Title of Invention

A METHOD OF PREPARING TEXTURE-COATED SILICA

Abstract Texture-coated silica can be prepared by spraying a fumod silica with water and a coating agent, for example a thermoplastic elastomer,/wnnc mixing in a suitable mixing vessel, then milling and subsequently drvitfe tne mixture. The texture-coated silica can be used as a delusterme aeent in/acquers and for improving the soft feel.
Full Text

Text-are-coatad silica
The invention relates to a "exture-coated sixjjuci, ^J ct process for its preparation and to its use
An. aerogel-like textured silica is known f r£m DiLJ2£_A£~-£3-$. That siiica is prepared by incorporating water with uniform distribution, into an air-dispersed fumed siiica and drying the resulting pulverulent mixcure.
That silica has the disadvantage that Ax has a pronounced tendency to sedimentation and can be re disdersed onlv with difficulty or not at ail.
Document j)E 15 92 363 describes organically modified precipitated silicas which are coated, for example, with a wax and can be used as delustering agents. Those known silicas exhibit poor transparency in various lacquer systems. Owing to their nigh moisture content, those silicas cannot be used An moisture-curing polyurethane systems. Lacquer systems that cannot readily be delustered, such as poly^rethane and epoxy lacquer systems, cannot be delusteted satisfactorily using the known silicas.
The object is, therefore to prepare a silica that does not exhibit those disadvantages.
The invention provided a texture-coated silica- In a preferred embodiment of the invention, the texture-coated silica can have a carbon content of from 1 to 3D wt.%. The silica according to the invention can have a BET surface area of from 30 to 450 m2 g. It can have a tamped density of from 10 to 100 q l. The DBP number can be from 2.4 to 3.8.
A 4 % aqueous suspension of the silica according to the invention can have a pH value of from 5 to 8.

Texture-coated means that the end product i The texture-coated silica according to the invention can be prepared by spraying a fumed silica with water and a coating agent while mixing in a suitable mixing vessel, then milling and subsequently drvinc the mixture.
Any known fumed silica can be used the fumed silica".
In a preferred embodiment of the invention, the fumed silicas according ro Table i can pe used.
Fumed silica are known from Ul Imann's Encyklopadie der technischen Chemie 4th edtion valume 21, pages 464 ff (1982).
They are prepared by means of flame hydrolysis, in which a vaporizable metal compound or metalloid compound, such as, for example, silicon tetrachloride, are burnt in a flame with gases containing hydrogen and oxygen.

JIS K 5l6l l (not screened) 8) based on material ignited for
3) following DIN ISO 787 11, 2 hours at 1000°C
ASTM D 280 JIS K 5101 21 9) -special packaging that protects
4) following DlN 55921, from moisture
ASTM D 1Z08, JIS K -5101 23 10) HCI content is a constituent of the
5) following DIN ISO 797 IX, ignition loss
ASTM D 1208, JIS K 5101 24 11) V product is supplied in 20 kg bags
6) follow ng DIN ISO 787 XVIII, 12) W product is at present supplied
JIS K 5101 20 only from the Rheinfalden factory

Of the fumed silicas listed' in Table 1, there can preferably be used all types of Aerosil with he exception of AEROSIL OX50, including' the uncomoressed Variants.
Thermoplastic elastomers can be used as coating agent. The thermoplastic elastomers can be used in the form of aqueous and or solvent-containing dispersions. Particular preference is given to the use, as thermoplastic elastomers, of'"dimethylpolysiloxane elastomers having terminal epoxy groups, especially having a molecular weight of greater than' 100,000.
The thermoplastic elsatomers can be prepared by:
(I) mixing,
(A) a rheologically stable polyamide resin having a melting point or glas^s transition temperature of 25.degree.c to 278. degree. c,
(B) a silicone base comprising
(Bf) 100 parts by weight of a diorganopolysiloxane gum having a plasticity of at least 30 and having an average of At least 2 alkenyl groups in its molecule and
(Blf) 5 to 200 parts by weight of a reinforcing filler, the weight ratio of said silicone base to said polyamide resin beinq greater than 35:65 to 85:15,
(C) for each 100 parts by weight of said polyamide resin,
a compatibilizer selected from
(i) 0.1 to 5 parts by weight of a coupling agent having a molecular weight of less than 800 which contains at least two groups independently selected from ethylenically unsaturated group, epoxy, anhvririHp. .qi'flnoL carboxvL oxazoline or alkoxy

having 1 to 20 carbcn atoms, in its molecule-
(ii) 0.1 to 10 parts by weight of a functional diorganopolysiloxane having at least one group selected from epoxy, anhydride, silanol carboxyl, amine, oxazoline or alkoxy having 1 to 20 carbon atoms, in its molecule, or
(iii) from 0,1 to 10 parts by weight of a copolymer comprising a~ least one diorganopolysiloxane block and at least one block selected from polyamide, polyether, polyurethane, polyurea, polycarbonate or polyacrylate,
(D) an organohydrido silicon compound which contains an
average of a" least 2 silicon-bonded hydrogen groups
in its molecule and
(E) a hydrosilation catalyst,
components (D) and {E) being present in an amount sufficient to cure said diorganopolysiloxane (B'); and (II) dynamically curing said diorganopolysiloxane (B'). The invention further relates to a thermoplastic elastomer whtch is prepared by the above method.
Component (A) of the present invention is a thermoplastic polyamide resin. These resins are well known by the generic term "nylon" and are long chain synthetic polymers containing amide (i.e., —C(O)—NH—) linkages along the main polymer chain. For the purposes of the present invention, tne polyamide resin has a melt point (m.p.), or glass transition temperature (Tg) if the polyamide is amorphous, of room temperature (i.e., 25 °C ) to 275 °C Attempts TO prepare TPSiV elastomers from polyamides having higher melt points (e.g., nylon 4 6) resulted in poor physical properties, the ultimate elongation of such

products being less than the required 25% according to the present invention. Furthermore, for the purposes of the' present invention, the polyamide resin is preferably dried . by passing a dry, inert gas over resin pelLets or powder at elevated temperatures. The degree of drying consistent with acceptable properties and processing debends on the particular polyamide and its value is generally recommended by the manufacturer or may be determined by a few simple experiments. It is generally preferred that the polyamide resin contains no more than, about O.l weight percent of moisture. Finally, the polyamide must also be rheologically stable under the mixing conditions required to prepare the .TPSiV elastomer, as described infra. This stability is evaluated on the neat resin at the appropriate processing temperature and a change of more than 20% in melt viscosity (mixing torque.)- within the t me generally required to prepare the corresponding TPSiVs (e.g., 10 to 30 minutes in a bowl mixer) indicates that the resin is outside the- scope of the present invention Thus, for example, a dried nylon 11 sample having a m.p of 198 °C was. mixed, in a bowl mixer under a nitrogen gas purge at about 210 to 220 °C for about 15 minutes and the observed mixing torque increased by approximately 200% Such a polyamide resin is not a suitable Candidate for the instant method.
Other than the above mentioned limitations, resin (A) can be any thermoplastic crystalline or amorphous high molecular weight solid homopolymer, copolymer or terpolymer having recurring amide units within the polymer chain. In copolymer' and terpolymer systems, more than 50 mole percent of the epeat units are amide-containing units. Examples of suitable polyamides are polylactams such as nylon 6, polyenantholactam (nylon .7), polycapryllactam (nylon 3), polyluryllactam (nylon 12), and the like; homopolymers of aminoacids such as polypyrrolidinone (nylon 4) ; copolyamides of dicarboxylic acid and diamine such as nylon 6 6, polyhexamethyleneazelamide (nylon 6 9) ,

