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Separate Experimental Investigation of the Influence

of Liquids’ Mass Densities and Viscosities on the


Frequency Response of Resonant Sensors Using
Designated Liquid Series
Martin Heinisch, Thomas Voglhuber-Brunnmaier, Isabelle Dufour
Erwin K. Reichel, Center for Integrated Sensor Systems Université de Bordeaux
and Bernhard Jakoby Danube University Krems, Austria IMS
Inst. f. Microelectronics and Microsensors Bordeaux, France
Johannes Kepler University
4040 Linz, Austria
Email: martin.heinisch@jku.at

Abstract— For resonant viscosity and mass density sensors, these liquid series (e.g., consisting of binary or ternary liquid
oscillating in a test liquid with viscosity η, mass density ρ and mixtures), appropriate models are necessary to determine the
temperature T , usually, resonance frequency fr and quality factor mixing ratio to obtain the desired η or ρ at a certain T .
Q are evaluated and subsequently related to η and ρ. As both,
fr and Q depend on η, ρ as well as on T , it is often difficult In the following, liquid series with constant mass densities
to separate the origin of these fr and Q changes. Separate but varying viscosities are called ‘viscosity series’, whereas the
experimental investigations of the effects of η and ρ on fr and Q term ‘mass density series’ is used for liquid series with con-
are thus desired. For this purpose, new models for binary and stant viscosities but varying mass densities. For the viscosity
ternary liquid mixtures have been elaborated for calculating the
series, used to get the measurement data depicted in Fig. 1,
necessary mixing ratio to obtain a desired η and ρ at a certain
T . This allows mixing liquid series with constant ρ but varying solutions of Acetone and Isopropanol have been mixed. The
η (and vice versa). These liquid series and their modeling are values for η and ρ for the associated solutions, characterized
discussed in detail and measurement results obtained with such with an Anton Paar SVM 3000 at 25 ◦ C are depicted and listed
resonant liquid series are shown. in Fig. 2(a). There, it is shown that the obtained soultions
yield viscosities from approximately 0.2 mPa·s to 2 mPa·s
I. I NTRODUCTION
for mass densities of roughly 0.78 g/cm3 . However a small
In general, resonant principles for viscosity and mass but clear trend in the mass densities can be observed. An
density measurements have in common, that the devices’ interesting result is the fact that the mass densities of the mixed
frequency responses, including a characteristic resonant mode, solutions can get lower than both unmixed mass densities.
are recorded upon immersion in a sample liquid. From the However, as these relatively small deviations in mass density
recorded frequency response, the liquid’s mass density ρ can be observed in the fr and Q measurements, see Fig. 2(b)
and viscosity η are deduced [1]. In many cases, resonance for measurements obtained with the U-shaped wire sensor
frequency fr and quality factor Q are first evaluated, which [5] and the spiral spring sensor [6] more precise viscosity
are then related to the liquid’s viscosity and mass density by and mass density series might become necessary to presume
an appropriate model, see Fig.1. There, the equations for a constant viscosities or mass densities, respectivley. This task
generalized model, which was introduced in [2] and according might be difficult to solve using binary mixtures but might be
parameters for a steel tuning fork [3] are given. Both equations achieved using ternary liquid mixtures. With an appropriate
nicely show that both quantities, fr and Q depend on η as model for ternary liquid mixtures, the mixing ratio necessary
well as on ρ. In fact, e.g. in [3], [4] it was shown that the to obtain viscosity and mass density series can be calculated.
sensitivity of fr on η and ρ is similar and is even higher for Such models (also considering the influence of the temperature
ρ in case of the sensitivity of Q. Resonant devices usually dependence of η and ρ) can hardly be found in literature.
show a significant cross-sensitivity of both, fr and Q to T .
These three dependencies of fr and Q make an (intuitive) II. V ISCOSITY AND MASS DENSITY OF TERNARY
comparison and characterization of resonant mass density and MIXTURES
viscosity sensors difficult. Liquid series with constant mass
densities but varying viscosities and vice versa can be used to Approaches for modeling the viscosity of ternary liquid
separately show the effect of η and ρ on fr and Q. For mixing mixtures are given in [7], [8]. However, in these models

