电负性
催化作用
卤素
析氧
过电位
金属有机骨架
材料科学
对苯二甲酸
光化学
无机化学
吸附
化学
物理化学
有机化学
电化学
电极
聚酯纤维
复合材料
烷基
作者
Yitian Hu,Yalei Fan,Lili Li,Jing Zhou,Zhiwei Hu,Jian‐Qiang Wang,Juncai Dong,Shenlong Zhao,Linjuan Zhang
出处
期刊:Small
[Wiley]
日期:2024-04-11
标识
DOI:10.1002/smll.202400042
摘要
Abstract Modulating the coordination environment of the metal active center is an effective method to boost the catalytic performances of metal–organic frameworks (MOFs) for oxygen evolution reaction (OER). However, little attention has been paid to the halogen effects on the ligands engineering. Herein, a series of MOFs X─FeNi‐MOFs (X = Br, Cl, and F) is constructed with different coordination microenvironments to optimize OER activity. Theoretical calculations reveal that with the increase in electronegativity of halogen ions in terephthalic acid molecular (TPA), the Bader charge of Ni atoms gets larger and the Ni‐3d band center and O‐2p bands move closer to the Fermi level. This indicates that an increase in ligand negativity of halogen ions in TPA can promote the adsorption ability of catalytic sites to oxygen‐containing intermediates and reduce the activation barrier for OER. Experimental also demonstrates that F─FeNi‐MOFs exhibit the highest catalytic activity with an ultralow overpotential of 218 mV at 10 mA cm −2 , outperforming most otate‐of‐the‐art Fe/Co/Ni‐based MOFs catalysts, and the enhanced mass activity by seven times compared with that for the sample before ligands engineering. This work opens a new avenue for the realization of the modulation of NiFe─O bonding by halogen ion in TPA and improves the OER performance of MOFs.
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