高体积含量非线性黏弹复合材料有效性质

提出了一个细观力学模型,可用于预测高体积含量非线性黏弹复合材料有效性质.该模型基于广义割线模量法、双球法以及Laplace-Carson变换技术.所提出的模型对玻璃微珠填充高密度聚乙烯(GB/HDPE)复合材料的应力应变关系进行了预测,结果与文献实验结果吻合;计算结果还表明在高体积百分比下文中所提出的方法比基于MT方法预测的粘性效应明显减弱;最后还将所提方法与线黏弹框架下的均质化模型做了比较,结果表明GB/HDPE表现出明显的非线性,线黏弹本构无法描述应变率对其力学行为的影响.     

A thermodynamic approach to the rheology of highly interactive filler-polymer mixtures. Part II. Comparison with polystyrene/nanosilica mixtures

The dynamic properties as a function of frequency and strain amplitude, steady-state viscosity as a function of shear rate, and transient shear stresses at startup and cessation of shear flow of polystyrene (PS)/fumed silica mixtures of various concentrations were investigated. An abrupt change in the viscoelastic properties was noticed at a concentration above 1% by volume. Observations by means of scanning electron microscopy (SEM) indicate the presence of a three-dimensional network through the bridging of filler particles by the adsorbed polymer. The viscoelastic behavior is simulated utilizing a theory proposed in Part I (Havet and Isayev 2001) based on a double network created by the entangled polymer matrix and the adsorbed polymer with filler concentration taken into account through the bridging density of polymer-filler interactions and a hydrodynamic reinforcement. The steps taken for determining the model parameters required to carry out the simulation are described. The major features of the rheological behavior of highly interactive polymer-filler mixtures are captured qualitatively and in some cases, quantitatively predicted.     

Homogenization of the viscoelastic heterogeneous materials with multi-coated reinforcements: an internal variables formulation

In this work, a new homogenization method to estimate the effective behavior of viscoelastic heterogeneous materials with multi-coated reinforcements is presented. Unlike classical methods that are based on the Laplace transform, the present internal variables formulation operates directly in the time domain. Using the Green’s function techniques, the micromechanical approach is based on establishing a new integral equation adapted to scale transition methods. Using this integral equation, we apply a generalized self-consistent scheme to determine the local stress concentration equations and the effective behavior of multi-coated inclusion-reinforced materials. To assess the reliability of our model, some applications to the isotropic viscoelastic heterogeneous materials with homothetic spherical inclusions are given. The model is applied to the case of two-phase and three-phase materials, and the results are compared to exact solutions. Results for three-phase materials are presented regarding the influence of soft and stiff viscoelastic interphase on the effective behavior of heterogeneous materials.     

Fully resolved simulations of viscoelastic suspensions by an efficient immersed boundary-lattice Boltzmann method

An efficient immersed boundary-lattice Boltzmann method (IB-LBM) is proposed for fully resolved simulations of suspended solid particles in viscoelastic flows. Stress LBM based on Giesekus and Oldroyd-B constitutive equation are used to model the viscoelastic stress tensor. A boundary thickening-based direct forcing IB method is adopted to solve the particle–fluid interactions with high accuracy for non-slip boundary conditions. A universal law is proposed to determine the diffusivity constant in a viscoelastic LBM model to balance the numerical accuracy and stability over a wide range of computational parameters. An asynchronous calculation strategy is adopted to further improve the computing efficiency. The method was firstly applicated to the simulation of sedimentation of a single particle and a pair of particles after good validations in cases of the flow past a fixed cylinder and particle migration in a Couette flow against FEM and FVM methods. The determination of the asynchronous calculation strategy and the effect of viscoelastic stress distribution on the settling behaviors of one and two particles are revealed. Subsequently, 504 particles settling in a closed cavity was simulated and the phenomenon that the viscoelastic stress stabilizing the Rayleigh–Taylor instabilities was observed. At last, simulations of a dense flow involving 11001 particles, the largest number of particles to date, were performed to investigate the instability behavior induced by elastic effect under hydrodynamic interactions in a viscoelastic fluid. The elasticity-induced ordering of the particle structures and fluid bubble structures in this dense flow is revealed for the first time. These simulations demonstrate the capability and prospects of the present method for aid in understanding the complex behaviors of viscoelastic particle suspensions.     

