Title of Invention

WETTABLE HYDROGELS COMPRISING REACTIVE, HYDROPHILIC, POLYMERIC INTERNAL WETTING AGENTS

Abstract The present invention relates to wettable silicone hydrogels comprising the reaction production of at least one siloxane containing component and at least one reactive, hydrophilic polymeric internal wetting agent. The present invention further relates to silicone hydrogel contact lenses comprising at least one oxygen permeable component, and an amount of reactive, hydrophilic polymeric internal wetting agent sufficient to impart wettability to said device.
Full Text WO 2006/039466 PCT/US2005/035149

In another example, reactive, hydrophilic polymeric IWAs can be made by
initiating the polymerization of a monomer (such as, for example, DMA) with a
5 lesser molar amount of an aroine-functionalized azo initiator (such as, for example,
2,2'-Azobis(2-mcthylpropionamide)dihydrochloride) and then reacting the amine
groups of the resulting low molecular weight polymers with materials containing
free radical polymerizable groups, such as 2-isocyanatoethyl methaerylate, 3-
isopropenyl-alpha, alpha-dimcthylbenzyl isocyanate, methacrylic anhydride, acrylic
10 acid, methacrylic acid, acryloyl chloride, or methacryloyl chloride. Examples of the
above compounds include low molecular weight hydrophilic polymers of Formulae
III and reactive, hydrophilic polymeric IWAs of Formulae IV.

WO 2006/039466 PCT/US2005/035149

In yet a further example, reactive, hydrophilic polymeric IWAs can also be
5 made by initiating the polymerization of a monomer (such as, for example, DMA)
with a lesser molar amount of a carboxylic acid-functionalized azo initiator (such as,
for example, 2,2'-Azobis[N-(2-carboxyethyl)-2-methylpropionamidine]tetrahydrate)
and then reacting the carboxylic acid groups of the resulting low molecular weight
hydrophilic polymer with materials containing free radical polymcrizable groups,
10 such as, for example, 2-arninoethyl methacrylate or 3-aminopropyl methacrylamide.
A person skilled in the art will recognize that incomplete reaction between
the low molecular weight hydrophilic polymer and the free radical polymerizable


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compound results in a mixture of products which include, in part, the starting low
molecular weight hydrophilic polymer, the reactive hydrophilic polymeric IWA, and
unreacted free radical polymerizable compounds. If low molecular weight
hydrophilic polymer is present in the final product mixture, it is not essential to
5 remove it from the product mixture. Instead, the low molecular weight hydrophilic
polymer may remain, serve as a diluent in the contact lens formulation and be
removed later during the purification of the lenses. Those of skill in the art will also
recognize that molecular weights of the reactive, hydrophilic polymeric IWAs will
vary depending on the reaction parameters, such as amount of initiator present,
10 reaction temperature, and monomer concentration. In addition, the presence of chain
transfer agents such thioglycolic acid and thiolactic acid can also be used to control
the molecular weights of the reactive, hydrophilic polymeric IWAs.
Examples of the above compounds include low molecular weight
hydrophilic polymers of Formulae V and reactive, hydrophilic polymeric internal
15 wetting agents of Formulae VI and VII.

WO 2006/039466 PCT/US2005/035149

One preferred class of reactive, hydrophilic polymeric IWAs include those
that contain a cyclic moiety in their backbone, more preferably, a cyclic amide or
5 cyclic imide. Reactive, hydrophilic polymeric IWAs include but are not limited to
macromers derived from poly-N-vinyl pyrrolidone, poly-N-vinyl-2-piperidone,
poly-N-vinyl-2-caprolactarn, poly-N-vmyl-3-methyl-2- caprolactam, poly-N-vinyl-
3-methyl-2-piperidone, poly-N-vinyl-4-methyl-2- piperidone, poly-N-vinyl-4-
methyl-2-caprolactam, poly-N-vinyl-3-ethyl-2~ pyrrolidone, and poly-N-vinyl-4,5-
10 dimethyl-2- pyrrolidone, polyvinylimidazole, poly-N-N-dimethylacrylamide,
polyvinyl alcohol, polyacrylic acid, polyethylene oxide, poly-2-(ethyl-oxa/,oline),

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heparin polysaceharides, polysaccharides, mixtures and copolymers (including block
or random, branched, mullichain, comb-shaped or star shaped) thereof where poly-
N-vinylpyrrolidonc (PVP) is particularly preferred. Copolymers might also be used
such as graft copolymers of PVP. These lactam containing polymers may also be
made reactive by treatment with alkali and transition metal borohydrides, such as
sodium borohydride (NaBH4), zinc borohydride, sodium triacetoxyborohydride,
bis(isopropoxytitanium) borohydride in solution, followed by reaction with suitable
polymerizable groups.
Another class of preferred reactive, hydrophilic polymeric IWAs include
reactive polymers and copolymers comprising pendant acyclic amide groups capable
of association with hydroxyl groups.
Examples of suitable reactive, hydrophilic polymeric IWAs include polymers
and copolymers comprising, in tire backbone, repeating units of Formula VIII

wherein Rc is a Cl to C3 alkyl group;
Ra is selected from H, straight or branched, substituted or unsubstituted Cl to
C4 alkyl groups,

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R is selected from H, straight or branched, substituted or unsubstituted Cl to
C4 alkyl groups, amino groups having up to two carbons, amide groups having up to
4 carbon atoms and alkoxy groups having up to two carbons and wherein the
number of carbon atoms in Ra and Rb taken together is 8, preferably 6 or less. As
5 used herein substituted alkyl groups include alkyl groups substituted with an aminc,
amide, ether or carboxy group.
In one preferred embodiment Ra and Rb are independently selected from H, and
substituted or unsubstituted Cl to C2 alkyl groups and preferably unsubstituted Cl to
C2 alkyl groups.
10 In another preferred embodiment Q is a direct bond, Ra and Rb are
independently selected from H, substituted or unsubstituted Cl to C2 alkyl groups.
Preferably the reactive, hydrophilic polymeric IWAs of the present invention
comprise a majority of the repeating unit of Formula Vlll, and more preferably at least
about 80 mole% of the repeating unit of Formula Vlll.
15 Specific examples of repeating units of Formula Vlll include repeating units
derived from N-vmyl-N-methylacetamide, N-vinylacetamide, N-vinyl-N-
methylpropionamido, N-vinyl-N-methyl-2-mcthylpropionamide, N-vinyl-2-
methylpropionamide, N-vinyl-N,N'-dhnethylurea, and the following acyclic
polyamides:
20

Additional repeating units may be formed from monomers selected from N-
vinyl amides, acrylamides, hydroxyalkyl (mcth) acrylates, alkyl (meth)aerylates or
25 other hydrophilic monomers and siloxane substituted acrylates or mcthacrylates.

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Specific examples of monomers which may be used to form reactive, hydrophilic
polymeric IWAs include as N-vinylpyrrolidone, NJsf-dimethylacrylamide, 2-
hydroxyethylmethacrylatc, vinyl acetate, acrylonitrile, methyl methacrylate,
hydroxypropyl methacrylate, 2-hydroxyethyl acrylate, and butyl methacrylate,
5 methacryloxypropyl tristrimethylsiloxysilane and the like and mixtures thereof.
Preferred additional repeating units monomers include of N-vinylpyrrolidone, N,N-
dimethylacrylamide, 2-hydroxyethylmcthacrylate and mixtures thereof.
in one embodiment the reactive, hydrophilic polymeric IWA comprises
poly(N-vmyl-N-methylacetainide).
10 In yet another embodiment the reactive, hydrophilic polymeric IWA
comprises a reactive high molecular weight copoiymcr derived from monomers
comprising vinyllactam monomers and vinyl carboxylate monomers. Preferably the
reactive high molecular weight copolymers have molecular weights (weight
average) of at least about 60,000 Daltons, more preferably between about 60,000 to
15 about 750,000 Daltons, more preferably still between about 100,000 to about
600,000 Daltons, and most preferably between about 180,000 to about 500,000
Daltons.
In one embodiment these reactive high molecular weight copolymers may be
synthesized in 3 steps. In the first step, a vinyllactam monomer and a vinyl
20 carboxylate monomer are copolymerized using a free radical initiator, resulting in a
high molecular weight hydrophilic copolymer. In the second step, the carboxylate
groups of the resultant copolymer are partially or completely hydrolyzed under
appropriate reaction conditions, resulting in a "modified" high molecular weight
copolymer that is capable of further reacting with one or more photo-polymerizable
25 compounds via hydroxyl groups on the polymer backbone. Partial hydrolysis gives
terpolymers comprising the units vinyllactam, vinyl alcohol, and vinyl carboxylate,
for example a terpolymer of vinylpyrrolidone, vinyl acetate, and vinyl alcohol. In
the third step, the modified high molecular weight hydrophilic copolymer is treated

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with a reactive group, as defined above, to generate the reactive, hydrophilic
polymeric IWA.
Suitable N-vinyllactams include N-vinyl-2-pyrrolidone, N-vinyl-2-
piperidone, N-vinyl-2-caprolactam, M-vinyl-3-methyl-2-pyrrolidone, N-vinyl-3-
5 methyl-2-piperidonc, N-vinyl-3-methyl-2-capralactam, N-vinyl-4-methyl-2-
pyrrolidone, N-vinyl-4-methyl-2-caprolactam, N-vinyl-5-methyl-2- pyrrolidone, N-
vinyl-5-melhyl-2-piperidone, N-vinyl-5,5-dimethyl-2- pyrrolidone, N-vinyl-3,3,5-
trimethyl-2-pyrrolidone, N-vinyl-5-mcthyl-5- cthyl-2-pyrrolidone, N-vinyl-3,4,5-
trimethyl-3-ethyl-2-pyrrolidone, N- vinyl-6-methyl-2-piperidone, N-vinyl-6-ethyl-2-
10 piperidone, N-vinyl-3,5-dimethyl-2-piperidone, N-vi nyl-4,4-dimethyl-2-piperidone,
N-vinyl-7-methyl-2-caprolactam, N-vinyl-7-ethyl-2-caprolactam, N-vinyl-3,5-
diraethyl-2-caprolactam, N-vinyl4,6-dimethyl-2-caprolactarn, N-vinyl-3,5,7-
trimethyl-2-caprolactaxn, N-vinylmaleimidc, vinylsuccinimide, mixtures thereof and
the like.
15 Preferred vinyllactams include heterocyclic monomers containing 4 carbon
atoms in the heterocyclic ring. A highly preferred vinyllactam is N-vinyl-2-
pyrrolidone.
Suitable vinyl carboxylate include compounds having both vinyl and
carboxylate functionality, preferably having up to 10 carbon atoms. Specific
20 examples of suitable vinyl carboxylates include vinyl heptanoate, vinyl hexanoatc,
vinyl pentanoate, vinyl butanoate, vinyl propanoate (vinyl propionate), vinyl
ethanoate (vinyl acetate), vinyl trifluoroacetate, mixtures thereof and the like. A
preferred vinyl carboxylate is vinyl acetate.
The high molecular weight copolymers may further comprise repeat units
25 derived from vinyl alcohols. Suitable vinyl alcohols include 2-hydroxyethyl 2-
methyl-2-propenoate, p-hydroxystyrene, 4-vinylbenzyl alcohol, dicthylene glycol
monomethacrylate, 2-[2-(2-hydroxyethoxy)ethoxy] ethyl 2-methyl-2-propenoate,
2,3-Dihydroxypropyl methacrylate, 2-hydroxy-l-(hydroxymethyl)ethyl 2-methyl-2-