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424
6
420

4
416

|A.U.|
2
412

0.6 2 0.6 2

0.8 0.8 1
1
1.0 1.0
0 0

Fig. 1. Top: A mechanical resonator, presented by a lumped elements oscillator here, immersed into a liquid: m0 : lumped mass, c0 : damping coefficient,
k0 : spring constant, u(t): displacement, Fex (t): excitation force, FF (t): fluid force, fr : resonance frequency, Q: quality factor, η: fluid’s dynamic viscosity,
ρ: fluid’s mass density. 3D plots: Modeled and measured values for resonance frequency and quality factor. The shaded surfaces for fr and Q were obtained
by evaluating the given equations for fr and Q for identified parameters for a circular steel tuning fork sensor. The intersection lines on the shaded surfaces
with the planes entitled ‘density series’ and ‘viscosity series’ indicate the values which would be obtained for fr and Q for constant ρ and η, respectively.
In this particular case for the related experiments, the viscosity series consist of aceteone-isopropanol solutions with mass densities of roughly 0.78 mg/cm3
and a viscosity range of 0.2 mPa·s to 2 mPa·s. The density series consist of solutions with a viscosity of 1 mPa·s and mass densities of 0.78 mg/cm3 to
1 mg/cm3 . The measured points are indicated by the black dots on the shaded surfaces.

the liquid mixture’s viscosity temperature dependence is not basic approaches – a model with temperature dependent con-
sufficiently considered. trol points and a model with mixture dependent temperature
coefficients have been developed. In both cases correcting or
For modeling a ternary liquid’s mixture viscosity and mass interpolating functions are necessary to complete the ideal
density and the influence of temperature on the latter, two

Acetone-Isopropanol solutions U-shaped wire Spring viscometer


2
624
930
1.5 623
929 622
1
621
928
0.5 620
927 619
180
0.784 160 100
140
0.782 80
120
0.78 100 60
80
0.778 40
0 20 40 60 80 100 0.5 1 1.5 2 0.5 1 1.5 2

(a) Viscosity series (b) Measured fr and Q

Fig. 2. a) Acetone-Isopropanol solution at 25 ◦ C. mA : mass acetone, mI : mass isopropanol. Note the scale of the density axis: the variation of density is
small (≈ 7 · 10−3 ), however, a clear trend can be observed. b) measurement results: the second measurement from the left for fr is surprisingly high. This
is due to the lower mass density of the mixture.
equations [9], [10], 1) Viscosity model: With the knowledge of the temperature
coefficients of the unmixed liquids’ viscosities
η(x1 , x2 , x3 , T ) = η1x1 (T ) η2x2 (T ) η3x3 (T ) (1) ∗
+b21 T ∗2 ∗
+b22 T ∗2
η1 (T ) = η01 eb11 T , η2 (T ) = η02 eb12 T ,
and (10)
and
ρ(ϕ1 , ϕ2 , ϕ3 , T ) = ϕ1 ρ1 (T ) + ϕ2 ρ2 (T ) + ϕ3 ρ3 (T ) (2) ∗
+b23 T ∗2
η3 (T ) = η03 eb13 T (11)
for achieving sufficient modeling accuracy. xi and ϕi are the in a first step, the deviations
molar and the volume fraction of component i, respectively. As
three-components mixture fractions satisfy the equation ξ1 = ∆η(x1d , x2d , x3d , Ti ) = η(x1d , x2d , x3d , Ti ) (12)
1 − ξ2 − ξ3 , (where ξi is either xi or ϕi ) Bézier triangles are −ηc (x1d , x2d , x3d , Ti )
a good candidate for such correcting functions.
from the measured values η(x1d , x2d , x3d , Ti ) at discrete,
A. Bézier triangle measured mixture fractions x1d , x2d , and x3d at temperatures
Ti , where
A Bézier triangle Sn of order n can be expressed as
ηc (Ti ) = η1 (Ti )x1d η2 (Ti )x2d η3 (Ti )x3d (13)
Sn = (α x1 + β x2 + γ x3 )n (3)
are calculated. These deviations are fit using Bézier triangles
where x1 = 1 − x2 − x3 . Products of α, β and γ (and their Sηn for every temperature Ti yielding control points Pj (Ti ).
powers) form the control points which will be replaced by The temperature dependence of these coefficients is then fit
Pj in the following. The control points at x1 = 1, x2 = 1 using a second order polynomial, i.e.
or x3 = 1 are set to zero for both approaches (temperature
dependent control points and mixture dependent temperature Pj (T ) = Pj0 + Pj1 T + Pj2 T 2 (14)
coefficients), i.e., αn = β n = γ n = 0 as there, no mixing yielding 3 ( (n+1)2(n+2) − 3) coefficients for the correction
takes place and the temperature dependent viscosities and mass function and thus, 9 + 3 ( (n+1)2(n+2) − 3) coefficients in total
densities are calculated using for the temperature dependent mixture coefficients model.
2
ηi = η0,i eb1,i (T −Tm )+b2,i (T −Tm ) (4) With the knowledge of these coefficients the viscosity of a
ternary liquid mixture η(x1 , x2 , x3 , T ) is calculated as follows:
and
First, using Eqs. 1 and 11 the first term in Eq. 8 is calculated.
ρi = ρ0,i + r1,i (T − Tm ) + r2,i (T − Tm )2 (5) Second, the temperature dependent control points Pj (T ) using
Eq. 14 are determined. Third, the second term in Eq.8, i.e.
where the subscript i stands for liquid 1,2 or 3 and Tm is a
∆η(x1 , x2 , x3 , T ) using these control points is evaluated. An
temperature value which can be used to keep the modeling
illustration of the effect of ∆η(x1 , x2 , x3 , T ) in Eq.8 for the
coefficients low. The equations for square (n = 2) and cubic
case of an Ethanol + 2-Butanone + 2,2,4-Trimethylpentane
(n = 3) Bézier rectangles, respectively read:
mixture [11] is shown in Fig. 3.
S2 = 2 P121 x1 x2 + 2 P131 x1 x3 + 2 P231 x2 x3 (6) 2) Mass density model: Analogous to the viscosity model,
S3 = 3 P121 x21 x2 + 3 P122 x1 x22 + 3 P131 x21 x3 the mass density model for ternary liquid mixtures using
temperature dependent mixtures coefficients, the deviations
+3 P132 x1 x23 + 3 P231 x22 x3 + 3 P232 x2 x23
+6 P1231 x1 x2 x3 ∆ρ(Ti ) = ρ(Ti ) − ρc (Ti ) (15)
Sn = ... (7) with

