One-pot vanadium-based organic frameworks for DEHP effective removal: Relationships between the synthetic strategy, characterization, adsorption and solar-driven photocatalytic activity

光催化 吸附 表征(材料科学) 降级(电信) 材料科学 金属有机骨架 X射线光电子能谱 化学工程 纳米技术 光化学 无机化学 化学 有机化学 催化作用 工程类 计算机科学 电信
作者
Ying Zhang,Li Ruohan,Zhengfang Zhang,Wei Mao,X. T. Zheng,Yuntao Guan
出处
期刊:Journal of Industrial and Engineering Chemistry [Elsevier BV]
卷期号:138: 528-542
标识
DOI:10.1016/j.jiec.2024.04.031
摘要

Metal-organic frameworks (MOFs) are promising photocatalysts, yet the incorporation of vanadium into MOFs is prospective to achieve broad visible-light response, functionalized and topography-selective photocatalysts. Herein, we developed a series of self-assembly and template-free vanadium-based frameworks (V-MOFs) via a one-pot synthesis method accelerating the efficient adsorption and solar-driven photocatalytic degradation of DEHP, where V ions were immobilized by -COO groups to form various favorable configurations and the monodispersed transient V3+/V4+/V5+ centers served as active sites facilitating the separation of photogenerated charges. The advantageous photoelectron leaping capability, electron-hole lifetime and catalytic active sites of the synthesized V-MOFs were verified. The Mantel test analysis was applied to obtain the optimal synthetic route by exploring the correlation among the synthesis factors, V-MOFs' characterization, and DEHP adsorption-degradation properties, the resultant V1-BDA@ and V1-H3BTB@ exhibited outstanding photocatalytic degradation and adsorption performances with a total DEHP (20 ppm) removal rate of 98 % in 240 min. The effective attack sites on DEHP were explained by Fukui function, and the photocatalytic degradation pathway of DEHP by V1-H3BTB@ was furtherly revealed.
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