Accepted Manuscript

On the constant parameters of Halpin-Tsai equation

Mahmood M. Shokrieh, Hadi Moshrefzadeh-Sani

PII: S0032-3861(16)30971-5
DOI: 10.1016/j.polymer.2016.10.049
Reference: JPOL 19149

To appear in: Polymer

Received Date: 3 August 2016

Revised Date: 24 October 2016
Accepted Date: 25 October 2016

Please cite this article as: Shokrieh MM, Moshrefzadeh-Sani H, On the constant parameters of Halpin-
Tsai equation, Polymer (2016), doi: 10.1016/j.polymer.2016.10.049.

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On the constant parameters of Halpin-Tsai equation

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Mahmood M. Shokrieh, 2Hadi Moshrefzadeh-Sani
1
Professor, 2Ph. D. Student

Composites Research Laboratory,

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Center of Excellence in Experimental Solid Mechanics and Dynamics,
School of Mechanical Engineering, Iran University of Science and Technology,

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Tehran, 16846-13114, Iran
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Coresponding Author: Shokrieh@iust.ac.ir

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Abstract AN
The Halpin-Tsai method is a well-known technique to calculate the stiffness of composites

reinforced by micro and nano particles. In this method, first the longitudinal and transverse
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moduli of composites are calculated. Then, the elastic modulus of randomly oriented composites

is obtained using an equation contains a constant coefficient. This coefficient is assumed to be

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constant and independent of the matrix and reinforcement properties. The aim of the present
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research is to calculate this coefficient with an analytical model and show that it depends on the
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matrix and reinforcement properties. In this regard, an analytical method called the Mori-Tanaka

laminated analogy (MT-LA) was developed which is able to calculate the elastic modulus of the
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randomly-oriented composites. Comparing the result of the MT-LA method with that of the
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Halpin-Tsai equation, the coefficient of Halpin-Tsai equation was obtained. It was shown that

this coefficient is not constant and depends on the volume fraction and the stiffness ratio of the

matrix to reinforcement. Finally, using this new coefficient, equations are presented which are

able to compute the elastic modulus of both platelet and fibrous randomly oriented composites.

Using the mechanical properties of the carbon nanotube (CNT), graphene sheet (GS) and the
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polymer, the elastic moduli of nanocomposites were calculated. The results were compared with

experimental data available in the literature. It was shown that more accurate results were

achieved by using this new coefficient in the Halpin-Tsai equation.

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Keywords: Halpin-Tsai method; laminated analogy approach; randomly oriented composites.

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1. Introduction

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The Halpin-Tsai [1] and modified role of mixture [2] methods are known as two most
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straightforward ways to calculate the elastic modulus of the randomly oriented composites.

These methods are widely used to calculate the modulus of nanocomposites reinforced by
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various nano particles [3,4]. The Halpin-Tsai method is very popular in both micro and nano

mechanics because of its simplicity [6-8]. In fact, this method is suggested to calculate the
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longitudinal and transvers properties of the aligned reinforcement composites and the stiffness of
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the randomly oriented composites is usually calculated as aEL + (1 − a) ET , where E L and E T

are the longitudinal and transvers moduli of the iso-oriented composites, respectively and a is a
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constant coefficient. The coefficient a is considered to be equal to 3/8 when the fibers are
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dispersed two-dimensionally [2]. van Es et al. [9] found that the value of the coefficient a is
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0.184 when the fibers are dispersed three-dimensionally. For the composites with the platelet-

reinforcement the coefficient a is considered to be equal to 0.49 [10], however some researchers

used a equal to 3/8 for this kind of composites [11-13]. The CNTs are dispersed three

dimensionally in the matrix but some researchers [14] also used a = 3/8 in their modeling,

although this value were suggested for the composites with 2-D dispersion of the reinforcement.
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To the best knowledge of the present authors, the coefficient a is always assumed to be constant

and independent of the matrix and reinforcement properties. It seems that there is a lack of

analytical studies to calculate this coefficient. In this paper to obtain the value of this coefficient,

a new analytical method (MT-LA) is developed which is able to calculate the elastic modulus of

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the randomly oriented composites directly. The MT-LA is a combination of the Mori-Tanaka

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[15] and the laminated-analogy [16] methods. Comparing the results of the MT-LA method with

the Halpin-Tsai equation, the new value of the coefficient a is obtained. It was shown that the

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coefficient a is not constant and depends on the volume fraction and the ratio of the stiffness of

the matrix to that of the reinforcement. The calculated results according to this non-constant

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coefficient and the Halpin-Tsai method were compared with some experimental data available in
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the literature. It was shown that more accurate results were achieved by the Halpin-Tsai model
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with non-constant coefficient.

