Mesoporous manganese Cobaltite nanocages as effective and reusable heterogeneous peroxymonosulfate activators for Carbamazepine degradation | Health & Environmental Research Online (HERO)

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Citation
Tags

HERO ID

4264747

Reference Type

Journal Article

Title

Mesoporous manganese Cobaltite nanocages as effective and reusable heterogeneous peroxymonosulfate activators for Carbamazepine degradation

Author(s)

Deng, J; Cheng, YQ; Lu, Yuan; Crittenden, JC; Zhou, ShiQ; Gao, Naiyun; Li, Jun

Year

2017

Is Peer Reviewed?

Yes

Journal

Chemical Engineering Journal
ISSN: 1385-8947

Volume

330

Page Numbers

505-517

DOI

10.1016/j.cej.2017.07.149

Web of Science Id

WOS:000414083300047

Abstract

Mesoporous MnxCo3 - O-x(4) nanocages with high cobalt content, large surface area and high pore volume were synthesized through a self-assembly method. The as-prepared MnxCo3 - O-x(4) nanocages displayed satisfactory catalytic activity toward peroxymonosulfate (PMS) and the metal ions leaching concentration could be negligible. Sulfate radical was identified as the predominant active species through radical quenching experiments and electron spin resonance spin-trapping technique. The kinetics of the oxidation process was of pseudo-first order. The increasing cobalt content in MnxCo3 - O-x(4) NCs was in favor of enhancing the decomposition of PMS. MnxCo3 - O-x(4) nanocages dosage, PMS concentration and reaction temperature put the promoting effect on the degradation, while initial CBZ concentration had the retarding impact. MnxCo3 - O-x(4) nanocages could efficiently operate over a wide pH range of 5.0-8.0. Coexisting chloride ions exerted a dual role in the decomposition of PMS and this role was concentration-dependent. XPS analysis confirmed the reversible valence equilibrium between metal ions and the recovery of surface adsorbed oxygen, which ensured their sustainable catalytic activity even after five consecutive runs. Based on the main intermediates identified by liquid chromatography-tandem mass spectrometry, a possible pathway of CBZ oxidation was proposed. The potential risk resulting from the highly toxic intermediates can also be effectively controlled by MnxCo3 - O-x(4) NCs activated PMS system.

Keywords

Pharmaceutical residues; Carbamazepine (CBZ); MnxCo3 - O-x(4) nanocages; Peroxymonosulfate (PMS); Sulfate radical (SO4 (-center dot)); Degradation