Tunable Molecular MoS2 Edge-Site Mimics for Catalytic Hydrogen Production

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• 作者：Benjamin R. Garrett ; Shane M. Polen ; Kevin A. Click ; Mingfu He ; Zhongjie Huang ; Christopher M. Hadad ; Yiying Wu
• 刊名：Inorganic Chemistry
• 出版年：2016
• 出版时间：April 18, 2016
• 年：2016
• 卷：55
• 期：8
• 页码：3960-3966
• 全文大小：386K
• 年卷期：0
• ISSN：1520-510X

文摘

Molybdenum sulfides represent state-of-the-art, non-platinum electrocatalysts for the hydrogen evolution reaction (HER). According to the Sabatier principle, the hydrogen binding strength to the edge active sites should be neither too strong nor too weak. Therefore, it is of interest to develop a molecular motif that mimics the catalytic sites structurally and possesses tunable electronic properties that influence the hydrogen binding strength. Furthermore, molecular mimics will be important for providing mechanistic insight toward the HER with molybdenum sulfide catalysts. In this work, a modular method to tune the catalytic properties of the S–S bond in MoO(S₂)₂L₂ complexes is described. We studied the homogeneous electrocatalytic hydrogen production performance metrics of three catalysts with different bipyridine substitutions. By varying the electron-donating abilities, we present the first demonstration of using the ligand to tune the catalytic properties of the S–S bond in molecular MoS₂ edge-site mimics. This work can shed light on the relationship between the structure and electrocatalytic activity of molecular MoS₂ catalysts and thus is of broad importance from catalytic hydrogen production to biological enzyme functions.