文献类型：期刊文献

英文题名：Frenkel-defected monolayer MoS2 catalysts for efficient hydrogen evolution

作者：Xu, Jie[1];Shao, Gonglei[2,3];Tang, Xuan[4];Lv, Fang[1];Xiang, Haiyan[2];Jing, Changfei[5];Liu, Song[2];Dai, Sheng[4];Li, Yanguang[1];Luo, Jun[5];Zhou, Zhen[3]

机构：[1]Soochow Univ, Inst Funct Nano & Soft Mat FUNSOM, Jiangsu Key Lab Carbon Based Funct Mat & Devices, Suzhou 215123, Peoples R China;[2]Hunan Univ, Coll Chem & Chem Engn, State Key Lab Chemo Biosensing & Chemometr, Changsha 410082, Hunan, Peoples R China;[3]Zhengzhou Univ, Engn Res Ctr Adv Funct Mat Mfg, Sch Chem Engn, Minist Educ, Zhengzhou 450001, Peoples R China;[4]East China Univ Sci & Technol, Feringa Nobel Prize Scientist Joint Res Ctr, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China;[5]Tianjin Univ Technol, Sch Mat Sci & Engn, Tianjin Key Lab Photoelect Mat & Devices, Tianjin 300384, Peoples R China

年份：2022

卷号：13

期号：1

外文期刊名：NATURE COMMUNICATIONS

收录：;WOS:【SCI-EXPANDED(收录号:WOS:000785774400017)】；

基金：We acknowledge the financial support from National Natural Science Foundation of China (51971157, 21975067, and 22175060), Natural Science Foundation of Jiangsu Province of China (BK20210729), Tianjin Science Fund for Distinguished Young Scholars (19JCJQJC61800), Shanghai Rising-star Program (20QA1402400), the Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning, and Fundamental Research Funds for the Central Universities from East China University of Science and Technology and Hunan University. J.X. and Y.L. acknowledge Suzhou Key Laboratory of Functional Nano & Soft Materials, Collaborative Innovation Center of Suzhou Nano Science & Technology, the 111 Project and Joint International Research Laboratory of Carbon-Based Functional Materials and Devices. J.X. also acknowledges the support from Excellent Youth Scholars Program of Soochow University. DFT calculaton has been carried out in Hefei Advanced Computing Center. Additional support was provided by the Frontiers Science Center for Materiobiology and Dynamic Chemistry and the Feringa Nobel Prize Scientist Joint Research Center at East China University of Science and Technology. We also thank Prof. Jeng-Han Wang and Dr. Yi-Tong Zhou for the helpful discussion and technique support.

语种：英文

摘要：While material defect sites are active for chemical reactions, it is important to understand how different defect types impact reactivity. Here, authors prepare Frenkel-defected MoS2 monolayers and demonstrate improved performances for H-2 evolution electrocatalysis than pristine or doped MoS2. Defect engineering is an effective strategy to improve the activity of two-dimensional molybdenum disulfide base planes toward electrocatalytic hydrogen evolution reaction. Here, we report a Frenkel-defected monolayer MoS2 catalyst, in which a fraction of Mo atoms in MoS2 spontaneously leave their places in the lattice, creating vacancies and becoming interstitials by lodging in nearby locations. Unique charge distributions are introduced in the MoS2 surface planes, and those interstitial Mo atoms are more conducive to H adsorption, thus greatly promoting the HER activity of monolayer MoS2 base planes. At the current density of 10 mA cm(-2), the optimal Frenkel-defected monolayer MoS2 exhibits a lower overpotential (164 mV) than either pristine monolayer MoS2 surface plane (358 mV) or Pt-single-atom doped MoS2 (211 mV). This work provides insights into the structure-property relationship of point-defected MoS2 and highlights the advantages of Frenkel defects in tuning the catalytic performance of MoS2 materials.