Chiral Heterojunctions for Spin‐Enhanced Photoreforming of Plastic Waste

ABSTRACT Manipulating the spin state of charge carriers via the chiral‐induced spin selectivity (CISS) effect enhances charge carrier dynamics and lowers kinetic barriers, thereby advancing the photocatalytic upcycling of plastics into renewable chemicals. Here, a chiral‐ligand‐induced interfacial assembly strategy was developed to construct heterojunctions for waste plastics photoreforming. Enantiopure cysteine grafted onto MOF‐808 directs the uniform growth of a TpPa‐COF shell enabling self‐adaptive lattice matching. The heterojunctions exploit the CISS effect to regulate the spin alignment of photogenerated charge carriers. Spin‐polarized electrons are funneled to Pt single atoms, delivering an H 2 evolution rate of 1255.74 µmol g −1 h −1 . During oxidation of polyethylene terephthalate‐derived ethylene glycol, spin‐polarized holes on Pt clusters favor the parallel spin alignment of *OH intermediates, directing the reaction pathway on chiral catalysts toward C2‐retained glycolic acid (865.96 µmol g −1 h −1 ; 90.53% selectivity). In contrast, antiparallel spin alignment on achiral counterparts drives C‐C bond cleavage, yielding the C1 product formic acid. Scalable synthesis, outdoor testing, and techno‐economic analysis demonstrate the practical viability of this approach for solar‐driven waste plastic upcycling.