J. Chem.

Thermodynamics 41 (2009) 103108

Contents lists available at ScienceDirect

J. Chem. Thermodynamics
journal homepage: www.elsevier.com/locate/jct

Heat capacities and electrical conductivities of

1-ethyl-3-methylimidazolium-based ionic liquids
Ya-Hung Yu, Allan N. Soriano, Meng-Hui Li *
R&D Center for Membrane Technology, Department of Chemical Engineering, Chung Yuan Christian University, Chung Li, Taiwan

a r t i c l e

i n f o

Article history:
Received 1 July 2008
Received in revised form 16 July 2008
Accepted 16 July 2008
Available online 25 July 2008
Keywords:
Heat capacity
Electrical conductivity
[Emim]-Based ionic liquids

a b s t r a c t
We present the heat capacities and electrical conductivities of ve [Emim] 1-ethyl-3-methylimidazoliumbased ionic liquids: [Emim][BF4] (tetrauoroborate), [Emim][CF3SO3] (triuoromethanesulfonate),
[Emim][C2N3] (dicyanamide), [Emim][C2H5SO4] (ethylsulfate), and [Emim][MDEGSO4] (2-(2-methoxyethoxy) ethylsulfate). The heat capacities were measured using a differential scanning calorimeter (DSC) over
the temperature ranging from (303.2 to 358.2) K. The electrical conductivities were measured over the
temperature ranging from (293.2 to 353.2) K using a commercial conductivity meter. The estimated
uncertainties of heat capacity Cp and electrical conductivity r measurements were 0.015 kJ  kg1  K1
and 0.001 mS  cm1, respectively. The measured Cp and r are presented as a function of temperature.
The temperature dependency of the CP value was correlated using an empirical equation. A modied version of VTF-type (VogelTammanFulcher) equation was used to describe the temperature dependency of
r values. The correlations give satisfactory results. Also, the results of this study are in good agreement
with the available literature data. The heat capacities and electrical conductivities presented in this work
are in good agreement with the available literature data. The results of this study can be applied to numerous chemical processes, since Cp and r data are essential information for rational design.
2008 Elsevier Ltd. All rights reserved.

1. Introduction
Aqueous alkanolamine solutions are industrially effective for
CO2 absorption, but this method usually requires higher energy
consumption and operational cost, and also comes with solvent
pollution. Ionic liquids (ILs), coined as green solvents, have been
recognized as a versatile alternative to the aqueous alkanolamine
solutions. The IL is a common name given to many different chemical compounds, which are composed solely of ions and have melting points around or below room temperature. The maximum
melting temperature to be accepted for a compound to be included
in the IL category is about 373 K [1]. The ILs also show thermal stability at high temperatures and at high solubility for both polar and
non-polar organic as well as inorganic substances. Consequently,
ILs could be in a position to replace ammable and volatile organic
solvents in chemical processes [2]. Because of these appealing
properties, they could be very useful in the future. A signicant
number of research groups have already done systematic measurement and collection of the thermophysical and transport properties of ILs [215].

* Corresponding author. Tel.: +886 3 265 4109; fax: +886 3 265 4199.
E-mail address: mhli@cycu.edu.tw (M.-H. Li).
0021-9614/$ - see front matter 2008 Elsevier Ltd. All rights reserved.
doi:10.1016/j.jct.2008.07.013

The heat capacity Cp and electrical conductivity r are two of the

basic pure component properties for any substance, and their
knowledge is necessary for many engineering applications. For
most ILs, these values are still lacking. As in the case of Cp measurement, so far the thoroughly studied ILs are ammonium-, pyridinium-, pyrrolidinium-, bis[(triuoromethyl)sulfonyl]amide-, and
imidazolium-based ILs [2,3,5,7,10,12,13,1625]. In the Cp measurement of imidazolium-based ILs, most of the work clustered on hexyl- and butyl-3-methylimidazolium [10,1214,17,18]. For the r
measurement, only those of ammonium-, pyrrolidinium-, and
bis[(triuoromethyl)sulfonyl]amide-based have been widely studied, while not much has been studied on imidazolium-based ILs
[4,9,11,16,2630]. Therefore heat capacities and electrical conductivities for ve [Emim]-based ILs have been measured. The heat
capacities were measured over the temperature ranging from
(303.2 to 358.2) K at atmospheric pressure condition and the electrical conductivity over the temperature ranging from (293.2 to
353.2) K at atmospheric pressure condition.
The ILs that have been investigated are listed in table 1. The
structures of cations and anions are shown in gure 1. In order
to check the accuracy of the apparatus and the experimental procedures used, heat capacity and electrical conductivity of standard
materials have also been measured. Water was used to check the
heat capacity measurements and the standard KCl solution for
electrical conductivity measurements.

