文献类型：期刊文献

英文题名：Hydrophobically modified Cu2O nanocube for selective CO2 electroreduction to C2+ products

作者：Li, Congcong[1];Guo, Zhongyuan[2,3];Mao, Xiaoqing[1];Shen, Yongjun[1];Yang, Saiwu[1];Jiang, Yingfang[1];Tang, Pinghui[1];Li, Hao[2];Li, Huihui[1];Li, Chunzhong[1,4]

机构：[1]East China Univ Sci & Technol, Sch Chem Engn, Key Lab Ultrafine Mat, Minist Educ, Shanghai, Peoples R China;[2]Tohoku Univ, Adv Inst Mat Res WPI AIMR, Sendai 9808577, Japan;[3]Zhejiang Univ, Coll Environm & Resource Sci, Hangzhou, Peoples R China;[4]East China Univ Sci & Technol, Shanghai Engn Res Ctr Hierarch Nanomat, Sch Mat Sci & Engn, Shanghai, Peoples R China

年份：2025

卷号：71

期号：11

外文期刊名：AICHE JOURNAL

收录：;EI(收录号：20253318977966);WOS:【SCI-EXPANDED(收录号:WOS:001549920000001)】；

基金：This work was supported by the National Natural Science Foundation of China (U22B20143, U24A20546, 22478121), Shanghai Municipal Science and Technology Major Project, the Science and Technology Commission of Shanghai Municipality (22dz1205900), JSPS KAKENHI (JP23K13703), and the Postdoctoral Fellowship Program of CPSF under the Grant Number (GZC20241472), and the AIMR Fusion Research. We also acknowledge the Center for Computational Materials Science, Institute for Materials Research, Tohoku University for the use of MASAMUNE-IMR (202412-SCKXX-0211).

语种：英文

外文关键词：C-C coupling; dual function; electrochemical CO2 reduction; hydrophobicity; multicarbon products

摘要：The electrochemical conversion of CO2 into carbonaceous fuels and chemicals emerges as a promising sustainable strategy toward energy-rich chemical feedstocks. However, CO2 reduction reaction (CO2RR) in aqueous environments is highly intricate, as protons may be directly reduced to H-2. Here, we propose a "dual-functional oleic acid (OA) coordination" strategy that simultaneously stabilizes Cu+/Cu-0 interface via covalent O-Cu chelating bonds and tailors hydrophobic gas-liquid-solid interfaces. The OA ligands form a bidentate configuration, anchoring Cu+ sites while exposing hydrophobic alkyl chains to enrich local CO2 concentration. As a result, the OA-Cu2O nanocube exhibits an impressive C2+ Faradaic efficiency (FE) of 74.7% at -0.92 V vs. RHE under a current density of 400 mA cm(-2), along with stable operation for 40 h at 189.8 mA cm(-2) in a membrane electrode assembly (MEA). Notably, the competing hydrogen evolution reaction (HER) is effectively suppressed to a low FE of 8.1%. Operando Raman and attenuated total reflection surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) reveals the improved the *CO coverage, blocking the sites for competing *H adsorption. The theoretical study further demonstrates that OA-induced electron-deficient regions strengthen *CO adsorption while repelling H2O, synergistically promoting C-C coupling and inhibiting proton access.