文献类型：期刊文献

英文题名：Sulfur Atomically Doped Bismuth Nanobelt Driven by Electrochemical Self-Reconstruction for Boosted Electrocatalysis

作者：Lin, Yunxiang[1];Yang, Li[1,3];Jiang, Hongliang[1,4];Zhang, Youkui[1,2];Bo, Yanan[1];Liu, Ping[1];Chen, Shuangming[1];Xiang, Bin[1];Li, Guang[3];Jiang, Jun[1];Xiong, Yujie[1];Song, Li[1]

机构：[1]Univ Sci & Technol China, Sch Chem & Mat Sci, Natl Synchrotron Radiat Lab, Hefei 230029, Anhui, Peoples R China;[2]Southwest Univ Sci & Technol, Sch Natl Def Sci & Technol, Mianyang 621010, Sichuan, Peoples R China;[3]Anhui Univ, Sch Phys & Mat Sci, Inst Phys Sci & Informat Technol, Hefei 230601, Anhui, Peoples R China;[4]East China Univ Sci & Technol, Sch Chem Engn, Shanghai 200237, Peoples R China

年份：2020

卷号：11

期号：5

起止页码：1746

外文期刊名：JOURNAL OF PHYSICAL CHEMISTRY LETTERS

收录：;EI(收录号：20201508388872);WOS:【SCI-EXPANDED(收录号:WOS:000518706000021)】；

基金：This work was financially supported in part by National Key R&D Program of China (2017YFA0303500), NSFC (U1932201, 21727801, 21978278, and 21902129), NSFC-MAECI (51861135202), CAS International Partnership Program (211134KYSB20190063), CAS Collaborative Innovation Program of Hefei Science Center (2019HSC-CIP002), CAS Key Research Program of Frontier Sciences (QYZDB-SSW-SLH018), and CAS Iterdisciplinary Innovation Team. L.S. acknowledges the support from Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Nankai University (111 project, B12015). We thank the Shanghai synchrotron Radiation Facility (14W1 and 14B1, SSRF), the Beijing Synchrotron Radiation Facility (1W1B and 4B9A, BSRF), the Hefei Synchrotron Radiation Facility (ARPES, MCD, Photoemission and Catalysis/Surface Science Endstations at NSRL), and the USTC Center for Micro and Nanoscale Research and Fabrication for help in characterizations.

语种：英文

外文关键词：Layered semiconductors - Nanobelts - Density functional theory - Electronic structure - Sulfur compounds - Ammonia - Electrocatalysis - Atoms - Bismuth compounds - Molybdenum compounds - Sulfur - Electrocatalysts

摘要：Recent years have witnessed various in-depth research efforts on self-reconstruction behavior toward electrocatalysis. Tracking the phase transformation and evolution of true active sites is of great significance for the development of self-reconstructed electrocatalysts. Here, the optimized atomic sulfur-doped bismuth nanobelt (S-Bi) is fabricated via an electrochemical self-reconstruction evolved from Bi2S3. Advanced technologies have demonstrated that the nonmetallic S atoms have been doped into the lattice Bi frame, leading to the reconstruction of local electronic structure of Bi. The as prepared S-Bi nanobelt exhibits a remarkable NH3 generation rate of 10.28 mu g h(-1) mg(-1) and Faradaic efficiency of 10.48%. Density functional theory calculations prove that the S doping can significantly lower the energy barrier of the rate-determining step and enlarge the N N bond for further dissociation toward N-2 fixation. This work not only establishes insights into the evolution process of electrochemically derived self-reconstruction but also unravels the root of the N-2 reduction reaction mechanism associated with the atomic nonmetal dopants.