pclyhexamethylene-sebacamide (nylon 6 10 pclyhexamethyleneisophthalamide (nylon 6,1
polyhexamethylenedodecar.cic acid (nylon 6 12) and the like; aromatic and partially aromatic polyamides; copolyamides such as copolymers of caprolactam and
hexamethyleneadipanu.de nylon 6,6 6) , oh a terpolyamice (e.g., nylon 6,6 6,6);-clock copolymers such as polyether pclyamides; or mixtures "hereof. Preferred polyamide resins are nylon 6, nylon 12, nylon 6 12 and nylon 6 6.
Silicone base (B) is a uniform blend of a diorganopolysiloxane gum (B1) and a reinforcing filler (B") .
Diorganopolysiloxane (B!; is a high consistency (gum) polymer or copolymer which contains at least 2 alkenyl groups having 2 to 2 0 carbarn atoms in its molecule. The alkenyl group is specifically exemplified by vinyl, allyl, burenyl, pentenyl, hexenyl and decenyl The position of the alkenyl functionality is not critical and it may be bonded at the molecular chain terminals, in non-terminal positions on the molecular chaan or at both positions. It is preferred that the Alkenyl group is vinyl or hexenyl and that this group is present at a level of 0.001 to 3 weight percent, preferably 0.01 to 1 weight percent, in the diorganopolvsiloXne gum.
The remaining (i.e., non-alkenyl) silicon-bonded organic groups in component (B') are independently selected from hydrocarbon or halogenated hydrocarbon groups which contain no aliphatic unsaturation. These may be specifically exemplified by alkyl groups having 1 to 20 carbon atoms, such as methyl, ethyl, propyl, butyl, pentyl and hexyl; cycloakyl groups, such as cyclohexyl and cycloheptyl; aryl groups having 6 to 12 carbon atoms, such as phenyl, tolyl and ^ylyl; aralkyl groups having 7 to 20 carbon atoms, such as l6enzyl and phenethyl; and halogenated alkyl groups having 1 to 20 carbon atoms, such as 3, 3, 3-trifluoropropyi

WO 2004 055105 (j>CT EP20O3 fl 12381 )
■ , ..... . ^
and chloromethyl. It will be understood, of course, that
these groups are selected such that the
diorganopolysiloxane gum (B') has a glass temperature (or
melt point) which is below room temperature and the gum is
therefore eiastomeric. Methyl preferably makes up at lease
50, more preferably at least 90, mole percent of the non-
unsaturated silicon-bonded organic groups in component
(B').
Thus, polydiorganosiloxane (B') can be a homopolymer or a copolymer containing such organic groups. Examples include gums comprising dimethylsiloxy units and phenylmethylsiloxy units; dimethylslloxy units and diphenyisiloxy units; and dimethylslloxy units, diphenyLsiloxy units and phenylmethylsiloxy units, among others. The molecular structure is also not critical and is exemplified by straight-chain and partially branched straight-chain, linear structures being preferred.
Specific illustrations of organopolysiloxane (B1) include: trimethylsiloxy-endblocked dimethylsiloxane-methylhexenylsiloxane copolymers; dimethylhexenlylsiloxy-endblocked dimethylsiloxane-methylhexenylsiloxane copolymers; trimethylsiloxy-endblocked dimethylsiloxane-methylvinylsiloxane copolymers; trimethylsiloxy-endblocked methylphenylsiloxane-dimethylsiloxane-methylvinylsiloxane copolymers; dimethylvinylsiloxy-endblocked dimethylpolysiloxanes; dimethyl vinylsiloxy-endblocked dimethylsiloxane-methylvinylsiloxane copolymers; dimethylvinylsiloxy-endblocked methylphenylpolysiloxanes ; dimethyl vinylsiloxy-endblocked methylphenylsiloxane-dimethyleiloxane-methylvinylsiloxane copolymers; and similar copolymers wherein at least one end group is dimethilhydroxysiloxy. Preferred systems for low temperature applications include methylphenylsiloxane-dimechylsiloxane-methylvinylsiloxane copolymers and

and chloromethyl. It will be understood, of course, that these groups are selected such that the
diorganopolysiloxane gum (B') has a glass temperature (or melt point) which is below room temperature and the gum is therefore eiastomeric. Methyl preferably makes up at leasr 50, more preferably at least 90, mole percent of the non— unsaturated1silicon-bonded organic groups in component (Bf ) .
Thus, polydiorganosiloxane (B') car be a homopolymer or a copolymer containing such organic groups. Examples include gums comprising dimethylsiloxy units and phenylmethylsiloxy units; dimethylsiloxy units and diphenyisiloxy units; and dimethylsiloxy units, diphenyLsiloxy units and phenylmethylsiloxy units, among others. The molecular structure is also not critical and is exemplified by straight-chain and partially branched straight-chain, linear structures being preferred.
Specific illustration of organopolysiloxane (B') include: trimethylsiloxy-endocked dimethylsiloxane-methylhexenylsiloxane copolymers; dimethylhexenlylsiloxy-endblocked dimethylsiloxane-methylhexenylsiloxane copolymers; trimethylsiloxy-endblocked dimethylsiloxane-methylvinylsiloxane copolymers; trimethylsiloxy-endblocked methylphenylsiloxane-dimethylsiloxane-methylvinylsiloxane copolymers; dimethylvinylsiloxy-endblocked dimethylpolysiloxanes; dimethylvinylsiloxy-endblocked dimethylsiloxane-methylvinylsiloxane copolymers; dimethylvinylsiloxy-endblocked methylphenylpolysiloxanes ; dimethylvinylsiloxy-endblocked methylphenylsiloxane-dimethylsiloxane-methylvinylsiloxane copolymers; and similar copolymers wherein at least one end group is dimethylhydroxysiloxy. Preferred systems for low temperature applications include methylphenylsiloxane-dime hylsiloxane-methylvinylsiloxane copolymers and

