by the use of a vibration
generator for damping tests ("G21-005D" manufactured by Shinken
Co., Ltd.) in a thermostat-controlled bath at 20°C. The
resulting vibration characteristics were amplified by a
mechanical impedance amplifier ("XG-81" manufactured by RION
Co., Ltd.) and the vibration spectra were analyzed by an FFT
spectrum analyzer ( "FFT spectrum analyzer HP 3582A" manufactured
by Yokogawa Hewlett Packard Co.) to determine a loss factor from
a peak in the frequency range from 2,000 to 3,000 Hz. A higher
loss factor means a higher level of sound-insulating property.
(3) Measurement of Visible Light Transmittance (Tv), Solar
Transmittance (Te), and Solar Reflectance (Re)
A visible light transmittance (Tv) at the wavelengths of
380 to 780 nm, a solar transmittance (Te) at the wavelengths
of 300 to 2100 nm, and a solar reflectance (Re) at the wavelengths
of 300 to 2100 nm were measured with a direct-recording
spectrophotometer ("UV-3100" manufactured by Shimadzu. Corp. )
in accordance with JIS Z 8722 and JIS R 3106.


As can be seen from Table 4, the interlayers for laminated
glass of Examples 3-1 and 3-2 which comprises a laminate of the
opaque and sound-insulating polyvinyl acetal resin layer (A)
containing silica powder or calcium carbonate powder as
fine-particle inorganic powder with the transparent polyvinyl
acetal resin layer (B) were found to provide the laminated glass
with a higher loss factor than the interlayer for laminated glass
of Comparative Example 3-1 which comprises a laminate of the
resin layers not being incorporated with inorganic powder.
Namely, such interlayers were shown to provide a laminated glass
with highly sound-insulating property.


(Examples of Fourth Invention)
(Example 4-1)
(1) Production of Polyvinyl Butyral Resin (a) and Resin Layer
A-1
A quantity of 191 parts by weight of a polyvinyl alcohol
having an average degree of polymerization of 1700 and a degree
of saponification of 88 .1 mol% were added to 2890 parts by weight
of purewater, followed by heat ingf or dissolution. Thereaction
system, after its temperature was adjusted to 12°C, was admixed

with 201 parts by weight of a 35 wt% hydrochloric acid catalyst
and 148 parts by weight of n-butyraldehyde, maintained at this
temperature to allow the reaction product to precipitate, then
maintained at 45°C for 3 hours to complete the reaction, washed
with excessive water to wash out unreacted n-butyraldehyde,
treated with an aqueous sodium hydroxide solution to neutralize
the hydrochloric acid catalyst, washed with excessive water
for 2 hours, and dried to give a polyvinyl butyral resin (a)
in the form of white powder. The resin (a) had an average degree
of butyralization of 63.8 mol% and a vinyl acetate content of
11.9 mol%.
A quantity of 100 parts by weight of the resin (a), 55 parts
by weight of triethylene glycol di-2-ethylbutyrate (3GH) as a
plasticizer, 0.1 part by weight of 2-(2'-hydroxy-5'-
methylphenyl)benzotriazole ("TINUVIN P" manufactured by
CIBA-GEIGY) as a UV absorber, and 0.1 part by weight of t-butyl
hydroxytoluene ("Sumilizer BHT" manufactured by Sumitomo
Chemical Co.) as an antioxidant were mixed, and the mixture was
sufficiently melt-kneaded with a mixing roll and press-molded
with a press-molding machine at 150°C for 30 minutes to produce
a resin layer A-1 having an average thickness of 0.15 mm.
(2) Production of Polyvinyl Butyral Resin (b) and Resin Layer
B-1
A quantity of 191 parts by weight of a polyvinyl alcohol
having an average degree of polymerization of 1700 and a degree
of saponification of 98.9 mol% was added to 2890 parts by weight
of purewater, f ollowed by heating for dissolution. Thereaction
system, after its temperature was adjusted to 12°C, was admixed
with a 35 wt% hydrochloric acid catalyst and 152 parts by weight

