Electron‐Delocalized Cu2+ Activates Spin Channels in Spinel Oxides to Selectively Produce 1O2 for Wastewater Treatment

Blocked electron transfer in the catalyst during advanced oxidation processes causes sluggish singlet oxygen (1O2) generation efficiency and sacrifices catalyst stability. In this work, we propose an electron‐delocalization strategy that unlocks ATd2+‐O‐BOh3+ electron‐transfer pathways within spinel oxide (Cu0.8Fe2.2O4), inducing the intermolecular electron transfer of peroxymonosulfate (PMS) for selective 1O2 generation. In‐situ characterizations and theoretical calculations confirm that the electron‐delocalized Cu2+ triggers a high spin‐state of O in FeTd2+‐O‐FeOh3+, thus creating a spin channel for the spontaneous intermolecular electron transfer of PMS from the FeOh3+ adsorption site to the FeTd2+ adsorption site through FeTd2+‐O‐FeOh3+. This process allows for the simultaneous oxidation and reduction of PMS, thereby reducing the energy barriers for the formation of SO4•– and SO5•– radicals. Subsequently, the interfacial SO4•– rapidly oxidizes SO5•– into 1O2, enhancing 1O2 generation efficiency without sacrificing catalyst stability. The selectivity of 1O2 in the Cu0.8Fe2.2O4/PMS system reaches 98.4%. Multiple pollutants are removed in the Cu0.8Fe2.2O4/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 1O2 generation to achieve the goal of practical applications.