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2. The Halpin-Tsai method

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The Halpin-Tsai method is a semi-empirical method, which usually uses to calculate the elastic
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modulus of both fibrous and platelet reinforcement composites. This method is very popular in

both micro and nano mechanics because of its simplicity. In this method, the longitudinal and
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transverse moduli (EL and ET) of composites were calculated. For the fibrous-composites, EL and
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ET are obtained from the following equations [1]:

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l
1 + η LV f 1 + 2ηT V f
E L = Em r , ET = Em
1 − η LV f 1 − ηT V f
Er Er (1)
−1 −1
Em Em
ηL = , ηT =
Er l Er
+ +2

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Em r Em

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For the platelet-reinforcement composites EL and ET are obtained from the following equations

[1]:

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l
1 + 2 η LV f 1 + 2ηT V f
E L = Em t , ET = Em
1 − η LV f 1 − ηT V f
Er
−1
Er
−1
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Em Em
ηL = , ηT =
Er l Er
+2 +2
Em t Em
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where Em and Er are the elastic moduli of the matrix and reinforcement, respectively Also, l is the
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length of the reinforcement. Moreover, r and t are the radius and thickness of the fibrous and
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platelet reinforcement, respectively. The elastic modulus of randomly-oriented composites (EC)

was obtained using the following equation [2]:

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EC = aEL + (1 − a) ET (3)
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where traditionally a = 0.375 (i.e., 3/8) for 2-D and a = 0.184 for 3-D dispersion of the fibrous
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reinforcements [9]. To the best knowledge of the present authors, the coefficient a is always

assumed to be constant. In this paper, using the MT-LA, the non-constant value of the coefficient

a is explored for different volume fractions and stiffness ratios of the reinforcement and matrix.
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3. The Mori-Tanaka laminated analogy (MT-LA) approach

In this paper the Mori-Tanaka [15] and the laminated analogy [16] methods were coupled

together to calculate the elastic modulus of the randomly oriented composites. In this regard, the

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Mori-Tanaka method is used to calculate the stiffness matrix of the aligned reinforcement

composites and then the stiffness of the randomly oriented composites is calculated by the

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laminated analogy approach.

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Some specific assumptions are assumed here:

- The effect of nano particle waviness was neglected.

-
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Both nanoparticle and matrix are linear elastic.
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- Perfect bond exists between the nano particles and matrix.

- There is no residual stress between the nano particles and matrix.

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One of the main limitations of the present method is neglecting the agglomeration of the
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nano particles. So, the modeling was done for nanocomposites with volume fraction less than
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1%.
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• The Mori-Tanaka method

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The Mori-Tanaka method is one of the advanced micromechanical method which is able to
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calculate the stiffness tensor of composites with different reinforcement shapes. The effect of

collective interactions of reinforcements is considerable in this method and it is known as a

common way to model the nanocomposites [17-19]. In this method, it is assumed that each

inclusion is embedded in an infinite pristine matrix subjected to an effective strain ε m or an

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effective stress σ m in the far field, where ε m and σ m denote the average strain and the average

stress over the matrix, respectively. The fourth-order tensor A relates the average strain of the

reinforcement εr and matrix ε m via ε r = A : ε m and it is given by:

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A = ( I + S : (C m ) − 1 : (C r − C m )) −1 (4)

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where S is the Eshelby tensor. The Eshelby tensor was calculated analytically for the ellipsoid

shape reinforcements, which is well documented in reference [20]. The effective stiffness tensor

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C of the aligned reinforcement composites of the same shape is given by:

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C = (V f C m + V f C r : A) : ((1 − V f ) I + V f A) −1 (5)
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where, C m and C r are the matrix and reinforcement stiffness tensor, respectively. Moreover, I
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is the fourth-order identity tensor. In the above equations a colon between two tensors denotes

contraction (inner product) over two indices.

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• Laminated analogy approach

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The laminate analogy (LA) is a method which was commonly used to calculate the stiffness and

strength of random short-fiber composites. This method was proposed by Halpin and Pagano
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[16]. In this method, it was assumed that the in-plane random material was treated as a stack of
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infinitesimally thin unidirectional plies bonded together with different fiber angle orientations. In

this approach, the layers are interactive and the state of the stress in each layer affected by other

layers properties. Chen [21] used the LA to calculate the stiffness and strength of composites.

