Spin-Steered Photosynthesis of H₂O₂ in Magnetic Single-Atom Modified Covalent Triazine Frameworks: A Density...

Covalent Organic Frameworks (COFs) demonstrate promising potential in the photocatalytic synthesis of H₂O₂ owing to favorable light absorption, superior charge separation, and considerable surface area. However, the efficiency of H₂O₂ photosynthesis is impeded by insufficient O₂ adsorption sites and a high reaction barrier. In this work, various metal single atoms (Fe, Co, Ni) are introduced onto covalent triazine frameworks (CTFs) with N-N coordination sites to significantly enhance O₂ adsorption and optimize H₂O₂ synthesis. Computational findings suggest that the presence of Fe, Co, and Ni not only enhances O₂ adsorption but also exerts an influence on the reaction pathway of H₂O₂. Significantly, Fe exhibits a distinct advantage in modulating O₂ adsorption through its unique electron spin state when compared to Co and Ni, as confirmed by crystal orbital Hamilton population (COHP) analysis. Additionally, this integration of metal atoms also improves light absorption and charge separation in CTFs. The study provides strategic insight into elevating H₂O₂ production by incorporating tailored metal single atoms into COFs.