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Complementary Operando Spectroscopy identification of in-situ generated metastable charge-asymmetry Cu2-CuN3 clusters for CO2 reduction to ethanol.
Su, Xiaozhi; Jiang, Zhuoli; Zhou, Jing; Liu, Hengjie; Zhou, Danni; Shang, Huishan; Ni, Xingming; Peng, Zheng; Yang, Fan; Chen, Wenxing; Qi, Zeming; Wang, Dingsheng; Wang, Yu.
Afiliação
  • Su X; Shanghai Synchrotron Radiation Facility, Zhangjiang Laboratory, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai, 201204, China.
  • Jiang Z; Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing, 100081, China.
  • Zhou J; Department of Chemistry, Tsinghua University, Beijing, 100084, China.
  • Liu H; Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai, 201800, China.
  • Zhou D; National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui, 230029, China.
  • Shang H; Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing, 100081, China.
  • Ni X; Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing, 100081, China.
  • Peng Z; School of Physical Science and Technology, ShanghaiTech University, Shanghai, 201210, China.
  • Yang F; School of Physical Science and Technology, ShanghaiTech University, Shanghai, 201210, China.
  • Chen W; School of Physical Science and Technology, ShanghaiTech University, Shanghai, 201210, China.
  • Qi Z; Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing, 100081, China. wxchen@bit.edu.cn.
  • Wang D; National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui, 230029, China.
  • Wang Y; Department of Chemistry, Tsinghua University, Beijing, 100084, China.
Nat Commun ; 13(1): 1322, 2022 Mar 11.
Article em En | MEDLINE | ID: mdl-35277523
Copper-based materials can reliably convert carbon dioxide into multi-carbon products but they suffer from poor activity and product selectivity. The atomic structure-activity relationship of electrocatalysts for the selectivity is controversial due to the lacking of systemic multiple dimensions for operando condition study. Herein, we synthesized high-performance CO2RR catalyst comprising of CuO clusters supported on N-doped carbon nanosheets, which exhibited high C2+ products Faradaic efficiency of 73% including decent ethanol selectivity of 51% with a partial current density of 14.4 mA/cm-2 at -1.1 V vs. RHE. We evidenced catalyst restructuring and tracked the variation of the active states under reaction conditions, presenting the atomic structure-activity relationship of this catalyst. Operando XAS, XANES simulations and Quasi-in-situ XPS analyses identified a reversible potential-dependent transformation from dispersed CuO clusters to Cu2-CuN3 clusters which are the optimal sites. This cluster can't exist without the applied potential. The N-doping dispersed the reduced Cun clusters uniformly and maintained excellent stability and high activity with adjusting the charge distribution between the Cu atoms and N-doped carbon interface. By combining Operando FTIR and DFT calculations, it was recognized that the Cu2-CuN3 clusters displayed charge-asymmetric sites which were intensified by CH3* adsorbing, beneficial to the formation of the high-efficiency asymmetric ethanol.

Texto completo: 1 Coleções: 01-internacional Base de dados: MEDLINE Tipo de estudo: Diagnostic_studies Idioma: En Revista: Nat Commun Assunto da revista: BIOLOGIA / CIENCIA Ano de publicação: 2022 Tipo de documento: Article País de afiliação: China

Texto completo: 1 Coleções: 01-internacional Base de dados: MEDLINE Tipo de estudo: Diagnostic_studies Idioma: En Revista: Nat Commun Assunto da revista: BIOLOGIA / CIENCIA Ano de publicação: 2022 Tipo de documento: Article País de afiliação: China