[JACS] 我室程俊教授、汪骋教授、林文斌客座教授发表论文:Molecular Iridium Complexes in Metal-Organic Frameworks Catalyze CO2 Hydrogenation via Concerted Proton and Hydride Transfer

2017年11月29日

我室程俊教授、汪骋教授、林文斌客座教授在 JACS 上发表论文:Molecular Iridium Complexes in Metal-Organic Frameworks Catalyze CO2 Hydrogenation via Concerted Proton and Hydride Transfer

文章链接:http://pubs.acs.org/doi/10.1021/jacs.7b10922

摘要:

Molecular iridium catalysts immobilized in metal-organic frame-works (MOFs) were positioned in the condensing chamber of a Soxhlet extractor for efficient CO2 hydrogenation. Droplets of hot water seeped through the MOF catalyst to create dynamic gas/liquid interfaces which maximize the contact of CO2, H2, H2O, and the catalyst to achieve a high turnover frequency of 410 h-1 under atmospheric pressure and at 85 oC. H/D kinetic isotope effect measurements and density functional theory calculations revealed concerted proton-hydride transfer in the rate-determining step of CO2 hydrogenation, which was difficult to unravel in homogeneou reactions due to base-catalyzed H/D exchange.

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