密度泛函理论
过电位
双金属片
自旋(空气动力学)
气凝胶
磁矩
催化作用
材料科学
电子能带结构
带隙
电子结构
轨道杂交
凝聚态物理
化学物理
纳米技术
分子轨道
化学
计算化学
物理化学
分子轨道理论
光电子学
物理
电极
热力学
分子
有机化学
电化学
作者
Cunyuan Gao,Juan Wang,René Hübner,Bin Cai,Mingwen Zhao,Yangyang Li,Bin Cai
出处
期刊:Small
[Wiley]
日期:2024-04-01
标识
DOI:10.1002/smll.202400875
摘要
"Spin" has been recently reported as an important degree of electronic freedom to promote catalysis, yet how it influences electronic structure remains unexplored. This work reports the spin-induced orbital hybridization in Ir─Fe bimetallic aerogels, where the electronic structure of Ir sites is effectively regulated by tuning the spin property of Fe atoms. The spin-optimized electronic structure boosts oxygen evolution reaction (OER) electrocatalysis in acidic media, resulting in a largely improved catalytic performance with an overpotential of as low as 236 mV at 10 mA cm-2. Furthermore, the gelation kinetics for the aerogel synthesis is improved by an order of magnitude based on the introduction of a magnetic field. Density functional theory calculation reveals that the increased magnetic moment of Fe (3d orbital) changes the d-band structure (i.e., the d-band center and bandwidth) of Ir (5d orbital) via orbital hybridization, resulting in optimized binding of reaction intermediates. This strategy builds the bridge between the electron spin theory with the d-band theory and provides a new way for the design of high-performance electrocatalysts by using spin-induced orbital interaction.
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