Elastic properties of particle-reinforced composites

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nonspherical particles of high packing density and interphase: DEM-FEM

simulation and micromechanical theory

Wenxiang Xu, Binbin Xu, Fenglin Guo

PII: S0045-7825(17)30590-X

DOI: http://dx.doi.org/10.1016/j.cma.2017.08.010

Reference: CMA 11549

Revised date : 10 July 2017

Accepted date : 9 August 2017

Please cite this article as: W. Xu, B. Xu, F. Guo, Elastic properties of particle-reinforced

composites containing nonspherical particles of high packing density and interphase: DEM-FEM

simulation and micromechanical theory, Comput. Methods Appl. Mech. Engrg. (2017),

http://dx.doi.org/10.1016/j.cma.2017.08.010

This is a PDF file of an unedited manuscript that has been accepted for publication. As a service to

our customers we are providing this early version of the manuscript. The manuscript will undergo

copyediting, typesetting, and review of the resulting proof before it is published in its final form.

Please note that during the production process errors may be discovered which could affect the

content, and all legal disclaimers that apply to the journal pertain.

Highlights

H ighlights

1. PRCs consist of ellipses of high packing density, compliant interphase and matrix.

2. A robust coupling model of DEM and FEM is proposed to estimate the moduli of PRCs.

5. The derived results provide a robust predictive toolkit for the design of PRCs.

Revised Manuscript

Click here to download Manuscript: Revised Manuscript.doc Click here to view linked References

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6 Wenxiang Xu*a, Binbin Xu a, b, Fenglin Guo b

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8 a

Institute of Soft Matter Mechanics, College of Mechanics and Materials, Hohai University, Nanjing 211100, China

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11 b

State Key Laboratory of Ocean Engineering, School of Naval Architecture, Ocean and Civil Engineering, Shanghai

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14 Jiao Tong University, Shanghai 200240, China

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17 A bstract: The physical and morphological properties of particles and interfaces can seriously impact

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the whole mechanical behavior of particle-reinforced composites. In this work, we devise a robust

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22 coupling model of the discrete element method (DEM) and the finite element method (FEM) to

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25 numerically investigate the effective elastic moduli of particle-reinforced composites consisting of

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28 elliptical particles of high packing density, compliant interfaces and homogeneous matrix. In the

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numerical model, a novel parametric equation for the topological geometry of an interface that is

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33 treated as an interphase model is formulated to realize a compliant (penetrable) layer with a constant

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36 finite thickness coated surrounding each elliptical particle. Additionally, a convenient strategy is

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39 implemented to cope with periodic boundary conditions containing numerous particles. On the other

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hand, we also propose a micromechanical theoretical framework to derive the effective elastic

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44 properties of such three-phase composites by incorporating the fraction of compliant interfaces that is

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47 theoretically computed by using the statistical geometry of composites. It is shown that our numerical

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50 and theoretical models lead to the prediction of elastic moduli of particle-reinforced composites with

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nonspherical particles of high packing density to a reasonable accuracy by comparing with available

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55 experimental data. Moreover, utilizing the proposed models, we systematically investigate the influence

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Correspondence to: Institute of Soft Matter Mechanics, College of Mechanics and Materials, Hohai University, Nanjing 211100, China.

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60 E-mail address: xuwenxiang@hhu.edu.cn (W. Xu).

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of the characteristics of particles and interphase such as the high packing density and geometries of

elliptical particles, and interphase fraction, thickness and stiffness on the elastic moduli of

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3 particle-reinforced composites. We find that these physical characteristics play significant roles in

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6 determining the mechanical behavior of composites, suggesting that the properties of such materials

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8 can be tailored via proper composites engineering and design.

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11 K eywords: Particle-reinforced composites; Nonspherical particle; Interphase; Discrete element model;

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14 Micromechanical theory; Elastic modulus

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17 1. Introduction

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It is well known that particles and interfaces are important components in various

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22 particle-reinforced composites (PRCs) like polymers, colloids, ceramics, normal concrete and asphalt

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25 concrete [1-5], which play important roles in the mechanical properties of PRCs. Owing to different

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28 technologies of the manufacturing for materials, interface zones may be a compliant interphase

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possessing a low stiffness or a relative high porosity with respect to matrix in MXD6-clay

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33 polymer-composites [3] and cementitious composites (the so-called interfacial transition zones, ITZs

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36 in concrete) [4, 5]. It is normally considered as a penetrable interfacial layer with a constant finite

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39 thickness surrounding each particle in PRCs [1-5], leading to a famous core-shell structure [6].

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Understanding the effects of particle and interphase characteristics on the effective elastic properties of

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44 PRCs and rigorously incorporating such structural information into homogenization scheme for

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47 material property predictions is a problem of great interest in materials research community. The

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50 resulting rigorous structure-property relations are also valuable for material design and microstructure

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optimization.

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55 Over the past decades, significant efforts have been devoted to theoretical and numerical assessing

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58 the effects of particle and interphase characteristics on the effective elastic properties of PRCs. In

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61 theoretical aspects, Kerner [7] seminally developed a three-phase composite model including spherical

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particles to study the effective elastic properties. Later, Christensen and Lo [8] applied the generalized

self-consistent scheme and the Eshelbys equivalent inclusion theory [9] to evaluate the effective shear

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3 moduli of three-phase PRCs. For PRCs containing nonspherical particles (e.g., ellipsoids, cylinders or

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6 planets) and interphase, some popular micromechanical schemes have been presented to formulate the

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8 elastic properties of such PRCs, such as bound models [10, 11], generalized self-consistent method

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11 (GSCM) [12, 13], Mori-Tanaka scheme (M-T) [14, 15], double-inclusion model [16, 17], differential

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14 effective medium approximation (D-EMA) [18], and exact contrast expansions [19]. We note that the

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17 bound models are based on the well-known variational principle originally introduced in the pioneering

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work of Hashin and Shtrikman [20]. The effective medium models (e.g., the GSCM, M-T,

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22 double-inclusion and D-EMA mentioned above) mainly stem from the famous Eshelbys equivalent

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25 inclusion formulation [9], However, a potential limitation for these micromechanical schemes is that

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28 the fraction (i.e., packing density) of particles is usually processed in a relative low level. In this work,

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we try to address the issue via the combination of numerical and theoretical explorations.

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33 Alternatively, numerical simulations provide an optional means to evaluate the elastic properties

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36 of PRCs containing nonspherical particles and interphase, especially for the high packing density of

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39 nonspherical particles. For instance, Zhou et al. [21] estimated the elastic modulus of concrete

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composed of convex polygonal grains and interphase by random sequential additions (RSA) and finite

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44 element method (FEM). Other similar studies can also be found in [22-25]. Additionally, Xu and

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47 coworkers [26] and Abyaneh et al. [27] applied the three-dimensional RSA of spheroidal particles and

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50 the lattice model to predict the effective properties of cementitious composites. Moreover, Patel and

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Zohdi [28] developed a statistically numerical scheme to estimate the effective properties of PRCs

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55 containing ellipsoidal particles. Recently, the authors [29] simulated the effective mechanical properties

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58 of fully-grade concrete consisting of multisized convex polyhedral particles by the coupling of RSA

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61 and FEM. Although the numerical studies above mentioned enriched our knowledge of the effective

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properties of three-phase PRCs with anisotropic-shaped particles, nonspherical particles of high

packing density and interphase are rarely involved in the literature. It is our intention in the present

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3 work to address this gap.

