Potential-Gated Spin Crossover Triggers Fe─N─C Catalyst Demetallation

IF 17.6 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Angewandte Chemie International Edition Pub Date : 2026-10-15 DOI:10.1002/anie.8986276

Haobo Li,Xinwei Wang,Bohan Cao,Fubo Tian,Zhiyao Duan

引用次数: 0

Abstract

From spin crossover to Fe dissolution: constant-potential ab initio molecular dynamics (CP–AIMD) simulations reveal an O2-independent degradation pathway at the Fe─N─C/water interface. Below 0.8 V, high-spin Fe(II) sites undergo out-of-plane distortion and water coordination, which trigger N protonation and Fe─N bond cleavage. Above 0.8 V, nearly planar Fe(III)─OH sites resist dissolution, suggesting spin-state control as a design strategy for durable Fe─N─C catalysts.

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电位门控自旋交叉触发Fe─N─C催化剂脱金属

从自旋交叉到Fe溶解：恒电位从头算分子动力学（CP-AIMD）模拟揭示了Fe─N─C/水界面上不依赖于o2的降解途径。在0.8 V以下，高自旋Fe（II）位发生面外畸变和水配位，引发N质子化和Fe─N键断裂。在0.8 V以上，近平面的Fe（III）─OH位抵抗溶解，表明自旋态控制是耐用的Fe─N─C催化剂的设计策略。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Angewandte Chemie International Edition 化学-化学综合

CiteScore

26.60

自引率

6.60%

发文量

3549

审稿时长

1.5 months

期刊介绍： Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.