Remotely Bonded Bridging Dioxygen Ligands Enhance Hydrogen Transfer in a Silica-Supported Tetrairidium Cluster Catalyst

Palermo, Andrew P.; Zhang, Shengjie; Okrut, Alexander; Schöttle, Christian; Grosso-Giordano, Nicolás A.; Runnebaum, Ron C.; Edwards, Kyle C.; Guan, Erjia; Ertler, Daniel; Solovyov, Andrew; Kistler, Joseph D.; Aydin, Ceren; Lu, Jing; Busygin, Igor; Dixon, David. A.; Gates, Bruce C.; Katz, Alexander

doi:10.1021/jacs.3c10660

Remotely Bonded Bridging Dioxygen Ligands Enhance Hydrogen Transfer in a Silica-Supported Tetrairidium Cluster Catalyst

Journal Article · Thu Feb 01 00:00:00 EST 2024 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.3c10660· OSTI ID:2305447

^[1]; Zhang, Shengjie ^[2]; Okrut, Alexander ^[3]; ^[3]; Grosso-Giordano, Nicolás A. ^[3]; ^[3]; Edwards, Kyle C. ^[2]; ^[4]; Ertler, Daniel ^[3]; Solovyov, Andrew ^[3]; Kistler, Joseph D. ^[4]; Aydin, Ceren ^[4]; Lu, Jing ^[4]; Busygin, Igor ^[3]; ^[2]; ^[4]; ^[3]

University of California, Berkeley, CA (United States); University of California, Davis, CA (United States); University of California, Davis
University of Alabama, Tuscaloosa, AL (United States)
University of California, Berkeley, CA (United States)
University of California, Davis, CA (United States)

A longstanding challenge in catalysis by noble metals has been to understand the origin of enhancements of rates of hydrogen transfer that result from bonding of oxygen near metal sites. We investigated structurally well-defined catalysts consisting of supported tetrairidium carbonyl clusters with single-atom (apical iridium) catalytic sites for ethylene hydrogenation. Reaction of the clusters with ethylene and H₂ followed by O₂ led to the onset of catalytic activity as a terminal CO ligand at each apical Ir atom was removed and bridging dioxygen ligands replaced CO ligands at neighboring (basal-plane) sites. The presence of the dioxygen ligands caused a 6-fold increase in the catalytic reaction rate, which is explained by the electron-withdrawing capability induced by the bridging dioxygen ligands, consistent with the inference that reductive elimination is rate determining. Electronic structure calculations demonstrate an additional role of the dioxygen ligands, changing the mechanism of hydrogen transfer from that involving equatorial hydride ligands to that involving bridging hydride ligands. This mechanism is made evident by an inverse kinetic isotope effect observed in ethylene hydrogenation reactions with H₂ and, alternatively, with D₂ on the cluster incorporating the dioxygen ligands, and is a consequence of quasi-equilibrated hydrogen transfer in this catalyst. The same mechanism accounts for rate enhancements induced by the bridging dioxygen ligands for the catalytic reaction of H₂ with D₂ to give HD. Here, we posit that the mechanism involving bridging hydride ligands facilitated by oxygen ligands remote from the catalytic site may have some generality in catalysis by oxide-supported noble metals.

View Accepted Manuscript (DOE)

Research Organization:: University of California, Davis, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231; FG02-04ER15513

OSTI ID:: 2305447

Alternate ID(s):: OSTI ID: 3013712

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 6 Vol. 146; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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