Contrasting Oxygen Reduction Reactions on Zero- and One-Dimensional Defects of MoS2 for Versatile Applications.,ACS Applied Materials & Interfaces

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Contrasting Oxygen Reduction Reactions on Zero- and One-Dimensional Defects of MoS2 for Versatile Applications.
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2019-11-26 , DOI: 10.1021/acsami.9b14502
Yu Hao ₁ , Peng-Lai Gong _{1,

2} , Li-Chun Xu , Jibin Pu ₁ , Liping Wang ₁ , Liang-Feng Huang _{1,

3}

Affiliation

Oxygen reduction reaction (ORR) is a key microscopic process in many electrochemical applications of materials, where the requirements of their ORR performances may vary strikingly, for example, during the uses of MoS2 as an electrocatalyst and anticorrosion/lubricating coating in aqueous/humid environments, ORR should be activated and inhibited, respectively. To reveal a complete ORR profile of MoS2, using first-principles calculations, we examine the stabilities of various possible zero-dimensional point defects on the surface and one-dimensional edge defects and comprehensively explore the ORR activities on pristine MoS2 surface and those defects in acid/alkaline solutions. It is found that the ORRs on the pristine surface and surfaces with point defects always require large overpotentials (>1.0 V), indicating a defect-immune resistance of the planar MoS2 surface against the ORR. However, the ORR overpotentials on edge defects can reach as low as 0.66 V, corresponding to a relatively high activity close to that of the prototypical catalyst Pt (overpotential ∼0.45 V). Such contrasting ORR behaviors of point and edge defects are also understood in depth by analyzing the underlying thermodynamic and electronic-structure mechanisms. This work not only quantitatively explains the performances of MoS2 in both galvanic corrosion and electrochemical catalysis but also provides a useful structure-ORR map that can facilitate adapting the realistic MoS2 to versatile electrochemical applications.

中文翻译：

MoS2零和一维缺陷上的对比氧还原反应，用途广泛。

在许多材料的电化学应用中，氧还原反应（ORR）是关键的微观过程，这些材料对ORR性能的要求可能会发生巨大变化，例如，在水/潮湿环境中使用MoS2作为电催化剂和防腐/润滑涂层期间，应分别激活和禁止ORR。为了揭示MoS2的完整ORR轮廓，使用第一性原理计算，我们检查了表面上各种可能的零维点缺陷和一维边缘缺陷的稳定性，并全面研究了原始MoS2表面上的ORR活性以及这些Mos2中的缺陷。酸/碱溶液。发现原始表面和具有点缺陷的表面上的ORR始终需要较大的过电势（> 1.0 V），表示平面MoS2表面对ORR的免疫缺陷抵抗力。但是，边缘缺陷上的ORR超电势可低至0.66 V，这对应于接近原型催化剂Pt的相对较高的活性（超电势约为0.45 V）。通过分析潜在的热力学和电子结构机理，还可以深入了解点缺陷和边缘缺陷的这种对比ORR行为。这项工作不仅定量地解释了MoS2在电腐蚀和电化学催化中的性能，而且提供了有用的结构ORR图，可以促进将实际的MoS2适应各种电化学应用。相当于接近典型催化剂Pt的较高活性（过电势约为0.45 V）。通过分析潜在的热力学和电子结构机理，还可以深入了解点缺陷和边缘缺陷的这种对比ORR行为。这项工作不仅定量地解释了MoS2在电腐蚀和电化学催化中的性能，而且提供了有用的结构ORR图，可以促进将实际的MoS2适应各种电化学应用。相当于接近典型催化剂Pt的较高活性（过电势约为0.45 V）。通过分析潜在的热力学和电子结构机理，还可以深入了解点缺陷和边缘缺陷的这种对比ORR行为。这项工作不仅定量地解释了MoS2在电腐蚀和电化学催化中的性能，而且提供了有用的结构ORR图，可以促进将实际的MoS2适应各种电化学应用。

更新日期：2019-11-28

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