Efficient removal of organophosphate esters by ligand functionalized MIL-101 (Fe): Modulated adsorption and DFT calculations

被引：40

作者：

Fan, Sheng ^{[1
]}

Lu, Xinru ^{[2
]}

Li, Haoliang ^{[1
]}

Du, Xiaodong ^{[1
]}

Huang, Xiaoyu ^{[2
]}

Ma, Yao ^{[1
]}

Wang, Juan ^{[1
]}

Tao, Xueqin ^{[2
]}

Dang, Zhi ^{[1
,3
,4
]}

Lu, Guining ^{[1
,3
]}

机构：

[1] South China Univ Technol, Sch Environm & Energy, Guangzhou 510006, Peoples R China

[2] Zhongkai Univ Agr & Engn, Coll Resources & Environm, Guangzhou 510225, Peoples R China

[3] South China Univ Technol, Key Lab Pollut Control & Ecosyst Restorat Ind Clus, Minist Educ, Guangzhou 510006, Peoples R China

[4] South China Univ Technol, Guangdong Prov Key Lab Solid Wastes Pollut Control, Guangzhou 510006, Peoples R China

来源：

CHEMOSPHERE | 2022年 / 302卷

基金：

中国国家自然科学基金;

关键词：

Organophosphate esters adsorption; Metal-organic frameworks; Ligand functionalization; Density functional theory; Adsorption mechanism; METAL-ORGANIC FRAMEWORKS; MOLECULAR-ORBITAL METHODS; TRIS(2-CHLOROETHYL) PHOSPHATE TCEP; GAUSSIAN-TYPE BASIS; FLAME RETARDANTS; AQUEOUS-SOLUTION; PHOTOCATALYTIC ACTIVITY; BASIS-SETS; PLASTICIZERS; DEGRADATION;

D O I：

10.1016/j.chemosphere.2022.134881

中图分类号：

X [环境科学、安全科学];

学科分类号：

08 ; 0830 ;

摘要：

Organophosphate esters (OPEs) are a new class of flame retardants present in diverse waters. The study focused on the removal of aqueous OPEs using functionalized MIL-101(Fe), which was a representative of the metal-organic frameworks (MOFs). Adsorption kinetics of tris(2-chloroethyl) phosphate (TCEP), tributyl phosphate (TnBP), and triphenyl phosphate (TPhP) were investigated. Additionally, TCEP was selected as the model contaminant to study the adsorption isotherms, thermodynamics, and effect of solution matrix properties. Adsorption mechanisms obtained from the experiments were confirmed using density functional theory (DFT) calculations. Adsorption kinetics indicated that functionalized MOFs provided a significant enhancement to the removal of TCEP. The maximum adsorption capacities q(m) of MIL-101(Fe), MIL-101(Fe)-NH2, MIL-101(Fe)-OH, and MIL-101(Fe)-CH3 at 298 K for TCEP were 76.040, 282.940, 119.680, and 181.274 mu mol/g, respectively. By comparing the adsorption behavior of functionalized MOFs, MIL-101(Fe)-NH2 was proved to be most efficient for TCEP removal. Based on the adsorption experiments and DFT calculations, TCEP removal was dominated by physical adsorption. The van der Waals (vdW) interactions and hydrogen bonding were assumed to be involved in the adsorption. This work proves that appropriate ligand functionalization is promising for the removal of aqueous OPEs, which also provides a new insight for the control of OPEs pollution.

引用

页数：11

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