Working-in-tandem mechanism of multi-dopants in enhancing electrocatalytic nitrogen reduction reaction performance of carbon- based materials

作     者：Wenqing Zhang Keke Mao Jingxiang Low Hengjie Liu Yanan Bo Jun Ma Qiaoxi Liu Yawen Jiang Jiuzhong Yang Yang Pan Zeming Qi Ran Long Li Song Yujie Xiong Wenqing Zhang;Keke Mao;Jingxiang Low;Hengjie Liu;Yanan Bo;Jun Ma;Qiaoxi Liu;Yawen Jiang;Jiuzhong Yang;Yang Pan;Zeming Qi;Ran Long;Li Song;Yujie Xiong

作者机构：Hefei National Laboratory for Physical Sciences at the MicroscaleCollaborative Innovation Center of Chemistry for Energy Materials(iChEM)School of Chemistry and Materials Scienceand National Synchrotron Radiation LaboratoryUniversity of Science and Technology of ChinaHefei 230041China School of Energy and Environment ScienceAnhui University of TechnologyMaanshan 243032China Institute of EnergyHefei Comprehensive National Science CenterHefei 230031China 

出 版 物：《Nano Research》 (纳米研究（英文版）)

年 卷 期：2021年第14卷第9期

页      面：3234-3239页

核心收录：

学科分类：081704[工学-应用化学] 07[理学] 070304[理学-物理化学(含∶化学物理)] 08[工学] 0817[工学-化学工程与技术] 0703[理学-化学] 

基　　金：financially supported in part by the National Key R&D Program of China(No.2017YFA0207301) the National Natural Science Foundation of China(Nos.21725102,U1832156,91961106,22075267,and 21950410514) CAS Key Research Program of Frontier Sciences(No.QYZDB-SSW-SLH018) CAS Interdisciplinary Innovation Team,Science and Technological Fund of Anhui Province for Outstanding Youth(No.2008085J05) Youth Innovation Promotion Association of CAS(No.2019444) Chinese Academy of Sciences Presidents International Fellowship Initiative(Nos.2019PC0114 and 2020T130627) China Postdoctoral Science Foundation(No.2019M652190) Young Elite Scientist Sponsorship Program by CAST,and DNL Cooperation Fund,CAS(No.DNL201922) 

主　　题：N2 reduction reaction metal-free catalyst heteroatoms doping asymmetric charge distribution electrocatalysis 

摘      要：Developing carbon-based electrocatalysts with excellent N2 adsorption and activation capability holds the key to achieve highly efficient nitrogen reduction reaction(NRR)for reaching its practical ***,we report a highly active electrocatalyst--metal-free pyrrolic-N dominated N,S co-doped carbon(pyrr-NSC)for *** on theoretical and experimental results,it is confirmed that the N and S-dopants practice a working-in-tandem mechanism on pyrr-NSC,where the N-dopants are utilized to create electropositive C sites for enhancing N2 adsorption and the S-dopants are employed to induce electron backdonation for facilitating N2 *** synergistic effect of the pyrrolic-N and S-dopants can also suppress the irritating hydrogen evolution reaction,further boosting the NRR *** work gives an indication that the combination of two different dopants on electrocatalyst can enhance NRR performance by working in the two tandem steps-the adsorption and activation of N2 molecules,providing a new strategy for NRR electrocatalyst design.