Journal
ACS CATALYSIS
Volume 9, Issue 3, Pages 2324-2333Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.8b04327
Keywords
CO2 reduction; electrocatalyst; oxalate; metal oxide; chromium; gallium; aqueous
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Funding
- National Science Foundation [CHE-1800400]
- National Science Foundation Graduate Research Fellowship Program [DGE-1148900]
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Electrochemical transformation of CO2 into commodity chemicals such as oxalate is a strategy for profitably remediating high atmospheric CO2 levels. Electrocatalysts for oxalate generation, however, have required prohibitively large applied potentials, forcing the use of nonaqueous electrolytes. Here, a thin film comprised of alloyed Cr and Ga oxides on glassy carbon is shown to electrocatalytically generate oxalate from aqueous CO2 with high Faradaic efficiencies at 690 mV overpotential. Oxalate is produced at a surface anion site via a CO-dependent pathway; the process is highly sensitive to the hydrogen-bonding environment and avoids the commonly invoked CO2 center dot- intermediate. Ultimately, this catalytic system accomplishes efficient CO2 to oxalate conversion in protic electrolyte.
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