Revista de Chimie, 2004: 55(6), 444-448.

BASIC PHENOMENOLOGICAL MODELLING OF RHEOLOGICAL BEHAVIOUR OF TERNARY PHASE IN PHASE POLYMER COMPOSITE SYSTEMS. I. UNIFORM DEFORMATION APPROACH Horia PAVEN, Chemical Research Institute-ICECHIM , Bucuresti, Splaiul Independentei, nr. 202 (htopaven@netscape.net)

The development of the proposed approach is mainly focused on the clarification of first phenomenological principles in the case of the basic model of uniform deformation, within the realm of a non-conventional hierarchical approach, in the case of ternary phase in phase composite polymer systems. Accordingly, the standpoint of behaviour laws- selection rules- mixing rules sequence is considered,

the use of intrinsic morpho-rheological interactions, expressing the morphologically controlled dependence of composite rheological variables versus the component ones, and the use of differential rheological operators represent the start point in establishing the behaviour law of model composite. As consequences, the corresponding selection rules - the quantitative and qualitative morpho-rheological effects as well as the specific mixing rules for the characteristic rheological quantities are given and illustrated in a suitable form for simulation and analysis.

Keywords: Rheological phenomenology, linear viscoelastic behaviour, ternary phase in phase composite systems, polymer components, uniform deformation modelling

The outstanding mechanical properties of polymer composite materials, including macro-, micro- and nano-level, and especially the unique combination of low density with high stiffness and strength which can be achieved with such materials have led not only to extensive research programs aiming at establishing the underlying essentials regarding the way in which the composite properties are controlled by thoses of components, composition, morphology and

different physical-chemical interactions, but also to highly sophisticated technologies. Consequently, there are now many authoritative references concerning the elastic properties of composites, wherein a great deal of valuable information is available /1-6/, /8-11/. Composite materials which contain one or more polymeric components exhibit, as is well known, but unfortunately often disregarded in practical applications , a significant amount of time-dependent behaviour in service conditions, a large number of significant contributions on viscoelastic properties of composites being also issued /3-7/, /12-17/. It is worth mentioning the fact that the viscoelastic-like characteristics are certainly rather profitable than troublesome for the rational user, provided these properties are properly understood and implemented in design, and in the literature there are many relevant contributions concerning the question of the behaviour of composite systems with linear viscoelastic components. Naturally, given the more complex character of viscoelastic behaviour, there are more facts to be considered with greatest caution, the standard relationships established for the elastic moduli or compliances needing to be carefully used in the framework of conventional approach of the well known, but often improperly employed, linear elastic-viscoelastic correspondence principle, when the simply insert of complex viscoelastic quantities in lieu of the elastic ones, without the necessary feeling of the procedure, may provide uncertain results. The forthcoming analysis of the ternary phase in phase composite system with components exhibiting linear viscoelastic behaviour is performed within the realm of a nonconventional hierarchical approach including the rheological behaviour laws(BL) - selection rules(SR) - mixing rules(MR) sequence /18-46/. As result of the intrinsic morpho-rheological interactions, expressing in a well defined manner the morphologically controlled dependence of composite rheological variables versus the component ones, the behaviour law of model composite arises in a natural way. Next, by using the rheological operators thus obtained, the corresponding selection rules providing the allowed rheological state of composite for given component ones are given, and the corresponding quantitative or qualitative morpho-rheological effects are pointed out.

Moreover, the specific mixing rules for the characteristic rheological quantities are given in a suitable form for simulation and analysis. Taking into account the large diversity and multi-level complexity of morphological architecture of real composite systems, the development of the proposed approach is mainly focused on the clarification of first principles in the case of the basic models of uniform deformation and uniform stress, respectively, in order to bridge the conceptual gap between binary and ternary phase in phase composite systems containing at least one polymer component.

Basic [3V] inter-relationships Let us consider the a / b / c ternary phase in phase composite system with a, b and c linear viscoelastic components in the {a}, {b} and {c} rheological states, respectively, described by the corresponding rheological orders (ma, na), (mb, nb) and (mc, nc) in virtue of component rheological equations Pa a = Qa a Pb b = Qb b Pc c = Qc c The component rheological operators are defined as (1.1) (1.2) (1.3)

Pa = p0,a + p1,a D + p 2,a D 2 + ... + p ma ,a D ma Qa = q0,a + q1,a D + q2,a D 2 + ... + qna ,a D na Pb = p0,b + p1,b D + p 2,b D 2 + ... + p mb ,b D mb Qb = q0,b + q1,b D + q 2,b D 2 + ... + q nb ,b D nb Pc = p0,c + p1,c D + p2,c D 2 + ... + pmc ,c D mc Qc = q0,c + q1,c D + q2,c D 2 + ... + qnc ,c D nc

