{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,10,24]],"date-time":"2026-10-24T02:34:59Z","timestamp":1792809299504,"version":"4.5.0"},"reference-count":48,"publisher":"American Chemical Society (ACS)","issue":"29","license":[{"start":{"date-parts":[[2026,7,17]],"date-time":"2026-07-17T00:00:00Z","timestamp":1784246400000},"content-version":"stm-asf","delay-in-days":0,"URL":"https:\/\/doi.org\/10.15223\/policy-029"},{"start":{"date-parts":[[2026,7,17]],"date-time":"2026-07-17T00:00:00Z","timestamp":1784246400000},"content-version":"stm-asf","delay-in-days":0,"URL":"https:\/\/doi.org\/10.15223\/policy-037"},{"start":{"date-parts":[[2026,7,17]],"date-time":"2026-07-17T00:00:00Z","timestamp":1784246400000},"content-version":"stm-asf","delay-in-days":0,"URL":"https:\/\/doi.org\/10.15223\/policy-045"}],"funder":[{"DOI":"10.13039\/100031910","name":"Changping Laboratory","doi-asserted-by":"publisher","award":["NA"],"award-info":[{"award-number":["NA"]}],"id":[{"id":"10.13039\/100031910","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/501100001809","name":"National Natural Science Foundation of China","doi-asserted-by":"publisher","award":["22225603"],"award-info":[{"award-number":["22225603"]}],"id":[{"id":"10.13039\/501100001809","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/501100001809","name":"National Natural Science Foundation of China","doi-asserted-by":"publisher","award":["22441051"],"award-info":[{"award-number":["22441051"]}],"id":[{"id":"10.13039\/501100001809","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/501100002855","name":"Ministry of Science and Technology of the People's Republic of China","doi-asserted-by":"publisher","award":["2021YFA1601400"],"award-info":[{"award-number":["2021YFA1601400"]}],"id":[{"id":"10.13039\/501100002855","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/501100002865","name":"Chongqing Municipal Science and Technology Bureau","doi-asserted-by":"publisher","award":["CSTB2024TIAD-STX0048"],"award-info":[{"award-number":["CSTB2024TIAD-STX0048"]}],"id":[{"id":"10.13039\/501100002865","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/na","name":"New Cornerstone Science Foundation","doi-asserted-by":"publisher","award":["NA"],"award-info":[{"award-number":["NA"]}],"id":[{"id":"10.13039\/na","id-type":"DOI","asserted-by":"publisher"}]}],"content-domain":{"domain":[],"crossmark-restriction":false},"short-container-title":[],"published-print":{"date-parts":[[2026,7,29]]},"abstract":"<jats:title>Abstract<\/jats:title>\n                  <jats:p>A critical challenge in the bench-to-bedside translation of controlled drug release strategies is the sharp decline in reaction efficiency as biological complexity increases. A platform capable of maintaining bioorthogonal-like drug release\u2500remaining minimally perturbed by physiological environments\u2500would address an unmet clinical need. This is particularly relevant for radiotherapy-mediated drug release, where the oxidative activation of prodrugs is often compromised by the rapid quenching of reactive intermediates in vivo. Herein, we engineer a hafnium-based nanoscale metal\u2013organic layer platform that leverages a unique \u201csurface-confinement effect\u201d to overcome this challenge. By covalently tethering prodrugs to the Hf-nMOLs surface, we constructed two-dimensional nanoreactors that spatially localize the activation process within an interface enriched with reactive species. This design effectively insulates the activation step from biological scavengers, ensuring efficient payload release efficiency across increasing biological complexity. When loaded with the topoisomerase I inhibitor Exatecan, the Hf-nMOLs system achieved an intratumoral drug-release G-value of 568 nM\u00b7Gy\u22121, resulting in potent radiosensitization and significant tumor-growth suppression under low-dose X-ray irradiation. This work presents a versatile strategy for robust radio-chemotherapeutic combinations, achieving the simultaneous release of diverse payloads activated by radiotherapy. Our findings also suggest that engineering nanoscale surface confinement may provide a generalizable materials strategy to help confer bioorthogonality to otherwise labile activation reactions.