A Molecular MoS2 Edge Site Mimic for Catalytic Hydrogen Generation
A Molecular MoS2 Edge Site Mimic for Catalytic Hydrogen Generation
复制标题
DOI：
10.1126/science.1215868
复制
发表时间：
2012-02-10
期刊：
影响因子：
56.9
通讯作者：
Chang, Christopher J.
中科院分区：
文献类型：
--
作者：
Karunadasa, Hemamala I.;Montalvo, Elizabeth;Chang, Christopher J.
无机固体是一类重要的催化剂，它们的活性通常来自结构上不同于非活性本体的稀疏活性位点。因此，合理地优化活性取决于在分子细节上研究这些活性位点的挑战。在这里，我们报告了一种分子，它模拟了二硫化钼（MoS 2）的三角形活性边缘位点片段的结构，二硫化钼是一种广泛使用的工业催化剂，已显示出作为铂的低成本替代品用于电催化制氢的前景。通过利用五吡啶配体的强大配位环境，我们合成了一种定义明确的Mo-IV-二硫键复合物并进行了结构表征，该复合物在电化学还原后可以从酸性有机介质和酸性水中催化产生氢气。
Inorganic solids are an important class of catalysts that often derive their activity from sparse active sites that are structurally distinct from the inactive bulk. Rationally optimizing activity is therefore beholden to the challenges in studying these active sites in molecular detail. Here, we report a molecule that mimics the structure of the proposed triangular active edge site fragments of molybdenum disulfide (MoS2), a widely used industrial catalyst that has shown promise as a low-cost alternative to platinum for electrocatalytic hydrogen production. By leveraging the robust coordination environment of a pentapyridyl ligand, we synthesized and structurally characterized a well-defined Mo-IV-disulfide complex that, upon electrochemical reduction, can catalytically generate hydrogen from acidic organic media as well as from acidic water.