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Magnetic field modulation of high spin hexa-coordinated iron sites to enhance catalytic activity
Applied Catalysis B: Environment and Energy ( IF 22.1 ) Pub Date : 2024-04-17 , DOI: 10.1016/j.apcatb.2024.124087
Hongyao Xue , Jiacheng Wang , He Cheng , Haiqin Zhang , Xiyue Li , Jianbo Sun , Xinyuan Wang , Liguang Lin , Yixue Zhang , Xiaobin Liao , Yan He

The external alternating magnetic field (AMF) strategy is the most promising research topic to solve the bottleneck of catalyst activity enhancement. However, the mechanism between the arrangement of the spin electrons under the AMF and the catalytic activity enhancement for water splitting is still unclear. Herein, we synthesize FeO@CNTs heterostructure as a research model and resolve the mechanism by system theoretical analysis and Raman characterization. The multiple orbital interactions of σ(, , ) and π(-, -) promote the hexa-coordinated Fe for both the reductive HER and oxidative OER processes. The AMF excites the transition from low to high spin configurations of the Fe sites, which accelerates charge transfer of unpaired electrons and optimizes adsorption and desorption interactions to intermediates during the reaction processes, resulting in a significant enhancement of the electrocatalytic activity (HER: 32 mV at 10 mA cm, OER: 179 mV at 100 mA cm).

中文翻译:


高自旋六配位铁位点的磁场调制以增强催化活性



外部交变磁场(AMF)策略是解决催化剂活性增强瓶颈最有前景的研究课题。然而,AMF下自旋电子的排列与水分解催化活性增强之间的机制仍不清楚。在此,我们合成了FeO@CNTs异质结构作为研究模型,并通过系统理论分析和拉曼表征解析了其机理。 σ(, , ) 和 π(-, -) 的多轨道相互作用促进了六配位 Fe 的还原 HER 和氧化 OER 过程。 AMF激发Fe位点从低自旋构型到高自旋构型的转变,加速了不成对电子的电荷转移,并优化了反应过程中中间体的吸附和解吸相互作用,从而显着增强了电催化活性(HER:32mV) 10mAcm 时,OER:100mAcm 时 179mV)。
更新日期:2024-04-17
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