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<p>Single-atom catalysts (SACs) have emerged as promising candidates for peroxymonosulfate (PMS)-based advanced oxidation processes (AOPs), offering high activity and atomic efficiency for environmental remediation. However, achieving SACs with robust structural stability, wide pH tolerance, and resistance to matrix interference remains a formidable challenge. Here, we report a loading-controlled strategy to construct oxygen-bridged bimetallic Ni-O-Ni sites on a carbon nitride framework via a coordination-recrystallization-static-air pyrolysis route. The Ni loading critically modulates the local coordination environment: while moderate loading promotes the formation of active Ni-O-Ni moieties, excess Ni leads to the emergence of less active Ni-N<sub>3</sub> configurations. The optimized Ni-O-Ni SAC exhibits exceptional catalytic performance for PMS activation, achieving 5.9- and 28.9-fold enhancements in the degradation of oxytetracycline (OTC) and rhodamine B (RhB), respectively, relative to pristine C<sub>3</sub>N<sub>5</sub>, and surpassing all 41 previously reported catalysts for OTC or RhB degradation. The catalyst also demonstrates excellent operational stability across a wide pH range (2.0–11.0) and strong resistance to common anionic interferences. Mechanistic investigations, including radical quenching experiments and density functional theory (DFT) calculations, reveal that the Ni-O-Ni site facilitates the selective generation of singlet oxygen (<sup>1</sup>O<sub>2</sub>) and superoxide radicals (·O<Stack> <sub>2</sub> <sup>-</sup> </Stack>) by lowering activation barriers. This work highlights the critical role of metal-oxygen-metal motifs in dictating reaction pathways and offers a versatile design principle for next-generation AOP catalysts toward sustainable water treatment.</p>

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Tailored Ni-O-Ni dimers drive radical/non-radical pathways in peroxymonosulfate oxidation processes to remove emerging contaminants

  • 期刊论文

  • 发表日期：

    2025年9月28日

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  • Guojia Yu,
  • Junlei Zhang,
  • Haoran Wei,
  • Wei Zhao,
  • Mingshan Zhu

摘要

Single-atom catalysts (SACs) have emerged as promising candidates for peroxymonosulfate (PMS)-based advanced oxidation processes (AOPs), offering high activity and atomic efficiency for environmental remediation. However, achieving SACs with robust structural stability, wide pH tolerance, and resistance to matrix interference remains a formidable challenge. Here, we report a loading-controlled strategy to construct oxygen-bridged bimetallic Ni-O-Ni sites on a carbon nitride framework via a coordination-recrystallization-static-air pyrolysis route. The Ni loading critically modulates the local coordination environment: while moderate loading promotes the formation of active Ni-O-Ni moieties, excess Ni leads to the emergence of less active Ni-N3 configurations. The optimized Ni-O-Ni SAC exhibits exceptional catalytic performance for PMS activation, achieving 5.9- and 28.9-fold enhancements in the degradation of oxytetracycline (OTC) and rhodamine B (RhB), respectively, relative to pristine C3N5, and surpassing all 41 previously reported catalysts for OTC or RhB degradation. The catalyst also demonstrates excellent operational stability across a wide pH range (2.0–11.0) and strong resistance to common anionic interferences. Mechanistic investigations, including radical quenching experiments and density functional theory (DFT) calculations, reveal that the Ni-O-Ni site facilitates the selective generation of singlet oxygen (1O2) and superoxide radicals (·O 2 - ) by lowering activation barriers. This work highlights the critical role of metal-oxygen-metal motifs in dictating reaction pathways and offers a versatile design principle for next-generation AOP catalysts toward sustainable water treatment.