{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,8,18]],"date-time":"2026-08-18T16:55:16Z","timestamp":1787072116469,"version":"build-2736575974"},"reference-count":53,"publisher":"American Chemical Society (ACS)","issue":"32","license":[{"start":{"date-parts":[[2026,8,4]],"date-time":"2026-08-04T00:00:00Z","timestamp":1785801600000},"content-version":"vor","delay-in-days":0,"URL":"https:\/\/creativecommons.org\/licenses\/by\/4.0\/"}],"funder":[{"DOI":"10.13039\/501100000741","name":"University of Warwick","doi-asserted-by":"publisher","id":[{"id":"10.13039\/501100000741","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/501100000266","name":"Engineering and Physical Sciences Research Council (EPSRC)","doi-asserted-by":"crossref","award":["EP\/W018977\/1"],"award-info":[{"award-number":["EP\/W018977\/1"]}],"id":[{"id":"10.13039\/501100000266","id-type":"DOI","asserted-by":"crossref"}]}],"content-domain":{"domain":[],"crossmark-restriction":false},"short-container-title":[],"published-print":{"date-parts":[[2026,8,18]]},"abstract":"<jats:title>Abstract<\/jats:title>\n                  <jats:p>Lignin, the most abundant aromatic biopolymer in nature, represents a highly promising renewable feedstock for the development of value-added polymer composites. However, its inherently poor compatibility with elastomeric matrices limits its effective utilization in high-performance and multifunctional lignin-filled systems. In this study, we report a cost-effective and sustainable cross-linking strategy to compatibilize and chemically integrate lignin within an acrylonitrile butadiene rubber (NBR) matrix through interfacial oxazoline chemistry, without the use of conventional sulfur- or peroxide-based curing agents. A small fraction of the pendant nitrile (\u2212C\u2261N) groups of NBR were selectively converted into oxazoline rings via reactive melt compounding. Furthermore, interfacial compatibility was enhanced by incorporating 4 phr ZnCl2, which promotes strong metal\u2013ligand coordination interactions between Zn2+ ions and oxazoline functionalities in the modified NBR. This approach results in the formation of a double cross-linked network comprising (i) permanent covalent linkages generated through oxazoline ring-opening reactions initiated by nucleophilic attack of lignin phenolic hydroxyl (\u2212OH) groups and (ii) dynamic sacrificial networks formed via Zn2+\u2013oxazoline, Zn2+\u2013cyano, and Zn2+\u2013phenolic hydroxyl\/carboxylate coordination interactions involving residual nitrile groups of NBR and phenolic hydroxyl\/Carboxylic acid groups of lignin. The presence of this dual cross-linking architecture significantly enhances mechanical performance. At 60 phr lignin loading, the oxazoline-modified NBR\/ZnCl2 composite exhibits an approximately 129% increase in tensile strength relative to the NBR\/ZnCl2 system without oxazoline modification. In contrast, the unmodified NBR\/ZnCl2 composite containing the same lignin loading shows a comparatively lower tensile strength improvement of 86%. The pronounced reinforcing effect of lignin in the oxazoline-modified system is attributed to its dual function as both a reinforcing filler and reactive cross-linking component, as well as to the synergistic contribution of permanent covalent bonds and reversible coordination interactions within the double cross-linked network.