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Y.-H. Yu et al. / J. Chem. Thermodynamics 41 (2009) 103108

TABLE 1
Ionic liquids investigated in this work
Ionic liquid
1-Ethyl-3-methylimidazolium
1-Ethyl-3-methylimidazolium
1-Ethyl-3-methylimidazolium
1-Ethyl-3-methylimidazolium
1-Ethyl-3-methylimidazolium

tetrauoroborate
triuoromethanesulfonate
dicyanamide
ethylsulfate
2-(2-methoxyethoxy) ethylsulfate

Abbreviation

Purity, Mass fraction

[Emim][BF4]
[Emim][CF3SO3]
[Emim][C2N3]
[Emim][C2H5SO4]
[Emim][MDEGSO4]

P0.970
P0.980
P0.999
P0.992
P0.982

was in the range (15 to 20) mg. Five replicate runs were carried out
for each measurement. The apparatus and the experimental procedures are the same as those described by Chiu et al. [31].
2.3. Electrical conductivity measurements
The electrical conductivity was measured using a SC-170 conductivity meter manufactured by Suntex. The uncertainty of the
conductivity measurement is 0.001 mS  cm1 for readings below
50 mS  cm1. The temperature was monitored using a digital thermometer (model 3002, CROPICO), with an uncertainty of 0.01 K. A
xed volume of sample (3 cm3) was placed in a test tube and
placed in a water bath where the temperature was controlled.
The conductivity cell was rst adjusted to zero in the air followed
by the calibration of standard KCl solution before the sample was
put in. The calibration of this equipment is the same as those described by Widegren et al. [4]. The conductivity cell was then
washed with deionised water and ethanol to remove any adhering
IL, and dried. To preserve the conductivity cell it was placed in
water or in dry air before it was used for the next measurement.
The measurements were done in ve replicate runs.
3. Results and discussion
FIGURE 1. Cation and anions of the ionic liquids investigated.

3.1. Heat capacity

2. Experimental
2.1. Chemicals
All ILs used in this work were supplied by TCI Co. Table 1 shows
the purity of the ILs that were used without further purication
since the experiments required a small amount of sample. The liquid water used for the calibration of the calorimeter was deionised, with a resistivity of 18.3 MX  cm and with a total organic
carbon mass fraction of less than 1.5  1010 produced by Barnstead
Thermodyne, model Easy Pure 1052. The standard KCl solution
used for the calibration of the cell of the conductivity meter was
supplied by Merck, with c = 0.1 mol  L1 and electrolytic conductivity of 1.415 mS  cm1 at T = 298.15 K.
2.2. Heat capacity measurements

The equations used to represent the Cp are the same as those described by Chiu et al. [31]. The Cp of liquid water was measured and
compared to the data of Osborne et al. [32] to verify the accuracy of
the DSC. Osborne and co-workers [32] were able to measure the
heat capacity of water with an uncertainty of (0.0001 to
0.0002) kJ  kg1  K1 at close intervals of temperature (1 K) by
using a large adiabatic calorimeter. Table 2 shows the comparison
of Cp results obtained by Osborne et al. [32] and those obtained in
this study. The average values given in the last column in table 2
have an average absolute deviation (AAD) of 0.11 from the available experimental data [32]. The (AAD) is dened as

TABLE 2
Heat capacities Cp of water
T/K

The heat capacity was measured using the differential scanning

calorimeter consisting of a DSC-2010 and a thermal analysis controller from TA Instruments. The DSC operating range is from the
room temperature to T = 998 K. Both the temperatures and the
heat ow associated with the transitions in materials can be easily
and rapidly measured with the system. The DSC operates with a
temperature repeatability of 0.1 K. Calorimetric sensitivity is
1 lW (rms) with a precision of 0.01 kJ  kg1  K1 based on the
measurements of metal samples. The purge gas was nitrogen with
a ow rate of 40 cm3  min1. The heating rate was set to be
5 K  min1. By using the sample encapsulating press, the liquid
sample was prepared in a hermetic sample pan. The internal volume of the hermetic pan was approximately 10 mm3. Sample mass

