N-coordinated iron sites dispersed in porous carbon frameworks to activate peroxymonosulfate for efficient sulfisoxazole degradation and real hospital wastewater decontamination

• Published in: Journal of hazardous materials 2024-12, Vol.480, p.136149, Article 136149
• Main Authors: Yu, Chunxiu, Gu, Lingyun, Wu, Zelin, Chen, Kexin, Wu, Yi, Zhang, Li, Long, Quan, Shi, Hongle, Xiong, Zhaokun, Lai, Bo
• Format: Article
• Language: English
• Subjects: Carbon - chemistry; Decontamination - methods; Hospital wastewater; Hospitals; Iron - chemistry; Peroxides - chemistry; Peroxymonosulfate; Porosity; Singlet oxygen; Sulfisoxazole; Sulfisoxazole - chemistry; Wastewater - chemistry; Water Pollutants, Chemical - chemistry; Water Purification - methods; Zeolitic imidazole framework
• ISSN: 0304-3894; 1873-3336; 1873-3336
• DOI: 10.1016/j.jhazmat.2024.136149

Herein, an N-coordinated Fe site dispersed in porous carbon frameworks (Fe-NC) fabricated from zeolitic imidazolate frameworks encapsulated with iron acetylacetonate (Fe(acac)3 @ZIFs) was employed to activate peroxymonosulfate (PMS) for the attenuation of sulfisoxazole (SIZ) and treating real hospital wastewater. The constructed Fe-NC/PMS system exhibited good catalytic stability for SIZ degradation, maintaining excellent degradation performance over multiple cycles with virtually no leaching. The quenching experiments, electron paramagnetic resonance (EPR) capture analyses, and semi-quantitative measurements showed that singlet oxygen (1O2) and high-valent metal-oxo species were mainly responsible for SIZ degradation by Fe-NC/PMS. Significantly, ultra-performance liquid chromatography coupled to quadrupole time-of-flight mass spectrometry (UHPLC-Q-TOF-MS/MS) was used to trace 134 pharmaceutical contaminants in real hospital wastewater. Effective degradation was achieved for 87 % of the pharmaceutical contaminants by the Fe-NC/PMS process. Seventy-four pharmaceutical contaminants were eliminated. Taken together, this work successfully established the Fe-NC/PMS technology using the developed iron-based materials and explored its application to real hospital wastewater treatment, providing an eco-friendly and effective strategy for treating wastewater. [Display omitted] •Iron and nitrogen co-doped porous carbon framework (Fe-NC) was synthesized.•Sulfisoxazole (SIZ) was efficiently degraded in the Fe-NC/PMS system.•High-valent metal-oxo species and singlet oxygen (1O2) were major contributors.•Effective degradation of pharmaceuticals in hospital wastewater was achieved.