THERMODYNAMICS AND CHEMICAL ENGINEERING DATA

Chinese Journal of Chemical Engineering, 19(3) 478483 (2011)

Density and Viscosity of Ternary Systems (Poloxamer 188 + Ethanol/
Acetone + Water) at Temperatures from 288.15 K to 308.15 K
*
LIU Qian (,), ZHANG Songhong ()), SHEN Shaochuan (,]), YUN Junxian
(=) and YAO Kejian (j)
**
State Key Laboratory Breeding Base of Green Chemistry Synthesis Technology, College of Chemical Engineering
and Materials Science, Zhejiang University of Technology, Hangzhou 310014, China
Abstract The densities and viscosities of ternary systems (Poloxamer 188 + ethanol/acetone + water) were meas-
ured at 288.15, 293.15, 298.15, 303.15, 308.15 K and atmospheric pressure for different mass fractions of Polox-
amer 188 (0 to 0.02) in aqueous solution and different solvent volume fractions of ethanol/acetone (0 to 0.3) in
Poloxamer 188 aqueous solution. The densities were measured by a pycnometer, while the viscosities were meas-
ured using two Ubbelohde capillary viscometers. The correlations of density and viscosity of these ternary systems
are obtained by fitting the experimental data at different temperatures, mass fractions and volume fractions.
Keywords density, viscosity, ternary system, Poloxamer 188, ethanol, acetone
1 INTRODUCTION
Poloxamer 188 is a nonionic block copolymer
chemical surfactant. It is well known to have cytoprotec-
tive, rheologic, anti-inflammatory and anti-thrombotic
activities combined with minimal toxicity [1]. It also
has various therapeutic uses in drug delivery systems [2].
As a steric stabilizer, Poloxamer188 is widely em-
ployed in the process of preparing solid lipid nanopar-
ticles based on antisolvent precipitation, such as sol-
vent injection [3, 4], particle formation by the liquid
flow-focusing [5, 6] or together with gas displacing [7].
These methods are based on lipid precipitation from a
lipid dissolved organic solvent such as ethanol and
acetone, lipid particle formation occurs when lipid
solution contacts with a Poloxamer 188 aqueous solu-
tion. Furthermore, these ternary systems (Poloxamer
188 + ethanol/acetone + water) also exist in prepara-
tion of CS-coated oily nanodroplets [8], as well as in
the preparation of other nanoparticles by modified
spontaneous emulsification solvent diffusion method
[9, 10]. Obviously, in order to prepare these nanoparti-
cles with small size and narrow diameter distribution,
it is necessary to learn about the process of nanoparti-
cles formation as well as mass transfer between
Poloxamer 188 aqueous solution and organic solvent
of lipid. Therefore it is needed to get the basic proper-
ties of these ternary systems.
The density and viscosity are two essential prop-
erties that affect mixing and phase separation. How-
ever, these data of the ternary systems are rare in lit-
erature. In this work, we carry out systematic meas-
urements of densities and viscosities of the ternary
system (Poloxamer 188 + ethanol/acetone + water) at
various temperatures. The mass fraction of Poloxamer
188 in aqueous surfactant solution is from 0 to 0.02,
while the volume fraction of ethanol/acetone solvent
in Poloxamer 188 aqueous solution is from 0 to 0.3.
Experimental data are correlated with polynomial
equations.
2 EXPERIMENTAL
2.1 Materials
Poloxamer 188 was supplied by BASF (China)
Co. Ltd. (Shanghai, China) with a purity higher than
99.0% (by mass). The ethanol and acetone were sup-
plied with a mass fraction purity better than 0.997.
Ultrapure water was prepared by Milli-Q Synthesis
(Millipore Co. Ltd, USA), with an electrical resistivity
of 18.2 Mcm at 298.15 K.
2.2 Apparatus and procedure
The aqueous solution of Poloxamer188 with dif-
ferent mass fraction was prepared using an electronic
balance with uncertainty of 0.0001 g and measuring
flasks.
The densities were determined by a pycnometer
having a bulb volume of about 25 ml. A cleaned and
dried pycnometer was weighed on an electronic bal-
ance, filled with water, and then immersed in a ther-
mostatic bath with 0.1 K. After the water temperature
reached the required temperature, the pycnometer was
removed from the thermostatic bath, cleaned, dried,
and weighed. Through this process, the mass values of
water under 288.15, 293.15, 298.15, 303.15, and
308.15 K were measured. By the same method, the
mass values of the ternary systems (Poloxamer 188 +
ethanol/acetone + water) were also measured. The
density of the ternary systems can be calculated by
w w
m
m