303.2
308.2
313.2
318.2
323.2
328.2
333.2
338.2
343.2
348.2
353.2
(AAD)
a

Cp/(kJ  kg1  K1)

Osborne et al. [32]

This study

4.1785
4.1782
4.1786
4.1795
4.1807
4.1824
4.1844
4.1868
4.1896
4.1928
4.1964

4.182 0.013a
4.183 0.013
4.182 0.012
4.184 0.013
4.186 0.013
4.187 0.012
4.189 0.012
4.191 0.012
4.194 0.012
4.197 0.012
4.202 0.012
0.11

Mean value standard deviation.

105

Y.-H. Yu et al. / J. Chem. Thermodynamics 41 (2009) 103108

n
1X
jelit  eexpt ji =elit ;
n i

1
600

525

450

where elit is the literature value, eexpt is the experimental value, and
n is the number of data points. Hence, the measured Cp values of liquid water for temperatures (303.2 to 353.2) K are in good agreement with those reported by Osborne et al. [32]. On the basis of
comparison with the literature values for water, the uncertainty
of the Cp measurements was estimated to be 0.015 kJ  kg1  K1.
Upon the calibration, the Cp values of ve [Emim]-based ionic
liquids were then measured at temperatures ranging from (303.2
to 358.2) K. To further validate that the measured Cp results in this
work were correct, available literature data were also compared.
Among the studied ILs, only [Emim][BF4] and [Emim][CF3SO3] have
literature values available. To this end, [Emim][BF4] was used to
demonstrate the accuracy of our Cp measurements through comparison with the available literature data of Waliszewski et al. [5]
At temperatures (303.2, 313.2, 323.2, 333.2, 343.2, and 353.2) K,
we report the values of Cp for [Emim][BF4] of (1.547, 1.569, 1.588,
1.598, 1.613, and 1.631) kJ  kg1  K1, respectively. These values
were very close to those reported by Waliszewski et al. [5], which
were (1.548, 1.565, 1.582, 1.600, 1.619, and 1.639) kJ  kg1  K1
at the same temperature. As presented in table 4, the present Cp
measurements are consistent with the Cp data of Waliszewski et
al. [5], as shown by the values of (AAD) of 0.67 and 0.49, respectively. The data of Waliszewski et al. [5] appear to have slightly
higher Cp values compared to the present Cp measurements. This
may be attributed to the difference in the water content of the IL
used in these two studies. The [Emim][BF4] used by Waliszewski
et al. [5] has a water mass percent of about 0.04, while the
[Emim][BF4] used in this study has a water mass percent of 60.9.
This observation proved once more why purity is the most serious
one among the many reasons to account for differences in the published experimental data for thermophysical properties [33].
The measured Cp values of the investigated ILs are presented in
table 3 (specic heat capacities) and are also shown in gure 2 (molar heat capacities). Results are presented between T = (303.2 and
358.2) K. The heat capacity increases linearly with an increase in
the temperature. Differences in the heat capacity for the investigated ILs are due to the changes in the anions. Since the investigated
ILs have a common cation, the molar heat capacity varies with
the anion, and decreases following the order [MDEGSO4] >
[C2H5SO4] > [CF3SO3] > [C2N3] > [BF4]. The anion types appear
to contribute independently to the Cp values of the ILs.
As also shown in gure 2, [Emim][C2H5SO4] is observed to have
the strongest temperature dependence of Cp, while [Emim][MDEGSO4] has the weakest temperature dependence of Cp. For the purpose of application, the measured Cp values of the investigated
ILs are expressed as a function of temperature as follows:

Cp / (J mol-1 K-1)

AAD

375

300

300

320

340

360

T/K
FIGURE 2. Plot of molar heat capacities against temperature for [Emim]-based ionic
liquids obtained from this work: ., [Emim][MDEGSO4] (M = 338.43); j,
[Emim][CF3SO3] (M = 260.24); , [Emim][C2H5SO4] (M = 236.29); N, [Emim][BF4]
(MW = 197.97); d, [Emim][C2N3] (M = 177.21); and lines, calculated using equation
(2).

