文献类型：期刊文献

英文题名：Curvature Effect of Pyridinic N-Modified Carbon Atom Sites for Electrocatalyzing CO2 Conversion to CO

作者：Zhao, Yuying[1,2] Yuan, Qixin[2] Sun, Kang[1] Wang, Ao[1] Xu, Ruting[1] Xu, Jing[2] Wang, Yan[2] Fan, Mengmeng[1,2] Jiang, Jianchun[1,2]

第一作者：Zhao, Yuying

机构：[1] Key Lab of Biomass Energy and Material, Jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources, Institute of Chemical Industry of Forest Products, Chinese Academy of Forestry, Jiangsu, Nanjing, 210042, China; [2] Jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources, International Innovation Center for Forest Chemicals and Materials, College of Chemical Engineering, Nanjing Forestry University, Nanjing, 210037, China

年份：2023

卷号：15

期号：31

起止页码：37593-37601

外文期刊名：ACS Applied Materials and Interfaces

收录：EI(收录号：20233314568950);Scopus(收录号：2-s2.0-85167480832)

语种：英文

外文关键词：Carbon dioxide - Density functional theory - Doping (additives) - Electric fields - Electrocatalysts - Electronic structure - Substrates

摘要：Carbon material is considered a promising electrocatalyst for the CO2 reduction reaction (CO2RR); especially, N-doped carbon material shows high CO Faradic efficiency (FECO) when using pyridinic N species as the active site. However, in the past decade, more efforts were focused on the preparation of various carbon nanostructures containing abundant pyridinic N species and few researchers studied the electronic structure modulation of the pyridinic N site. The curvature of the carbon substrate is an easily controllable parameter for modulating the local electronic environment of catalytic sites. In this research, carbon nanotubes (CNTs) with different diameters are applied to modulate the electronic environment of pyridinic N by the curvature effect. The pyridinic N sites doped on CNTs with the average curvature of 0.04 show almost 100% FECO at the current density of 3 mA cm-2 at ?0.6 V vs RHE and 91% FECO retention after 12 h test, which is superior to most of the carbon-based electrocatalysts. As demonstrated by density functional theory simulation, the pyridinic N site forms a strong local electric field around the nearby C active site and protrudes out of the curved CNT surface like a tip, which remarkably enriches the protons around the adsorbed CO2 molecule. ? 2023 American Chemical Society.