= (1)

Received 2010-11-14, accepted 2011-02-25.
* Supported by the National Natural Science Foundation of China (20606031).
** To whom correspondence should be addressed. E-mail: yaokj@zjut.edu.cn
Chin. J. Chem. Eng., Vol. 19, No. 3, June 2011 479
where is the density of the ternary system,
w
the
density of water, m the mass of the ternary system and
m
w
the mass of water. The density of water at each
temperature was from the literature [11]. Three runs
were made for each sample, uncertainties in density
measurements were estimated to be within 1 kgm
3

at the 95% confidence interval.
The viscosities were measured using calibrated
Ubbelohde capillary viscometer of 0.57 mm or 0.64
mm diameter. (As the measured range was wide, two
viscometer of different diameter were needed). The
viscometer was calibrated with ultrapure water at
temperatures of 288.15, 293.15, 298.15, 303.15, and
308.15 K. The viscosity of water at each temperature
was from the literature [11]. The instrument constant
of viscometer was measured by the linear relationship
between the efflux time and the viscosity of water at
different temperatures. A cleaned and dried viscometer
filled with the ternary system prepared was immersed
vertically in a thermostatic bath for twenty minutes.
After the temperature of the ternary system achieved
the required temperature, the efflux time of the ternary
system was recorded with a digital stopwatch with an
uncertainty of 0.01 s. All experiments were made at
least twice, the deviation was less than 0.5 s, and the
obtained data were averaged. The viscosity of the ter-
nary system, , was calculated by
Ct q = (2)
where t is the efflux time of the ternary system, and C
is the instrument constant. The measurements of vis-
cosity were the same as described in Ref. [12, 13].
3 RESULTS AND DISCUSSION
In Tables 1 and 2, physical properties of ethanol
and acetone are measured and compared to several
values in literature to assure that there are no signifi-
cant effects due to impurities.
Table 1 Comparison of experimental densities () and
viscosities () of ethanol with literature values
/kgm
3
/mPas
T/K
Exp. Lit. Exp. Lit.
288.15 794 793.69 [14] 1.311 1.3182 [14]
293.15 790 789.7 [15] 1.187 1.2050 [14]
298.15 785 785.25 [16] 1.077 1.0710 [14]
303.15 782 781.3 [17] 0.985 0.9817 [18]
308.15 777 776.50 [16] 0.898 0.895 [17]
Table 2 Comparison of experimental densities () and
viscosities () of acetone with literature values
/kgm
3
/mPas
T/K
Exp. Lit. Exp. Lit.
288.15 794 796.87 [19] 0.335 0.335 [20]
293.15 789 790.02 [21] 0.319 0.321 [21]
298.15 785 785.44 [21] 0.305 0.305 [20]
303.15 779 779.66 [22] 0.289 0.292 [22]
308.15 773 773.91 [19] 0.277 0.279 [20]
Table 3 Experimental densities for the ternary system (Poloxamer 188 + ethanol + water)
/kgm
3
/kgm
3

288.15 K 293.15 K 298.15 K 303.15 K 308.15 K

288.15 K 293.15 K 298.15 K 303.15 K 308.15 K
0.005 0 1002 1000 999 998 996 0.01 0.10 989 987 986 985 983
0.01 0 1002 1001 999 998 997 0.01 0.15 983 981 980 978 976
0.015 0 1003 1002 1000 999 997 0.01 0.20 978 977 974 972 970
0.02 0 1004 1002 1000 999 997 0.01 0.25 973 971 968 966 963
0 0.05 993 992 991 989 988 0.01 0.30 966 963 961 958 955
0 0.10 987 985 984 983 981 0.015 0.05 993 992 991 989 988
0 0.15 981 979 978 976 974 0.015 0.10 987 986 984 982 981
0 0.20 975 974 972 970 969 0.015 0.15 981 979 978 976 974
0 0.25 971 969 966 965 962 0.015 0.20 976 974 972 970 968
0 0.30 965 963 960 957 954 0.015 0.25 970 967 966 963 960
0.005 0.05 994 993 992 991 989 0.015 0.30 964 962 959 956 954
0.005 0.10 988 987 986 984 983 0.02 0.05 995 994 992 991 989
0.005 0.15 983 981 980 978 976 0.02 0.10 988 986 985 983 982
0.005 0.20 978 976 974 972 970 0.02 0.15 982 981 979 977 976
0.005 0.25 972 970 968 965 963 0.02 0.20 976 975 973 971 969
0.005 0.30 969 966 963 961 958 0.02 0.25 971 969 967 964 962
0.01 0.05 994 993 992 991 989 0.02 0.30 964 962 959 957 955
Chin. J. Chem. Eng., Vol. 19, No. 3, June 2011 480
A series of experiments were made to determine
densities and viscosities of the ternary systems (Polox-
amer 188 + ethanol/acetone + water) at temperatures
of 288.15, 293.15, 298.15, 303.15, and 308.15 K. The
experimental densities and viscosities of the ternary
system (Poloxamer 188 + ethanol + water) are listed
in Tables 3 and 4, respectively, and the experimental
densities and viscosities of the ternary system
(Poloxamer 188 + acetone + water) are listed in Tables 5
and 6, respectively, where T, , are the absolute
Table 4 Experimental viscosities for the ternary system (Poloxamer 188 + ethanol + water)
/kgm
3
/kgm
3

