Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume -, Issue -, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202306456
Keywords
CO2 Electrochemical Reduction; DFT Calculations; Heterostructure; in-Situ Characterization; Selectivity to Ethanol
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This study elucidates the structural reconstruction of CuO/SnO2 during CO2 elecrochemical reduction and reveals the intrinsic relationship between structural reconstruction and product selectivity. The ability to control the product selectivity through specific electrode potentials and evolved heterostructures provides new insights for designing efficient CO2ER catalysts.
Heterostructured oxides with versatile active sites, as a class of efficient catalysts for CO2 electrochemical reduction (CO2ER), are prone to undergo structure reconstruction under working conditions, thus bringing challenges to understanding the reaction mechanism and rationally designing catalysts. Herein, we for the first time elucidate the structural reconstruction of CuO/SnO2 under electrochemical potentials and reveal the intrinsic relationship between CO2ER product selectivity and the in situ evolved heterostructures. At -0.85 V-RHE, the CuO/SnO2 evolves to Cu2O/SnO2 with high selectivity to HCOOH (Faradaic efficiency of 54.81 %). Mostly interestingly, it is reconstructed to Cu/SnO2-x at -1.05 V-RHE with significantly improved Faradaic efficiency to ethanol of 39.8 %. In situ Raman spectra and density functional theory (DFT) calculations reveal that the synergetic absorption of *COOH and *CHOCO intermediates at the interface of Cu/SnO2-x favors the formation of *CO and decreases the energy barrier of C-C coupling, leading to high selectivity to ethanol.
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