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首页> 外文期刊>Advanced energy materials >Unsaturated Sulfur Edge Engineering of Strongly Coupled MoS_2 Nanosheet-CCarbon Macroporous Hybrid Catalyst for Enhanced Hydrogen Generation
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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-碳大孔杂化催化剂的不饱和硫边缘工程，用于增强氢的产生

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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的低氢吸附自由能和强酸/碱耐受性使其成为用于氢析出反应（HER）的优异的pH通用电催化剂。然而，其有限的活性边缘位点密度主要抑制了催化活性。本文中，报道了一种新策略，该策略用于制备一类具有工程化的不饱和硫边的强耦合MoS2纳米片-碳大孔杂化催化剂，以通过控制前体分解和随后的磺化/脱氧来增强HER催化作用。表面化学状态分析和第一性原理计算均证明，所得催化剂表现出理想的价电子态，具有高度暴露的不饱和硫边缘和优化的氢吸附自由能，从而显着提高了固有的HER催化活性。此类电催化剂对HER表现出优异且稳定的催化活性，在0.5 mA H2SO4中的136 mV和在1 M KOH中的10 m C（155）的小过电势是10 mA cm（-2），这是迄今为止MoS2-C杂化电催化剂的最佳报告。这项工作为改善二维材料产生氢的固有催化活性开辟了一条新途径。

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

    Xu Qiucheng; Liu Yu; Jiang Hao; Hu Yanjie; Liu Honglai; Li Chunzhong;

  • 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
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  • 关键词

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

    机译：电催化剂;析氢反应;MoS2;纳米晶体;不饱和硫边;

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