Spin-selection-favored peroxymonosulfate activation on reaction-induced Co–N1O2 sites enables 1O2-biased yet radical-parallel oxidation

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ID: 315519
2026
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Abstract
Abstract Transformations in metal coordination environments, particularly their impact on spin-state transitions, remain underexplored in peroxymonosulfate (PMS)-based advanced oxidation processes (AOPs). In this study, we synthesize a Co1/C3N5 single-atom catalyst using a coordination–recrystallization strategy followed by argon pyrolysis. The Co–N2O1 sites evolve to Co–N1O2 upon PMS activation, enabling spin-selection-favored activation and efficient pollutant degradation. The evolved site enables spin-selection-favored PMS activation that co-generates sulfate radicals (·SO4⁻) and singlet oxygen (1O2), operating in a 1O2-biased yet radical-parallel regime. Within this regime, Co1/C3N5 achieves a 5.3-fold increase in the pseudo-first-order rate constant (kapp) for oxytetracycline degradation relative to pristine C3N5 under identical conditions, and it consistently outperforms more than 30 state-of-the-art PMS-based catalysts. The catalyst further exhibits broad-spectrum activity toward structurally diverse antibiotics and dyes, while maintaining durability in matrix-rich waters and under continuous-flow operation. Overall, this work links reaction-induced single-site evolution to spin-aware oxygen transfer, providing concise design guidance for selective and robust PMS-activated AOP catalysts.
Reference Key
openalex_W7163169346 Use this key to autocite in the manuscript while using SciMatic Manuscript Manager or Thesis Manager
Authors J W Zhang, Guojia Yu, Qi Zhang, Haoran Wei, Wei Zhao, S Y Li, Zhiyao Duan, Sihui Zhan
Journal national science review
Year 2026
DOI
10.1093/nsr/nwag334
URL
https://doi.org/10.1093/nsr/nwag334
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