文献类型：期刊文献

英文题名：Dual-confinement of reconstructed covalent organic framework for enhanced CO2 electrolysis in acid

作者：Li, Xinyan[1];Gu, Hongxu[2];Xu, Jipeng[3];Wang, Huan[1];Wu, Jiachen[1];Xu, Yining[1];Lian, Cheng[3];Cheng, Qilin[1];Zhang, Weiwei[2];Liu, Pengfei[1];Yang, Huagui[1];Zhu, Wei-Hong[2]

机构：[1]East China Univ Sci & Technol, Key Lab Ultrafine Mat, Shanghai Engn Res Ctr Hierarch Nanomat, Sch Mat Sci & Engn,Minist Educ, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Feringa Nobel Prize Scientist Joint Res Ctr,Fronti, Sch Chem & Mol Engn,Joint Int Res Lab Precis Chem, Key Lab Adv Mat,Inst Fine Chem,Sch Chem & Mol Engn, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Shanghai Engn Res Ctr Hierarch Nanomat, Sch Chem & Mol Engn, State Key Lab Chem Engn, Shanghai 200237, Peoples R China

年份：2026

卷号：69

期号：2

起止页码：803

外文期刊名：SCIENCE CHINA-MATERIALS

收录：;EI(收录号：20260219899547);WOS:【SCI-EXPANDED(收录号:WOS:001656604000001)】；

基金：This work was financially supported by the National Natural Science Foundation of China (22379043, 22422805, 22375062 and T2488302), the Shanghai Pilot Program for Basic Research (22TQ1400100-10 and 22TQ1400100-12), the Science and Technology Commission of Shanghai Municipality (22ZR1415700, 24DX1400200 and 24160711900), the Young Elite Scientists Sponsorship Program by China Association for Science and Technology (CAST) (2023QNRC001), the Fundamental Research Funds for the Central Universities and the Scientific Research Innovation Capability Support Project for Young Faculty (ZYGXONJSKYCXNLZCXM-M10). The authors also thank the Frontiers Science Center for Materiobiology and Dynamic Chemistry, the crew of the 1W1B beamline at the Beijing Synchrotron Radiation Facility (BSRF) for their constructive assistance with the X-ray absorption fine structure measurements and data analyses, and the Research Center of Analysis and Test of East China University of Science and Technology (ECUST) for assistance with materials characterizations.

语种：英文

外文关键词：acidic CO2 electrocatalysis; covalent organic framework; multicarbon products; microenvironment

摘要：Electrochemical CO2 reduction reaction (CO2RR) offers an attractive approach to produce chemicals and fuels, especially for the value-added multicarbon (C2+) products. However, due to the strong competition reactions of hydrogen evolution and mono-carbon production, precise modulation of reaction pathways at the molecular level is challenging. Here, we propose a dual-confinement effect of CO2 reactant and *CO intermediate in CO2RR, induced by tuning the pore configuration of reconstructed covalent organic framework (RC-COF), which effectively improves C2+ selectivity. Attributed to the dual-confinement effect, we achieved a maximum C2+ selectivity of 67.0% at 500 mA cm(-2) over the COF modified Cu electrode, which maintains a high carbon products Faradaic efficiency over 90% across a board current density range (100-500 mA cm(-2)) in acidic electrolyte. Experimental and theoretical results prove that the highly crystalline RC-COF-1 with ordered micro-pores has advantages in modulating the adsorption and diffusion of reactants and intermediates. Our study provides deep insights into microenvironment modulation in CO2RR, and underscores the critical role of COF pore configuration for other heterogeneous catalysis reactions.