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

He Liang, Ruiping Liu, Chengzhi Hu, Xiaoqiang An, Xiwang Zhang, Huijuan Liu, Jiuhui Qu

Research output: Contribution to journalArticleResearchpeer-review

8 Citations (Scopus)

Abstract

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 Matérial 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 ciprofloxacin (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. ·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.

Original languageEnglish
Article number124692
Number of pages10
JournalJournal of Hazardous Materials
Volume406
DOIs
Publication statusPublished - 15 Mar 2021

Keywords

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

Cite this