{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,9,1]],"date-time":"2026-09-01T09:18:44Z","timestamp":1788254324162,"version":"build-2803163510"},"reference-count":60,"publisher":"American Chemical Society (ACS)","issue":"33","license":[{"start":{"date-parts":[[2026,8,12]],"date-time":"2026-08-12T00:00:00Z","timestamp":1786492800000},"content-version":"vor","delay-in-days":0,"URL":"https:\/\/creativecommons.org\/licenses\/by-nc-nd\/4.0\/"}],"funder":[{"DOI":"10.13039\/100000057","name":"National Institute of General Medical Sciences","doi-asserted-by":"publisher","award":["1R35GM154998"],"award-info":[{"award-number":["1R35GM154998"]}],"id":[{"id":"10.13039\/100000057","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/100000057","name":"National Institute of General Medical Sciences","doi-asserted-by":"publisher","award":["1R35GM155450"],"award-info":[{"award-number":["1R35GM155450"]}],"id":[{"id":"10.13039\/100000057","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/100000057","name":"National Institute of General Medical Sciences","doi-asserted-by":"publisher","award":["P20GM113131"],"award-info":[{"award-number":["P20GM113131"]}],"id":[{"id":"10.13039\/100000057","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/100000078","name":"Division of Materials Research","doi-asserted-by":"publisher","award":["2340569"],"award-info":[{"award-number":["2340569"]}],"id":[{"id":"10.13039\/100000078","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/100000078","name":"Division of Materials Research","doi-asserted-by":"publisher","award":["2443178"],"award-info":[{"award-number":["2443178"]}],"id":[{"id":"10.13039\/100000078","id-type":"DOI","asserted-by":"publisher"}]}],"content-domain":{"domain":[],"crossmark-restriction":false},"short-container-title":[],"published-print":{"date-parts":[[2026,8,26]]},"abstract":"<jats:title>Abstract<\/jats:title>\n                  <jats:p>A central challenge in biomaterials design is developing cross-linking reactions that are fast, selective, synthetically accessible, and compatible with the nucleophile-rich environments required for cell encapsulation. Native chemical ligation (NCL) offers an attractive route to amide-linked hydrogels under mild aqueous conditions, yet its implementation in biomaterials has been constrained by slow kinetics, free-thiol byproducts, and inhibition in complex media. Here, we demonstrate that deliberate electrophile design through incorporation of a strain-encoded \u03b2-thiolactone enables rapid and selective NCL-mediated hydrogel formation through rapid recyclization of off-target intermediates. A penicillamine-derived \u03b2-thiolactone cross-linker synthesized directly on four-arm polyethylene glycol (PEG, 10 kDa) exhibits fast gelation in complete cell culture media while maintaining orthogonality to embedded human dermal fibroblasts. Relative to a conventional alkyl thioester and a \u03b3-thiolactone analogue, the strained \u03b2-thiolactone displays accelerated gelation and enhanced tolerance to competing endogenous thiols. Mechanistically, geminal dimethyl substitution promotes rapid \u03b2-thiolactone recyclization, suppressing unproductive thiol exchange while productive NCL proceeds through an irreversible S-to-N acyl shift. Because unreacted \u03b2-thiolactones persist under physiological conditions, the network remains chemically addressable after gelation, enabling temporally delayed functionalization with N-Cys-containing molecules. This combination of rapid network formation and postgelation addressability enables direct peptide incorporation, hydrogel microfiber fabrication, and long-term three-dimensional cell encapsulation.