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Gives the way to determine Normal stres coefficient for a POLYMERIC material

Gives the way to determine Normal stres coefficient for a POLYMERIC material

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Rheologica Acta

Rheol Acta 27:567-574 (1988)

Original Contributions

Primary normal-stress coefficient prediction at high shear rates*)

Chr. Friedrich and L. HeymannAcademy of Sciences of the GDR, Institute of Mechanics, Karl-Marx-Stadt (GDR)

Abstract:

On the basis of a brief analysis of well known normal-stress calculationmethods, the necessity of improved models of prediction is elaborated. A modifiedform of the so-called mirror relation which meets these requirements is presented. Incombination with the Carreau viscosity equation, an analytical solution is given whichleads to a Carreau normal-stress coefficient equation and, thus, to a simple methodof calculation. The comparison between measured normal stresses and those deter-mined by experiments shows that the values calculated in accordance with the present-ed method agree well with the measured values, especially within the range of highshear rates. The parameters fi and K to be selected for this purpose are determinedin dependence on the slope of the viscosity function el at high shear rates for eachpolymer individually, using empirical relations so that the global selection of parame-ters, which is common practice with other methods, is obviated. In an appendix amethod for deriving the relations between material functions on the basis of operatorcalculation is given.

Key words:

Material function, normal-stress prediction, mirror relation, K ramers-Kronig relation, polymer solution

1. Introduction

The calculation of the first normal-stress difference N1and coefficient 01 (~) = N1 (~))/~2, where ~) is the shear rate,from the viscosity function r/(~)) is of importance in tworespects. Firstly, the functional relations between thesetwo functions is of interest in the evaluation of rheolo-gical constitutive equations. In [1, 2] it was pointed outthat an operator Y which, in the most general cases,relates the two functions mentioned with each other is aptto make a statement on constitutive hypotheses. Second-ly, this connection may be utilized to predict the normal-stress function, respectively, its coefficient whose mea-surement is complicated, from the easier measurableviscosity function.Knowledge of the first normal-stress difference is ofgreat importance for a large number of technologicalprocesses and for understanding natural processes. Thus,for instance, the ratio of the first normal-stress coefficientto the viscosity function determines the effective relax-ation time, while the ratio of the initial coefficients*) Extended version of a paper read at the 2nd Symposium onRheology of the GDR in Tabarz/Thuringia, December 7-ll,1987

308

01 (0)/t/(0) determines the longest relaxation time. Fur-thermore, phenomena such as extrudate swell and sec-ondary flow which are of importance to a number oftechnological operations are described by means of nor-mal stresses.Following the second consideration, a number of pa-pers dealing with different methods of normal-stress pre-diction [2-8] have been published. There, the questionarose repeatedly whether such an approach is funda-mentally feasible.In this connection, a brief explanation should be given.As the generally four different stress components for thedescription of a fluid in simple shear flow as well as thethree equivalent material functions are of one and thesame molecular origin, the three material functions can-not be independent of each other. This is evidenced byexperimental facts such as the correlation between thetime constant 2 v determined from the viscosity functionand the time constant 2E determined via the first normal-stress difference [8, 14]).v0.3<--<1.2EAn analysis of the papers dealing with normal-stress cal-culations shows on the one hand that, with Deborah

568 Rheologica Acta, Vol. 27, No. 6 (1988)numbers

De

= 2 9 (2 being the characteristic time con-stant of the fluid) smaller than unity, the accuracy ofcalculation may be very high. On the other hand, thecalculated 01-values considerably deviate from the mea-sured values at high Deborah numbers. The reason forthese deviations is that the calculated and measured func-tions decrease with different orders. Even in accessiblemeasurement ranges, underdetermination of the normalstresses up to a power of 10 is possible. Extrapolation ofthese values may yield even greater deviations. Besides,the selection of the front or shift parameters required forthe prediction seems to be very coarse (a distinction isdrawn only between those for polymer solutions andthose for melts); however, a material-specific selectionreally should be possible.It is, therefore, the purpose of this paper to derive anormal-stress calculation algorithm which predicts thecorrect order of magnitude of the function of the firstnormal-stress coefficient and, in addition, is simpleenough to be governed by elementary calculations. Fur-thermore, the selection of the parameters required for theprediction shall be material-specific and simple. The use-fulness of the procedure will be tested by the quality ofreproduction of the normal-stress coefficient in case ofhigh shear rates but also by its initial value.

2. Development of a prediction model

2.1 General relations

Consider a form of material function as it is obtainedfor most of the single-integral models (see, for instance,[1, 21)

tl(g = y ~b(s) F~(9s) ds

(1)

o

with t/(O)= t/o representing the Newtonian zero-shearviscosity and

0o

01 (9) = ~ (~ s) F2 (9 s) ds

(2)

0

with 0~ (0) = 010 designating the initial value of the firstnormal-stress coefficient.~b s) is a distribution function which, in most cases, canbe identified by the memory or relaxation function. Func-tions F 1 and F2 are influence functions which, in accor-dance with the constitutive hypotheses, describe a changein the distribution function in dependence on shear con-ditions.Corresponding to the theory of linear operators [11, 12],Eqs. (1) and (2) may also be written as

=dl (~), (1')

01 = ~2 (~), (2')

where sd1 and d 2 are linear, homogenous operators theinverses of which are postulated to exist. Inverting Eq. (1')and substituting in (2'), we obtain the desired generalrelation between the material functions01

=

d2 [dl

1 (t/)] (3)

or, in generalized notation [11],01 = 3- (q) with ~-- = d2" d,- 1 (3')where the product of operators is not commutative.

