Single atom and defect engineering of CuO for efficient electrochemical reduction of CO2 to C2H4

Autor: Senlin Chu, Changwoo Kang, Woonghyeon Park, Yu Han, Song Hong, Leiduan Hao, Hao Zhang, Tsz Woon Benedict Lo, Alex W. Robertson, Yousung Jung, Buxing Han, Zhenyu Sun
Jazyk: angličtina
Rok vydání: 2022
Předmět:
Zdroj: SmartMat, Vol 3, Iss 1, Pp 194-205 (2022)
Druh dokumentu: article
ISSN: 2688-819X
DOI: 10.1002/smm2.1105
Popis: Abstract Electrochemical CO2 transformation to high‐value ethylene (C2H4) at high currents and efficiencies is desired and yet remains a grand challenge. We show for the first time that coupling single Sb atoms and oxygen vacancies of CuO enable synergistic electrocatalytic reduction of CO2 to C2H4 at low overpotentials. Highly dispersed Sb atoms occupying metal substitutional sites of CuO are synthesized under mild conditions. The overall CO2 reduction faradaic efficiency (FE) reaches 89.3 ± 1.1% with an FE toward C2H4 exceeding 58.4% at a high‐current density of 500 mA/cm2. Addition of the p‐block metal is found to induce transformation of CuO from flakes to nanoribbons rich in nanoholes and oxygen vacancies, greatly enhancing CO2 adsorption and activation while suppressing hydrogen evolution. Further density functional theory calculations with in situ X‐ray diffraction reveal that combining Sb sites and oxygen vacancies prominently lessen the dimerization energy of adsorbed CO intermediate, thus boosting the conversion of CO2 to produce C2H4. This study provides a new perspective for promoting selective C–C coupling for electrochemical CO2 reduction.
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