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Synthesis and Performance Characterizations of Transition Metal Single Atom Catalyst for Electrochemical CO2 Reduction
Published on: April 10, 2018
Copper Oxidation State Stabilization and Oxygen Vacancy Engineering in Perovskite Catalysts for Selective
Meng-Qi Zhang1, Meng Shi1, Ke-Xin Du1
1School of Chemical and Environmental Engineering, Anhui Polytechnic University, Wuhu, Anhui241000, P. R. China.
None:
The selective electroreduction of CO2 to multicarbon products requires stabilization of Cuδ+ sites, which are prone to over-reduction. A synergistic strategy addressing this challenge was demonstrated through the incorporation of variable-valence rare-earth elements into the A-site of a layered perovskite structure. Optimal Ce doping (x = 0.06) simultaneously stabilizes Cuδ+ and enriches oxygen vacancies (Ovs). The catalyst achieves 79.02% faradaic efficiency for C2H4 at -0.9 V vs RHE, with a partial current density of 66.38 mA cm-2 and exceptional operational stability exceeding 42 h with negligible current decay. Experiments and DFT calculations reveal that Ce induces charge redistribution around Cu-O units, enhances the density of states near the Fermi level, and upshifts the d-band center from -2.08 to -1.53 eV, strengthening intermediate adsorption and lowering the *CO dimerization barrier. The synergy between stabilized Cuδ+ and Ovs provides a rational design for selective CO2-to-C2H4 conversion.
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