Curved interface-induced Jahn-Teller effect in single-atom catalysts for water purification
Ke Zhu, François Maréchal, Zhuofeng Hu, Xiaoying Liang, Zechao Zhuang, Xin Li, Jiarui Yang, Rongliang Qiu, Dingsheng Wang, Kai Yan
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-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. Regulating the Jahn-Teller effect in single-atom catalysts enables superior peroxymonosulfate activation. The Mn-N4-C catalysts achieve high-efficiency water purification performance and long-term stability in simulated industrial-scale reactors.