<\/jats:p>","DOI":"10.1021\/jacs.6c10046","type":"journal-article","created":{"date-parts":[[2026,7,17]],"date-time":"2026-07-17T21:59:57Z","timestamp":1784325597000},"page":"31472-31486","source":"Crossref","is-referenced-by-count":1,"title":["Surface-Confinement\nEffect Enables Bioorthogonal Drug\nRelease in Tumors"],"prefix":"10.1021","volume":"148","author":[{"given":"Zhiyu","family":"Tu","sequence":"first","affiliation":[{"name":"Peking University , , ,","place":["Beijing, China, 100871"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ziyang","family":"Sang","sequence":"additional","affiliation":[{"name":"Peking University , , ,","place":["Beijing, China, 100871"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yang","family":"Xu","sequence":"additional","affiliation":[{"name":"Peking University , , ,","place":["Beijing, China, 100871"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Junshi","family":"Ao","sequence":"additional","affiliation":[{"name":"Peking University , , ,","place":["Beijing, China, 100871"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yihang","family":"Chen","sequence":"additional","affiliation":[{"name":"Peking University , , ,","place":["Beijing, China, 100871"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Weiqiu","family":"Liang","sequence":"additional","affiliation":[{"name":"Peking University , , ,","place":["Beijing, China, 100871"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Junyi","family":"Chen","sequence":"additional","affiliation":[{"name":"Peking University , , ,","place":["Beijing, China, 100871"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5587-4165","authenticated-orcid":true,"given":"Zhibo","family":"Liu","sequence":"additional","affiliation":[{"name":"Peking University , , ,","place":["Beijing, China, 100871"]},{"name":"Changping Laboratory , ,","place":["Beijing, China, 102206"]},{"name":"Peking University Cancer Hospital & Institute , , ,","place":["Beijing, China, 100142"]},{"name":"Peking University , , ,","place":["Beijing, China, 100871"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,7,17]]},"reference":[{"key":"2026073109204149400_cit1","doi-asserted-by":"publisher","first-page":"12","DOI":"10.3322\/caac.21820","article-title":"Cancer statistics, 2024","volume":"74","author":"Siegel","year":"2024","journal-title":"Ca-Cancer J. Clin."},{"key":"2026073109204149400_cit2","doi-asserted-by":"publisher","first-page":"1129","DOI":"10.1002\/cncr.21324","article-title":"The role of radiotherapy\nin cancer treatment","volume":"104","author":"Delaney","year":"2005","journal-title":"Cancer"},{"key":"2026073109204149400_cit3","doi-asserted-by":"publisher","first-page":"171","DOI":"10.1016\/S0140-6736(21)00233-6","article-title":"Contemporary radiotherapy:\nPresent and future","volume":"398","author":"Chandra","year":"2021","journal-title":"The Lancet"},{"key":"2026073109204149400_cit4","doi-asserted-by":"publisher","first-page":"527","DOI":"10.1038\/nrclinonc.2015.120","article-title":"Opportunities and\nchallenges of radiotherapy for treating\ncancer","volume":"12","author":"Schaue","year":"2015","journal-title":"Nat. Rev. Clin. Oncol."