文献类型：期刊文献

英文题名：Locally-doped MoS2 monolayer with in-plane bifunctional heterostructure toward overall water splitting

作者：Duan, Zhuo-Jun[1];Xia, Hang[1];Li, Han-Ze[2];Shao, Gong-Lei[3];Ren, Yi-Zhang[1];Tang, Xuan[4];Liu, Qiu-Nan[5];Hong, Jin-Hua[6];Dai, Sheng[4];Lin, Yung-Chang[7];Suenaga, Kazu[5];He, Yong-Min[1];Liu, Song[1]

机构：[1]Hunan Univ, Coll Chem & Chem Engn, Changsha 410082, Peoples R China;[2]Xiangtan Univ, Sch Phys & Optoelect, Xiangtan 411105, Peoples R China;[3]Zhengzhou Univ, Interdisciplinary Res Ctr Sustainable Energy Sci &, Sch Chem Engn, Zhengzhou 450001, Peoples R China;[4]East China Univ Sci & Technol, Feringa Nobel Prize Scientist Joint Res Ctr, Sch Chem & Mol Engn, Key Lab Adv Mat Joint Int Res Lab Precis Chem & Mo, Shanghai 200237, Peoples R China;[5]Osaka Univ, Inst Sci & Ind Res ISIR Sanken, Osaka 5670047, Japan;[6]Hunan Univ, Coll Mat Sci & Engn, Changsha 410082, Peoples R China;[7]Natl Inst Adv Ind Sci & Technol, Nanomat Res Inst, Tsukuba 3058565, Japan

年份：2025

卷号：44

期号：5

起止页码：3130

外文期刊名：RARE METALS

收录：;EI(收录号：20250817915076);WOS:【SCI-EXPANDED(收录号:WOS:001424992500001)】；

基金：This study was financially supported by the National Natural Science Foundation of China (Nos. 22175060 and 22376062), JSPS Grant-in-Aid for Scientific Research (Nos. JP21H05235, JP22H05478 and JP22F22358) and China Postdoctoral Science Foundation (No. 2022M722867), and the Key Research Project of Higher Education Institutions in Henan Province (No. 23A530001).

语种：英文

外文关键词：Locally-doped monolayer; In-plane heterostructure; MoS2; Bifunctional catalysts; Overall water splitting

摘要：Exploring earth-abundant, highly active bifunctional electrocatalysts for efficient hydrogen and oxygen evolution is crucial for water splitting. However, due to their distinct free energies and conducting behaviors (electron/hole), balancing the catalytic efficiency between hydrogen and oxygen evolution remains challenging for achieving bifunctional electrocatalysts. Here, we report a locally-doped MoS2 monolayer with an in-plane heterostructure acting as a bifunctional electrocatalyst and apply it to the overall water splitting. In this heterostructure, the core region contains Mo/S vacancies, while the ring region was doped by Fe atoms (in two substitution configurations: 1FeMo and 3FeMo-VS clusters) with a p-type conductive characteristic. Our micro-cell measurements, combined with density functional theory (DFT) calculations, reveal that the vacancies-rich core region presents remarkable hydrogen evolution reaction (HER) activity while the Fe-doped ring gives an excellent oxygen evolution reaction (OER) activity, thus forming an in-plane bifunctional electrocatalyst. Finally, as a proof-of-concept for overall water splitting, we constructed a full-cell configuration based on a locally-doped MoS2 monolayer, which achieved a cell voltage of 1.87 V at 10 mAcm(-2), demonstrating outstanding performance in strong acid electrolytes. Our work provides insight into the hetero-integration of bifunctional electrocatalysts at the atomic level, paving the way for designing transition metal dichalcogenide catalysts with activity-manipulated regions capable of multiple reactions.