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CO2 Hydrogenation to Formate and Formic Acid by Bimetallic Palladium-Copper Hydride Clusters
Gaoxiang Liu1, Patricia Poths2, Xinxing Zhang3
1Department of Chemistry, Johns Hopkins University, 3400 N. Charles Street, Baltimore, Maryland 21218, United States.
Abstract:
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. This study represents the first example of CO2 hydrogenation by bimetallic hydride clusters.
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