文献类型：期刊文献

英文题名：Unraveling the Mechanism of Cu/CeO2 Interface Modulation for CO2 Electroreduction Into C2+/CH4

作者：Xiong, Lei[1];Fu, Xianbiao[1];Zhang, Jun[2];Liu, Shuang[3];Li, Shanshan[3];Lu, Shaojie[1];Wang, Dong[4,5];Yue, Qin[1]

机构：[1]Univ Elect Sci & Technol China, Inst Fundamental & Frontier Sci, Chengdu 610054, Peoples R China;[2]Southwest Inst Chem Co Ltd, State Key Lab Ind Vent Gas Reuse, Chengdu 610225, Peoples R China;[3]Sichuan Univ, Coll Chem, Chengdu 610040, Peoples R China;[4]East China Univ Sci & Technol, Ctr Computat Chem, State Key Lab Green Chem Engn & Ind Catalysis, 130 Meilong Rd, Shanghai 200237, Peoples R China;[5]East China Univ Sci & Technol, Res Inst Ind Catalysis, Sch Chem & Mol Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China

年份：2025

卷号：35

期号：24

外文期刊名：ADVANCED FUNCTIONAL MATERIALS

收录：;EI(收录号：20250417749515);WOS:【SCI-EXPANDED(收录号:WOS:001404442300001)】；

基金：This project was supported financially by the National Key R&D Program of China (2021YFB3501900), the National Natural Science Foundation of China (22475031 and 22273021), the National Youth Top-notch Talent Support Program of China, and Shanghai Science and Technology Development Funds (22QA1402900).

语种：英文

外文关键词：C2+/CH4 selectivity; CO2RR; Cu/CeO2 interface; strong/weak adsorption

摘要：Cu shows unique characteristics for electrochemical CO2 reduction reaction (CO2RR) to hydrocarbons and oxygenates due to the moderate adsorption energy of the key intermediate *CO. However, it remains a challenge to selectively control CO2RR towards C-1 (e.g., CH4) or C2+ (e.g., C2H4 and C2H5OH) through simple interface engineering. Herein, a series of inverse catalysts, composed of CeO2 nanoparticles over Cu substrate (Cu-CeO2-x), are subtly designed to tackle the issues. It is verified CeO2 decoration induces highly active Cu/CeO2 interfacial sites that enhance the adsorption and conversion of CO2 and *CO intermediates into C2+ or CH4, while the Cu sites are conducive to *CO generation. With the increase of CeO2 deposition, the C2+ and CH4 selectivity present a volcano-type and increasing tendency with maximum faradic efficiency of 62.6% and 51.3%, respectively. In-situ infrared spectroscopy and theoretical calculations reveal that moderate CeO2 loading allows the Cu/CeO2 interfacial sites to cooperate efficiently with the Cu sites to promote the coupling of *CO/*CHO intermediates, thus enhancing the C2+ selectivity. In contrast, excessive CeO2 loading suppresses the C & horbar;C coupling but boosts unilaterally the hydrogenation, thus promoting the CH4 production. This work provides effective strategies to regulate the CO2RR selectivity by modulating metal/oxide interfaces.