288.15 K 293.15 K 298.15 K 303.15 K 308.15 K

288.15 K 293.15 K 298.15 K 303.15 K 308.15 K
0.005 0 1.246 1.102 0.970 0.870 0.783 0.01 0.10 1.994 1.701 1.415 1.243 1.098
0.01 0 1.382 1.214 1.077 0.949 0.854 0.01 0.15 2.366 1.989 1.646 1.425 1.242
0.015 0 1.539 1.322 1.171 1.035 0.926 0.01 0.20 2.717 2.254 1.898 1.623 1.373
0.02 0 1.670 1.448 1.270 1.122 1.003 0.01 0.25 3.106 2.560 2.127 1.807 1.559
0 0.05 1.359 1.172 1.029 0.912 0.818 0.01 0.30 3.487 2.820 2.338 1.964 1.686
0 0.10 1.615 1.379 1.197 1.051 0.930 0.015 0.05 1.793 1.536 1.335 1.177 1.043
0 0.15 1.928 1.623 1.390 1.204 1.058 0.015 0.10 2.147 1.803 1.547 1.349 1.185
0 0.20 2.322 1.928 1.588 1.364 1.186 0.015 0.15 2.601 2.170 1.832 1.588 1.342
0 0.25 2.671 2.193 1.835 1.522 1.313 0.015 0.20 2.974 2.439 2.051 1.753 1.477
0 0.30 3.010 2.434 2.019 1.708 1.427 0.015 0.25 3.367 2.727 2.284 1.936 1.660
0.005 0.05 1.483 1.306 1.135 0.999 0.894 0.015 0.30 3.702 2.968 2.466 2.062 1.771
0.005 0.10 1.761 1.511 1.308 1.140 1.010 0.02 0.05 1.966 1.729 1.458 1.277 1.133
0.005 0.15 2.089 1.747 1.513 1.305 1.143 0.02 0.10 2.381 2.002 1.725 1.493 1.277
0.005 0.20 2.452 2.083 1.764 1.479 1.286 0.02 0.15 2.776 2.306 1.968 1.699 1.473
0.005 0.25 2.862 2.356 1.973 1.679 1.404 0.02 0.20 3.162 2.611 2.201 1.873 1.618
0.005 0.30 3.202 2.613 2.174 1.841 1.595 0.02 0.25 3.551 2.900 2.431 2.040 1.757
0.01 0.05 1.627 1.411 1.228 1.087 0.972 0.02 0.30 3.894 3.176 2.633 2.209 1.891
Table 5 Experimental densities for the ternary system (Poloxamer 188 + acetone + water)
/kgm
3
/kgm
3

