ZIF-8 assisted synthesis of magnetic core-shell Fe3O4@CuS nanoparticles for efficient sulfadiazine degradation via H2O2 activation: Performance and mechanism

Haojie Zhang; Chan Zhou; Hanxuan Zeng; Huiying Wu; Lingfang Yang; Lin Deng; Zhou Shi

doi:10.1016/j.jcis.2021.03.057

ZIF-8 assisted synthesis of magnetic core-shell Fe₃O₄@CuS nanoparticles for efficient sulfadiazine degradation via H₂O₂ activation: Performance and mechanism

J Colloid Interface Sci. 2021 Jul 15:594:502-512. doi: 10.1016/j.jcis.2021.03.057. Epub 2021 Mar 17.

Authors

Haojie Zhang¹, Chan Zhou¹, Hanxuan Zeng¹, Huiying Wu¹, Lingfang Yang¹, Lin Deng², Zhou Shi³

Affiliations

¹ Key Laboratory of Building Safety and Energy Efficiency, Ministry of Education, Department of Water Engineering and Science, College of Civil Engineering, Hunan University, Changsha 410082, China.
² Key Laboratory of Building Safety and Energy Efficiency, Ministry of Education, Department of Water Engineering and Science, College of Civil Engineering, Hunan University, Changsha 410082, China. Electronic address: lindeng@hnu.edu.cn.
³ Key Laboratory of Building Safety and Energy Efficiency, Ministry of Education, Department of Water Engineering and Science, College of Civil Engineering, Hunan University, Changsha 410082, China. Electronic address: shiz61@hnu.edu.cn.

PMID: 33774406
DOI: 10.1016/j.jcis.2021.03.057

Abstract

A novel magnetic core-shell Fe₃O₄@CuS have been successfully synthesized by chemical etching and cation exchange method using Zeolitic imidazolate frameworks (ZIF) as the template. The morphology and microstructural properties characterization indicated that Fe₃O₄@CuS nanoparticles were rhombic dodecahedral shape, highly stable, and magnetic with a large specific surface area (772.20 m²/g). The catalytic activity of Fe₃O₄@CuS was assessed on sulfadiazine (SDZ) degradation by H₂O₂ activation. Multi-factors affecting the SDZ removal was adequately investigated. Approximately 93.2% SDZ (50 μM) was removed with 0.2 g/L Fe₃O₄@CuS and 5 mM H₂O₂ in 90 min. In particular, Fe₃O₄@CuS exhibited a quality catalytic performance within a wide pH range of 3.0-11.0. Radical scavenger tests and electron paramagnetic resonance (EPR) analysis confirmed that •O₂^-, •OH, and ¹O₂ all contributed to the SDZ degradation, and •OH played the dominant role. Meanwhile, mechanism investigation suggested that the effective catalytic activity of Fe₃O₄@CuS could be ascribed to the sulphur-enhanced copper-based Fenton reaction on the CuS shell, sulphur-enhanced iron-based Fenton reaction on the Fe₃O₄ core, and the effective electron transfer between the shell and core. Finally, the possible SDZ degradation pathways were further proposed on the basis of the intermediates identification. This work put forward a new strategy to synthesize magnetic core-shell Fe₃O₄@CuS using ZIF-8 as the template with outstanding performance for H₂O₂ activation to degrade SDZ.

Keywords: Core-shell; Fe(3)O(4)@CuS; Heterogeneous catalysis; Hydrogen peroxide; Sulfadiazine degradation.