<\/jats:p>","DOI":"10.1021\/acsomega.6c04348","type":"journal-article","created":{"date-parts":[[2026,8,4]],"date-time":"2026-08-04T17:06:46Z","timestamp":1785863206000},"page":"48120-48130","source":"Crossref","is-referenced-by-count":0,"title":["Sustainable Dual\nCross-Linking Strategy of Lignin\nwith Oxazoline-Modified Nitrile Rubber for Mechanically Robust Elastomeric\nComposites"],"prefix":"10.1021","volume":"11","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-1746-8326","authenticated-orcid":true,"given":"Kunal","family":"Manna","sequence":"first","affiliation":[{"name":"University of Warwick , , ,","place":["Coventry, U.K., CV4 7AL"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Samson","family":"Gnanadass","sequence":"additional","affiliation":[{"name":"University of Warwick , , ,","place":["Coventry, U.K., CV4 7AL"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jaipal","family":"Gupta","sequence":"additional","affiliation":[{"name":"University of Warwick , , ,","place":["Coventry, U.K., CV4 7AL"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"James J. C.","family":"Busfield","sequence":"additional","affiliation":[{"name":"Queen Mary University of London , , Mile End Road , ,","place":["London, U.K., E1 4NS"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6465-2871","authenticated-orcid":true,"given":"Biqiong","family":"Chen","sequence":"additional","affiliation":[{"name":"University of Liverpool , , Crown Street , ,","place":["Liverpool, U.K., L69 7ZD"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6686-6005","authenticated-orcid":true,"given":"Ton","family":"Peijs","sequence":"additional","affiliation":[{"name":"University of Warwick , , ,","place":["Coventry, U.K., CV4 7AL"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1079-5885","authenticated-orcid":true,"given":"Chaoying","family":"Wan","sequence":"additional","affiliation":[{"name":"University of Warwick , , ,","place":["Coventry, U.K., CV4 7AL"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,4]]},"reference":[{"key":"2026081811112055700_cit1","doi-asserted-by":"crossref","first-page":"329","DOI":"10.1007\/978-981-97-2075-0_11","article-title":"Elastomeric-Based\nComposite Materials for Engineering Applications","volume-title":"Polymer Composites: Fundamentals and Applications","author":"Sahu","year":"2024"},{"issue":"7","key":"2026081811112055700_cit2","doi-asserted-by":"publisher","first-page":"6550","DOI":"10.1021\/acssuschemeng.8b04936","article-title":"High Performance\nThermoplastic Elastomers with Biomass\nLignin as Plastic Phase","volume":"7","author":"Huang","year":"2019","journal-title":"ACS Sustainable Chem.\nEng."},{"issue":"3","key":"2026081811112055700_cit3","doi-asserted-by":"publisher","first-page":"1811","DOI":"10.1039\/C4GC02409E","article-title":"Utilization\nof Softwood\nLignin as Both Crosslinker and Reinforcing Agent in Silicone Elastomers","volume":"17","author":"Zhang","year":"2015","journal-title":"Green Chem."},{"key":"2026081811112055700_cit4","doi-asserted-by":"publisher","DOI":"10.1016\/j.jclepro.2021.126841","article-title":"Treasuring\nWaste Lignin as Superior\nReinforcing Filler in High Cis-Polybutadiene Rubber: A Direct Comparative\nStudy with Standard Reinforcing Silica and Carbon Black","volume":"299","author":"Hait","year":"2021","journal-title":"J. Cleaner Prod."},{"issue":"15","key":"2026081811112055700_cit5","doi-asserted-by":"publisher","first-page":"5337","DOI":"10.1039\/D1GC01115D","article-title":"Bioresourced\nFillers\nfor Rubber Composite Sustainability: Current Development and Future\nOpportunities","volume":"23","author":"Chang","year":"2021","journal-title":"Green Chem."},{"issue":"5","key":"2026081811112055700_cit6","doi-asserted-by":"publisher","first-page":"1175","DOI":"10.1039\/C5GC02616D","article-title":"Towards Lignin-Based\nFunctional Materials in a Sustainable\nWorld","volume":"18","author":"Kai","year":"2016","journal-title":"Green Chem."},{"issue":"10","key":"2026081811112055700_cit7","doi-asserted-by":"publisher","first-page":"5212","DOI":"10.1021\/acssuschemeng.6b00903","article-title":"New Insights\non the Chemical Modification of Lignin: Acetylation versus Silylation","volume":"4","author":"Buono","year":"2016","journal-title":"ACS Sustainable Chem. 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