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propenoatc, 2-hydroxyethyl aciylate, 2-hydroxypropyl acrylate, butanediol
monoacrylatc, butanediol monoinethacrylate, 3-[(4-ethenylphenyl)methoxy]-l ,2-
propanediol, 3-(etheiry]phenyi)mcthoxy-l,2-propanediol mix of ra-and p-isomers, 2-
(ethenylphenyl)methoxyacetic acid mixture of m- and p-isomers, xylitol 1-
5 methacrylate and xylitol 3-methacrylate, N-2-hydroxyethyl methacrylamide, N-2-
hydroxyethyl acryl amide.
A class of reactive, hydrophilic polymeric IWAs of this embodiment
comprise units in their polymer chain derived from the following monomer units (all
numbers are preceded by the word "about"):
10

Concentration (mole%)
Vinyllactam vinyl alcohol vinyl carboxylate Reactivegroup
85-99.9 0.1-15 0-15 0.1-15
85-99 0.1-10 0-10 0.1-10
85-99 0.1-10 0-5 0.1-5
The reactive, hydrophilic polymeric IWAs formed from high molecular
weight copolymers may also be formed from copolymers derived from polyamides,
polylactones, polyimides, polylactams and functionalized polyamides, polylactones,
15 polyimides, polylactams, polycarboxylates, such as N-vinyl-2-pyrrolidone (NVF)
and vinyl acetate (VA) functionalized by initiating the polymerization of NVP and
VA with a lesser molar amount of an azo initiator, hydrolyzing or partially
hydrolyzing the carboxylate groups, and then reacting the hydroxyl groups of the
resulting high molecular weight hydrophilic copolymcr with materials containing
20 radical polymerizable groups, such as 2-isocyanatoeth3'l methacrylate, methacrylic
anhydride, acryloyl chloride, or methacryloyl chloride to form the high molecular

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weight photo-polymerizable hydrophilic copolymer (HMWPPHC). Suitable azo
catalysts are known in the art and include AIBN, 2,2'-azobis{2-[l-(2-hydroxyethyl)~
2-imida/.olin-2-yl]propanc}dihydrochloride, 2,2'-azobis{2-methyl-N-[ 1,1 -
bis(hydroxymcthyl)-2-hydroxyethyl] propionamide, 2,2'-azobis[2~melhyl-N-(2-
5 hydroxyethyl)propionamide], 2,2'-azobis{2-methyl-N-[2-(l-
hydroxybutyl)|propionarnide}, 2,2'-azobis(2-methylpropionamide)dihydrochloride,
or 2,2'-azobis[N-(2-carboxyethyl)-2-methylpropionamidine|tetrahydrate). Reactive,
hydrophilic polymeric IWAs made with glycidyl methacrylate may also be used.
The glycidyl methacrylate ring can be opened to give a diol that may be used in
10 conjunction with another hydrophilic polymer in a mixed system to increase the
compatibility of the reactive, hydrophilic polymeric IWAs, compatibilizing
components and any other groups that impart compatibility. Examples of the above
described reactive, hydrophilic polymeric IWAs include compounds Formulae IX
and X
15

WO 2006/039466 PCT/US2005/035149

The reactive, hydrophilic polymeric IWAs may be used in amounts from
about 1 to about 15 weight percent, more preferably about 3 to about 15 percent,
5 most preferably about 5 to about 12 percent, all based upon the total of all reactive
components.
In some embodiments it is preferred that the reactive, hydrophilic polymeric
IWA be soluble in the diluent at processing temperatures. Manufacturing processes
that use water or water-soluble diluents may be preferred due to their simplicity and


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reduced cost. In these embodiments reactive, hydrophilic polymeric IWAs that are
water soluble at processing temperatures are preferred.
In addition to the reactive, hydrophilic polymeric IWAs, the hydrogels of the
present invention further comprise one or more silicone-contaimng components and,
5 optionally one or more hydrophilic components. The silicone-containing and
hydrophilic components used to make the polymer of this invention can be any of
the known components used in the prior art to make siliconc hydrogels. These terms
silicone-containing component and hydrophilic component are not mutually
exclusive, in that, the silicone-containing component can be somewhat hydrophilic
10 and the hydrophilic component can comprise some silicone, because the silicone-
containing component can have hydrophilic groups and the hydrophilic components
can have siliconc groups.
Further, silicone-containing componcnt(s) and hydrophilic components) can
be reacted prior to polymerization to form a prepolyrner which is later polymerized
15 in the presence of a diluent to form the polymer of this invention. When
prepolymers or macromers are used, it is preferred to polymerize at least one
silicone-containing monomer and at least one hydrophilic monomer in the presence
of the diluent, wherein the silicone-containing monomers and the hydrophilic
monomers differ. The term "monomer" used herein refers to low molecular weight
20 compounds (i.e. typically having number average molecular weights less than 700)
that can be polymerized. Thus, it is understood that the terms "silicone-containing
components" and "hydrophilic components" include monomers, macromonomers
and prepolymers.
A silicone-containing component is one thai contains at least one [—Si—O—
25 Si] group, in a monomer, rnacromer or prepolymer. Preferably, the Si and attached O
are present in the silicone-containing component in an amount greater than 20 weight
percent, and more preferably greater than 30 weight percent of the total molecular
weight of the silicone-containing component. Useful silicone-contaimng components

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preferably comprise polyrnerizable functional groups such as acrylatc, methacrylate,
acrylamide, rnethaerylamide, N-vinyl lactam, N-vinylamide, and styryl functional
groups. Examples of xilicone-containing components which are useful in this
invention may be found in U.S. Pat. Nos. 3,808,178; 4,120,570; 4,136,250; 4,153,641;
5 4,740,533; 5,034,461 and 5,070,215, and EP080539. All of the patents cited herein are
hereby incorporated in their entireties by reference. These references disclose many
examples of olefinic silicone-containing components.
Further examples of suitable silicone-containing monomers are
polysiloxanylalkyl(ineth)acrylic monomers represented by the following formula:
10
Formula XI

wherein: Z denotes II or lower alkyl and preferably II or methyl; X denotes O or
15 NR ; each R independently denotes hydrogen or methyl,
each R1-R3 independently denotes a lower alkyl radical or a phenyl radical, and
j is 1 or 3 to 10.
Examples of these polysiloxanylalkyl (meth)acrylic monomers include
methacryloxypropyl tris(trimcthylsiloxy) silane, pentamethyldisiloxanyl
20 methylmethacrylate, and inethyldi(trimethylsiloxy)methacryloxymethyl silane.
Methacryloxypropyl tris(trimethylsiloxy)silane is the most preferred.
One preferred class of silicone-containing components is a
poly(organosiloxane) prepolymer represented by Formula XII:
Formula XII

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wherein each A independently denotes an activated unsaturated group, such as an
ester or amide of an acrylic or a methacrylic acid or an alkyl or aryl group
(providing that at least one A comprises an activated unsaturated group capable of
5 undergoing radical polymerization); each of R5, R6, R7 and R8 are independently
selected from the group consisting of a monovalent hydrocarbon radical or a halogen
substituted monovalent hydrocarbon radical having 1 to 18 carbon atoms which may
have ether linkages between carbon atoms;
R denotes a divalent hydrocarbon radical having from 1 to 22 carbon atoms,
10 and
m is 0 or an integer greater than or equal to 1, and preferable 5 to 400, and
more preferably 10 to 300. One specific example is a, co-bismcthacryloxypropyl
poly-dimethylsiloxane. Another preferred example is mPDMS
(monomethacryloxypropyl terminated mono-n-butyl terminated
is polydimethylsiloxane).
Another useful class of silicone containing components includes silicone-
containing vinyl carbonate or vinyl carbamate monomers of the following formula:
Formula XIII

2 o wherein: Y denotes O, S or Nil; RSi denotes a silicone-containing organic radical; R
denotes hydrogen or lower alkyl, and preferably H or methyl; d is 1, 2, 3 or 4; and q
is 0 or 1. Suitable silicone-containing organic radicals RSi| include the following:

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Wherein p is 1 to 6; or an alkyl radical or a fluoroalkyl radical having 1 to 6
carbon atoms; e is 1 to 200; q is 1, 2, 3 or 4; and s is 0, 1, 2, 3, 4 or 5.
The siliconc-contain ing vinyl carbonate or vinyl carbamate monomers
specifically include: 1,3-bis[4-(vinyloxycarbonyloxy)but-l-yl]tetramethyl-isiloxane
3-(vmyloxycarbonylthio) propyl-[tris (trimethykiloxysilane]; 3-
[tris(trimethylsiloxy)silyl] propyl allyl carbamate; 3-[tris(trimeth)'lsiloxy)wilyl]
propyl vinyl carbamate; trimethylsilylethyl vinyl carbonate; trimethylsilylmethyl
vinyl carbonate, and

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Another class of silicone-containing components includes compounds of the
following formulae:
Formulae XIV-XV
5 (*D*A*D*G)fl *D*D*EI;
E(*D*G*D*A)a *D*G*D*E1 or;
E(*D*A*D*G)n *D*A*D*E1
wherein:
D denotes an alkyi diradical, an alkyl cycloalkyl diradical, a cycloalkyl
10 diradical, an aryl diradical or an alkylaryl diradical having 6 to 30 carbon atoms,
G denotes an alkyl diradical, a cycloalkyl diradical, an alkyl cycloalkyl
diradical, an aryl diradical or an alkylaryl diradical having 1 to 40 carbon atoms and
which may contain ether, thio or arnine linkages in the main chain;
* denotes a urethanc or ureido linkage;
15 a is at least 1;
A denotes a divalent polymeric radical of formula:
Formula XVI