diphenylsiloxane-dimethylsiloxar.e-methylvinylsiloxane copolymers, particularly whereir. the mriflr content of the dimethylsiloxane units is abou~ 93%.
Component (B1) may also consist of combinations of two or more organopolysilcxanes. Most preferably, component (37 ) is a polydimethylsiloxane homopolyme which is terminated with a vinyl group at each end of its molecule cr is such a homopolymer which also contains at least one vinyl group along its main chain.
For the purposes of the present invention, the molecular weight of the diorganopolysiloxane gum is sufficient to impart a Williams plasticity number of at least about 30 as determined by the American Society for Tesoing and Materials (ASTM) test method 926. The plascicity number, as used herein,- is defined a^ the thickness in millimeters. times,. 100 of a cylindrical test specimen 2 cm in. volume and approximately 10 mm in height after the specimen has been subjected to a compressive load of 4 9 Newtons for three minutes at 25 °C.
When the plasticity oi this component is less than abou~ 30, as in the case of the low viscosity fluid siioxanes employed by Arkles', cited supra, the TPSiVs prepared by dynamic vulcanization according to the instant method exhibit poor uniformity such that at high silicone contents (e.g., 50 to 70 weight percent) there are regions of essentially only silicone and those of essentially only thermoplastic resin, and the blends are weak and friable. The gums of the present invention are considerably more viscous than the silicone fluids employed in the prior art. For example, silicones contemplated by Arkles, cited supra, have an upper viscosity limit of 100,000 cS (0.1 m2 s) and, although the plasticity of fluids of such low viscosity are not readily measured by the ASTM D 926 procedure, it was determined that this corresponds zo a plasticity of

approximately 24. Although there is no absolute upper limit on the plasticity of component (B'), practical considerations of processability in conventional mixing equipment generally restrict this value, trererably, the plasticity number should be about ICO to 200, most preferably about 120 to 185.
Methods for preparing high consistency unsaturated group-containing polydiorganosiloxanes are well known and they do not require a detailed discussion in this specification. For exampler a typical method for preparing an alkenyl-functional polymer comprises the case-catalyzed equilibration of cyclic and or linear diorganopoiysiloxanes in the presence of similar alkenyl functional species.
Component The fumed form of silica is a preferred reinforcing filler based on its high surface area, which can be up to 450 m2 gram and a fumed silica having a surface area of 50 to 400 m2 g, most preferably 200 to 380 m2 g, is highly preferred. Preferably, the fumed silica filler is treated to render its surface hydrophobic, as typically practiced in the silicone rubber art. This can be accomplished by reacting the silica with a liquid organosilicon compound which contain^ silanol groups or hydroyzable precursors of silanol groups. Compounds that can be used as filler treating agents, also referred to as anti-creeping agents or plasticizers in the silicone rubber art, include such ingredients as low molecular weight liquid hydroxy- or alkoxy-terminated polydiorganosiloxanes, hexaorgapiodisiloxanes, cyclodimethylsiiazanes and hexaoroanondisilazanes. It is referred that the creatine

compound is,, an oligomeric hydroxy-terminated
diorganopolysiloxane having an average degree of
polymerization (DP) of 2 to about 100, more preferably
about 2 co about 10 and it is used at a level of about 5 to
50 parts by weight for each 100 parts by weight of the
silica filler- When component (B') is the preferred vinyl-
functional or hexenyl-functional polydimethyisiioxane, this
treating agent is preferably a hydroxy-terminated
polydimethylsiloxane.
For the purposes of the present invention, 5 to 200 parts by weight, preferably 5 to 150 and most preferably 20 to 100 parts by weight, of the reinforcing filler (B") are uniformly blended with 100 pa&ts by weight of gum (B') to prepare silicone base (B) . This blending is typically carried out at room temperature using a two-roll mill, internal mixer or other suitable device, as well known in the silicone rubber art. Alternatively, the silicone base can be formed in-situ during mixing prior to dynamic vulcanization of the gum, as further described infra. In the latter case, the temperature of mixing is kept below the softening point or melting point of the polyamide resin until the reinforcing filler is well dispersed in the diorganopolysiloxane gum.
The compatibilizer (C) may be a coupling agent, an organofunctional diorganopolysiloxane or a siloxane copolymer. For the purposes of the present invention, at least one compatibilizer is included in the preparation of the thermoplastic elastomer.
In one embodiment, the compatibilizer is (i) a coupling agent having a molecular weight of less than 800 which contains at yeast two groups in its molecule which are independently selected from ethylenically unsaturated groups {e. g. , vinyl, allyl, butenyl, pentenyl, hexenyl, acrylate and methacrylate) , epoxy, anhydride, silanol, hydroxyl, alkoxy having 1 to 2D. nreferably from 1 to 10,

more preferably from 1 to 4, carbon atoms, carboxyl or oxazoline. The latter group has the structure
wherein the carbon atoms of the. ring may contain one or more substituents selected from hydrocarbon groups having 1 to 4 carbon atoms. The coupling aqent can have an organic or
siloxane-based skeletal structure As long as it contains at least two of the above mentioned groups, these being located at.terminal positions, along the backbone or both. In the case of siloxane backbones, the above mentioned functional organic groups (i.e , r.on-silanol) are attached to silicon atoms via Si—C bonds {e.g., through a divalent hydrocarbon group such as trimethylene, tetramethylene and dimethylene) or a divalent organic group containing oxygen and or nitrogen heteroatoms such as ester, ether or amide. Although the groups may be the same, it is generally preferred that at least one of these is an ethylenically unsaturated group, preferably vinyl, while at least one other group is selected from the above mentioned epoxy, anhydride, alkoxv, silanol, hvdroxyi, carboxyl or oxazoline groups.
Examples of suit *w -w^**-^ -gents include allyl glycidyl
ether, glycidyl methicrylate, 1,2-epoxy-7-octene, 1,2-epoxy-9-decene, l,27epoxy-5-hexene, allyl succinic anhydride, vinyloxazolines, vinyloxazoline derivatives such as 2-isopropenyl-2-oxazoline, gamma-glycidoxypropylme£hyldimethoxysilane, gammaglycidoxypyltrimethoxysilane,- beta- (3, 4-epoxycyclohexyl ethyltrimethoxysilane, 1, 3-phenylene-bis (2-oxazoline), poly(propylene glycol)diglycidyl ether, diglycidyl ether of bisphenol A, tris(2,3-