(1.1.1) (1.1.2) (1.2.1) (1.2.2) (1.3.1) (1.3.2)

where a , a ; b , b ; c , c are the component rheological variables - the stress and strain, respectively, and Dk = dk/dtk represents the k-th order time derivative. In the case of Voigt-like, uniform deformation, composite model, the [3V] basic morpho-rheological interaction, i.e., the [3V] morphologically controlled interaction of the component rheological states, can be symbolised in the form
3V {a} + {b} + {c} [] {a / b / c}[3V] 3V (ma, na) + (mb, nb) + (mc, nc) [] (m[3V], n[3V])

(1.4.1.1) (1.4.1.2)

As a direct consequence of the relationships between the composite and component rheological variables

[ 3V ] = a = b = c

(1.4.2.1) (1.4.2.2)

[ 3V ] = v a a + vb b + v c c

where [ 3V ] , [ 3V ] are the [3V] model composite rheological variables, and v a , vb , vc represent the component volume fractions, (v a + vb + vc = 1) , the corresponding [3V] rheological equation, which express the [3V] model composite behaviour law, is
P[ 3V ] = Q[ 3V ]

(1.5)

where the composite rheological operators versus the component ones are given as
P[3V ] = Pa Pb Pc Q[ 3V ] = v a Pb Pc Qa + vb Pa Pc Qa + v c Pa Pb Qc

(1.6.1) (1.6.2)

Accordingly, the set of [3V] selection rules results as follows

m[ 3V ] = Ord.{P[3V]} = ma + mb + mc n[ 3V ] = Ord.{Q[3V]} = max ( ma + mb + nc ,

(1.7.1)

m a + mc + n b , mb + mc + n a )

(1.7.2)

the corresponding morpho-rheological interaction parameters being presented in table 1.1

--------------------------------------------------------------------------Table 1.1 [3V] Morpho-rheological interaction parameters --------------------------------------------------------------------------Moreover, the corresponding [3V] specific mixing rules for the viscoelastic moduli yields, in the case of complex moduli
* * * M [*3V ] = v a M a + vb M b + vc M c

(1.8)

while for storage and loss moduli one obtains

M [3V ] = v a M a + vb M b + v c M c M [ V ] = v a M a + vb M b + v c M c 3

(1.8.1) (1.8.2)

[3V] morpho-rheological effects In order to illustrate the quantitative and qualitative forms of [3V] morpho-rheological effects, three simple rheological models are considered for components, e.g., - Hooke: {1} (m = 0, n = 0), P{1} = p 0 ,r , Q{1} = q 0, r ; r = 1, 2, 3; - Kelvin-Voigt: {2} (m = 0, n = 1), P{2} = p 0,r , Q{2} = q0,r + q1,r D ; r = 1, 2, 3; - Poynting-Thomson-Zener: {3} (m = 1, n = 1),
P{3} = p 0, r + p1,r D , Q{3} = q 0,r + q1,r D ; r = 1, 2, 3;

the results being summarized in table 1.2. --------------------------------------------------------Table 1.2 [3V] morpho-rheological effects ---------------------------------------------------------