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R independently denotes an alkyl or fluoro-substituted alkyl group having 1 to 10
carbon atoms which may contain ether linkages between carbon atoms; r is at least
1; and p provides a moiety weight of 400 to 10,000; each of E and E1 independently
denotes a polymcrizable unsaturated organic radical represented by formula:
5 Formula XVII

wherein: R12 is hydrogen or methyl; R13 is hydrogen, an alkyl radical having 1 to 6
10 carbon atoms, or a - CO -Y-R15 radical wherein Y is —O—,Y—S— or —Nil—;
R14 is a divalent radical having 1 to 12 carbon atoms; X denotes —CO— or —
OCO—; Z denotes —O— or —NH—; Ar denotes an aromatic radical having 6 to
30 carbon atoms; a is 0 to 6; b is 0 or 1; e is 0 or 1; and c is 0 or 1.
A preferred silicone-containing component is represented by the following
15 formula:
Formula XVIII

wherein R16 is a diradical of a diisocyanate after removal of the isocyanate group,
such as the diradical of isophorone diisocyanate. Another preferred silicone
20 containing macromer is compound of formula X (in which x + y is a number in the
range of 10 to 30) formed by the reaction of fluoroether, hydroxy-tenninated
polydimethylsiloxane, isophorone diisocyanate and isocyanatoethylmethacrylate.
Formula XIX

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Other silicone-containing components suitable for use in this invention
include those described is WO 96/31792 such as macromers containing
polysiloxane, polyalkylene ether, diisocyanate, polyfluorinated hydrocarbon,
5 polyfluorinated ether and polysaccharide groups. U.S. Pat. Nos. 5,321,108;
5,387,662 and 5,539,016 describe polysiloxancs with a polar fluorinated graft or side
group having a hydrogen atom attached to a terminal difluoro-substitutcd carbon
atom. Such polysiloxancs can also be used as the siliconc monomer in this
invention.
10 The hydrogels may further comprise hydrophilic components, such as those
which are capable of providing at least about 20% and preferably at least about 25%
water content to the resulting lens when combined with the remaining reactive
components. When present, suitable hydrophilic components may be present in
amounts up to about 60 weight %, preferably between about 10 to about 60
15 weight%, more preferably between about 15 to about 50 weight % and more
preferably still between about 20 to about 40 weight %, all based upon the weight of
all reactive components. The hydrophilic monomers that may be used to make the
polymers of this invention have at least one polymerizable double bond and at least
one hydrophilic functional group. Examples of functional groups with
20 polymerizable double bonds include acrylic, methacrylic, acrylamido,
rnethacrylarnido, fumaric, maleic, styryl, isopropenylphenyl, O-vinylcarbonate, O-
vinylcarbamate, allylic, O-vinylacetyl and N-vinyllactam and N-vinylamido double
bonds. Such hydrophilic monomers may themselves be used as crosslinking agents.

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"Acrylic-type" or "acrylic-containing" monomers arc those monomers containing
the acrylic group (CR'H=CRCOX)
wherein R is H or CH3, R" is II, alkyl or carbonyl, and X is 0 or N, which are also
known to polymerize readily, such as N,N-dimethylacrylarnide (DMA), 2-
5 hydroxyethyl acrylate , glycerol methacryiate, 2-hydroxyethyl methacrylamide,
polyethyleneglycol monomethacrylate, rnethacrylie acid, acrylic acid and mixtures
thereof.
Hydrophilic vinyl-containing monomers which may be incorporated into the
hydrogels of the present invention include monomers such as N-vinyl lactams (e.g.
10 N-vinyl pyrrolidone (N VP)), N-vinyl-N-methyl acctamide, N-vinyl-N-ethyl
acetamidc, N-vinyl-N-ethyl fonnamide, N-vinyl formamide, N-2-hydroxyethyl vinyl
carbamate, N-carboxy-B-alanine N-vinyl ester, with NVP being preferred.
Other hydrophilic monomers that can be employed in the invention include
polyoxyethylene polyols having one or more of the terminal hydroxyl groups
15 replaced with a functional group containing a polymerizable double bond.
Examples include polyethylene glycol with one or more of the terminal hydroxyl
groups replaced with a functional group containing a polymerizable double bond.
lixamples include polyethylene glycol reacted with one or more molar equivalents of
an end-capping group such as isocyanatoethyl methacryiate ("1EM"), methacrylic
20 anhydride, methacryloyl chloride, vinylbenzoyl chloride, or the like, to produce a
polyethylene polyol having one or more terminal polymerizable olefinic groups
bonded to the polyethylene polyol through linking moieties such as carbamate or
ester groups.
Still further examples are the hydrophilic vinyl carbonate or vinyl carbamate
25 monomers disclosed in U.S. Pat. No.5,070,215, and the hydrophilic oxazolone
monomers disclosed in U.S. Pat. No. 4,910,277. Other suitable hydrophilic
monomers will be apparent to one skilled in the art.

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More preferred hydrophilic monomers which may be incorporated into the
polymer of the present invention include hydrophilic monomers such as N,N-
dimethyl acrylamide (DMA), 2-hydroxyethyl acrylate, glycerol methacrylate, 2-
hydroxyetliyl methacrylamide, N-vinylpyrrolidonc (NVP), and polyethyleneglycol
5 monomethacrylate.
Most preferred hydrophilic monomers include DMA, NVP and mixtures
thereof.
When the reactive, hydrophilic polymeric IWAs of the present invention are
incorporated into a silicono hydrogel formulation, it may be desirable to include at
10 least one a hydroxyl containing component to help compatibilize the reactive,
hydrophilic polymeric 1WA of the present invention and the silicone containing
components. The hydroxyl containing component that may be used to make the
polymers of this invention have at least one polymerizable double bond and at least
one hydrophilic functional group. Examples of polymerizable double bonds include
15 acrylic, methacrylic, acrylamido, methacrylamido, fumaric, maleic, styryl,
isopropenylphcnyl, O-vinylcarbonate, O-vinylcarbamate, allylic, O-vinylacetyl and
N-vinyllactam and N-vinylamido double bonds. The hydroxyl containing
component may also act as a crosslinking agent. In addition the hydroxyl containing
component comprises a hydroxyl group. This hydroxyl group may be a primary,
20 secondary or tertiary alcohol group, and may be located on an allcyl or aryl group.
Examples of hydroxyl containing monomers that may be used include but are not
limited to 2-hydroxyethyl methacrylate, 2-hydroxyethyl acrylate, 2-hydroxyethyl
methacrylamide, 2-hydroxyethyl acrylamide, N-2-hydroxyethyl vinyl carbamate, 2-
hydroxyethyl vinyl carbonate, 2-hydroxypropyl methacrylate, hydroxyhexyl
25 methacrylate, hydroxyoctyl methacrylate and other hydroxyl functional monomers
as disclosed in U.S. Patents 5,006,622; 5,070,215; 5,256,751 and 5,311,223.
Preferred hydroxyl containining monomers include 2~hydroxyethyl methacrylate,
and hydroxyl functional monomers including silicone or siloxane functionalities,

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28
such as the hydroxyl-functionalized siliconc containing monomers disclosed in
WO03/022321, and the compatibilizing components comprising at least one active
hydrogen and at least one siloxane group as disclosed in WO03/022322, the
disclosure of which is incorporated herein by reference. Specific examples of
5 include 2-propenoic acid, 2- methyl-2-hydroxy-3-[3-| 1,3,3,3- tetramcthyl-1-
[trimethylsilyl)oxy]disiloxanyl]propoxy]propyl ester (which can also be named (3-
methaciyloxy-2-hydroxypropyloxy)propylbis(trimethylsiloxy)methylsilane), 3-
methacryloxy-2- hydroxypropyloxy)propyltris(trimethylsiloxy)silane, bis-3-
methacryloxy-2-hydroxypropyloxypropyl polydimethylsiloxane, 3-methacryloxy-2-
l0 (2-hydroxyethoxy)propyloxy) propylbis(trimethylsiloxy)methylsilane, N-2-
methacryloxyethyl-0-(methyl-bis-trimcthylsiloxy-3-propyl)silyl carbamate and
N,N,N',N'-tetrakis(3-mcthacryloxy-2-hydroxypropyl)-a,co-bis-3-aminopropyl-
polydimethylsiloxane and mixtures thereof include 2-hydroxyethyl methacrylate,
3 -mcthacryloxy-2-hydroxypropyloxy)propyIbis(trimethylsiloxy)methylsilane), 3 -
15 methacryloxy-2- hydroxypropyloxy)propyltris(trimethylsiloxy)silane and mixtures
thereof are preferred.
When a compatibilizing component is used, effective amounts of
compatibilizing component in the polymer formulation include about 5 percent
(weight percent, based on the total weight of the reactive components) to about 90
20 percent, preferably about 10 percent to about 80 percent, most preferably, about 20
percent to about 50 percent.
Alternatively the reactive, hydrophilic polymeric IWAs may be included in
hydrophilic hydrogels. Generally these hydrogels arc made from the hydrophilic
monomers listed above. Commercially available hydrogel formulations include, but
25 are not limited to etafilcon, polymacon, vifilcon, genfilcon A and lenefilcon A.
Generally the reactive components arc mixed in a diluent to form a reaction
mixture. Suitable diluents are known in the art.

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Classes of suitable diluents for silicone hydrogel reaction mixtures include
ethers, esters, alkanes, alkyl balides, silanes, amides, alcohols and combinations
thereof. Amides and alcohols are preferred diluents with alcohols having 2 to 20
carhons, amides having 10 to 20 carbon atoms derived from primary amines and
5 carboxylic acids having 8 to 20 carbon atoms. In some embodiments primary and
tertiary alcohols are preferred. Preferred classes include alcohols having 5 to 20
carhons and carboxylic acids having 10 to 20 carbon atoms.
Specific diluents which may be used include 1 -ethoxy-2-propanol,
diisopropylaminoethanol, isopropanol, 3,7-dimethyl-3-oetanol, 1-decanol, 1-
10 dodecanol, 1-octanol, 1-pentanol, 2-pentanol, 1-hexanol, 2-hcxanol, 2-octanol, 3-
methyl-3-pentanol, fert-amyl alcohol, tert-butanol, 2-butanol, 1-butanol, 2-methyl-2-
pentanol, 2-propanol, 1-propanol, ethanol, 2-ethyl-l-butanol, SiGMA acetate, l-lert-
butoxy-2-propanol, 3,3-dimethyl-2-butanol, tert-butoxyethanol, 2-octyl-l-
dodecanol, decanoic acid, octanoic acid, dodecanoic acid, 2-
15 (diisopropylamino)ethanol mixtures thereof and the like.
Preferred diluents include 3,7-dimethyl-3-octanol, 1-dodecanol, 1-decanol,
1-octanol, 1-pentanol, 1-hexanol, 2-hexanol, 2-octanol, 3-methyl-3-pentanol, 2-
pentanol, t-amyl alcohol, tert-butanol, 2-butanol, 1-butanol, 2-methyl-2-pentanol, 2-
ethyl-1 -butanol, ethanol, 3,3-dimethyl-2-butanol, 2-octyl-1-dodecanol, decanoic
20 acid, octanoic acid, dodecanoic acid, mixtures thereof and the like.
More preferred diluents include 3,7-dimethyl-3-octanol, 1-dodecanol, 1-
decanol, 1-octanol, 1-pentanol, 1-hexanol, 2-hexanol, 2-octanol, 1-dodecanol, 3-
methyl-3-pentanol, 1-pentanol, 2-pentanol, tert-amyl alcohol, tert-butanol, 2-
butanol, 1-butanol, 2-rnethyl-2-pentanol, 2-ethyl-l-butanol, 3,3-dimethyl-2-butanol,
25 2-octyl-1 -dodecanol, mixtures thereof and the like.
Suitable diluents for non-siliconc containing reaction mixtures include
glycerin, cthylene glycol, ethanol, rncthanol, ethyl acetate, methylene chloride,
polyethylene glycol, polypropylene glycol, low molecular weight PVP, such as

