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首页> 外文期刊>Advanced energy materials >Benchmarking the Activity, Stability, and Inherent Electrochemistry of Amorphous Molybdenum Sulfide for Hydrogen Production
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Benchmarking the Activity, Stability, and Inherent Electrochemistry of Amorphous Molybdenum Sulfide for Hydrogen Production

机译：基于用于氢气生产的无定形钼硫化物的活性，稳定性和固有电化学

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摘要

Anodically electrodeposited amorphous molybdenum sulfide (AE-MoSx) has attracted significant attention as a non-noble metal electrocatalyst for its high activity toward the hydrogen evolution reaction (HER). The [Mo3S13](2-) polymer-based structure confers a high density of exposed sulfur moieties, widely regarded as the HER active sites. However, their intrinsic complexity conceals full understanding of their exact role in HER catalysis, hampering their full potential for water splitting applications. In this report, a unifying approach is adopted accounting for modifications in the inherent electrochemistry (EC), HER mechanism, and surface species to maximize the AE-MoSx electroactivity over a broad pH region (0-10). Dramatic enhancements in HER performance by selective electrochemical cycling within reductive (overpotential shift, eta(HER) approximate to -350 mV) and electro-oxidative windows (eta(HER) approximate to -290 mV) are accompanied by highly stable performance in mildly acidic electrolytes. Joint analysis of X-ray photoelectron spectroscopy, Raman, and EC experiments corroborate the key role of bridging and terminal S ligands as active site generators at low pH, and reveal molybdenum oxysulfides (Mo5+OxSy) to be the most active HER moiety in AE-MoSx in mildly acidic-to-neutral environments. These findings will be extremely beneficial for future tailoring of MoSx materials and their implementation in commercial electrolyzer technologies.
机译：阳极电沉积的无定形钼硫化物（AE-MOSX）作为其高惰性金属电催化剂引起了其高活性的显着关注，朝向氢进化反应（她）。 [Mo3S13]（2-）基于聚合物的结构赋予高密度的暴露硫部分，被广泛被认为是她的活性位点。然而，它们的内在复杂性隐藏在她的催化中完全了解它们的确切角色，阻碍了它们的水分分裂应用的全部潜力。在本报告中，采用统一方法核算固有电化学（EC），其机制和表面物种中的修饰，以最大化宽pH区域（0-10）上的AE-MOSX电激性。通过选择性电化学循环在还原（过势移位，ETA（ETA（）近似至-350mV）和电氧化窗口（ETA（她）近似到-290mV）的表现剧烈增强伴随着轻度酸性的高度稳定性能电解质。 X射线光电子能谱，拉曼和EC实验的联合分析证实了桥接和末端S配体作为低pH值的关键作用，并显示钼硫化物（MO5 + OXSY）成为AE中最活跃的部分-MOSX在轻度酸性到中性环境中。这些发现对于将来的MOSX材料裁缝及其在商业电解槽技术中的实施非常有利。

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  • 来源
    《Advanced energy materials》 |2019年第8期|1802614.1-1802614.17|共17页
  • 作者

    Escalera-Lopez Daniel; Lou Zhiheng; Rees Neil V.;

  • 作者单位

    Univ Birmingham Sch Chem Engn Ctr Hydrogen & Fuel Cell Res Birmingham B15 2TT W Midlands England|Univ Birmingham Sch Phys & Astron Nanoscale Phys Res Lab Birmingham B15 2TT W Midlands England;

    Univ Birmingham Sch Chem Engn Ctr Hydrogen & Fuel Cell Res Birmingham B15 2TT W Midlands England;

    Univ Birmingham Sch Chem Engn Ctr Hydrogen & Fuel Cell Res Birmingham B15 2TT W Midlands England;

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  • 原文格式 PDF
  • 正文语种 eng
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  • 关键词

    active sites; benchmarking; hydrogen evolution; molybdenum sulfide; pH;

    机译：活跃的网站;基准;氢气进化;硫化钼;pH;

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