Multi-scale constitutive modeling of the small deformations of semi-crystalline polymers

A multi-scale constitutive model for the small deformations of semi-crystalline polymers such as high density Polyethylene is presented. Each macroscopic material point is supposed to be the center of a representative volume element which is an aggregate of randomly oriented composite inclusions. Each inclusion consists of a stack of parallel crystalline lamellae with their adjacent amorphous layers.Micro-mechanically based constitutive equations are developed for each phase. A viscoplastic model is used for the crystalline lamellae. A new nonlinear viscoelastic model for the amorphous phase behavior is proposed. The model takes into account the fact that the presence of crystallites confines the amorphous phase in extremely thin layers where the concentration of chain entanglements is very high. This gives rise to a stress contribution due to elastic distortion of the chains. It is shown that the introduction of chains’ elastic distortion can explain the viscoelastic behavior of crystalline polymers. The stress contribution from elastic stretching of the tie molecules linking the neighboring lamellae is also taken into account.Next, a constitutive model for a single inclusion considered as a laminated composite is proposed. The macroscopic stress-strain behavior for the whole RVE is found via a Sachs homogenization scheme (uniform stress throughout the material is assumed).Computational algorithms are developed based on fully implicit time-discretization schemes.     

一种预测颗粒增强复合材料界面力学性能的新方法

界面在颗粒增强复合材料中起到传递载荷的关键作用, 界面性能对复合材料整体力学行为产生重要影响. 然而由于复合材料内部结构较为复杂, 颗粒与基体间的界面强度和界面断裂韧性难以确定, 尤其是法向与切向界面强度的分别预测缺乏有效方法. 本文以氧化锆颗粒增强聚二甲基硅氧烷(PDMS)复合材料为研究对象, 提出一种预测颗粒增强复合材料界面力学性能的新方法. 首先, 实验获得纯PDMS基体材料及单颗粒填充PDMS试样的单轴拉伸应力$\!-\!$应变曲线, 标定出PDMS基体材料的单轴拉伸超弹性本构关系; 其次, 建立与单颗粒填充试样一致的有限元模型, 选择特定的黏结区模型描述界面力学行为, 通过样品不同阶段拉伸力学响应的实验与数值结果对比, 分别给出颗粒与基体界面的法向强度、切向强度及界面断裂韧性; 进一步应用标定的界面力学参数, 开展不同尺寸及不同数目颗粒填充试样的实验与数值结果比较, 验证界面性能预测结果的合理性. 本文提出的界面力学性能预测方法简便、易操作、精度高, 对定量预测颗粒增强复合材料的力学性能具有一定帮助, 亦对定量预测纤维增强复合材料的界面性能具有一定参考意义.      

冲击载荷作用下颗粒材料动态力学响应的近场动力学模拟

颗粒材料在冲击载荷作用下的动态力学行为是学术界关注的热点问题. 新近问世的近场动力学(peridynamics)理论将材料视为由大量有限体积和有限质量的物质点组成,基于非连续性和非局部作用假定建模,建立空间积分形式的运动方程,自然适应于颗粒材料动态力学行为的描述与分析. 发展了描述颗粒间接触作用的物质点尺度的排斥力模型,考虑近场动力学方法中非局部长程力特征,改进了近场动力学中的初始微观弹脆性(prototype microelastic brittle, PMB) 模型的本构力函数,并消除了原PMB 模型中存在的“边界效应” 问题. 计算分析了冲击载荷作用下碳化钨陶瓷颗粒体系的动态力学响应,得到了不同冲击速度下颗粒体系的冲击波速,PD计算结果与试验结果高度一致;通过颗粒物质点尺度作用描述单颗粒尺度的接触作用,很好地再现了颗粒的转动与平动、颗粒挤压变形以及颗粒破碎等现象;刚性冲击板附近同时存在严重的颗粒破碎与轻微的颗粒损伤,远离冲击板的部分颗粒出现破损,且颗粒破碎主要是由颗粒间挤压、碰撞以及相对滑动剪切作用造成的. 研究结果表明,所发展的计算模型和分析方法能很好地反映颗粒材料动态力学行为,具有广泛的应用价值.      

