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

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Abstract

Single-atom catalysts (SACs)-based advanced oxidation processes (AOPs) are ideal green and efficient water purification technology, but intrinsic mechanisms and interface effects are full of challenges. Herein, we have achieved precise Jahn–Teller (J-T) effect control of atomic metal-N 4 -C (M-N 4 -C: M = Mn, Fe, Co, Ni) for the first time 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 4 -C site leading to the bending of the C plane could induce the intensity of the J-T effect, weakening the d-p orbital hybridization ability with HSO 4 * 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 indicated promising practical wastewater treatment on an industrial scale. This work presents a perspective on the rational design of tuning metal d orbital in SACs for sustainable environmental remediation.

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