Construction of coherent interface between Cu 2 O and CeO 2 via electrochemical reconstruction for efficient carbon dioxide reduction to methane.

Developing an efficient electrocatalyst that enables the efficient electrochemical conversion from CO ₂ to CH ₄ across a wide potential range remains a formidable challenge. Herein, we introduce a precatalyst strategy that realizes the in situ electrochemical reconstruction of ultrafine Cu ₂ O nanodomains, intricately coupled on the CeO ₂ surface (Cu ₂ O/CeO ₂ ), originating from the heterointerface comprised of ultrafine CuO nanodomains on the CeO ₂ surface (CuO/CeO ₂ ). When served as the electrocatalyst for the electrochemical CO ₂ reduction reaction, Cu ₂ O/CeO ₂ delivers a selectivity higher than 49 % towards CH ₄ over a broad potential range from -1.2 V to -1.7 V vs. RHE, maintaining negligible activity decay for 20 h. Notably, the highest selectivity for CH ₄ reaches an impressive 70 % at -1.5 V vs. RHE. Through the combination of comprehensive analysis including synchrotron X-ray absorption spectroscopy, spherical aberration-corrected high-angle annular dark field scanning transmission electron microscope as well as the density functional theoretical calculation, the efficient production of CH ₄ is attributed to the coherent interface between Cu ₂ O and CeO ₂ , which could converted from the original CuO and CeO ₂ interface, ensuring abundant active sites and enhanced intrinsic activity and selectivity towards CH ₄ .
Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.
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