Introduction of oxygen vacancy to manganese ferrite by Co substitution for enhanced peracetic acid activation and 1O2 dominated tetracycline hydrochloride degradation under microwave irradiation

Shuo Li; Yalun Yang; Heshan Zheng; Yongjie Zheng; Chuan-Shu He; Bo Lai; Jun Ma; Jun Nan

doi:10.1016/j.watres.2022.119176

Introduction of oxygen vacancy to manganese ferrite by Co substitution for enhanced peracetic acid activation and ¹O₂ dominated tetracycline hydrochloride degradation under microwave irradiation

Water Res. 2022 Oct 15:225:119176. doi: 10.1016/j.watres.2022.119176. Epub 2022 Sep 28.

Authors

Shuo Li¹, Yalun Yang², Heshan Zheng², Yongjie Zheng², Chuan-Shu He³, Bo Lai⁴, Jun Ma⁵, Jun Nan⁵

Affiliations

¹ College of Chemistry and Chemical Engineering, Qiqihar University, Qiqihar, 161006, China; Urban Water Resources Development and Northern National Engineering Research Center, Harbin, 150090, China; School of Environment, Harbin Institute of Technology, Harbin, 150090, China.
² College of Chemistry and Chemical Engineering, Qiqihar University, Qiqihar, 161006, China.
³ Department of Environmental Science and Engineering, School of Architecture and Environment, Sichuan University, Chengdu 610065, China. Electronic address: hecs@scu.edu.cn.
⁴ Department of Environmental Science and Engineering, School of Architecture and Environment, Sichuan University, Chengdu 610065, China. Electronic address: laibo@scu.edu.cn.
⁵ Urban Water Resources Development and Northern National Engineering Research Center, Harbin, 150090, China; School of Environment, Harbin Institute of Technology, Harbin, 150090, China.

PMID: 36191527
DOI: 10.1016/j.watres.2022.119176

Abstract

High microwave-response cobalt-substituted manganese ferrite (CMFO-0.5) was successfully synthesized as a heterogeneous catalyst for efficient peracetic acid (PAA) activation and tetracycline hydrochloride (TCH) degradation with singlet oxygen (¹O₂) as the dominated reactive oxidized species (ROS). The removal efficiency of TCH could reach 98.16% within 6 min under microwave irradiation when the CMFO-0.5 was added at 20 mg/L. It's found that the Co substitution could produce the oxygen vacancies (OVs), improve the microwave (MW) absorbing performance and enhance the internal electron transfer efficiency of materials. The phenomenon why ¹O₂ as the dominated ROS rather than hydroxyl radical (•OH) and organic radicals (R-O•) would be explained by the following aspects: the oxygen adsorbed on the OVs can accept the electron transformed from PAA to form superoxide radical (•O₂^-), which will disproportionate to form ¹O₂; the energy generated by the non-thermal effect of MW can dissociate PAA to generate peroxy-group for ¹O₂ generation. Furthermore, the possible TCH degradation pathways were proposed based on DFT theory calculations and product identification, and the toxicity predictions of the degradation products were also performed by the Ecological Structure-Activity Relationship Model (ECOSAR) software. Additionally, the decrease of acute toxicity of treated TCH, excellent stability and strong resistance towards water matrix fully demonstrate the superiority of the proposed system for practical application in wastewater treatment.

Keywords: Cobalt-substituted manganese ferrite; Microwave; Oxygen vacancies; Peracetic acid activation; Singlet oxygen.

MeSH terms

Cobalt
Hydroxyl Radical
Microwaves
Oxidation-Reduction
Oxygen
Peracetic Acid*
Reactive Oxygen Species
Singlet Oxygen
Superoxides
Tetracycline*
Water

Substances

Tetracycline
Peracetic Acid
manganese ferrite
Oxygen
Hydroxyl Radical
Singlet Oxygen
Reactive Oxygen Species
Superoxides
cobalt ferrite
Cobalt
Water