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Here, we introduce a fully green, photo\u2010driven process for polystyrene (PS) upcycling, enabled by a synergistic thermal\u2010focusing and space\u2010confined catalysis. Using earth\u2010abundant MoO\n                    <jats:sub>3\u2010x<\/jats:sub>\n                    , it can efficiently absorb sunlight to generate localized heat, dynamically melting adjacent PS and spontaneously forming a core\u2010shell MoO\n                    <jats:sub>3\u2010x<\/jats:sub>\n                    @PS structure. Critically, the intrinsically low thermal conductivity of PS creates a self\u2010forming insulating layer, which traps thermal energy at the catalyst\u2010polymer interface. This self\u2010focusing thermal localization effect sustains a microscopic high\u2010temperature reaction zone under ambient conditions, dramatically enhancing energy efficiency. The concentrated heat cleaves inert C\u2500C bonds, while photogenerated charge carriers facilitate selective oxidative degradation. Consequently, we achieve 75.0% PS conversion with 70.5% combined yield of valuable products, predominantly benzoic acid crystals that spontaneously separate post\u2010reaction. Operating without solvents or external heating, our strategy transforms waste PS into valuable chemicals using only sunlight. This work establishes a new paradigm for solid\u2010state photothermal upcycling, leveraging interfacial thermal localization to enable a truly sustainable light\u2010to\u2010chemicals circular path.\n                  <\/jats:p>","DOI":"10.1002\/adma.74031","type":"journal-article","created":{"date-parts":[[2026,7,12]],"date-time":"2026-07-12T06:38:18Z","timestamp":1783838298000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Dynamic Self\u2010Focusing Photothermal Localization Induced Mild Solvent\u2010Free Upcycling of Polystyrene"],"prefix":"10.1002","volume":"38","author":[{"given":"Shuang","family":"Tang","sequence":"first","affiliation":[{"name":"Institute of Microscale Optoelectronics International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of Education Shenzhen University  Shenzhen P. R. China"},{"name":"Institute of Technology for Future Industry Shenzhen University of Information Technology  Shenzhen P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chuntian","family":"Qiu","sequence":"additional","affiliation":[{"name":"ZJU\u2010Hangzhou Global Scientific and Technological Innovation Center Zhejiang University  Hangzhou P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6114-1112","authenticated-orcid":false,"given":"Bin","family":"Zhang","sequence":"additional","affiliation":[{"name":"ZJU\u2010Hangzhou Global Scientific and Technological Innovation Center Zhejiang University  Hangzhou P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5708-8379","authenticated-orcid":false,"given":"Nailiang","family":"Yang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Biochemical Engineering Key Laboratory of Biopharmaceutical Preparation and Delivery Institute of Process Engineering Chinese Academy of Sciences  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0907-1601","authenticated-orcid":false,"given":"Yang\u2010Sen","family":"Xu","sequence":"additional","affiliation":[{"name":"Institute of Technology for Future Industry Shenzhen University of Information Technology  Shenzhen P. R. 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