Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 59, Issue 8, Pages 3033-3037Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201912719
Keywords
CO2 electroreduction; density functional theory; high activity; selectivity control; syngas production
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Funding
- US Department of Energy, Basic Energy Sciences, Catalysis Science Program [DE-FG02-13ER16381]
- Center for Functional Nanomaterials (CFN) [DE-SC0012704]
- National Science Foundation [TG-CHE190032, ACI-1548562]
- National Key R&D Program of China [2017YFA0303500]
- China Scholarship Council (CSC) [201806340016, 201806010243]
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The electrochemical CO2 reduction reaction (CO2RR) to yield synthesis gas (syngas, CO and H-2) has been considered as a promising method to realize the net reduction in CO2 emission. However, it is challenging to balance the CO2RR activity and the CO/H-2 ratio. To address this issue, nitrogen-doped carbon supported single-atom catalysts are designed as electrocatalysts to produce syngas from CO2RR. While Co and Ni single-atom catalysts are selective in producing H-2 and CO, respectively, electrocatalysts containing both Co and Ni show a high syngas evolution (total current >74 mA cm(-2)) with CO/H-2 ratios (0.23-2.26) that are suitable for typical downstream thermochemical reactions. Density functional theory calculations provide insights into the key intermediates on Co and Ni single-atom configurations for the H-2 and CO evolution. The results present a useful case on how non-precious transition metal species can maintain high CO2RR activity with tunable CO/H-2 ratios.
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