B. Models with temperature dependent control points ρc (Ti ) = ρ1 (Ti ) x1d + ρ2 (Ti ) x2d + ρ3 (Ti ) x3d (16)
In this modeling approach, the ternary liquid mixtures’ vis- are evaluated which subsequently are used to fit a fit Bézier tri-
cosity and mass density are modeled, using the ideal equations angle at all temperatures Ti yielding again coefficients Pi (Ti )
for ternary mixtures Eqs. 1 and 2 and completing then by which in turn are used to fit the second order polynomial of
additive functions ∆η and ∆ρ, i.e., the form of Eq. 14.
For both, the binary as well as the ternary liquid mixture
models, the number of measurements has to be at least as high
η(x1 , x2 , x3 , T ) = η1x1 (T ) η2x2 (T ) η3x3 (T ) + ∆η(x1 , x2 , x3 , T ) as the number of modeling coefficients. A fifth order Bézier
(8) triangle for the case of the temperature dependent control
and points model for ternary mixtures has 63 coefficients, and thus
requires at least 21 mixtures measured at three temperatures.
ρ(ϕ1 , ϕ2 , ϕ3 , T ) = ϕ1 ρ1 (T ) + ϕ2 ρ2 (T ) + ϕ3 ρ3 (T )
However, more measurements are generally of interest, to
+∆ρ(ϕ1 , ϕ2 , ϕ3 , T ). (9) proof if the modeled behavior is valid. In the literature research
Comparison of measured data ( ) and the results from ideal equations at 25 °C, i.e.
where

1.1 1.1
1.1 1.1

0.9
0.9
0.9 0.9
0.7
0.7
0.7 0.7
0.5
0.5
0.5 0.5
0.3
1
0 0.75
0.25 0.5 1 0.3 0
0.3 0.3 0.75 1
0
0.5
0.75 0.25 1 0 0.25 0.5 0.75 0.5 0.5 0.25
0.25 0.5 0.75 0.5 0.75 0.5 0.75 0.25 0.25 0 1 0.75
1 1 0 0 0.25 1 0

Comparison between modeld and measured data

1.1
1.1 1.1
1.1
0.9
0.9 0.9
0.9
0.7
0.7 0.7
0.7
0.5

0.5 0.5
0.5 0.3
1
0.75
0 0.5 1
0.25 0.3 0.75 0.3 0
0.3 0.25 0.5 1
0
0.5
0.75 0.5 0.75 1 0 0.25
0.5 0.75 0.25 0.75 0.5 0.5 0.25
0.25 0.5 0.75 0 0 0.25 1 0 0.25 0 1 0.75
1 1

Fig. 3. llustration of the effect of ∆η(x1 , x2 , x3 , T ) in Eq.8 for the case of an Ethanol + 2-Butanone + 2,2,4-Trimethylpentane mixture [11]

performed for this study, mainly measurement results at three R EFERENCES


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ACKNOWLEDGMENT acetone – ethanol – isopropanol in a temperature range from 5◦ C to
45◦ C, Work in Progress.
We are indebted to the Austrian COMET program (Aus- [13] M. Heinisch, Viscosity and mass densitity of the ternary liquid mixture
trian Centre of Competence in Mechatronics, ACCM) for the ethanol – glycerol – water in a temperature range from 5◦ C to 45◦ C,
Work in Progress.
financial support.

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