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

Zhu, Ke; Wang, Ligang; Hu, Zhuofeng; Liang, Xiaoying; Zhuang, Zechao; Li, Xin; Yang, Jiarui; Qiu, Rongliang et al. · Nat Commun · 2025

basic_science · Level V

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Abstract

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, 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 d-p 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.