Electron‐Delocalized Cu <sup>2+</sup> Activates Spin Channels in Spinel Oxides to Selectively Produce <sup>1</sup> O <sub>2</sub> for Wastewater Treatment
Le‐Yang Hao, Zijun Tang, Chu‐Yi Cai, Yuchen Zhao, Lei Tian, Nan Li, Zhao‐Qing Liu
Abstract
Abstract Blocked electron transfer in the catalyst during advanced oxidation processes causes sluggish singlet oxygen ( 1 O 2 ) generation efficiency and sacrifices catalyst stability. In this work, we propose an electron‐delocalization strategy that unlocks A Td 2+ ─O─B Oh 3+ electron‐transfer pathways within spinel oxide (Cu 0.8 Fe 2.2 O 4 ), inducing the intermolecular electron transfer of peroxymonosulfate (PMS) for selective 1 O 2 generation. In situ characterizations and theoretical calculations confirm that the electron‐delocalized Cu 2+ triggers a high spin‐state of O in Fe Td 2+ ─O─Fe Oh 3+ , thus creating a spin channel for the spontaneous intermolecular electron transfer of PMS from the Fe Oh 3+ adsorption site to the Fe Td 2+ adsorption site through Fe Td 2+ ─O─Fe Oh 3+ . This process allows for the simultaneous oxidation and reduction of PMS, thereby reducing the energy barriers for the formation of SO 4 •− and SO 5 •− radicals. Subsequently, the interfacial SO 4 •− rapidly oxidizes SO 5 •− into 1 O 2 , enhancing 1 O 2 generation efficiency without sacrificing catalyst stability. The selectivity of 1 O 2 in the Cu 0.8 Fe 2.2 O 4 /PMS system reaches 98.4%. Multiple pollutants are removed in the Cu 0.8 Fe 2.2 O 4 /PMS system without interference from coexisting substances. The scale‐up experiment realizes 100% contaminant removal during the continuous operation process (48 h). This work exhibits a novel strategy for selective 1 O 2 generation to achieve the goal of practical applications.