of n-butyraldehyde, maintained at this temperature to allow the
reaction product to precipitate, maintained at 45°C for 3 hours
to complete the reaction, washed with excessive water to wash
out unreacted n-butyr aldehyde, treated with an aqueous sodium
hydroxide solution to neutralize the hydrochloric acid catalyst,
washed again with excessive water for 2 hours, and dried to give
a polyvinyl butyral resin (b) in the form of white powder. The
resin (b) was found to show an average degree of butyralization
of 68.0 mol% and a vinyl acetate content of 1.1 mol%.
A quantity of 100 parts by weight of the resin (b) , 35 parts
by weight of triethylene glycol di-2-ethylbutyrate (3GH) as a
plasticizer, 0.1 part by weight of 2-(2'-hydroxy-5'-
methylphenyl)benzotriazole ("TINUVIN P" manufactured by
CIBA-GEIGY Co.) asaUV absorber, 0.1 part by weight of t-butyl
hydroxytoluene ("Sumilizer BHT" manufactured by Sumitomo
Chemical Co.) as an antioxidant, and 4 .0 parts by weight of silica
powder having an average particle size of 5 µm as inorganic fine
particles were mixed, and the mixture was sufficiently
melt-kneaded with a mixing roll and press-molded with a
press-molding machine at 150°C for 30 minutes to produce a resin
layer B-1 having an average thickness of 0.20 mm.
(3) Production of Resin Layer C
A 100 parts by weight quantity of the white powder of a
polyvinyl butyral resin (b) produced under the above item (2),
40 parts by weight of triethylene glycol di-2-ethylbutyrate (3GH)
as a plasticizer, 0.1 part by weight of 2-(2'-hydroxy-5'-
methylphenyl)benzotriazole ("TINUVIN P" manufactured by
CIBA-GEIGY Co. ) as a UV absorber, and 0 .1 part by weight of t-butyl
hydroxytoluene ("Sumilizer BHT" manufactured by Sumitomo

Chemical Co. ) as an antioxidant were mixed, and the mixture was
sufficiently melt-kneaded with a mixing roll and press-molded
with a press-molding machine at 150°C for 30 minutes to produce
a resin layer C having an average thickness of 0.30 mm.
(4) Production of Interlayer for Laminated Glass and Laminated
Glass
The above-described resin layers A-1, B-1, and C as used
were stacked in the order of resin layer B-1/resin layer A-1/resin
layer C, and sandwiched between two transparent float glass
sheets (30 cm long x 30 cm wide x 2.5 mm thick), and the sandwiched
body was then placed in a rubber bag, followed by deaeration
under a vacuum of 2.6 kPa for 20 minutes. The rubber bag was
transferred in an oven at 90°C, while being kept deaerated, and
vacuum-pressed while being furthermore maintained at 90°C for
30 minutes, and the thus preliminarily bonded laminated glass
was subjected to pressure-bonding in an air-type oven for 20
minutes under the conditions of 135°C and 1.2 MPa of pressure
to thereby carry out the concurrent production of an interlayer
and a laminated glass; namely, an interlay for laminated glass
and a laminated glass were produced concurrently.
(Example 4-2)
(1) Production of Resin Layer B-2
A quantity of 100 parts by weight of the resin (b) , 40 parts
by weight of triethylene glycol di-2-ethylbutyrate (3GH) as a
plasticizer, 0.1 part by weight of 2-(2'-hydroxy-5'-
methylphenyl)benzotriazole {"TINUVIN P" manufactured by
CIBA-GEIGY Co. ) asaUV absorber, 0 .1 part by weight of t-butyl
hydroxytoluene ("Sumilizer BHT" manufactured by Sumitomo
Chemical Co .) as an antioxidant, and 7 . 5 parts by weight of calcium