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6 In this study, we mainly focus on elliptical particles, as a canonical model of nonspherical shapes

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8 over a broad range of aspect ratios, which have been widely used in numerous material systems. We

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11 attempt to present a numerical model that adopts the coupling of the discrete element method (DEM)

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14 and FEM to estimate the effective elastic moduli of PRCs composed of elliptical particles of high

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17 packing density, compliant interphase and homogeneous matrix. Perfect bonding conditions are here

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used for both the particle/interphase and the interphase/matrix. Meanwhile, we also try to formulate a

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22 theoretical model to predict the effective elastic properties of such PRCs through the combination of

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25 the Mori-Tanaka average scheme and the Eshelbys equivalent inclusion theory on the basis of the

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28 recent contribution [14]. Moreover, the interphase physical characteristics like the interfacial fraction

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and thickness are derived and incorporated into the predictions of the effective elastic properties of

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33 PRCs in the present numerical and theoretical work.

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36 The rest of this article is organized as follows. Section 2 describes a numerical model for the

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39 estimation of the effective elastic modulus of PRCs with elliptical particles of high packing density and

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interphase, where the foundation of DEM, the topological geometry of an interface, the interphase

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44 fraction, and the coupling of DEM and FEM are elaborated in detail, respectively. Section 3 illustrates a

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47 micromechanical framework to theoretically compute the effective elastic properties of such PRCs,

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50 among the fraction of compliant interfaces is formulated through the statistical geometry of composites

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and geometrical probability. In Section 4, some results are given and discussed. Finally, this article is

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55 completed with some concluding remarks in Section 5.

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58 2. Numerical model

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61 In this section, we firstly describe DEM to establish two-phase PRCs consisting of monodisperse

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non-overlapping elliptical particles and homogeneous matrix. Subsequently, a parametric equation for

the topological geometry of an interfacial layer with a constant dimension is proposed to generate

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3 three-phase PRCs. Previous works for the geometric construction of an interfacial layer, such as

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6 [24-27], has demonstrated by uniformly enlarging the semi-axes (e.g., a1 and b1) of an elliptical particle

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8 to a constant dimension t, namely, a1+t and b1+t. Unfortunately, such simplified fashion meets the

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11 limitation of the accuracy of the core-shell structure that shells coating around cores are specified the

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14 same thickness. To be specific, the previous operations cannot ensure the shell possessing the same

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17 dimension around an elliptical particle, due to the difference of the surface curvature of an ellipse,

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especially in the large aspect ratio. Then, the DEM-FEM coupling model is presented to estimate the

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22 effective elastic modulus of three-phase PRCs.

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25 2.1 The discrete element model (D EM)

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28 DEM stemmed from Cundall and Strack [30] has been extensively used in granular media, PRCs,

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chemical engineering and mineral engineering [31-38]. The main idea of DEM is to find the

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33 equilibrium contact forces and displacements of an assembly of particles based on a series of

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36 calculations tracing the movements of the individual particles. These movements attribute to the initial

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39 unbalance forces like gravity or the propagation of disturbances originating from the boundaries. Thus,

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there are two strategies to implement the accumulation of particles. One is that particles are randomly

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44 casted in a sample space and allowed to move under the condition of gravity. Another is that the

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47 boundaries are controlled to move inward and to push the particles together like bulldozers. Herein, the

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50 later strategy is adopted in this work.

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The classical Newtons second law and a force-displacement law are alternately applied in DEM,

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55 where both laws are respectively used to derive the contact forces and the motion locus of a particle.

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58 Suppose an overlap potential between particle i and particle j can be decomposed into the normal and

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61 tangential components n and t at a time step t . The normal and tangential directions depend on the

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determination of the location of the specific point C, as shown in Fig. 1. Herein, we define the point C

as the midpoint of the segment joining two contact points C i and C j that follow the contribution from

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C i and C j are also referred as the lowest geometric

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6 potential points introduced in [36], which can be obtained through a series of linear transformations of

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8 the coordinate system presented in the preliminary work [34]. As shown in Fig. 1, the normal direction

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11 is prescribed from C i pointing to C j and its counterclockwise angle is defined as the positive value.

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14 Then, the tangential direction is perpendicular to the normal direction and satisfies the right-hand rule.

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17 Therefore, the segment distance between C i and C j is the normal component n(t), and the

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corresponding tangential component can be obtained by the incremental method, namely, t(tt(t-t)

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22 + vtt, where vt is the tangential velocity in the current time step. It is noted that vt equals to 0 at the

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25 initial time whose value in next time step can be obtained by the coordinate transformation of the

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28 previous velocities in the global coordinate system.

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The corresponding normal and tangential forces between adjacent particles are thus expressed by

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33 Fn (t ) kn n (t ), Ft (t ) Ft (t t ) kt t (t ) (1)

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36 where F n and kn are the normal force and stiffness, respectively. F t and k t are the tangential force and

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39 stiffness, respectively. According to the Coulomb-type friction law, the magnitude of F t is checked

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against the maximum possible value ( F t)max, that is

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44 ( Ft )max Fn tan u c (2)

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47 where u is the smaller value of the interparticle friction angles in contact and its value does not depend

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50 only on the density and shape of particles, but also on the experimental conditions. For convenience of

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simulation, we adopt the experimental data reported by Schanz and Vermeer [39] that the friction angle

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55 was presented in the range of 40 to 50 degrees for dense sands. In this work, the friction angle is set to

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58 be 40 degrees for the implementation of DEM. c is the smaller one of their cohesions. Once F t and F n

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61 are determined for each particle, they can be resolved into components in the x and y directions of the

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Cartesian coordinate system, as shown in Fig. 1. Also, the moment on particle i can be obtained by M =

F T i, where T i represents the position vector from point C to the centroid of particle i.

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3 If an individual particle overlaps with more than one particles, the sums of these contact force

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6 components F x and F y are applied to the individual particle. Plus, the resultant moment M is

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8 just derived in terms of the scalar operation, since the direction of M is always perpendicular to the

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11 plane of the paper. Consequently, the accelerations of the individual particle are calculated through

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14 Newtons second law:

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17 a F / m, M / I (3)

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where a and m are the acceleration generating the displacement and the mass of the particle,

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22 respectively. and I are the angular acceleration and the moment of inertial of the particle, respectively.

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25 In DEM, velocities and accelerations are normally assumed to be constant in one short time step t, so

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28 that velocities and displacements of particles in t can be obtained as follows.

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30 v v 0 a t , 0 t (4)

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33 u u 0 v t , 0 t (5)

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36 where v and and the linear and angular velocities. u and are the displacement and angular rotation.

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39 The subscript 0 represents the corresponding quantity of the previous step. The velocities in the global

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coordinate system can also be decomposed into two components in the local coordinate system again to

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44 calculate the tangential overlap and the damping forces in the normal and tangential direction if needed.

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47 The above process can be repeated until all particles reach equilibrium.

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50 It is worth stressing that the key issue of the above implementation for DEM of elliptical particles

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is to identify the contact detection and the overlap potential for adjacent ellipses. Fortunately, in our

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55 previous works, a robust numerical algorithm for the quantitative contact of ellipses has been

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58 developed [34], even more the algorithm can also be directly extended to the contact of

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61 three-dimensional ellipsoids [35]. In the numerical algorithm, a series of linear transformations of the

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coordinate system are executed to transform an ellipse (ellipsoid) into a unit circle (sphere) with its

center located at the origin of the coordinate system. Also, a novel golden section search algorithm

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3 instead of solving a complex fourth-order (six-order) polynomial equation reported in the literature is

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6 presented to numerically derive the overlap potential of adjacent ellipses (ellipsoids). More detailed

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8 descriptions on the operation of the numerical algorithm can be found in [34, 35]. In addition, other

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11 promising lines of theoretical research on DEM can also found in the literature [36-38].

