文献类型：期刊文献

英文题名：Pyridine-grafted nitrogen-doped carbon nanotubes achieving efficient electroreduction of CO2 to CO within a wide electrochemical window

作者：Zhang, Yuning[1];Jiang, Hao[2];Niu, Dongfang[1];Manke, Ingo[3];Yang, Chao[3];Zhu, Minghui[1];Zhang, Xinsheng[1];Chen, Renjie[4]

机构：[1]East China Univ Sci & Technol, Sch Chem Engn, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Petr Proc Res Ctr, Sch Chem Engn, Shanghai 200237, Peoples R China;[3]Helmholtz Ctr Berlin Mat & Energy, Hahn Meitner Pl 1, D-14109 Berlin, Germany;[4]Beijing Inst Technol, Sch Mat Sci & Engn, Beijing Key Lab Environm Sci & Engn, Beijing 100081, Peoples R China

年份：2022

卷号：10

期号：4

起止页码：1852

外文期刊名：JOURNAL OF MATERIALS CHEMISTRY A

收录：;EI(收录号：20220511565229);WOS:【SCI-EXPANDED(收录号:WOS:000741067800001)】；

基金：This work was financially supported by the National Natural Science Foundation of China (No. 21972042), the Helmholtz Association and was partially funded by the German Research Foundation (DFG, Project No. MA 5039/4-1). We also thank the Research Center of Analysis and Test of East China University of Science and Technology for the help on the characterization.

语种：英文

外文关键词：Doping (additives) - Electrocatalysts - Molecules - Electrolytic reduction - Grafting (chemical) - Reaction kinetics - Carbon nanotubes - Density functional theory - Nitrogen - Hydrogen - Reaction intermediates - Pyridine - Yarn

摘要：Nitrogen-doped carbon nanomaterials for electrochemical reduction of CO2 (CO2ER) to CO have been extensively investigated, evaluated, and applied recently. Nevertheless, their weak adsorption capacity for CO2 usually results in a rapidly decayed CO faradaic efficiency (FECO) in the course of pursuing a commercial CO current density (j(CO)) by increasing the overpotential. Herein, we axially graft pyridine molecules on nitrogen-doped carbon nanotubes to construct a metal-free composite electrocatalyst (Py-N4CNTs-800) with enhanced CO2 affinity for CO2ER to efficiently generate CO. Py-N4CNTs-800 exhibits a prominent FECO of 96% at -0.99 V (vs. reversible hydrogen electrode, RHE) with a desirable j(CO) of 18.4 mA cm(-2), and FECO can even be maintained above 90% in a wide electrochemical potential window (-0.79 to -1.19 V). In situ infrared spectra unambiguously indicate that grafted axial pyridine molecules can facilitate the CO2 adsorption and suppress the occurrence of competitive hydrogen evolution reaction (HER). Density functional theory (DFT) calculations enlighten that the introduction of pyridine molecules could dramatically stabilize the key intermediate *COOH, which effectively accelerates the reaction kinetics rate. Notably, Py-N4CNTs-800 delivers a promising j(CO) of 217 mA cm(-2) at -0.9 V in a flow cell, showing a bright prospect of function strengthened carbon nanomaterial for industrial applications.