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In this study, we introduced an efficient electrochemical strategy to convert polyethylene terephthalate (PET)\u2010derived ethylene glycol (EG) into organosulfur compounds with high yields. A specially designed iron single\u2010atom catalyst (SAC) supported on nitrogen\u2010doped hollow carbon spheres (NHCS), which feature high catalytic activity of the Fe\u2010N\n                    <jats:sub>3<\/jats:sub>\n                    motifs, was employed, which facilitates the C\u2500C bond cleavage during EG oxidation, and generates formaldehyde (CH\n                    <jats:sub>2<\/jats:sub>\n                    O) species. These intermediates subsequently react with S\u2010containing nucleophiles, that is, SO\n                    <jats:sub>3<\/jats:sub>\n                    <jats:sup>2\u2212<\/jats:sup>\n                    , to form hydroxymethanesulfonate (HMS) via C\u2500S bond formation. Our method achieves a remarkable faradaic efficiency of over 60% and an unprecedented production rate of 1800\u00a0\u00b5mol cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    h\n                    <jats:sup>\u22121<\/jats:sup>\n                    for HMS. Additionally, we validate the use of PET as feedstock for C\u2500S bond formation, achieving a considerable faradaic efficiency of over 25% and an unprecedented production rate of 900\u00a0\u00b5mol cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    h\n                    <jats:sup>\u22121<\/jats:sup>\n                    . Our approach promises to enhance sustainability and profitability in plastic value chain management and revolutionize the production of pharmaceuticals, textile chemicals, and agrochemicals.\n                  <\/jats:p>","DOI":"10.1002\/anie.202507901","type":"journal-article","created":{"date-parts":[[2025,8,5]],"date-time":"2025-08-05T08:02:14Z","timestamp":1754380934000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":34,"title":["Electrochemical Upgrading Plastic to Organosulfurs Through Fe\u2010N\n                    <sub>3<\/sub>\n                    Single Atom Catalyst Under Ambient Conditions"],"prefix":"10.1002","volume":"64","author":[{"given":"Qing","family":"Xia","sequence":"first","affiliation":[{"name":"Department of Mechanical Engineering The Hong Kong Polytechnic University  Hung Hom Kowloon Hong Kong SAR"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shanhe","family":"Gong","sequence":"additional","affiliation":[{"name":"Department of Mechanical Engineering The Hong Kong Polytechnic University  Hung Hom Kowloon Hong Kong SAR"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jie","family":"Wu","sequence":"additional","affiliation":[{"name":"Department of Mechanical Engineering The Hong Kong Polytechnic University  Hung Hom Kowloon Hong Kong SAR"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yanjie","family":"Zhai","sequence":"additional","affiliation":[{"name":"Department of Mechanical Engineering The Hong Kong Polytechnic University  Hung Hom Kowloon Hong Kong SAR"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Weisong","family":"Li","sequence":"additional","affiliation":[{"name":"Department of Mechanical Engineering The Hong Kong Polytechnic University  Hung Hom Kowloon Hong Kong SAR"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yingying","family":"Zhou","sequence":"additional","affiliation":[{"name":"Department of Mechanical Engineering The Hong Kong Polytechnic University  Hung Hom Kowloon Hong Kong SAR"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4780-2161","authenticated-orcid":false,"given":"Xiao","family":"Zhang","sequence":"additional","affiliation":[{"name":"Department of Mechanical Engineering The Hong Kong Polytechnic University  Hung Hom Kowloon Hong Kong SAR"},{"name":"Research Center for Carbon\u2010Strategic Catalysis The Hong Kong Polytechnic University  Hung Hom Kowloon Hong Kong SAR"},{"name":"The Hong Kong Polytechnic University Shenzhen Research Institute  Shenzhen 518057 China"},{"name":"PolyU\u2010Daya Bay Technology and Innovation Research Institute The Hong Kong Polytechnic University  Huizhou Guangdong China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2025,8,5]]},"reference":[{"key":"e_1_2_9_1_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41586-020-2149-4"},{"key":"e_1_2_9_2_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41929-022-00821-3"},{"key":"e_1_2_9_3_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41586-022-04599-z"},{"key":"e_1_2_9_4_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.envpol.2020.115745"},{"key":"e_1_2_9_5_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.jwpe.2020.101612"},{"key":"e_1_2_9_6_1","doi-asserted-by":"publisher","DOI":"10.1002\/cssc.202100904"},{"key":"e_1_2_9_7_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41578-020-0190-4"},{"key":"e_1_2_9_8_1","doi-asserted-by":"publisher","DOI":"10.1002\/cssc.202300142"},{"key":"e_1_2_9_9_1","doi-asserted-by":"publisher","DOI":"10.1039\/D3GC04174C"},{"key":"e_1_2_9_10_1","doi-asserted-by":"publisher","DOI":"10.1039\/D3GC01872E"},{"key":"e_1_2_9_11_1","doi-asserted-by":"publisher","DOI":"10.1002\/ange.202117205"},{"key":"e_1_2_9_12_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41929-021-00648-4"},{"key":"e_1_2_9_13_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-021-25048-x"},{"key":"e_1_2_9_14_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.jechem.2024.01.010"},{"key":"e_1_2_9_15_1","doi-asserted-by":"publisher","DOI":"10.1021\/acscatal.2c01128"},{"key":"e_1_2_9_16_1","doi-asserted-by":"crossref","DOI":"10.1016\/j.cej.2024.155106","volume":"498","author":"Hao S. 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