},{"issue":"4","key":"2026073109204149400_cit5","doi-asserted-by":"publisher","DOI":"10.1016\/S1470-2045(24)00664-8","article-title":"Innovative, early-phase\nclinical trials of drug\u2013radiotherapy combinations","volume":"26","author":"Levy","year":"2025","journal-title":"Lancet Oncol."},{"key":"2026073109204149400_cit6","doi-asserted-by":"publisher","first-page":"215969","DOI":"10.1016\/j.canlet.2022.215969","article-title":"Drug conjugate-based\nanticancer therapy - Current status\nand perspectives","volume":"552","author":"Yang","year":"2023","journal-title":"Cancer Lett."},{"key":"2026073109204149400_cit7","doi-asserted-by":"publisher","first-page":"21546","DOI":"10.1002\/anie.202005612","article-title":"External-Radiation-Induced\nLocal Hydroxylation Enables Remote Release\nof Functional Molecules in Tumors","volume":"59","author":"Fu","year":"2020","journal-title":"Angew. Chem.,\nInt. 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Cancer Res."},{"key":"2026073109204149400_cit24","doi-asserted-by":"publisher","first-page":"18698","DOI":"10.1021\/jacs.3c04602","article-title":"Nanoscale Metal\u2013Organic\nFramework with an X-ray Triggerable Prodrug for Synergistic Radiotherapy\nand Chemotherapy","volume":"145","author":"Xu","year":"2023","journal-title":"J. Am. Chem. Soc."},{"key":"2026073109204149400_cit25","doi-asserted-by":"publisher","first-page":"33149","DOI":"10.1021\/jacs.4c12140","article-title":"Nanoscale Mixed-Ligand Metal\u2013Organic Framework for X-ray Stimulated\nCancer Therapy","volume":"146","author":"Zhen","year":"2024","journal-title":"J. Am. Chem. 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Am. Chem. Soc."},{"key":"2026073109204149400_cit29","doi-asserted-by":"publisher","first-page":"944","DOI":"10.1021\/accountsmr.1c00161","article-title":"Nanoscale\nMetal\u2013Organic Layers for Biomedical\nApplications","volume":"2","author":"Xu","year":"2021","journal-title":"Acc. Mater. Res."},{"key":"2026073109204149400_cit30","doi-asserted-by":"publisher","first-page":"7763","DOI":"10.1039\/C6RA26663K","article-title":"Formation mechanism\nof hafnium oxide nanoparticles by a hydrothermal\nroute","volume":"7","author":"Wan","year":"2017","journal-title":"RSC Adv."},{"key":"2026073109204149400_cit31","doi-asserted-by":"publisher","first-page":"2351","DOI":"10.1038\/s41467-018-04703-w","article-title":"Nanoscale metal-organic\nframeworks enhance radiotherapy to potentiate checkpoint blockade\nimmunotherapy","volume":"9","author":"Ni","year":"2018","journal-title":"Nat. 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Chem."},{"key":"2026073109204149400_cit35","doi-asserted-by":"publisher","first-page":"12873","DOI":"10.1002\/anie.201705873","article-title":"HKOH-1: A Highly Sensitive\nand Selective Fluorescent Probe for Detecting Endogenous Hydroxyl\nRadicals in Living Cells","volume":"56","author":"Bai","year":"2017","journal-title":"Angew. Chem., Int.\nEd."},{"key":"2026073109204149400_cit36","doi-asserted-by":"publisher","first-page":"633","DOI":"10.3109\/00498259309059401","article-title":"Generalized cytochrome P450-mediated oxidation and\noxygenation reactions in aromatic substrates with activated N-H, O-H,\nC-H, or S-H substituents","volume":"23","author":"Koymans","year":"1993","journal-title":"Xenobiotica"},{"key":"2026073109204149400_cit37","doi-asserted-by":"publisher","first-page":"1169","DOI":"10.1039\/p29960001169","article-title":"Substrate-dependent\nchanges of the\noxidative O-dealkylation mechanism of several chemical and biological\noxidizing systems","volume":"25","author":"Urano","year":"1996","journal-title":"J. Chem. Soc., Perkin Trans.