The synergistic interactions of reaction parameters in heterogeneous peroxymonosulfate oxidation: Reaction kinetic and catalytic mechanism

Xiaonan Hu; Yang Ye; Yanxi Chen; Min Liu; Wenchao Zhang; Mingshan Zhu

doi:10.1016/j.jhazmat.2021.126841

The synergistic interactions of reaction parameters in heterogeneous peroxymonosulfate oxidation: Reaction kinetic and catalytic mechanism

J Hazard Mater. 2022 Jan 5:421:126841. doi: 10.1016/j.jhazmat.2021.126841. Epub 2021 Aug 6.

Authors

Xiaonan Hu¹, Yang Ye¹, Yanxi Chen¹, Min Liu², Wenchao Zhang³, Mingshan Zhu⁴

Affiliations

¹ Guangdong Key Laboratory of Environmental Pollution and Health, School of Environment, Jinan University, Guangzhou 511443, PR China.
² School of Physics and Electronics, Central South University, Changsha 410083, PR China.
³ School of Metallurgy and Environment, Central South University, Changsha 410083, PR China.
⁴ Guangdong Key Laboratory of Environmental Pollution and Health, School of Environment, Jinan University, Guangzhou 511443, PR China. Electronic address: zhumingshan@jnu.edu.cn.

PMID: 34388915
DOI: 10.1016/j.jhazmat.2021.126841

Abstract

The reaction parameters including catalyst dosage, oxidant amount, initial contaminant concentration and pH etc. play the crucial roles in the heterogeneous persulfate oxidation processes, while the synergistic interactions among these reaction parameters are still obscure. We herein took an efficient heterogeneous persulfate oxidation system "bimetallic Mn_xCo_3-xO₄ solid solution (MnCo) activated peroxymonosulfate (PMS)" for carbamazepine (CBZ) removal from water. MnCo/PMS system exhibited outstanding performance that CBZ was completely removed within 10 min. The CBZ degradation performance was ascribed to the radical oxidation of SO₄^·- and O₂·^-, the nonradical oxidation of ¹O₂, the redox cycles between Mn and Co species and synergistic interactions among MnCo, PMS and CBZ. By monotonously or synchronously adjusting the MnCo dosage, PMS amount and initial CBZ concentration, the inherent connections of different reaction parameters were established. Strong and different synergistic interactions between MnCo and PMS, and among MnCo, PMS and CBZ, were existed due to the formation of three different reaction modes when reaction parameters met certain conditions. The features of the modes were "two-stage, the following auto-deceleration", "one-stage, constant velocity" and "two-stage, the following auto-acceleration". This discovery may provide new insights into the synergistic interactions of reaction parameters in advanced oxidation processes for wastewater treatment.

Keywords: Carbamazepine; Mn(x)Co(3−x)O(4) solid solution; Peroxymonosulfate activation; Reaction parameters; Synergistic interactions.

Publication types

Research Support, Non-U.S. Gov't

MeSH terms

Catalysis
Oxidation-Reduction
Peroxides*
Water Purification*

Substances

Peroxides
peroxymonosulfate