CO2 Hydrogenation to Formate and Formic Acid by Bimetallic Palladium–Copper Hydride Clusters

Liu, Gaoxiang; Poths, Patricia; Zhang, Xinxing; Zhu, Zhaoguo; Marshall, Mary; Blankenhorn, Moritz; Alexandrova, Anastassia N.; Bowen, Kit H.

doi:10.1021/jacs.0c01855

CO₂ Hydrogenation to Formate and Formic Acid by Bimetallic Palladium–Copper Hydride Clusters

Journal Article · Mon Apr 06 00:00:00 EDT 2020 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.0c01855· OSTI ID:1765339

^[1]; Poths, Patricia ^[2]; ^[3]; Zhu, Zhaoguo ^[4]; Marshall, Mary ^[4]; Blankenhorn, Moritz ^[4]; ^[2]; ^[4]

Johns Hopkins Univ., Baltimore, MD (United States); UCLA
Univ. of California, Los Angeles, CA (United States)
Nankai Univ., Tianjin (China)
Johns Hopkins Univ., Baltimore, MD (United States)

Mass spectrometric analysis of the anionic products of interaction between bimetallic palladium-copper tetrahydride anions, PdCuH₄^–, and carbon dioxide, CO₂, in a reaction cell shows an efficient generation of the PdCuCO₂H₄^– intermediate and formate/formic acid complexes. Multiple structures of PdCuH₄^– and PdCuCO₂H₄^– are identified by a synergy between anion photoelectron spectroscopy and quantum chemical calculations. The higher energy PdCuH₄^– isomer is shown to drive the catalytic hydrogenation of CO₂, emphasizing the importance of accounting for higher energy isomers for cluster catalytic activity. In conclusion, this study represents the first example of CO₂ hydrogenation by bimetallic hydride clusters.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of California, Los Angeles, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: SC0019152

OSTI ID:: 1765339

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 17 Vol. 142; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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