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Unsaturated Sulfur Edge Engineering of Strongly Coupled MoS_2 Nanosheet-CCarbon Macroporous Hybrid Catalyst for Enhanced Hydrogen Generation

机译:强耦合MOS_2纳米片 - CCAROBON型杂交杂交催化剂的不饱和硫边缘工程,用于增强氢气

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摘要

The low hydrogen adsorption free energy and strong acid/alkaline resistance of layered MoS2 render it an excellent pH-universal electrocatalyst for hydrogen evolution reaction (HER). However, the catalytic activity is dominantly suppressed by its limited active-edge-site density. Herein, a new strategy is reported for making a class of strongly coupled MoS2 nanosheet-carbon macroporous hybrid catalysts with engineered unsaturated sulfur edges for boosting HER catalysis by controlling the precursor decomposition and subsequent sodiation/desodiation. Both surface chemical state analysis and first-principles calculations verify that the resultant catalysts exhibit a desirable valence-electron state with high exposure of unsaturated sulfur edges and an optimized hydrogen adsorption free energy, significantly improving the intrinsic HER catalytic activity. Such an electrocatalyst exhibits superior and stable catalytic activity toward HER with small overpotentials of 136 mV in 0.5 M H2SO4 and 155 mV in 1 M KOH at 10 mA cm(-2), which is the best report for MoS2-C hybrid electrocatalysts to date. This work paves a new avenue to improve the intrinsic catalytic activity of 2D materials for hydrogen generation.
机译:层状MOS2的低氢吸附可自由能和强酸/碱性电阻使其成为氢进化反应(她)的优异的pH通用电催化剂。然而,通过其有限的主动边缘部位密度占据催化活性。这里,据报道,通过控制前体分解和随后的加密/退化来制备具有工程不饱和硫边缘的一类强耦合的MOS2纳米片 - 碳大孔杂交催化剂,以使其催化剂升高。表面化学质子分析和第一原理计算验证所得催化剂具有高耐硫边缘暴露的理想价 - 电子状态和优化的氢吸附能量,显着改善了催化活性的内在催化活性。这种电催化剂在0.5M H 2 SO 4和155mV下在10 mA cm(-2)中,在0.5M H 2 SO 4和155mV中表现出优异的过电并在0.5MKOH中的催化活性,这是迄今为止MOS2-C杂交电催化剂的最佳报告。这项工作铺设了一种新的途径,以改善2D材料的固有催化活性。

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  • 来源
    《Advanced energy materials》 |2019年第2期|1802553.1-1802553.8|共8页
  • 作者单位

    East China Univ Sci & Technol Sch Mat Sci & Engn Minist Educ Key Lab Ultrafine Mat Shanghai 200237 Peoples R China;

    East China Univ Sci & Technol Sch Chem Engn State Key Lab Chem Engn Shanghai 200237 Peoples R China;

    East China Univ Sci & Technol Sch Mat Sci & Engn Minist Educ Key Lab Ultrafine Mat Shanghai 200237 Peoples R China;

    East China Univ Sci & Technol Sch Mat Sci & Engn Minist Educ Key Lab Ultrafine Mat Shanghai 200237 Peoples R China;

    East China Univ Sci & Technol Sch Chem Engn State Key Lab Chem Engn Shanghai 200237 Peoples R China;

    East China Univ Sci & Technol Sch Mat Sci & Engn Minist Educ Key Lab Ultrafine Mat Shanghai 200237 Peoples R China;

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

    electrocatalysts; hydrogen evolution reaction; MoS2; nanocrystals; unsaturated sulfur edge;

    机译:电催化剂;氢气进化反应;MOS2;纳米晶体;不饱和硫缘;

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