epoxypropy)isocyanurate and unsaturated diamides such as CH2=CH-(qH2)8"CO-NH-(CH2)o-NK-GO-(CH2)3-CH=C^2r inter alia.
The concentration of these coupling agents can be from 0.1 to 5 parts by weight for each 100 parts by weight of the polyamide (A) , preferably, from 0.2 to 3 parts by weight.
In another embodiment, the compatibilizer is (ii) a functional diorganopolysiloxane haying a number average molecular weight of at least 800, preferably 800 to 50,000, more preferably, from 800 to 15,(100. The functional diorganopolysiloxane (ii). is polymer or copolymer in which the organic groups are independently selected from hydrocarbon or halogenated hydrocarbon groups which contain no aliphatic unsaturation, as described above for component (B1) including preferred Embodiments thereof. However, at least one functional group selected from epoxy, anhydride, silanol, alkoxy having 1 to 20, preferably from 1 to 10, more preferably' from l to 4, carbon atoms, amine, carboxyl or oxazoline, as described above, must be present in this polymer or copolvmer
Examples of suitab e component (ii) include epoxy-functional polydimethylsiloxanes, such as mono (2,3-epoxy) propyletheir-terminated polydimethylsiloxane, epoxypropoxypropyl-terminated polydimethylsiloxane, (epoxycyclohexylethyl) methyls iloxane-dimethylsiloxane copolymers, and (epoxypropoxypropyl) methyls iloxane-dimethylsiloxane copolymers; amine-functional polydimethylsiloxanes, such as aminopropyl-terminated polydimethylsiloxane, aminoethylaminopropyl-terminated polydimethylsiloxane, aminopropyl-grafted polydimethylsiloxane, aminoethylaminopropyl-grafted polydimethylsiloxane; polydimethylsiloxanes containing anhydride groups, such as succinic anhydride-terminated polydimethylsiloxane and succinic anhydride-grafted polydimethylsiloxane; silanol-terminated polydimethylsiloxanes; polydimethylsiloxanes containing

»
carboxyl groups, such as (mono)carboxydecyl-terminated
polydimethylsiloxane and carboxydecyl-terminated
polydimethylsiloxane; and polydimethylsiloxanes containing
oxazoline groups, such as vinylxoazoline grafted
polydimethylsiloxane.
The concentration of the functional diorganopolysiloxane
can be from 0.5 to 10 parts by weight for each 100 parts by
weight of the polyamide (A), preferably, from 0.5 to 5
parts by weight-
In the case of compatibilizers (i) and (ii) , it is sometimes preferred to mix the compatibilizer with the ■ polyamide resin at a temperature above the melt point of the resin prior to addition of the silicone base. While not wishing to be held to. any theory or mechanism, it is believed that this procedure results in a reaction between the functional groups of the compatibilizer and either the amide or end groups of the resin, thereby maximizing compatibilization efficiency. Alternatively, it is sometimes advantageous to add the compatibilizer to a mixture of the polyamide and the silicone base. In any event, the preferred technique can be readily determined by routine experimentation.
In yet another embodiment, the compatibilizer is (iii) a block or graft copolymer comprising at least one diorganopolysiloxane block and at least one block selected from polyamide , polyether, polyurethane, polyurea, polycarbonate or polyacrylate. For example, copolymer (iii) can have a structure such as AB, (AB)n, ABA, BAB, A-g-B and B-g-A, wherein n is an integer having a value greater than 1, A represents a diorganopolysiloxane block and B represents one of the above mentioned organic blocks. The diorganopolysiloxane block is a polymer or copolymer in which all of the organic groups are independently selected from hydrocarbon or halogenated hydrocarbon groups which contain no aliphatic unsaturation. these arouos being

previously described in connection with component (B'). Thus, for example, this component can be selected from diorganopolysiloxane-polyether block or graft copolymers, diorganopolysiloxane-polyamide block or graft copolymers, diorganopolysilox'ane-pciyurethane block or graft copolymers, diorganopolysiloxane-poiyurea bVock or grart copolymers, 'diorganopolysiroxane-polycarbonate block or graft copolymers, diorganopolysiloxane-po yacrylate block or graft copolymers or diorganopolysiloxane-polymethacrylate block or graft copolymers, wherein the diorganopolysiloxane is preferably a polydimethylsiloxane block. It is preferred that the number average molecular weight of copolymer (iii) is 1,500 Ao 50,000, more . . preferably,2,000 to 20,000.
Examples of copolymer (iii) include polyamide-
polydimethylsiloxane copolymer's, such as the siloxane-based
polyamides prepared by reacting -an SiH-functional
dimethylsiloxane and a reaction product of an olefinic acid
with a diamine (as described in U.S. Pat. No. 5,981,680 to Petroff et al.); copolymers prepared by reacting a,w-
bis (aminoalkyl)polydimethylsiloxane and hydroxy-terminated polyamide prepolymers iiaving a molecular weight of 1,500 to 3,000; copolymers prepared by reacting a,w-
bis (aminoalkyl) -functional polydimethylsiloxane and aromatic, aliphatic or cycloaliphatic diisocyanates having an average molecular weight of, e.g., 1,500 to 3,000; and copolymers of poly(alkylene oxide) and polydimethylsiloxane, such as poly (ethylene oxide)-polydimethylsiloxane-poly(ethylene oxide) block copolymers and poly(propylene oxide)-polydimethylsiloxane-poly(propylene oxide) block copolymers, as well as graft copolymer^ of such systems.
The concentration of these copolymers can be from 0.5 to 10 parts t y weight for each 100 parts by weight of polyamide (A), preferably from 0.5 to 5 parts by weight.

The organohydrido silicon compound (D) is a crosslinker (cure agent) for diorganopolysiloxane (3') of £he present composition and is an organopolysiloxane whion contains at least 2 silicon-bonded hydrogen atoms in eaon molecule, but having at least about 0.1 weight percent: hydrogen, preferably 0.2 to 2 and most: preferably o 5 to 1-7, percent hydrogen bonded to silicon. Those skillea in the art will, of course, appreciate that either component (B!) or component (D), or both, must have a functionality greater than 2 if diorganopolysiloxane (B') is to be cured (i.e., the sum of these functionalities must be greater than 4 on average). The position of the silicon-bonded hydrogen in component (D) is not critical, anal it may be bonded at the molecular chain terminals, in non-terminal positions along the molecular chain or at both positions. The silicon-bonded organic groups of component (D) are independently selected from any of the (non-alkenyl) hydrocarbon or halogenated hydrocarbon groups described above in connection with diorganopolysiloxane (B'), including preferred embodiments thereof. The molecular structure of component (D) is also not critical and is exemplified by straight-chain, partially branched straight-chain, branched, cyclic and network structures, linear polymers or copolymers being preferred, this component should be compatible with diotganopolysiloxane (B') (i.e., it is effective in curing component (B'))-
Component (D) is exemplified by the following: low molecular siloxanes, such as PhSi (OsiMe2H) 3; trimethylsiloxy-endblocked methylhydridopolysiloxanes ; trimethylsiloxy-endblocked dimethylsiloxane-methylhydriposiloxane copolymers ;
dimethylhvaridosiloxy-endblocked dimethylpolysiloxanes ; dimethylhydrogensiloxy-endblocked methylhydrogenpolysiloxanes;
dimethylhydridosiloxy-endblocked dimethylsiloxane-methmhydridosiloxane copolymers;

