Role of in-situ electro-generated H2O2 center dot center dot center dot bridge in tetracycline degradation governed by mechanochemical Si-O anchoring Cu2+ as electron shuttle during E-peroxone process
Role of in-situ electro-generated H2O2 center dot center dot center dot bridge in tetracycline degradation governed by mechanochemical Si-O anchoring Cu2+ as electron shuttle during E-peroxone process
Li, Shangyi 1Huang, Jun 1Wang, Yujue 1Yu, Gang1
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作者信息
1. Tsinghua Univ
折叠
Abstract
The efficient mineralization of tetracycline (TC) and reaction mechanism were investigated by designing heterogeneous H2O2 center dot center dot center dot bridge linked with active sites in higher valency species. CuSi-BM60 was synthesized by anchoring Cu2+ on Si-O functional groups of MCM-48 by mechanochemical technology to assist electro-peroxone treatment (E-peroxone). Results suggested that catalysts as electron shuttle enhanced electron transfer and reactive oxygen species (ROSs) generation, showing a complete tetracycline (TC) degradation and excellent mineralization (73.2%, 60 min). Cu sites significantly raised the interaction with in-situ electro-generated H2O2, generating uneven electron cloud distribution by Si-O center dot center dot center dot Cu center dot center dot center dot HO-OH* bonding bridge, which enlarged H-O bonding length/angle near Cu and decreased orbital energy level gap. This work provided new insights into the complex of ball milling mediated Cu2+ with H2O2 accompanied by the cycle of H-O bonding cleavage and regeneration for efficient ROSs production during E-peroxone.
NSTL
Elsevier