Electrocatalytic CO2 reduction into value-added multicarbon products offers a means to close the anthropogenic carbon cycle using renewable electricity. However, the unsatisfactory catalytic selectivity for multicarbon products severely hinders the practical application of this technology. In this paper, we report a cascade AgCu single-atom and nanoparticle electrocatalyst, in which Ag nanoparticles produce CO and AgCu single-atom alloys promote C-C coupling kinetics. As a result, a Faradaic efficiency (FE) of 94 ± 4% toward multicarbon products is achieved with the as-prepared AgCu single-atom and nanoparticle catalyst under ~720 mA cm-2 working current density at -0.65 V in a flow cell with alkaline electrolyte. Density functional theory calculations further demonstrate that the high multicarbon product selectivity results from cooperation between AgCu single-atom alloys and Ag nanoparticles, wherein the Ag single-atom doping of Cu nanoparticles increases the adsorption energy of *CO on Cu sites due to the asymmetric bonding of the Cu atom to the adjacent Ag atom with a compressive strain.
Du, Cheng, et al. "Cascade electrocatalysis via AgCu single-atom alloy and Ag nanoparticles in CO<sub>2</sub> electroreduction toward multicarbon products." Nature Communications, vol. 14, no. 1, Oct. 2023. https://doi.org/10.1038/s41467-023-41871-w
Du, Cheng, Mills, Joel P., Yohannes, Asfaw G., et al., "Cascade electrocatalysis via AgCu single-atom alloy and Ag nanoparticles in CO<sub>2</sub> electroreduction toward multicarbon products," Nature Communications 14, no. 1 (2023), https://doi.org/10.1038/s41467-023-41871-w
@article{osti_2470252,
author = {Du, Cheng and Mills, Joel P. and Yohannes, Asfaw G. and Wei, Wei and Wang, Lei and Lu, Siyan and Lian, Jian-Xiang and Wang, Maoyu and Guo, Tao and Wang, Xiyang and others},
title = {Cascade electrocatalysis via AgCu single-atom alloy and Ag nanoparticles in CO<sub>2</sub> electroreduction toward multicarbon products},
annote = {Electrocatalytic CO2 reduction into value-added multicarbon products offers a means to close the anthropogenic carbon cycle using renewable electricity. However, the unsatisfactory catalytic selectivity for multicarbon products severely hinders the practical application of this technology. In this paper, we report a cascade AgCu single-atom and nanoparticle electrocatalyst, in which Ag nanoparticles produce CO and AgCu single-atom alloys promote C-C coupling kinetics. As a result, a Faradaic efficiency (FE) of 94 ± 4% toward multicarbon products is achieved with the as-prepared AgCu single-atom and nanoparticle catalyst under ~720 mA cm-2 working current density at -0.65 V in a flow cell with alkaline electrolyte. Density functional theory calculations further demonstrate that the high multicarbon product selectivity results from cooperation between AgCu single-atom alloys and Ag nanoparticles, wherein the Ag single-atom doping of Cu nanoparticles increases the adsorption energy of *CO on Cu sites due to the asymmetric bonding of the Cu atom to the adjacent Ag atom with a compressive strain.},
doi = {10.1038/s41467-023-41871-w},
url = {https://www.osti.gov/biblio/2470252},
journal = {Nature Communications},
issn = {ISSN 2041-1723},
number = {1},
volume = {14},
place = {United States},
publisher = {Nature Publishing Group},
year = {2023},
month = {10}}
Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); Natural Sciences and Engineering Research Council of Canada (NSERC); New Frontiers Research Fund-Transformation (NFRFT); John R. Evans Leaders Fund (JELF)