{"title":"Molecular Mechanisms of Silicone Network Formation: Bridging Scales from Curing Reactions to Percolation and Entanglement Analyses.","authors":"Pascal Puhlmann, Dirk Zahn","doi":"10.3390/polym17192619","DOIUrl":null,"url":null,"abstract":"<p><p>The curing of silicone networks from dimethylsilanediol and methylsilanetriol chainbuilder-crosslinker precursor mixtures is investigated from combined quantum/molecular mechanics simulations. Upon screening different crosslinker content from 5 to 15%, we provide a series of atomic-resolution bulk models all featuring 98-99% curing degree, albeit at rather different arrangement of the chains and nodes, respectively. To elucidate the nm scale alignment of the polymer networks, we bridge scales from atomic simulation cells to graph theory and demonstrate the analyses of 3-dimensional percolation of -O-Si-O- bonds, polydimethylsiloxane branching characteristics and the interpenetration of loops. Our findings are discussed in the context of the available experimental data to relate heat of formation, curing degree and elastic properties to the molecular scale structural details-thus promoting the in-depth understanding of silicone resins.</p>","PeriodicalId":20416,"journal":{"name":"Polymers","volume":"17 19","pages":""},"PeriodicalIF":4.9000,"publicationDate":"2025-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12526733/pdf/","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Polymers","FirstCategoryId":"5","ListUrlMain":"https://doi.org/10.3390/polym17192619","RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"POLYMER SCIENCE","Score":null,"Total":0}
引用次数: 0
Abstract
The curing of silicone networks from dimethylsilanediol and methylsilanetriol chainbuilder-crosslinker precursor mixtures is investigated from combined quantum/molecular mechanics simulations. Upon screening different crosslinker content from 5 to 15%, we provide a series of atomic-resolution bulk models all featuring 98-99% curing degree, albeit at rather different arrangement of the chains and nodes, respectively. To elucidate the nm scale alignment of the polymer networks, we bridge scales from atomic simulation cells to graph theory and demonstrate the analyses of 3-dimensional percolation of -O-Si-O- bonds, polydimethylsiloxane branching characteristics and the interpenetration of loops. Our findings are discussed in the context of the available experimental data to relate heat of formation, curing degree and elastic properties to the molecular scale structural details-thus promoting the in-depth understanding of silicone resins.
采用量子/分子力学联合模拟的方法研究了由二甲基硅二醇和甲基硅三醇构建链交联剂前驱体混合物形成的硅网络的固化过程。通过筛选不同交联剂含量在5%到15%之间的材料，我们得到了一系列原子分辨率的体模型，它们的固化度都在98-99%之间，尽管它们的链和节点的排列方式不同。为了阐明聚合物网络的纳米尺度排列，我们将原子模拟细胞的尺度连接到图论，并演示了- o - si - o -键的三维渗透、聚二甲基硅氧烷的分支特征和环的相互渗透的分析。我们的研究结果在现有实验数据的背景下进行了讨论，将形成热、固化程度和弹性性能与分子尺度结构细节联系起来，从而促进了对有机硅树脂的深入了解。
期刊介绍：
Polymers (ISSN 2073-4360) is an international, open access journal of polymer science. It publishes research papers, short communications and review papers. Our aim is to encourage scientists to publish their experimental and theoretical results in as much detail as possible. Therefore, there is no restriction on the length of the papers. The full experimental details must be provided so that the results can be reproduced. Polymers provides an interdisciplinary forum for publishing papers which advance the fields of (i) polymerization methods, (ii) theory, simulation, and modeling, (iii) understanding of new physical phenomena, (iv) advances in characterization techniques, and (v) harnessing of self-assembly and biological strategies for producing complex multifunctional structures.
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