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Elucidating the Electrocatalytic CO2 Reduction Reaction over a Model Single-Atom Nickel Catalyst |
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| Authors: | Dr Song Liu Prof Hong Bin Yang Dr Sung-Fu Hung Jie Ding Weizheng Cai Linghui Liu Dr Jiajian Gao Dr Xuning Li Xinyi Ren Zhichong Kuang Prof Yanqiang Huang Prof Tao Zhang Prof Bin Liu |
| Institution: | 1. CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Road, Dalian, 116023 China
University of Chinese Academy of Sciences, Beijing, 100049 China School of Chemical and Biomedical Engineering, Nanyang Technological University, 62 Nanyang Drive, Singapore, 637459 Singapore;2. School of Chemical and Biomedical Engineering, Nanyang Technological University, 62 Nanyang Drive, Singapore, 637459 Singapore;3. Department of Chemistry, National (Taiwan) University, No. 1, Sec. 4, Roosevelt Rd, Taipei, 10617 Taiwan;4. CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Road, Dalian, 116023 China;5. CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Road, Dalian, 116023 China School of Chemistry and Chemical Engineering, Chongqing University, Shapingba 174, Chongqing, 400044 P. R. China;6. CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Road, Dalian, 116023 China University of Chinese Academy of Sciences, Beijing, 100049 China |
| Abstract: | Designing effective electrocatalysts for the carbon dioxide reduction reaction (CO2RR) is an appealing approach to tackling the challenges posed by rising CO2 levels and realizing a closed carbon cycle. However, fundamental understanding of the complicated CO2RR mechanism in CO2 electrocatalysis is still lacking because model systems are limited. We have designed a model nickel single-atom catalyst (Ni SAC) with a uniform structure and well-defined Ni-N4 moiety on a conductive carbon support with which to explore the electrochemical CO2RR. Operando X-ray absorption near-edge structure spectroscopy, Raman spectroscopy, and near-ambient X-ray photoelectron spectroscopy, revealed that Ni+ in the Ni SAC was highly active for CO2 activation, and functioned as an authentic catalytically active site for the CO2RR. Furthermore, through combination with a kinetics study, the rate-determining step of the CO2RR was determined to be *CO2−+H+→*COOH. This study tackles the four challenges faced by the CO2RR; namely, activity, selectivity, stability, and dynamics. |
| Keywords: | Aktive Zentren Einzelatomkatalyse Elektrochemie In-situ-Reaktionen Reaktionsmechanismen |