cyclic methylhydrcgenpoiysiloxanes;
cyclic dimethylsiloxane-methylhydridosiloxane copolymers;
tetrakis(dimethylhydrcgensiloxy)silane;
silicone resins composed of (CH3) ^HSiO, subi av (CH3)3 SiOi £,
and SiC>4 2 units; and
silicone resins composed of (CH3)2 Hsi01 :, (CH3) 3 SiOi £,
CK3Si 03 2, PhSi03 2 and SiC- 2 units,
wherein Me and Ph hereinafter denote methyl and phenyl
groups, respectively.
Particularly preferred organohydrido silicon compounds are polymers or copolymers comprising RLTSiO units ended with either R3SiOi 2 or HR2Si0i 2, wherein R is independently selected from alkyl groups having l to 20 carbon atoms, phenyl or trifluoropropyl, preferably methyl. It is also preferred that the viscosity of component (D) ,1s about 0.5 to 1,000'mPa-s at 25 °C, preferably 2 to 500 mPa-s. Further, this component preferably has 0.5 to 1.7 weight percent hydrogen bonded to silicon. It is highly preferred that component (D) is selected .from a polymer consisting essentially of methylhydrLaosiloxane units or a copolymer consisting essentially of dimethylsiloxane units and methylhydridosiloxane units, having 0.5 to 1.7 percent hydrogen bonded to silicon and having a viscosity of 2 to 500 mPa-s at 25.degree C. It is understood that such a highly preferred system will have terminal groups selected from trimethylsiloxVor dimethylhdridosiloxy groups.
Component (D) may Also be a combination of two or more of the above described systems. The organohydrido silicon compound (D) is used at a level such that the molar ratio of SiH therein to Si-alkenyl in component (B') is greater than 1 and preferably below about 50, more preferably 3 to 30, most preferably 4 to 20.
These SiH-fnnctional materials are well known in the art and many of them are commercially available.

Hydrosilation catalyst (E) is a catalyst that accelerates the cure of diorganopolysiloxane (B') in the present composition. This hydrosilation catalyst As exemplified by platinum catalysts, such as platinum black, platinum supported on silica, platinum supported on carbon, chloroplatinic acid, alcohol solutions of chloroplatinic acid, platinum olefin complexes, platanum alkenylsiloxane complexes, platinum beta-diketone complexes, platinum phosp'fiine complexes and the like; rhodium catalysts, such as rhodium chloride and rhodium chloride di (n-butyl) sulfide complex and the like; and palladium catalysts, such' as palladium on carbon, palladium chloride and the like. _ Component (E) is preferably a platinum-based catalyst such ars chloroplatinic acid; platinum dichloride; platinun tetrachloride; a platinum complex catalyst produced by reacting chloroplatinic acid and divinyltetramethyldisiloxane which is diluted with dimethylvinylsiloxy endblocked polydimethyisiloxane, prepared according to U.Sr. Pat. No. 3,419,593 to Willing; and a neutralized complex of platinous chloride and divinyltetramethyldisiloxane, prepared according to U.S. Pat. No. 5,175,325 to Brown et al. Most preferably, catalyst (E) is a neutralized complex of platinous chloride and divinyltetramethyldisiloxane.
Component (E) is added to the present composition in a catalytic quantity sufficient to promote the reaction of components (B') And (D) and thereby cure the diorganopolysiloxane to form an elastomer. The catalyst is preferably added so as to provide about 0.1 to 500 parts per million (ppm) of metal atoms based on the total weight of the thermoplastic elastomer composition, more preferably 0.25 to 100 ppm.
In preferred embodiments of the present invention, a hindered phenol
optional component is an organic compound havinq at least
one group of the structure
R
in its molecule. In the above formula R is an alkyl group having one to four carbon atoms and R' is a hydrocarbon group having four :o eight carbon atoms. For the purposes of the present invention, a group according to formula (i) can be attached to hydrogen ro form a 1,5-di-organophenol. Preferably, one to four of these groups are attached to an organic moiety of correspond valence such that the contemplated compound has a aolecular weight (Mw) of less than about 1,500, Most preferably, four such groups are present in component (F) and this compound has a molecular weight of less than 1,200 This monovalent (or polyvalent) organic moiety can contain heteroatoms such as oxygen, nitrogen, phosphorous and sulfur. The R' groups in the above formula may be illustrated by t-butyl, n-pentyl, butenyl, hexenyl, cyclopentyl, cyclohexyl and phenyl. It is preferred that both R and R' are t-butyl.
Non-limiting specific examples of component (F) include various hindered phenols marketed by Ciba Specialty Chemicals Corporation under the trade name Irganox1'*: Irganox™ 1076=octadecyl 3,5-di-tert-butyl-4-hydroxyhydrocinnamate, Irganox™ 1035=thiodiethylene bis (3, 5-di-tert-butyl-4-
hydroxyhydrocinnamate) ,
Irganox™ MDl o24=l, 2-bis (3, 5-di-tert-butyi-4-
hydroxyhydrOcinnamcyl) hydrazine,
Irganox™ 3 330=1, 3, 5-trimethyl-2, 4, 6-tris (3, 5-di-tert-
butyl-4-hydroxybenzyl) benzene,
Irganoxy 1425 WL=calcium bis(monoethyl(3,5-di-tert-butyi-

4-hydroxybenzyl)phosphonate) and
Irganox™ 3114=1,3,5-tris- (3, 5~di-tert-buty -4-
hydroxybenzyl)- 1, 3,5-triazine-2, 4, 6{1H, 3H,5R)-trione.
Preferred hindered phenols are IrganoxTm 245 {triethyleneglycol bis(3-(3'-tert-buty -4'-hydroxy-5' -methylphenyl)propionate) }, Irganox™ 10 98 {N,N'-hexamethylenebis (3,5-di-tert-butyI-l-hydroxyhydrocinnamamide) } and Irganox™ 1010 {tetrakis (methylene (3, 5-di-tert-butyl-4-hydroxy-hydrocinnamate) )methane} .'
From 0.1 to 5 parts by weight of hindered phenol (F) are
preferably employed for each 100 parts by weight of
polyamide (A), plus silicone base (B) . Preferably 0.1 to
0.75 parts by weight, more preferably 0.475 to 0.525 parts
by weight, of (F) are added for each 100 parts by weight of
(A) plus ..(B) -
In addition to the above-mentioned components, a minor amount of an optional additive (G) can be incorporated in the compositions of the present invention. Preferably, this' optional component is added at a level of 0.5 to 40 weight percent based on the total composition, more preferably 0.5 to 20 weight percent. This optional additive can be illustrated by, but not limited to, reinforcing fillers for polyamide resins, such as glass fibers and carbon fibers; extending fillers, such as quartz, barium sulfate, calcium carbonate, and diatomaceous earth; pigments, such as iron oxide and titanium oxide; electrically conducting fillers, such as carbon black and finely divided metals; heat stabilizers, such as hydrated cerric oxide; antioxidants; flame retardants, such as halogenated hydrocarbons, alumina trihydrate, maonesium hydroxide and organophosphorous compounds; and other fire retardant (FR) materials. A preferred FR additive is calcium silicate particulate, preferably a wollastonite having an average particle size

