Enhanced Degradation of Antibiotic by Peroxydisulfate Catalysis with CuO@CNT: Simultaneous 1O2 Oxidation and Electron-Transfer Regime

Jia Liu; Chao Ding; Sicheng Gong; Kun Fu; Huiping Deng; Jun Shi

doi:10.3390/molecules27207064

Molecules (Oct 2022)

Enhanced Degradation of Antibiotic by Peroxydisulfate Catalysis with CuO@CNT: Simultaneous 1O2 Oxidation and Electron-Transfer Regime

Jia Liu,
Chao Ding,
Sicheng Gong,
Kun Fu,
Huiping Deng,
Jun Shi

Affiliations

Jia Liu: Key Laboratory of Yangtze River Water Environment Ministry of Education, Shanghai Institute of Pollution Control and Ecological Security, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, China
Chao Ding: Key Laboratory of Yangtze River Water Environment Ministry of Education, Shanghai Institute of Pollution Control and Ecological Security, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, China
Sicheng Gong: Key Laboratory of Yangtze River Water Environment Ministry of Education, Shanghai Institute of Pollution Control and Ecological Security, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, China
Kun Fu: Key Laboratory of Yangtze River Water Environment Ministry of Education, Shanghai Institute of Pollution Control and Ecological Security, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, China
Huiping Deng: Key Laboratory of Yangtze River Water Environment Ministry of Education, Shanghai Institute of Pollution Control and Ecological Security, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, China
Jun Shi: Key Laboratory of Yangtze River Water Environment Ministry of Education, Shanghai Institute of Pollution Control and Ecological Security, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, China

DOI: https://doi.org/10.3390/molecules27207064
Journal volume & issue: Vol. 27, no. 20
p. 7064

Abstract

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The nonradical process in the peroxydisulfate (PDS) oxidation system is a promising method for antibiotic removal in water. In this study, CuO@CNT was successfully synthesized by a facile approach to catalyze PDS. The removal efficiency of the antibiotic sulfamethoxazole (SMX) was 90.6% in 50 min, and the stoichiometric efficiency (ΔSMX/ΔPDS) was 0.402. The very different degradation efficiency of common organic contaminants revealed the selective oxidation of the surveyed system. The process of 1O2 oxidation and the electron-transfer regime was exhibited by chemical quenching tests, electron paramagnetic resonance (EPR) determination, a UV–vis spectrophotometer, X-ray photoelectron spectroscopy (XPS) detection, and cyclic voltammetry (CV) measurements. Sustainable catalysis was promoted by the circulation between the surface electron-rich centers of Cu(II) and Cu(III). Dissolved oxygen (DO) and a metastable Cu(III) intermediate contributed to the generation of 1O2. Still, a portion of SMX was removed by the mildly activated PDS. Moreover, the influence factors (pH, dosage, water matrix) were examined, and suppressions were acceptable by common anions and real water. Distinguished from the radical process, unique intermediate products were ascertained via the theoretical calculation and liquid chromatography–mass spectrometry (LC-MS) detection. Furthermore, CuO@CNT showed a satisfactory activation ability in the cycling experiments. Overall, this study developed CNT to be a supporter of CuO, unveiled the mechanism of catalysis, and evaluated the application potential of the nonradical process.

Published in Molecules

ISSN: 1420-3049 (Online)
Publisher: MDPI AG
Country of publisher: Switzerland
LCC subjects: Science: Chemistry: Organic chemistry
Website: http://www.mdpi.com/journal/molecules

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