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Dynamic Surface Reconstruction of Amphoteric Metal (Zn, Al) Doped Cu 2 O for Efficient Electrochemical CO 2 Reduction to C 2+ Products.

Yufei JiaYunxuan DingTao SongYunlong XuYaqing LiLele DuanFei LiLicheng SunKe Fan
Published in: Advanced science (Weinheim, Baden-Wurttemberg, Germany) (2023)
The recognition of the surface reconstruction of the catalysts during electrochemical CO 2 reduction (CO2RR) is essential for exploring and comprehending active sites. Although the superior performance of Cu-Zn bimetallic sites toward multicarbon C 2+ products has been established, the dynamic surface reconstruction has not been fully understood. Herein, Zn-doped Cu 2 O nano-octahedrons are used to investigate the effect of the dynamic stability by the leaching and redeposition on CO2RR. Correlative characterizations confirm the Zn leaching from Zn-doped Cu 2 O, which is redeposited at the surface of the catalysts, leading to dynamic stability and abundant Cu-Zn bimetallic sites at the surface. The reconstructed Zn-doped Cu 2 O catalysts achieve a high Faradaic efficiency (FE) of C 2+ products (77% at -1.1 V versus reversible hydrogen electrode (RHE)). Additionally, similar dynamic stability is also discovered in Al-doped Cu 2 O for CO2RR, proving its universality in amphoteric metal-doped catalysts. Mechanism analyses reveal that the OHC-CHO pathway can be the C-C coupling processes on bare Cu 2 O and Zn-doped Cu 2 O, and the introduction of Zn to Cu can efficiently lower the energy barrier for CO2RR to C 2 H 4 . This research provides profound insight into unraveling surface dynamic reconstruction of amphoteric metal-containing electrocatalysts and can guide rational design of the high-performance electrocatalysts for CO2RR.
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