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Accelerated Transfer and Spillover of Carbon Monoxide through Tandem Catalysis for Kinetics-boosted Ethylene Electrosynthesis |
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| Authors: | Jiayi Chen Dr Dashuai Wang Xiaoxuan Yang Wenjun Cui Prof?Dr Xiahan Sang Zilin Zhao Dr Liguang Wang Dr Zhongjian Li Dr Bin Yang Prof?Dr Lecheng Lei Prof?Dr Jinyang Zheng Prof?Dr Liming Dai Prof?Dr Yang Hou |
| Institution: | 1. Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, 310027 China
These authors contributed equally to this work.;2. Institute of Zhejiang University - Quzhou, Quzhou, 324000 China These authors contributed equally to this work.;3. Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, 310027 China;4. Nanostructure Research Center, Wuhan University of Technology, Wuhan, 430070 China;5. Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, 310027 China Institute of Zhejiang University - Quzhou, Quzhou, 324000 China;6. Donghai Laboratory, Zhoushan, China Institute of Process Equipment, Zhejiang University, Hangzhou, China;7. Australian Carbon Materials Centre(A-CMC), School of Chemical Engineering, University of New South Wales, Sydney, NSW 2052 Australia |
| Abstract: | 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. |
| Keywords: | *CO Spillover *CO Transfer C2+ Products CO2 Electroreduction Single Atom Catalyst |