Molecular Iridium Complexes in Metal-Organic Frameworks Catalyze CO Hydrogenation via Concerted Proton and Hydride Transfer.

Molecular iridium catalysts immobilized in metal-organic frameworks (MOFs) were positioned in the condensing chamber of a Soxhlet extractor for efficient CO hydrogenation. Droplets of hot water seeped through the MOF catalyst to create dynamic gas/liquid interfaces which maximize the contact of CO,...

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Detalles Bibliográficos
Publicado en:	Journal of the American Chemical Society Vol. 139; no. 49; pp. 17747 - 17751
Autores principales:	Bing An, Lingzhen Zeng, Mei Jia, Zhe Li, Zekai Lin, Yang Song, Yang Zhou, Jun Cheng, Cheng Wang, Wenbin Lin
Formato:	Artículo
Publicado:	American Chemical Society 12/13/2017
Materias:	Iridium compounds Metal-organic frameworks Catalytic hydrogenation Carbon dioxide Hydride transfer reactions Proton transfer reactions Density functional theory
Acceso en línea:	Ver este registro en EBSCOhost

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