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14 In order to improve the efficiency of the present DEM, on the one hand, we divide a sample space

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17 (e.g., a square area) into some subspaces, in which each subspace is numbered, as shown in Fig. 2(a).

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The random generated particles in a subspace are just labeled as the same flag as the corresponding

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22 subspace. In doing so, it is very convenient to compute the contact forces of a labeled particle, since the

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25 search for adjacent particles is only implemented in the neighboring eight subspaces for the

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28 two-dimensional (2D) case. As an introductory example, we can clearly see from Fig. 2(a) that an

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ellipse within the subspace with the number 11 potentially contacts with those ellipses within the

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33 subspaces with the number 6, 7, 8, 10, 12, 14, 15 or 16. On the other hand, we put forward to a

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36 convenient periodic compensation scheme for satisfying periodic boundary conditions specified in this

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39 work, as shown in Fig. 2(b). In one-time step t, we prescribe the upper and left boundaries move

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inward, so that the particles within the subspaces of the first line and column are thereupon pushed to

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44 move inward. When these particles update their locations, they are immediately copied to the bottom

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47 and right regions, forming the borders of the compensatory additional particles, as shown in Fig. 2(b).

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50 The formed two particle-borders move inward with the same velocity as the upper and left boundaries.

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Finally, copying the particles in the subspaces of the last row and column to the left and top regions

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55 generates a packing model with periodic boundary conditions, as shown in Fig. 2(b). Fig. 3 depicts two

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58 introductory DEM structures representing two-phase PRCs with monodisperse non-overlapping

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61 ellipses of different aspect ratios and homogeneous matrix.

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2.2 The accurate construction of interphase

It is very crucial to precisely realize the topological geometry of an interfacial layer around an

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3 elliptical particle, for the construction of three-phase PRCs and then the accurate estimation of

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6 mechanical properties of such PRCs. Unlike polyhedrons or cylinders, whose interfacial layers can be

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8 geometrically constructed by the Minkowsky sum manner [25, 40], the interfacial layer with a constant

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11 dimension around an ellipse (ellipsoid) meets a huge challenge through the Minkowsky sum manner,

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14 owing to the nature of the difference of the surface curvature of an ellipse. In this section, we will

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17 develop a parametric equation for the accurate generation of the topological structure of an interfacial

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layer with a constant dimension around an arbitrary ellipse.

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22 First of all, we transform an arbitrary ellipse into a unit circle with its center located at the origin

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25 through three coordinate transformations, namely, the rotation, translation and scaling transformations,

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28 as shown in Fig. 4. The detailed operation can be found in [34]. Suppose that a straight-line L is tangent

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to the unit circle in the coordinate system x3-y3, and the tangent point is denoted as A (cos(), sin()).

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33 Thus, the linear equation for L can simply expressed as

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36 sin( ) y cos( ) x 1 0 (6)

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39 In the coordinate system x2-y2, the corresponding tangent point A 1 and the slope of the

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straight-line perpendicular to L 1 are written as (a1cos(), b1sin()) and a1sin() / (b1cos()), respectively.

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44 We construct a unit vector n perpendicular to L 1 at the point A 1, meanwhile n is also the normal vector

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47 of the ellipse at point A 1:

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49 (b1 cos( ), a1 sin( ))

50 n (7)

51 a12 sin 2 ( ) b12 cos 2 ( )

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54 Then, we can use the addition of the vector to get any one-point P1 on the interface in the coordinate

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57 system x2-y2:

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59 P1 A 1 n t (8)

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where t is the dimension of interface. Actually, Eq. (8) stands for the parametric equation for the

interface on the standard ellipse. Furthermore, the standard ellipse can be inversely transformed into the

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3 original arbitrary ellipse. Consequently, the parametric equation for an interfacial layer with a constant t

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6 around an arbitrary ellipse can be presented by

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8 P R TP1 (9)

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11 where P represents the assembly of points on the interface around an arbitrary ellipse. R and T are the

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14 rotation and translation matrices of coordinate transformations, of which the display-formats have been

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17 introduced in the previous work [34]. Fig. 5 shows some typical patterns for the topological geometries

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of the interfacial layer around an elliptical particle, where the green, blue and red curves represent the

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22 profiles of the elliptical particle, the interface with a constant dimension realized by the proposed

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25 parametric model and the approximate interface constructed by the simplified fashion mentioned above,

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28 respectively. It can be explicitly seen that the difference between both interfacial topological geometries

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realized by the above two methods, especially for an ellipse of the large aspect ratio.

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33 2.3 The coupling of D EM and F EM

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36 On the basis of the two-phase PRCs and the interfacial construction demonstrated above,

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39 three-phase PRCs composed of elliptical particles of high packing density, compliant interphase and

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homogeneous matrix can be established, among the intersections between an interfacial layer and

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44 particles and neighboring interfacial layers may occur, as shown in Fig. 6. In doing so, the overlapping

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47 interfacial fraction should be addressed before the prediction of elastic properties of PRCs. We adopt a

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50 Monte Carlo random point sampling scheme to statistically evaluate the interfacial fraction, and its

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operation strategy is elaborated in the Supplementary Information (see S1).

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55 Subsequently, the geometric information about the particles and interfaces, such as their positions,

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58 sizes and directions, is imported in the finite element software like Due to the potential

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61 overlap of interfaces, the definition of the material properties for different phases meets difficulty.

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Herein, we discretize the whole three-phase structures by using the 6-node triangular element in the

!, since the triangular element type has the great adaptation to

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3 complex geometry. The mesh size of elements is set to be a half of the dimension of interfaces, which is

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6 small enough to investigate the interphase effect. Fig. 7 displays a typical detailed meshing structure for

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8 three-phase PRCs, where there are about 150,000 nodes and 70,000 elements, and the size ratio

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11 between the cell and particles is set to be 8.5.

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14 According to the average strain and stress theorems, the average stress ij and strainij of a

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17 volume element V can be computed as average integral both on external boundary and volume:

18

1 1 1 1

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ij

V V ( x)dV V v Ti (S ) x j dS ,

ij

ij

V V ij ( x )dV

V v [ui (S )n j u j (S )ni ]dS

(10)

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22 where x, n, S, T (S) and u(S) denote the position vector, the outward unit normal vector, the volume

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25 surface, the boundary traction and the boundary displacement fields, respectively. Through the

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28
"

lowing:

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30 ij C ijkl kl , ij S ijkl kl (11)

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33 where C ijkl and Sijkl are the apparent stiffness and compliance tensors, respectively. Then the boundary

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36 displacement field of a PRC sample can be solved by ABAQUS as static mechanical problems. After

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39 the average strainij is calculated by the above Eq. (10), the apparent stiffness tensor or compliance

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tensor can be easily derived by Eq. (11). For the present 2D case, only the engineering moduli E 11,22

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44 corresponding to the axial strain and stress are here solved by the coupling of FEM and DEM. It is

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47 worth stressing that particles in a limited sample do not satisfy ideally the random orientation, so that

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50 C ijkl or Sijkl are not perfectly isotropic unless the selected sample is large enough. In other words, the

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sample meets the requirement of representative volume element (RVE), which will be concerned in

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55 Section 4.2. Consequently, the apparent elastic properties are equal to the effective properties of PRCs

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58 no matter what homogeneous displacement or traction boundary conditions are applied.