carbonate particles having an average particle size of 3 µm as
inorganic fine particles were mixed, and the mixture was
sufficiently melt-kneaded with a mixing roll and press-molded
with a press-molding machine at 150°C for 30 minutes to produce
a resin layer B-2 having an average thickness of 0.30 mm.
(2) Production of Interlayer for Laminated Glass and Laminated
Glass
An interlayer and a laminated glass were produced
concurrently in the same manner as described in Example 4-1 except
that the above-de scribed resin layers A-1 and B-2 were used as
stacked in the order of resin layer B-2/resin layer A-1/resin
layer B-2.
(Example 4-3)
(1) Production of Resin Layer B-3
A resin layer B-3 having an average thickness of 0.15 mm
was produced in the same manner as described in Example 4-2 except
that 7.5 parts by weight of calcium carbonate powder having an
average particle size of 3 µm used as inorganic fine particles
was replaced with 5 . 0 parts by weight of a dark red-brown pigment
obtained by mixing equal amounts of four pigments , namely carbon
black, C. I .Pigment red 207, C.I .Pigment blue 151 and C.I .Pigment
yellow 110.
(2) Production of Interlayer for Laminated Glass and Laminated
Glass
An interlayer and a laminated glass were produced
concurrently in the same manner as described in Example 4-1 except
that the above-described resin layers A-1, B-1 and C were used
as stacked in the order of resin layer B-3/resin layer C/resin
layer A-1/resin layer C.

(Example 4-4)
(1) Production of Resin Film A-2
A quantity of 100 parts by weight of the resin (a), 55 parts
by weight of triethylene glycol di-2-ethylbutyrate (3GH) as a
plasticizer, 0.1 part by weight of 2-(2'-hydroxy-5'-
methylphenyl)benzotriazole ("TINUVIN P" manufactured by
CIBA-GEIGY Co.) as a UV absorber, 0 .1 part by weight of t-butyl
hydroxytoluene ("Sumilizer BHT" manufactured by Sumitomo
Chemical Co.) as an antioxidant, and 8. 3 parts by weight of calcium
carbonate powder having an average particle size of 3 µm as
inorganic fine particles were mixed, and the mixture was then
sufficiently melt-kneaded with a mixing roll and press-molded
with a press-molding machine at 150°C for 30 minutes to produce
an opaque and sound-insulating resin layer A-2 having an average
thickness of 0.15 mm.
(2) Production of Interlayer for Laminated Glass and Laminated
Glass
An interlayer and a laminated glass were produced
concurrently in the same manner as described in Example 4-1 except
that the above-described resin layers A-2 and B-2 were used as
stacked in the order of resin layer B-2/resin layer A-2/resin
layer B-2.
(Comparative Example 4-1)
An interlayer and a laminated glass were produced
concurrently in the same manner as described in Example 4-1 except
that the above-described resin layers A-1 and C were used as
stacked in the order of resin C/resin A-1/resin layer C.
(Example 4-5)
(1) Production of Resin Layer A-3

A quantity of 100 parts by weight of the resin (a) obtained
in Example 4-1, 60 parts by weight of triethylene glycol
di-2-ethylbutyrate (3GH) as a plasticizer, 2.5 parts by weight
of fine ITO particles (manufactured by Mitsubishi Materials Co. )
as heat-ray shielding fine particles, 0.1 part by weight of
2-(2'-hydroxy-5'-methylphenyl)benzotriazole ("TINUVIN P"
manufactured by CIBA-GEIGY Co. ) as a UV absorber, and 0.1 part
by weight of t-butyl hydroxytoluene ("Sumilizer BHT"
manufactured by Sumitomo Chemical Co. ) as an antioxidant were
mixed, and the mixture was sufficiently melt-kneaded with a
mixing roll and press-molded with a press-molding machine at
150°C for 30 minutes to produce a resin layer A-3 having an average
thickness of 0.15 mm.
(2) Production of Interlayer for Laminated Glass and Laminated
Glass
An interlayer for laminated glass and a laminated glass
were produced in the same manner as described in Example 4-1
except that the resin layer A-1 was replaced with the resin layer
A-3.
(Example 4-6)
(1) Production of Resin Layer B-4
A quantity of 100 parts by weight of the resin (b) obtained
in Example 4-1, 40 parts by weight of triethylene glycol
di-2-ethylbutyrate (3GH) as a plasticizer, 3 parts by weight
of fine ITO particles (manufactured by Mitsubishi Materials Co.)
as heat-ray shielding fine particles, 0.1 part by weight of
2-(2'-hydroxy-5'-methylphenyl)benzotriazole ("TINUVIN P"
manufactured by CIBA-GEIGY Co.) as a UV absorber, 0.1 part by
weight of t-butyl hydroxytoluene ( "Sumilizer BHT" manufactured

