There has been an intense research effort to develop 2-H MoS₂ based catalysts to reduce or eliminate the use of Pt/C at higher metal loading for the hydrogen evolution reaction (HER) in catalytic hydrolysis of water, which enables the capture of renewable energy sources as fuel and chemical. However, the study of its uncommon polymorph, 1T-MoS₂, and particularly the doping effect with transition metal (TM) is rather limited due to the instability of this phase. Here, we report a simple ambient temperature modification method using sonication to dope the single layer 1T-^SMoS₂ with various TM precursors. It is found that 1T-^SMoS₂ is more active than corresponding 2H-^SMoS₂ and the inclusion of 3 wt % Pt or Pd can also further enhance the HER activity. STEM-EELS and XAS show that the active single TM atom doping on this surface accounts for the high activity. Kinetic and DFT analyses also illustrate that the metallic nature of 1T-^SMoS₂ greatly facilitates the proton reduction step from water, rendering it non-rate-limiting in contrast to that of 2H-^SMoS₂. The inclusion of the TM single doper such as Pd, despite at low loading, can offer the dramatic acceleration of the rate limiting recombination of H to H₂. As a result, a bifunctional catalysis for HER over this tailored composite structure is demonstrated that outperforms most reported catalysts in this area.

中文翻译：

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通过隔离过渡金属原子的声化学掺杂将单层1T-MoS ₂工程化为双功能电催化剂。

进行了大量的研究工作以开发基于2-H MoS ₂的催化剂，以减少或消除在较高的金属负载量下Pt / C用于水催化水解中的析氢反应（HER），从而能够捕获可再生能源。能源用作燃料和化学物质。然而，由于该相的不稳定性，对其稀有多晶型物1T-MoS _2的研究，尤其是过渡金属（TM）的掺杂效果相当有限。在这里，我们报告了一种简单的环境温度修改方法，该方法使用超声处理将各种TM前驱物掺杂到单层1T- ^S MoS _2中。发现1T- ^S MoS ₂的活性高于相应的2H- ^SMoS ₂和包含3 wt％的Pt或Pd也可以进一步增强HER活性。STEM-EELS和XAS表明，在此表面上掺杂的单个TM原子具有很高的活性。动能和DFT分析还说明1T-的金属性质^小号的MoS ₂大大促进从水质子还原步骤，使得在对比的是2H-的它的非限速^小号的MoS ₂。即使在低负荷下也包含TM单一掺杂剂（例如Pd），可以显着加速H到H _2的限速复合。结果表明，在这种定制的复合结构上，HER的双功能催化性能优于该领域大多数报道的催化剂。