of 2 to 30 pm. Further, optional component (G) can be a
plasticizers for the silicone gum component, such as
polydimethylsiloxane oil, and or a plasticizer for the
polyamide component. Examples of the latter include
phthalate esters such as dicyclohexyl phthalate, dimethyl
phthalate, dioctyl phthalate, butyl bazzyl phthalate and
benzyl phthalate; trimellitate estersr such as C1 -C9 alkyi
trimellitate; sulfonamides such as n-cyclohexyl-p-
toiuenesulfonamide, N~ethyl-o,p-toluenesulfonamide and o-
toluenesulfonamide, and liquid oligomeric plasticizers.
Preferred plasticizers are liquids of low volatility which
minimize emissions of plasticizer at the common melt
temperatures of polyamides. . .
The above additives are typically added to the final thermoplastic composition after dynamic cure, but they may also be added at any point in the preparation provided they do not interfere with the dynamic vulcanization mechanism. Of course, the above additional ingredients are only used at levels which do not significantly detract from the desired properties of the final composition.
According to the method of the present invention, the thermoplastic elastomer is prepared by thoroughly dispersing silicone base (B) and.compatibilizer (C) in polyamide (A) and dynamically vulcanizing the diorganopolysiloxane in the base using organohydrido silicon compound (D) and catalyst (E) . For the purposes of the present invention, the weight ratio of silicone base (B) to polyamide resin (A) is greater than 35:65. It has been found that when this ratio is 35:65 or less, the resulting vulanizate generally has a modulus more resembling the polyamide resin than a thermoplastic elastomer, on the other hand, the above mentioned ratio should be no more than about 85:15 since the compositions tend to Joe weak and resemble cured silicone elastomers above this value. Notwithstanding this upper limit, the

maximum ratio of (B) to (A) for any given. combination of components is also limited by processability considerations since too high a silicone base content results in at least a partially crosslinked continuous phase which is no longer thermoplastic. For the purposes of the present invention, this practical limit is readily determined by routine experimentation and represents the highest level of component (B) which allows the TPSiV to be compression molded- It is, however, preferred that the final thermoplastic elastomer can also be readily processed in other conventional plastic operations, such as injection molding and extrusion and, in thisr case, the weight ratio of components (B) to (A) should be no more than about 75:25. Such a preferred thermoplastic elastomer which is subsequently re-processed often has a tensile strength and elongation which are within 10% of the corresponding values for the original TPSiV (i.e., the thermoplastic elastomer is little changed by re-prooessing) . Although the amount of silicone base consistent with the above mentioned requirements depends upon £he particular polyamide resin and other components selected, it is preferred that the weight ratio of components (B) to (A) is 40:60 to 75:25, more preferably 40:60 to 70:30.
Mixing is carried out in any device which is capable of uniformly dispersing the components in the polyamide resin, such as an internal mixer or a twin-screw extruder, the latter being preferred for commercial preparations. The temperature is preferably kept as low as practical consistent with good mixing so as not to degrade the resin. Depending upon the particular system, order of mixing is generally not critical and, for example, components (A) , (C) , (D) and, optionally, (F) can be added to (B) at a temperature above the softening point (i.e., melt point or glass temperature) of (A), catalyst (E) then being introduced to initiate dynamic vulcanization. However, components (B) through (F) should be well dispersed in

resin. (A) before dynamic vulcanization begins. As previously mentioned, it is also contemplated that the silicone base can be formed in-situ. For Example, the reinforcing filler may be added to a mixer already containing the polyamide resin and diorganopolysiloxane gum at a temperature below the softening point of the resin to thoroughly disperse the filler in the gum. The temperature is then raised to melt the resin, the other ingredients are added and mixing dynamic vulcanization are carried out. Optimum temperatures, mixing timed and other conditions of the mixing operation depend upon the particular resin and other components under consideration and these may be determined by routine experimentation by those skilled in the art. It is, however, preferred to carry out the mixing and dynamic vulcanization under a dry, inert atmosphere (i.e., one that does not adversely react with-the components or otherwise interfere with the hydrosilation cure), such as dry nitrogen, helium or argon.
As noted above, in order to be within the scope of the present invention, the tensile strength or elongation, or both, of the TPSiV elastomer must be at least 25% greater than that of a corresponding simple blend. A further requirement of the invention is that the TPSiV has at least 25% elongation, as determined by the test described infra. In this context, the term "simple blend" (or physical blend) denotes a Composition wherein the weight proportions of resin (A) , baase (B) and compatibilizer (C) are identical to the proportions in the TPSiV, but no cure agents are employed (i.e., either component (D) or (E) , or both, are omitted and the gum is therefore not cured) . In order to determine if a particular composition meets the above criterion, the tensile strength of the TPSiV is measured on dumbbells having a length of 25.4 mm and a width of 3.2 mm and a typical thickness of 1 to 2 mm, according to ASTM method D fl2, at an extension rate of 5-0 mm min. At least three such samples are evaluated and the results averaged

after removing obvious low readings due to sample inhomogeneity (e.g., such as voids, contamination or inclusions). These values are then compared to the corresponding average tensile and elongation values of a sample prepared 'from the simple blend composition. When at least a 25% improvement in tensile and oy elongation over the simple blend is not realized there ils no benefit derived from the dynamic vulcanization and such TPSiVs are not within the scope of the present invention.
The thermoplastic elastomer prepared by the above described method can then be processed by conventional techniques,. such as extrusion, vacuum forming, injection molding, blow molding, overmolding or compression molding. Moreover, these compositions can be re-processed (recycled) with little or no degradation of mechanical properties.
Because the volume of the silica decreases only slightly when the water and the coating agent are incorporated, it is to be assumed that the originally present association of the primary particles of the air-dispersed fumed silica is substantially retained. The charging with water and of the coating material probably leads to the start of dissolution of the silica surface, so that dissolved silica is present there. During the subsequent drying operation, that dissolved silica cementi the primary particles to their points of contact.
Thus, by charging a fumed silica in a targeted manner with water and the coating agent and subsequently drying it, there forms a substance corresponding to Kistler's aerogels which is stable to dispersion and has a high macropore volume and a very low apparent density (bulk weight).
It has further been found that the apparent structure present before the incorporation of the water and the coating agent, determined by the packing density of the fumed silica in air, which structure is expressed by its

apparent density (bulk weight), has a pronounced influence on the product obtainable by the process according to the invention: the more bulky the starting product, the more bulky the end product that is obtained.
I" has proved advantageous to use fumed silica having a
camped density of from 10 to 130 g 1, {preferably from 15 to
33 g 1, especially about 20 g 1, to, prepare the products
according to the invention.
In addition, it is found to be advantageous to choose fumed silica having a large surface area and hence small primary particles. According to an advantageous embodiment of the process according to the invention, silica having BET surface areas of from 100 to 480 m2 g, especially from 250 to 410 m2 g, is used.
Complete wetting of the primary particles can be achieved if only from 5 to 20 wt.%, especially from 7 to 15 wt.%, water and the coating agent are incorporated into the silica with uniform distribution. Because the water that has been incorporated hai to be removed again by drying, it is desirable for economic reasons to use a minimal amount of water. However, the required amount is dependent to a certain extent on the nature of the incorporation.
The building up of the texture according to the process of the invention can pa markedly promoted if compounds having a basic reaction, such as, for example, ammonia, sodium hydroxide, potassium hydroxide, water-soluble amines, water glass or the like, are added to the water and the coating agent. The amonnts added are advantageously so chosen that a pH value of from 7 to 14, preferably from 8 to 12, especially from 10 to 11, is established in the water.
The alkali used act as solubilizers for silica and bring about an increase in the macroporosity of the process products

