摘要
Visible light regulates electronic states to promote Fenton-like catalysis. • Dual single-atom CoMo-CN catalyst enhences micropollutant degradation and mineralization. • CoMo-CN/PMS/vis-light system achieves highly selective singlet oxygen generation. Singlet oxygen ( 1 O 2 ) plays a critical role in oxidative transformations, yet achieving selective and rapid generation via peroxymonosulfate (PMS), a recently developed strategy, remains a nontrivial challenge. Here we demonstrate that visible light can function as an unconventional electronic-state regulator to control PMS activation toward 1 O 2 production. Using a dual single-atom CoMo catalyst anchored on graphitic carbon nitride, irradiation induces a reversible and opposite electronic-state modulation of Co and Mo through dynamic charge redistribution. This reconfiguration weakens the overly strong interaction between Co sites and oxygenated intermediates, thereby lowering the desorption barrier of 1 O 2 and increasing reaction flux along a disproportionation-like pathway. The system exhibits markedly enhanced PMS activation, accelerated pollutant degradation, deep mineralization, broad substrate applicability, and robust performance under complex water matrices and device-relevant conditions. Notably, charge-carrier recombination in transition-metal-modified semiconductors, typically detrimental to conventional photocatalysis, is instead advantageous for PMS activation. Our findings establish light as a mild and reversible regulator of metal electronic states, providing a general framework for catalytic behavior tuning beyond conventional photocatalysis. Synopsis Visible light acts to modulate electronic-state in a Co-Mo dual single-atom catalyst (Co reduced, Mo oxidized) to enhance selective 1 O 2 generation from peroxymonosulfate, enabling efficient removal of organic micropollutants from water. Download: Download high-res image (201KB) Download: Download full-size image
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