by Sumitomo Chemical Co.) as an antioxidant, and 4.0 parts by-
weight of silica having an average particle size of 5 µm as
inorganic fine particles were mixed, and the mixture was
sufficiently melt-kneaded with a mixing roll and press-molded
at 150°C for 30 minutes with a press-molding machine to produce
a resin layer B-4 having an average thickness of 0.20 mm.
(2) Production of Interlayer for Laminated Glass and Laminated
Glass
An interlayer for laminated glass and a laminated glass
were produced in the same manner as described in Example 4-1
except that the resin layer B-1 was replaced with the resin layer
B-4.
(Example 4-7)
The interlayer for laminated glass and laminated glass were
produced in the same manner as described in Example 4-2 except
that the resin layer A-1 was replaced with the resin layer A-3
produced in Example 4-5.
(Example 4-8)
(1) Production of Resin Layer B-5
A quantity of 100 parts by weight of the above-described
resin (b), 43 parts by weight of triethylene glycol
di-2-ethylbutyrate (3GH) as a plasticizer, 4 parts by weight
of fine ITO particles (manufactured by Mitsubishi Materials Co. )
as heat-ray shielding fine particles, 0.1 part by weight of
2-(2'-hydroxy-5'-methylphenyl)benzotriazole ("TINUVIN P "
manufactured by CIBA-GEIGY Co.) as a UV absorber, 0.1 part by
weight of t-butyl hydroxytoluene ( "Sumilizer BHT" manufactured
by Sumitomo Chemical Co.) as an antioxidant, and 7.5 parts by
weight of calcium carbonate having an average particle size of

3 urn as inorganic fine particles were mixed, and the mixture
was sufficientlymelt-kneadedwithamixing roll and press-molded
with a press-molding machine at 1'50°C for 30 minutes to produce
a resin layer B-5 having an average thickness of 0.30 mm.
(2) Production of Interlayer for Laminated Glass and Laminated
Glass
An interlayer for laminated glass and a laminated glass
were produced in the same manner as described in Example 4-2
except that the resin layer B-2 was replaced with the resin layer
B-5.
(Example 4-9)
An interlayer for laminated glass and a laminated glass
were produced in the same manner as described in Example 4-3
except that the resin layer A-1 was replaced with the resin layer
A-3 produced in Example 4-5.
(Example 4-10)
(1) Production of Resin Layer B-6
A quantity of 100 parts by weight of the resin (b) obtained
in Example 4-1, 35 parts by weight of triethylene glycol
di-2-ethylbutyrate (3GH) as a plasticizer, 3.5 parts by weight
of fine ITO particles (manufactured by Mitsubishi Materials Co. )
as heat-ray shielding fine particles, 0.1 part by weight of
2-(2'-hydroxy-5'-methylphenyl)-benzotriazole ("TINUVTN P"
manufactured by CIBA-GEIGY Co.) as a UV absorber, 0.1 part by
weight of t-butyl hydroxy toluene ("Sumilizer BHT" manufactured
by Sumitomo Chemical Co.) as an antioxidant, and 5.0 parts by
weight of a dark red-brown pigment obtained by mixing equal
amounts of four pigments, namely carbon black, C.I.Pigment red
207, C.I.Pigment blue 151 and C.I.Pigment yellow 110, as