An extended micromechanics method for probing interphase properties in polymer nanocomposites

Inclusions comprised on filler particles and interphase regions commonly form complex morphologies in polymer nanocomposites. Addressing these morphologies as systems of overlapping simple shapes allows for the study of dilute particles, clustered particles, and interacting interphases all in one general modeling framework. To account for the material properties in these overlapping geometries, weighted-mean and additive overlapping conditions are introduced and the corresponding inclusion-wise integral equations are formulated. An extended micromechanics method based on these overlapping conditions for linear elastic and viscoelastic heterogeneous material is then developed. An important feature of the proposed approach is that the effect of both the geometric overlapping (clustered particles) and physical overlapping (interacting interphases) on the effective properties can be distinguished. We apply the extended micromechanics method to a viscoelastic polymer nanocomposite with interphase regions, and estimate the properties and thickness of the interphase region based on experimental data for carbon-black filled styrene butadiene rubbers.     

Rhéologie des matériaux en cours de prise : Approche théorique

The rheological behavior of setting heterogeneous materials is studied from a theoretical approach by means of the homogenization technique of periodic medium. These materials considered as suspensions of gas bubbles at finite concentration in a viscoelastic matrix with low compressibility, present the macroscopic behavior of a compressible viscoelastic medium. The shear and volume macroscopic moduli are of the same order of magnitude and directly proportional to that of the fluid. The effective compressibility of the gas (out of thermal equilibrium) is added to these fluid contributions.     

New integral formulation and self-consistent modeling of elastic–viscoplastic heterogeneous materials

Predicting the overall behavior of heterogeneous materials, from their local properties at the scale of heterogeneities, represents a critical step in the design and modeling of new materials. Within this framework, an internal variables approach for scale transition problem in elastic–viscoplastic case is introduced. The proposed micromechanical model is based on establishing a new system of field equations from which two Navier’s equations are obtained. Combining these equations leads to a single integral equation which contains, on the one hand, modified Green operators associated with elastic and viscoplastic reference homogeneous media, and secondly, elastic and viscoplastic fluctuations. This new integral equation is thus adapted to self-consistent scale transition methods. By using the self-consistent approximation we obtain the concentration law and the overall elastic–viscoplastic behavior of the material. The model is first applied to the case of two-phase materials with isotropic, linear and compressible viscoelastic properties. Results for elastic–viscoplastic two-phase materials are also presented and compared with exact results and variational methods.     

黏弹性材料等效分数阶微观结构标准线性固体模型

从黏弹性材料微观链结构出发,以橡胶基黏弹性材料超弹性理论分子网链高斯(Gauss)统计模型和黏滞流动理论为基础,研究黏弹性材料的微观结构、填料等对黏弹性性能的影响.用温频等效原理描述温度对黏弹性材料力学性能的影响,建立了可以有效描述黏弹性材料耗能特性的等效分数阶微观结构标准线性固体模型.采用动态热机械分析仪(DMA)对高聚物黏弹性材料力学性能、耗能能力进行测试.试验表明:在低温区域,储能模量较大,随着温度的升高,储能模量下降显著;能量损耗因子在高温和低温区域数值较小,在玻璃化转变温度附近数值较高.根据测试数据对所提等效分数阶微观结构标准线性固体模型进行验证,该力学模型能够较好地描述黏弹性材料储能模量和能量损耗因子随温度的变化趋势.用9050A和ZN22黏弹性材料对模型的有效性进一步验证,结果表明:9050A和ZN22黏弹性材料具有较好的耗能能力,所提出的等效分数阶微观结构标准线性固体模型能够准确地描述微观结构和填料对黏弹性材料宏观性能的影响,能够准确地描述黏弹性材料在不同温度和频率下的动态力学性能.     

