{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,9,29]],"date-time":"2026-09-29T06:58:29Z","timestamp":1790665109984,"version":"4.1.0"},"reference-count":55,"publisher":"Wiley","license":[{"start":{"date-parts":[[2026,9,28]],"date-time":"2026-09-28T00:00:00Z","timestamp":1790553600000},"content-version":"vor","delay-in-days":0,"URL":"http:\/\/onlinelibrary.wiley.com\/termsAndConditions#vor"},{"start":{"date-parts":[[2026,9,28]],"date-time":"2026-09-28T00:00:00Z","timestamp":1790553600000},"content-version":"tdm","delay-in-days":0,"URL":"http:\/\/doi.wiley.com\/10.1002\/tdm_license_1.1"}],"content-domain":{"domain":["advanced.onlinelibrary.wiley.com"],"crossmark-restriction":true},"short-container-title":["Advanced Materials"],"abstract":"<jats:title>ABSTRACT<\/jats:title>\n                  <jats:p>\n                    Direct photocatalytic upcycling of nonbiodegradable plastics using single\u2011atom catalysts (SACs) remain limited by the symmetric coordination of isolated metal sites, which constrains intermediate binding and charge transfer. Here, we reconstruct the heptazine units of polymeric carbon nitride (PCN) via a salt\u2010induced strategy, transforming S\u2500CoPCN with a predominantly symmetric Co\u2500N\n                    <jats:sub>4<\/jats:sub>\n                    coordination environment into A\u2500CoPCN featuring predominantly asymmetric Co\u2500N\n                    <jats:sub>3<\/jats:sub>\n                    configurations. Under white\u2010light irradiation at room temperature and 1\u00a0bar O\n                    <jats:sub>2<\/jats:sub>\n                    , A\u2500CoPCN enables the conversion of polystyrene to benzoic acid with a yield of 39.6% and a carbon recovery of 71.6%. Compared with previously reported systems that often require elevated temperatures, high O\n                    <jats:sub>2<\/jats:sub>\n                    pressures, or external oxidants, this system operates under markedly milder conditions. The catalyst further demonstrates broad applicability across diverse nonbiodegradable plastics, including polystyrene, polyisobutylene, polylactic acid, polypropylene, polyethylene, and polyvinyl acetate. Mechanistic studies combining advanced spectroscopy and density functional theory calculations reveal that symmetry breaking suppresses electron delocalization, upshifts the Co d\u2010band center, and lowers exciton binding energy, thereby facilitating charge separation and transfer, promoting O\n                    <jats:sub>2<\/jats:sub>\n                    adsorption and activation to generate reactive \u2022O\n                    <jats:sub>2<\/jats:sub>\n                    <jats:sup>\u2212<\/jats:sup>\n                    species for efficient plastic upcycling. This work identifies coordination asymmetry as a key design principle for SACs and provides a general strategy for enhancing photocatalytic plastic upcycling.\n                  <\/jats:p>","DOI":"10.1002\/adma.75166","type":"journal-article","created":{"date-parts":[[2026,9,29]],"date-time":"2026-09-29T06:16:39Z","timestamp":1790662599000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Reduced Electron Delocalization via Symmetry Breaking at Single\u2010Atom Cobalt Sites for Efficient Photocatalytic Plastic Upcycling"],"prefix":"10.1002","author":[{"given":"Yanglin","family":"Chen","sequence":"first","affiliation":[{"name":"School of Materials Science and Engineering Nanyang Technological University  Singapore Singapore"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ganghua","family":"Zhou","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Nanyang Technological University  Singapore Singapore"},{"name":"School of Mechanical Engineering College of Environmental Science and Engineering Institute of Technology for Carbon Neutralization Yangzhou University  Yangzhou Jiangsu P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ziyu","family":"Mei","sequence":"additional","affiliation":[{"name":"Key Laboratory for Anisotropy and Texture of Materials School of Material Science and Engineering Northeastern University  Shenyang P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xingyu","family":"Wang","sequence":"additional","affiliation":[{"name":"School of Chemistry Chemical Engineering and Biotechnology Nanyang Technological University  Singapore Singapore"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Limo","family":"He","sequence":"additional","affiliation":[{"name":"Department of Chemical and Biomolecular Engineering National University of Singapore  Singapore Singapore"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7712-7083","authenticated-orcid":false,"given":"Riyanka","family":"Karmakar","sequence":"additional","affiliation":[{"name":"School of Physical and Mathematical Sciences Nanyang Technological University  Singapore Singapore"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Weidong","family":"Hou","sequence":"additional","affiliation":[{"name":"Institute of Nanochemistry and Nanobiology School of Environmental and Chemical Engineering Shanghai University  Shanghai P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4936-967X","authenticated-orcid":false,"given":"Xingwang","family":"Zhu","sequence":"additional","affiliation":[{"name":"School of Mechanical Engineering College of Environmental Science and Engineering Institute of Technology for Carbon Neutralization Yangzhou University  Yangzhou Jiangsu P. R. 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4049-2719","authenticated-orcid":false,"given":"Tze Chien","family":"Sum","sequence":"additional","affiliation":[{"name":"School of Physical and Mathematical Sciences Nanyang Technological University  Singapore Singapore"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6502-2313","authenticated-orcid":false,"given":"Han Sen","family":"Soo","sequence":"additional","affiliation":[{"name":"School of Chemistry Chemical Engineering and Biotechnology Nanyang Technological University  Singapore Singapore"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Can","family":"Xue","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Nanyang Technological University  Singapore 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