inorganic fine particles, were mixed, and the mixture was
sufficiently melt-kneaded with a mixing roll and press-molded
at 150°C for 30 minutes with a press-molding machine to produce
a resin layer B-6 having an average thickness of 0.30 mm.
(2) Production of Interlayer for Laminated Glass and Laminated
Glass
An interlayer for laminated glass and a laminated glass
were produced in the same manner as described in Example 4-3
except that the resin layer B-3 was replaced with the resin layer
B-6.
(Example 4-11)
(1) Production of Resin Layer A-4
A quantity of 100 parts by weight of the resin (a) as produced
in Example 4-1, 60 parts by weight of triethylene glycol
di-2-ethylbutyrate (3GH) as a plasticizer, 3 parts by weight
of fine ITO particles (manufactured by Mitsubishi Materials)
as heat-ray shielding fine particles, 0.1 part by weight of
2-(2'-hydroxy-5'-methylphenyl)-benzotriazole ("TINUVIN P"
manufactured by CIBA-GEIGY Co.) as a UV absorber, 0.1 part by
weight of t-butyl hydroxy toluene ( "Sumilizer BHT" manufactured
by Sumitomo Chemical Co.) as an antioxidant, and 8.3 parts by
weight of calcium carbonate particles having an average particle
size of 3 µm as inorganic fine particles were mixed, and the
mixture was sufficiently melt-kneaded with a mixing roll
press-molded with a press -molding machine at 150°C for 30 minutes
to produce an opaque and sound-insulating resin layer A-4 having
an average thickness of 0.15 mm.
(2) Production of Interlayer for Laminated Glass and Laminated
Glass

An interlayer for laminated glass and a laminated glass
were produced in the same manner as described in Example 4-4
except that the resin layer A-2 was replaced with the resin layer
A-4.
(Example 4-12)
(1) Production of Resin Layer B-7
A quantity of 100 parts by weight of the resin (b) obtained
in Example 4-1, 40 parts by weight of triethylene glycol
di-2-ethylbutyrate (3GH) as a plasticizer, 2 parts by weight
of fine ITO particles (manufactured by Mitsubishi Materials Co. )
as heat-ray shielding fine particles, 0.1 part by weight of
2-(2'-hydroxy-5'-methylphenyl)benzotriazole ("TINUVIN P"
manufactured by CIBA-GEIGY Co.) as a UV absorber, 0.1 part by
weight of t-butyl hydroxytoluene ("Sumilizer BHT" manufactured
by Sumitomo Chemical Co.) as an antioxidant, and 7.5 parts by
weight of calcium carbonate having an average particle size of
3 µm as inorganic fine particles were mixed, and the mixture
was sufficiently melt-kneaded with a mixing roll, press-molded
with a press-molding machine at 150°C for 30 minutes to produce
a resin layer B-7 having an average thickness of 0.30 mm.
(2) Production of Interlayer for Laminated Glass and Laminated
Glass
An interlayer for laminated glass and a laminated glass
were produced in the same manner as described in Example 4-7
except that the resin layer B-2 was replaced with the resin layer
B-7.
(Evaluation)
For the laminated glass sheets produced individually in
Examples 4-1 to 4-4 and Comparative Example 4-1, a haze value