Modeling of steady and time-dependent responses in filled, uncured, and crosslinked rubbers

Filled polymer systems have been a subject of interest for rheologists for several decades. Their applications range from paints and pigments to high performance composite materials. Presently, there is a lack of complete understanding of the behavior of these materials under varying kinematic and dynamic conditions. Moreover, there is a lack of a comprehensive theory, which can simultaneously describe the rheology of filled rubbers, their chemorheology, and their behavior in the final fully cured state. The present work is aimed at capturing a wide range of rheological (viscoelastic and kinetic) properties of filled rubbers with one set of constitutive/kinetic equations and a flexible relaxation spectrum. The various experiments covered are yield-flow transition in creep, shear start up responses, dynamic behavior in the melt state, and the changes during the cure stage. In the post cure state, the manifestations in Mullins stress softening-hysteresis and recovery, large strain stress relaxations, and dynamic behavior are also demonstrated. Finally, the non-linearities during large strain dynamic deformations, accompanied by non-isothermal, viscoelastic, and structure effects are exemplified. Received: 24 July 2000 Accepted: 13 November 2000     

炭黑填充橡胶材料的修正三链模型和Mullins模型

本文探讨了炭黑颗粒填充橡胶材料的本构模型。考虑到橡胶单个分子链与周围分子网络的约束作用和炭黑颗粒对橡胶的补强作用,提出了一种修正三链模型,用Edwards管模型描述分子链之间的相互作用和约束,采用应变放大因子来考虑炭黑含量的影响。并在修正三链模型的基础上,利用橡胶分子网络重构理论,提出了一种适合表征橡胶Mullins现象的本构模型。通过与实验数据比较分析,修正三链模型可较准确地表征未填充橡胶材料不同变形模式的力学性能和炭黑颗粒填充橡胶材料的单向拉伸力学行为,Mullins模型也可较好地描述橡胶材料的Mullins现象。     

Microstructure and melt flow behavior of a starch-based polymer

Results on some physical properties and on melt processing of a starch-based polymer under steady-state shearing are presented. A peculiar microstructure involving a strong pseudoplastic behavior at high shear rates as well as yield stress at lower ones is discussed. A model is proposed to explain the characteristic viscoelastic behavior of this material based on hydrophylic and hydrophobic interactions between starch and vinyl-alcohol copolymers.In spite of the highly structured and composite nature of this class of materials, the full body of results reveals that they can be easily processed by means of common manufacturing techniques involving melt pumping and die forming. A comparison with a low density polyethylene (LDPE) grade for film blowing is also shown.     

聚硅氧烷硅胶的黏超弹性力学行为研究

聚硅氧烷硅胶是一类以Si——O键为主链、硅原子上直接连接有机基团的无色透明高分子聚合物, 因其具有优异的超弹性性能而广泛应用于精密减震结构、柔性电子器件等领域. 在聚硅氧烷硅胶减震结构和柔性电子器件的设计中, 材料在大变形和动态加载下的黏超弹性力学行为的精确描述至关重要. 本文针对该问题进行了系统的研究:首先, 将该硅胶的超弹性和黏弹性行为进行解耦, 确定其黏超弹性本构方程的基本框架;其次, 基于单轴拉压、平面拉伸试验确定其准静态超弹性模型的各项参数;再次, 利用霍普金森压杆冲击试验确定其黏弹性模型的各项参数;在此基础上, 将超弹性和黏弹性模型合并为适用于大应变和大应变率的黏超弹性动态本构模型;最后, 利用落锤冲击试验对该硅胶薄片的冲击变形行为进行了研究, 并利用上述建立的动态本构模型对落锤冲击过程进行了有限元模拟. 结果表明:本文建立的黏超弹性本构模型可有效预测该硅胶在冲击载荷下的力学行为, 从而为聚硅氧烷硅胶减震结构和柔性电子器件的优化设计提供了理论和应用基础.      

