Elucidating the Multifaceted Influence Pathway of Spin Regulation on Carrier Dynamics and O 2 Transformation in a Chiral LDO Photocatalytic Framework

ABSTRACT In photocatalysis, the rapid recombination of photogenerated carriers, leading to short lifetimes and the inefficient conversion of oxygen (O 2 ) into active species, has long restricted the application efficiency of catalytic materials in environmental governance and energy fields. Traditional strategies mostly focus on heterojunction construction or noble metal doping to optimize charge separation, but they neglect precise regulation of electron spin degrees of freedom, making it difficult to achieve synergistic optimization of carrier dynamics and reaction pathways. In this study, LDO with chiral structures were fabricated using organic templates, directional transfer of chirality from organic molecules to the inorganic LDO lattice was achieved, constructing a photocatalytic system with spin regulation capabilities. The study reveals that chiral structures break inversion symmetry and, through the induced chirality‐induced spin selectivity (CISS) mechanism, directionally filter electrons of specific spin orientations. This significantly prolongs the lifetime of photogenerated carriers and promotes the efficient conversion of oxygen (O 2 ) into singlet oxygen ( 1 O 2 ) and superoxide radicals (•O 2 − ), exhibiting excellent capabilities in antibacterial applications and tetracycline degradation under visible light irradiation. This work provides a new paradigm for designing efficient photocatalysts based on the degree of freedom of electron spin.