表面改性
催化作用
化学
配体(生物化学)
电子转移
吸附
降级(电信)
金属有机骨架
化学工程
电子定域函数
工作职能
密度泛函理论
金属
光化学
电子
计算化学
有机化学
物理化学
物理
工程类
电信
受体
量子力学
生物化学
计算机科学
作者
Yuwei Xue,Ran Gao,Shuangjie Lin,Qing Zhong,Qian Zhang,Junming Hong
标识
DOI:10.1016/j.jcis.2024.02.118
摘要
Ligand functionalization is an effective way to endow Metal-organic frameworks (MOF) with versatility for multiple applications by introducing or displaying substituents without changing the origin framework. In this work, the original MIL-101(Fe) was modified by functional groups, including –NH2, –NO2, –CH3, and -Cl substituents. The Bader charge results and electron localization function (ELF) quantitatively indicated that the functional ligands with different properties can regulate the electron structure of transition-metal centers through interface-charge redistribution. Accompanying the higher adsorption and utilization rate of peroxymonosulfate (PMS), more than 96% of acetaminophen (APAP) was degraded with a mineralization rate of 44.5% under the NH2-BDC/PMS system. In terms of mechanism, the amino group not only accelerated the regeneration of Fe(II) via the NCFe electron-transfer path, but also stimulated the appearance of high-valent Fe species. Meanwhile, the degradation pathways of APAP were proposed by integrating the results of liquid chromatograph-mass spectrometry (LC-MS) and Frontier molecular-orbital theory. Finally, the NH2-BDC/PMS system reveals long-term stability, nonselectivity, low biotoxicity as well as secondary pollution for pollutant degradation, which is a considered candidate for further environmental applications.
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