Fe-N4O-C Nanoplates Covalently Bonding on Graphene for Efficient CO 2 Electroreduction and Zn-CO2 Batteries
Electrochemical carbon dioxide (CO2) reduction into value-added products holds great promise in moving toward carbon neutrality but remains a grand challenge due to lack of efficient electrocatalysts. Herein, the nucleophilic substitution reaction is elaborately harnessed to synthesize carbon nanopl...
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Published in | Advanced functional materials Vol. 33; no. 27 |
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Main Authors | , , , , , , , , , |
Format | Journal Article |
Language | English |
Published |
United States
Wiley
24.03.2023
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Subjects | |
Online Access | Get full text |
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Summary: | Electrochemical carbon dioxide (CO2) reduction into value-added products holds great promise in moving toward carbon neutrality but remains a grand challenge due to lack of efficient electrocatalysts. Herein, the nucleophilic substitution reaction is elaborately harnessed to synthesize carbon nanoplates with a Fe-N4O configuration anchored onto graphene substrate (Fe-N4O-C/Gr) through covalent linkages. Density functional theory calculations demonstrate the unique configuration of Fe-N4O with one oxygen (O) atom in the axial direction not only suppresses the competing hydrogen evolution reaction, but also facilitates the desorption of *CO intermediate compared with the commonly planar single-atomic Fe sites. The Fe-N4O-C/Gr shows excellent performance in the electroreduction of CO2 into carbon monoxide (CO) with an impressive Faradaic efficiency of 98.3% at -0.7 V versus reversible hydrogen electrode (RHE) and a high turnover frequency of 3511 h-1. Furthermore, as a cathode catalyst in an aqueous zinc (Zn)-CO2 battery, the Fe-N4O-C/Gr achieves a high CO Faradaic efficiency (≈91%) at a discharge current density of 3 mA cm-2 and long-term stability over 74 h. Here this work opens up a new route to simultaneously modulate the geometric and electronic structure of single-atomic catalysts toward efficient CO2 conversion. |
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Bibliography: | Ministry of Science and Technology of China BNL-224189-2023-JAAM USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO) National Natural Science Foundation of China (NSFC) SC0012704; 22105107; 2021YFA1201900; 020/C029201005 Central Universities |
ISSN: | 1616-301X 1616-3028 |