层间距宽化二硫化钼的一步合成及其电催化析氢性能  

One-step synthesis and enhanced electrocatalytic hydrogen evolution performance of interlayer-expanded molybdenum disulfide

作　　者：郑学军[1,2] 陈隆源 王经纬 朱红伟 何文远[1,2,3] ZHENG Xuejun;CHEN Longyuan;WANG jingwei;ZHU hongwei;HE Wenyuan(School of Mechanical Engineering and Mechanics,Xiangtan University,Xiangtan 411105,Hunan,China;Key Laboratory of Welding Robot and Application Technology of Hunan Province,Xiangtan University,Xiangtan 411105,Hunan,China;Research Institute of Green Intelligent Manufacturing,Xiangtan University in Foshan,Foshan 528399,Guangdong,China)

机构地区：[1]湘潭大学机械工程与力学学院,湖南湘潭411105 [2]湘潭大学湖南省焊接机器人及应用技术重点实验室,湖南湘潭411105 [3]佛山湘潭大学绿色智造研究院,广东佛山528399

出　　处：《材料工程》2023年第10期84-92,共9页Journal of Materials Engineering

基　　金：国家自然科学基金项目(11832016);国家重点研发计划项目(2021YFB4000802);湖南创新型省份建设专项项目(2020GK2014);广东省基础与应用基础研究基金项目(2022A1515110091)。

摘　　要：提出一种通过增加反应物中硫脲比例来合成层间距宽化的二硫化钼(E-MoS_(2))的一步合成方法。该方法中,过量硫脲高温下转化为硫氰酸铵原位嵌入MoS_(2)层间使层间距宽化,避免传统E-MoS_(2)的复杂合成过程和外来插层分子的引入。该方法合成的E-MoS_(2)微米花展现出良好的析氢性能:在电流密度为-10 mA/cm~2时的析氢过电位为285 mV,塔菲尔斜率为68.5 mV/dec,远低原始MoS_(2)的析氢过电位(588 mV)和塔菲尔斜率(122.2 mV/dec)。该E-MoS_(2)析氢性能的提升可归因于:层间距的宽化优化MoS_(2)的电子结构,从而提高导电性,降低氢吸附自由能;且合成过程中硫氰酸铵分子的原位嵌入抑制MoS_(2)的生长,减小其微米花尺寸,使其暴露出更多的活性位点。因此,该E-MoS_(2)微米花有望成为一种有前景的非贵金属析氢电催化剂。A simple one-step hydrothermal method to synthesize interlayer-expanded molybdenum disulfide microflowers(E-MoS_(2)) by increasing the proportion of thiourea in the reactant was proposed.In the method,ammonium thiocyanate,the product of thiourea conversion in hydrothermal reaction,is embedded into the interlayer of MoS_(2) formed in situ to expand the layer spacing,which avoids the complex synthesis process of traditional E-MoS_(2) and the introduction of foreign species and templates.The E-MoS_(2) reveals a small Tafel slope of 68.5 mV/dec and a low overpotential of_(2)85 mV at-10 mA/cm~2,markedly lower than those of initial MoS_(2) counterpart(122.2 mV/dec and 588 mV,respectively),indicating its excellent hydrogen evolution performance.Compared with the original MoS_(2),the enhanced hydrogen evolution performance of E-MoS_(2) can be attributed to the following reasons:the expansion of interlayer spacing optimizes the electronic structure of MoS_(2),thereby improving its conductivity and reducing the hydrogen adsorption free energy;the in situ intercalation of ammonium thiocyanate inhibits the growth and reduces the size of microflowers during the synthesis process,thus exposing more active sites for E-MoS_(2).Therefore,the E-MoS_(2) is expected to be a promising non-noble metal electrocatalyst for hydrogen evolution reaction.

关 键 词：层间距宽化 MoS_(2) 硫氰酸铵 电催化析氢 

分 类 号：O643[理学—物理化学]