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Conventional industrial production of HMS relies on toxic and volatile formaldehyde, presenting considerable safety and environmental risks. Herein, we report a solar\u2010driven photocatalytic route for the synthesis of HMS from waste SO\n                    <jats:sub>2<\/jats:sub>\n                    and polyethylene terephthalate (PET)\u2010derived ethylene glycol (EG) under ambient conditions, using a Cu single\u2010atom\u2010decorated TiO\n                    <jats:sub>2<\/jats:sub>\n                    catalyst (Cu\n                    <jats:sub>1<\/jats:sub>\n                    \/TiO\n                    <jats:sub>2<\/jats:sub>\n                    ). The optimized Cu\n                    <jats:sub>1<\/jats:sub>\n                    \/TiO\n                    <jats:sub>2<\/jats:sub>\n                    catalyst achieves an HMS yield rate of \u223c 2.31\u00a0mmol g\n                    <jats:sub>cat<\/jats:sub>\n                    <jats:sup>\u22121<\/jats:sup>\n                    h\n                    <jats:sup>\u22121<\/jats:sup>\n                    with a 77.5% carbon selectivity, along with a H\n                    <jats:sub>2<\/jats:sub>\n                    evolution rate of \u223c 4.36\u00a0mmol g\n                    <jats:sub>cat<\/jats:sub>\n                    <jats:sup>\u22121<\/jats:sup>\n                    h\n                    <jats:sup>\u22121<\/jats:sup>\n                    . Mechanistic studies reveal that the atomically dispersed Cu sites act as electron sinks, which enhance charge separation and induce electronic modulation of TiO\n                    <jats:sub>2<\/jats:sub>\n                    . This modulation facilitates the adsorption and activation of reactants while lowering the energy barrier for the formation of a key *CHOH\u2500CH\n                    <jats:sub>2<\/jats:sub>\n                    OH intermediate via EG dehydrogenation. This resulting intermediate then undergoes nucleophilic attack by hole\u2010generated \u2022SO\n                    <jats:sub>3<\/jats:sub>\n                    <jats:sup>\u2212<\/jats:sup>\n                    , triggering C\u2500C cleavage to form HMS. This work establishes a sustainable and waste\u2010valorizing route for organosulfur synthesis.\n                  <\/jats:p>","DOI":"10.1002\/anie.1777088","type":"journal-article","created":{"date-parts":[[2026,4,22]],"date-time":"2026-04-22T05:22:16Z","timestamp":1776835336000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":6,"title":["Solar\u2010Driven Photocatalytic C\u2500S Coupling for Organosulfur Synthesis Via Upcycling SO\n                    <sub>2<\/sub>\n                    and Plastic Waste"],"prefix":"10.1002","volume":"65","author":[{"given":"Yifei","family":"Liang","sequence":"first","affiliation":[{"name":"Key Laboratory of Photochemical Conversion and Optoelectronic Materials &amp; CAS\u2010HKU Joint Laboratory on New Materials Technical Institute of Physics and Chemistry Chinese Academy of Sciences  Beijing P. R. China"},{"name":"University of Chinese Academy of Sciences  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0032-2600","authenticated-orcid":false,"given":"Fulai","family":"Liu","sequence":"additional","affiliation":[{"name":"Key Laboratory of Photochemical Conversion and Optoelectronic Materials &amp; CAS\u2010HKU Joint Laboratory on New Materials Technical Institute of Physics and Chemistry Chinese Academy of Sciences  Beijing P. R. China"},{"name":"University of Chinese Academy of Sciences  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Fan","family":"Liu","sequence":"additional","affiliation":[{"name":"University of Chinese Academy of Sciences  Beijing P. R. China"},{"name":"Functional Crystals Lab Technical Institute of Physics and Chemistry Chinese Academy of Sciences  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5559-8749","authenticated-orcid":false,"given":"Rui","family":"Shi","sequence":"additional","affiliation":[{"name":"Key Laboratory of Photochemical Conversion and Optoelectronic Materials &amp; CAS\u2010HKU Joint Laboratory on New Materials Technical Institute of Physics and Chemistry Chinese Academy of Sciences  Beijing P. R. China"},{"name":"University of Chinese Academy of Sciences  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jing","family":"Li","sequence":"additional","affiliation":[{"name":"Key Laboratory of Photochemical Conversion and Optoelectronic Materials &amp; CAS\u2010HKU Joint Laboratory on New Materials Technical Institute of Physics and Chemistry Chinese Academy of Sciences  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9993-6399","authenticated-orcid":false,"given":"Lei","family":"Kang","sequence":"additional","affiliation":[{"name":"University of Chinese Academy of Sciences  Beijing P. R. China"},{"name":"Functional Crystals Lab Technical Institute of Physics and Chemistry Chinese Academy of Sciences  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6689-8923","authenticated-orcid":false,"given":"Yong","family":"Chen","sequence":"additional","affiliation":[{"name":"Key Laboratory of Photochemical Conversion and Optoelectronic Materials &amp; CAS\u2010HKU Joint Laboratory on New Materials Technical Institute of Physics and Chemistry Chinese Academy of Sciences  Beijing P. R. China"},{"name":"University of Chinese Academy of Sciences  Beijing P. R. 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