Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 58, Issue 21, Pages 6972-6976Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201901575
Keywords
CO2 reduction; electrocatalysts; metal centers; single-atom catalysts
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Funding
- Australian Government
- Australian Research Council [DP160103107, FT170100224, LE160100051]
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Polynary single-atom structures can combine the advantages of homogeneous and heterogeneous catalysts while providing synergistic functions based on different molecules and their interfaces. However, the fabrication and identification of such an active-site prototype remain elusive. Here we report isolated diatomic Ni-Fe sites anchored on nitrogenated carbon as an efficient electrocatalyst for CO2 reduction. The catalyst exhibits high selectivity with CO Faradaic efficiency above 90% over a wide potential range from -0.5 to -0.9V (98% at -0.7V), and robust durability, retaining 99% of its initial selectivity after 30hours of electrolysis. Density functional theory studies reveal that the neighboring Ni-Fe centers not only function in synergy to decrease the reaction barrier for the formation of COOH* and desorption of CO, but also undergo distinct structural evolution into a CO-adsorbed moiety upon CO2 uptake.
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