Instead of alkaline compounds, it is also possible to add
to the water and the coating agent free silica or
hycrolytic silica and or substances that liberate alkali.
Free silica, for example silica produced by acidification
or ion exchange of silicate solutions or by hydrolytic
cleavage of organiosiliccn compounds, for example of
tetramethyl 'silicate, likewise promotes the building up of
the texture. An example of a substance that liberates
alkali and silica hydrolytically is sodium
methylsiliconate♦
Uniform distribution of the water and the coating agent in the silica can be carried out by adding them dropwise or spraying them into the silica which is in mixing movement, at temperatures of the silica of from 20 to 100°C, preferably from. 40 to 70°C, especially from 50 to 60°C. The mixing movement is advantageously effected by stirring.
A further variant of the introduction of water consists in spraying the water and the coating agent into the silica in a fluidized mass stream , for example using a down pipe.
It has also proved advantageous to carry out the charging with water at moderacely elevated temperatures. This can be effected either by preheating the water that is to be incorporated with the coating agent, or by preheating the silica, or by preheating both components. For example, the water to be incorporated with the coating agent can have a temperature of from 20 to 100°C, preferably from 50 to 100°C, especially from 90 to 100°C.
The building up of the texture can also be promoted by steaming the charged silica for a short time in a closed chamber. .The steaming leads to particularly good distribution of the water. It has proved advantageous to steam the silica charged with water, before it is dried, in a close vessel for approximately from 5 to 60 minutes, preferably from 10 to 30 minutes, especially for about

20 minutes, at temperatures up to the boiling point of the water, preferably from 50 to 80°C, especially about 60°C.
A further possible method of improving the distribution of
the 'water and of the coating agent consists in milling the silica charged with the water and the coating agent, for example in pinned disk mills or air-jea mills.
Drying is then carried out, during whion. the preformed texture is presumably fixed by way of the primary particles which have begun to dissolve at the surface or which are coated at the surface with free silica.
The nature of the drying is not critical.
It is possible to dry the resulting mixture of silica and water and coating agent, which phenomonologically always resembles a dry powder, in, for example, a rack drier, a disk drier, a Buttner drier, a flow drier or a microwave drier. However, it is also possible for the silica charged with water and coating agent to be milled and dried simultaneously in a steam ot water-jet mill, with'a separate process step thus being saved.
If separate drying of the pulverulent mixture obtained after charging with water and coating agent is carried out, it can be followed by dry milling in a pinned disk mill or an air-jet mill.
The silica according to the invention can be used as a delustering agent in lacguers, whereby it has the following advantages:
• no sedimentation, or ready re-dispersibility,
• the lustering efficiency is not impaired,
• improvement in haptics,
• possibility of more highly transparent clear lacquers,

• low moisture contents, therefore can be used in moisture-curing PU systems (polyurethane systems),
• better rheology, because less thixotropic.
The silica according to the invention can be used especially in•polyurethane lacquers .
The invention also provides a solvent-bcrne coating system
containing the texture-coated silica according to the
invention.
The invention also provides an aqueous coating system
containing the texture-coared silica according to the
invention.
The invention,relates also yco the use of the solvent-borne and of the aqueous coating system in the coating of films, plastics, wood, etc..
The invention also provides plastics bodies having a soft-
feel surface.
The soft-feel effect in particular can be improved by the
use of the texture-coated silica according to the
invention.
The subject-matter of the invention is therefore suitable for any objects touched by the bare skin, especially on the hands. These include especially portable telephones, cameras, computer casings (notebooks), bags, dashboards, seats, etc..

Examples
Preparation of the texture-coated silica acording to the
invention
A hydrophilic fumed silica (Aercsil 3C0) having the following physiccchemical properties is used:
specific surface area according
to BET [m- g]: 290.C
p'hvalue: 4.2
tamped density", .[g 1] : . 35
loss on drying [%] : 0.8
DBP number [%]: 305.0
. .C content [%] : 0
The following coating agent is used:
A white, aqueous, anionic dispersion of a silicone elastomer having epoxy functions, which contains 3.0 % ethanol, 1.0 % methanol ancy has a solids content of""50 %, a viscosity of'about 150 mPas and a density of 1. The dispersed silicone elastomer particles have an average particle size of from 3 to 4 (am and a Shore A hardness of 70. The coating agent that is used is prepared from this dispersion by additions of water and NH4OH (25 %), or water and NaOH, or water and water glass.
A ploughshare mixer is used as the mixing vessel, the coating agent is applied by spraying at room temperature by means of a binary nozzle.
There is used ass the silicone elastomer a suspension having the following physicochemical parameters:
appearance: white liquid. ■
average partricle size: 3-4 \im
viscosity: 150 mPas
solids content: 50%
type of uspension: anionic

hardness of the solid: (Shore A hardness)
Comparison example:
For comparison purposes, water (rendered alkaline) on its own is used instead of coating agent in Example 15.








In various preliminary tests it becomes clear that all products improve the? haptics, all further tests being carried out on Example 5 as a representative example.



Determination of the physicochemical parameters
BET surface area
The BET surface area is determined in accordance with
DIN 66 131 using nitrogen.
Tamped density
Determination of the tamped density following DIN ISO
787 XI
Fundamental principles cf the tamped density determination The tamped density (formerly tamped valume) is equal to the quotient of the weight and the volume of a powder after tamping in a. tamping volumeter: under„ defined-conditions. According to DIN ISO 787 XI the ramped density is given in g cm . Because of the very low tamped density of the oxides, the value herein is given in g 1. Furthermore, drying and screening and repetition of the tamping operation are not carried out.
Devices for determining the tamped. density
tamping volumeter
measuring cylinder
laboratory balance (readable to 0.01 g)
Carrying out the tamped density determination
200 ± 10 ml of oxide are introduced into the measuring
cylinder of the tamping volumeter in such a manner that no
spaces remain and the surface is horizontal.
The weight of the introduced sample is determined to an
accuracy of 0.01 g. The measuring cylinder containing the
sample is placecd into the measuring cylinder holder of the
tamping volumeter and tamped 1250 times.
The volume of the tamped oxide is read off to an accuracy
of 1 ml.