2.2 Special cases

On the basis of Eqs. (3), we obtain for concrete rheolo-gical constitutive equations (i. e., concrete F 1 and F2) oper-ators 3- by means of which the normal-stress coefficientcan be calculated. Wagner's model [4], for instance, yields

~'~1 = -- ~" ~, ~2 = 92. ~, (4)

where ~ is the differential operator ~ =

d/dp, p = m 9

and 5¢ the Laplace operator (see Appendix). Equation (4)yields for Yand, consequently,

1

dq

01 -- (5)

m dg"

On the basis of the Laplace operator, also the equationfor the mirror behavior, i.e.,

dO~ (g 9) 2 drld9 9 d9

and, in integrated form,il dr/01 (K ~) = - 2 . 9-- ~7 d9 (6)can be derived (see Appendix).In terms of this equation and the Carreau equationt/(9) = t/~o + (go - 700) [1 + (2 v • gz]-N (7)results of normal-stress calculation were presented in[7, 8]. The shift factor K was selected such that, within therange of 2 v 9 ~" 1, the measured normal stresses agreewith those calculated. Consequently, normal-stress calcu-lation with lower Deborah numbers is sufficiently accu-rate as already mentioned. With high Deborah numbers,however, the function values for the coefficient decreasefaster than the experimental values. This behavior is con-firmed by a consideration of the order of growth forEq. (6) [1]. Accordingly,~2m = 1 + ~ > c~2 (8)

Friedrich and Heymann, Primary normal-stress coefficient prediction at high shear rates 569applies, i.e., that, in case of mirror behavior, the order 0{2mof the decrease of the normal-stress coefficient calculatedthrough the order of the viscosity function 0{1 is greaterthen the actual value % observed in experiments.A way of overcoming this incorrect behavior was pre-sented in [2] where shear-rate dependent elastic defor-mation was introduced. The power term was normalizedby means of a time constant which was obtained from thedescription of viscous properties (lower index V). In com-bination with Eq. (6), this modification yields an im-proved prediction model~1 (K 9)= -2 ~(2;! ')p dr/dg' (9)dg'which, in case of high shear rates, will behave as

01 (9) = o {9-(1 +~,-e~} (10)

so that it admits the setting of 0{2 through ft.Having described a feature of Eq. (9) for any viscosityfunction by means of Eq. (10), let us continue by findingthe exact solution of Eq. (9) in combination with Eq. (7).By substituting Eq. (7) in Eq. (9) and with the substitutionof z = [1 + (2v9)2] i we obtain a tabulated integral [12]having the following solution

s

B~ (., .) is here the incomplete Beta function. By convert-ing the incomplete Beta function into the hypergeometricfunction 2F1 (.,. ;. ;z) [12], we obtain a useful solution2(~o- ~) 2v 0{1

01(K 9) = [1 + (~v 9)21 ~ +~-e~/2 0{~ + 1 -/3 (12)

'2/:1[ ~1+1-fl2 , 1-2 fl' %+3-/~.2 z].Now, Eq. (12) consists of two terms; a first term which wemay describe as Carreau equation for the coefficient ofthe first normal-stress difference, and a second one, whichis a correcting term• Actually, the latter term

0{ 1

y-0{1+1-/3.2Fl[~l+l-fl 1-/3. °q+3-fl. 1 ]2 ' 2 ' 2 ' 1 + (2v 9) ~withY=for 2 v 9 = 0,0{1 for 2v 9 ~ oe0{1 + 1 - fl practically for2v~) > 10,nearly shows no change over the entire ranges of shearrates. For a set of reasonable parameters (see Table 1)0{1 = 0.6 and fi = 0.3, this function increases monotonicalfrom its initial value of 0.641 to a final value of 0.923.On this basis, it is now possible to use equation01(K9) = 2(t/o- t/~) 2v 0{10{~+l-fl

• [1 + (2v"

9) 2] -(al +

I -/~3/2 (14)

for the calculation of normal stresses in case of high shearrates and the equation01o = 2(t/o- t/o~) 2v (15)for determining the initial coefficient 01o.Thus, we have an analytical expression which allows usto simply calculate the normal-stress coefficient or itsinitial value with the aid of other information from vis-cosity function (see section 3). The usefulness of Eqs. (14)and (15), as well as the selection of the parameters stillmissing, will be described in the following section.

3. Results and discussion

For the fluids given in Table 1, the parameters for theCarreau viscosity equation are given. The fluids are ex-clusively polymer solutions which allow the experimentaldetermination of the normal-stress coefficient up toDeborah numbers of 104 The stresses measured for thesefluids are given in figures 1-3. The parameters 0{1, fi andK contained in the table were determined so that thecalculated coefficients of the first normal-stress differenceagree with those measured at high Deborah numbers

(De

> 10).The parameters K and fi, however, must be knownpreviously in order to be able to predict the normalstresses. To enable the determination of these two con-stants in dependence on the given parameters of the givenviscosity function, a correlation between fl and 0{1 (seefigure 4) as well as K and 0{1 (see figure 5) was established.A linear dependency was selected for the first of the tworelations and the following equation was obtainedfl = 0.80 - 0.67.0{ 1 (16)For the second relation, a step-function type dependencywas selected as a first approximation. This relation isexpressed as1 for 0{1 < 0.65,K = 0.6 for 0{1 > 0.65.(17)

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