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Here, a chiral\u2010ligand\u2010induced interfacial assembly strategy was developed to construct heterojunctions for waste plastics photoreforming. Enantiopure cysteine grafted onto MOF\u2010808 directs the uniform growth of a TpPa\u2010COF shell enabling self\u2010adaptive lattice matching. The heterojunctions exploit the CISS effect to regulate the spin alignment of photogenerated charge carriers. Spin\u2010polarized electrons are funneled to Pt single atoms, delivering an H\n                    <jats:sub>2<\/jats:sub>\n                    evolution rate of 1255.74 \u00b5mol\u00a0g\n                    <jats:sup>\u22121<\/jats:sup>\n                    \u00a0h\n                    <jats:sup>\u22121<\/jats:sup>\n                    . During oxidation of polyethylene terephthalate\u2010derived ethylene glycol, spin\u2010polarized holes on Pt clusters favor the parallel spin alignment of *OH intermediates, directing the reaction pathway on chiral catalysts toward C2\u2010retained glycolic acid (865.96 \u00b5mol g\n                    <jats:sup>\u22121<\/jats:sup>\n                    h\n                    <jats:sup>\u22121<\/jats:sup>\n                    ; 90.53% selectivity). In contrast, antiparallel spin alignment on achiral counterparts drives C\u2010C bond cleavage,\u00a0yielding the C1 product formic acid. Scalable synthesis, outdoor testing, and techno\u2010economic analysis demonstrate the practical viability of this approach for solar\u2010driven waste plastic upcycling.\n                  <\/jats:p>","DOI":"10.1002\/adma.75215","type":"journal-article","created":{"date-parts":[[2026,9,30]],"date-time":"2026-09-30T10:32:08Z","timestamp":1790764328000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Chiral Heterojunctions for Spin\u2010Enhanced Photoreforming of Plastic Waste"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0004-0670-6626","authenticated-orcid":false,"given":"Jian","family":"Li","sequence":"first","affiliation":[{"name":"State Key Laboratory of Advanced Separation Membrane Materials School of Chemical Engineering and Technology School of Materials Science and Engineering Tiangong University  Tianjin P. R. China"},{"name":"Cangzhou Institute of Tiangong University  Cangzhou P. R. 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