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Dual regulation of geometry and water activation over coherent interface-rich inverse CeO2/CuO catalysts enabling highly selective CO2 electroreduction from C2H4 to CH4

Yue Shen,Jielian Yang,Bing Chen,Chunyan Zhou,Liya Zhou,Binbin Luo,Qi Pang,Peican Chen,Xuetang Xu,Anxiang Guan

Developing efficient electrocatalysts capable of achieving effective electrochemical CO 2 -to-CH 4 conversion over a broad potential window remains a significant challenge in the field. Herein, we present a facile strategy for the synthesis of inverse CeO 2 /CuO catalysts through a hydrothermal approach, wherein CeO 2 nanodomains are supported on the surface of CuO. This catalyst exhibits exceptionally high CH 4 selectivity across the investigated voltage range, with a peak Faradaic efficiency of 63.6% and a corresponding partial current density of −472.9 mA cm −2 at −1.6 V vs. RHE, while the pure CuO catalyst without CeO 2 component was found to be active for electroreducing CO 2 to C 2+ products (C 2 H 4 ), as the adjacent Cu sites were beneficial for adsorbing multiple *CO intermediates and subsequent C C coupling. The incorporation of CeO 2 into Cu 1 Ce 9 -O x exerts a dual regulatory effect, synergistically suppressing C C coupling by reducing *CO coverage and optimizing *CO protonation kinetics for enhanced CH 4 selectivity. The presence of CeO 2 not only blocks the active sites of CuO for CO 2 -to-*CO intermediate conversion (thus lowering *CO coverage) but also facilitates water dissociation to generate abundant *H species, which subsequently migrate to Cu sites in Cu 1 Ce 9 -O x catalyst through the coherent interface between CuO and CeO 2 . These *H species subsequently facilitate the hydrogenation of *CO intermediates, ultimately resulting in CH 4 formation. Density functional theory (DFT) calculations demonstrate that CuCe-O x catalyst with strong H 2 O dissociation capability decreases the energy barrier for *CHO formation and favors *CO → *CHO conversion, thereby promoting CO 2 RR-to-CH 4 conversion. This work provides an effective strategy to enhance *H generation and the hydrogenation of *CO intermediates, thereby offering a feasible approach to improve CH 4 production efficiency in electrochemical CO 2 conversion. Compared with pristine CuO, CeO 2 nanodomains anchored on CuO surfaces redirect CO 2 electroreduction selectivity from C 2 H 4 to CH 4 . The presence of CeO 2 not only modulate *CO intermediate coverage but also accelerate H 2 O dissociation to produce abundant *H species, thereby promoting *CO protonation and boosting CH 4 formation with enhanced Faradaic efficiency. Download: Download high-res image (170KB) Download: Download full-size image