It is notable that as result of the symmetrical form of of composite rheological operators in respect the permutation of components, invariance consequences are observed. Moreover, from the standpoint of morpho-rheological effects different outcomes take place. Firstly, it results, there are well defined cases in which the composite has the same rheological state, i.e., the same rheological potential: - {1} rheological state, for the {1}/{1}/{1} composite; - {2}, for {1}/{1}/{2}, {1}/{2}/{1}, {1}/{2}/{2}, {2}/{1}/{1}, {2}/{1}/{2}, {2}/{2}/{1} and {2}/{2}/{2}; - {3}, for {1}/{1}/{3}, {1}/{3}/{1} and {3}/{1}/{1} composite; - {4}, for {1}/{2}/{3}, {1}/{3}/{2}, {2}/{1}/{3}, {2}/{2}/{3}, {2}/{3}/{1}, {2}/{3}/{2}, {3}/{1}/{2}, {3}/{2}/{1} and {3}/{2}/{2}; - {5}, for {1}/{3}/{3}, {3}/{1}/{3} and {3}/{3}/{1} composite; - {6}, for {2}/{3}/{3}, {3}/{2}/{3} and {3}/{3}/{2}; - {7} rhelogical state, for {3}/{3}/{3} composite. Moreover, it appears that the rheological order of composite rheological equation may be identical to that of highest order component, typical quantitative morpho-rheological effects being pointed out as follows: - {1} rheological state, for {1}/{1}/{1} composite; - {2}, for {1}/{1}/{2}, {1}/{2}/{1}, {1}/{2}/{2}, {2}/{1}/{1}, {2}/{1}/{2}, {2}/{2}/{1} and {2}/{2}/{2}; - {3} rheological state, for {1}/{1}/{3}, {1}/{3}/{1} and {3}/{1}/{1}. Furthermore, there are well defined qualitative morpho-rheological effects, when the rheological order of composite is higher than of all components: - {4} rheological state, for {1}/{2}/{3}, {1}/{3}/{2}, {2}/{1}/{3}, {2}/{2}/{3}, {2}/{3}/{1}, {2}/{3}/{2}, {3}/{1}/{2}, {3}/{2}/{1} and {3}/{2}/{2} composites; - {5}, for {1}/{3}/{3}, {3}/{1}/{3}, and {3}/{3}/{1}; - {6}, for {2}/{3}/{3}, {3}/{2}/{3}, {3}/{3}/{2}; - {7} rheological state, for {3}/{3}/{3} composite.

[3V] primary mixing rules In order to illustrate the manner in which the composite rheological parameters result, in virtue of behaviour law, versus the component rheological parameters and composition, two typical situations are considered for the components: - the (1, 1) - rheological model, i.e. the mono-relaxant (retardant) , and - the (2, 2) - rheological model of bi-relaxant (retardant) behaviour. In the former case, of (1, 1) components, the corresponding rheological operators are
Pa = p 0,a + p1,a D , Pb = p 0,b + p1,b D , Pc = p 0,c + p1,c D , Qa = q 0,a + q1,a D Qb = q 0,b + q1,b D Qc = q 0,c + q1,c D

(1.9.1) (1.9.2) (1.9.3)

the resulting composite rheological operators being

P[3V ] = p0 + p1 D + p 2 D 2 + p3 D 3 Q[3V ] = q0 + q1 D + q 2 D 2 + q3 D 3
p 0 p 0,[ 3V ] = p 0,a p 0,b p 0 ,c p1 p1,[3V ] = p 0, a ( p 0,b p1,c + p 0,c p1,b ) + p 0,b p 0,c p1,a

(1.10.1) (1.10.2)

where the composite rheological parameters are given versus those of components as (1.10.1.1) (1.10.1.2) (1.10.1.3) (1.10.1.4) (1.10.2.1)

p 2 p 2,[3V ] = p0,a p1,b p1,c + p0,a ( p0,b p1,c + p 0,c p1,b ) + + p 0,b p 0,c p1,a
p 3 p 3,[ 3V ] = p1, a p1,b p1,c

and
q 0 q 0,[ 3V ] = v a p 0,b p 0,c + vb p 0,a p 0,c q 0,b + v c p 0,a p 0,c q 0,c

q1 q1,[ 3V ] = v a [( p 0,b p1,c + p 0,c p1,b )q 0,a + p 0,b p 0,c q1,a ] + + vb [( p 0,a p1,c + p 0,c p1,a )q0,b + p 0,a p 0,c q1,b ] + + vc [( p 0,a p1,b + p 0,b p1,a )q 0,c + p 0,a p 0,b q1,c ] (1.10.2.2)

q 2 q 2,[ 3V ] = v a [( p 0,b p1,c + p 0,c p1,b )q1,a + p1,b p1,c q 0,a ] + + vb [( p 0,a p1,c + p 0,c p1,a )q1,b + p1,a p1,c q 0,b ] + + vc [( p 0,a p1,b + p 0,b p1,a )q1,c + p1,a p1,b q 0,c ]
q 3 q 3,[3V ] = v a p1,b p1,c q1, a + vb p1,a p1,c q1,b + v c p1, a p1,b q1,c

(1.10.2.3)

(1.10.2.4)

In the latter case, of (2, 2) components, the corresponding rheological operators are defined as

Pa = p0,a + p1,a D + p 2,a D 2 , Pb = p0,b + p1,b D + p 2,b D 2 , Pc = p0,c + p1,c D + p 2,c D 2 ,

Qa = q0,a + q1,a D + q 2,a D 2 Qb = q0,b + q1,b D + q 2,b D 2 Qc = q0,c + q1,c D + q 2,c D 2

