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Robust Electrocatalytic CO2 Reduction in Acid Enabled by "Molecularly Charged" Cobalt Phthalocyanine: A Profound Understanding from Electric Double Layer.
Jiao, Zhenyang; Song, Daqi; Wei, Le; Ma, Mutian; Hua, Wei; Zheng, Zhangyi; Wang, Min; Su, Yanhui; Ke, Xiaoxing; Lyu, Fenglei; Deng, Zhao; Zhong, Jun; Peng, Yang.
Affiliation
  • Jiao Z; Soochow Institute for Energy and Materials Innovations, College of Energy, Soochow University, Suzhou 215006, P. R. China.
  • Song D; Soochow Institute for Energy and Materials Innovations, College of Energy, Soochow University, Suzhou 215006, P. R. China.
  • Wei L; Beijing Key Laboratory of Microstructure and Properties of Solids, College of Materials Science and Engineering, Beijing University of Technology, Beijing 100124, P. R. China.
  • Ma M; Soochow Institute for Energy and Materials Innovations, College of Energy, Soochow University, Suzhou 215006, P. R. China.
  • Hua W; Soochow Institute for Energy and Materials Innovations, College of Energy, Soochow University, Suzhou 215006, P. R. China.
  • Zheng Z; Soochow Institute for Energy and Materials Innovations, College of Energy, Soochow University, Suzhou 215006, P. R. China.
  • Wang M; Soochow Institute for Energy and Materials Innovations, College of Energy, Soochow University, Suzhou 215006, P. R. China.
  • Su Y; Soochow Institute for Energy and Materials Innovations, College of Energy, Soochow University, Suzhou 215006, P. R. China.
  • Ke X; Beijing Key Laboratory of Microstructure and Properties of Solids, College of Materials Science and Engineering, Beijing University of Technology, Beijing 100124, P. R. China.
  • Lyu F; Soochow Institute for Energy and Materials Innovations, College of Energy, Soochow University, Suzhou 215006, P. R. China.
  • Deng Z; Jiangsu Key Laboratory of Advanced Negative Carbon Technologies, Soochow University, Suzhou 215006, P. R. China.
  • Zhong J; Soochow Institute for Energy and Materials Innovations, College of Energy, Soochow University, Suzhou 215006, P. R. China.
  • Peng Y; Jiangsu Key Laboratory of Advanced Negative Carbon Technologies, Soochow University, Suzhou 215006, P. R. China.
J Phys Chem Lett ; 15(28): 7342-7350, 2024 Jul 18.
Article in En | MEDLINE | ID: mdl-38989694
ABSTRACT
Electrocatalytic CO2 reduction (eCO2R) in acid holds promise in renewable electricity-powered CO2 utilization with high efficiency, but the hydrogen evolution reaction (HER) often prevails and results in a low eCO2R selectivity. Here, using cobalt phthalocyanine/Ketjen black (CoPc/KB) as the model catalysts, we systematically study the effect of active site density, operational current density, and hydrated cations on the acidic eCO2R selectivity and decipher it through the componential dynamics of electric double layer (EDL). The optimal CoPc-4/KB demonstrates a near-unity CO Faradaic efficiency from 50 to 400 mA cm-2 and superb operational stability (>120 h) at 100 mA cm-2. Aided by in situ Raman and infrared spectroscopies, we reveal that the proper cations establish an electrostatic shield for mitigating bulk H+ penetration and mediate the interfacial water structure for suppressing HER. This study should elicit further profound thinking on robust eCO2R system design from the perspective of multiphasic and dynamic EDL.
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Full text: 1 Collection: 01-internacional Database: MEDLINE Language: En Journal: J Phys Chem Lett Year: 2024 Type: Article
Fulltext
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Full text: 1 Collection: 01-internacional Database: MEDLINE Language: En Journal: J Phys Chem Lett Year: 2024 Type: Article