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61 3. M icromechanical theory framewor k

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At a microscopic scale, the average field theory is often used to evaluate the effective properties of

heterogeneous materials [12-17]. The average field theory can give the quantitative relation between

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3 the average strain and stress of microscopic heterogeneous materials by defining the effective

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6 mechanical properties, as depicted in Eqs. (10) and (11). Suppose a three-phase PRC is subjected to the

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8 displacement boundary condition with a constant strain tensor 0. The elastic modulus tensors for

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11 individual phase are marked as C p, C i and C m, in which the superscripts p, i , and m represent particles,

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14 interphase and matrix, respectively. Also, the overall effective elasticity stiffnessC of PRC is defined

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17 by

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C C 0 (12)

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22 where and are the volume average stress and strain tensors of PRC given by

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25 f p p f i i f m m f p C p p f i C i i f m C m m (13)

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28 = f p p fi i fm m (14)

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where fp, f i and fm are the fractions of particles, interphase and matrix, respectively. Normally, the

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33 fraction of particles is given in a PRC. In other words, the fraction of interphase (interfaces) is strongly

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36 related to the fraction of matrix:

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fi 1 f p fm (15)

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41

42

Previous efforts have been spent analytically assessing the fraction of compliant interphase around

43

44 three-dimensional (3D) convex-shaped particles, like spheres [42], ellipsoids [43], convex polyhedra

45

46

47 [44] and spherocylinders [45]. Moreover, we recently developed a general formula for the fraction of

48

49

50 compliant interphase around 3D arbitrary convex-shaped particles [46]. All theoretical efforts are based

51

52

53

on the seminal work by Torquato and coworkers [47], who developed a theory of the nearest-surface

54

55 distribution functions to calculate the so-

However, those

56

57

58 previous contributions are not suitable for the present 2D case, since the scaled-particle theory [48] for

59

60

61 the 3D case is entirely different from that for the 2D case in the derivation of the radial distribution

62 12

63

64

65

function at the contact value [47]. Therefore, it raises to concern on the fraction of compliant interphase

1

2

3 3.1 Theoretical model for the interfacial fraction in 2D case

4

5

6 By means of the statistical geometry of composites and the core-shell structure, the void exclusion

7

8 probability in two-phase composite media composed of 2D circular particles and voids is derived by

9

10

11 [47]

12

13

r 2 +2 R r R 2 r 2

14

eV r 1 exp (16)

15

1 1

2

16

17

18 where e V(r ) is defined as the probability of find

V empty of composite media, which is a

19

20

21 circular cavity of radius r centered at an arbitrary point. In other words, the void exclusion probability

22

23

24 e V(r) represents the expected fraction of voids in such two-phase composite media. is the number

25

26 density of circular particles with radius R.

depicts a number-averaged treatment. is a dimensionless

27

28

29 reduced density defined by

30

31

32 R2

A (17)

33 2

34

35

36 where

A is the average area of particles(x) is the gamma function. In fact, is the area fraction of

37

38

39 hard circular particles in two-phase media, i.e., = fp.

40

41

42

Considering a two-phase composite structure composed of circular particles and matrix, the void

43

44 exclusion probability e V(r) is essentially equivalent to the matrix exclusion probability, namely, the

45

46

47 fraction of matrix in the two-phase composite structure (i.e., e V(r ) = fm). Similarly, in a three-phase

48

49

50 composite structure with the core-shell model mentioned above, the quantity e V(r ) can still be mapped

51

52

53

into the fraction of matrix, since each particle and its surrounding layer with a constant dimension r can

54

55 be regarded as a composite particle, so that the three-phase structure is reduced to a two-phase system

56

57

58 containing composite particles and matrix. Also, fm r

59

60

61 overlap enough to fill up the remaining matrix. The quantity is designed to take into account the

62 13

63

64

65

overlap potential of compliant interphase. Consequently, the interfacial fraction around circular

particles is displayed the following formula on the basis of Eqs. (15) and (16).

1

2

t 2 +2 R t R 2 t 2

3

4 f i 1 f p 1 exp

1 f p 1 f p

2

5

6

(18)

Pc t 2

7

t2+ P t 2

= 1 f p 1 exp

8 c

9

1 f p 4 1 f 2

10 p

11

12

13

where t and P c are the interfacial dimension (i.e., r = t) and the perimeter of a circular particle,

14

15 respectively.

16

17

18 When the theory is applied to the three-phase elliptical particle composite structure, e V(t) still

19

20

21 stands for the fraction of matrix not occupied by all elliptical particles and interphase. However, e V(t ) is

22

23

24 subjected to the number density, size and the mean perimeter of elliptical particles. In terms of the

25

26 quantitative stereology [49], the number density of 2D solids equals to the ratio of the area fraction of

27

28

29 solid phase to the mean area of solids, namely, = fp / A. On the other hand, an equivalent diameter

30

31

32 D eq, defined as the diameter of an equivalent sphere having the same volume as a non-spherical particle,

33

34

35 was introduced to characterize the size of the non-spherical particle in previous lines of research

36

37 [43-46]. We here adopt D eq as the size of an elliptical particle, so that the mean area of elliptical

38

39

40 particles can denoted as A = D 2eq / 4. Plus, the perimeter P e of an ellipse can be approximately

41

42

43 expressed as [25]

44

Deq 1

1 , a / b

45 2

h h 2 h3 h4

46 Pe 1 , h (19)

1

e e

2

2

47 4 64 256 16384

48

49

50 where a e and be are the lengths of the semi-major and semi-minor axes of an ellipse, respectively. It

51

52

53

should be pointed out that, in a structure cell, the shape of each ellipse is assigned to be identical so as

54

55 to clearly understand the impact of morphological detail of anisotropic particles. Consequently, upon

56

57

58 substituting Eq. (19) into Eq. (18), the fraction of compliant interphase around elliptical particles can be

59

60

61 derived by

62 14

63

64

65

4f

t 2 + H D t H 2 f D 2 t 2

f i = 1 f p 1 exp 2p eq p eq

(20)

Deq

p

1 f Deq 1 f p

2 2

1

2

3 with

4

5

6 H

1

1 h h2

h3

h4

7 2 4 64 256 16384

8

9

10 If a composite structure with the size of elliptical particles is designed as the mean value or

11

12

13

monodispersity, we may prescribe a geometric size factor to reflect the coupling effect between the

14

15

t / D eq. Thus, the interfacial fraction in such

16

17

18 three-phase PRCs is reduced to

19

20

2 + H f H 2 2

21

22

f i = 1 f p 1 exp 4 f p

p (21)

23 1 f p 1 f p

2

24

25

26 3.2 Theoretical model for elastic moduli in 2D case

27

28

29 In the recent theoretical work [14], a two-phase PRC is Eshelby s inhomogeneous inclusion

30

31

32 problem and the total stress field is given by

33

34

35 m C p (0 m ) C m (0 m ) (22)

36

37 where!m is an average strain perturbation in matrix from 0 due to the existence of particles, as well as

38

39

40 the corresponding average stress perturbation !m

!m = C !! m. and are the stress

41

42

43 perturbation and strain perturbation, respectively. * is
stress-free.

