Kwangwook Ko, Piper L. MacNicol, Mingming Zhu, Lei Zhang, Saifudin M. Abubakar and Jeremiah A. Johnson*,
{"title":"Entropy Drives the Predictive Discovery of an Optimal Cleavable Comonomer for ROMP","authors":"Kwangwook Ko, Piper L. MacNicol, Mingming Zhu, Lei Zhang, Saifudin M. Abubakar and Jeremiah A. Johnson*, ","doi":"10.1021/acscentsci.5c00521","DOIUrl":"https://doi.org/10.1021/acscentsci.5c00521","url":null,"abstract":"<p >Ring-opening metathesis polymerization (ROMP) of norbornene derivatives enables access to polymeric materials for applications ranging from targeted drug delivery to high-performance thermosets; however, the carbon–carbon backbones of ROMP-derived poly(norbornenes) resist deconstruction under mild, selective conditions. Cleavable comonomers (CCs) have been introduced to address this limitation, yet their implementation has been hindered by prohibitive costs and/or suboptimal reactivity. Moreover, the discovery of existing CCs has been largely empirical, lacking clear design principles. Here, we identify the entropy of ring-opening as one of the key determinants of ROMP copolymerization behavior of the best-performing CCs reported to date. Guided by this insight, we establish predictive design criteria and introduce <b>Me</b><sub><b>4</b></sub><b>Si</b><sub><b>2</b></sub><b>O9</b>, a CC that exhibits near-ideal room temperature copolymerization with a broad range of norbornene-based (macro)monomers. <b>Me</b><sub><b>4</b></sub><b>Si</b><sub><b>2</b></sub><b>O9</b> is significantly less expensive than leading silyl ether-based CCs and enables uniform incorporation of cleavable linkages into polymer backbones at low loadings. Beyond delivering a cost-effective and high-performance CC, this work provides fundamental insights into ROMP copolymerization that will enable predictive CC development and expand the functional scope of deconstructable polymeric materials.</p><p >A novel predictive workflow and entropy-maximizing design enabled the development of a cost-effective cleavable comonomer─<b>Me</b><sub><b>4</b></sub><b>Si</b><sub><b>2</b></sub><b>O9</b>─that uniformly embeds deconstructable bonds in ROMP-derived polymers.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 8","pages":"1408–1416"},"PeriodicalIF":10.4,"publicationDate":"2025-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acscentsci.5c00521","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144902052","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Lauren M. Orr, Sydney J. Tomlinson, Hannah R. Grupe, Melissa Lim, Emily Ho, Halime Yilmaz, Grace Zhou, Barbara Leon, James A. Olzmann* and Daniel K. Nomura*,
{"title":"","authors":"Lauren M. Orr, Sydney J. Tomlinson, Hannah R. Grupe, Melissa Lim, Emily Ho, Halime Yilmaz, Grace Zhou, Barbara Leon, James A. Olzmann* and Daniel K. Nomura*, ","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 7","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":12.7,"publicationDate":"2025-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acscentsci.5c00959","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144678344","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Brian Choi, Toby G. Johnson, Arthur Acuña, Hader E. Elashal and A. James Link*,
{"title":"","authors":"Brian Choi, Toby G. Johnson, Arthur Acuña, Hader E. Elashal and A. James Link*, ","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 7","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":12.7,"publicationDate":"2025-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acscentsci.5c00408","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144678375","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Hyejin Lee, Hongjun Jang, Hwan Myung, Angela Rivera, Anna F. Averette, Joseph Heitman, Jiyong Park, Deukjoon Kim, Hyoungsu Kim and Jiyong Hong*,
{"title":"","authors":"Hyejin Lee, Hongjun Jang, Hwan Myung, Angela Rivera, Anna F. Averette, Joseph Heitman, Jiyong Park, Deukjoon Kim, Hyoungsu Kim and Jiyong Hong*, ","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 7","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":12.7,"publicationDate":"2025-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acscentsci.5c00332","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144678376","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Maria Sara Raju, Maxime Aragon-Alberti, Kevin Cardenas, Ivan Breslavetz, Geert L. J. A. Rikken, Cyrille Train and Matteo Atzori*,
{"title":"","authors":"Maria Sara Raju, Maxime Aragon-Alberti, Kevin Cardenas, Ivan Breslavetz, Geert L. J. A. Rikken, Cyrille Train and Matteo Atzori*, ","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 7","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":12.7,"publicationDate":"2025-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acscentsci.5c00772","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144678377","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Suman Mandal, Minh Dang Nguyen, Nikhil Ranjan Jana* and T. Randall Lee*,
{"title":"","authors":"Suman Mandal, Minh Dang Nguyen, Nikhil Ranjan Jana* and T. Randall Lee*, ","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 7","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":12.7,"publicationDate":"2025-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acscentsci.5c00519","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144678379","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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