Insight into catalytic reduction of CO₂ to methane with silanes using Brookhart's cationic Ir(iii) pincer complex.

ABSTRACT: Using density functional theory computations, we investigated in detail the underlying reaction mechanism and crucial intermediates present during the reduction of carbon dioxide to methane with silanes, catalyzed by the cationic Ir-pincer complex ((POCOP)Ir(H)(acetone)⁺, POCOP = 2,6-bis(dibutylphosphinito)phenyl). Our study postulates a plausible catalytic cycle, which involves four stages, by sequentially transferring silane hydrogen to the CO₂ molecule to give silylformate, bis(silyl)acetal, methoxysilane and the final product, methane. The first stage of reducing carbon dioxide to silylformate is the rate-determining step in the overall conversion, which occurs via the direct dissociation of the silane Si-H bond to the C[double bond, length as m-dash]O bond

SUBMITTER: Fang S 

PROVIDER: S-EPMC9078678 | biostudies-literature | 2018 Feb

REPOSITORIES: biostudies-literature