Ph-dependent degradation of diclofenac by a tunnel-structured manganese oxide

Ching Yao Hu, Yu Jung Liu, Wen Hui Kuan

Research output: Contribution to journalArticlepeer-review

Abstract

The mechanism of diclofenac (DIC) degradation by tunnel-structured γ-MnO2, with superior oxidative and catalytic abilities, was determined in terms of solution pH. High-performance liquid chromatography with mass spectroscopy (HPLC-MS) was used to identify intermediates and final products of DIC degradation. DIC can be efficiently oxidized by γ-MnO2 in an acidic medium, and the removal rate decreased significantly under neutral and alkaline conditions. The developed model can successfully fit DIC degradation kinetics and demonstrates electron transfer control under acidic conditions and precursor complex formation control mechanism under neutral to alkaline conditions, in which the pH extent for two mechanisms exactly corresponds to the distribution percentage of ionized species of DIC. We also found surface reactive sites (Srxn), a key parameter in the kinetic model for mechanism determination, to be exactly a function of solution pH and MnO2 dosage. The main products of oxidation with a highly active hydroxylation pathway on the tunnel-structured Mn-oxide are 5-iminoquinone DIC, hydroxyl-DIC, and 2,6-dichloro-N-o-tolylbenzenamine.

Original languageEnglish
Article number2203
JournalWater (Switzerland)
Volume12
Issue number8
DOIs
Publication statusPublished - Aug 2020

Keywords

  • Diclofenac (DIC)
  • Ph-dependent degradation mechanism
  • Reactive site
  • Tunnel-structured manganese oxide
  • γ-MnO

ASJC Scopus subject areas

  • Biochemistry
  • Geography, Planning and Development
  • Aquatic Science
  • Water Science and Technology

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