Highly Efficient CO2 Electroreduction on ZnN4‐based Single‐Atom Catalyst |
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Authors: | Fa Yang Dr Ping Song Xiaozhi Liu Bingbao Mei Prof Wei Xing Prof Zheng Jiang Prof Lin Gu Prof Weilin Xu |
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Institution: | 1. State Key Laboratory of Electroanalytical Chemistry, Jilin Province Key Laboratory of Low Carbon Chemical Power, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, P. R. China;2. University of Science and Technology of China, Hefei, China;3. Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing, China;4. School of Physical Sciences, University of Chinese Academy of Sciences, Beijing, China;5. Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai, China;6. Collaborative Innovation Center of Quantum Matter, Beijing, China |
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Abstract: | The electrochemical reduction reaction of carbon dioxide (CO2RR) to carbon monoxide (CO) is the basis for the further synthesis of more complex carbon‐based fuels or attractive feedstock. Single‐atom catalysts have unique electronic and geometric structures with respect to their bulk counterparts, thus exhibiting unexpected catalytic activities. A nitrogen‐anchored Zn single‐atom catalyst is presented for CO formation from CO2RR with high catalytic activity (onset overpotential down to 24 mV), high selectivity (Faradaic efficiency for CO (FECO) up to 95 % at ?0.43 V), remarkable durability (>75 h without decay of FECO), and large turnover frequency (TOF, up to 9969 h?1). Further experimental and DFT results indicate that the four‐nitrogen‐anchored Zn single atom (Zn‐N4) is the main active site for CO2RR with low free energy barrier for the formation of *COOH as the rate‐limiting step. |
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Keywords: | carbon dioxide electroreduction single-atom catalysts zinc |
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