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无定型钼硫化物/还原氧化石墨烯的辐射合成及其电催化析氢性能
作者单位:1. Beijing National Laboratory for Molecular Sciences, Radiochemistry and Radiation Chemistry Key Laboratory of Fundamental Science, College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, P. R. China;2. Aviation Key Laboratory of Science and Technology on Stealth Materials, Beijing Institute of Aeronautical Materials, Beijing 100095, P. R. China
基金项目:the National Natural Science Foundation of China(11405168);the National Natural Science Foundation of China(11505011)
摘    要:钼硫化物被认为是一种高效的电催化析氢反应的催化剂,因此其合成方法受到了广泛的研究和关注。本文以四硫代钼酸铵和氧化石墨为前驱体,利用γ射线对其辐照还原,一步法制备了钼硫化物/还原氧化石墨烯(Mo S_x/RGO)复合材料。通过X射线光电子能谱、X射线衍射、透射电子显微镜、Raman光谱等表征手段确认复合材料中的Mo Sx为无定型结构,且氧化石墨烯得到了有效的还原。同时系统研究了吸收剂量、前驱体配比对复合材料作为析氢反应催化剂性能的影响。结果发现,Mo Sx/RGO复合材料具有优异的催化性能,其催化起始电压为110 m V,在电流密度为10 m A·cm~(-2)时过电势仅为160 m V,Tafel斜率为46 m V·dec~(-1),说明该催化剂催化析氢机理为Volmer-Heyrovesy机理。此外,Mo Sx/RGO复合材料还具有良好的催化稳定性。

关 键 词:钼硫化物  还原氧化石墨烯  辐射还原  电催化析氢  Volmer-Heyrovesy机理  
收稿时间:2017-05-03

Radiation Induced Synthesis of Amorphous Molybdenum Sulfide/Reduced Graphene Oxide Nanocomposites for Efficient Hydrogen Evolution Reaction
Authors:Pengfei CAO  Yang HU  Youwei ZHANG  Jing PENG  Maolin ZHAI
Institution:1. Beijing National Laboratory for Molecular Sciences, Radiochemistry and Radiation Chemistry Key Laboratory of Fundamental Science, College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, P. R. China;2. Aviation Key Laboratory of Science and Technology on Stealth Materials, Beijing Institute of Aeronautical Materials, Beijing 100095, P. R. China
Abstract:Molybdenum sulfide is an efficient catalyst for the hydrogen evolution reaction (HER) and its synthesis has attracted significant attention in recent years. In this work, molybdenum sulfide/reduced graphite oxide (MoSx/RGO) was prepared by the γ-ray induced reduction of ammonium tetrathiomolybdate and graphite oxide. The composition, morphology, and structure of the MoSx/RGO composites were determined by X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), transmission electron microscopy (TEM), and Raman spectroscopy. The results confirmed the formation of amorphous MoSx/RGO composites. Subsequently, the effects of the absorbed dose and precursor ratio on the performance of the composite material as the catalyst for HER were studied systematically. The resultant MoSx/RGO composites were found to show excellent catalytic activity towards HER. With a catalyst loading of 0.275 mg·cm-2, an onset overpotential of 110 mV, a Tafel slope of 46 mV·dec-1, and a current density of 10 mA·cm-2 at the overpotential of 160 mV can be achieved. These results can be considered as the proof of Volmer-Heyrovesy mechanism. In addition, the MoSx/RGO catalyst also showed an excellent long-time stability during the evaluation for HER.
Keywords:Molybdenum sulfide  Reduced graphene oxide  Radiation synthesis  Hydrogen evolution reaction  Volmer-Heyrovesy mechanism  
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