基于微形态模型的颗粒材料中波的频散现象研究

基于颗粒材料冲击与波动响应特性的调控波传播行为的超材料设计受到广泛关注,设计这类材料需要对颗粒材料的波传播机制及调控机理有深入认识. 波在颗粒材料中传播的频散现象及频率带隙等行为与材料的非均匀性密切相关,通常讨论频散现象是基于弹性理论框架建立微结构连续体或高阶梯度连续体等广义连续体模型来进行. 本研究基于细观力学给出了一个颗粒材料的微形态连续体模型. 在该模型中,考虑了颗粒的平动和转动,且颗粒间的相对运动分解为两部分:即宏观平均运动和细观真实运动. 基于此分解,提出了一个完备的变形模式,得到了对应于不同应变及颗粒间运动的宏细观本构关系. 结合宏观变形能的细观变形能求和表达式,获得了基于细观量表示的宏观本构模量. 应用所建议模型考察了波在弹性颗粒介质的传播行为,给出了不同形式的波的频散曲线,结果显示此模型具有预测频率带隙的能力.      

Rheological properties of long glass fiber filled polypropylene

Long glass fiber-filled polypropylene (PP) composites are produced by pultrusion, and the extrudate is cut at different lengths producing composites containing long fibers of controlled length. The rheological properties of such composites in the molten state have been studied using different rheometers. A capillary rheometer has been constructed and mounted on a molding-injection machine. The shear viscosity of filled PP determined from the capillary rheometer, after corrections for entrance effects, was found to be very close to that of unfilled PP. However, large excess pressure losses at the capillary entrance were observed and these data have been used to obtain an apparent elongational viscosity. The apparent elongational viscosity was shown to be considerably larger than the shear viscosity for PP and filled PP, and it increased markedly with fiber length and fiber content. Rotational rheometers with a parallel-plate geometry were used to investigate the viscoelastic properties of these composites and their behavior was found to be non-linear, exhibiting a yield stress. A model is proposed to describe the shear viscosity from a solid-like behavior at low stresses to fluid-like behavior at high shear stresses taking into account fiber content and orientation. A modified model, proposed for elongational flow, describes relatively well the apparent elongational data.     

Global–local analysis of granular media in quasi-static equilibrium

A method of global–local analysis is developed for quasi-static equilibrium problems for granular media. The two-scale modeling based on mathematical homogenization theory enables us to formulate two separate boundary value problems in terms of macro- and microscales. The macroscale problem governs the equilibrium of a global structure composed of granular assemblies, while the microscale one is posed for the particulate nature of a local structure with the friction-contact mechanism between particles. The local structure is identified with a periodic representative volume element, or equivalently, a unit cell, over which averaging is performed. The mechanical behavior of unit cells is analyzed by a discrete numerical model, in which spring and friction devices connect rigid particles, whereas the continuum-based finite element method is used for the macroscopic one. Representative numerical examples are presented to demonstrate the capability of the proposed two-scale analysis method for granular materials.     

Nonlinear effects in deformation of filled elastomers with nanodimensional fillers

Various nonlinear effects manifesting themselves in the deformation of filled elastomers are analyzed, and the advantages and restrictions in the use of several constitutive relations proposed to describe the nonlinear viscoelastic behavior of the materials under study are discussed. We also note that further development of models of nonlinear deformation of filled elastomers under finite strains, which would permit describing their deformation properties more completely, is highly desirable.     

Non-linear viscoelastic behavior of fumed silica suspensions

Suspensions of fumed silica exhibit a wide range of rheological properties depending on the nature and magnitude of the interparticle forces. In a non-polar fluid, the particles interact through hydrogen bonding and can form a three-dimensional network. The microstructure formation is responsible for the non-linear viscoelastic behavior of fumed silica suspensions, even at very small strain. These non-linear rheological properties have been studied in small amplitude oscillatory experiments as a function of particle size, surface treatment of particles, suspending medium polarity and solids concentration. The non-linear viscoelastic behavior is characterized by a non-sinusoidal waveform of the signal response. For suspensions in a non-polar fluid, both the elastic and the loss moduli are shown to be sensitive to the strain amplitude: the elastic modulus is decreasing with increasing strain whereas the loss moduli is initially increasing with strain. We have chosen to examine the dissipated energy which is clearly related to the breakup of the suspension structure. A comparison of model predictions and the experimental data shows the limitations of these models, recently proposed in the literature to describe the behavior of colloidal suspensions. Received: 9 March 1998 Accepted: 17 November 1998