α‐Diimine nickel complexes immobilized into fluorotetrasilicic mica interlayers are prepared by the reaction of an α‐diimine ligand and nickel‐ion‐exchanged fluorotetrasilicic mica, and these are used for the copolymerization of ethylene with linear α‐olefins (1‐hexene, 1‐octene, and 1‐decene), cyclic olefins (norbornene and cyclopentene), or polar vinyl monomers (methyl acrylate and 5‐hexenenitrile). The copolymerization of ethylene with α‐olefins affords linear low‐density polyethylene including methyl and alkyl branches. The incorporation of cyclopentene into the main chain is proved by the 13C NMR spectrum of the ethylene/cyclopentene copolymer. No significant activity is observed during the copolymerization of ethylene with norbornene, methyl acrylate, or 5‐hexenenitrile.

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