WO 2006/039466 PCT/US2005/035149
3 0
disclosed in US 4,018,853, US 4,680,336 and US 5,039,459, including, but not
limited to boric acid esters of dihydric alcohols, combinations thereof and the like.
Mixtures of diluents may be used. The diluents may be used in amounts up
to about 50% by weight of the total of all components in the reaction mixture. More
5 preferably the diluent is used in amounts less than about 45% and more preferably in
amounts between about 15 and about 40% by weight of the total of all components
in the reaction mixture.
In another embodiment, the diluent comprises a low molecular weight
hydrophilic polymer without photo-polymerizable reactive groups. The diluent may
10 also comprise additional components such as release agents. Suitable release agents
are water soluble and aid in lens deblocking.
It is generally necessary to add one or more cross-linking agents, also
referred to as cross-linking monomers, to the reaction mixture, such as ethylene
glycol dimcthacrylate ("EGDMA"), trimethylolpropane trimethacrylate
15 ("TMPTMA"), glycerol trimethacrylate, polyethylene glycol dimethacrylatc
(wherein the polyethylene glycol preferably has a molecular weight up to, e.g., about
5000), and other polyacrylate and polymethacrylate esters, such as the end-capped
polyoxyethylene polyols described above containing two or more terminal
methacrylate moieties. The cross-linking agents are used in the usual amounts, e.g.,
20 from about 0.000415 to about 0.0156 mole per 100 grams of reactive components in
the reaction mixture. (The reactive components are everything in the reaction
mixture except the diluent and any additional processing aids which do not become
part of the structure of the polymer.) Alternatively, if the hydrophilic monomers
and/or the silicone-containing monomers act as the cross-linking agent, the addition
25 of a crosslinking agent to the reaction mixture is optional. Examples of hydrophilic
monomers which can act as the crosslinking agent and when present do not require
the addition of an additional crosslinking agent to the reaction mixture include

WO 2006/039466 PCT/US2005/035149
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polyoxyethylenc polyols described above containing two or more terminal
methacrylatc moieties.
An example of a silicone-containing monomer which can act as a
crosslinking agent and, when present, does not require the addition of a crosslinking
5 monomer to the reaction mixture includes a, avbismethacryloxypropyl
polydimethylsiloxanc.
The reaction mixture may contain additional components such as, but not
limited to, UV absorbers, medicinal agents, antimicrobial compounds, reactive tints,
pigments, copolymerizable and nonpolymerizable dyes, release agents and
10 combinations thereof.
A polymerization catalyst or initiator is preferably included in the reaction
mixture. The polymerization initiators includes compounds such as lauryl peroxide,
bcnzoyl peroxide, isopropyl percarbonale, azobisisobutyronitrile, and the like, that
generate free radicals at moderately elevated temperatures, and photoinitiator
15 systems such as aromatic alpha-hydroxy ketones, alkoxyoxybenzoins,
acetophenones, acylphosphine oxides, bisacylphosphine oxides, and a tertiary aminc
plus a diketone, mixtures thereof and the like. Illustrative examples of
photoinitiators are 1-hydroxycyclohexylphenylketone, 2-hydroxy-2-methyl-l-
phenyl propan-1-onc, bi.s(2,6-dimethoxybcnzoyl)-2,4-4-trimethylpentyl phosphine
20 oxide (DMBAPO), bis(2,4,6~trimethylberizoyl)-phenyl phosphineoxidc (Irgacure
819), 2,4,6-trimethylbenzyldiphenyl phosphine oxide and 2,4,6-trimcthylbenzoyl
diphenylphosphine oxide, benzoin methyl ether and a combination of
camphorquinone and ethyl 4-(N,N-dimethylamino)bcnzoate. Commercially
available visible light initiator systems include Irgacure 819, Irgacure 1700, Irgacure
25 1800, Irgacure 819, Irgacure 1850 (all from Ciba Specialty Chemicals) and Lucirin
TPO initiator (available from BASF). Commercially available UV photoinitiators
include Darocur 1173 and Darocur 2959 (Ciba Specialty Chemicals). These and
other photoinitators which may be used are disclosed in Volume III, Photoinitiators

WO 2006/039466 PCT/US2005/035149
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for Free Radical Cationic & Anionic Photopolymerization, 2nd Edition by J.V.
Crivcllo & K. Dietliker; edited by G. Bradley; John Wiley and Sons; New York;
1998, which is incorporated herein by reference. The initiator is used in the reaction
mixture in effective amounts to initiate photopolymerization of the reaction mixture,
5 e.g., from about 0.1 to about 2 parts by weight per 100 parts of reactive monomer.
Polymerization of the reaction mixture can be initiated using the appropriate choice
of heat or visible or ultraviolet light or other means depending on the polymerization
initiator used. Alternatively, initiation can be conducted without a photoinitiator
using, for example, e-beam. However, when a photoinitiator is used, the preferred
10 initiators are bisacylphosphine oxides, such as bis(2,4,6-trimethylbenz,oyl)-phenyl
phosphinc oxide (Irgacure 819®) or a combination of l-hydroxycyclohexyl phenyl
ketone and bis(2,6-dimethoxybenzoyl)-2,4-4-trimethylpentyl phosphine oxide
(DMBAPO), and the preferred method of polymerization initiation is visible light.
The most preferred is bis(2,4,6-trimethylbeiizoyl)-phenyl phosphine oxide (Irgacure
15 81909).
The invention further comprises, consists and consists essentially of a
silicone hydrogel containing a covalently attached reactive, hydrophilic, polymeric
IWA and biomedical device, ophthalmic device and contact lenses formed from the
formulations shown below: (all numbers are preceded by the word "about")
20

Wt%
RHP1WA OPC HM OC
1-15 5-75, or5-60, or10-50 0-70, or5-60, or10-50 0-90, or10-80, or20-50
3-15 5-75, or5-60, or10-50 0-70, or5-60, or10-50 0-90, or10-80, or20-50
5-12 5-75, or5-60, or10-50 0-70, or5-60, or10-50 0-90, or10-80, or20-50

WO 2006/039466 PCT/US2005/035149
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RHHWA is reactive, hydrophilic polymeric internal wetting agent
OPC is oxygen permeable component
HM is hydrophilic monomer
CC is compatibilizirig component
5
The reaction mixtures of the present invention can be formed by any of the
methods know to those skilled in the art, such as shaking or stirring, and used to
form polymeric articles or devices by known methods.
For example, the biomedical devices of the invention may be prepared by
10 mixing reactive components and the diluent(s) with a polymerization initator and
curing by appropriate conditions to form a product that can be subsequently formed
into the appropriate shape by lathing, cutting and the like. Alternatively, the
reaction mixture may be placed in a mold and subsequently cured into the
appropriate article.
15 Various processes are known for processing the reaction mixture in the
production of contact lenses, including spincasting and static casting. Spincasting
methods are disclosed in U.S. Pat. Nos. 3,408,429 and 3,660,545, and static casting
methods are disclosed in U.S. Pat. Nos. 4,113,224 and 4,197,266. The preferred
method for producing contact lenses comprising the polymer of this invention is by
20 the molding of the silicone hydrogels, which is economical, and enables precise
control over the final shape of the hydrated lens. For this method, the reaction
mixture is placed in a mold having the shape of the final desired silicone hydrogel,
i.e., water-swollen polymer, and the reaction mixture is subjected to conditions
whereby the monomers polymerize, to thereby produce a polymer/diluent mixture in
25 the shape of the final desired product. Then, this polymer/diluent mixture is treated
with a solvent to remove the diluent and ultimately replace it with water, producing
a silicone hydrogel having a final size and shape which are quite similar to the size
and shape of the original molded polymer/diluent article. This method can be used

WO 2006/039466 PCT7US2005/035149
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to form contact lenses and is further described in U.S. Pat. Nos. 4,495,313;
4,680,336; 4,889,664; and 5,039,459, incorporated herein by reference.
The biomedical devices, and particularly ophthalmic lenses of the present
invention have a balance of properties which makes them particularly useful. Such
5 properties include clarity, water content, oxygen permeability and contact angle.
Thus, in one embodiment, the biomedical devices are contact lenses having a water
content of greater than about 17%, preferably greater than about 20% and more
preferably greater than about 25%.
As used herein clarity means substantially free from visible haze. Preferably
10 clear lenses have a haze value of less than about 150%, more preferably less than
about 100%.
Suitable oxygen permeabilities are preferably greater than about 40 barrer
and more preferably greater than about 60 barrer.
Also, the biomedical devices, and particularly ophthalmic devices and
15 contact lenses have contact angles (advancing) which are less than about 80°,
preferably less than about 70° and more preferably less than about 65°. In some
preferred embodiments the articles of the present invention have combinations of the
above described oxygen permeability, water content and contact angle. All
combinations of the above ranges are deemed to be within the present invention.
20 The non-limiting examples below further describe this invention.
The dynamic contact angle or DCA, was measured at 23°C, with borate
buffered saline, using a Wilhelmy balance. The wetting force between the lens
surface and borate buffered saline is measured using a Wilhelmy microbalance while
the sample strip cut from the center portion of the lens is being immersed into the
25 saline at a rate of 100 microns/sec . The following equation is used
F = 2γpcosθ or θ = cos-1(F/2γp)
where F is the wetting force, γ is the surface tension of the probe liquid, p is the
perimeter of the sample at the meniscus and 0 is the contact angle. Typically, two

