Screening of single-atomic catalysts loaded on two-dimensional transition metal dichalcogenides for electrocatalytic oxygen reduction via high throughput ab initio calculations.

IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Journal of Colloid and Interface Science Pub Date : 2025-01-10 DOI:10.1016/j.jcis.2025.01.060
Hao Sun, Liyao Gao, Yizhe Li, Qingzhen Xu, Yaping Li, Wen Liu
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Abstract

The design and screening of low cost and high efficiency oxygen reduction reaction (ORR) electrocatalysts is vital in the realms of fuel cells and metal-air batteries. Existing studies largely rely on the calculation of absorption free energy, a method established 20 years ago by Jens K. Nørskov. However, the study of electrocatalysts grounded solely on free energy calculation often lacks in-depth analysis, particularly overlooking the influence of solvent and electrode potential. In this regard, we here present a novel approach using constant-potential and ab initio molecular dynamics (AIMD) simulation to screen single-atom catalysts loaded on transition metal dichalcogenides (SA@TMDs) for ORR. An extensive investigation of 1584 SA@TMDs results in 20 high performing ORR catalysts with overpotential less than 0.33 V and high working stability. In addition, our study shows that the electrode potential has different effects on the adsorption energy of *OOH, *O and *OH, which leads to a reversal of the rate-determining step (RDS) of the ORR. This work presents not only credible, high-performance catalyst candidates for experimental exploration, but also significantly improves our understanding on the reaction mechanism of ORR under realistic reaction conditions.

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利用高通量从头计算筛选负载二维过渡金属二硫族化合物的电催化氧还原单原子催化剂。
低成本、高效率氧还原反应电催化剂的设计和筛选在燃料电池和金属-空气电池领域具有重要意义。现有的研究很大程度上依赖于吸收自由能的计算,这是延斯·k·诺斯科夫(Jens K. Nørskov)在20年前建立的一种方法。然而,单纯基于自由能计算的电催化剂研究往往缺乏深入的分析,特别是忽略了溶剂和电极电位的影响。在这方面,我们提出了一种新的方法,使用恒势和从头算分子动力学(AIMD)模拟来筛选负载过渡金属二硫族化合物(SA@TMDs)的单原子催化剂进行ORR。对1584 SA@TMDs进行了广泛的研究,得到了20种过电位小于0.33 V、工作稳定性高的高性能ORR催化剂。此外,我们的研究表明,电极电位对*OOH, *O和*OH的吸附能有不同的影响,导致ORR的速率决定步骤(RDS)逆转。这项工作不仅为实验探索提供了可信的、高性能的催化剂候选物,而且大大提高了我们对现实反应条件下ORR反应机理的理解。
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来源期刊
CiteScore
16.10
自引率
7.10%
发文量
2568
审稿时长
2 months
期刊介绍: The Journal of Colloid and Interface Science publishes original research findings on the fundamental principles of colloid and interface science, as well as innovative applications in various fields. The criteria for publication include impact, quality, novelty, and originality. Emphasis: The journal emphasizes fundamental scientific innovation within the following categories: A.Colloidal Materials and Nanomaterials B.Soft Colloidal and Self-Assembly Systems C.Adsorption, Catalysis, and Electrochemistry D.Interfacial Processes, Capillarity, and Wetting E.Biomaterials and Nanomedicine F.Energy Conversion and Storage, and Environmental Technologies
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