MARTINI-based simulation method for step-growth polymerization and its analysis by size exclusion characterization: a case study of cross-linked polyurethane

被引:15
作者
Ghermezcheshme, Hassan [1 ]
Makki, Hesam [1 ]
Mohseni, Mohsen [1 ]
Ebrahimi, Morteza [1 ]
de With, Gijsbertus [2 ]
机构
[1] Amirkabir Univ Technol, Dept Polymer & Color Engn, 424 Hafez Ave, Tehran, Iran
[2] Eindhoven Univ Technol, Dept Chem Engn & Chem, Lab Phys Chem, POB 513, NL-5600 MB Eindhoven, Netherlands
关键词
COARSE-GRAINED MODEL; MOLECULAR-DYNAMICS SIMULATIONS; NANOTUBE NANOCOMPOSITES ROLE; FORCE-FIELD EXTENSION; MULTISCALE SIMULATIONS; MECHANICAL-PROPERTIES; POLYETHYLENE-GLYCOL; THERMAL-PROPERTIES; GLASS-TRANSITION; EPOXY NETWORKS;
D O I
10.1039/c9cp03407b
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Simulation studies of step-growth polymerization, e.g., polymerization of polyurethane systems, hold great promise due to having complete control over the reaction conditions and being able to perform an in-depth analysis of network structures. In this work, we developed a (completely automated) simulation method based on a coarse-grained (CG) methodology, i.e., the MARTINI model, to study the cross-linking reaction of a diol, a tri-isocyanate molecule and one-hydroxyl functional molecule to form a polyurethane network without and with dangling chains. This method is capable of simulating the cross-linking reactions not only up to very high conversions, but also under rather complicated reaction conditions, i.e., a non-stoichiometric ratio of the reactants, solvent evaporation and multi-step addition of the reactants. We introduced a novel network analysis, similar to size-exclusion chromatography based on graph theory, to study the growth of the network during the polymerization process. By combining the reaction simulations with these analysis methods, a set of correlations between the reaction conditions, reaction mechanisms and final network structure and properties is revealed. For instance, a two-step addition of materials for the reaction, i.e., first the dangling chain to the tri-isocyanate and then the diol, leads to the highest integrated network structure. We observed that different reaction conditions lead to different glass transition temperatures (T-g) of the network due to the distinct differences in the final network structures obtained. For example, by addition of dangling chains to the network, the T-g decreases as compared to the network without dangling chains, as also is commonly observed experimentally.
引用
收藏
页码:21603 / 21614
页数:12
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