C p;m a bT cT2 ;

where Cp,m is the molar heat capacity in (J  mol1  K1) and T is the
absolute temperature in K. The parameters a, b, and c were determined by tting all the data from this work and from the available
literature data that were consistent with the present measurements. Table 4 shows the results of the calculation of Cp,m using
equation (2) based on the selected Cp data. As presented in table
4, the agreement of Cp measurements among different investigators
is very satisfactory. The determined empirical parameters a, b, and c
for each ionic liquid represent well the present experimental results
and the selected literature data as shown by the overall (AAD) of
about 0.43 for a total of 140 data points, as presented in table 4.
The determined parameters a, b, and c of equation (2) are also presented in table 4 along with the correlation coefcient (R2). The correlation as in equation (2) represents the present experimental data
satisfactorily as well as the selected literature data for the investigated systems as shown by the value of R2 equal to unity.
3.2. Electrical conductivity
The r values of the standard KCl solution were measured to calibrate the cell of the conductivity meter. The measurements were
done before the measurements on each sample to ensure that
the conductivity cell was functioning properly. Table 5 contains a

TABLE 3
Heat capacities Cp of the investigated ionic liquids
T/K

303.2
308.2
313.2
318.2
323.2
328.2
333.2
338.2
343.2
348.2
353.2
358.2
a

Cp/(kJ  kg1  K1)

[Emim][BF4]

[Emim][CF3SO3]

[Emim][C2N3]

[Emim][C2H5SO4]

[Emim][MDEGSO4]

1.547 0.018a
1.558 0.018
1.569 0.014
1.580 0.017
1.588 0.018
1.593 0.017
1.598 0.018
1.608 0.022
1.613 0.022
1.623 0.022
1.631 0.021
1.634 0.021

1.458 0.011
1.466 0.011
1.473 0.011
1.481 0.010
1.489 0.011
1.497 0.012
1.505 0.011
1.513 0.009
1.521 0.011
1.529 0.011
1.536 0.013
1.544 0.014

1.851 0.018
1.862 0.018
1.879 0.018
1.891 0.018
1.911 0.018
1.923 0.018
1.934 0.018
1.944 0.018
1.955 0.018
1.969 0.018
1.984 0.018
1.999 0.019

1.819 0.009
1.827 0.010
1.841 0.011
1.850 0.012
1.868 0.011
1.881 0.012
1.893 0.012
1.905 0.009
1.917 0.010
1.932 0.008
1.951 0.010
1.962 0.008

1.696 0.014
1.701 0.014
1.706 0.014
1.711 0.015
1.716 0.015
1.720 0.015
1.726 0.014
1.731 0.014
1.736 0.013
1.742 0.013
1.747 0.012
1.753 0.012

Mean value standard deviation.

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Y.-H. Yu et al. / J. Chem. Thermodynamics 41 (2009) 103108

TABLE 4
Molar heat capacity Cp,m of the investigated ionic liquids using equation (2)
System

T/K

No. of data points

Reference

(AAD)A

aA/ (J  mol1  K1)

b A/
(J  mol1  K2)

105 cA/(J  mol1  K3)

R2

[Emim][BF4]

283.15 to 358.15
303.2 to 358.2
313.13 to 425.15
303.2 to 358.2
303.2 to 358.2
303.2 to 358.2
303.2 to 358.2

16
12
64
12
12
12
12
140

Waliszewski et al. [5]

This study
Diedrichs and Gmehling [2]
This study
This study
This study
This study

0.67
0.49
0.60
0.20
0.11
0.09
0.02
0.43

279.24

0.10312

66.350

1.0

271.10

0.35907

0.307

1.0

104.71
401.52
531.92

0.96220
0.35939
0.03759

74.546
148.871
58.252

1.0
1.0
1.0

[Emim][CF3SO3]
[Emim][C2N3]
[Emim][C2H5SO4]
[Emim][MDEGSO4]
Overall
A

Calculated from equation (2).

