Oxygen defective titanate nanotubes induced by iron deposition for enhanced peroxymonosulfate activation and acetaminophen degradation: Mechanisms, water chemistry effects, and theoretical calculation

Jun Ma; Long Chen; Yue Liu; Tianyuan Xu; Haodong Ji; Jun Duan; Fengbin Sun; Wen Liu

doi:10.1016/j.jhazmat.2021.126180

Oxygen defective titanate nanotubes induced by iron deposition for enhanced peroxymonosulfate activation and acetaminophen degradation: Mechanisms, water chemistry effects, and theoretical calculation

J Hazard Mater. 2021 Sep 15:418:126180. doi: 10.1016/j.jhazmat.2021.126180. Epub 2021 May 27.

Authors

Jun Ma¹, Long Chen², Yue Liu³, Tianyuan Xu⁴, Haodong Ji², Jun Duan⁵, Fengbin Sun⁶, Wen Liu²

Affiliations

¹ School of Environmental Science and engineering, Taiyuan University of Science and Technology, Taiyuan, Shanxi 030024, China.
² The Key Laboratory of Water and Sediment Sciences, Ministry of Education, College of Environmental Sciences and Engineering, Peking University, Beijing 100871, China; State Environmental Protection Key Laboratory of All Material Fluxes in River Ecosystems, Peking University, Beijing 100871, China.
³ The Key Laboratory of Water and Sediment Sciences, Ministry of Education, College of Environmental Sciences and Engineering, Peking University, Beijing 100871, China.
⁴ School of Resource and Geosciences, China University of Mining and Technology, Xuzhou, Jiangsu 221116, China.
⁵ The Key Laboratory of Water and Sediment Sciences, Ministry of Education, College of Environmental Sciences and Engineering, Peking University, Beijing 100871, China; State Environmental Protection Key Laboratory of All Material Fluxes in River Ecosystems, Peking University, Beijing 100871, China. Electronic address: duanjun@pku.edu.cn.
⁶ The Key Laboratory of Water and Sediment Sciences, Ministry of Education, College of Environmental Sciences and Engineering, Peking University, Beijing 100871, China; State Environmental Protection Key Laboratory of All Material Fluxes in River Ecosystems, Peking University, Beijing 100871, China. Electronic address: fengbintamu@163.com.

PMID: 34102367
DOI: 10.1016/j.jhazmat.2021.126180

Abstract

The large consumption of acetaminophen (APAP) worldwide and unsatisfactory treatment efficiencies by conventional wastewater treatment processes give rise to the seeking of new technology for its effective removal. Herein, we proposed a facile one-step hydrothermal method to synthesize defective iron deposited titanate nanotubes (Fe/TNTs) for peroxymonosulfate (PMS) activation and APAP degradation. The retarded first-order reaction rate of APAP degradation by Fe/TNTs was 5.1 times higher than that of neat TNTs. Characterizations indicated iron deposition effectively induced oxygen vacancies and Ti³⁺, facilitating the electrical conductivity and PMS binding affinity of Fe/TNTs. Besides, oxygen vacancies could act as an electron mediator through PMS activation by iron. Moreover, the formation of Fe-O-Ti bond facilitated the synergistic redox coupling between Fe and Ti, further enhancing the PMS activation. SO₄^•- was the major radical, causing C-N bond cleavage and decreasing the overall toxicity. In contrast, APAP degradation by neat TNTs-PMS system mainly works through nonradical reaction. The Fe/TNTs activated PMS showed desired APAP removal under mild water chemistry conditions and good reusability. This work is expected to expand the potential application of titanate nanomaterials for PMS activation, and shed light on facile synthesis of oxygen defective materials for sulfate-radical-based advanced oxidation processes.

Keywords: Acetaminophen; Density functional theory; Oxygen vacancies; Peroxymonosulfate; Titanate nanotubes.

Publication types

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

MeSH terms

Acetaminophen* / toxicity
Iron
Nanotubes*
Oxygen
Peroxides
Water

Substances

Peroxides
Water
peroxymonosulfate
Acetaminophen
Iron
Oxygen