Journal
ACS CATALYSIS
Volume 12, Issue 9, Pages 5275-5283Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.2c00646
Keywords
CO2 reduction; CO reduction; asymmetric C-C coupling; electrocatalysis; Cu-Pd bimetallic alloy catalysts
Categories
Funding
- National Science Foundation [CBET-1803482, CBET-1930013]
- U.S. Department of Energy's Office of Energy Efficiency and Renewable Energy (EERE) under the Bioenergy Engineering for Product Synthesis (BEEPS) program of the Bioenergy Technologies Office (BETO) [DE-EE0008501]
- Extreme Science and Engineering Discovery Environment (XSEDE) through NSF [DMR-140068]
- U.S. Department of Energy Office of Science User Facility, at Brookhaven National Laboratory [DE-SC0012704]
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This study reports the selective reduction of CO to acetate using Cu-Pd bimetallic electrocatalysts and explores the underlying mechanism. The results demonstrate that the bimetallic catalyst exhibits high activity and selectivity for the conversion of CO to acetate.
Electroreduction of carbon monoxide (CO) possesses great potential for achieving the renewable synthesis of hydrocarbon chemicals from CO2. We report here selective reduction of CO to acetate using Cu-Pd bimetallic electrocatalysts. High activity and selectivity are demonstrated for CO-to-acetate conversion with >200 mA/cm(2) in geometric current density and >65% in Faradaic efficiency (FE). An asymmetrical C-C coupling mechanism is proposed to explain the composition-dependent catalytic performance and high selectivity toward acetate. This mechanism is supported by the computationally predicted shift of the *CO adsorption from the top-site configuration on Cu (or Cu-rich) surfaces to the bridge sites of Cu-Pd bimetallic surfaces, which is also associated with the reduction of the CO hydrogenation barrier. Further kinetic analysis of the reaction order with respect to CO and Tafel slope supports a reaction pathway with *CO-*CHO recombination following a CO hydrogenation step, which could account for the electroreduction of CO to acetate on the Cu-Pd bimetallic catalysts. Our work highlights how heteroatomic alloy surfaces can be tailored to enable distinct reaction pathways and achieve advanced catalytic performance beyond monometallic catalysts.
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