Chiral Heterojunctions for Spin-Enhanced Photoreforming of Plastic Waste.

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 H2 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.