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Revisiting the Role of Active Sites for Hydrogen Evolution Reaction through Precise Defect Adjusting

机译：通过精确的缺陷调整重新探究活性氢在放氢反应中的作用

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摘要

2D transition metal dichalcogenides (TMDs) have presented outstanding potential for efficient hydrogen evolution reaction (HER) to replace traditional noble metal catalysts. Here, to achieve enhanced HER performance, specific areas of the few-layer 1T'-MoTe2 film are precisely controlled with a focused ion beam to create particular active sites. Electrochemical measurements indicate that the HER performance, although inconspicuous in pristine 1T'-MoTe2 ultrathin films prepared through the chemical vapor deposition method, can be greatly enhanced after patterning and precisely controlled by the morphologies as well as the amounts of the defects, reaching a small onset potential and a record-low Tafel slope of 44 mV per decade for few-layer TMDs. Conductivity tests, visualized copper electrodeposition, and density functional theory calculations also confirm that the enhancement of HER performance comes from the exposed edges by patterning. In this pioneering work, not only is the catalysis mechanism of the edge active sites of 1T'-MoTe2 unveiled, but also a universal route to study the properties of 2D materials is demonstrated.
机译：2D过渡金属二卤化金属（TMD）具有有效的氢释放反应（HER）替代传统贵金属催化剂的巨大潜力。在这里，为了获得增强的HER性能，用聚焦离子束精确控制了几层1T'-MoTe2膜的特定区域，以创建特定的活性位点。电化学测量表明，尽管在通过化学气相沉积法制备的原始1T'-MoTe2超薄膜中没有显着的HER性能，但是在构图后可以大大提高HER性能，并通过形态和缺陷量对其进行精确控制，甚至达到很小的水平几层TMD的初始电位和创纪录的低Tafel斜率为每十年44 mV。电导率测试，可视化的铜电沉积和密度泛函理论计算还证实，HER性能的增强来自于通过构图而暴露的边缘。在这项开创性工作中，不仅揭示了1T'-MoTe2边缘活性位点的催化机理，而且还展示了研究2D材料性能的通用途径。

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  • 来源
    《Advanced Functional Materials》 |2019年第33期|1901290.1-1901290.9|共9页
  • 作者

    Zhuang Peiyuan; Sun Yangye; Dong Pei; Smith Will; Sun Zhengzong; Ge Yuancai; Pei Yu; Cao Ziyi; Ajoyan Pulickel M.; Shen Jianfeng; Ye Mingxin;

  • 作者单位

    Fudan Univ, Inst Special Mat & Technol, Shanghai 200433, Peoples R China;

    Fudan Univ, Dept Chem, Shanghai 200433, Peoples R China|Fudan Univ, Shanghai Key Lab Mol Catalysis & Innovat Mat, Shanghai 200433, Peoples R China;

    Rice Univ, Dept Mat Sci & NanoEngn, Houston, TX 77005 USA|George Mason Univ, Dept Mech Engn, Fairfax, VA 22030 USA;

    George Mason Univ, Dept Mech Engn, Fairfax, VA 22030 USA;

    Fudan Univ, Dept Chem, Shanghai 200433, Peoples R China|Fudan Univ, Shanghai Key Lab Mol Catalysis & Innovat Mat, Shanghai 200433, Peoples R China;

    Fudan Univ, Inst Special Mat & Technol, Shanghai 200433, Peoples R China;

    Fudan Univ, Inst Special Mat & Technol, Shanghai 200433, Peoples R China;

    Fudan Univ, Inst Special Mat & Technol, Shanghai 200433, Peoples R China;

    Rice Univ, Dept Mat Sci & NanoEngn, Houston, TX 77005 USA;

    Fudan Univ, Inst Special Mat & Technol, Shanghai 200433, Peoples R China;

    Fudan Univ, Inst Special Mat & Technol, Shanghai 200433, Peoples R China;

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

    1T'-MoTe2; defect engineering; focused ion beam (FIB); hydrogen evolution; transition metal dichalcogenides (TMDs);

    机译：1T'-MOTE2;缺陷工程;聚焦离子束（FIB）;氢气进化;过渡金属二硫代甲胺（TMDS）;

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