Patent GB-728227-A (GB)
Title: Improvements in or relating to surface-coated silicon-containing particulate material and rubbery composition and method of making same
IPC: C08K3/34
Filed: 1952-05-22
Abstract: An elastomeric composition comprises a rubbery conjugated diene polymer and, as a reinforcing filler, finely-divided solid silicon monoxide or polymeric silicon oxyimide coated with an organopolysiloxane (see Group III), e.g. in amount of 100 parts by weight of the rubber to 30-80 parts of the filler.  Other fillers, accelerators, vulcanizing agents and anti-oxidants may be added.  In example 6, a composition consisting of butadiene-styrene copolymer, propenylpolysiloxane-coated silicon monoxide, zinc oxide, palm oil, stearic acid and tetramethyl thiuram disulphide, was vulcanised by heating at 285 DEG  F. Synthetic rubbers specified are the polymers of butadiene-1 : 3, 2 : 3 - dimethylbutadiene - 1 : 3, 1 : 4 - dimethylbutadiene-1 : 3 or copolymers thereof with one another or with acrylonitrile, styrene, methyl acrylate, ethyl acrylate, ethyl methacrylate or isobutylene, and polymers of chloroprene. Polysiloxanes that may be used are derived by hydrolysis of silanes, a long list of which is given, the preferred ones containing radicals having olefinic unsaturation, e.g. vinyl-chloro-, -dichloro- and -trichloro-, vinyl-bromo-, -dibromo- and -tribromo-, divinyl-chloro- and dichloro-, propenyl-chloro-, -dichloro-, -trichloro-and -tribromo-, 3-butenyl-chloro- and -trichloro-, 2-butenyldichloro-, di-3-butenyldichloro-, 4 - pentenyltrichloro-, 2 - pentenyltrichloro-, 1 - butenyltribromo-, 3 - pentenyltribromo-, D 2 - tetrahydrobenzyl - trichloro - and -tribromo- and D 3 - tetrahydrobenzyl - trichloro-and -tribromo-silanes.  U.S.A. Specifications 2,386,259, 2,390,378 and 2,398,672 are referred to in this connection.ALSO:A reinforcing filler for elastomeric compositions (see Groups IV (a) and V) consists of silicon monoxide or polymeric silicon oxyimide, desirably having an average particle size of 5 to 200 millimicrons, coated with an organopolysiloxane. The siloxane may be applied by spraying or by introducing a vapour or mist of the siloxane into an air dispersion of the particulate siliceous material, with subsequent drying.  The weight of the siloxane coating is desirably 0.3 to 20 per cent. of the uncoated material. In example (1) silicon monoxide is coated by forming the siloxane in situ by reacting propenyl trichlorosilane vapour with water vapour or mist in the presence of silicon monoxide particles. The siliceous material may be coated with any polysiloxane, but those containing hydrocarbon radicals having olefinic unsaturation are preferred.  In making polymeric silicon oxyimide, as described in U.S.A. Specification 2,666,754, silicon monoxide, formed as a gaseous combustion product by heating pure silica sand and powdered carbonaceous fuel, is discharged into a reaction chamber containing ammonia gas (preferably in stoichiometric excess) and little or no oxygen.  Rapid reaction between the gases results in formation of the polyoxyimide.ALSO:An elastomeric composition comprises a natural rubber, e.g caoutchouc, and as a reinforcing filler finely divided solid silicon monoxide or polymeric silicon oxyimide coated with an organo-polysiloxane (see Group III), e.g. in amount of 100 parts by weight of the rubber to 30-80 parts of the coated siliceous material. Other fillers, accelerators, vulcanizing agents and antioxidants may also be added.  In examples, compositions consisting of natural rubber, zinc oxide, pine tar, stearic acid, 2-mercapto benzothiazole, phenyl betanaphthylamine, sulphur, didodecylamine and (1, 2) propenylpolysiloxane-coated silicon monoxide, (3) diphenylpolysiloxane-coated silicon monoxide, (4) ethylpolysiloxane-coated silicon monoxide, and (5) propenylpolysiloxane-coated polymeric silicon oxyimide, are vulcanized by heating at 285 DEG  F.