The development of nonprecious electrochemical catalysts for water splitting is a key step to achieve a sustainable energy supply for the future. Molybdenum disulfide (MoS₂) has been extensively studied as a promising low‐cost catalyst for hydrogen evolution reaction (HER), whereas HER is only catalyzed at the edge for pristine MoS₂, leaving a large area of basal plane useless. Herein, on‐surface self‐assembly is demonstrated to be an effective, facile, and damage‐free method to take full advantage of the large ratio surface of MoS₂ for HER by using multiscale simulations. It is found that as supplement of edge sites of MoS₂, on‐MoS₂ M(abt)₂ (M = Ni, Co; abt = 2‐aminobenzenethiolate) owns high HER activity, and the self‐assembled M(abt)₂ monolayers on MoS₂ can be obtained through a simple liquid‐deposition method. More importantly, on‐surface self‐assembly provides potential application for overall water splitting once the self‐assembled systems prove to be of both HER and oxygen evolution reaction activities, for example, on‐MoS₂ Co(abt)₂. This work opens up a new and promising avenue (on‐surface self‐assembly) toward the full exploitation of the basal plane of MoS₂ for HER and the preparation of bifunctional catalysts for overall water splitting.

中文翻译：

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MoS2大面积基础平面的开发和通过表面自组装制备双功能催化剂

开发用于水分解的非贵金属电化学催化剂是实现未来可持续能源供应的关键步骤。二硫化钼（MoS ₂）作为氢释放反应（HER）的有前途的低成本催化剂已被广泛研究，而HER仅在原始MoS ₂的边缘被催化，而使大面积的基底平面无用。在此，通过使用多尺度模拟，证明了表面自组装是一种有效，便捷且无损坏的方法，可以充分利用MoS ₂的大比例表面用于HER。发现作为MoS ₂边缘位点的补充，在MoS ₂ M（abt）_2上（M = Ni，Co; abt = 2-氨基苯硫醚）具有较高的HER活性，并且可以通过简单的液体沉积方法在MoS ₂上获得自组装的M（abt）₂单层。更重要的是，一旦证明自组装系统具有HER和放氧反应活性，例如，on-MoS ₂ Co（abt）₂，则表面自组装将为整体水分解提供潜在的应用。这项工作为全面开发用于HER的MoS ₂基础平面和制备用于整体水分解的双功能催化剂开辟了新的前景广阔的途径（表面自组装）。