Synergistic effect of dual sites on bimetal-organic frameworks for highly efficient peroxide activation

被引：95

作者：

Liang, He ^{[1
,2
]}

Liu, Ruiping ^{[3
]}

Hu, Chengzhi ^{[1
,5
]}

An, Xiaoqiang ^{[3
]}

Zhang, Xiwang ^{[4
]}

Liu, Huijuan ^{[3
]}

Qu, Jiuhui ^{[1
,3
,5
]}

机构：

[1] Chinese Acad Sci, Res Ctr Ecoenvironm Sci, State Key Lab Environm Aquat Chem, Beijing 100085, Peoples R China

[2] Northeast Normal Univ, Sch Environm, Changchun 130117, Jilin, Peoples R China

[3] Tsinghua Univ, Ctr Water & Ecol, Sch Environm, State Key Joint Lab Environm Simulat & Pollut Con, Beijing 100084, Peoples R China

[4] Monash Univ, Dept Chem Engn, Clayton, Vic 3800, Australia

[5] Univ Chinese Acad Sci, Beijing 100039, Peoples R China

来源：

JOURNAL OF HAZARDOUS MATERIALS | 2021年 / 406卷

基金：

中国国家自然科学基金;

关键词：

Fenton-like reactions; Bimetal-organic frameworks; Dual site engineering; Ciprofloxacin; Reaction mechanism;

D O I：

10.1016/j.jhazmat.2020.124692

中图分类号：

X [环境科学、安全科学];

学科分类号：

08 ; 0830 ;

摘要：

Active site engineering is of significant importance for developing high activity metal-organic frameworks (MOFs) for catalytic applications. Herein, we develop a one-pot strategy to construct bimetal organic frameworks with Fe-Co dual sites for Fenton-like catalysis. Density functional theory (DFT) demonstrated that the introducing Co heteroatoms into MIL-101(Fe) (MIL represents Material Institute Lavoisier) was favorable for the formation of electron-deficient centers around benzene rings and electron-rich centers around Fe/Co. This synergistic effect could effectively decrease the energy barrier of H2O2 activation. Due to the facilitated charge transfer in the coordinated structures, MIL-101(Fe,Co) with engineered dual sites exhibited exceptionally high efficiency for the degradation of cipmfloxacin (CIP). The reaction rate of MIL-101(Fe,Co)/H2O2 system was 0.12 min(-1), which was nearly 7.5 times higher than that of pristine MIL-101(Fe). The reaction mechanism of heterogeneous Fenton-like catalysis was fundamentally investigated by series of in-situ techniques, such as DRIFTS and Raman. center dot OH radicals generated by H2O2 activation endowed the inspiring ability of MIL-101(Fe,Co) for water decontamination. This work offers a facile principle of exploring MOFs-based Fenton-like catalysts with a wide working pH range for environmental applications.

引用

页数：10