44

45

46 Similarly, for a three-phase PRC, the presences of interphase and particles usually raise the

47

48 perturbed strains i and p, and the
stress-frees *i and *p for interphase

49

50

51 and particles with respect to matrix. Following up Eq. (22), the average strain of each phase in the PRC

52

53

54 can be expressed as

55

56

57 m 0 m , i 0 m i , p 0 m p (23)

58

59 i and p have been formulated by Hori [16]

60

61

62 15

63

64

65

fp i

i S i i

fi

S S p p i , p S p p Si S p i (24)

1

2

where Si and Sp are

s for interphase and particles, respectively. From the

3

4 strain distribution is related to * as [9]

5

6

7 (0 m ), p, i (25)

8

9

10 where M p and M i are the fourth-order tensors:

11

12 1

13

f

1

f

14 M S p p Si S p S p p Si S p i S p p Si S p p

p

15 f f

i i

16

17

18 1

f

1

f

19

20

M S i S p S p p S p p Si S p p S p p Si S p i

i

f f

21 i i

22

23

24 with

25

C C m C m , p, i

1

26

27

28

29 when Eq. (25) is substituted into Eq. (24), i andp are rewritten as

30

31

f

32 i Si M i p Si S p 0 m , p

S p M p Si S p M i 0 m (26)

33

fi

34

35

36 by substituting Eq. (26) into Eq. (23), the average strain of each phase is further arranged by

37

38

f

39 m 0 m , i I Si M i p Si S p m , p

I S p M p Si S p M i m (27)

40 fi

41

42

43 where I is the fourth-order identity tensor. Upon substituting Eq. (27) into Eq. (13), the constitutive

44

45

46 relation of the three-phase PRC is formulated as

47

48

fp

49 f m C m f p C p

I S p M p S i S p M i f i C i I S i M i S i S p m (28)

50 fi

51

52

53

From Eqs. (14) and (27), another form for the constitutive relation is given by

54

55

fp

56 = f m I f p

I S p M p S i S p M i f i I S i M i S i S p m (29)

57 fi

58

59 Upon substituting Eqs. (28) and (29) into Eq. (12), the effective elasticity stiffnessC of the three-phase

60

61

62 16

63

64

65

PRC is derived by

f

1 C f m C m f p C p
I S p M p S i S p M i f i C i I S i M i p S i S p

2 fi

3 1

(30)

fp i p

f m I f p
I S M S S M f i I S M S S

4 p p i p i i i

5

6 fi

7

8 In the present three-phase PRCs, the

rs Si and Sp are same, namely, Si = Sp = S (see

9

10

11 Supplementary Information, S2), owing to the coaxial nature for an elliptical particle and its

12

13

14 surrounding interface. Thus, the fourth-order tensors M p and M i are reduced to

15

M S , p, i

16 1

17 (31)

18

19

with

20

21

22 Km Gm

C C m C m e1 I h e2 I d , e1x

1

23 , e = , p, i

K Km G Gm

2

24

25

26 where I h and I d are the four-order tensors given by Ihijkl = (1/3)ijkl and Idijkl = 0.5(ikjl +ilj k -1.5ijkl).

27

28

29 K and G are the bulk and shear moduli of individual phase, respectively. Furthermore, Eq. (30) is

30

31

32 rearranged by

33

34 1

35 C f m C m f p C p
I SM p f i C i
I SM i f m I f p
I SM p f i
I SM i (32)

36

37 On the other hand, the present PRC consist of elliptical particles and interphase randomly distributed in

38

39

40 a homogeneous matrix, as shown in Fig. 6. The effective mechanical properties of PRCs are

41

42

43 transversely isotropic. Consequently, the effective stiffness for PRCs is dependent of five independent

44

45

46 stiffness coefficients and its stiffness matrix can be written as [50]

47

48

C11 C12 C13 0 0 0

49

C12 C11 C13 0 0 0

50

51 C13 C13 C 33 0 0 0

52 C 0 0 0 C 44 0 0

(33)

53

54 0 0 0 0 C 44 0

55

0 1

56

0 0 0 0 C11 C12

57 2

58

59 Appendix A gives the detailed derivation for the effective stiffness components C ij of the present

60

61

62 17

63

64

65

three-phase PRCs. The stiffness components C ij are directly related to the effective mechanical

1

2

C 33 C112 2C12 C132 2C11C132 C 33 C122 C C C132 1

3

4

E eff , eff 12 33 , G eff C11 C12 (34)

C11C33 C13 2

C11C 33 C13

2

2

5

6

7 where E eff, eff and G eff are the effective elastic modulus, Poisson ratio and shear modulus of PRCs,

8

9

10 respectively.

11

12

13 4. Results and discussion

14

15 4.1 The esti mation of interfacial fraction

16

17

18 In accordance of the numerical and theoretical schemes for the interfacial fraction described above,

19

20

21 we observe the dependence of the interfacial fraction on the particle fraction and the aspect ratio, as

22

23

24 shown in Fig. 8. It can be seen from theoretical and numerical results that the dependence of the

25

26 interfacial fraction f i on the particle fraction fp possesses a well consistency for different aspect ratios.

27

28

29 To be specific, f i increases when fp increases up to about 0.6, which is also in good agreement with that

30

31

32 for 3D convex-shaped particles elucidated in previous contributions [43-46]. Nevertheless, as fp

33

34

35 continues to grow, f i yet gradually decreases. It seems to be the first time to our knowledge that such a

36

37 correlation under the high packing density of particles is explored. As mentioned above, f i is mapped

38

39

40 onto the probability of filling up matrix in composites. Actually, interfaces significantly occupy to the

41

42

43 remaining matrix as fp > 0.6. When the number of particles continues to increase, some interfacial

44

45

46 zones are occupied by the increased particles, so that the interfacial volume fraction gradually

47

48 decreases when fp exceeds 0.6. In practice, this is also one of theoretical reasons why interfacial

49

50

51 transition zones in high-performance concrete are normally lower than that in normal concrete [51].

52

53

54 It is worth noting that, for the numerical results of f i shown in Fig. 8, interfaces may generate a

55

56

57 percolating network as fp increases from 0.4 to 0.5, since the increase tendency of f i becomes slow

58

59 when fp exceeds 0.5. Such the percolation behavior can induce the dramatic change of elastic modulus

60

61

62 18

63

64

65

of PRCs, which will be discussed in the following section 4.3 (see Fig. 10). Unfortunately, the

percolation threshold of interfaces (or the percolation threshold of particles) cannot be unambiguously

1

2

3 determined in this work, though the issue is of importance that may be statistically analyzed through

4

5

6 the extensive finite-size scaling scheme [52] in the near future.

7

8 On the other hand, Fig. 8 manifests that fi increases with the increase of . When nonspherical

9

10

11 particles degenerate isotropic spheres, f i reaches the minimal value. In other words, elliptical particles

12

13

14 raise the increase of the interfacial fraction with respect to spherical particles. Such phenomena are

15

16

17 consistent with the 3D results [43, 44, 46], but opposite to the 2D results claimed by Zheng et al. [53].

18

19

This case is attributable to the circumference of an ellipse larger than that of the circle with the same

20

21

22 area. As such, in the process of the design of high performance concrete, the selections of gravels and

23

24

25 sands are usually required close to spherical particles as much as possible as excellent aggregates, in

26

27

28 order to reduce interfacial effects.

29

30

31

4.2 RVE size for elastic properties

32

33 In order to ensure the reliability of numerical results for elastic moduli, RVE for numerical

34

35

36 simulations should be determined before exploring the elastic properties of PRCs. A classical definition

37

38

39 for RVE reported by Hill [54] is introduced as a sample that is entirely representative of the whole

40

41

42

mixture on average and contains a sufficient number of particles. Thus, the overall properties are

43

44 macroscopically uniform and independent of boundary conditions. It is obvious that, in a certain

45

46

47 fraction of particles, the more the number of particles contains, the bigger the size of samples is. When

48

49

50 the size of samples satisfies the requirement of RVE, the measured value of elastic modulus is identical.

51

52

53

In this section, the effect of the number of particles on the elastic modulus of PRCs is numerically

54

55 analyzed, among the number of particles is applied to determine the size of RVE. In order to improve

56

57

58 the computational efficiency of DEM-FEM, a rectangular sample is divided into m cells along each

59

60

61 side. One particle is randomly placed in each cell before moving inside the rectangular boundaries.