Evaluation of the tamped density determination
g initial weight x 1000
ramped density (g 1) = Y
mi read-off voLume
pp value
_;he pH value is determined in 4 % aqueous dispersion, in "he case of hydrophobic oxides in water methanol 1:1.
Reagents for determining the pH value
distilled or demineralised water, pH > 5.5
methanol, p.a.
buffer solutions pH 7.00 pH 4.66
Devices for determining the pH value
laboratory balance (readable to o 1 g)
glass beaker, 250 ml
magnetic stirrer
magnetic rod, . length 4 cm
combined pH electrode
pH meter
Dispensette, 100 ml
Procedure for determining the pH value
The determination is carried out following DIN ISO 787 IX: Calibration: Before the pH value is measured, the meter is calibrated with the buffet solutions. If several measurements are carried out in succession, it is sufficient to calibrate the meter once.
4 g of hydrophilic oxide are stirred in a 250 ml glass
beaker with 96 g (96 ml) of water with the aid of a
Dispensette and for five minutes by means of a magnetic
stirrer (speed about 1000 min-1) with the pH electrode
immersed.
4 g of hydrophobic oxide are made into a paste with 48 g (61 ml) of methanol in a 250 ml glass beaker, and the suspension is diluted with 48 g (48 ml) of water and

stirred for five minutes by means of a magnetic stirrer (speed about 1000 min-1) with the pH electrode immersed. After the stirrer has been switched off, the pH value is read off after the mixture has been allowed to stand for one minute. The result is read off to one decimal place.
Loss on drying
In contrast to the weighed portion of 10 g mentioned in DIN ISO 787 II, a weighed portion of i g is used for determining the.loss on drying,
The cover is fitted before cooling is carried out. A second drying operation is not carried out.
About 1 g of the sample is weighed, to an accuracy of 0.1 mg, avoiding the formation of dustf into a weighing pan which has a ground-glass cover and has been dried at 105°C, and is dried for two hours at 105°C in a drying cabinet. After cooling with the cover in place in a desiccator over blue gel, the samole isr re-weighed.
g loss in weight
% loss on drying at 105°C = *x 100
' g initial weight
The result is read off to one decimal place.
Ignition loss
Devices for determining the ignition loss
porcelain crucible with crucible lid
muffle furnace
analytical balance (readable to 0.1 mg)
desiccator
Carrying out the determination of the ignition loss Debartina from DIN 55 9-21, 0.3 to 1 g of the material,

which has not been pre-dried, is weighed to an accuracy of
0.1 mg, into a porcelain crucible, having a crucible lid,
which has previously been ignited, and is ignited for
2 hours at 1000°C in a muffle furnace,
The formation of dust is carefully to be avoided. It has
proved advantageous for the weighed Samples to be placed
into the muffle furnace while it is still cold.
More pronounced air turbulence in the porcelain crucibles
is avoided by slow heating of the furnace.
After 1000°C has been reached, the sample is ignited
further for 2 hours. The crucible is then covered with a
crucible lid and the ignition loss of the crucible is
determined in a desiccator ovsrr blue gel.
Evaluation of the icnition loss determination
Because the ignition loss, is based on the sample dried for
2 hours at 105°C, the calculation formula is as follows:
l00 - LD
m0 x - mi
100
% ignition loss =hx 100
100 - LD
rao x
100
m0 = initial weight g)
LD = loss on drying (%)
mi = weight of the ignited sample (g)
The result is read off to one decimal place.
DBF number
Devices for determining the DBP number . .
top-pan balance
poly-beaker (250 ml)
Brabender plastograph with metering unit

Reagent
Dibutyl phthalate (commercial grade}
Implementation
1. Checking of the switch-off point
-Switch on the plastcgraph without the metering pump. -Open the flap covering the operating element (beneath
the display)
between the switch-off value "1000" and the alarm "AI
H.A.",'after 5 seconds the display returns to normal
mode.
2. Calibration
-Switch on the plastcgraph without the metering pump. -Switch on the kneader (press both Start buttons
simultaneously-With the "Cal" button depressed press the "Funk"
button once, the display alternates between the
current zero point ana "Lo S.C.". -Press the "Cal" button again, after four seconds
(calibration) the device displays the current overall
range "10000" and "Fu S.C". -Press the "Cal" button again, after four seconds
(calibration) the device shows the friction-corrected
zero point "tare" -Press the "Cal" Button again and wait 5 seconds. -Carry out the steps "Switch-off point" and
"Calibration operation" once daily as required before
the measurements!
3. Measurement
-12.5 g sample are weighed into a poly-beaker and placed into the kneading -chamber. If instructed, a different initial weight may also be used (e.g. 8 or 2-0 g) . The DB? metering unit is switched on. As soon

as the, filling procedure (display F) is complete, the
plastograph is ready for operation. - The measurement begins by simultaneous pressing of the
Start buttons. -The metering unit meters in 4 ml of DBP min until the
switch-off point that has been set (1000) is reached. -The device switches off automatically. -The DBP consumption can now be read off on the display
of the metering device.
Calculation
Dosimat display x 1.047 x 100 DBP (%) =
initial weight (g)
Always give the result together with the initial weight.




















Documents:

1263-chenp-2005 abstract duplicate.pdf

1263-chenp-2005 claims duplicate.pdf

1263-chenp-2005 description (complete) duplicate.pdf

1263-chenp-2005-abstract.pdf

1263-chenp-2005-claims.pdf

1263-chenp-2005-correspondnece-others.pdf

1263-chenp-2005-correspondnece-po.pdf

1263-chenp-2005-description(complete).pdf

1263-chenp-2005-form 1.pdf

1263-chenp-2005-form 26.pdf

1263-chenp-2005-form 3.pdf

1263-chenp-2005-form 5.pdf

1263-chenp-2005-other-documents.pdf

1263-chenp-2005-pct.pdf


Patent Number 222308
Indian Patent Application Number 1263/CHENP/2005
PG Journal Number 47/2008
Publication Date 21-Nov-2008
Grant Date 05-Aug-2008
Date of Filing 15-Jun-2005
Name of Patentee DEGUSSA AG
Applicant Address Bennigsenplatz 1, 40474 Düsseldorf,
Inventors:
# Inventor's Name Inventor's Address
1 SPITZNAGEL, Kurt August-Bebel-Strasse 1, 63457 Hanau,
2 MEYER, Jurgen Grossostheimer Strasse 51, 63811 Stockstadt,
3 CHRISTIAN, Hans-Dieter Am Hörsteiner Weg 16a, 63755 Alzenau,
PCT International Classification Number C08K 9/02
PCT International Application Number PCT/EP2003/012381
PCT International Filing date 2003-11-06
PCT Conventions:
# PCT Application Number Date of Convention Priority Country
1 60/433,957 2002-12-18 U.S.A.