Modulation of the Phase Transformation of Fe2O3 for Enhanced Water Oxidation under a Magnetic Field,ACS Catalysis

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Modulation of the Phase Transformation of Fe2O3 for Enhanced Water Oxidation under a Magnetic Field
ACS Catalysis ( IF 11.3 ) Pub Date : 2024-01-04 , DOI: 10.1021/acscatal.3c05032
Guangjian Song _{1,

2} , Ming Wei _{1,

2} , Jing Zhou ₃ , Liuhua Mu _{1,

4} , Sanzhao Song ₁

Affiliation

Ferromagnetic catalysts in the presence of an external magnetic field can promote the reaction kinetics of the oxygen evolution reaction (OER) by enhancing spin-selective electron transfer as intermediates and products confer spin-dependent behavior. It has been found that γ-Fe₂O₃ with ferromagnetism exhibits an enhanced performance for the OER activity, but its preparation is limited. Herein, we report an adsorption-pyrolysis process in air in which the transformation of α-Fe₂O₃ into γ-Fe₂O₃ is precisely regulated by controlling the content of Co ions. Interestingly, a small, constant external magnetic field (∼200 mT) was applied at the anode, resulting in a significant impact on the OER performance of the obtained series of catalysts with different contents of γ-Fe₂O₃ under alkaline conditions. Theoretical results reveal that the same spin configuration of Fe and O atoms in γ-Fe₂O₃ provides a spin conduction channel, which enhances the ability to selectively remove spin-oriented electrons from the reactants and accelerates the accumulation of triplet oxygen molecules during the OER process, thereby promoting the OER. These findings provide a strategy toward the controllable phase transformation of Fe₂O₃ and deep insights for understanding the OER behavior of Fe-based electrocatalysts under magnetic fields.

中文翻译：

磁场下增强水氧化的 Fe2O3 相变调控

在存在外部磁场的情况下，铁磁催化剂可以通过增强自旋选择性电子转移来促进析氧反应（OER）的反应动力学，因为中间体和产物具有自旋依赖性行为。研究发现，具有铁磁性的γ-Fe ₂ O ₃表现出增强的OER活性，但其制备受到限制。在此，我们报道了空气中的吸附热解过程，其中通过控制Co离子的含量来精确调节α-Fe ₂ O ₃转化为γ-Fe ₂ O _{3 。}有趣的是，在阳极施加一个小的、恒定的外部磁场（~200 mT），对所获得的不同γ-Fe ₂ O ₃含量系列催化剂在碱性条件下的OER性能产生显着影响。理论结果表明，γ-Fe ₂ O ₃中Fe和O原子的相同自旋构型提供了自旋传导通道，增强了从反应物中选择性去除自旋取向电子的能力，并加速了三线态氧分子在反应过程中的积累。 OER进程，从而促进OER。_{这些发现为 Fe 2} O ₃的可控相变提供了策略，并为理解磁场下铁基电催化剂的 OER 行为提供了深刻的见解。

更新日期：2024-01-04

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