(1.11.1) (1.11.2) (1.11.3)

the resulting composite rheological operators being

P[3V ] = p0 + p1 D + p 2 D 2 + p3 D 3 + p 4 D 2 + p5 D 5 + p6 D 6 Q[3V ] = q0 + q1 D + q 2 D 2 + q3 D 3 + q 4 D 2 + q5 D 5 + q6 D 6

(1.12.1) (1.12.2)

where the composite rheological parameters in terms of the component ones are
p 0 p 0,[ 3V ] = p 0,a p 0,b p 0 ,c p1 p1,[3V ] = p 0, a p 0,b p1,c + ( p 0,a p1,b + p 0.b p1,a ) p 0 ,c

(1.12.1.1) (1.12.1.2) (1.12.1.3)

p 2 p 2,[3V ] = p0,a p0,b p 2,c + ( p0,a p1,b + p0,b p1,a ) p1,c + + ( p 0,a p 2,b + p1,a p1,b + p 0,b p 2,a ) p 0,c
p3 p3,[ 3V ] = ( p 0,a p1,b + p 0,b p1,a ) p 2,c + + ( p0,a p 2,b + p1,a p1,b + p 0,b p 2,a ) p1,c + + ( p1,a p 2,b + p1,b p 2,a ) p 0,c

(1.12.1.4)

p 4 p 4,[3V ] = ( p0,a p 2,b + p1,a p1,b + p 0,b p 2,a ) p 2,c + + ( p1,a p 2,b + p1,b p 2,a ) p1,c + p 0,c p 2,a p 2,b
p 5 p 5,[ 3V ] = ( p1,a p 2,b + p1,b p 2, a ) p 2,c + p1,c p 2, a p 2,b

(1.12.1.5) (1.12.1.6)

p 6 p 6,[ 3V ] = p 2,a p 2,b p 2,c

(1.12.1.7)

and
q 0 q 0,[3V ] = v a p 0,b p 0,c q 0,a + vb p 0,a p 0,c q 0,b + v c p 0, a p 0,b q 0,c (1.12.2.1)

q1 q1,[3 R ] = v a [ p 0,b p 0,c q1,a + ( p 0,b p1,c + p 0,c p1,b )q 0,a ] + + vb [ p 0,a p 0,c q1,b + ( p 0,a p1,c + p 0,c p1,a )q 0,b ] + + v c [ p 0,a p 0,b q1,c + ( p0,a p1,b + p 0,b p1,a )q 0,c ] (1.12.2.2)

q 2 q 2,[ 3V ] = v a [ p 0,b p0,c q 2,a + ( p 0,b p1,c + p0,c p1,b )q1,a + + ( p 0,b p 2,c + p1,b p1,c + p 0,c p 2,b )q0,a ] + + vb [ p 0,a p 0,c q 2,b + ( p 0,a p1,c + p0,c p1,a )q1,b + + ( p 0,a p 2,c + p1,a p1,c + p 0,c p 2,a )q 0,b ] + + vc [ p0, a p0,b q 2,c + ( p0, a p1,b + p0,b p1,a )q1,c + + ( p 0,a p 2,b + p1,a p1,b + p0,b p 2,a )q0,c ] q3 q3,[ 3V ] = v a [( p 0,b p1,c + p 0,c p1,b )q1,a + + ( p 0,b p 2,c + p1,b p1,c + p 0,c p 2,b )q1,a + + ( p1,b p 2,c + p1,c p 2,b )q 0,a ] + + vb [( p 0,a p1,c + p 0,c p1,a )q 2,b + + ( p 0,a p 2,c + p1,a p1,c + p 0,c p 2,a )q1,b + + ( p1,a p 2,c + p1,c p 2,a )q 0,b ] + + vc [( p 0,a p1,b + p 0,b p1,a )q 2,c + + ( p 0,a p 2,b + p1,a p1,b + p 0,b p 2,a )q1,c + + ( p1,a p 2,b + p1,b p 2,a )q 0,c ] (1.12.2.4) (1.12.2.3)

q 4 q 4,[3V ] = v a [( p 0,b p 2,c + p1,b p1,c + p 0,c p 2,b )q 2,a + + ( p1,b p 2,c + p1,c p 2,b )q1,a + p 2,b p 2,c q 0,a ] + + vb [( p 0,a p 2,c + p1,a p1,c + p 0,c p 2,a )q 2,b + + ( p1,a p 2,c + p1,c p 2,a )q1,b + p 2,a p 2,c q 0,b ] + + vc [( p 0,a p 2,b + p1,a p1,b + p 0,b p 2,a )q 2,c + + ( p1,a p 2,b + p1,b p 2,a )q1,c + p 2,a p 2,b q0,c ] (1.12.2.5)

