Spin Manipulation of Heterogeneous Molecular Electrocatalysts by an Integrated Magnetic Field for Efficient Oxygen Redox Reactions

IF 27.4 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Advanced Materials Pub Date : 2024-09-17 DOI:10.1002/adma.202408461

Zixun Yu, Di Zhang, Yangyang Wang, Fangzhou Liu, Fangxin She, Jiaxiang Chen, Yuefeng Zhang, Ruijie Wang, Zhiyuan Zeng, Li Song, Yuan Chen, Hao Li, Li Wei

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Abstract

Understanding the spin-dependent activity of nitrogen-coordinated single metal atom (M-N-C) electrocatalysts for oxygen reduction and evolution reactions (ORR and OER) remains challenging due to the lack of structure-defined catalysts and effective spin manipulation tools. Herein, both challenges using a magnetic field integrated heterogeneous molecular electrocatalyst prepared by anchoring cobalt phthalocyanine (CoPc) deposited carbon black on polymer-protected magnet nanoparticles, are addressed. The built-in magnetic field can shift the Co center from low- to high-spin (HS) state without atomic structure modification, affording one-order higher turnover frequency, a 50% increased H₂O₂ selectivity for ORR, and a ≈4000% magnetocurrent enhancement for OER. This catalyst can significantly minimize magnet usage, enabling safe and continuous production of a pure H₂O₂ solution for 100 h from a 100 cm² electrolyzer. The new strategy demonstrated here also applies to other metal phthalocyanine-based catalysts, offering a universal platform for studying spin-related electrochemical processes.

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利用集成磁场对异质分子电催化剂进行自旋操纵，以实现高效的氧氧化还原反应

由于缺乏结构确定的催化剂和有效的自旋操纵工具，了解氮配位单金属原子（M-N-C）电催化剂在氧还原和氧进化反应（ORR 和 OER）中的自旋依赖性活性仍然具有挑战性。在此，通过将沉积碳黑的酞菁钴（CoPc）锚定在聚合物保护的磁性纳米粒子上制备的磁场集成异质分子电催化剂解决了这两个难题。内置磁场可以在不改变原子结构的情况下将钴中心从低自旋（HS）态转移到高自旋（HS）态，从而使翻转频率提高一个数量级，对 ORR 的 H2O2 选择性提高 50%，对 OER 的磁电流增强≈4000%。这种催化剂可以大大减少磁铁的使用量，从而可以在 100 平方厘米的电解槽中安全、连续地生产 100 小时的纯 H2O2 溶液。这里展示的新策略也适用于其他基于金属酞菁的催化剂，为研究自旋相关电化学过程提供了一个通用平台。

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

Advanced Materials 工程技术-材料科学：综合

CiteScore

43.00

自引率

4.10%

发文量

2182

审稿时长

2 months

期刊介绍： Advanced Materials, one of the world's most prestigious journals and the foundation of the Advanced portfolio, is the home of choice for best-in-class materials science for more than 30 years. Following this fast-growing and interdisciplinary field, we are considering and publishing the most important discoveries on any and all materials from materials scientists, chemists, physicists, engineers as well as health and life scientists and bringing you the latest results and trends in modern materials-related research every week.

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