<\/jats:p>","DOI":"10.1021\/jacs.6c05244","type":"journal-article","created":{"date-parts":[[2026,8,12]],"date-time":"2026-08-12T07:02:23Z","timestamp":1786518143000},"page":"35411-35423","source":"Crossref","is-referenced-by-count":0,"title":["Strain-Accelerated\n\u03b2-Thiolactone Native\nChemical Ligation with Kinetic Control Enables Rapid and Selective\nHydrogelation for Biofabrication"],"prefix":"10.1021","volume":"148","author":[{"given":"Matthew E.","family":"Currier","sequence":"first","affiliation":[{"name":"University of New Hampshire , , 23 Academic Way, Parsons Hall , , ,","place":["Durham, New Hampshire, United States, 03824"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4060-9959","authenticated-orcid":true,"given":"Tran M.","family":"Truong","sequence":"additional","affiliation":[{"name":"University of New Hampshire , , 23 Academic Way, Parsons Hall , , ,","place":["Durham, New Hampshire, United States, 03824"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Dylan M.","family":"Sager","sequence":"additional","affiliation":[{"name":"University of New Hampshire , , 23 Academic Way, Parsons Hall , , ,","place":["Durham, New Hampshire, United States, 03824"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kaelin E.","family":"Marshall","sequence":"additional","affiliation":[{"name":"University of New Hampshire , , 23 Academic Way, Parsons Hall , , ,","place":["Durham, New Hampshire, United States, 03824"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-3003-9902","authenticated-orcid":true,"given":"Linqing","family":"Li","sequence":"additional","affiliation":[{"name":"University of New Hampshire , , 33 Academic Way, Kingsbury Hall, Room W301 , , ,","place":["Durham, New Hampshire, United States, 03824"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0000-1555-5533","authenticated-orcid":true,"given":"Nathan J.","family":"Oldenhuis","sequence":"additional","affiliation":[{"name":"University of New Hampshire , , 23 Academic Way, Parsons Hall , , ,","place":["Durham, New Hampshire, United States, 03824"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,12]]},"reference":[{"issue":"5","key":"2026090104513555700_cit1","doi-asserted-by":"publisher","first-page":"405","DOI":"10.1038\/nmeth.3839","article-title":"A Practical Guide to Hydrogels for Cell Culture","volume":"13","author":"Caliari","year":"2016","journal-title":"Nat. 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Eng."},{"issue":"11","key":"2026090104513555700_cit5","doi-asserted-by":"publisher","first-page":"1612","DOI":"10.1039\/C4BM00187G","article-title":"Design of thiol\u2013ene\nphotoclick hydrogels using\nfacile techniques for cell culture applications","volume":"2","author":"Sawicki","year":"2014","journal-title":"Biomater. Sci."},{"issue":"38","key":"2026090104513555700_cit6","doi-asserted-by":"publisher","first-page":"6974","DOI":"10.1002\/anie.200900942","article-title":"Bioorthogonal Chemistry: Fishing for Selectivity in\na Sea of Functionality","volume":"48","author":"Sletten","year":"2009","journal-title":"Angew. Chem., Int. Ed."},{"issue":"1","key":"2026090104513555700_cit7","doi-asserted-by":"publisher","DOI":"10.1002\/chem.202502315","article-title":"Bioorthogonal\nChemistry in Biomolecule Quantification: A Review of\nReactions and Strategies","volume":"32","author":"Yang","year":"2026","journal-title":"Chem. - Eur. 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Sci."},{"issue":"52","key":"2026090104513555700_cit28","doi-asserted-by":"publisher","first-page":"14070","DOI":"10.1002\/anie.201308007","article-title":"A Dendritic\nThioester Hydrogel Based on Thiol\u2013Thioester Exchange as a Dissolvable\nSealant System for Wound Closure","volume":"52","author":"Ghobril","year":"2013","journal-title":"Angew. Chem.,\nInt. Ed."