\n2"},{"key":"2026073109204149400_cit38","doi-asserted-by":"publisher","first-page":"1391","DOI":"10.1039\/b002191l","article-title":"The reaction of the OH radical with\npentafluoro-, pentachloro-, pentabromo- and 2,4,6-triiodophenol in\nwater: Electron transfer vs. addition to the ring","volume":"29","author":"Fang","year":"2000","journal-title":"J. Chem. Soc., Perkin Trans. 2"},{"issue":"4","key":"2026073109204149400_cit39","doi-asserted-by":"publisher","first-page":"1336","DOI":"10.1039\/D1CS00451D","article-title":"Metal-free\nbioorthogonal click chemistry\nin cancer theranostics","volume":"51","author":"Wu","year":"2022","journal-title":"Chem. Soc. 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Rev."},{"key":"2026073109204149400_cit43","doi-asserted-by":"publisher","first-page":"437","DOI":"10.1038\/nrc1367","article-title":"Exploiting tumour hypoxia in cancer\ntreatment","volume":"4","author":"Brown","year":"2004","journal-title":"Nat. Rev. Cancer"},{"issue":"1","key":"2026073109204149400_cit44","first-page":"80","article-title":"Efficacy\nof Camptothecin Analog DX-8951f\n(Exatecan Mesylate) on Human Pancreatic Cancer in an Orthotopic Metastatic\nModel1","volume":"63","author":"Sun","year":"2003","journal-title":"Cancer Res."},{"key":"2026073109204149400_cit45","doi-asserted-by":"publisher","first-page":"166","DOI":"10.1038\/s41586-022-04437-2","article-title":"Effective drug combinations\nin breast, colon and pancreatic cancer cells","volume":"603","author":"Jaaks","year":"2022","journal-title":"Nature"},{"key":"2026073109204149400_cit46","doi-asserted-by":"publisher","first-page":"399","DOI":"10.1038\/s41577-023-00973-8","article-title":"Immunotherapy combination approaches: Mechanisms, biomarkers\nand clinical observations","volume":"24","author":"Butterfield","year":"2024","journal-title":"Nat. Rev. Immunol."},{"key":"2026073109204149400_cit47","doi-asserted-by":"publisher","first-page":"19","DOI":"10.1016\/j.addr.2015.10.022","article-title":"Recent advances of cocktail chemotherapy\nby combination drug delivery systems","volume":"98","author":"Hu","year":"2016","journal-title":"Adv. Drug\nDelivery Rev."},{"key":"2026073109204149400_cit48","doi-asserted-by":"publisher","first-page":"57","DOI":"10.1038\/nrclinonc.2016.96","article-title":"Combine and conquer: Challenges for targeted therapy\ncombinations in early phase trials","volume":"14","author":"Lopez","year":"2017","journal-title":"Nat. Rev.\nClin. Oncol."}],"container-title":["Journal of\nthe American\nChemical Society"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/pubs.acs.org\/doi\/pdf\/10.1021\/jacs.6c10046","content-type":"application\/pdf","content-version":"vor","intended-application":"unspecified"},{"URL":"https:\/\/pubs.acs.org\/jacsat\/article-pdf\/148\/29\/31472\/66343880\/jacs.6c10046.pdf","content-type":"application\/pdf","content-version":"vor","intended-application":"syndication"},{"URL":"https:\/\/pubs.acs.org\/jacsat\/article-pdf\/148\/29\/31472\/66343880\/jacs.6c10046.pdf","content-type":"unspecified","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2026,7,31]],"date-time":"2026-07-31T13:20:49Z","timestamp":1785504049000},"score":1,"resource":{"primary":{"URL":"https:\/\/pubs.acs.org\/jacsat\/article\/148\/29\/31472\/5237461\/Surface-Confinement-Effect-Enables-Bioorthogonal"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2026,7,17]]},"references-count":48,"journal-issue":{"issue":"29","published-online":{"date-parts":[[2026,7,17]]},"published-print":{"date-parts":[[2026,7,29]]}},"URL":"https:\/\/doi.org\/10.1021\/jacs.6c10046","relation":{},"ISSN":["0002-7863","1520-5126"],"issn-type":[{"value":"0002-7863","type":"print"},{"value":"1520-5126","type":"electronic"}],"subject":[],"published":{"date-parts":[[2026,7,17]]}}}