Oxyanion Engineering Renewable Lattice Oxygen Mechanism of CoFe Oxide for Enhanced Water Oxidation

IF 18.5 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Advanced Functional Materials Pub Date : 2025-06-19 DOI:10.1002/adfm.202505936

Xiaorong He, Meihuan Liu, Feng Liu, Xuanzhi Liu, Hanxiao Liao, Pengfei Tan, Jun Pan

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Abstract

Lattice oxygen mechanism (LOM) promises CoFe-based catalysts with superior oxygen evolution reaction (OER) performance in alkaline media. However, the imbalance between rapid consumption and sluggish regeneration of lattice oxygen causes oxygen vacancy accumulation and catalyst structure collapse during OER, resulting in poor activity and stability. To surmount this challenge, an oxyanion-tailored strategy by adsorbing phosphate ions on CoFe oxide to realize renewable LOM is proposed. The longer Co─O bond with enhanced Co─O hybridization after adsorbing phosphate ion (PO₄³⁻)stimulates the evolution of lattice oxygen for boosting OER. Meanwhile, the local surficial Co(Fe)OOH formed on CoFe oxide modified by PO₄³⁻during OER with high adsorption capacity serves as a service station, providing oxygenous intermediates to offset released lattice oxygen of CoFe oxide with satisfied durability. Therefore, the overpotential of CoFe oxide is reduced by 42 mV after adsorbing PO₄³⁻ and the PO₄³⁻ modified CoFe oxide shows an extremely robustness over 300 h with a low attenuation of 0.02 mA h⁻¹, outperforming that of pure CoFe oxide (attenuation: 0.26 mA h⁻¹). This work represents a momentous step toward optimizing the catalytic performances of cobalt–iron-based catalysts by regulating renewable lattice oxygen mechanism.

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氧化铁强化水氧化的氧化阴离子工程可再生晶格氧机理

晶格氧机制（LOM）使钴基催化剂在碱性介质中具有优异的析氧反应（OER）性能。然而，晶格氧的快速消耗和缓慢再生之间的不平衡导致OER过程中氧空位积累和催化剂结构崩溃，导致活性和稳定性差。为了克服这一挑战，提出了一种氧阴离子定制策略，通过将磷酸盐离子吸附在氧化铁上来实现可再生LOM。吸附磷酸离子（PO43−）后，Co─O键变长，Co─O杂化增强，促进了晶格氧的演化，提高了OER。同时，PO43−修饰的CoFe氧化物在OER过程中形成的局部表面Co(Fe)OOH具有较高的吸附能力，充当了一个服务站，为CoFe氧化物释放的点阵氧提供了含氧中间体，具有较好的耐久性。因此，吸附PO43 -后，氧化铁的过电位降低了42 mV，并且PO43 -修饰的氧化铁在300 h内表现出极强的鲁棒性，衰减为0.02 mA h−1，优于纯氧化铁（衰减为0.26 mA h−1）。这项工作代表了通过调节可再生晶格氧机制来优化钴铁基催化剂催化性能的重要一步。

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来源期刊

Advanced Functional Materials 工程技术-材料科学：综合

CiteScore

29.50

自引率

4.20%

发文量

2086

审稿时长

2.1 months

期刊介绍： Firmly established as a top-tier materials science journal, Advanced Functional Materials reports breakthrough research in all aspects of materials science, including nanotechnology, chemistry, physics, and biology every week. Advanced Functional Materials is known for its rapid and fair peer review, quality content, and high impact, making it the first choice of the international materials science community.