q5 q5,[ 3V ] = v a [( p1,b p 2,c + p1,c p 2,b )q 2,a + p 2,b p 2,c q1,a ] + + vb [( p1,a p 2,c + p1,c p 2, a )q 2,b + p 2,a p 2,c q1,b ] + + vc [( p1,a p 2,b + p 2,a p1,b )q 2,c + p 2,a p 2,b q1,c ]
q 6 q 6,[ 3V ] = v a p 2,b p 2,c q 2, a + vb p 2,a p 2,c q 2,b + v c p 2,a p 2,b q 2,c (1.12.2.7)

(1.12.2.6)

It is remarkable to quote that, as result of [3V] morpho-rheological interactions, there are typical dependences of composite rheological operators versus those of components: the composite P operators are given solely in terms of similar component operators (and P and Q component operators (and accordingly, mixed consequently, also for the rheological parameters), while the composite Q operators are expressed in terms of both rheological parameters are involved, too).

Conclusions

The uniform deformation approach for ternary phase in phase composite systems with linear viscoelastic components including polymeric materials, either partially or totally, achieved from the standpoint of rheological behaviour laws - selection rules - mixing rules, yields essential facts on the peculiarities of potential rheological response. Taking into account the features of Voigt-like morpho-rheological interactions, the characteristic rheological operators of composite result in terms of those of components, providing the basis for the identification of selection rules as well as for the establishment of corresponding primary and specific mixing rules. By using for components well defined rheological models, the morpho-rheological consequences can be evidenced both for direct detection of component combinations for which results the same composite rheological state, as well as for unveiling quantitative and qualitative effects.

References

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Table 1.1 [3 V] morpho-rheological interaction parameters

[3 V]

ma 1 1 1 0

na 0 0 0 1

mb 1 1 0 1

nb 0 0 1 0

mc 1 0 1 1

nc 0 1 0 0

m1 n1 n2 n3

Table 1.2 [3V] morpho-rheological effects

Crt. No.

a/b/c Composite m a

Components b n 0 0 0 0 0 0 0 0 0 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 m 0 0 0 0 0 0 1 1 1 0 0 0 0 0 0 1 1 1 0 0 0 0 0 0 1 1 1 n 0 0 0 1 1 1 1 1 1 0 0 0 1 1 1 1 1 1 0 0 0 1 1 1 1 1 1 m 0 0 1 0 0 1 0 0 1 0 0 1 0 0 1 0 0 1 0 0 1 0 0 1 0 0 1 c n 0 1 1 0 1 1 0 1 1 0 1 1 0 1 1 0 1 1 0 1 1 0 1 1 0 1 1 m1 0 0 1 0 0 1 1 1 2 0 0 1 0 0 1 1 1 2 1 1 2 1 1 2 2 2 3 n1 0 1 1 0 1 1 1 2 2 0 1 1 0 1 1 1 2 2 1 2 2 1 2 2 2 3 3 n2 0 0 1 1 1 2 1 1 2 0 0 1 1 1 2 1 1 2 1 1 2 2 2 3 2 2 3 n3 0 0 1 0 0 1 1 1 2 1 1 2 1 1 2 2 2 3 1 1 2 1 1 2 2 2 3 [3 V] m 0 0 1 0 0 1 1 1 2 0 0 1 0 0 1 1 1 2 1 1 2 1 1 2 2 2 3 n 0 1 1 1 1 2 1 2 2 1 1 2 1 1 2 2 2 3 1 2 2 2 2 3 2 3 3

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27

{1} / {1} / {1} {1} / {1} / {2} {1} / {1} / {3} {1} / {2} / {1} {1} / {2} / {2} {1} / {2} / {3} {1} / {3} / {1} {1} / {3} / {2} {1} / {3} / {3} {2} / {1} / {1} {2} / {1} / {2} {2} / {1} / {3} {2} / {2} / {1} {2} / {2} / {2} {2} / {2} / {3} {2} / {3} / {1} {2} / {3} / {2} {2} / {3} / {3} {3} / {1} / {1} {3} / {1} / {2} {3} / {1} / {3} {3} / {2} / {1} {3} / {2} / {2} {3} / {2} / {3} {3} / {3} / {1} {3} / {3} / {2} {3} / {3} / {3}

0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 1 1 1 1 1 1 1 1 1