物理化学学报 >> 2017, Vol. 33 >> Issue (12): 2542-2549.doi: 10.3866/PKU.WHXB201706151

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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

曹朋飞1,胡杨1,张有为2,彭静1,翟茂林1,*()   

  1. 1 北京大学化学与分子工程学院,放射化学与辐射化学重点学科实验室,北京分子科学国家实验室,北京100871
    2 北京航空材料研究院,隐身材料科技重点实验室,北京100095
  • 收稿日期:2017-05-03 发布日期:2017-09-05
  • 通讯作者: 翟茂林 E-mail:mlzhai@pku.edu.cn
  • 基金资助:
    国家自然科学基金(11405168);国家自然科学基金(11505011)

Radiation Induced Synthesis of Amorphous Molybdenum Sulfide/Reduced Graphene Oxide Nanocomposites for Efficient Hydrogen Evolution Reaction

Pengfei CAO1,Yang HU1,Youwei ZHANG2,Jing PENG1,Maolin ZHAI1,*()   

  1. 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
  • Received:2017-05-03 Published:2017-09-05
  • Contact: Maolin ZHAI E-mail:mlzhai@pku.edu.cn
  • Supported by:
    the National Natural Science Foundation of China(11405168);the National Natural Science Foundation of China(11505011)

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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（MoSx/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MoSx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，MoSx/RGO复合材料具有优异的催化性能，其催化起始电压为110 mV，在电流密度为10 mA·cm-2时过电势仅为160 mV，Tafel斜率为46 mV·dec-1，说明该催化剂催化析氢机理为Volmer-Heyrovesy机理。此外，MoSx/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

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.

Key words: Molybdenum sulfide, Reduced graphene oxide, Radiation synthesis, Hydrogen evolution reaction, Volmer-Heyrovesy mechanism