Tunable electronic structures and oxygen electrocatalytic mechanisms in Fe-N-C catalysts doped with B, P, S, and O heteroatoms

IF 6.9 2区材料科学 Q2 CHEMISTRY, PHYSICAL

Applied Surface Science Pub Date : 2025-01-15 DOI:10.1016/j.apsusc.2025.162439

Yue Zhang , Jianguang Feng , Chenchen Ma , Xiaoyun Gu , Liyan Yu , Lifeng Dong

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Abstract

The oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) are pivotal processes for the operation of metal-air batteries, directly impacting their efficiency and performance. The coordination environment of M-N-C catalysts play a crucial role in defining the structure–activity relationship and electrocatalytic behavior of these materials. This study investigates the bifunctional (ORR/OER) activity of Fe-N-C catalysts doped with heteroatoms (B, P, S) and their oxidized forms using density functional theory (DFT). Analysis of electron distribution within these doped Fe-N-C catalysts reveal that heteroatom incorporation induces electron modulation, enhancing the electrocatalytic activity of the nanomaterials. The findings indicate that the presence of oxygen in the doped structures significantly boosts catalytic performance, with oxidized phosphorus doped Fe-N-C catalyst supported on graphene (FeN₄PO-G) displaying the highest bifunctional activity. This work sheds light on the synergistic effects of non-metal and transition metal doping on the ORR and OER mechanisms in graphene-based electrocatalysts, providing a foundation for the rational design of advanced, high-performance catalysts.

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掺杂B、P、S和O杂原子的Fe-N-C催化剂的可调谐电子结构和氧电催化机理

氧还原反应（ORR）和析氧反应（OER）是金属-空气电池运行的关键过程，直接影响电池的效率和性能。M-N-C催化剂的配位环境对确定这些材料的构效关系和电催化行为起着至关重要的作用。本研究利用密度泛函理论（DFT）研究了掺杂杂原子（B， P， S）及其氧化形式的Fe-N-C催化剂的双功能（ORR/OER）活性。对Fe-N-C掺杂催化剂内部电子分布的分析表明，杂原子掺入诱导了电子调制，提高了纳米材料的电催化活性。研究结果表明，氧的存在显著提高了结构的催化性能，氧化磷掺杂的Fe-N-C催化剂在石墨烯负载（FeN4PO-G）上表现出最高的双功能活性。本研究揭示了非金属和过渡金属掺杂对石墨烯基电催化剂的ORR和OER机制的协同作用，为合理设计先进、高性能的催化剂提供了基础。

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来源期刊

Applied Surface Science 工程技术-材料科学：膜

CiteScore

12.50

自引率

7.50%

发文量

3393

审稿时长

67 days

期刊介绍： Applied Surface Science covers topics contributing to a better understanding of surfaces, interfaces, nanostructures and their applications. The journal is concerned with scientific research on the atomic and molecular level of material properties determined with specific surface analytical techniques and/or computational methods, as well as the processing of such structures.