288.15 K 293.15 K 298.15 K 303.15 K 308.15 K

288.15 K 293.15 K 298.15 K 303.15 K 308.15 K
0.005 0 1002 1000 999 998 996 0.01 0.10 989 988 986 985 983
0.01 0 1002 1001 999 998 997 0.01 0.15 985 984 982 980 977
0.015 0 1003 1002 1000 999 997 0.01 0.20 980 978 976 973 971
0.02 0 1004 1002 1000 999 997 0.01 0.25 975 972 970 967 964
0 0.05 995 994 992 991 989 0.01 0.30 969 966 963 960 957
0 0.10 990 988 986 985 984 0.015 0.05 995 994 992 991 990
0 0.15 985 983 981 979 977 0.015 0.10 990 989 988 986 984
0 0.20 980 977 975 974 971 0.015 0.15 987 985 983 981 979
0 0.25 975 972 969 967 965 0.015 0.20 981 978 976 974 971
0 0.30 969 966 963 960 958 0.015 0.25 974 972 969 967 964
0.005 0.05 994 993 992 990 988 0.015 0.30 969 967 963 961 959
0.005 0.10 988 987 986 984 983 0.02 0.05 997 996 994 993 991
0.005 0.15 983 982 980 978 976 0.02 0.10 992 991 989 987 985
0.005 0.20 978 976 975 973 970 0.02 0.15 987 985 983 981 979
0.005 0.25 973 971 968 966 963 0.02 0.20 982 980 978 975 973
0.005 0.30 967 965 962 960 957 0.02 0.25 977 974 971 968 966
0.01 0.05 994 993 992 991 989 0.02 0.30 971 968 964 962 958
Chin. J. Chem. Eng., Vol. 19, No. 3, June 2011 481
temperature, mass fraction of Poloxamer 188 in aque-
ous solution and volume fraction of ethanol/acetone
solvent in Poloxamer 188 aqueous solution, respec-
tively. Mass fraction is from 0 to 0.2, and volume
fraction is from 0 to 0.3. When value remains un-
changed, the density of the ternary systems decreases
as value increases, while the viscosity of the ternary
systems increases. Moreover, when value remains
unchanged, both density and viscosity of the ternary
systems increase as value increases.
Polynomial equations [23] are fitted to the ex-
perimental data. In the range of this experiment, den-
sity can be described as Eq. (3), which follows a linear
behavior with temperature, mass fraction and volume
fraction, while viscosity can be described as Eq. (4),
which follows a quadratic behavior with temperature,
mass fraction and volume fraction for the ternary systems,
0 1 2 3
T o o o u o e = + + + (3)
2 2
0 1 2 3 4 5
2
6 7 8 9
T T
T T
q | | | u | e | | u
| e | e | u | eu
= + + + + + +
+ + + (4)
where
0

3
,
0

9
are the parameters obtained by
regression analysis and given in Table 7.
In order to analyze the performance of the fitted
equations, the standard deviation, , the coefficient of
determination, R
2
, relative deviation and absolute av-
erage relative deviation (AAAD) are used, which are
defined by
( )
1/ 2
2
,exp ,cal
1
( 1)
n
i i
i
Y Y n o
=
(
=
(

(5)
2
2
,exp ,cal ,exp ,cal
1 1 1
2 2
2 2
,exp ,exp ,cal ,cal
1 1 1 1
n n n
i i i i
i i i
n n n n
i i i i
i i i i
R
n Y Y Y Y
n Y Y n Y Y
= = =
= = = =
=
( | || |

( | |
\ .\ . (
(
| | | |
(

| |
(
\ . \ .




(6)
relative deviation
,cal ,exp
,exp
i i
i
Y Y
Y

= (7)
,cal ,exp
1 ,exp
1
AAAD
n
i i
i i
Y Y
n Y
=

=

(8)
where Y can be either density or viscosity, Y
i,exp
and
Y
i,cal
are the experimental values and the calculated
values from the fitted equations, respectively, and n is
the number of data points.
Figures 1 to 4 show the relative deviation between
the experimental and calculated values of density and
viscosity. The density and viscosity measurements are
well correlated by Eqs. (3) and (4) in the range of this
experiment. In all cases, the coefficients of determination
Table 6 Experimental viscosities for the ternary system (Poloxamer 188 + acetone + water)
/kgm
3
/kgm
3

