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

2021 
Abstract In the peroxone process (O3/H2O2), OH yield ratio with respect to O3 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. 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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