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Conversion of Intercalated MoO3 to Multi-Heteroatoms-Doped MoS2 with High Hydrogen Evolution Activity
Authors:Weiwei Yang  Shuqing Zhang  Qian Chen  Chao Zhang  Yi Wei  Huaning Jiang  Yunxiang Lin  Mengting Zhao  Qianqian He  Xingguo Wang  Yi Du  Li Song  Shubin Yang  Anmin Nie  Xiaolong Zou  Yongji Gong
Affiliation:1. School of Materials Science and Engineering, Beihang University, Beijing, 100191 China;2. Shenzhen Geim Graphene Center and Low-Dimensional Materials and Devices Laboratory, Tsinghua-Berkeley Shenzhen Institute, Tsinghua University, Shenzhen, 518055 China;3. State Key Laboratory of Organic–Inorganic Composites, Beijing Key Laboratory of Electro-chemical Process and Technology for Materials, Beijing University of Chemical Technology, Beijing, 100029 China;4. National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, 230029 China;5. School of Physics and BUAA-UOW Joint Research Centre, Beihang University, Beijing, 100191 China

Institute for Superconducting and Electronic Materials, Australian Institute for Innovative Materials, University of Wollongong, Wollongong, 2500 Australia;6. Center for High Pressure Science, State Key Laboratory of Metastable Materials Science and Technology, Yanshan University, Qinhuangdao, 066004 China

Abstract:Lack of effective strategies to regulate the internal activity of MoS2 limits its practical application for hydrogen evolution reactions (HERs). Doping of heteroatoms without forming aggregation or an edge enrichment is still challenging, and its effect on the HER needs to be further explored. Herein, a two-step method is developed to obtain multi-metal-doped H-MoS2, which includes intercalation of the layered MoO3 precursor with a following sulfurization. Benefiting from the capability of the intercalation method to uniformly and simultaneously introduce different elements into the van der Waals gap, this method is universal to obtain multi-heteroatoms co-doped MoS2 without forming clusters, phase separation, and an edge enrichment. It is demonstrated that the doping of adjacent cobalt and palladium monomers on MoS2 greatly enhances the HER catalytic activity. The overpotential at 10 mA cm−2 and Tafel slope of Co and Pd co-doped MoS2 is found to be 49.3 mV and 43.2 mV dec−1, respectively, representing a superior acidic HER catalytic activity. This intercalation-assisted method also provides a new and general strategy to synthesize uniformly doped transition metal dichalcogenides for various applications.
Keywords:doping  hydrogen evolution reaction  MoS2  synergistic effects
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