WO 2006/039466 PCT/US2005/035149
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contact angles are obtained from a dynamic wetting experiment - advancing contact
angle and receding contact angle. Advancing contact angle is obtained from the
portion of the wetting experiment where the sample is being immersed into the
probe liquid, and these are the values reported herein. At least four lenses of each
5 composition are measured and the average is reported.
The water content was measured as follows: lenses to be tested were allowed
to sit in packing solution for 24 hours. Each of three test lens were removed from
packing solution using a sponge tipped swab and placed on blotting wipes which
have been dampened with packing solution. Both sides of the lens were contacted
10 with the wipe. Using tweezers, the test lens were placed in a weighing pan and
weighed. The two more sets of samples were prepared and weighed as above. The
pan was weighed three times and the average is the wet weight.
The dry weight was measured by placing the sample pans in a vacuum
oven which has been preheated to 60°C for 30 minutes. Vacuum was applied until
15 at least 0.4 inches Hg is attained. The vacuum valve and pump were turned off and
the lenses were dried for four hours. The purge valve was opened and the oven was
allowed reach atmospheric pressure. The pans were removed and weighed. The
water content was calculated as follows:
20 Wet weight = combined wet weight of pan and lenses - weight of weighing pan
Dry weight = combined dry weight of pan and lens - weight of weighing pan
% water content = (wet weight - dry weights x 100
wet weight
25 The average and standard deviation of the water content are calculated for the
samples are reported.
Modulus was measured by using the crosshead of a constant rate of
movement type tensile testing machine equipped with a load cell that is lowered to
the initial gauge height. A suitable testing machine includes an Instron model 1122.
3 0 A dog-bone shaped sample having a 0.522 inch length, 0.276 inch "ear" width and

WO 2006/039466 PCT/US2005/035149
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0.213 inch "neck" width was loaded into the grips and elongated at a constant rate of
strain of 2 in/min. until it broke. The initial gauge length of the sample (Lo) and
sample length at break (Lf) were measured. Twelve specimens of each composition
were measured and the average is reported. Tensile modulus was measured at the
5 initial linear portion of the stress/strain curve.
Haze is measured by placing a hydrated test lens in borate buffered saline in
a clear 20 x 40 x 10 mm glass cell at ambient temperature above a flat black
background, illuminating from below with a fiber optic lamp (Titan Tool Supply Co.
fiber optic light with 0.5" diameter light guide set at a power setting of 4-5.4) at an
10 angle 66° normal to the lens cell, and capturing an image of the lens from above,
normal to the lens cell with a video camera (DVC 1300C: 19130 RGB camera with
Navitar TV Zoom 7000 zoom lens) placed 14 mm above the lens platform. The
background scatter is subtracted from the scatter of the lens by subtracting an image
of a blank cell using EPIX XCAP V 1.0 software. The subtracted scattered light
15 image is quantitatively analyzed, by integrating over the central 10 mm of the lens,
and then comparing to a -1.00 diopter CSI Thin Lens®, which is arbitrarily set at a
haze value of 100, with no lens set as a haze value of 0. Five lenses are analyzed
and the results are averaged to generate a haze value as a percentage of the standard
CSI lens.
20 Oxygen permeability (Dk) may be determined by the polarographic method
generally described in ISO 9913-1: 1996(E), but with the following variations. The
measurement is conducted at an environment containing 2.1% oxygen. This
environment is created by equipping the test chamber with nitrogen and air inputs
set at the appropriate ratio, for example 1800 ml/min of nitrogen and 200 ml/min of
25 air. The t/Dk is calculated using the adjusted po2- Borate buffered saline was used.
The dark current was measured by using a pure humidified nitrogen environment
instead of applying MMA lenses. The lenses were not blotted before measuring.
Four lenses were stacked instead of using lenses of varied thickness. A curved

WO 2006/039466 PCT/US2005/035149
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sensor was used in place of a flat sensor. The resulting Dk value is reported in
barrers.
The following abbreviations are used throughout the Examples and have the
5 following meanings.

SiGMA 2-propenoic acid, 2-methyl-2-hydroxy-3- [3-[l,3,3,3-
tetramethyl-1 - [trimethylsilyl)oxy]disiloxanyl]propoxy]
propyl ester
DMA N,N-dimethylacrylamide
10 HEMA 2-hydroxyethyl methacrylate
mPDMS 800-1000 MW (Mn) monomethacryloxypropyl terminated
mono-n-butyl terminated polydimethylsiloxane
Norbloc 2-(2'-hydroxy-5-memacrylyloxyethylphenyl)-2H-
benzotriazole
15 CGI 1850 1:1 (weight) blend of 1-hydroxycyclohexyl phenyl ketone and
bis(2,6-dimethoxybenzoyl)- 2,4-4-trimethylpentyl phosphine
oxide
CGI 819 2,4,6-trimethylbenzyldiphenyl phosphine oxide
LMWHP low molecular weight hydrophilic polymer comprised of a
20 poly(N-vinyl pyrrolidone) backbone with either hydroxyl,
amine, carboxylic acid, or carboxylate end groups
HMWHC high molecular weight hydrophilic copolymer comprised of
poly(N-vinyl pyrrolidone)-co-(9-vinylcarbazole) (97.5/2.5)
RHPIWA reactive, hydrophilic polymeric IWA comprised of a poly(N-
25 vinyl pyrrolidone) backbone with covalently attached photo-
polymerizable end groups
IPA isopropyl alcohol
D3O 3,7-dimethyl-3-octanol

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TEGDMA tetraethyleneglycol dimethacrylate
EGDMA ethyleneglycol dimethacrylate
MMA methyl methaciylate
THF tetrahydrofiiran
5 Dioxane 1,4-dioxane
DMF N,N-dimethylfonnamide
DMAc N,N-dimethylacetamide
PVPlow Poly(N-vinyl pyrrolidone), -2500 MW
10 Example 1
9-Vinylcarbazole (0.79 gm, 4.1 mmol) (Aldrich, Milwaukee, WI), 2,2'-
Azobis[N-(2-carboxyethyl)-2-methylpropionamidine]tetrahydrate (0.16 gm, 0.46
mmol) (Wako Chemicals USA, St. Louis, MO) and freshly distilled N-vinyl-2-
pyrrolidone (NVP) (15.1 gm, 136 mmol) were added to a 250 mL round bottom
15 flask equipped with magnetic stirrer and nitrogen inlet. Methyl alcohol (19.2 gm)
and distilled water (23.4 gm) were added to the reaction mixture. The mixture was
degassed using 3 freeze-pump-thaw cycles and then allowed to warm to ambient
temperature. The reaction mixture was heated at 60°C for 16 hours, then precipitated
three times using acetone as asolvent to yield a white polymer with Mn, Mw, and
20 polydispersity values of 166,000,420,000, and 2.6, respectively. Molecular weights
were measured by gel permeation chromatography (GPC) using poly(2-
vinylpyridine) standards and hexafluoroisopropanol as mobile phase. 1H NMR
(D2O): A= 7.0-8.2 (bm, 8H, carbazole aromatic H), 3.4-3.8 (bm, 1H, -CH2CH-), 2.8-
3.3 (bm, 2H, -C[O]NCH2-), 2.0-2.4 (bm, 2H, -C[O]CH2-), 1.8-2.0 (bm, 2H, -
25 CH2CH2CH2-), 1.4-1.7 (bm, 2H, -CH2CH-).
Example 2

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9-Vinylcarbazole (Aldrich, Milwaukee, WI) (1.9 gm, 9.6 mmol), 2,2'-
azobis[N-(2-carboxyethyl)-2-methylpropionatnidine]tetrahydrate(Wako Chemicals
USA, St Louis, MO) (0.56 gm, 1.4 mmol) and freshly distilled N-vinyl-2-
pyrrolidone (NVP) (52.8 gm, 475 mmol) were added to a 1 L round bottom flask
5 equipped with magnetic stirrer and nitrogen inlet. Methyl alcohol (231.4 gm) was
added to the reaction mixture. The mixture was degassed using 3 freeze-pump-thaw
cycles and then allowed to warm to ambient temperature. The reaction mixture was
heated at 60°C for 4 hours, then isolated by precipitation (3 times) into diisopropyl
ether to yield a white polymer with Mn, Mw, and polydispersity values of 30,000,
10 110,000, and 3.7, respectively, using poly(2-vinylpyridine) standards and
hexafluoroisopropanol as mobile phase.
Example 3
Polymer from Example 2 (27.0 gm, 239 mmol), DMAC (173 gm), 4-
15 dimethylaminopyridine (DMAP, Avocado Research Chemicals, Heysham, England)
(1.2 gm, 9.6 mmol), pyridine (20 mL), methacrylic anhydride (Aldrich, Milwaukee,
WI) (7.43 g, 48.2 mmol) and hydroquinone (50 mg, 0.5 mmol, Aldrich, Milwaukee,
WI) were charged to a 500 mL round bottom flask equipped with magnetic stirrer
and nitrogen inlet. The reaction mixture was heated at 70°C for 6 hours and then
2 o isolated by precipitation into diisopropyl ether (three times) to afford a white solid
with Mn, Mw, and polydispersity values of 33,000,109,000, and 3.3, respectively,
using poly(2-vinylpyridine) standards and hexafluoroisopropanol as mobile phase.
Example 4
25 N-vinylpyrrolidone (50.0 gm, 450 mmol), 2-mercaptopropionic acid
(Aldrich, Milwaukee, WI) (0.97 g, 9.2 mmol), 9-vinylcarbazole (1.8 g, 9.2 mmol),
and 2,2,'-azobis[N-(2-carboxyethyl)-2-methylpropionamidine]tetrahydrate(Wako
Chemicals USA, St. Louis, MO) (0.53 gm, 1.3 mmol), DMAC (143 gm), and

WO 2006/039466 PCT/US2005/035149
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distilled water (40 mL) were charged to a 500 mL round bottom flask equipped with
a nitrogen inlet and magnetic stirrer. The reaction mixture was frozen using an
external CCVacetone bath and then placed under vacuum. The solution was
backfilled with nitrogen, thawed, and frozen again under vacuum for a total of 3
5 freeze-pump-thaw cycles. The solution was heated to 60°C under nitrogen for 6
hours. Hydroquinone (50 mg, 0.5 mmol, Aldrich, Milwaukee, WI) was added to the
reaction mixture, which was then cooled to 5°C. 1 -Hydroxybenzotriazole (Aldrich,
Milwaukee, WI) (3.7 gm, 28 mmol), 2-aminoethyl methacrylate hydrochloride
(Aldrich, Milwaukee, WI) (4.6 gm, 28 mmol), and l-[3-(dimethylamino)propyl]-3-
10 ethylcarbodiimide hydrochloride (EDC) (Aldrich, Milwaukee, WI) (5.3 gm, 28
mmol) were added and the mixture was stirred for 1 hour at 5°C, followed by an
additional 20 hours at room temperature. The reaction mixture was diluted with
DMAC (250 mL) and then poured slowly into 70:30 f-butyl methyl ether/hexanes to
precipitate out the white solid (90 percent). The polymer was dissolved in 2-
15 propanol and re-precipitated an additional 2 times. The resultant PVP macromer had
Mn, Mw, and polydispersity values of 41,000,155,000, and 3.7, respectively.
Example 5
N-vinylpyrrolidone (42.6 gm, 384 mmol), 9-vinylcarbazole (0.59 gm, 3.0
20 mmol), 2,2'-azobis{2-[l-(2-hydroxyethyl)-2-imidazolin-2-
yl]propane}dihydrochloride (Wako Chemicals USA, St. Louis, MO) (2.67 gm, 7.89
mmol), and methyl alcohol (160 gm) were charged to a 500 mL round bottom flask
equipped with a nitrogen inlet and magnetic stirrer. The reaction mixture was
subjected to 3 freeze-pump-thaw cycles and then heated to 60°C under nitrogen for
25 6 hours. The polymer was isolated as a white solid (85 percent) by precipitation into
diisopropyl ether 3 times and then dried.
The resultant polymer (15.8 gm, 141 mmol) was dissolved in anhydrous 1,4-
dioxane (Aldrich, Milwaukee, WI) (400 mL). Hydroquinone (50 mg, 0.5 mmol) was

