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Herein, we report the bio\u2010inspired activation of a series of UV\u2010absorbing <jats:italic>N<\/jats:italic>\u2010nitrosamide derivatives (NOA) under red light exposure, enabling the quantitative release of nitric oxide (NO) gasotransmitter via an MET process. The cornerstone of our design is the covalent linkage of a 2,4\u2010dinitroaniline moiety, which acts as an electron mediator to the <jats:italic>N<\/jats:italic>\u2010nitrosamide groups. This facilitates efficient electron transfer from the excited palladium(II) <jats:italic>meso<\/jats:italic>\u2010tetraphenyltetrabenzoporphyrin (PdTPTBP) photocatalyst and the selective activation of NOA. Our approach has been validated with distinct photocatalysts and various <jats:italic>N<\/jats:italic>\u2010nitrosamides, including those derived from carbamates, amides, and ureas. Notably, the modulation of the linker length between the electron mediator and <jats:italic>N<\/jats:italic>\u2010nitrosamide groups serves as a regulatory mechanism for controlling NO release kinetics. Moreover, this biomimetic NO release platform demonstrates effective operation under both normoxic and hypoxic conditions, and it enables localized delivery of NO under physiological conditions, exhibiting significant anticancer efficacy within the phototherapeutic window and enhanced selectivity towards tumor cells.<\/jats:p>","DOI":"10.1002\/anie.202409981","type":"journal-article","created":{"date-parts":[[2024,7,22]],"date-time":"2024-07-22T15:25:43Z","timestamp":1721661943000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":9,"title":["Biomimetic Activation of <i>N<\/i>\u2010Nitrosamides with Red Light\u2010Triggered Nitric Oxide Release via Mediated Electron Transfer"],"prefix":"10.1002","author":[{"given":"Guihai","family":"Gan","sequence":"first","affiliation":[{"name":"Department of Pharmacy The First Affiliated Hospital of University of Science and Technology of China (USTC) and CAS Key Laboratory of Soft Matter Chemistry Department of Polymer Science and Engineering University of Science and Technology of China  Hefei Anhui Province 230026 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhiqiang","family":"Shen","sequence":"additional","affiliation":[{"name":"Department of Pharmacy The First Affiliated Hospital of University of Science and Technology of China (USTC) and CAS Key Laboratory of Soft Matter Chemistry Department of Polymer Science and Engineering University of Science and Technology of China  Hefei Anhui Province 230026 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shaoqiu","family":"Zheng","sequence":"additional","affiliation":[{"name":"Department of Pharmacy The First Affiliated Hospital of University of Science and Technology of China (USTC) and CAS Key Laboratory of Soft Matter Chemistry Department of Polymer Science and Engineering University of Science and Technology of China  Hefei Anhui Province 230026 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Guoying","family":"Zhang","sequence":"additional","affiliation":[{"name":"Department of Pharmacy The First Affiliated Hospital of University of Science and Technology of China (USTC) and CAS Key Laboratory of Soft Matter Chemistry Department of Polymer Science and Engineering University of Science and Technology of China  Hefei Anhui Province 230026 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Dalong","family":"Yin","sequence":"additional","affiliation":[{"name":"Department of Hepatobiliary Surgery and Centre for Leading Medicine and Advanced Technologies of IHM The First Affiliated Hospital of University of Science and Technology of China Division of Life Sciences and Medicine University of Science and Technology of China  Hefei Anhui 230001 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shiyong","family":"Liu","sequence":"additional","affiliation":[{"name":"Department of Pharmacy The First Affiliated Hospital of University of Science and Technology of China (USTC) and CAS Key Laboratory of Soft Matter Chemistry Department of Polymer Science and Engineering University of Science and Technology of China  Hefei Anhui Province 230026 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6969-1343","authenticated-orcid":false,"given":"Jinming","family":"Hu","sequence":"additional","affiliation":[{"name":"Department of Pharmacy The First Affiliated Hospital of University of Science and Technology of China (USTC) and CAS Key Laboratory of Soft Matter Chemistry Department of Polymer Science and Engineering University of Science and Technology of China  Hefei Anhui Province 230026 China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2024,9,12]]},"reference":[{"key":"e_1_2_7_1_1","unstructured":"\u00a0"},{"key":"e_1_2_7_2_2","doi-asserted-by":"publisher","DOI":"10.1073\/pnas.84.24.9265"},{"key":"e_1_2_7_3_2","doi-asserted-by":"publisher","DOI":"10.1073\/pnas.74.8.3203"},{"key":"e_1_2_7_4_2","doi-asserted-by":"publisher","DOI":"10.1038\/d41586-018-07457-z"},{"key":"e_1_2_7_5_2","doi-asserted-by":"publisher","DOI":"10.1038\/nature14332"},{"key":"e_1_2_7_6_1","unstructured":"\u00a0"},{"key":"e_1_2_7_7_2","doi-asserted-by":"publisher","DOI":"10.1039\/c2cs15273h"},{"key":"e_1_2_7_8_2","doi-asserted-by":"crossref","unstructured":"Y. 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