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Correlation of Cooperatively Localized Rearrangement on the “Fluidized Domain” of Polymers to Their Nonexponentially Viscoelastic Behaviors at Double Aging Processes (I): A Set of Reduced Universal Equations on the Stress Relaxation Modulus and Creep Comp
Ying Liu,Ming-shi Song*,Yan Jin,Gui-xian Hu,Da-ming Wu
Author NameAffiliationE-mail
Ying Liu School of Materials Science and Engineering, Beijing University of Chemical Technology, Beijing 100029, China  
Ming-shi Song* School of Mechanical and Electrical Engineering, Beijing University of Chemical Technology, Beijing 100029, China songmingshi@mail.buct.edu.cn 
Yan Jin School of Materials Science and Engineering, Beijing University of Chemical Technology, Beijing 100029, China  
Gui-xian Hu School of Mechanical and Electrical Engineering, Beijing University of Chemical Technology, Beijing 100029, China  
Da-ming Wu School of Materials Science and Engineering, Beijing University of Chemical Technology, Beijing 100029, China  
Abstract:
Based on the structure of glass (or liquid) polymers consisting of α-domain, β-co-domain, and entanglement constituent chain networks, and the nonexponentially viscoelastic behavior, a “heterophase fluctuation” model was proposed. It was found that the dynamics of cooperative rearrangement on the “fluidized domain” has a great shear rate, domain size, and temperature dependences. When the shear rate, domain size, and temperature dependences were taken account into the cooperatively localized rearrangement on the fluidized domain by the degradation of primary α-domain and the reformation of secondary β-co-domain constituent chains. A new dynamic theory of cooperatively localized rearrangement on the fluidized domain constituent chains with different size and different network chain length during physical and mechanical aging was established. The total viscoelastic free en-ergy of deformation resulting from the change in conformations of α-domain, β-co-domain, crytallite, crosslinked, and trapped entanglement constituent chains during aging processes was calculated by the combining method of kinetics and statistical mechanics. The constitu- tive equations and reduced stress relaxation modulus and creep compliances for three types of polymers were also derived. Finally, two reduced universal equations on creep compliance and stress relaxation modulus with a non-linear and two nonexponential parameters α and β were theoretically derived from the dynamic theory and a statistically extended mode coupling theory for double aging effects of polymers was developed. Results show that the two reduced universal equations have the same form as Kohlraush-Williams-Watts (K-W-W) stretched exponential function. The nonlinearity and the nonexponentiality are, respectively, originated from the memory effects of nonthermal and thermal history. The correlation of nonlinearity, α and β to the aging time, aging temperature, and the mesomorphic structure of fluidized domains was also established.
Key words:  Heterophrase fluctuation model, Kinetics of aging, Dynamics of de-aging, Creep and stress relaxation, K-W-W decay function, Fluidized domain constituent chain
FundProject:
Correlation of Cooperatively Localized Rearrangement on the “Fluidized Domain” of Polymers to Their Nonexponentially Viscoelastic Behaviors at Double Aging Processes (I): A Set of Reduced Universal Equations on the Stress Relaxation Modulus and Creep Comp
刘颖,宋名实*,金艳,胡桂贤,吴大鸣
摘要:
基于α-和β-微区、微晶、交联和缠结链组网络结构和非线性粘弹性复相涨落模型,提出了双重(物理和力学)老化下不同尺寸和末端向量高分子链组的流动化微区内关联性局部化重排动力学新理论,它能把初级α-微区的降解作用和次级β-微区的再生效应对剪切速率、尺寸大小和温度依赖性有机结合起来.然后用统计力学和动力学结合法计算了三种不同类型高聚物在等温等压双重老化过程中多元链组的总构象改变自由能,证实了它起源于多元链组的尺寸大小、形状和体积的变化.推导出了它们单向拉伸下的本构方程、应力松弛模量和蠕变柔量表征式以及它们相对应的两组对比态普适方程.结果表明该两组对比态下应力松弛模量和蠕变柔量普适方程均具有同K-W-W伸展指数函数完全一致的形式.最终又建立了该两组对比态普适方程中三个分子参数同老化条件、温度和高聚物起始结构之间的相关性.
关键词:  复相涨落模型,物理老化动力学,退老化动力学,蠕变和应力松弛,K-W-W衰减函数,流动化微区链组
DOI:10.1088/1674-0068/23/01/45-64
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