A process for (i) producing a silylated product, comprising reacting a mixture comprising (a) an unsaturated compound containing at least one unsaturated functional group, (b) a silyl hydride containing at least one silylhydride functional group, and (c) a catalyst, optionally in the presence of a solvent, to produce a dehydrogenative silylated product, a hydrosilylated product, or a combination of a dehydrogenative silylated product and a hydrosilylated product, or (ii) producing a crosslinked material, comprising reacting a mixture comprising (a) a silyl-hydride containing polymer, (b) a vinyl-substituted siloxane, a vinyl substituted polysiloxane, an unsaturated polyolefin, or combinations thereof and (c) a catalyst, optionally in the presence of a solvent, in order to produce the crosslinked material, wherein the catalyst is a complex of the Formula; Formula, or a combination of two or more thereof: wherein each occurrence of R 1, R 2, R 3, R 4, and R 5 is independently chosen from hydrogen, a C1-C18 alkyl, or an aryl, where R 1 -R 5, other than hydrogen, may optionally contain at least one heteroatom; each occurrence of R 6 and R 7 is independently chosen from a C1-C18 alkyl, or an aryl, where R 6 and R 7 may optionally contain at least one heteroatom; optionally any two neighboring groups of R 1, R 2, R 3, R 4, R 5, R 6, and R 7 taken together may form a ring being a saturated or unsaturated cyclic structure, optionally containing one or more heteroatoms; and R 8 and R 9 is each independently, chosen from an alkyl or aryl group optionally containing at least one heteroatom, or R 8 and R 9 are connected so as to form a dicarboxylate chelating group; and the carboxylate is derived from straight-chain, branched or cyclic aliphatic carboxylic acid, dicarboxylic acid, or aromatic carboxylic acid, and which optionally contains one or more heteroatoms chosen from O, N, S, P, Si, F, Cl, Br, I, or a combination of two or more thereof; wherein the mixture is free of a separate reducing agent and a promoter. (i) producing a silylated product, comprising reacting a mixture comprising (a) an unsaturated compound containing at least one unsaturated functional group, (b) a silyl hydride containing at least one silylhydride functional group, and (c) a catalyst, optionally in the presence of a solvent, to produce a dehydrogenative silylated product, a hydrosilylated product, or a combination of a dehydrogenative silylated product and a hydrosilylated product, or (ii) producing a crosslinked material, comprising reacting a mixture comprising (a) a silyl-hydride containing polymer, (b) a vinyl-substituted siloxane, a vinyl substituted polysiloxane, an unsaturated polyolefin, or combinations thereof and (c) a catalyst, optionally in the presence of a solvent, in order to produce the crosslinked material, wherein each occurrence of R 1, R 2, R 3, R 4, and R 5 is independently chosen from hydrogen, a C1-C18 alkyl, or an aryl, where R 1 -R 5, other than hydrogen, may optionally contain at least one heteroatom; each occurrence of R 6 and R 7 is independently chosen from a C1-C18 alkyl, or an aryl, where R 6 and R 7 may optionally contain at least one heteroatom; optionally any two neighboring groups of R 1, R 2, R 3, R 4, R 5, R 6, and R 7 taken together may form a ring being a saturated or unsaturated cyclic structure, optionally containing one or more heteroatoms; and R 8 and R 9 is each independently, chosen from an alkyl or aryl group optionally containing at least one heteroatom, or R 8 and R 9 are connected so as to form a dicarboxylate chelating group; and the carboxylate is derived from straight-chain, branched or cyclic aliphatic carboxylic acid, dicarboxylic acid, or aromatic carboxylic acid, and which optionally contains one or more heteroatoms chosen from O, N, S, P, Si, F, Cl, Br, I, or a combination of two or more thereof; wherein the mixture is free of a separate reducing agent and a promoter.