Achieving Near Infrared Photodegradation by the Synergistic Effect of Z-Scheme Heterojunction and Antenna of Rare Earth Single Atoms

Abstract

Near-infrared light response catalysts have received great attention in renewable solar energy conversion, energy production, and environmental purification. Here, near-infrared photodegradation is successfully achieved in rare earth single atom anchored NaYF₄@g-C₃N₄ heterojunctions by the synergistic effect of Z-scheme heterojunction and antenna of rare earth single atoms. The UV–vis light emitted by Tm³⁺ can not only be directly absorbed by g-C₃N₄ to generate electron–hole pairs, realizing efficient energy transfer, but also be absorbed by NaYF₄ substrate, and generating photo-generated electrons at its impurity level, transferring the active charge to the valence band of g-C₃N₄, forming a Z-scheme heterojunction and further improving the photocatalytic efficiency. Importantly, Tm single atoms has multiple functions such as acting as charge transfer channels to facilitate charge transfer, regulating the critical distance of energy transfer, and prolonging electron–hole pair lifetime. Under NIR light, it exhibited remarkable performance in degrading antibiotics (the removal rate of TC reached 91% for 6 h) while maintaining excellent stability. The LC-MS/MS technology is used to reveal the reaction intermediates, active species, and reaction pathways, and the complex mechanism of photodegradation is further proposed. This study provides experimental and theoretical support for designing and synthesizing catalysts with near-infrared light response characteristics.