Highly selective electrocatalytic CO 2 reduction to ethanol by metallic clusters dynamically formed from atomically dispersed copper

Xu, Haiping; Rebollar, Dominic; He, Haiying; Chong, Lina; Liu, Yuzi; Liu, Cong; Sun, Cheng-Jun; Li, Tao; Muntean, John V.; Winans, Randall E.; Liu, Di-Jia; Xu, Tao

doi:10.1038/s41560-020-0666-x

DOE OSTI · 1671779

Highly selective electrocatalytic CO 2 reduction to ethanol by metallic clusters dynamically formed from atomically dispersed copper

Xu, Haiping·Rebollar, Dominic·He, Haiying·Chong, Lina·Liu, Yuzi·Liu, Cong·Sun, Cheng-Jun·Li, Tao·Muntean, John V.·Winans, Randall E.·Liu, Di-Jia·Xu, Tao

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Abstract

Direct electrochemical conversion of CO 2 to ethanol offers a promising strategy of lowering CO 2 emission while storing energy from renewable electricity. However, current electrocatalysts offer only limited selectivity toward ethanol. Here we report a copper catalyst synthesized by a unique Cu-Li amalgm method over a commercial carbon support that achieved Faradaic efficiency (FE) higher than 91% at -0.7 V (RHE) and the active potential as low as -0.4 V (RHE) during direct electrocatalytic CO 2 -to-ethanol conversion. The catalyst also demonstrated stability over an extended period of operation. A strong correlation between the catalytic selectivity and the initial Cu atoms dispersion was found and Operando X-ray absorption spectroscopy identified a dynamic and reversible transformation from atomically dispersed copper atoms to Cu n (n = 3 and 4) under the electrochemical reaction. Frist-principles calculations further elucidate the possible catalytic mechanism of CO 2 reduction over Cu n .

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY CO2 catalysis conversion electrochemical ethanol

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Xu, Haiping, Rebollar, Dominic, He, Haiying, Chong, Lina, Liu, Yuzi, Liu, Cong, Sun, Cheng-Jun, Li, Tao, Muntean, John V., Winans, Randall E., Liu, Di-Jia, Xu, Tao. 2020-07-27. Highly selective electrocatalytic CO 2 reduction to ethanol by metallic clusters dynamically formed from atomically dispersed copper. https://doi.org/10.1038/s41560-020-0666-x

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