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<p>Although single-atom catalysts (SACs) are emerging as advanced heterogeneous catalysts for Fenton-like reactions, enhancing their performance by precisely tailoring <i>d</i>–<i>p</i> orbital hybridization remains challenging. Herein, single Cu atoms with a unique Cu-N<sub>2</sub>S asymmetric coordination structure are designed and fabricated to catalyze photo-Fenton reactions. Density functional theory (DFT) calculation reveals that strong <i>d</i>–<i>p</i> orbital hybridization elevates the HOMO energy level and promotes splitting of <i>d</i>-orbital energy levels, thereby regulating the adsorption affinity of single-atom Cu sites toward H<sub>2</sub>O<sub>2</sub> via a unique anti-<i>d</i>-band-center principle. Consequently, the Cu-N<sub>2</sub>S single sites exhibit unique photo-switching behavior, transforming the inactive sites into Fenton-active ones under light irradiation, thereby enabling sustained and enhanced generation of hydroxyl radicals for efficient degradation of various organic micropollutants. The developed photo-Fenton system achieves 98.9% removal of sulfamethoxazole, along with broad pH applicability (pH 3-11), high tolerance for complex water matrices, and exceptional durability for long-term operation. This work highlights the critical role of single-atom coordination symmetry in modulating electronic orbital structures, providing an avenue for the rational design of advanced Fenton-like catalysts.</p>

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Tailoring d–p orbital hybridization of single-atom Cu-N2S sites for enhanced photo-Fenton reaction

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2026年7月28日

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  • Minjia Yan,
  • Xiaoxin Shao,
  • Yu Li,
  • Zhixing Wang,
  • Xi-Lin Wu,
  • Linguo Lu,
  • Guo-Ping Sheng

摘要

Although single-atom catalysts (SACs) are emerging as advanced heterogeneous catalysts for Fenton-like reactions, enhancing their performance by precisely tailoring d–p orbital hybridization remains challenging. Herein, single Cu atoms with a unique Cu-N2S asymmetric coordination structure are designed and fabricated to catalyze photo-Fenton reactions. Density functional theory (DFT) calculation reveals that strong d–p orbital hybridization elevates the HOMO energy level and promotes splitting of d-orbital energy levels, thereby regulating the adsorption affinity of single-atom Cu sites toward H2O2 via a unique anti-d-band-center principle. Consequently, the Cu-N2S single sites exhibit unique photo-switching behavior, transforming the inactive sites into Fenton-active ones under light irradiation, thereby enabling sustained and enhanced generation of hydroxyl radicals for efficient degradation of various organic micropollutants. The developed photo-Fenton system achieves 98.9% removal of sulfamethoxazole, along with broad pH applicability (pH 3-11), high tolerance for complex water matrices, and exceptional durability for long-term operation. This work highlights the critical role of single-atom coordination symmetry in modulating electronic orbital structures, providing an avenue for the rational design of advanced Fenton-like catalysts.