4.8 Article

The mechanism of Metal-H2O2 complex immobilized on MCM-48 and enhanced electron transfer for effective peroxone ozonation of sulfamethazine

Journal

APPLIED CATALYSIS B-ENVIRONMENTAL
Volume 280, Issue -, Pages -

Publisher

ELSEVIER
DOI: 10.1016/j.apcatb.2020.119453

Keywords

Peroxone; Electron transfer; Complex species; Co10Ce10@MCM-48; SMT

Funding

  1. National Natural Science Foundation of China [51978288]
  2. Major Science and Technology Program for Water Pollution Control and Treatment in China [2017ZX07202-004]
  3. Innovation Project of Graduate School of South China Normal University [2019LKXM005]

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In the peroxone process, the Co-Ce synergistic effect enhances the production of (OH)-O-center dot, leading to superior performance of SMT mineralization by Co10Ce10@MCM-48 catalysts.
In the peroxone process (O-3/H2O2), (OH)-O-center dot yield ratio with respect to O-3 consumption was low due to the competition experiments. Singular effectiveness of Co-Ce as a supporting ligand in the interface of ozone-H2O2-catalysts and related complexes formed on catalysts enhanced the electron transfer between ozone chain reaction and various chemical state of Ce/Co. A computationally determined stereochemical structure corroborated that the Co-Ce synergistic effect led to the region around Co atom (electron donor) with low Gibbs free energy to form (OH)-O-center dot. Meanwhile, reactive oxygen species (ROSs) were tend to attack the sites with very negative natural population charge or high frontier electron density (FED) values of sulfamethazine (SMT) by LC-MS/MS and density functional theory (DFT) calculations. Benefiting from the unique superoxide complexes and synergetic effect of Co-Ce, the Co10Ce10@MCM-48 catalysts showed superior performance of SMT mineralization (64.1 %, 120 min), which resolved the low-efficient ROSs generation in bare peroxone reaction.

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