and a loss factor were measured using the following methods.
The evaluation results are shown in Table 6.
For each of the laminated glass sheets produced in Examples
4-5 to 4-12, a haze value, a loss factor, a visible light
transmittance (Tv), a solar transmittance (Te), and a solar
reflectance (Re) were measured using the following methods . The
evaluation results of Examples 4-5 to 4-8 and Examples 4-9 to
4-12 are shown in Tables 7 and 8, respectively.
(1) Measurement of Haze Value
A haze value in the rays of light at the wavelengths of
340 to 1800 nm was measured with an integrating turbidimeter
(manufactured by Tokyo Denshoku Co. ) in accordance with JIS K
6714 "Methacryl Resin Plate for Aircraft".
(2) Measurement of Loss Factor
A sample (25 mm wide x 300 mm long) was cut from the laminated
glass, and subjected to vibration by the use of a vibration
generator for damping tests ("G21-005D" manufactured by Shinken
Co.) in a thermostat-controlled bath at 20°C. The resulting
vibration characteristics were amplified by a mechanical
impedance amplifier ("XG-81" manufactured by RION Co. ) and the
vibration spectra were analyzed by an FFT spectrum analyzer ( "FFT
Spectrum Analyzer HP 3582A" manufactured by Yokogawa Hewlett
Packard Co.) to determine a loss factor from the peak in the
frequency range from 2,000 to 3,000 Hz. A higher loss factor
means a higher level of sound-insulating property.
In the above-mentioned measurements, the laminated glass
was illuminated from the above with a 114 W incandescent lamp
for 30 minutes, whereby the loss factors were measured before
and after illumination with the incandescent lamp to determine

whether or not the laminated glass underwent a change in
sound-insulating property due to light illumination and als
the degree of such change.
(3) Measurement of Visible Light Transmittance (Tv), Solan
Transmittance (Te), and Solar Reflectance (Re)
A visible light transmittance (Tv) at the wavelengths oi
380 to 780 nm, a solar transmittance (Te) at the wavelengths
of 300 to 2100 nm, and a solar reflectance (Re) at the wavelengths
of 300 to 2100 nm were measured with a direct-recording
spectrophotometer ("UV-3100" manufactured by Shimadzu Corp.)
in accordance with JIS Z 8722 and JIS R 3106.







INDUSTRIAL APPLICABILITY
The laminated glass obtained by using the interlayer for
laminated glass of the present invention is suitably used in
the application fields where light shielding property is
particularly required, among roof and side window panes of
automobiles except windshields as well as windows of buildings,
and the like.

WE CLAIM :
1. An interlayer for laminated glass, which is
composed of an opaque and sound-insulating polyvinyl acetal
resin composition containing fine-particle inorganic powder
and 45 parts by weight or more of a plasticizer per 100
parts by weight of a polyvinyl acetal resin.
2. The interlayer for laminated glass as claimed in
claim 1, wherein the opaque and sound-insulating polyvinyl
acetal resin composition further contains heat-ray
shielding fine particles.
3. An interlayer for laminated glass, which comprises
at least two kinds of layers of (A) an opaque and sound-
insulating polyvinyl acetal resin layer containing fine-
particle inorganic powder and 45 parts by weight or more of
a plasticizer per 100 parts by weight of a polyvinyl acetal
resin, and (B) a transparent polyvinyl acetal resin layer,
the layers being laminated together.
4. The interlayer for laminated glass as claimed in
claim 3, wherein at least either one of (A) the opaque and
sound-insulating polyvinyl acetal resin layer and (B) the
transparent polyvinyl acetal resin layer contains heat-ray
shielding fine particles.

5. The interlayer for laminated glass as claimed in
any one of claims 1 to 4, wherein the fine-particle
inorganic powder is calcium carbonate or silica.
6. A laminated glass comprising at least two
transparent glass sheets, wherein the interlayer for
laminated glass as claimed in any one of claims 1 to 5 is
bonded between at least two glass sheets.
7. The laminated glass as claimed in claim 6, wherein
the laminated glass has a haze value of not less than 20%.


ABSTRACT

INTERMEDIATE FILM FOR LAMINATED GLASS AND LAMINATED GLASS
The present invention provides an interlayer for
laminated glass which comprises at least one layer composed
of an opaque ethylene-vinyl acetate copolymer resin
composition or opaque polyvinyl acetal resin composition,
and also provides the laminated glass using such
interlayers. The interlayer for laminated glass and the
laminated glass according to the present invention can
offer excellent privacy protection.