WO 2006/039466 PCT/US2005/035149
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added to the reaction mixture, followed by 2-isocyanatoethyl methacrylate (Aldrich,
Milwaukee, WI) (2.2 gm, 14 mmol) and 100 microL of 0.33M stannous octoate
(made by dissolving stannous octoate (Aldrich, Milwaukee, WI) in anhydrous
toluene). The reaction mixture was heated to 70°C for 8 hours and then poured
5 slowly into diisopropyl ether to yield a white solid (88 percent). The polymer was
re-dissolved in 2-propanol and precipitated 2 additional times. The resultant PVP
macromer had Mn, Mw, and polydispersity values of 8,000,46,000, and 6.0,
, respectively.
10 Example 6
N-vinylpyrrolidone (50.4 gm, 453 mmol), 2-mercaptopropionic acid
(Aldrich, Milwaukee, WI) (1.0 gm, 9.2 mmol), 9-vinylcarbazole (1.78 gm, 9.4
mmol), and 2,2'-azobis(2-methylpropionamide)dihydrochloride (Wako Chemicals
USA, St. Louis, MO) (2.5 gm, 9.3 mmol), DMAC (150 gm), and distilled water (100
15 mL) were charged to a 500 mL round bottom flask equipped with a nitrogen inlet
and magnetic stirrer. The reaction mixture was frozen using an external CC2/acetone
bath and then placed under vacuum. The solution was backfilled with nitrogen,
thawed, and frozen again under vacuum for a total of 3 freeze-pump-thaw cycles.
The solution was heated to 60°C under nitrogen for 6 hours. Hydroquinone (50 mg,
20 0.5 mmol) was added to the reaction mixture, which was then cooled to 10°C. 1-
Hydroxybenzotriazole (3.9 gm, 30 mmol), 2-aminoethyl methacrylate hydrochloride
(4.6 gm, 28 mmol), and EDC (5.7 gm, 30 mmol) were added and the mixture was
stirred for 1 hour at 5°C, followed by an additional 40 hours at room temperature.
The reaction mixture was diluted with DMAC (200 mL) and then poured slowly into
25 70:30 The polymer was dissolved in 2-propanol and re-precipitated an additional 2 times.
The resultant PVP macromer had Mn, Mw, and polydispersity values of 9,800,
44,000, and 4.5, respectively.

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Example 7: Contact Lens Formation
The reaction components and diluent (tert-amyl alcohol) listed in Table 2
were mixed together with stirring, shaking, or rolling for at least about 3 hours at
5 23°C, until all components were dissolved. The reactive components are reported as
weight percent of all reactive components and the diluent and low molecular weight
PVP (PVP low) are weight percents of reaction mixture.
The reactive components were purged for approximately 15 minutes using
N2. Approximately 40-50 microliters of the reaction formulations were pipetted onto
10 clean polypropylene concave mold halves and covered with the complementary
polypropylene convex mold halves. The mold halves were compressed and the
mixtures were cured at 55°C for about 30 minutes in the presence of visible light
(0.4 mW/cm2 using Philips TL 20W/03T fluorescent bulbs, as measured by an
International Light radiometer/photometer). The molds were allowed to cool to room
15 temperature. The top mold halves were removed and the lenses gently removed
using tweezers. The lenses were released in water at 90°C for about 20 minutes and
then placed in vials containing borate buffered packing solution.

20 Table 2
Example
7A 7B 7C 7D 7E 7F
Component
SiGMA 30.5 30.5 30.5 30.5 30 30
Ex l 6.1 0 0 0 0 0
Ex 2 0 6.1 0 0 0 0
Ex 3 0 0 6.1 0 0 0
Ex 4 0 0 0 6.1 0 0
Ex 5 0 0 0 0 6 0
Ex 6 0 0 0 0 0 6
DMA 31.5 31.5 31.5 31.5 31 31
mPDMS 22.3 22.3 22.3 22.3 22 22

WO 2006/039466 PCT/US2005/035149

-43 -
HEMA 8.6 8.6 8.6 8.6 8.5 8.5
Norbloc 0 0 0 0 1.5 1.5
CGI 1850 0 0 0 0 0 0
CGI 819 0.23 0.23 0.23 0.23 0.23 0.23
TEGDMA 0 0 0 0 0 0
EGDMA 0.76 0.76 0.76 0.76 0.75 0.75
PVPlow 11 11 11 11 11 11
t-amyl 29 29 29 29 29 29
alcohol
percent
The reactive, hydrophilic polymeric IWAs (RHPIWA) were synthesized in
the presence of small amounts (~ 1 mol percent) of fluorescent vinyl monomers.
5 Covalently attached fluorescent "probes", or fluorophores, were used to detect the
diffusion of unreacted monomers from the production of the reactive, hydrophilic
polymeric IWAs from the contact lenses. The concentration of fluorescent probe in
the RHPIWA is low enough so that the physical properties of the labeled RHPIWA
are similar to that of unlabeled RHPIWA.
10 The fluorescent probes and fluorescently labeled macromers were first tested
to determine whether conditions necessary to make lenses, such as for example, light
intensity and heat, affect the emission of fluorescence of the fluorophore. The
resultant fluorescently labeled macromers were then combined with reactive
components and diluents to make contact lenses. The release of PVP macromers
15 labeled with fluorescent carbazole groups was measured from the extraction media
using a Shimadzu RF5301-PC spectrofluorometer (excitation λ = 343 nm, emission
λ - 348 nm, slit width = 3 nm). A standard calibration curve of PVP macromer
standards was used to correlate the amount of PVP macromer release from lenses.
As a control, a high molecular weight hydrophilic copolymer (HMWHC) was used
20 based on PVP (containing 2.5 mol percent carbazole groups) with Mn, Mw, and PD
values of 94,800, 511,000, and 5.4, respectively. The molecular weight of the
internal wetting agent (Mn), and amount of internal wetting agent extracted after 50-

WO 2006/039466 PCT/US2005/035149

- 44 -

100 hrs are shown in Table 3.
Table 3
Ex.# 7A 7B 7C 7D 7E 7F
Mn 166,000 30,000 33,000 41,000 8,000 9,800
Extraction 100 104 96 52 102 99
Time (hrs)
Internal 420 (2.6) 110 109 155 46 (6.0) 44 (4.5)
wetting agent (3.7) (3.3) (3.7)
Mwx 10-3
(PDI)
Percent 12 50 35 5 25 20
wetting agent
released
The results of Examples 7A through 7F show that the reaction mixture
s components and their amounts may be varied. All lenses showed low haze.
The reactive, hydrophilic polymeric internal wetting agents in Examples 7C
through 7F) were comparable or lower in molecular weight than the low molecular
weight hydrophilic polymer of Example 2 (used in formulation 7B) having no
photo-polymerizable groups. The percent release of the reactive, hydrophilic
10 polymeric IWAs (Examples 7C-F) from contact lenses was lower (5-35%) as
compared to polymers without photo-polymerizable groups (Example 7B, 50%).
Example 7A used a non-reactive high molecular weight hydrophilic copolymers.
Figure 1 shows the percent of internal wetting agent loss in IPA as a function of
time. Example 7D, which comprises a reactive, hydrophilic polymeric IWA lost less
15 than about 5% of the IWA, while Example 7A (which contained a non-reactive
hydrophilic, polymeric IWA) lost about 12% of the IWA. Based on Example 4,
comparable and even slower release rates can be achieved using lower molecular
hydrophilic polymeric IWAs with photo-polymerizable end group(s).
The Examples also show that reactive, hydrophilic polymeric IWAs may be
20 synthesized using several synthetic routes, and resulting in resulting in reactive,

WO 2006/039466 PCT/US2005/035149
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hydrophilic polymeric IWAs with different structures, particularly at the end groups.
The lenses from Example 7F were analyzed to determine contact angle,
water content and mechanical properties. The results are shown in Table 4, below.

Table 4
Advancing contact angle 52°
Water content 45.2%
Modulus ll0psi
Elongation at break 124%
5
Thus the reactive, hydrophilic polymeric IWAs produce contact lenses with
desirable properties.
Example 8
10 Reactive, hydrophilic polymeric IWA was synthesized as in Example 3,
except without the use of 9-vinylcarbazole to yield a white polymer with Mn, Mw,
and polydispersity values of 38,000,113,000, and 3.0, respectively.
Example 9
15 Reactive, hydrophilic polymeric IWA was synthesized as in Example 4,
except without the use of 9-vinylcarbazole to yield a white polymer with Mn, Mw,
and polydispersity values of 34,500,138,000, and 4.0, respectively.
Example 10
20 Reactive, hydrophilic polymeric IWA was synthesized as in Example 5,
except without the use of 9-vinylcarbazole to yield a white polymer with Mn, Mw,
and polydispersity values of 8,500,42,000, and 4.9, respectively.
Example 11

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Reactive, hydrophilic polymeric IWA was synthesized as in Example 6,
except without the use of 9-vinylcarbazole to yield a white polymer with Mn, Mw,
and polydispersity values of 10,000,40,000, and 4.0, respectively.
5 Example 12: Contact Lens Formation
Lenses containing the reactive, hydrophilic polymeric internal wetting agents
of Examples 8-11 (no fluorophore) were made as in Example 7. The cure intensity,
temperature, and time were maintained 4.0 mW/cm2,55°C, and 12 minutes,
respectively. Again, low haze was observed in all lenses.
10
Example 13
NVP (50.5 gm, 454 mmol), vinyl acetate (6.7 gm, 78 mmol), 9-
Vinylcarbazole (1.0 gm, 5.4 mmol), 2,2'-Azobis[N-(2-carboxyethyl)-2-
methylpropionamidine]tetrahydrate (0.578 gm, 1.39 mmol), methyl alcohol (170
15 gm), and distilled water (27 gm) were added to a 500 mL round bottom flask
equipped with magnetic stirrer and nitrogen inlet. The mixture was degassed using 3
freeze-pump-thaw cycles and then allowed to warm to ambient temperature. The
reaction mixture was heated at 60°C for 6 hours, and then isolated by precipitation
(3 times) into diisopropyl ether to yield a white polymer. The polymer was
20 redissolved in distilled water (1 L) and NaOH was added (3.6 gm, 89 mmol). The
reaction mixture was heated to 70°C for 4 hours and then concentrated by rotary
evaporation of the solvent. The polymer was precipitated from cold acetone,
redissolved in 2 L distilled water, and dialyzed for 72 hours against water and 48
hours against isopropyl alcohol using 3500 molecular weight cut-off Spectra/Por®
25 dialysis membrane (purchased from VWR). The polymer was isolated by removal of
solvent to yield an off-white solid with Mn, Mw, and polydispersity values of
49,000,191,000, and 3.9, respectively.

