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Creating Fluorine-Doped MoS2 Edge Electrodes with Enhanced Hydrogen Evolution Activity
Small Methods ( IF 10.7 ) Pub Date : 2021-09-12 , DOI: 10.1002/smtd.202100612 Ruihua Zhang 1 , Mengru Zhang 1 , Hao Yang 2 , Gen Li 1 , Shuming Xing 1 , Mengyan Li 1 , Yiling Xu 1 , Qiuyue Zhang 1 , Sheng Hu 1, 3 , Honggang Liao 1 , Yang Cao 1, 3
Small Methods ( IF 10.7 ) Pub Date : 2021-09-12 , DOI: 10.1002/smtd.202100612 Ruihua Zhang 1 , Mengru Zhang 1 , Hao Yang 2 , Gen Li 1 , Shuming Xing 1 , Mengyan Li 1 , Yiling Xu 1 , Qiuyue Zhang 1 , Sheng Hu 1, 3 , Honggang Liao 1 , Yang Cao 1, 3
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The edge sites of MoS2 are catalytically active for hydrogen evolution reactions (HER). However, pristine edge sites usually contain only intrinsic atoms or defects, limiting the tuning of on-site hydrogen species adsorption and desorption, the critical steps for HER. In addition, the number of atoms on pristine edges is small compared to that of electrochemically inert atoms in bulk. Thus, it is desirable to develop a scalable technique of creating a large number of highly HER-active edge sites. Here, a plasma etching strategy is developed for creating MoS2 edge electrodes with a controllable number of active sites that enable the quantitative characterization of their HER activity using a local probe method. Fluorine atoms with large electronegativity are doped on the MoS2 edge sites that lead to a fivefold activity enhancement compared to that from pristine edges and is attributed to the more moderate binding energy for hydrogen species. The scalability of such a method is further demonstrated by activating MoS2 catalyst in macroscopic quantities with enhanced HER performance and stability. The work provides two-dimensional materials as a platform for understanding the doping effect on the edge sites at atomic-level, and offers a novel route for the design of efficient catalysts.
中文翻译：
创建具有增强的析氢活性的氟掺杂的 MoS2 边缘电极
MoS 2的边缘位点对析氢反应（HER）具有催化活性。然而，原始边缘位点通常只包含本征原子或缺陷，限制了现场氢物质吸附和解吸的调整，这是 HER 的关键步骤。此外，与大量电化学惰性原子相比，原始边缘上的原子数量很少。因此，需要开发一种可扩展的技术来创建大量具有高度 HER 活性的边缘位点。在这里，开发了一种等离子体蚀刻策略，用于创建具有可控数量的活性位点的MoS 2边缘电极，从而能够使用局部探针方法对其 HER 活性进行定量表征。具有大电负性的氟原子掺杂在 MoS 上与原始边缘相比，2 个边缘位点的活性提高了五倍，这归因于氢物种的更适中的结合能。这种方法的可扩展性通过在宏观数量上激活 MoS 2催化剂而得到进一步证明，同时提高了 HER 性能和稳定性。该工作提供了二维材料作为理解原子级边缘位点掺杂效应的平台，并为设计高效催化剂提供了一条新途径。
更新日期：2021-11-12
中文翻译：
创建具有增强的析氢活性的氟掺杂的 MoS2 边缘电极
MoS 2的边缘位点对析氢反应（HER）具有催化活性。然而，原始边缘位点通常只包含本征原子或缺陷，限制了现场氢物质吸附和解吸的调整，这是 HER 的关键步骤。此外，与大量电化学惰性原子相比，原始边缘上的原子数量很少。因此，需要开发一种可扩展的技术来创建大量具有高度 HER 活性的边缘位点。在这里，开发了一种等离子体蚀刻策略，用于创建具有可控数量的活性位点的MoS 2边缘电极，从而能够使用局部探针方法对其 HER 活性进行定量表征。具有大电负性的氟原子掺杂在 MoS 上与原始边缘相比，2 个边缘位点的活性提高了五倍，这归因于氢物种的更适中的结合能。这种方法的可扩展性通过在宏观数量上激活 MoS 2催化剂而得到进一步证明，同时提高了 HER 性能和稳定性。该工作提供了二维材料作为理解原子级边缘位点掺杂效应的平台，并为设计高效催化剂提供了一条新途径。
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