Homogeneous to heterogeneous redox mediator enhancing ferrate(VI) oxidation of sulfamethoxazole: Role of ferrate(VI) activation and electron shuttle

被引：0

作者：

Wang D. ^{[1
,2
]}

Yu Y. ^{[1
]}

He J. ^{[1
]}

Zhang J. ^{[1
]}

Yang C. ^{[3
]}

Ma J. ^{[1
]}

机构：

[1] School of Environment, Harbin Institute of Technology, Harbin

[2] Department of Civil and Environmental Engineering, The Hong Kong University of Science and Technology

[3] College of Environment and Ecology, Chongqing University, Chongqing

来源：

Chemosphere | 2024年 / 362卷

基金：

中国国家自然科学基金;

关键词：

ABNO; Electron shuttle; Emerging contaminants; Ferrate; Heterogeneous catalysis; Nitroxide redox mediator;

D O I：

10.1016/j.chemosphere.2024.142752

中图分类号：

学科分类号：

摘要：

Ferrate (Fe(VI)) is a promising oxidant for water remediation, yet it has limited reactivity towards certain recalcitrant but important emerging contaminants, such as sulfamethoxazole. Here, this study demonstrates that nitroxide redox mediators, specifically 9-azabicyclo[3.3.1]nonasne N-oxyl (ABNO), can catalyze Fe(VI) reaction with sulfamethoxazole by functioning both as Fe(VI) activator and electron shuttle. The underlying mechanism is explained as: (i) Fe(VI) activation: a series of one-electron transfers between Fe(VI) and ABNO produces highly reactive Fe(V)/Fe(IV) and ABNO+; (ii) electron shuttle: the newly formed active ABNO+ reacts with the sulfamethoxazole, contributing to its removal. Concurrently, ABNOH is generated and subsequently converted back to ABNO by reactive species, thereby completing the redox cycle. The as-developed heterogeneous redox mediator, ABNO@SiO2, retained its catalytic properties and effectively catalyzed Fe(VI) to remove sulfamethoxazole at environmentally relevant pH levels. © 2024 Elsevier Ltd

引用

共 28 条

[1]

Canas A.I., Camarero S., Laccases and their natural mediators: biotechnological tools for sustainable eco-friendly processes, Biotechnol. Adv., 28, 6, pp. 694-705, (2010)

[2]

Dong H.Y., Qiang Z.M., Lian J.F., Qu J.H., Promoted oxidation of diclofenac with ferrate (Fe(VI)): role of ABTS as the electron shuttle, J. Hazard Mater., 336, pp. 65-70, (2017)

[3]

Huang Z.-S., Wang L., Liu Y.-L., Zhang H.-Y., Zhao X.-N., Bai Y., Ma J., Ferrate self-decomposition in water is also a self-activation process: role of Fe (V) species and enhancement with Fe (III) in methyl phenyl sulfoxide oxidation by excess ferrate, Water Res., 197, (2021)

[4]

Kurniawati S., Nicell J.A., Efficacy of mediators for enhancing the laccase-catalyzed oxidation of aqueous phenol, Enzym. Microb. Technol., 41, 3, pp. 353-361, (2007)

[5]

Lee Y., Kissner R., von Gunten U., Reaction of ferrate(VI) with ABTS and self-decay of ferrate(VI): kinetics and Mechanisms, Environ. Sci. Technol., 48, 9, pp. 5154-5162, (2014)

[6]

Luo M., Zhou H., Zhou P., Lai L., Liu W., Ao Z., Yao G., Zhang H., Lai B., Insights into the role of in-situ and ex-situ hydrogen peroxide for enhanced ferrate (VI) towards oxidation of organic contaminants, Water Res., 203, (2021)

[7]

Luo M.F., Zhang H., Zhou P., Xiong Z.K., Huang B.K., Peng J.L., Liu R., Liu W., Lai B., Efficient activation of ferrate(VI) by colloid manganese dioxide: comprehensive elucidation of the surface-promoted mechanism, Water Res., 215, (2022)

[8]

Luo Q., Wang Z.Y., Feng M.B., Chiang D.R., Woodward D., Liang S.T., Lu J.H., Huang Q.G., Factors controlling the rate of perfluorooctanoic acid degradation in laccase-mediator systems: the impact of metal ions, Environ. Pollut., 224, pp. 649-657, (2017)

[9]

Schwarzenbach R.P., Escher B.I., Fenner K., Hofstetter T.B., Johnson C.A., von Gunten U., Wehrli B., The challenge of micropollutants in aquatic systems, Science, 313, 5790, pp. 1072-1077, (2006)

[10]

Shao B., Dong H., Sun B., Guan X., Role of ferrate (IV) and ferrate (V) in activating ferrate (VI) by calcium sulfite for enhanced oxidation of organic contaminants, Environ. Sci. Technol., 53, 2, pp. 894-902, (2018)

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