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Angew Chem Int Ed Engl. 2019 Mar 18. doi: 10.1002/anie.201900781. [Epub ahead of print]

Enhancing Activity and Reducing Cost for Electrochemical Reduction of CO2 by Supporting Palladium on Metal Carbides.

Author information

1
Collaborative Innovation Center of Chemical Science and Engineering, School of Chemical Engineering and Technology, Tianjin University, Tianjin, 300072, P. R. China.
2
Department of Chemical Engineering, Columbia University, 500 W. 120th St., New York, NY, 10027, USA.
3
Chemistry Department, Brookhaven National Laboratory, Upton, NY, 11973, USA.

Abstract

Electrochemical CO2 reduction reaction (CO2 RR) with renewable electricity is a potentially sustainable method to reduce CO2 emissions. Palladium supported on cost-effective transition-metal carbides (TMCs) are studied to reduce the Pd usage and tune the activity and selectivity of the CO2 RR to produce synthesis gas, using a combined approach of studying thin films and practical powder catalysts, in situ characterization, and density functional theory (DFT) calculations. Notably, Pd/TaC exhibits higher CO2 RR activity, stability and CO Faradaic efficiency than those of commercial Pd/C while significantly reducing the Pd loading. In situ measurements confirm the transformation of Pd into hydride (PdH) under the CO2 RR environment. DFT calculations reveal that the TMC substrates modify the binding energies of key intermediates on supported PdH. This work suggests the prospect of using TMCs as low-cost and stable substrates to support and modify Pd for enhanced CO2 RR activity.

KEYWORDS:

CO2 electroreduction; carbides; computational chemistry; in situ X-ray spectroscopy; palladium hydride

PMID:
30884064
DOI:
10.1002/anie.201900781

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