文献类型：期刊文献

英文题名：Steering CO2 Electroreduction to C2+ Products via Enhancing Localized CO Coverage and Local Pressure in Conical Cavity

作者：Li, Congcong[1];Zhang, Tingting[1];Liu, Heng[2];Guo, Zhongyuan[2,3];Liu, Zhongliang[1];Shi, Haojun[4];Cui, Jialin[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 200237, Peoples R China;[2]Tohoku Univ, Adv Inst Mat Res WPI AIMR, Sendai 9808577, Japan;[3]Zhejiang Univ, Coll Environm & Resource Sci, Hangzhou 310058, Peoples R China;[4]East China Univ Sci & Technol, Shanghai Engn Res Ctr Hierarch Nanomat, Sch Mat Sci & Engn, Shanghai 200237, Peoples R China

年份：2024

卷号：36

期号：18

外文期刊名：ADVANCED MATERIALS

收录：;EI(收录号：20240615498041);WOS:【SCI-EXPANDED(收录号:WOS:001156456000001)】；

基金：C.L., T.Z., and H.L. contributed equally to this work. This work was supported by the National Natural Science Foundation of China (Grant Nos. 21838003, 21771170, and 22008069), Shanghai Municipal Science and Technology Major Project, the Science and Technology Commission of Shanghai Municipality (Project No. 22dz1205900), Shanghai Rising-Star Program (Program No. 20QA1402700), JSPS KAKENHI (Grant No. JP23K13703), and the Iwatani Naoji Foundation. The authors thank the Shanghai Synchrotron Radiation Facility (14W1, SSRF). H.L. acknowledges the Center for Computational Materials Science, Institute for Materials Research, Tohoku University for the use of MASAMUNE-IMR (Project No. 202212-SCKXX-0204) and the Institute for Solid State Physics (ISSP) at the University of Tokyo for the use of their supercomputers. The authors also acknowledge Beijing PARATERA Tech Co., Ltd., and the National Computational Infrastructure (NCI, Australia) for providing High Performance Computer resources.

语种：英文

外文关键词：CC coupling; *CO coverage; conical cavity structure; electrochemical CO2 reduction; local pressure; multicarbon products

摘要：The electrochemical carbon dioxide (CO2) reduction reaction (CO2RR) involves a multistep proton-coupled electron transfer (PCET) process that generates a variety of intermediates, making it challenging to transform them into target products with high activity and selectivity. Here, a catalyst featuring a nanosheet-stacked sphere structure with numerous open and deep conical cavities (OD-CCs) is reported. Under the guidance of the finite-element method (FEM) simulations and theoretical analysis, it is shown that exerting control over the confinement space results in diffusion limitation of the carbon intermediates, thereby increasing local pressure and subsequently enhancing localized *CO coverage for dimerization. The nanocavities exhibit a structure-driven shift in selectivity of multicarbon (C2+) product from 41.8% to 81.7% during the CO2RR process.