键交换机制：揭示 Volmer-Tafel 途径和用于预测硼烯析氢反应活性的电子描述符,ACS Applied Energy Materials

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键交换机制：揭示 Volmer-Tafel 途径和用于预测硼烯析氢反应活性的电子描述符
ACS Applied Energy Materials ( IF 5.4 ) Pub Date : 2023-08-21 , DOI: 10.1021/acsaem.3c01570
Erakulan E. Siddharthan ₁ , Sourav Ghosh ₁ , Ranjit Thapa _{1,

2}

Affiliation

氢作为燃料是有害化石燃料的有前途的替代品，因此通过电催化析氢反应（HER）生产氢是一个重要的研究问题。利用密度泛函理论，在硼烯片上研究了通过 Volmer-Tafel (V-T) 途径的H _2演化。结果表明，该片材表现出与铂相当的高活性。对解释实验结果的机制进行更好的理论理解是一个现有的问题。为了解决这个问题，我们提出H ₂通过塔菲尔步骤中的键交换机制演化。_{与直接H 2}的现有模型相比，通过该机制的活化能大大降低进化并且与 HER 活化能方面的实验结果吻合良好。还在其他 HER 催化剂上进行了测试和观察，例如氮掺杂石墨烯、2H-MoS ₂和 Pt(111)，这证明所提出的机制对于 HER 是正确的。提出了一种基于电子特性的描述符，该描述符与硼烯片上的 HER 活性具有良好的相关性。这项工作为 HER 的理论模型提供了见解，并可以进一步找到更好的方法来理解该反应。电子描述符还可以在类似的硼同素异形体和反应上进行测试。

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Bond Exchange Mechanism: Unveiling the Volmer–Tafel Pathway and an Electronic Descriptor for Predicting Hydrogen Evolution Reaction Activity of Borophene

Hydrogen as a fuel is a promising alternative to harmful fossil fuels, thereby its production by electrocatalytic hydrogen evolution reaction (HER) is an important research problem. Using density functional theory, H₂ evolution through the Volmer–Tafel (V–T) pathway is studied on borophene sheets. The results reveal that the sheets exhibit high activity, comparable to platinum. A better theoretical understanding of the mechanism that explains the experimental results is an existing issue. To address this issue, we have proposed that H₂ evolves through a bond-exchange mechanism in the Tafel step. The activation energy through this mechanism is drastically reduced, compared to the existing model of direct H₂ evolution and matches well with the experimental results in terms of activation energy for HER. It is also tested and observed on other HER catalysts, such as nitrogen-doped graphene, 2H-MoS₂, and Pt(111), which proves the proposed mechanism is correct for HER. An electronic property-based descriptor is proposed that shows a good correlation with HER activity on the borophene sheets. This work sheds insights into theoretical modeling of HER and can further lead to better methods toward the understanding of the reaction. Also the electronic descriptor can be tested on similar boron allotropes and reactions.

更新日期：2023-08-21

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