Sulfide-modified zero-valent iron activated periodate for sulfadiazine removal: Performance and dominant routine of reactive species production

Chen Ling; Shuai Wu; Jiangang Han; Tailu Dong; Changqing Zhu; Xiuwen Li; Lijie Xu; Ying Zhang; Minghua Zhou; Yuwei Pan

doi:10.1016/j.watres.2022.118676

Sulfide-modified zero-valent iron activated periodate for sulfadiazine removal: Performance and dominant routine of reactive species production

Water Res. 2022 Jul 15:220:118676. doi: 10.1016/j.watres.2022.118676. Epub 2022 May 26.

Authors

Chen Ling¹, Shuai Wu¹, Jiangang Han¹, Tailu Dong¹, Changqing Zhu², Xiuwen Li², Lijie Xu¹, Ying Zhang³, Minghua Zhou⁴, Yuwei Pan⁵

Affiliations

¹ College of Biology and the Environment, Nanjing Forestry University, Nanjing 210037, China.
² State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210023, China.
³ Key Laboratory of Pollution Process and Environmental Criteria, Ministry of Education, College of Environmental Science and Engineering, Nankai University, Tianjin 300350, China. Electronic address: [email protected].
⁴ Key Laboratory of Pollution Process and Environmental Criteria, Ministry of Education, College of Environmental Science and Engineering, Nankai University, Tianjin 300350, China. Electronic address: [email protected].
⁵ College of Biology and the Environment, Nanjing Forestry University, Nanjing 210037, China. Electronic address: [email protected].

PMID: 35640509
DOI: 10.1016/j.watres.2022.118676

Abstract

In this work, sulfide-modified zero-valent iron (S-Fe⁰) was used to activate periodate (IO₄^-, PI) for sulfadiazine (SDZ) removal. 60 μM SDZ could be completely removed within only 1 min by S-Fe⁰/PI process. Compared with other oxidants including H₂O₂, peroxymonosulfate (PMS), peroxydisulfate (PDS), S-Fe⁰ activated PI exhibited better performance for SDZ removal but with lower Fe leaching. Compared with Fe⁰/PI process, S-Fe⁰/PI process could reduce more than 80% Fe⁰ and PI dosage. Inorganic ions and nature organic matters had negligible effect on SDZ removal in S-Fe⁰/PI system inducing its good SDZ removal efficiency in natural fresh water. 80.2% SDZ still could be removed within 2 min after 7th run. S-Fe⁰/PI process also exhibited 2.5 - 20.1 folds enhancement for various pollutants removal compared with Fe⁰/PI process. Scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), electrochemical tests, and density functional theory (DFT) calculation were conducted to confirm the presence of sulfurs could enhance the reactivity of S-Fe⁰ thus increased the efficiency of PI activation for antibiotics removal. Electron paramagnetic resonance spectroscopy (EPR) tests, radical quenching experiments, quantitative detection and DFT calculation were performed to illustrate the role of multiple reactive species in SDZ removal and the dominant pathway of multiple reactive species production. IO₃^·, ^·OH, O₂^-·, ¹O₂, Fe^IV, and SO₄^·- all participated in SDZ removal. ^·OH played the major role in SDZ removal and the dominant routine of ^·OH production was IO₄^- → O₂^-· → H₂O₂ → ^·OH. Meanwhile, S-Fe⁰/PI process could efficiently mineralize SDZ and reduce the toxicity. Comparison with other PI activation approaches and SDZ treatment techniques further demonstrated S-Fe⁰ was an efficient catalyst for PI activation and present study process was a promising approach for antibiotics removal.

Keywords: Density functional theory; Periodate; Reactive species; Sulfide-modified zero-valent iron.

MeSH terms

Anti-Bacterial Agents
Hydrogen Peroxide
Iron* / chemistry
Periodic Acid
Sulfadiazine* / chemistry
Sulfides

Substances

Anti-Bacterial Agents
Sulfides
Sulfadiazine
Periodic Acid
metaperiodate
Hydrogen Peroxide
Iron