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Regulating the interface electron distribution of iron-based MOFs through ligand functionalization enables efficient peroxymonosulfate utilization and catalytic performance.
- Source :
-
Journal of Colloid & Interface Science . Jun2024, Vol. 663, p358-368. 11p. - Publication Year :
- 2024
-
Abstract
- [Display omitted] 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 –NH 2 , –NO 2 , –CH 3 , 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 40.17% under the NH 2 -BDC/PMS system. In terms of mechanism, the amino group not only accelerated the regeneration of Fe(II) via the N C Fe 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 NH 2 -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. [ABSTRACT FROM AUTHOR]
Details
- Language :
- English
- ISSN :
- 00219797
- Volume :
- 663
- Database :
- Academic Search Index
- Journal :
- Journal of Colloid & Interface Science
- Publication Type :
- Academic Journal
- Accession number :
- 176099813
- Full Text :
- https://doi.org/10.1016/j.jcis.2024.02.118