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<p>Single-atom catalysts (SACs)-based advanced oxidation processes (AOPs) are an ideal green and efficient water purification technology, but intrinsic mechanisms and interface effects pose significant challenges. Herein, we have achieved precise Jahn-Teller (J-T) effect control of atomic metal-N<sub>4</sub>-C (M-N<sub>4</sub>-C: M = Mn, Fe, Co,&#xa0;and Ni) to boost the AOPs, showing a volcano-fit-like behavior. Theoretical calculation and experiments reveal the adsorption of O-O of peroxymonosulfate on the M-N<sub>4</sub>-C site, leading to the local C plane bending and inducing the intensity of the J-T effect of Mn, Fe and Co, weakening the <i>d</i>-<i>p</i> orbital hybridization ability with *HSO<sub>4</sub> intermediates for reducing the energy barrier for reactive oxygen species production. Importantly, the long-term activity of 100 h in a 20 L flow reactor indicates promising practical wastewater treatment on an industrial scale. This work presents a perspective on the rational design of tuning the metal d orbital in SACs for sustainable environmental remediation.</p>

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Curved interface-induced Jahn-Teller effect in single-atom catalysts for water purification

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2025年12月11日

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  • Ke Zhu,
  • Ligang Wang,
  • Zhuofeng Hu,
  • Xiaoying Liang,
  • Zechao Zhuang,
  • Xin Li,
  • Jiarui Yang,
  • Rongliang Qiu,
  • Dingsheng Wang,
  • Kai Yan

摘要

Single-atom catalysts (SACs)-based advanced oxidation processes (AOPs) are an ideal green and efficient water purification technology, but intrinsic mechanisms and interface effects pose significant challenges. Herein, we have achieved precise Jahn-Teller (J-T) effect control of atomic metal-N4-C (M-N4-C: M = Mn, Fe, Co, and Ni) to boost the AOPs, showing a volcano-fit-like behavior. Theoretical calculation and experiments reveal the adsorption of O-O of peroxymonosulfate on the M-N4-C site, leading to the local C plane bending and inducing the intensity of the J-T effect of Mn, Fe and Co, weakening the d-p orbital hybridization ability with *HSO4 intermediates for reducing the energy barrier for reactive oxygen species production. Importantly, the long-term activity of 100 h in a 20 L flow reactor indicates promising practical wastewater treatment on an industrial scale. This work presents a perspective on the rational design of tuning the metal d orbital in SACs for sustainable environmental remediation.