Halpin et al. [22] extended the LA to estimate the stiffness of the woven fabric composites. It
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was also shown that LA is able to calculate the elastic modulus of hybrid composites [23,24]. To

the best knowledge of the present authors, the LA method has not been employed to estimate the

mechanical properties of nanocomposites.

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In the present article, the LA approach is employed to calculate the stiffness of nanocomposites.

First, the LA approach is extended to a three dimensional form called 3-D LA. Then, using the

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stiffness matrix of the aligned reinforcement composites (obtained by the Mori-Tanaka method),

the elastic modulus of the nanocomposites is calculated by the 3-D LA.

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The random orientation of reinforcements in composites is one of the big challenges in modeling

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of this kind of materials. The first step of the modeling is to make the equivalent laminated
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composites (ELC) with appropriate simplifications and assumptions. The ELC is a laminated

composite equivalent to the randomly-oriented composites. Then, using the classical lamination
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theory (CLT) the elastic modulus of the ELC is obtained. The reinforcements with similar
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orientation are considered to be located in one layer of the ELC. As shown in Fig. 1, the

orientation of the reinforcement is defined by α and β angels. These angels are varied from 0o
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to 90o. Therefore, the ELC consists of several iso-oriented reinforcement layers, which their
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orientation angels are between 0o to 90o (Fig. 1). In the modeling process, selecting numbers of

layers of the ELC is optional. It is clear that increasing the numbers of layers improves the
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accuracy of the model. As the volume fraction of the layers is identical, the thickness of the
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layers is also identical.

The stiffness matrix of each layer is obtained by rotating the on-axis stiffness matrix around the y

and z axes. Finally, assuming that the strain field is identical for all layers, the stiffness matrix of

the ELC is calculated.

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Fig. 1 Equivalent laminated composites
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The stiffness matrix ( [C ] ) of the aligned-reinforcement composites with elliptical reinforcement

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is obtained by the Mori-Tanaka model. This orthotropic stiffness matrix is defined in the on-axis
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coordinate system. However, in the present model matrix is defined in the off-axis coordinate

system. In this regard, first the stiffness matrix [C ] is transformed to  C *  by rotating around
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the y axis by an angel of β . Then, the matrix  C *  is transformed to  C **  by rotating around

β αβ
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the vertical axis (z) by an angel of α as follows:

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C *  = [Tσ ]β [ C ][Tε ]β

−1
β

C **  = [Tσ ]α C *  [Tε ]α

−1
αβ β

(6)
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where [Tε ] and [Tσ ] are the strain and stress transformation matrices, respectively [25].

• The stiffness matrix of the ELC

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The average stress in the ELC is calculated as:

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N

∑σ i
k
hw
1 N
σi = k =1
= ∑σ k

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i h , i , j = 1, 2, ..., 6 (7)
wH H k =1

where k and N are the layer number and the total number of layers, respectively. Moreover, w

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and H are the width and the total thickness of composites, respectively. The load per unite width
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is calculated as:
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N
Ni = ∑Cij**kε j h , i, j = 1, 2, ..., 6 (8)
k =1
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The stiffness matrix A is also calculated as:

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N
Aij = ∑Cij**k h , i, j = 1, 2, ..., 6 (9)
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k =1

Finally, using the compliance matrix aij=Aij-1, the modulus of composites is obtained as follows:
C
AC

1
EC = (10)
Ha11

4. Calculating the value of the coefficient a

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The elastic modulus of the fibrous and platelet reinforcement composites is calculated by the

MT-LA method, then using Eq. 3 the value of the coefficient a is obtained as follows

EC − ET
a= (11)
EL − ET

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where EL and ET are calculated with the Halpin-Tsai equation and EC is also obtained by the MT-

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LA method.

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It is noted that the number of layers (N) in the LA method could be chosen optionally and the

final results depends on this optional number, but this accuracy of the results increases by

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increasing the number of layers. In Fig. 2, the variations of the EC/Em versus the number of layers
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for the CNT and GS nanocomposites are shown. As shown, the modulus of the composites is

converged to a constant magnitude when N>4000, therefore 5000 layers were chosen for the
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modeling. It is assumed that the effective modulus of the CNT and GS are 446.67 GPa [26] and
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250 GPa [27], respectively. High aspect ratio nanoparticles are used in this section. The aspect
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ratio of both CNT and GS are assumed to be 1500 [28-29]. Where the aspect ratio of the CNT is

the ratio of the length to the diameter (l/d) and the aspect ratio of the GS is the ratio of the length
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to the thickness (l/t).