Documents:

03049-kolnp-2007-abstract.pdf

03049-kolnp-2007-claims 1.0.pdf

03049-kolnp-2007-claims 1.1.pdf

03049-kolnp-2007-correspondence others.pdf

03049-kolnp-2007-description complete.pdf

03049-kolnp-2007-form 1.pdf

03049-kolnp-2007-form 13.pdf

03049-kolnp-2007-form 3.pdf

03049-kolnp-2007-form 5.pdf

03049-kolnp-2007-gpa.pdf

03049-kolnp-2007-others.pdf

03049-kolnp-2007-priority document.pdf

3049-KOLNP-2007-(16-09-2011)-ABSTRACT.pdf

3049-KOLNP-2007-(16-09-2011)-AMANDED CLAIMS.pdf

3049-KOLNP-2007-(16-09-2011)-DESCRIPTION (COMPLETE).pdf

3049-KOLNP-2007-(16-09-2011)-EXAMINATION REPORT REPLY RECIEVED.pdf

3049-KOLNP-2007-(16-09-2011)-FORM 1.pdf

3049-KOLNP-2007-(16-09-2011)-FORM 2.pdf

3049-KOLNP-2007-(16-09-2011)-FORM 3.pdf

3049-KOLNP-2007-(16-09-2011)-OTHERS.pdf

3049-KOLNP-2007-(30-12-2011)-CORRESPONDENCE.pdf

3049-KOLNP-2007-ASSIGNMENT 1.1.pdf

3049-KOLNP-2007-ASSIGNMENT.pdf

3049-KOLNP-2007-CORRESPONDENCE OTHERS 1.1.pdf

3049-KOLNP-2007-CORRESPONDENCE.pdf

3049-KOLNP-2007-EXAMINATION REPORT.pdf

3049-KOLNP-2007-FORM 13.pdf

3049-KOLNP-2007-FORM 18 1.1.pdf

3049-kolnp-2007-form 18.pdf

3049-KOLNP-2007-FORM 3 1.2.pdf

3049-KOLNP-2007-FORM 3-1.1.pdf

3049-KOLNP-2007-FORM 5.pdf

3049-KOLNP-2007-GPA.pdf

3049-KOLNP-2007-GRANTED-ABSTRACT.pdf

3049-KOLNP-2007-GRANTED-CLAIMS.pdf

3049-KOLNP-2007-GRANTED-DESCRIPTION (COMPLETE).pdf

3049-KOLNP-2007-GRANTED-FORM 1.pdf

3049-KOLNP-2007-GRANTED-FORM 2.pdf

3049-KOLNP-2007-GRANTED-SPECIFICATION.pdf

3049-KOLNP-2007-REPLY TO EXAMINATION REPORT.pdf

3049-KOLNP-2007-TRANSLATED COPY OF PRIORITY DOCUMENT.pdf


Patent Number 253301
Indian Patent Application Number 3049/KOLNP/2007
PG Journal Number 28/2012
Publication Date 13-Jul-2012
Grant Date 11-Jul-2012
Date of Filing 20-Aug-2007
Name of Patentee SEKISUI CHEMICAL CO., LTD.
Applicant Address 4-4, NISHITENMA 2-CHOME, KITA-KU, OSAKA-SHI OSAKA
Inventors:
# Inventor's Name Inventor's Address
1 HASEGAWA, TSUYOSHI C/O SEKISUI CHEMICAL CO., LTD., 1259, IZUMI, MINAKUCHICHO, KOKA-SHI, SHIGA 528-8585
PCT International Classification Number C03C 27/12
PCT International Application Number PCT/JP2006/301510
PCT International Filing date 2006-01-31
PCT Conventions:
# PCT Application Number Date of Convention Priority Country
1 2005-162909 2005-06-02 Japan
2 2005-162910 2005-06-02 Japan
3 2005-278955 2005-09-26 Japan
4 2005-158081 2005-05-30 Japan
5 2005-278957 2005-09-26 Japan