288.15 K 293.15 K 298.15 K 303.15 K 308.15 K

288.15 K 293.15 K 298.15 K 303.15 K 308.15 K
0.005 0 1.246 1.102 0.970 0.870 0.783 0.01 0.10 1.643 1.461 1.240 1.095 0.975
0.01 0 1.382 1.214 1.077 0.949 0.854 0.01 0.15 1.781 1.524 1.321 1.160 1.032
0.015 0 1.539 1.322 1.171 1.035 0.926 0.01 0.20 1.896 1.613 1.394 1.225 1.084
0.02 0 1.670 1.448 1.270 1.122 1.003 0.01 0.25 2.020 1.683 1.452 1.269 1.118
0 0.05 1.251 1.095 0.962 0.857 0.772 0.01 0.30 2.092 1.784 1.500 1.312 1.155
0 0.10 1.373 1.191 1.038 0.922 0.827 0.015 0.05 1.648 1.428 1.249 1.104 0.986
0 0.15 1.484 1.288 1.120 0.990 0.881 0.015 0.10 1.783 1.534 1.340 1.180 1.052
0 0.20 1.600 1.374 1.182 1.038 0.922 0.015 0.15 1.901 1.632 1.419 1.245 1.107
0 0.25 1.699 1.450 1.262 1.103 0.981 0.015 0.20 2.070 1.724 1.491 1.305 1.159
0 0.30 1.772 1.512 1.304 1.140 1.005 0.015 0.25 2.161 1.798 1.553 1.355 1.198
0.005 0.05 1.371 1.189 1.048 0.932 0.837 0.015 0.30 2.217 1.894 1.631 1.385 1.221
0.005 0.10 1.505 1.303 1.141 1.012 0.904 0.02 0.05 1.801 1.557 1.364 1.198 1.070
0.005 0.15 1.623 1.401 1.219 1.074 0.957 0.02 0.10 2.011 1.721 1.453 1.276 1.133
0.005 0.20 1.734 1.488 1.290 1.134 1.009 0.02 0.15 2.129 1.817 1.525 1.337 1.183
0.005 0.25 1.833 1.568 1.355 1.187 1.050 0.02 0.20 2.242 1.910 1.605 1.398 1.231
0.005 0.30 1.896 1.614 1.396 1.228 1.083 0.02 0.25 2.332 1.977 1.658 1.449 1.268
0.01 0.05 1.511 1.310 1.153 1.021 0.913 0.02 0.30 2.375 2.022 1.739 1.471 1.293

Chin. J. Chem. Eng., Vol. 19, No. 3, June 2011 482
Table 7 Coefficients of Eqs. (3) and (4), standard deviation, , and coefficient of determination R
2
for the ternary systems
/kgm
3
/mPas
Coefficient
Poloxamer188+
ethanol + water
Poloxamer188+
acetone + water
Coefficient
Poloxamer188+
ethanol + water
Poloxamer188+
acetone + water

0
1112.0 1122.0
0
141.575 88.837

1
0.379 0.422
1
0.935 0.572

2
123.09 116.23
2
71.349 22.017

3
109.33 192.00
3
362.383 278.987

4
0.0016 0.0009

5
0.355 2.364

6
42.922 139.676

7
1.129 0.874

8
0.2239 0.0661

9
29.616 2.111
1.27 0.97 3.595 1.627
R
2
0.990 0.992 0.997 0.998


Figure 1 Relative deviations of densities of the ternary
system (Poloxamer 188 + ethanol + water) between the
experimental and calculated values (The dashed lines
are two absolute average relative deviations)
Figure 2 Relative deviations of densities of the ternary
system (Poloxamer 188 + acetone + water) between the
experimental and calculated values (The dashed lines
are two absolute average relative deviations)

Figure 3 Relative deviations of viscosities of the ternary
system (Poloxamer 188 + ethanol + water) between the
experimental and calculated values (The dashed lines
are two absolute average relative deviations)
Figure 4 Relative deviations of viscosities of the ternary
system (Poloxamer 188 + acetone + water) between the
experimental and calculated values (The dashed lines
are two absolute average relative deviations)
Chin. J. Chem. Eng., Vol. 19, No. 3, June 2011 483
are more than 0.99. The AAAD values of density of
the ternary system (Poloxamer 188 + ethanol + water)
and the ternary system (Poloxamer 188 + acetone +
water) are 0.09% and 0.082%, respectively. The AAAD
values of viscosity of the ternary system (Poloxamer
188 + ethanol + water) and the ternary system (Polox-
amer 188 + acetone + water) are 1.625% and 0.857%,
respectively.
4 CONCLUSIONS
In this paper, the density and viscosity of the ter-
nary systems (Poloxamer 188 + ethanol/acetone + water)
were measured. The experimental results show that
the density decreases while the viscosity increases
with the increase of the volume fraction of etha-
nol/acetone. Both the density and viscosity increase as
mass fraction increases. In the range of this experi-
ment, density follows a linear behavior, while viscos-
ity follows a quadratic behavior with temperature,
mass fraction and volume fraction. The agreement
between the experimental and fitted values for the
density and viscosity is very good.
NOMENCLATURE
AAAD absolute average relative deviation
C instrument constant
m mass, g
m
w
mass of water, g
n number of data points
R
2
coefficient of determination
T temperature, K
t time, s
Y
i,cal
calculated value of density or viscosity
Y
i,exp
experimental value of density or viscosity
parameter
parameter
viscosity, mPas
density, kgm
3

w
density of water, kgm
3

standard deviation
volume fraction
mass fraction
Subscripts
cal calculated value
exp experimental value
w water
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