학술논문
Steering the Reaction Pathway of CO 2 Electroreduction by Tuning the Coordination Number of Copper Catalysts.
Document Type
Academic Journal
Author
Jiao J; Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular and Process Engineering, School of Chemistry and Molecular Engineering, East China Normal University, Shanghai 200062, China.; Institute of Eco-Chongming, Chongming District, Shanghai 202162, China.; Kang X; Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Centre for Excellence in Molecular Sciences, Centre for Carbon Neutral Chemistry, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China.; School of Chemistry and Chemical Engineering, University of Chinese Academy of Sciences, Beijing 100049, China.; Yang J; Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Centre for Excellence in Molecular Sciences, Centre for Carbon Neutral Chemistry, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China.; School of Chemistry and Chemical Engineering, University of Chinese Academy of Sciences, Beijing 100049, China.; Jia S; Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular and Process Engineering, School of Chemistry and Molecular Engineering, East China Normal University, Shanghai 200062, China.; Institute of Eco-Chongming, Chongming District, Shanghai 202162, China.; Peng Y; Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Centre for Excellence in Molecular Sciences, Centre for Carbon Neutral Chemistry, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China.; Liu S; Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Centre for Excellence in Molecular Sciences, Centre for Carbon Neutral Chemistry, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China.; Chen C; Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular and Process Engineering, School of Chemistry and Molecular Engineering, East China Normal University, Shanghai 200062, China.; Institute of Eco-Chongming, Chongming District, Shanghai 202162, China.; Xing X; Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China.; He M; Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular and Process Engineering, School of Chemistry and Molecular Engineering, East China Normal University, Shanghai 200062, China.; Institute of Eco-Chongming, Chongming District, Shanghai 202162, China.; Wu H; Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular and Process Engineering, School of Chemistry and Molecular Engineering, East China Normal University, Shanghai 200062, China.; Institute of Eco-Chongming, Chongming District, Shanghai 202162, China.; Han B; Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular and Process Engineering, School of Chemistry and Molecular Engineering, East China Normal University, Shanghai 200062, China.; Institute of Eco-Chongming, Chongming District, Shanghai 202162, China.; Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Centre for Excellence in Molecular Sciences, Centre for Carbon Neutral Chemistry, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China.; School of Chemistry and Chemical Engineering, University of Chinese Academy of Sciences, Beijing 100049, China.
Source
Publisher: American Chemical Society Country of Publication: United States NLM ID: 7503056 Publication Model: Print-Electronic Cited Medium: Internet ISSN: 1520-5126 (Electronic) Linking ISSN: 00027863 NLM ISO Abbreviation: J Am Chem Soc Subsets: PubMed not MEDLINE; MEDLINE
Subject
Language
English
Abstract
Cu-based catalysts are optimal for the electroreduction of CO 2 to generate hydrocarbon products. However, controlling product distribution remains a challenging topic. The theoretical investigations have revealed that the coordination number (CN) of Cu considerably influences the adsorption energy of *CO intermediates, thereby affecting the reaction pathway. Cu catalysts with different CNs were fabricated by reducing CuO precursors via cyclic voltammetry (Cyc-Cu), potentiostatic electrolysis (Pot-Cu), and pulsed electrolysis (Pul-Cu), respectively. High-CN Cu catalysts predominantly generate C 2+ products, while low-CN Cu favors CH 4 production. For instance, over the high-CN Pot-Cu, C 2+ is the main product, with the Faradaic efficiency (FE) reaching 82.5% and a partial current density ( j ) of 514.3 mA cm -2 . Conversely, the low-CN Pul(3)-Cu favors the production of CH 4 , achieving the highest FE CH4 value of 56.7% with a j CH4 value of 234.4 mA cm -2 . In situ X-ray absorption spectroscopy and Raman spectroscopy studies further confirm the different *CO adsorptions over Cu catalysts with different CN, thereby directing the reaction pathway of the CO 2 RR.