{"title":"离散丁内酯-己内酯共聚物的结晶和熔融行为:端基的影响","authors":"Huijun Xu, Ao Feng, Zhihao Huang, Rui Tan, Zefan Wang, Xiaohua Zhang, Zhengbiao Zhang","doi":"10.1021/acs.macromol.5c00593","DOIUrl":null,"url":null,"abstract":"Discrete oligomers are ideal candidates for the investigation of the crystallization behaviors of polymers since the molecular weight distribution and the precision of molecular structures play a crucial role in the crystallization behaviors of polymers. We precisely synthesize discrete alternative co-oligomers (<i>o</i>(γ-BL-<i>alt</i>-ε-CL)s) with different end groups based on ε-caprolactone (ε-CL) and γ-butyrolactone (γ-BL) as monomers using an iterative exponential growth (IEG) strategy and systematically study the crystallization and melting behaviors of the <i>o</i>(γ-BL-<i>alt</i>-ε-CL)s with precise monomer sequence. The roles that the end group plays in the crystallization and melting of co-oligomers are highlighted. The <i>o</i>(γ-BL-<i>alt</i>-ε-CL)s with different end groups (<i>tert</i>-butyldiphenylsilyl, benzoyl, acetyl) crystallize in an extended-chain conformation. Observation on the decrease of the crystallization rate of co-oligomers with the increase of the size of the end groups is associated with the slow dynamics or slow relaxation of co-oligomer chains with the large end group. The melting–recrystallization during the heating process for the <i>o</i>(γ-BL-<i>alt</i>-ε-CL)s with small end group is attributed primarily to the reduced steric hindrance effect. For the <i>o</i>(γ-BL-<i>alt</i>-ε-CL)s with large end groups, the rearrangement of co-oligomer chains is substantially hindered by steric effects, which lead to a significant suppression of the melting–recrystallization.","PeriodicalId":51,"journal":{"name":"Macromolecules","volume":"35 1","pages":""},"PeriodicalIF":5.1000,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Crystallization and Melting Behaviors of Discrete Butyolactone–Caprolactone Alternative Co-Oligomer: The Effect of End Groups\",\"authors\":\"Huijun Xu, Ao Feng, Zhihao Huang, Rui Tan, Zefan Wang, Xiaohua Zhang, Zhengbiao Zhang\",\"doi\":\"10.1021/acs.macromol.5c00593\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Discrete oligomers are ideal candidates for the investigation of the crystallization behaviors of polymers since the molecular weight distribution and the precision of molecular structures play a crucial role in the crystallization behaviors of polymers. We precisely synthesize discrete alternative co-oligomers (<i>o</i>(γ-BL-<i>alt</i>-ε-CL)s) with different end groups based on ε-caprolactone (ε-CL) and γ-butyrolactone (γ-BL) as monomers using an iterative exponential growth (IEG) strategy and systematically study the crystallization and melting behaviors of the <i>o</i>(γ-BL-<i>alt</i>-ε-CL)s with precise monomer sequence. The roles that the end group plays in the crystallization and melting of co-oligomers are highlighted. The <i>o</i>(γ-BL-<i>alt</i>-ε-CL)s with different end groups (<i>tert</i>-butyldiphenylsilyl, benzoyl, acetyl) crystallize in an extended-chain conformation. Observation on the decrease of the crystallization rate of co-oligomers with the increase of the size of the end groups is associated with the slow dynamics or slow relaxation of co-oligomer chains with the large end group. The melting–recrystallization during the heating process for the <i>o</i>(γ-BL-<i>alt</i>-ε-CL)s with small end group is attributed primarily to the reduced steric hindrance effect. For the <i>o</i>(γ-BL-<i>alt</i>-ε-CL)s with large end groups, the rearrangement of co-oligomer chains is substantially hindered by steric effects, which lead to a significant suppression of the melting–recrystallization.\",\"PeriodicalId\":51,\"journal\":{\"name\":\"Macromolecules\",\"volume\":\"35 1\",\"pages\":\"\"},\"PeriodicalIF\":5.1000,\"publicationDate\":\"2025-04-24\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Macromolecules\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1021/acs.macromol.5c00593\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"POLYMER SCIENCE\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Macromolecules","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/acs.macromol.5c00593","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"POLYMER SCIENCE","Score":null,"Total":0}
Crystallization and Melting Behaviors of Discrete Butyolactone–Caprolactone Alternative Co-Oligomer: The Effect of End Groups
Discrete oligomers are ideal candidates for the investigation of the crystallization behaviors of polymers since the molecular weight distribution and the precision of molecular structures play a crucial role in the crystallization behaviors of polymers. We precisely synthesize discrete alternative co-oligomers (o(γ-BL-alt-ε-CL)s) with different end groups based on ε-caprolactone (ε-CL) and γ-butyrolactone (γ-BL) as monomers using an iterative exponential growth (IEG) strategy and systematically study the crystallization and melting behaviors of the o(γ-BL-alt-ε-CL)s with precise monomer sequence. The roles that the end group plays in the crystallization and melting of co-oligomers are highlighted. The o(γ-BL-alt-ε-CL)s with different end groups (tert-butyldiphenylsilyl, benzoyl, acetyl) crystallize in an extended-chain conformation. Observation on the decrease of the crystallization rate of co-oligomers with the increase of the size of the end groups is associated with the slow dynamics or slow relaxation of co-oligomer chains with the large end group. The melting–recrystallization during the heating process for the o(γ-BL-alt-ε-CL)s with small end group is attributed primarily to the reduced steric hindrance effect. For the o(γ-BL-alt-ε-CL)s with large end groups, the rearrangement of co-oligomer chains is substantially hindered by steric effects, which lead to a significant suppression of the melting–recrystallization.
期刊介绍:
Macromolecules publishes original, fundamental, and impactful research on all aspects of polymer science. Topics of interest include synthesis (e.g., controlled polymerizations, polymerization catalysis, post polymerization modification, new monomer structures and polymer architectures, and polymerization mechanisms/kinetics analysis); phase behavior, thermodynamics, dynamic, and ordering/disordering phenomena (e.g., self-assembly, gelation, crystallization, solution/melt/solid-state characteristics); structure and properties (e.g., mechanical and rheological properties, surface/interfacial characteristics, electronic and transport properties); new state of the art characterization (e.g., spectroscopy, scattering, microscopy, rheology), simulation (e.g., Monte Carlo, molecular dynamics, multi-scale/coarse-grained modeling), and theoretical methods. Renewable/sustainable polymers, polymer networks, responsive polymers, electro-, magneto- and opto-active macromolecules, inorganic polymers, charge-transporting polymers (ion-containing, semiconducting, and conducting), nanostructured polymers, and polymer composites are also of interest. Typical papers published in Macromolecules showcase important and innovative concepts, experimental methods/observations, and theoretical/computational approaches that demonstrate a fundamental advance in the understanding of polymers.