WO 2006/039466 PCT/US2005/035149
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Example 14
The high molecular weight polymer product from Example 13 (21 gin, 200
mmol), anhydrous triethylamine (11.6 gm, 115 mmol), 4-(dimethylamino)pyridine
(Aldrich, Milwaukee, WI) (6.1 gm, 50 mmol), hydroquinone (Aldrich, Milwaukee,
5 WI) (50 mg, 0.5 mmol) and anhydrous 1,4-dioxane (300 mL) were charged to a 500
mL round bottom flask equipped with a nitrogen inlet and magnetic stirrer.
Methacryloyl chloride (Aldrich, Milwaukee, WI) (6.0 gm, 57 mmol) was added
dropwise to the reaction mixture. The mixture was subsequently heated at 60°C for 4
hours. The polymer was isolated by precipitation into 50/50 t-butyl methyl
10 ether/hexanes to yield an off-white solid with Mn, Mw, and polydispersity values of
54,000, 200,000, and 3.7, respectively.
Example 15
NVP (50.7 gm, 457 mmol), vinyl acetate (3.7 gm, 43 mmol), 9-
15 vinylcarbazole (0.90 gm, 4.9 mmol), 2,2'-Azobis[N-(2-carboxyethyl)-2-
methylpropionamidine]tetrahydrate (0.38 gm, 0.91 mmol), methyl alcohol (75 gm),
and distilled water (75 gm) were added to a 500 mL round bottom flask equipped
with magnetic stirrer and nitrogen inlet The mixture was degassed using 3 freeze-
pump-thaw cycles and then allowed to warm to ambient temperature. The reaction
20 mixture was heated at 60°C for 18 hours, and then isolated by precipitation (3 times)
into 50/50 diisopropyl ether/hexanes to yield a white polymer. The polymer was
redissolved in distilled water (1 L) and NaOH was added (1.7 gm, 43 mmol). The
reaction mixture was heated to 60°C for 6 hours and then concentrated by rotary
evaporation of the solvent at 60°C. The polymer was precipitated from 70/30
25 acetone/hexanes, redissolved in 2 L distilled water, and dialyzed for 72 hours against
water and 48 hours against isopropyl alcohol using 3500 molecular weight cut-off
Spectra/Por® dialysis membrane (purchased from VWR). The polymer was isolated

WO 2006/039466 PCT/US2005/035149
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by removal of solvent to yield an off-white solid with Mn, Mw, and polydispersity
values of 86,000,310,000, and 3.6, respectively.
Example 16
5 The high molecular weight polymer product from Example 15 (25 gm, 240
mmol), hydroquinone (Aldrich, Milwaukee, WI) (50 mg, 0.5 mmol), 2-
isocyanatoethyl methacrylate (Aldrich, Milwaukee, WI) (3.21 gm, 20.4 mmol) and
100 millililters of 0.33M stannous octoate [made by dissolving stannous octoate
(Aldrich, Milwaukee, WI) in anhydrous toluene], and anhydrous 1,4-dioxane (300
10 mL) were charged to a 500 mL round bottom flask equipped with a nitrogen inlet
and magnetic stirrer. The reaction mixture was heated to 70°C for 8 hours and then
poured slowly into diisopropyl ether to yield a white solid (92 percent). The polymer
was dissolved in 2-propanol and precipitated 2 additional times affording an off-
white solid with Mn, Mw, and polydispersity values of 86,000, 320,000, and 3.7,
15 respectively.
Example 17
The reaction components and diluent (tert-amyl alcohol) listed in Table 3
were mixed together and processed to make lenses in accordance with the procedure
20 described in Example 7, above.
In one embodiment, reactive, hydrophilic polymeric IWAs were synthesized
in the presence of small amounts (~ 1 mol percent) of fluorescent vinyl monomers.
The general structure is shown in Formulae XIX, where 9-vinylcarbazole units are
present between 0.1 and 2 mol percent.
25

WO 2006/039466 PCT/US2005/035149

Small amounts of covalently attached fluorescent "probes", or fluorophores,
were used to detect the diffusion of the polymers listed in Table 3 from contact
5 lenses, as described in Example 7. The lens compositions, molecular weight of the
internal wetting agent, and amount of internal wetting agent extracted after 50-100
hrs are shown in Table 5, below.

WO 2006/039466 PCT/US2005/035149
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Table 5
Component 17A 17B 17C 17D 17E 17F
SiGMA 30.5 30.5 30.5 30.5 30 30
Ex l 6.1 0 0 0 0 0
Ex 2 0 6.1 0 0 0 0
Ex 13 0 0 6.1 0 0 0
Ex 14 0 0 0 6.1 0 0
Ex 15 0 0 0 0 6.1 0
Ex 16 0 0 0 0 0 6.1
DMA 31.5 31.5 31.5 31.5 31.5 31.5
MPDMS 22.3 22.3 22.3 22.3 22.3 22.3
HEMA 8.6 8.6 8.6 8.6 8.6 8.6
Norbloc 0 0 0 0 0 0
CGI 819 0.23 0.23 0.23 0.23 0.23 0.23
TEGDMA 0 0 0 0 0 0
EGDMA 0.76 0.76 0.76 0.76 0.76 0.76
PVPlow 11 11 11 11 11 11
t-amyl 29 29 29 29 29 29
alcohol %
Percent PVP macromer released from lens after extraction in 2-propanol
Extraction 100 104 98 96 100 99
Time (hrs)
IWA Mwx 420 110 191 200 310 320 (3.7)
10-3 (PDI) (2.6) (3.7) (3.9) (3.7) (3.6)
Weight % 12 50 26 0.3 18 0.4
release of
IWA
The results of Examples 17A through F show that the reaction mixture
5 components and their amounts may be varied. All lenses showed low haze.
As shown in Table 5, the rate of release of the polymers without reactive
groups (Examples 17C and 17E) was faster than that of the high molecular weight
control (Example 17A) and slower than that of the low molecular weight control
(Example 17B) after ~100 hours in isopropanol. Examples 17D and 17F, which
10 contained reactive, hydrophilic polymeric IWAs of the present invention, displayed

WO 2006/039466 PCT/US2005/035149
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insignificant release of the internal wetting agents. This is significant since
preservation of the internal wetting agent helps maintain lens wettability in addition
to other previously described lens properties since the initial weight percent of
components in the reaction mixture remains relatively constant after curing and
5 extraction in organic solvents.
Example 18
Synthesis was carried out as in Example 13 without the use of 9-
vinylcarbazole. In addition, methyl alcohol in the reaction mixture was replaced by
10 an equal weight of distilled water. Polymer Mn, Mw, and polydispersity was:
45,000,225,000, and 5.0.
Example 19
Synthesis was carried out as in Example 14 without the use of 9-
15 vinylcarbazole. In addition, methyl alcohol in the reaction mixture was replaced by
an equal weight of distilled water. Polymer Mn, Mw, and polydispersity were:
49,000,230,000, and 4.7.
Examples 20
20 Lenses containing the low molecular weight hydrophilic polymer of Example
18 and the reactive, hydrophilic polymer IWA of Example 19 were made as in
Example 17 using similar amounts of reaction components, but without the addition
of fluorophore. The cure intensity, temperature, and time were similarly held at 4.0
mW/cm2, 55°C, and 12 minutes, respectively. Low haze was observed in all lenses.
25

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What is claimed is:
1. A silicone hydrogel formed from a reaction mixture comprising at least
one oxygen permeable component and at least one reactive, hydrophilic polymeric
5 internal wetting agent.
2. The hydrogel of claim 1 wherein said internal wetting agent has a Mw of
about 5,000 to about 2,000,000 Daltons.
3. The hydrogel of claim 1 wherein said internal wetting agent has a Mw of
about 5,000 to about 180,000 Daltons.
10 4. The hydrogel of claim 1 wherein said internal wetting agent has a Mw of
about 5,000 to about 150,000 Daltons.
5. The hydrogel of claim 1 wherein said internal wetting agent has a Mw of
about 60,000 to about 2,000,000 Daltons.
6. The hydrogel of claim 1 wherein said internal wetting agent has a Mw of
is about 1800,000 to about 1,500,000 Daltons
7. The hydrogel of claim 1 comprising a mixture of reactive, hydrophilic
polymeric IWAs.
8. The hydrogel of claim 1 wherein said internal wetting agent is derived from
at least one polymer selected from the group consisting of polyamides, polylactones,
20 polyimides, polytectams and functionalized polyamides, polylactones, polyimides,
polylactams and copolymers and mixtures thereof.
9. The hydrogel of claim 1 wherein said internal wetting agent is derived from
at least one polymer selected from the group consisting of polymers of Formulae of II,
IV, VI and VH
25 Formula II

WO 2006/039466 PCT/US2005/035149


WO 2006/039466 PCT7US2005/035149



10. The hydrogel of claim 1 wherein said internal wetting agent is derived
from at least one polymer comprising repeating units of Formula VIII
5



wherein Q is a direct bond,

10 wherein Rc is a Cl to C3 alkyl group;
Ra is selected from H, straight or branched, substituted or unsubstituted Cl to
C4 alkyl groups,
Rb is selected from H, straight or branched, substituted or unsubstituted Cl to
C4 alkyl groups, amino groups having up to two carbons, amide groups having up to
15 4 carbon atoms and alkoxy groups having up to two carbons and wherein the


WO 2006/039466 PCT/US2005/035149
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number of carbon atoms in Ra and Rb taken together is 8, preferably 6 or less. As
used herein substituted alkyl groups include alkyl groups substituted with an amine,
amide, ether or carboxy group.
5 11. The hydrogel of claim 1 wherein said reactive, hydrophilic polymeric
internal wetting agent is present in an amounts from about 1 to about 15 weight
percent, based upon total weight of all reactive components.
12. The hydrogel of claim 1 wherein said internal wetting agent is present in an
amounts from about 3 to about 15 percent, based upon total weight of all reactive
10 components.
13. The hydrogel of claim 1 wherein said internal wetting agent is present in an
amounts from about 5 to about 12 percent, based upon total weight of all reactive
components.
15
14. The hydrogel of claim 10 wherein said internal wetting agent further
comprises repeating units selected from the group consisting of N-vinylpyrrolidone,
N,N-dimethylacrylamide, 2-hydroxyethylmethacrylate, vinyl acetate, acrylonitrile,
methyl methacrylate, siloxane substituted acrylates or methacrylates, alkyl
20 (meth)acrylates and mixtures thereof.
15. The hydrogel of claim 10 wherein said internal wetting agent further
comprises repeating units selected from the group consisting of N-vinylpyrrolidone,
N,N-dimethylacrylamide, 2-hydroxyethylmethacrylate and mixtures thereof.
25
16. The hydrogel of claim 10 wherein said repeating unit comprises N-vinyl-
N-methylacetamide.