C
AC
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Fig. 2 Modulus of the ELC versus the numbers of layers
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The variation of the coefficient a versus the volume fraction of the high aspect ratio
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reinforcements is shown in Figs. 3-5. As shown in all these figures, the coefficient a increases by

increasing the Er/Em, however for Er/Em>200 this increase is negligible. As shown in Fig. 3, for
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the 2-D fiber-reinforcement distribution, the magnitude of coefficient a decreases by increasing

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the volume fraction. While, as shown in Fig. 4, for the 3-D fiber-reinforcement distribution, the
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coefficient a increases by increasing the volume fraction. Also, as shown in Fig. 5, for the

platelet-reinforcement composites the magnitude of coefficient a decreases by increasing the

volume fraction of the reinforcement.

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Fig. 3 Coefficient a versus the volume fraction, for 2-D dispersion of the reinforcement
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D
TE
C EP
AC

Fig. 4 Coefficient a versus the volume fraction, for 3-D dispersion of the fibrous reinforcement
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Fig. 5 Coefficient a, versus the volume fraction, for 3-D dispersion of the platelet-reinforcements
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The value of the coefficient a is obtained by the curve fitting of the above curves as follows. For
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composites with 2-D dispersion of the fibrous reinforcements:

E 
a = 0.339 − 0.035V f − 0.642  m 
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(12)
 Er 
C

For composites with 3-D dispersion of the fibrous reinforcements:

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E 
a = 0.13 + 0.0815Vf −1.669  m  (13)
 Er 

For composites with 3-D dispersion of the platelet reinforcements:

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E 
a = 0.443 − 0.07Vf −1.468  m  (14)
 Er 

Using Eqs. 12-14 into Eq. 3, the elastic modulus of the randomly oriented composites could be

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calculated.

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5. Verification of the present model

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In this section, using the new values of coefficient a in the Halpin-Tsai equation, the elastic

modulus of the CNT and GS-nanocomposites were calculated. The results compared with some

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experimental data available in the literature. The mechanical properties of the CNT are taken
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from the analytical results of Popov et al. [26]. Moreover, the properties of the GS are taken from
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references [30,27]. The results are presented in Tables 2 and 3.

The coefficient a is usually considered to be equal to 3/8 for fibrous reinforcements [2]. In
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reference [9], it was shown that the value of the coefficient a is 0.184 when the fibers are
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dispersed three-dimensionally. In the present work, according to Eq. 13 it is found that the

coefficient a is equal to 0.13 when the Vf and Em/Er are negligible, this value is comparable with
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0.184 which is suggested by the van Es et al. [9]. In Table 2, the modulus of the CNT
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nanocomposites are calculated using the Halpin-Tsai equation with different values of the
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coefficient a (3/8, 0.184 and using Eq. 13) and compared with some experimental data available

in the literature. Table 2 shows that the elastic moduli obtained by the Halpin-Tsai equation in

most cases are closer to the experimental results when the value of the coefficient a was

calculated using Eq. 13.

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Table 2. The elastic modulus of CNT/epoxy nanocomposites using the Halpin-Tsai equation with

different values of the coefficient a (3/8, 0.184 and using Eq. 13)

Composites Composites Composites

Composites
Matrix volume modulus modulus modulus
modulus

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modulus (Halpin-Tsai Error (Halpin-Tsai Error (Halpin-Tsai, Error
Researcher fraction
(experimental)
(%) (%) (%)
Em (GPa) Vf % a = 3/8) a = 0.184 ) a = Eq . 13 )
EC (GPa)
EC (GPa) EC (GPa ) E C (GPa )

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Zhu et al. [31] 2.026 0.882 2.650±0.12 3.504 32.2 2.760 4.15 2.519 4.91

Manchado et 0.370 1.100 1.476 34.2 1.162 5.63 1.069 2.81

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0.855
al. [32] 0.563 1.180 1.800 52.5 1.320 11.86 1.181 0.09

