橡胶基体与补强剂粒子通过界面相互作用而形成高度"结构化"的三维黏弹性材料.讨论了结合橡胶(BdR)形成机制、分子弛豫特性、补强机理、非线性黏弹性的基础研究进展,分析了已有研究结果所存在的矛盾或争议,结合本课题组在高填充橡胶材料黏弹性方面的研究,探讨了结构-性能关系并提出展望.虽然BdR形成机制(物理吸附、化学吸附)、补强机理(针对"孤立粒子"的Einstein-Smallwood、Guth-Gold方程及其修正形成、针对"粒子团簇"的粒子簇动态团聚模型、针对"粒子网络"的逾渗模型和拥挤网络模型)、非线性行为(粒子-粒子相互作用说、粒子-橡胶(界面)相互作用说、粒子网络说、互穿网络说)等长期存在争议,长达一个多世纪的研究已基本弄清橡胶材料的结构(动力学)非均质性、应变(应变速率)放大效应、界面相互作用(粒子表面高分子存在能动性梯度)等基本事实.在分析BdR对橡胶黏弹行为影响研究结果的基础上,提出今后橡胶科学研究的两个重要方向,即将结构(动力学)非均质性纳入补强与非线性黏弹性理论范畴,以BdR或粒子-橡胶凝胶为纽带建立微观效应(多时间尺度的分子运动、多空间尺度的粒子分散状态)-宏观性能关系.
Highly filled elastomers are "structured"three-dimensionally viscoelastic materials formed through interfacial interactions between the rubbery matrix and the fine reinforcing particles such as carbon black and silica.There exist great disputes or contradictory research results about mechanisms of the formation(physical or chemical absorption) of bound rubber(BdR),molecular relaxation of the matrix,reinforcement(EinsteinSmallwood and Guth-Gold equations and their modified forms for "isolated particles",dynamic cluster-cluster aggregation model for"particle clusters",and rigidity percolation and jamming models for"particle network") and nonlinear viscoelasticity(hypotheses in relation to destroying and rebuilding of particle-particle interaction,particle-rubber interaction,particle network and particle-rubber interpenetrating network) of highly filled rubbers in a long time.Nevertheless,the structure and dynamics heterogeneities,strain(strain rate) amplification effect introduced by presence of particles,and the interfacial interactions featured by the presence of a molecular dynamics gradient in the close vicinity around the particles become clear and well-accepted throughout the scientific researches more than one century.On the basis of summarizing some primary results involving influences of BdR on the macroscopic viscoelasticity of rubber materials,the authors propose two important research directions for rubber science in relation to their investigating the viscoelasticity of highly filled rubbers.The first one is to include the structure and dynamics heterogeneities in theories of reinforcement and nonlinear viscoelasticity and the second is to create relationships between microscopic effects(molecular relaxation on different time scales and particle dispersion on different spatial scales) and macroscopic properties for rubber materials via BdR or the particle-rubber gel in filled compounds.