TABLE 5
A sample measurement of electrical conductivity r of the standard KCl solution

r/(mS  cm1)

T/K

298.2
299.2
301.2
303.2
308.2
313.2
318.2
323.2
a

Merck Co.a

This study

1.408
1.434
1.491
1.547
1.685
1.836
1.981
2.137

1.411
1.430
1.494
1.550
1.680
1.830
1.983
2.140

the accuracy of the present r data. The discrepancy in the measurements may be attributed to the differences in purity of the ILs used in
these two studies. Vila et al. [6] used [Emim][BF4] having a water
mass percent of 61.0, while this study used [Emim][BF4] with a
water mass percent of 6 0.9. Again, another proof that purity was
one of the most serious reasons for the differences in the experimental data of thermophysical properties [33].
Our values of the r for the investigated ILs are presented in
table 6 and are also shown in gure 3. Among the investigated

Merck Calibration Laboratory for pH value and electrical conductivity.

7.5

6.0

4.5

/ (S m-1)

sample of the measured r values of standard KCl solution along

with the r values from the standard analysis done by the chemical
supplier (Merck Calibration Laboratory for pH value and electrical
conductivity). As presented in this table, the present r measurements were very close to those by the Merck Calibration Laboratory, thus validating the present experimental procedure for the
measurements of r data.
Upon the calibration of the conductivity meter cell, the r values of
the ionic liquids investigated were then measured for temperatures
ranging from (293.2 to 353.2) K. To justify further that the r values
obtained in this work are correct, available literature data were also
compared. Of the ve ILs investigated, only two of them have literature values for comparison, viz. [Emim][BF4] and [Emim][C2H5SO4].
To this end, [Emim][BF4] was used to show the accuracy of the present r values by comparing the r data from this work to the available
literature data of Vila et al. [6]. For temperatures of (303.2, 313.2,
323.2, 333.2, 343.2, and 353.2) K, this study found that the values
of r for [Emim][BF4] were (1.789, 2.320, 2.910, 3.590, 4.350, and
5.180) S  m1, respectively. These values are very close to those values reported by Vila et al. [6], which were (1.788, 2.280, 2.850, 3.560,
4.350, and 5.220) S  m1 at the same temperature, thus validating

3.0

1.5

0.0

288

306

324

342

360

T/K
FIGURE 3. Plot of electrical conductivities against temperature for [Emim]-based
ionic liquids obtained from this work: ., [Emim][MDEGSO4] (M = 338.43); j,
[Emim][CF3SO3] (M = 260.24); , [Emim][C2H5SO4] (M = 236.29); N, [Emim][BF4]
(MW = 197.97); d, [Emim][C2N3] (M = 177.21); and lines, calculated using equation
(3).

TABLE 6
Electrical conductivities r of the investigated ionic liquids
T/K

293.2
298.2
303.2
308.2
313.2
318.2
323.2
328.2
333.2
343.2
353.2
a

r/(S  m1)
[Emim][BF4]

[Emim][CF3SO3]

[Emim][C2N3]

[Emim][C2H5SO4]

[Emim][MDEGSO4]

1.377 0.009a
1.569 0.010
1.789 0.003
2.040 0.010
2.320 0.013
2.590 0.013
2.910 0.012
3.250 0.012
3.590 0.011
4.350 0.013
5.180 0.011

0.834 0.010
0.979 0.010
1.155 0.012
1.340 0.013
1.523 0.011
1.737 0.011
1.936 0.012
2.170 0.014
2.420 0.013
2.940 0.010
3.510 0.013

1.890 0.013
2.200 0.015
2.550 0.013
2.900 0.010
3.290 0.013
3.680 0.013
4.100 0.014
4.540 0.011
5.020 0.011
5.930 0.012
6.860 0.010

0.310 0.008
0.398 0.009
0.493 0.003
0.603 0.010
0.722 0.010
0.852 0.010
1.002 0.009
1.167 0.009
1.341 0.009
1.735 0.010
2.150 0.010

0.110 0.011
0.147 0.009
0.194 0.009
0.244 0.010
0.307 0.013
0.378 0.011
0.459 0.012
0.545 0.012
0.641 0.011
0.859 0.013
1.124 0.013

Mean value standard deviation.

