The dynamic regulation effect in X@Fe-N4/C electrocatalyst for the sequential oxygen reduction reaction

IF 4.9 2区化学 Q2 CHEMISTRY, PHYSICAL

Colloids and Surfaces A: Physicochemical and Engineering Aspects Pub Date : 2025-02-25 DOI:10.1016/j.colsurfa.2025.136512

Xiaoming Zhang , Suli Wang , Zhangxun Xia , Huanqiao Li , Shansheng Yu , Gongquan Sun

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引用次数: 0

Abstract

Metal-nitrogen-carbon based single atom catalysts (SACs) have been the subject of oxygen reduction reaction (ORR) electrocatalysts for electrochemical devices. Nevertheless, the scaling relationship of ΔG_*OOH, ΔG_*OH and ΔG_*O represents a significant obstacle to further enhancement of ORR efficiency for SACs. Accordingly, a confinement model X@M-N₄/C electrocatalyst was constructed. The density functional theory calculations demonstrate that the overpotential of Br@Fe-N₄/C54 (0.47 V vs. RHE) for ORR is significantly lower than that of Fe-N₄/C54 (0.67 V vs. RHE). The variation in distance between the Br and Fe atoms during the ORR process provides evidence that supports the hypothesis that the Br atom regulates the Fe-N₄ active center, through in-situ dynamic non-bonding coordination (d_Fe-Br>3 Å). The confined Br atom results in an increase in ΔG_*OH and a decrease in ΔG_*O. This results in a disruption of the linear relationship and a reduction in the overpotential associated with the rate-determining elementary reaction (*O+H⁺+e^-→*OH). The Fe-N₄ active center facilitates the sequential ORR catalytic process through in-situ dynamic regulation of the trapped Br atom. This conclusion is also applicable to Br@Fe-N₄/graphene and Br@Fe-N₄/CNT. The findings of our research represent a significant advancement in the field of enhancing the performance of SACs for multi-electron electrocatalytic reactions.

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来源期刊

Colloids and Surfaces A: Physicochemical and Engineering Aspects 化学-物理化学

CiteScore

8.70

自引率

9.60%

发文量

2421

审稿时长

56 days

期刊介绍： Colloids and Surfaces A: Physicochemical and Engineering Aspects is an international journal devoted to the science underlying applications of colloids and interfacial phenomena. The journal aims at publishing high quality research papers featuring new materials or new insights into the role of colloid and interface science in (for example) food, energy, minerals processing, pharmaceuticals or the environment.