Spin-selection-favored peroxymonosulfate activation on reaction-induced Co–N1O2 sites enables 1O2-biased yet radical-parallel oxidation
4 affiliations
- 1School of Materials Science and Engineering, Northwestern Polytechnical University , Xi’an 710072 ,
- 2School of Ecology and Environmental Science, Institute for Ecological Research and Pollution Control of Plateau Lakes, Yunnan University , Kunming 650500 ,
- 3National Engineering Research Center for Marine Aquaculture, Zhejiang Key Laboratory of Petrochemical Environmental Pollution Control, Zhejiang Ocean University , Zhoushan 316000 ,
- 4School of Environmental Science & Engineering, Tianjin University , Tianjin 300350 ,
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 water 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.
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BibTeX
@article{zhang2026spinselectionfavored,
title = {{Spin-selection-favored peroxymonosulfate activation on reaction-induced Co–N1O2 sites enables 1O2-biased yet radical-parallel oxidation}},
author = {J W Zhang and Guojia Yu and Qi Zhang and Haoran Wei and Wei Zhao and S Y Li and Zhiyao Duan and Sihui Zhan},
journal = {National Science Review},
year = {2026},
month = jun,
doi = {10.1093/nsr/nwag334},
url = {https://doi.org/10.1093/nsr/nwag334},
note = {CC BY},
}
RIS
TY - JOUR
TI - Spin-selection-favored peroxymonosulfate activation on reaction-induced Co–N1O2 sites enables 1O2-biased yet radical-parallel oxidation
AU - J W Zhang
AU - Guojia Yu
AU - Qi Zhang
AU - Haoran Wei
AU - Wei Zhao
AU - S Y Li
AU - Zhiyao Duan
AU - Sihui Zhan
PY - 2026
DA - 2026/06/02
JO - National Science Review
DO - 10.1093/nsr/nwag334
UR - https://doi.org/10.1093/nsr/nwag334
AB - 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 water 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.
SN - 2053-714X
SN - 2095-5138
ER -