Tuning the activity and selectivity of electroreduction of CO2 to synthesis gas using bimetallic catalysts

Ji Hoon Lee, Shyam Kattel, Zhao Jiang, Zhenhua Xie, Siyu Yao, Brian M. Tackett, Wenqian Xu, Nebojsa S. Marinkovic and Jingguang G. Chen ()
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Ji Hoon Lee: Columbia University
Shyam Kattel: Florida A&M University
Zhao Jiang: Xi’an Jiaotong University
Zhenhua Xie: Columbia University
Siyu Yao: Brookhaven National Laboratory
Brian M. Tackett: Columbia University
Wenqian Xu: Advanced Photon Source, Argonne National Laboratory
Nebojsa S. Marinkovic: Columbia University
Jingguang G. Chen: Columbia University

Nature Communications, 2019, vol. 10, issue 1, 1-8

Abstract: Abstract The electrochemical carbon dioxide reduction reaction to syngas with controlled CO/H2 ratios has been studied on Pd-based bimetallic hydrides using a combination of in situ characterization and density functional theory calculations. When compared with pure Pd hydride, the bimetallic Pd hydride formation occurs at more negative potentials for Pd-Ag, Pd-Cu, and Pd-Ni. Theoretical calculations show that the choice of the second metal has a more significant effect on the adsorption strength of *H than *HOCO, with the free energies between these two key intermediates (i.e., ΔG(*H)–ΔG(*HOCO)) correlating well with the carbon dioxide reduction reaction activity and selectivity observed in the experiments, and thus can be used as a descriptor to search for other bimetallic catalysts. The results also demonstrate the possibility of alloying Pd with non-precious transition metals to promote the electrochemical conversion of CO2 to syngas.

Date: 2019
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DOI: 10.1038/s41467-019-11352-0

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