WO 2006/039466 PCT/US2005/035149
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17. The hydrogel of claim 1 wherein said oxygen permeable component
comprises at least one silicone containing component.
18. The hydrogel of claim 17 wherein said at least one silicone containing
5 component is selected from the group consisting of silicone containing monomers,
silicone containing macromers and mixtures thereof.
19. The hydrogel of claim 17 wherein said at least one silicone containing
component is selected from the group consisting of polysiloxyalkyl(meth)acrylic
10 monomers, poly(organosiloxane) prepolymers, silicone containing vinyl carbonate
monomers, silicone containing vinyl carbamate monomers, and mixtures thereof.
20. The hydrogel of claim 1 further comprising at least one hydrophilic
monomer.
15
21. The hydrogel of claim 20 wherein said hydrophilic monomer is present
in amounts up to about 60 weight % based upon weight of all reactive components.
22. The hydrogel of claim 20 wherein said hydrophilic monomer is present
20 in amounts between about 10 to about 60 weight%, based upon weight of all reactive
components.
23. The hydrogel of claim 20 wherein said hydrophilic monomer is present
in amounts between about 20 to about 40 weight %, based upon weight of all
25 reactive components.
24. The hydrogel of claim 20 wherein said hydrophilic monomer is selected
from the group consisting of N,N-dimethyl acrylamide (DMA), 2-hydroxyethyl

WO 2006/039466 PCT/US2005/035149
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acrylate, 2-hydroxyethyl methactylate, glycerol methacrylate, 2-hydroxyethyl
methacrylamide, N-vinylpyrrolidone, polyethyleneglycol monomethacrylate, and
mixtures thereof.
5 25. The hydrogel of claim 1 further comprising at least one compatibilizing
component.
26. The hydrogel of claim 25 wherein said compatibilizing component is
selected from hydroxyl containing monomers and macromers.
10
27. The hydrogel of claim 25 wherein said compatibilizing component is
selected from the group consisting of 2-hydroxyethyl methacrylate, 2-hydroxyethyl
acrylate, 2-hydroxyethyl methacrylamide, 2-hydroxyethyl acrylamide, N-2-
hydroxyethyl vinyl carbamate, 2-hydroxyethyl vinyl carbonate, 2-hydroxypropyl
15 methacrylate, hydroxyhexyl methacrylate, hydroxyoctyl methacrylate and hydroxyl
functional monomers comprising silicone or siloxane groups and mixtures thereof.
28. The hydrogel of claim 25 wherein said compatibilizing component is
selected from the group consisting of 2-hydroxyethyl methacrylate, 3-methacryloxy-
20 2-hydroxypropyloxy)propylbis(trimethylsiloxy)methylsilane, 3-methacryloxy-2-
hydroxypropyloxy)propyltris(trimethylsiloxy)silane, bis-3-methacryloxy-2-
hydroxypropyloxypropyl polydimethylsiloxane, 3-methacryloxy-2-(2-
hydroxyethoxy)propyloxy) propylbis(trimethylsiloxy)methylsilane, N-2-
methacryloxyethyl-O-(methyl-bis-trimethylsiloxy-3-propyl)silyl carbamate and
25 N,N,N',N'-tetrakis(3-methacryloxy-2-hydroxypropyl)-α,ω-bis-3-aminopropyl-
polydimethylsiloxane and mixtures thereof.
29. The hydrogel of claim 25 wherein said compatibilizing component is
selected from the group consisting of 2-hydroxyethyl methacrylate, 3-methacryloxy-

WO 2006/039466 PCT/US2005/035149
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2-hydroxypropyloxy)propylbis(trimethylsiloxy)methylsilane), 3-methacryloxy-2-
hydroxypropyloxy)propyltris(trimethylsiloxy)silane and mixtures thereof.
30. The hydrogel of claim 25 wherein said compatibilizing component is
5 present in amounts between about 5 to about 90 weight percent, based on total
weight of the reactive components.
31. The hydrogel of claim 25 wherein said compatibilizing component is
present in amounts between about 10 to about 80 weight percent based on total
weight of the reactive components.
10
32. The hydrogel of claim 25 wherein said compatibilizing component is
present in amounts between about 20 to about 50 weight percent, based on total
weight of the reactive components.
15 33. A contact lens formed from the hydrogel of claim 1.
34. The hydrogel of claim 1 wherein said reactive, hydrophilic polymeric
IWA comprises a reactive high molecular weight copolymer derived from
monomers comprising vinyllactam monomers and vinyl carboxylate monomers.
20 35. The hydrogel of claim 34 wherein said reactive, hydrophilic polymeric
IWA has a molecular weight (weight average) of at least about 60,000 Daltons.
36. The hydrogel of claim 34 wherein said reactive, hydrophilic polymeric
IWA has a molecular weight (weight average) of between about 60,000 to about
750,000 Daltons.
25 37. The hydrogel of claim 34 wherein said reactive, hydrophilic polymeric
IWA has a molecular weights (weight average) of between about 180,000 to about
500,000 Daltons.

WO 2006/039466 PCT/US2005/035149
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38. The hydrogel of claim 34 wherein said vinyllactams monomers are
selected from the group consisting of N-vinyl-2-pyrrolidone, N-vinyl-2-piperidone,
N-vinyl-2-caprolactam, N-vinyl-3-methyl-2-pyrrolidone, N-vinyl-3-methyl-2-
piperidone, N-vinyl-3-methyl-2-caprolactam, N-vinyl-4-methyl-2- pyrrolidone, N-
5 vinyl-4-methyl-2-caprolactam, N-vinyl-5-methyl-2- pyrrolidone, N-vinyl-5-methyl-
2-piperidone, N-vinyl-5,5-dimethyl-2- pyrrolidone, N-vinyl-3,3,5-trimethyl-2-
pyrrolidone, N-vinyl-5-methyl-5- ethyl-2-pyrrolidone, N-vinyl-3,4,5-trirnethyl-3-
ethyl-2-pyrrolidone, N- vinyl-6-methyl-2-piperidone, N-vinyl-6-ethyl-2-piperidone,
N-vinyl-3,5-dimethyl-2-piperidone, N-vi nyl-4,4-dimethyl-2-piperidone, N-vinyl-7-
10 methyl-2-caprolactam, N-vinyl-7-ethyl-2-caprolactam, N-vinyl-3,5- dimethyl-2-
caprolactam, N-vinyl4,6-dimethyl-2-caprolactam, N-vinyl-3,5,7-trimethyl-2-
caprolactam, N-vinylmaleimide, vinylsuccinimide and mixtures thereof.
39. The hydrogel of claim 34 wherein said vinyllactam monomers are
selected from the group consisting of heterocyclic monomers containing 4 carbon
15 atoms in the heterocyclic ring.
40. The hydrogel of claim 34 wherein said vinyllactams monomer comprises
N-vinyl-2-pyrrolidone.
41. The hydrogel of claim 34 wherein said vinyl carboxylate monomers are
selected from the group consisting of compounds having 1 to 10 carbon atoms and
20 bom vinyl and carboxylate functionality.
42. The hydrogel of claim 34 wherein said vinyl carboxylate monomers are
selected from the group consisting of vinyl heptanoate, vinyl hexanoate, vinyl
pentanoate, vinyl butanoate, vinyl propanoate (vinyl propionate), vinyl ethanoate
(vinyl acetate) and mixtures thereof.
25 43. The hydrogel of claim 34 wherein said vinyl carboxylate monomer
comprises vinyl acetate.
44. The hydrogel of claim 34, wherein said reactive, hydrophilic polymeric
IWA is selected from the group consisting of compounds of Formula DC, X

WO 2006/039466 PCT/US2005/035149

and mixtures thereof.

The present invention relates to wettable silicone hydrogels comprising the reaction
production of at least one siloxane containing component and at least one reactive,
hydrophilic polymeric internal wetting agent. The present invention further relates to
silicone hydrogel contact lenses comprising at least one oxygen permeable component,
and an amount of reactive, hydrophilic polymeric internal wetting agent sufficient to
impart wettability to said device.

Documents:

http://ipindiaonline.gov.in/patentsearch/GrantedSearch/viewdoc.aspx?id=9KcTWsh+9NiM/O1f15b7Mw==&loc=wDBSZCsAt7zoiVrqcFJsRw==


Patent Number 271381
Indian Patent Application Number 1084/KOLNP/2007
PG Journal Number 08/2016
Publication Date 19-Feb-2016
Grant Date 18-Feb-2016
Date of Filing 28-Mar-2007
Name of Patentee JOHNSON & JOHNSON VISION CARE, INC
Applicant Address 7500 CENTURION PARKWAY, SUIT 100 JACKSONVILLE, FL 32256 U.S.A.
Inventors:
# Inventor's Name Inventor's Address
1 STEPHEN C. ARNOLD 24 OAKWOOD VILLAGE APARTMENT 6, FLANDERS, NEW JERSEY 07836
2 WALTER R. LAREDO 34 FOXHILL LANE, HILLSBOROUGH, NEW JERSEY, 08844
3 KEVIN MCCABE 1053 WATERFALL DRIVE, JACKSONVILLE, FLORIDA 32225
4 SUSAN ORR 4213 TRADEWINDS DRIVE, JACKSONVILLE, FLORIDA 32250
5 AZAAM ALLI 3489 ADVANTAGE LANE, JACKSONVILLE, FLORIDA 32277
PCT International Classification Number G02B 1/04
PCT International Application Number PCT/US2005/035149
PCT International Filing date 2005-09-28
PCT Conventions:
# PCT Application Number Date of Convention Priority Country
1 10/954,559 2004-09-30 U.S.A.