Villoria and 2.875 0.120 2.909 3.075 5.7 2.974 2.23 2.939 1.04

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Miravete [33] 2.587 0.470 2.659 3.372 26.8 2.970 11.69 2.843 6.93
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Fidelus et al. 0.009 3.013 2.959 1.7 2.952 2.01 2.949 2.09
2.945
[34] 0.043 3.088 3.016 2.3 2.98 3.49 3.00 2.80

0.032 3.040 2.953 2.8 2.926 3.75 2.927 3.71

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Geng et al. [28] 2.900 0.064 3.164 3.000 5.0 2.952 6.67 2.954 6.63

0.160 3.158 3.167 0.3 3.032 3.98 3.035 3.87

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Song and Youn 0.290 1.418 1.697 19.6 1.45 2.25 1.376 2.94
1.210
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[35] 0.580 1.616 2.184 35.1 1.69 4.57 1.543 4.51

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For the composites with the platelet-reinforcement, the coefficient a is usually considered to be

equal to 0.49 when the reinforcements are dispersed three-dimensionally [10]. According to Eq.
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14, it was found that the coefficient a is equal to 0.443 when Vf and Em/Er are negligible, this
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value is close to 0.49 which was suggested in reference [10]. The elastic modulus of the

GS/epoxy nanocomposites are calculated using the Halpin-Tsai equation with two different

values of the coefficient a (0.49 and using Eq. 14). The results are compared with some

experimental data available in the literature in Table 3. This table shows that the elastic moduli
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obtained by the Halpin-Tsai equation in most cases are closer to the experimental results when

the value of the coefficient a was calculated using Eq. 14.

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Table 3. The elastic modulus of GS/epoxy nanocomposites and using the Halpin-Tsai equation with

different values of the coefficient a (0.49 and using Eq. 13)

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Composites Composites modulus Composites
volume
Matrix modulus modulus (Halpin- Tsai modulus (Halpin-

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fraction
Researcher (experimental) a = 0.49 ) Error (%) Tsai, a = Eq.14 ) Error (%)
Em (GPa)
Vf %
Em (GPa) Em (GPa) Em (GPa)

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Yasmin et al. [29] 3.5 1.130 4.55 4.68 2.85 4.53 0.43

0. 280 3.65 3.72 1.91 3.68 0.82

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Potts et al. [36]
3.43 0. 560 4.19 4.01 4.29 3.93 6.20

1.130 4.39 4.61 5.01 4.45 1.36

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Zheng and Wong 0.566 2.85 3.06 7.51 2.97 4.30

2.8
[37] 2.260 3.11 3.86 24.32 3.73 20.12
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0.600 2.70 2.69 0.37 2.65 1.85

Kim and Macosko
2.35 1.800 3.09 3.40 10.03 3.27 5.82
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[38]
2.400 3.69 3.74 1.35 3.58 2.98

0.005 2.56 2.58 0.78 2.57 0.39

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0.106 2.62 2.65 1.14 2.61 0.38

Shokrieh et al. [13] 2.5
0.264 2.70 2.88 6.66 2.84 5.18
C

0.528 2.73 3.27 19.78 3.19 16.84

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Conclusions

The elastic modulus of randomly oriented composites is traditionally calculated by using the

Halpin-Tsai equation. This equation contains a constant coefficient which is assumed to be

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constant and independent of the matrix and reinforcement properties. The aim of the present

research is to calculate this coefficient with an analytical model and show that it depends on the

matrix and reinforcement properties. In this regards a new approach called the MT-LA method

was presented which is able to calculate the elastic modulus of the randomly oriented

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composites, containing fibrous or platelet reinforcements. The new values of this coefficient

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were obtained by combining the MT-LA and the Halpin-Tsai method. It is shown that this

coefficient depends on the volume fraction and stiffness-ratio of the matrix and reinforcement.

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Using this new coefficient, the elastic modulus of the CNT and GS nanocomposites were

calculated and compared with some experimental data available in the literature. It was shown

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that more accurate results were achieved by using this new coefficient in the Halpin-Tsai
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equation.
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Research Highlights

• By combining the Mori-Tanaka (MT) and Laminated Analogy (LA) methods, a new
model (MT-LA) was presented.
• The MT-LA calculates the elastic modules of the randomly oriented composites, like

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nanotube or graphene nanocomposites.
• Using the MT-LA, it was proved that the so called constant coefficient of Halpin-Tsai

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(HT) method is a variable and not a constant.
• It is found that this coefficient depends on the volume fraction and the stiffness ratio of

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the matrix to reinforcement.

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