62 19

63

64

65

Consequently, m2 random particles and the size of samples with periodic boundary conditions can be

obtained. The number of particles in samples is prescribed from 16 to 100 with an increment of 2(m+1).

1

2

3 Fig. 9 shows the change of the relative elastic modulus E eff / E m for PRCs with the number of particles

4

5

6 under different aspect ratios of particles. From Fig. 9, one can see that the dispersion of numerical

7

8 results for E eff decreases with the increase of the number of particles in samples. When the number of

9

10

11 particles is greater than 49, the average value of elastic moduli of 10 samples tends to stable. Also,

12

13

14 when the number of particles reaches 64, the size of numerical samples satisfies RVE and the

15

16

17 corresponding sample size is 8.5 times the size of particles.

18

19

4.3 Test for the numerical model and micromechanical theory framework

20

21

22 We apply the numerical model and micromechanical theoretical framework introduced above to

23

24

25 estimate the effective elastic moduli of PRCs and compare the derived numerical and theoretical results

26

27

28 with the experimental data for mortar reported by Yang [41], as shown in Fig. 10. In Yangs experiment,

29

30

31

cubic specimens (50 50 50 mm) and different particle fractions (fp = 0.1, 0.2, 0.3, 0.4 and 0.5) are

32

33 cast and tested by the compressive test, and both interfacial thicknesses of t = 20 m and 40 m are

34

35

36 examined in those experimental specimens. For purpose of comparison, we adopt the experimental

37

38

39 parameters into our numerical and theoretical models. Fig. 10 shows in the range of fp 0.4 that the

40

41

42

numerical and theoretical results for both interfacial thicknesses are in agreement with the experimental

43

44 data, specifically the numerical results. As fp > 0.4, the numerical results from the DEM-FEM model

45

46

47 are also basically consistent with the theoretical results, even though the numerical results are slightly

48

49

50 lower than the theoretical results, which their relative errors are limited within the scope of 12% for t =

51

52

53

20 m and 9% for t = 40 m, respectively. It is exceptionally important that suggesting the present

54

55 micromechanical framework is suitable for the prediction of elastic properties of PRCs containing

56

57

58 elliptical particles of high packing density.

59

60

61 In addition, Fig. 10 presents that elastic modulus versus the particle fraction almost satisfies the

62 20

63

64

65

linear-spring relationship within the scope of fp 0.4, but as fp > 0.4, the elastic modulus nonlinearly

increases with the increase of particle fraction. Such the phenomenon may attribute to the percolation

1

2

3 generation for the particle and interface phases when the particle packing density exceeds 0.4, which

4

5

6 corresponds to the percolation generation of interphase described in Fig.8. It is well known that the

7

8 dramatic changes in the physico-mechanical properties of PRCs occurs when inclusions form a

9

10

11 percolating network through the composite. Fig. 10 does not however present an obvious abrupt change

12

13

14 of elastic moduli of PRCs near the percolation thresholds of particles or interfaces, owing to the relative

15

16

17 small contrast of the moduli between the particle and matrix phases limited by the experimental data.

18

19

On the other hand, we also compute the elastic moduli of two-phase PRCs without interphase using the

20

21

22 micromechanical theory framework, as shown in Fig. 10. One can clearly see that the two-phase

23

24

25 theoretical results are apparently higher than the experimental data, numerical results and the

26

27

28 three-phase theoretical results. It means that the interphase effect dominates the overall elastic

29

30

properties of PRCs and needs to be considered in the design of the elastic properties of PRCs.

31

32

33 4.4 Effect of particle shape

34

35

36 As depicted in Fig. 8, the shape of elliptical particles characterized by the aspect ratio of has

37

38

39 affected the interfacial fraction. In this section, we further explore the effect of particle shape on the

40

41

42

elastic moduli of three-phase PRCs through the DEM-FEM model and the micromechanical theory

43

44 framework. Since the elastic properties of PRCs under the relative low packing density of particles (e.g.,

45

46

47 fp 0.4) have been broadly studied in previous references [21-29], we just focus on the issue of the

48

49

50 high particle packing density. Fig. 11 displays respectively the numerical and theoretical results for the

51

52

53

relative elastic moduli E eff / E m of PRCs versus the high packing density of particles with = 1, 2 and 3.

54

55 One can see from the theoretical and numerical results corresponding to a specific particle fraction, that

56

57

58 the change of the relative elastic moduli is very small with the increase from = 1 to = 3. It seems to

59

60

61 imply that the shape of elliptical particles has weak sensitive to the elastic moduli of PRCs with respect

62 21

63

64

65

to the high packing density of particles. Such the exploration is similar to the numerical estimation for

elastic moduli of concrete with the relative low packing density of aggregates reported by Zhou et al.

1

2

3 [21]. From Fig. 11, at first glance, the difference between theoretical and numerical results for a certain

4

5

6 seems to be distinct. Actually, the largest relative error between both results is only 10.7%

7

8 corresponding to = 1 and fp = 0.55. Also, the reason attributes to the difference between both results

9

10

11 for the interfacial fraction shown in Fig. 8 and a certain machine error from implementing the

12

13

14 DEM-FEM model.

15

16

17 4.5 Effect of elastic modulus of interphase

18

19

Although Figs. 8 and 10 have manifested interphase as an important phase links particle to matrix

20

21

22 and its physical properties affected the overall elastic properties of PRCs, it is a huge challenge to

23

24

25 capture separately the elastic modulus of interphase through experiments. Recently, Shah and

26

27

28 coworkers [55] used Backscatter Electron and nanoindentation techniques to experimentally study the

29

30

elastic modulus of interphase (e.g., ITZs) in rock-filled concrete, and found that the elastic modulus of

31

32

33 ITZs is a variance with the porosity. In addition, in most of theoretical or numerical researches [21-29,

34

35

36 41, 42, 53], the elastic modulus of interphase is normally assumed to be a certain percentage of that of

37

38

39 bulk matrix. We here follow the previous predominant lines of study. Fig. 12 depicts the effect of the

40

41

42

ratio of the elastic modulus of interphase and that of bulk matrix on the effective elastic moduli of

43

44 PRCs under the high packing density of particles. One can clearly see that the selection of E i has a

45

46

47 pronounced influence on E eff. To be specific, E eff increases with the increase of E i as a matter of fact. On

48

49

50 the other hand, the relative error between the numerical and theoretical results gradually reduces from

51

52

53

14% to 0.9% with increasing the ratio of E i/ E m from 0.2 to 1.0. Such the deviation maybe originates

54

55 from the error of meshing interphase in the numerical simulations, since the three-phase PRCs

56

57

58 degenerate to two-phase structure consisting of particles and bulk matrix as E i/ E m = 1.0, reducing the

59

60

61 complexity of mesh generation scheme.

