Activated Graphene Functionalized 2,4‐DNP Hydrazine for Photocatalytic C─S/C─N Bond Activation and NADH Regeneration

ABSTRACT The development of a metal‐free, efficient, and cost‐effective photocatalyst is crucial for advancing green chemical transformations and bio‐redox processes. This work reports 2,4‐dinitrophenylhydrazine‐functionalized KOH‐activated Aloe vera ‐derived graphene (G@DNP photocatalyst) as a metal‐free, visible‐light‐active photocatalyst for NADH cofactor regeneration and C─S/C─N bond activation under ambient conditions. The synergy that comes into play when electron‐deficient DNP moieties couple with highly conjugated activated graphene (G) derived from A. vera results in rapid photo‐induced electron flow, minimum charge recombination, and high light‐absorption capabilities. On visible light irradiation, G@DNP photocatalyst selectively reduces NAD + to NADH and catalyzes selective C─S/C─N bond transformations in organic substrates with high yield. Extensive characterization supports the strong interaction between graphene and DNP chromophore, validating its high photocatalytic efficiency. Moreover, this study highlights the multifunctionality and sustainability and offers a versatile platform for cofactor regeneration and light‐mediated organic synthesis, providing promising applications in artificial photosynthesis and green chemistry.