Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 62, Issue 10, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202215406
Keywords
*CO Spillover; *CO Transfer; C2+ Products; CO2 Electroreduction; Single Atom Catalyst
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Researchers developed a method to engineer single nickel atoms on a pyridinic nitrogen-enriched carbon support, which served as a donor for adjacent copper nanoparticles to improve the selectivity of electroreduction of CO2 to C2H4. The presence of isolated nickel atoms and adjacent pyridinic nitrogen species facilitated the desorption of *CO, leading to an enhanced *CO coverage on the copper nanoparticles and improved selectivity.
Cu-based catalysts have been widely applied in electroreduction of carbon dioxide (CO2ER) to produce multicarbon (C2+) feedstocks (e.g., C2H4). However, the high energy barriers for CO2 activation on the Cu surface is a challenge for a high catalytic efficiency and product selectivity. Herein, we developed an in situ *CO generation and spillover strategy by engineering single Ni atoms on a pyridinic N-enriched carbon support with a sodalite (SOD) topology (Ni-SOD/NC) that acted as a donor to feed adjacent Cu nanoparticles (NPs) with *CO intermediate. As a result, a high C2H4 selectivity of 62.5 % and an industrial-level current density of 160 mA cm(-2) at a low potential of -0.72 V were achieved. Our studies revealed that the isolated NiN3 active sites with adjacent pyridinic N species facilitated the *CO desorption and the massive *CO intermediate released from Ni-SOD/NC then overflowed to Cu NPs surface to enrich the *CO coverage for improving the selectivity of CO2ER to C2H4.
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