62 22

63

64

65

4.6 Effect of geometric size factor

In this section, we investigate the effect of geometric size factor (i.e., the ratio of the interfacial

1

2

3 thickness and the average particle size, t / D eq) on the elastic moduli of PRCs with various high packing

4

5

6 densities of particles. Without loss of generality, we specified the constant interfacial thickness to

7

8 change the average particle size. Eventually, such the effect of also reflects the impact of the average

9

10

11 particle size. Fig. 13 shows the elastic moduli of PRCs nonlinearly increase with the decrease of or

12

13

14 the increase of D eq under different high fp. As an explanatory reason, the effect of on the fraction of

15

16

17 compliant interfaces for 3D cases has been illuminated in our previous work [46] (see Fig. 2 in the

18

19

reference [46]), in which readers can clearly see that the interfacial fraction gradually increases to a

20

21

22 constant value with increasing under a certain fp. As a weak phase, the enhancement of interfacial

23

24

25 fraction induces the reduction of the overall elastic properties of PRCs with increasing . From Fig. 13,

26

27

28 the discrepancy between theoretical and numerical results for a certain appears to be dramatic. But the

29

30

largest relative error between both results is only limited within the scope of 10% corresponding to 1/

31

32

33 = 5 and fp = 0.6. Such the error may attribute to two reasons. One is that, at the high packing density of

34

35

36 particles, the generation of percolating networks of the particle phase and interphase results in the

37

38

39 nonlinear change in the elastic moduli of PRCs. However, the present theoretical scheme does not

40

41

42

explicitly characterize the percolation-type behaviors near the percolation threshold, though the

43

44 simulated results shown in Figs. 8 and 10 seem to indicate the percolation threshold of particles is

45

46

47 within the interval of 0.4 and 0.5, of which the issue will be quantitatively addressed in the further work.

48

49

50 The other is the machine error for the statistical analysis of elastic moduli of PRCs in simulation. It

51

52

53

bears reiterating that these interesting explorations are very important to guide researchers to design

54

55 PRCs for their mechanical applications by controlling the geometric size factor.

56

57

58 5. Conclusions

59

60

61 In summary, we have presented a robust numerical model coupling of the discrete element method

62 23

63

64

65

(DEM) and finite element method (FEM) in details to predict the effective elastic moduli of

particle-reinforced composites (PRCs) containing elliptical particles of high packing density up to 0.8,

1

2

3 compliant interphase and homogeneous matrix. Whilst we devised a theoretical micromechanical

4

5

6 framework incorporating interphase physical characteristics like interfacial fraction, thickness, moduli

7

8 and Poisson ratio into the effective elastic properties of PRCs by using the combination of the

9

10

11 Mori-Tanaka scheme and the equivalent inclusion theory. These numerical and theoretical

12

13

14 models addressed how the interphase characteristics and the geometries of particles dominate

15

16

17 quantitatively the elastic properties of PRCs with a high particle packing density. By comparing the

18

19

available experimental data, the proposed numerical and theoretical models are validated to be efficient

20

21

22 tools for the reasonable estimation of elastic properties of PRCs with a high particle packing density

23

24

25 and interphase. The derived numerical and theoretical results elucidated that, the high particle packing

26

27

28 density plays a predominant role in the interfacial fraction and elastic moduli of PRCs with respect to

29

30

the particle shape. Moreover, the elastic modulus of interphase and the reciprocal geometric size factor

31

32

33 have a positive impact on the elastic moduli of PRCs. These numerical and theoretical observations

34

35

36 provide researchers with significant insights on optimizing the particle geometries and interphase

37

38

39 characteristics for the design of particle-reinforced composites with the high packing density of

40

41

42

nonspherical particles.

43

44 A cknowledgments

45

46

47 This work was supported by the National Natural Science Foundation Project of China [grant

48

49

50 numbers 11402076, 51679078 and 51679265]; the Natural Science Foundation for Jiangsu Province

51

52

53

[grant number BK2017030243]; the Fundamental Research Funds for the Central Universities [grant

54

55 number 2016B06314]; and Research Fund of State Key Laboratory of Simulation and Regulation of

56

57

58 Water Cycle in River Basin [grant number IWHR-SKL-201709].

59

60

61 A ppendix A . Derivation of the elements C ij of the effective stiff matrix

62 24

63

64

65

In Eqs. (31) and (32), C m, C p and C i are isotropic material constant matrices of matrix, particle and

interface, respectively, and their elements can be expressed by individual engineering elastic constants

1

2

3 as

4

5 y 4 y 2 2

6 K 3G K y Gy

3

K y Gy

3

0 0 0

7

8 K y 2Gy 4

K y Gy

2

K y Gy 0 0 0

9 3 3 3

10

11 C K y 2Gy

y

2

K y Gy

4

K y Gy 0 0 0 , y m, p, i (A.1)

12 3 3 3

13

14 0 0 0 Gy 0 0

15 0 0 0 0 Gy 0

16

17 0 0 0 0 0 G y

18

19

Substituting of Eq. (A.1) into Eq. (31), the components of matrices of in Eq. (31) are written by the

20

21

22 engineering elastic constants:

23

24

25 e1 +2e2 e1 -e2 e1 -e2 0 0 0

26

e1 -e2 e1 +2e2 e1 -e2 0 0 0

27

28

e1 -e2 e1 -e2 e1 +2e2 0 0 0

29

1 0 3

30 h d

e1 I e2 I 0 0 e2 0 0 (A.2)

2

31 3

32

0 3

33 0 0 0 e2 0

34 2

35 3

36 0 0 0 0 0 e2

37

2

38

39 Thus, the matrices M of Eq. (31) are expressed by substituting S2 (Supplementary Information) and

40

41

42

Eq. (A.2) as

43

44 M 11 M 12 M 12 0 0 0

45

46 M 21 M 22 M 23 0 0 0

47 M 21 M 23 M 22 0 0 0

48 M S

1

(A.3)

49 0 0 0 M 44 0 0

50 0 0 0 0 M 55 0

51

52 0 0 0 0 0 M 55

53

54

55 where the elements in the matrices are

56

57

58

59

60

61

62 25

63

64

65

1 1 1 1

1

e1 e2 s23 e1 2e2 s22

1

e1 e2 s12 e1 e2 s12

M 11 3 3 , M 12 3 3

M0 1 1 1 1

1

3

e1 2e2 s22 3

e1 e2 s23

M0

3

e1 e2 s23 3

e1 2e2 s22

2

3

4 1 1 1 1

5

e e2 s21

1 3 1 3

e1 e2 s23 1 3

e1 e2 s12 3

e1 2e2 s11

6 M 21 = , M 22

M0 1 1 1 1

e1 e2 s21 e1 2e2 s22 e1 2e2 s22 e1 e2 s21

7 M0

8

9

3 3 3 3

10

1 1

e 2e2 s11 e1 e2 s12

11

12

1 3 1 3 1 1

13 M 23 , M 44

, M 55

M0 1 1 0.5e2 s44 0.5e2 s55

14

15 3

e1 e2 s21 3

e1 e2 s23

16

17

1 1 1

18

19 3

e1 2e2 s11 3

e1 -e2 s12 3

e1 -e2 s12

20

1 1 1

21

22

M 0

3

e1 -e2 s21 3

e1 2e2 s22 3

e1 -e2 s23

23

1 1 1

24

25 3

e1 -e2 s21 3

e1 -e2 s23 3

e1 2e2 s22

26

27

28 where sij are the components of the Eshelby tensor S (see S2). Subsequently, the terms I+SM in Eq.

