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This study presents a comparative investigation on the photoinduced electron transfer dynamics of three perylene diimide (PDI) polymers, o\u00a0PDI, m\u00a0PDI, and p\u00a0PDI, that differ by their phenylenediamine linkers. Notably, o\u00a0PDI, which is constructed with ortho-phenylenediamine linkers, exhibits the fastest two-electron CS and the subsequent FC generation among this series. These superior properties are attributed to its large molecular dipole moment and driving force for multielectron accumulation. The high photocatalytic activity of o\u00a0PDI was further verified through two independent two-electron quenching experiments and the oxygen reduction reaction (ORR). The latter efficiently generates H2O2, particularly in the case of o\u00a0PDI, leading to the rapid degradation of uric acid (UA). This work elucidates the mechanism of photoinduced accumulative electron transfer in PDI-based polymers and provides a theoretical framework for the rational design of efficient multielectron accumulation systems in advanced photocatalytic applications.<\/jats:p>","DOI":"10.1021\/jacsau.6c00868","type":"journal-article","created":{"date-parts":[[2026,8,20]],"date-time":"2026-08-20T11:01:31Z","timestamp":1787223691000},"page":"5214-5224","source":"Crossref","is-referenced-by-count":0,"title":["Photoinduced Accumulative\nElectron-Transfer Dynamics\nin Perylene Diimide Polymers as Photoredox Catalysts"],"prefix":"10.1021","volume":"6","author":[{"given":"Zicong","family":"Situ","sequence":"first","affiliation":[{"name":"Beijing University of Posts and Telecommunications (BUPT) , , ,","place":["Beijing, P. R. China, 100876"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xingqing","family":"Li","sequence":"additional","affiliation":[{"name":"Beijing University of Posts and Telecommunications (BUPT) , , ,","place":["Beijing, P. R. China, 100876"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ying-Xin","family":"Qiao","sequence":"additional","affiliation":[{"name":"Shantou University , , ,","place":["Shantou, P. R. China, 515063"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chao","family":"Yang","sequence":"additional","affiliation":[{"name":"Beijing University of Posts and Telecommunications (BUPT) , , ,","place":["Beijing, P. R. China, 100876"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yanqi","family":"Chen","sequence":"additional","affiliation":[{"name":"Beijing University of Posts and Telecommunications (BUPT) , , ,","place":["Beijing, P. R. China, 100876"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Mengke","family":"Tang","sequence":"additional","affiliation":[{"name":"Beijing University of Posts and Telecommunications (BUPT) , , ,","place":["Beijing, P. R. China, 100876"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5416-9608","authenticated-orcid":true,"given":"Yang","family":"Li","sequence":"additional","affiliation":[{"name":"Beijing University of Posts and Telecommunications (BUPT) , , ,","place":["Beijing, P. R. China, 100876"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4618-4960","authenticated-orcid":true,"given":"Yan","family":"Wan","sequence":"additional","affiliation":[{"name":"Beijing Normal University , , ,","place":["Beijing, P. R. China, 100875"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9439-7621","authenticated-orcid":true,"given":"Hongwei","family":"Song","sequence":"additional","affiliation":[{"name":"South China University of Technology , , ,","place":["Guangzhou, P. R. China, 510640"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8125-9684","authenticated-orcid":true,"given":"Qing-Xiao","family":"Tong","sequence":"additional","affiliation":[{"name":"Shantou University , , ,","place":["Shantou, P. R. China, 515063"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8859-1535","authenticated-orcid":true,"given":"Jing-Xin","family":"Jian","sequence":"additional","affiliation":[{"name":"Shantou University , , ,","place":["Shantou, P. R. 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Soc."},{"issue":"12","key":"2026092808093162800_cit5","doi-asserted-by":"publisher","first-page":"1910","DOI":"10.1021\/ar9001735","article-title":"Self-Assembly\nStrategies for Integrating Light Harvesting and Charge Separation\nin Artificial Photosynthetic Systems","volume":"42","author":"Wasielewski","year":"2009","journal-title":"Acc. Chem.\nRes."},{"issue":"3","key":"2026092808093162800_cit6","doi-asserted-by":"publisher","first-page":"840","DOI":"10.1021\/ar500386x","article-title":"Accumulative\nCharge Separation for Solar Fuels Production: Coupling Light-Induced\nSingle Electron Transfer to Multielectron Catalysis","volume":"48","author":"Hammarstro\u0308m","year":"2015","journal-title":"Acc. Chem. 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