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Herein, we constructed a metalloporphyrin\u2013anthracene sp\n                    <jats:sup>2<\/jats:sup>\n                    covalent\u2010organic framework (COF) electrocatalyst,\n                    <jats:bold>\n                      TAPP\u2010Fe\n                      <jats:sup>III<\/jats:sup>\n                      \u2010An\n                    <\/jats:bold>\n                    , which displays high structural stability and outstanding capability in activating O\n                    <jats:sub>2<\/jats:sub>\n                    and multi\u2010reactants. This enables it to effectively electro\u2010degrade PS into high\u2010value benzoyl products (yield, 23.2%,\n                    <jats:italic>M<\/jats:italic>\n                    <jats:sub>w<\/jats:sub>\n                    residue 0.3%) and re\u2010convert 20% of C\n                    <jats:sub>1<\/jats:sub>\n                    products into high\u2010value 1\u2010formyl\u20101,2,3,4\u2010tetrahydroquinoline (anticancer drug intermediate) with 9.4% yield, through a tandem quinoline carbonylation reaction. This breaks the traditional dilemma where PS degradation produces low\u2010value byproducts that are difficult to re\u2010utilize. Electrochemical experiments combined with theoretical calculations reveal that the valence tautomerism (Fe\n                    <jats:sup>II<\/jats:sup>\n                    \u2013Fe\n                    <jats:sup>III<\/jats:sup>\n                    \u2013Fe\n                    <jats:sup>IV<\/jats:sup>\n                    ) of metal center and active An ligand endow\n                    <jats:bold>\n                      TAPP\u2010Fe\n                      <jats:sup>III<\/jats:sup>\n                      \u2010An\n                    <\/jats:bold>\n                    catalyst with the ability to activate O\n                    <jats:sub>2<\/jats:sub>\n                    (generating\n                    <jats:sup>1<\/jats:sup>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    , \u2022O\n                    <jats:sub>2<\/jats:sub>\n                    <jats:sup>\u2212<\/jats:sup>\n                    , and \u2022OH) and multi\u2010reactants (PS and CO), thus enabling efficient PS electrodegradation (to benzoyl products) in tandem with low\u2010value C\n                    <jats:sub>1<\/jats:sub>\n                    products carbonylation (to anticancer drug intermediate). In this process, the generated C\n                    <jats:sub>1<\/jats:sub>\n                    products (HCOOH, CO) were re\u2010activated by TAPP\u2010Fe\n                    <jats:sup>III<\/jats:sup>\n                    centers, and then react with 1,2,3,4\u2010tetrahydroquinoline for high\u2010value conversion. This work pioneers a tandem conversion strategy for PS waste degradation and low\u2010value C\n                    <jats:sub>1<\/jats:sub>\n                    products upgrading.\n                  <\/jats:p>","DOI":"10.1002\/anie.5012045","type":"journal-article","created":{"date-parts":[[2026,9,14]],"date-time":"2026-09-14T07:47:56Z","timestamp":1789372076000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Covalent\u2010Organic Framework\u2010Manipulated Multi\u2010Reactant Activation Enables Polystyrene Electrodegradation in Tandem With Over\u2010Oxidation Product Upgrading"],"prefix":"10.1002","author":[{"given":"Yu","family":"Chen","sequence":"first","affiliation":[{"name":"Guangdong Provincial Key Laboratory of Carbon Dioxide Resource Utilization School of Chemistry South China Normal University  Guangzhou P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiao\u2010Hong","family":"Chen","sequence":"additional","affiliation":[{"name":"Guangdong Provincial Key Laboratory of Carbon Dioxide Resource Utilization School of Chemistry South China Normal University  Guangzhou P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qian\u2010Qian","family":"Huang","sequence":"additional","affiliation":[{"name":"Guangdong Provincial Key Laboratory of Carbon Dioxide Resource Utilization School of Chemistry South China Normal University  Guangzhou P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Si\u2010Ying","family":"Huang","sequence":"additional","affiliation":[{"name":"Guangdong Provincial Key Laboratory of Carbon Dioxide Resource Utilization School of Chemistry South China Normal University  Guangzhou P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Run\u2010Han","family":"Li","sequence":"additional","affiliation":[{"name":"Guangdong Provincial Key Laboratory of Carbon Dioxide Resource Utilization School of Chemistry South China Normal University  Guangzhou P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ya\u2010Fang","family":"Guan","sequence":"additional","affiliation":[{"name":"Guangdong Provincial Key Laboratory of Carbon Dioxide Resource Utilization School of Chemistry South China Normal University  Guangzhou P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2596-4928","authenticated-orcid":false,"given":"Jiang","family":"Liu","sequence":"additional","affiliation":[{"name":"Guangdong Provincial Key Laboratory of Carbon Dioxide Resource Utilization School of Chemistry South China Normal University  Guangzhou P. R. 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