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Unraveling the rate-determining step of C2+ products during electrochemical CO reduction.
Deng, Wanyu; Zhang, Peng; Qiao, Yu; Kastlunger, Georg; Govindarajan, Nitish; Xu, Aoni; Chorkendorff, Ib; Seger, Brian; Gong, Jinlong.
Afiliación
  • Deng W; Key Laboratory for Green Chemical Technology of Ministry of Education, School of Chemical Engineering and Technology, Tianjin University, Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin, 300072, China.
  • Zhang P; Joint School of National University of Singapore and Tianjin University, International Campus of Tianjin University, Binhai New City, Fuzhou, 350207, China.
  • Qiao Y; Department of Physics, Technical University of Denmark, 2800 Kgs, Lyngby, Denmark.
  • Kastlunger G; Key Laboratory for Green Chemical Technology of Ministry of Education, School of Chemical Engineering and Technology, Tianjin University, Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin, 300072, China.
  • Govindarajan N; Joint School of National University of Singapore and Tianjin University, International Campus of Tianjin University, Binhai New City, Fuzhou, 350207, China.
  • Xu A; Department of Physics, Technical University of Denmark, 2800 Kgs, Lyngby, Denmark.
  • Chorkendorff I; Department of Physics, Technical University of Denmark, 2800 Kgs, Lyngby, Denmark.
  • Seger B; Department of Physics, Technical University of Denmark, 2800 Kgs, Lyngby, Denmark.
  • Gong J; Department of Physics, Technical University of Denmark, 2800 Kgs, Lyngby, Denmark.
Nat Commun ; 15(1): 892, 2024 Jan 30.
Article en En | MEDLINE | ID: mdl-38291057
ABSTRACT
The electrochemical reduction of CO has drawn a large amount of attention due to its potential to produce sustainable fuels and chemicals by using renewable energy. However, the reaction's mechanism is not yet well understood. A major debate is whether the rate-determining step for the generation of multi-carbon products is C-C coupling or CO hydrogenation. This paper conducts an experimental analysis of the rate-determining step, exploring pH dependency, kinetic isotope effects, and the impact of CO partial pressure on multi-carbon product activity. Results reveal constant multi-carbon product activity with pH or electrolyte deuteration changes, and CO partial pressure data aligns with the theoretical formula derived from *CO-*CO coupling as the rate-determining step. These findings establish the dimerization of two *CO as the rate-determining step for multi-carbon product formation. Extending the study to commercial copper nanoparticles and oxide-derived copper catalysts shows their rate-determining step also involves *CO-*CO coupling. This investigation provides vital kinetic data and a theoretical foundation for enhancing multi-carbon product production.

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Nat Commun Asunto de la revista: BIOLOGIA / CIENCIA Año: 2024 Tipo del documento: Article País de afiliación: China Pais de publicación: Reino Unido

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Nat Commun Asunto de la revista: BIOLOGIA / CIENCIA Año: 2024 Tipo del documento: Article País de afiliación: China Pais de publicación: Reino Unido