硼在FeC和FeNC单原子ORR催化剂中的取代和配位效应：DFT研究

IF 3 3区化学 Q3 CHEMISTRY, PHYSICAL

Computational and Theoretical Chemistry Pub Date : 2025-03-19 DOI:10.1016/j.comptc.2025.115192

L.L. Sun , Z.Y. Wang , Y.H. Wang , Y. Wang , Y.C. Li

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引用次数: 0

摘要

开发耐用、经济的阴极催化剂是提高燃料电池氧还原反应性能的关键。采用密度泛函理论（DFT）对b取代铁基石墨烯单原子催化剂进行了系统分析。通过对计算地层能量的分析，从49个候选地层中确定了12个稳定构型。第一配位球层中的b取代导致含氧中间体吸附过强，从而增加过电位。相比之下，在第二配位球中取代B的FeN4B4和FeN4B5催化剂的过电位分别为0.32 V和0.36 V。这种增强归因于b原子诱导的电子结构重构和化学键性质的调制。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

Substitution and coordination effects of boron in FeC and FeNC single-atom catalysts for ORR: A DFT study

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Substitution and coordination effects of boron in FeC and FeNC single-atom catalysts for ORR: A DFT study

The development of durable and cost-effective cathode catalysts is critical to improving the oxygen reduction reaction (ORR) of fuel cells. The B-substituted Fe-based graphene single atom catalysts (SACs) were systematically analyzed using density functional theory (DFT). After analysis of the computational formation energy, 12 stable configurations are identified from 49 candidates. B-substituted in the first coordination sphere layer resulted in excessively strong adsorption of oxygen-containing intermediates, thereby increasing the overpotential. In contrast, the FeN₄B₄ and FeN₄B₅ catalysts, with B substitution in the second coordination sphere, exhibited low overpotentials of 0.32 V and 0.36 V, respectively. This enhancement is attributed to the B-atom-induced reconfiguration of the electronic structure and modulation of chemical bonding properties.

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来源期刊

Computational and Theoretical Chemistry CHEMISTRY, PHYSICAL-

CiteScore

4.20

自引率

10.70%

发文量

331

审稿时长

31 days

期刊介绍： Computational and Theoretical Chemistry publishes high quality, original reports of significance in computational and theoretical chemistry including those that deal with problems of structure, properties, energetics, weak interactions, reaction mechanisms, catalysis, and reaction rates involving atoms, molecules, clusters, surfaces, and bulk matter.