文献类型：期刊文献

英文题名：Effect of Charge on Carbon Support on the Catalytic Activity of Cu2O toward CO2 Reduction to C2 Products

作者：Wang, Yating[1];Cheng, Ling[2];Ge, Wangxin[1];Zhu, Yihua[1];Zhang, Jie[3];Chen, Rongzhen[1];Zhang, Ling[1];Li, Yuhang[1];Li, Chunzhong[1,2]

机构：[1]East China Univ Sci & Technol, Shanghai Engn Res Ctr Hierarch Nanomat, Sch Mat Sci & Engn, Key Lab Ultrafine Mat,Minist Educ, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Sch Chem Engn, Shanghai 200237, Peoples R China;[3]Univ Shanghai Sci & Technol, Sch Energy & Power Engn, Shanghai 200093, Peoples R China

年份：2023

卷号：15

期号：19

起止页码：23306

外文期刊名：ACS APPLIED MATERIALS & INTERFACES

收录：;EI(收录号：20232114116906);WOS:【SCI-EXPANDED(收录号:WOS:000985530300001)】；

基金：This work was supported by the National Natural Science Foundation of China (Grant Nos. 22178104, U22B20143, 21838003, 22008069), Shanghai Municipal Science and Technology Major Project, the Shanghai Scientific and Technological Innovation Project (Grant No. 22dz1205900), "the Fundamental Research Funds for the Central Universities," Shanghai Rising-Star Program (Grant No. 23QA1402200), and the Shanghai Sailing Program (Grant No. 20YF1410200).

语种：英文

外文关键词：CO2 electroreduction; charge-promotion effects; electrokinetics; in situ characterization; supported Cu

摘要：Electrochemical carbon dioxide (CO2) reduction for C2 products has been studied on a series of supported Cu-based catalysts; however, the charge-promotion effects from the substrates for the selectivity of CO2 reduction are still unclear. Here we localize nanosized Cu2O on three carbon-based substrates that provide different charge-promotion effects: positively charged boron-doped graphene (BG), negatively charged nitrogen-doped graphene (NG), and weak negatively charged reduced graphene oxide (rGO). We demonstrate that the charge-promotion effects lead to an increase in faradaic efficiency (FE) for C2 products with an order of rGO/Cu < BG/Cu < pure Cu < NG/Cu and an FEC2/FEC1 ratio from 0.2 to 7.1. By performing in situ characterization, electrokinetic investigations, and density functional theory (DFT) calculations, we reveal that the negatively charged NG is favorable for stabilizing Cu+ species under CO2 reduction, which strengthens CO* adsorption to further boost C-C coupling for C2 products. As a result, we achieve a high C2+ FE of similar to 68% at high current densities of 100-250 mA cm-2.