},{"issue":"38","key":"2026090104513555700_cit29","doi-asserted-by":"publisher","first-page":"23637","DOI":"10.1039\/D1RA01934A","article-title":"On-Demand Retrieval\nof Cells Three-Dimensionally Seeded in Injectable Thioester-Based\nHydrogels","volume":"11","author":"Ishikawa","year":"2021","journal-title":"RSC Adv."},{"issue":"7","key":"2026090104513555700_cit30","doi-asserted-by":"publisher","first-page":"1982","DOI":"10.1039\/C7SC04744D","article-title":"Coupling of Sterically\nDemanding Peptides by \u03b2-Thiolactone-Mediated Native Chemical\nLigation","volume":"9","author":"Chen","year":"2018","journal-title":"Chem. Sci."},{"issue":"9","key":"2026090104513555700_cit31","doi-asserted-by":"publisher","first-page":"4068","DOI":"10.1021\/jo500577c","article-title":"Chemistry\nof the \u03b2-Thiolactones:\nSubstituent and Solvent Effects on Thermal Decomposition and Comparison\nwith the \u03b2-Lactones","volume":"79","author":"Noel","year":"2014","journal-title":"J. Org. Chem."},{"issue":"9","key":"2026090104513555700_cit32","doi-asserted-by":"publisher","first-page":"3389","DOI":"10.1021\/jo9001728","article-title":"S N2-Type Nucleophilic\nOpening of \u03b2-Thiolactones (Thietan-2-Ones)\nas a Source of Thioacids for Coupling Reactions","volume":"74","author":"Crich","year":"2009","journal-title":"J. Org. Chem."},{"issue":"5","key":"2026090104513555700_cit33","doi-asserted-by":"publisher","first-page":"1735","DOI":"10.1021\/cr940337h","article-title":"Gem-Disubstituent Effect: Theoretical Basis and Synthetic\nApplications","volume":"105","author":"Jung","year":"2005","journal-title":"Chem. 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A."},{"issue":"2","key":"2026090104513555700_cit36","doi-asserted-by":"publisher","first-page":"367","DOI":"10.1122\/1.549853","article-title":"Analysis of Linear\nViscoelasticity of a Crosslinking\nPolymer at the Gel Point","volume":"30","author":"Winter","year":"1986","journal-title":"J. Rheol."},{"issue":"20","key":"2026090104513555700_cit37","doi-asserted-by":"publisher","first-page":"7762","DOI":"10.1021\/ma049072r","article-title":"Rheological\nMonitoring of Polyacrylamide\nGelation: Importance of Cross-Link Density and Temperature","volume":"37","author":"Calvet","year":"2004","journal-title":"Macromolecules"},{"issue":"4","key":"2026090104513555700_cit38","doi-asserted-by":"publisher","first-page":"541","DOI":"10.1122\/1.4948428","article-title":"Universal Aspects\nof Hydrogel Gelation Kinetics, Percolation\nand Viscoelasticity from PA-Hydrogel Rheology","volume":"60","author":"Adibnia","year":"2016","journal-title":"J. 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Cell Sci."},{"key":"2026090104513555700_cit48","doi-asserted-by":"publisher","first-page":"24","DOI":"10.1016\/j.biomaterials.2018.06.042","article-title":"Cellular Interactions\nwith Hydrogel\nMicrofibers Synthesized via Interfacial Tetrazine\nLigation","volume":"180","author":"Liu","year":"2018","journal-title":"Biomaterials"},{"issue":"5","key":"2026090104513555700_cit49","doi-asserted-by":"publisher","first-page":"299","DOI":"10.1093\/rb\/rbx017","article-title":"Wet-Spinning\nFabrication of Shear-Patterned Alginate Hydrogel Microfibers and the\nGuidance of Cell Alignment","volume":"4","author":"Yang","year":"2017","journal-title":"Regener. Biomater."},{"issue":"7","key":"2026090104513555700_cit50","doi-asserted-by":"publisher","first-page":"3017","DOI":"10.1021\/acs.biomac.2c00504","article-title":"Tunable Synthesis of\nHydrogel Microfibers via Interfacial Tetrazine Ligation","volume":"23","author":"George","year":"2022","journal-title":"Biomacromolecules"},{"issue":"3","key":"2026090104513555700_cit51","doi-asserted-by":"publisher","first-page":"326","DOI":"10.1038\/nmat4489","article-title":"Hydrogels with Tunable\nStress Relaxation\nRegulate Stem Cell Fate and Activity","volume":"15","author":"Chaudhuri","year":"2016","journal-title":"Nat. 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