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J Am Chem Soc. 2017 Nov 8;139(44):15848-15857. doi: 10.1021/jacs.7b08607. Epub 2017 Oct 25.

Electrochemical CO2 Reduction over Compressively Strained CuAg Surface Alloys with Enhanced Multi-Carbon Oxygenate Selectivity.

Author information

1
Joint Center for Artificial Photosynthesis, Lawrence Berkeley National Laboratory , Berkeley, California 94720, United States.
2
Department of Chemical and Biomolecular Engineering, University of California , Berkeley, California 94720, United States.
3
SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory , Menlo Park, California 94025, United States.
4
Department of Chemical Engineering, Stanford University , Stanford, California 94305, United States.

Abstract

The electrochemical reduction of carbon dioxide using renewably generated electricity offers a potential means for producing fuels and chemicals in a sustainable manner. To date, copper has been found to be the most effective catalyst for electrochemically reducing carbon dioxide to products such as methane, ethene, and ethanol. Unfortunately, the current efficiency of the process is limited by competition with the relatively facile hydrogen evolution reaction. Since multi-carbon products are more valuable precursors to chemicals and fuels than methane, there is considerable interest in modifying copper to enhance the multi-carbon product selectivity. Here, we report our investigations of electrochemical carbon dioxide reduction over CuAg bimetallic electrodes and surface alloys, which we find to be more selective for the formation of multi-carbon products than pure copper. This selectivity enhancement is a result of the selective suppression of hydrogen evolution, which occurs due to compressive strain induced by the formation of a CuAg surface alloy. Furthermore, we report that these bimetallic electrocatalysts exhibit an unusually high selectivity for the formation of multi-carbon carbonyl-containing products, which we hypothesize to be the consequence of a reduced coverage of adsorbed hydrogen and the reduced oxophilicity of the compressively strained copper. Thus, we show that promoting copper surface with small amounts of Ag is a promising means for improving the multi-carbon oxygenated product selectivity of copper during electrochemical CO2 reduction.

PMID:
28988474
DOI:
10.1021/jacs.7b08607
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