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Y.-H. Yu et al. / J. Chem. Thermodynamics 41 (2009) 103108

TABLE 7
Electrical conductivity of the investigated ionic liquids using equation (3)
System

T/K

[Emim][BF4]

258.1
293.2
258.1
293.2
293.2
293.2
293.2

[Emim][CF3SO3]
[Emim][C2N3]
[Emim][C2H5SO4]
[Emim][MDEGSO4]
Overall
a

to
to
to
to
to
to
to

433.1
353.2
433.1
353.2
353.2
353.2
353.2

No. of data points

Reference

(AAD)a

r1a/(S  m1)

Eaa/meV

Tga/K

12
11
11
11
11
11
11
78

Vila et al. [6]

This study
Vila et al. [6]
This study
This study
This study
This study

0.93
0.74
0.50
0.50
0.35
0.29
0.44
0.54

361.20

91.60

102.66

98.28

57.34

153.52

81.77
77.86
64.93

37.24
52.95
57.80

178.62
181.85
187.89

Calculated from equation (3).

ILs, [Emim][C2N3] has the largest value of r and [Emim][MDEGSO4]

has the smallest value of r. The IL [Emim][C2N3] has the strongest
temperature dependence on r values, while [Emim][MDEGSO4]
has the weakest temperature dependence on r values.
From the present experimental results, the inuence of the anion sizes in the temperature dependence of the electrical conductivity was also interpreted. Generally, lower size molecules
usually have higher ionic mobility and so higher electrical conductivity. This was generally the major observation in the ILs studied
as shown in gure 3, with some inconsistent behaviour in the case
of [Emim][C2H5SO4] and [Emim][CF3SO3] with molar masses as
236.29 and 260.24, respectively. This same behaviour, the increase
of r value with the anion size, had been observed and explained
previously by Vila et al. [34] when studying the electrical conductivity of a highly concentrated aqueous solution of aluminium
halide salts and imidazolium-based ionic liquids. In that work,
Vila et al. [34] concluded that the anion size has two effects in electrical conductivity, i.e., the decrease of the surface electrical charge
density and the effect of size for dynamical movement (hopping to
adjacent holes); thus, a decrease or an increase of r value with the
anion size could be observed.
For the purpose of comparison and application, the r values of
the studied [Emim]-based ILs are estimated using the method employed by Vila et al. [6], in which they employed a modied version
of VTF-type (VogelTammanFulcher) equation, which consequently reads

r r1 exp 


Ea
;
kB T  T g

where r1 is the maximum electrical conductivity (that it would

have at innite temperature) in S  m1, Ea is the activation energy
for electrical conduction (which indicates the energy needed for
an ion to hop to a free hole) in meV, kB is the Boltzmanns constant,
and Tg is the glass transition temperature in K.
Using equation (3), the parameters r1, Ea, and Tg were determined by tting the present r measurements and selected literature data, in which same criteria were used in the selection as
discussed previously. Table 7 contains the results of the calculation
of r using equation (3) from the different investigators. As presented in table 7, the agreement of r measurements among different investigators is satisfactory. The determined parameters r1, Ea,
and Tg for the investigated ionic liquids are also presented in table
7. The determined parameters r1, Ea, and Tg for each ionic liquid
correlated well with the present r measurements and the available
literature data as shown by the overall (AAD) of about 0.54% for a
total of 78 data points. It was also observed in table 7 that the maximum conductivity value r1, the maximum Ea, and the minimum
Tg correspond to [Emim][BF4].
4. Conclusions
The heat capacities and electrical conductivities of ve [Emim]based ILs were measured over the temperature ranging from

(303.2 to 358.2) K and from (293.2 to 353.2) K, respectively. The

heat capacity was measured using a DSC and the electrical conductivity was measured using a conductivity meter. The Cp and r values of standard materials have been measured too in order to
check the accuracy of the apparatus and the experimental procedures used. Using (liquid water + KCl) solution as standard materials, the accuracy of the apparatus and the experimental procedures
used was justied. The Cp and r values from this work are in good
agreement with the available experimental data. The measured Cp
and r of each IL is expressed as a function of temperature. An
empirical equation was used to correlate the temperature dependency of Cp values and a modied VTF-type (VogelTammanFulcher) equation was employed to establish the temperature
dependency of r values. The correlations show satisfactory results.
Acknowledgement
This research was supported by a Grant, NSC 96-2221-E-033020, of the National Science Council of the Republic of China.
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JCT 08-235