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Switching Product Selectivity in CO2 Electroreduction via Cu-S Bond Length Variation.
Wei, Xiaoqian; Li, Zijian; Jang, Haeseong; Gyu Kim, Min; Liu, Shangguo; Cho, Jaephil; Liu, Xien; Qin, Qing.
Afiliación
  • Wei X; College of Chemical Engineering, Qingdao University of Science and Technology, Qingdao, 266042, China.
  • Li Z; Department of Chemistry, City University of Hong Kong, Hong Kong SAR, 999077, China.
  • Jang H; Department of Advanced Materials Engineering, Chung-Ang University, Anseong-si, Gyeonggi-do, 17546, Korea.
  • Gyu Kim M; Beamline Research Division, Pohang Accelerator Laboratory (PAL), Pohang, 37673, South Korea.
  • Liu S; College of Chemical Engineering, Qingdao University of Science and Technology, Qingdao, 266042, China.
  • Cho J; Department of Energy Engineering, School of Energy and Chemical Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan, 689-798, South Korea.
  • Liu X; College of Chemical Engineering, Qingdao University of Science and Technology, Qingdao, 266042, China.
  • Qin Q; College of Chemical Engineering, Qingdao University of Science and Technology, Qingdao, 266042, China.
Angew Chem Int Ed Engl ; 63(39): e202409206, 2024 Sep 23.
Article en En | MEDLINE | ID: mdl-38975661
ABSTRACT
Regulating competitive reaction pathways to direct the selectivity of electrochemical CO2 reduction reaction toward a desired product is crucial but remains challenging. Herein, switching product from HCOOH to CO is achieved by incorporating Sb element into the CuS, in which the Cu-S ionic bond is coupled with S-Sb covalent bond through bridging S atoms that elongates the Cu-S bond from 2.24 Što 2.30 Å. Consequently, CuS with a shorter Cu-S bond exhibited a high selectivity for producing HCOOH, with a maximum Faradaic efficiency (FE) of 72 %. Conversely, Cu3SbS4 characterized by an elongated Cu-S bond exhibited the most pronounced production of CO with a maximum FE of 60 %. In situ spectroscopy combined with density functional theory calculations revealed that the altered Cu-S bond length and local coordination environment make the *HCOO binding energy weaker on Cu3SbS4 compared to that on CuS. Notably, a volcano-shaped correlation between the Cu-S bond length and adsorption strength of *COOH indicates that Cu-S in Cu3SbS4 as double-active sites facilitates the adsorption of *COOH, and thus results in the high selectivity of Cu3SbS4 toward CO.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Angew Chem Int Ed Engl Año: 2024 Tipo del documento: Article País de afiliación: China Pais de publicación: Alemania

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Angew Chem Int Ed Engl Año: 2024 Tipo del documento: Article País de afiliación: China Pais de publicación: Alemania