Electron transfer in MOF-derived cobalt-magnesium oxide–carbon microsphere composite catalytic ozonation of thiamphenicol

Separation and Purification Technology(2024)

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摘要
Cobalt-magnesium oxide–carbon microsphere composite (Co-MgO-CMS), Cobalt-carbon nanosheet composite (Co-CNS), and magnesium oxide–carbon nanorod composite (MgO-CNR) were synthesized by the MOFs self-sacrificing template method. And they were used as the catalysts for catalytic ozonation of thiamphenicol (20 mg/L) in water at an initial pH of 7.0. The phase of Co-MgO-CMS is mainly composed of metallic cobalt, magnesium oxide and carbon according to X-ray diffraction and transmission electron microscopy analyses. Thiamphenicol removal efficiency is enhanced through Co-MgO-CMS catalytic ozonation (75.4 %, in 6 min), compared with those in ozonation alone (39.8 %), Co-CNS catalytic ozonation (43.2 %), MgO-CNR catalytic ozonation (65.1 %) and Mg-Co binary oxide (Mg2CoOy) catalytic ozonation (69.0 %). Self-increasing of solution pH, protonated hydroxyl groups and electron transfer on metallic Co and lattice Co2+ are advantageous for the ozone decomposition into reactive oxygen species in Co-MgO-CMS catalytic ozonation. Owing to the metallic Co in Co-MgO-CMS, the electron transfer ability of Co-MgO-CMS is better than that of Mg2CoOy according to the in situ electrochemical test. Moreover, electron transfers directly from metallic Co to ozone. While protonated hydroxyl groups are the key for electron transfer on lattice Co2+. A possible degradation pathway for thiamphenicol in Co-MgO-CMS catalytic ozonation is proposed according to the detected intermediates. This work provides insight into improvement on electron transfer ability of concerted acid-base catalyst in heterogeneous catalytic ozonation.
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关键词
MOFs self-sacrificing template method,Catalytic ozonation,Thiamphenicol,Electron transfer ability,Concerted acid-base catalyst
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