29

30

(32) are given by

31

32

33 a11 a12 a12 0 0 0

34

35 a21 a22 a23 0 0 0

36 a21

a23 a22 0 0 0

37 I SM (A.4)

38 0 0 0 a44 0 0

39 0 0 0 0 a55 0

40

41 0 0 0 0 0 a55

42

43

44 where the elements in the matrices are

45

46

47 a11 1 s11 M 11 2s12 M 21 , a12 =s11 M 12 s12 M 22 s12 M 23

48

49

50 a21 s21 M 11 s22 M 21 s23 M 21 , a22 1 s21 M 12 s22 M 22 s23 M 23

51

52 a23 a32 s21 M 12 s22 M 23 s23 M 22 , a44 1+s44 M 44 , a55 1+s55 M 55

53

54

55 As the matrices I+SM have been known, the inverse matrix in Eq. (32) can be similarly formulated

56

57

58 by

59

60

61

62 26

63

64

65

b11 b12 b12 0 0 0

b21 b22 b23 0 0 0

b b22 0 0 0

1 1 b

f m I f p I SM p f i I SM i = 21 23 (A.5)

2

3 0 0 0 b44 0 0

4 0 0 0 0 b55 0

5

0 0 0 0 0 b55

6

7

8 where the elements in the matrix are

9

10

1 f m f i a22 f p a22 f i a23 f p a23p f i a12i f p a12p f i a12i f p a12p

i p i

11 1

12 b11 , b12

13 b0 f i a23

i

f p a23p f m f i a22

i

f p a 22p b0 f m f i a22i

f p a22p f i a23

i

f p a 23p

14

15 1 f i a21

i

f p a21p f i a21

i

f p a21p 1 f m f i a11 f p a11

i p

f i a12i f p a12p

16 b21 , b22

17 b0 f m f i a22

i

f p a22p f i a23

i

f p a 23p b0 f i a21

i

f p a21p f m f i a 22

i

f p a 22p

18

19 1 f i a12i f p a12p f i a23

i

f p a 23p 1 1

20 b23 , b44 , b55

21 b0 f m f i a11i f p a11p f i a21 f p a 21

i p

f m f i a44 f p a44

i p

f m f i a55i f p a55p

22

23 f m f i a11i f p a11p f i a12i f p a12p f i a12i f p a12p

24

25 b0 f i a21 i

f p a21p f m f i a22i

f p a 22p f i a 23

i

f p a 23p

26 f i a21

i

f p a21p f i a23

i

f p a 23p f m f i a 22

i

f p a 22p

27

28

29 Therefore, on the substitution of Eqs. (A.1), (A.4) and (A.5) into Eq. (32), the elements C ij of the

30

31

32 effective stiff matrixC (see Eq. (33)) can be obtained by

33

1 1 1

34

35

C11 3c11 2c12 3c22 4c55 , C12 c11 6c12 c22 4c55 , C13 c12 c23 , C33 c22 ,

8 8 2

36

1

37 C 44 c44 c55

38 2

39

40 with

41

42

4 4 4 2 2

43 c11 K m G m

f K G K m G m F11 2 K G K m G m F21

44 3

45

p ,i
3 3
3 3

46

2 4 4 2 2

c12 K m G m

f K G K m G m F12 K G K m G m F22 F23

47

48 3

49 p ,i
3 3
3 3

50

4 4 4 2 2

c22 K m G m

f K G K m G m F22 K G K m G m F12 F23

51

52

53

3 p ,i
3 3
3 3

54

55 2 4 4 2 2

56 c23 K m G m

f K G K m G m F23 K G K m G m F12 F22

57 3 p ,i
3 3
3 3

58

59 c44 G m

f G G m F 44

60 pi

,

61

62 27

63

64

65

c55 G m f G G m F 55

pi

,

where

1

2

3 F11 =a11 b11 2 a12 b21 , F12 =a11 b12 a12 b22 a12 b23 , F21 =a21

b11 a22 b21 a23 b21

4

5

6 F22 =a21 b12 a22 b22 a23 b23 , F23 a21

b12 a22

b23 a23b22 , F44 a44 b44 , F55 a55 b55

7

8

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1

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3 concrete with elliptical aggregate particles, Mag. Concr. Res. 61 (2) (2009) 109117.

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6 [54] R. Hill, Elastic properties of reinforced solids: Some theoretical principles, J. Mech. Phys. Solids

7

8 11 (5) (1963)

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10

11 [55] Y. T. Xie, D. J. Corr, F. Jin, H. Zhou, S. P. Shah, Experimental study of the interfacial transition

12

13

14 zone (ITZ) of model rock-filled concrete (RFC), Cem. Concr. Compos. 55 (55) (2015)

15

16

17

18

19

20

21

22

23

24

25

26

27

28 F igure captions:

29

30

31 F ig.1 Schematic view for the components of contact forces of adjacent particles

32

33

34 F ig.2 (a) the regional division for a sample space and (b) periodic boundary compensation scheme for

35

36

37 DEM

38

39 F ig.3 Two-phase PRCs with 400 overlapping elliptical particles realized by DEM: (a) the aspect ratio

40

41

42 of = 1.5 and the packing density of p = 0.85 and (b) the aspect ratio of = 2.0 and the packing

43

44

45 density of p = 0.80

46

47

48 F ig.4 Schematic diagram for the coordinate transformations of an arbitrary ellipse

49

50 F ig.5 Topological geometries of the interfacial layer around an ellipse (green curve) constructed by the

51

52

53 parametric equation (blue curve) and the the simplified manner (red curve)

54

55

56 F ig.6 Three-phase PRCs composed of the ellipse packing density of p = 0.8. The basic parameters

57

58

59

[41], in which the average size of particles is 450 , the average aspect

60

61

62 33

63

64

65

ratio of particles is = 2.021, two interfacial dimensions of t = 20 (left) and t = 40 (right)

1

2

3 F ig.8 The interfacial fraction f i versus the particle fraction fp with = 1, 2 and 3, where t = 40 and

4

5

6 D eq = 450 followed

[41]

7

8 F ig.9 The relative elastic modulus E eff / E m for PRCs versus the number of particles in (a) = 1.0, (b)

9

10

11 = 1.5, (c) = 2.0 and (d) = 2.5, where p = 0.7, D eq = 1 mm, t = 40 m, E p / E m = 2.5 and E i / E m = 0.5

12

13

14 F ig.10 Comparisons of the elastic moduli from the present DEM-FEM model and micromechanical

15

16

17 framework with the experimental data (three experimental data corresponding to the individual fp)

18

19

reported by Yang [41] and with for the predicted moduli of two-phase PRCs without interphase from

20

21

22 the present micromechanical framework. Basic parameters follow Yangs experiment that E m = 20.76

23

24

25 GPa, E p = 80 GPa, m = 0.2, p = 0.21, i = 0.3, = 2.021, D eq = 450 . (a) t = 20 and E i = 0.43 E m,

26

27

28 (b) t = 40 and E i = 0.65 E m [41]

29

30

F ig.11 The relative effective elastic moduli E eff/ E m versus high packing fraction fp with = 1, 2 and 3.

31

32

33 Basic parameters are specified to be E m = 20 GPa, E p =2.5 E m, E i = 0.5 E m, m = p = i = 0.2, D eq = 450

34

35

36 and t = 40

37

38

39 F ig.12 The effective elastic moduli E eff versus E i/ E m with the high packing density fp = 0.8. Basic

40

41

42

parameters are specified to be E m = 20 GPa, E p = 2.5 E m, m = p = i = 0.2, D eq = 450 , t = 40 and

43

44 = 1.5

45

46

47 F ig.13 The relative effective elastic moduli E eff/ E m versus the reciprocal geometric size factor 1/

48

49

50 ( D eq/t) with three high packing densities fp = 0.6, 0.7 and 0.8 (solid lines and points represent the

51

52

53

theoretical and numerical results with respect to the individual fp, respectively). Basic parameters are

54

55 specified to be E m = 20 GPa, E p = 2.5 E m, E i = 0.5 E m, m = p = i = 0.2, D eq = 450 , t = 100 and

56

57

58 = 1.5

59

60

61

62 34

63

64

65

Fig.1

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Fig.2

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Fig.3(a)

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Fig.3(b)

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Fig.4

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Fig.5

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Fig.6(a)

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Fig.6(b)

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Fig.7

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Fig.8

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Fig.9(a)

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Fig.9(b)

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Fig.9(c)

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Fig.9(d)

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Fig.10(a)

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Fig.10(b)

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Fig.11

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Fig.12

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Fig.13

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