Chemical Physics 539 (2020) 110933

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Chemical Physics
journal homepage: www.elsevier.com/locate/chemphys

High correlate simple equations for temperature and pressure dependence of T

the viscosity of ionic liquids
Leila Darabi, Morteza Zare
⁎

Department of Chemistry, Faculty of Science, Shahid Chamran University of Ahvaz, Ahvaz 43337, Iran

ARTICLE INFO ABSTRACT

Keywords: In this work, a new simple linear equation was proposed to represent the pressure dependence of the viscosity of
Ionic liquid ionic liquids. Literature experimental viscosity data were utilized and correlated as a function of pressure. The
High pressure viscosity data of various ionic liquids including imidazolium, pyridinium, pyrrolidinium, and ammonium with a
Viscosity variety of anions were considered to examine the generality of the proposed equation. We showed that this
Correlation
equation provides accurate descriptions of the viscosity of ionic liquids as a function of pressure. Therefore, the
Pressure–viscosity coefficient
proposed linear equation combines simplicity and accuracy. In addition, a new equation was proposed to in­
corporate both the temperature and pressure dependence of the viscosity (η–T–p). The results indicated that the
η–T–p model shows high accuracy with an overall average absolute relative deviation of 2.69% in the tem­
perature range of 283.15–363.15 K and the pressure range of 0.06–300 MPa. Moreover, we analyzed the
pressure-viscosity coefficient, which quantifies the effect of pressure on the fluid’s viscosity. The calculated
pressure-viscosity coefficient was found to increase with increasing alkyl chain length of the cation.

1. Introduction pressure are important, especially considering their practical applica­

Ionic liquids (ILs) are defined as molten salts with melting points
below 100 °C [1]. These liquids are composed of bulky organic cations
and organic or inorganic anions. A variety of cations and anions can be
used to create an entire family of materials having different physico­
chemical properties for applications in very different fields such as
chemical engineering, polymer sciences, material chemistry, catalysis,
and electrochemistry [2–8]. The ILs are good candidates for the re­
placement of volatile organic solvents and conventional lubricants,
owing to their promising properties like negligible vapor pressure, low
melting point, wide liquid range, non-flammability, and high thermal
stability [9–12].
The viscosity of fluids is an important factor in chemical engineering
applications. When compared to the conventional organic solvents,
ionic liquids are much more viscous and display a broader range of
viscosities, from 10 to greater than 105 mPa.s [13], depending on the
type of cation and anion present. High to low viscous ILs can be useful
depending on a particular application. The high viscosity of many ILs is
useful for applications as lubricants, while low viscosity allows that ILs
can be used as a solvent in order to minimize pumping costs and in­
crease mass transfer rates.
The viscosity behavior of ILs as a function of temperature and
tions as new lubricants, in determining the load-carrying capacity of the
fluid and the film formation on the sliding surfaces [11,12]. The pres­
sure-viscosity coefficient ( ), which is a very important parameter to
determine the suitability of a lubricant, is used to characterize the
variation of viscosity with pressure [14,15].
Most of the published studies on ILs are related to the variation of
viscosity with temperature, while high-pressure studies are scarce.
Harris et al. [16–19] reported the high-pressure viscosity of some imi­
dazolium-based ILs. They utilized the modified Litovitz and Vogel-
Fulcher-Tammann (VFT) equations to represent the temperature and
pressure dependence of the viscosity. The high-pressure viscosity of five
imidazolium-based ILs have been measured by Ahosseini et al. [20] and
correlated using a hybrid Tait–Litovitz equation. A study on the visc­
osity of eight pyridinium-based ILs has been reported by Bandres et al.
[21] for wide pressure and temperature ranges. They fitted the ex­
perimental data to a seven-parameter Tait-like fitting equation. Atilhan
et al. [22] reported a combined high-pressure experimental and com­
putational study on the viscosity of four imidazolium-based ILs and
used the Tait-like equation for viscosity data correlation. The high-
pressure viscosity data have been published for several imidazolium-
and pyrrolidinium-based ILs by Gacino et al. [23–25] and correlated
with the modified Litovitz and VFT equations. In 2018, Dakkach et al.

⁎
Corresponding author.
E-mail address: m.zare@scu.ac.ir (M. Zare).

https://doi.org/10.1016/j.chemphys.2020.110933
Received 28 December 2019; Received in revised form 18 June 2020; Accepted 16 July 2020
Available online 01 August 2020
0301-0104/ © 2020 Elsevier B.V. All rights reserved.
L. Darabi and M. Zare Chemical Physics 539 (2020) 110933

Table 1
Ionic liquids studied in this work. The references to the viscosity data are also included.
IL abbreviation Chemical Name Ref.

[C2mim][Tf2N] 1-ethyl-3-methylimidazolium bis[(trifluoromethyl)sulfonyl]imide [22]

[C4mim][Tf2N] 1-butyl-3-methylimidazolium bis[(trifluoromethyl)sulfonyl]imide [17,22]
[C6mim][Tf2N] 1-hexyl-3-methylimidazolium bis[(trifluoromethyl)sulfonyl]imide [20]
[C10mim][Tf2N] 1-decyl-3-methylimidazolium bis[(trifluoromethyl)sulfonyl]imide [20]
[C4mim][BF4] 1-butyl-3-methylimidazolium tetrafluoroborate [19]
[C6mim][BF4] 1-hexyl-3-methylimidazolium tetrafluoroborate [20]
[C8mim][BF4] 1-octyl-3-methylimidazolium tetrafluoroborate [16]
[C4mim][PF6] 1-butyl-3-methylimidazolium hexafluorophosphate [18,22]
[C6mim][PF6] 1-hexyl-3-methylimidazolium hexafluorophosphate [17,20]
[C8mim][PF6] 1-octyl-3-methylimidazolium hexafluorophosphate [30]
[C4mmim][(C2F5)3PF3] 1-butyl-2,3-dimethylimidazolium tris(pentafluoroethyl)trifluorophosphate [23]
[C2mim][C2H5SO4] 1-ethyl-3-methylimidazolium ethylsulfate [24]
[C2mim][CF3SO3] 1-ethyl-3-methylimidazolium trifluoromethanesulfonate [28]
[C3py][BF4] 1-propylpyridinium tetrafluoroborate [21]
[C4py][BF4] 1-butylpyridinium tetrafluoroborate [21]
[C42mpy][BF4] 1-butyl-2-methylpyridinium tetrafluoroborate [21]
[C43mpy][BF4] 1-butyl-3-methylpyridinium tetrafluoroborate [21]
[C44mpy][BF4] 1-butyl-4-methylpyridinium tetrafluoroborate [21]
[C83mpy][BF4] 1-octyl-3-methylpyridinium tetrafluoroborate [21]
[C43mpy][N(CN)2] 1-butyl-3-methylpyridinium dicyanamide [21]
[C43mpy][Tf2N] 1-butyl-3-methylpyridinium bis(trifluoromethylsulfonyl)imide [26]
[C4py][CF3SO3] 1-butylpyridinium trifluoromethanesulfonate [21]
[C4mpyrr][CF3SO3] 1-butyl-1-methylpyrrolidinium trifluoromethanesulfonate [25]
[C4mpyrr][Tf2N] 1-butyl-1-methylpyrrolidinium bis[(trifluoromethyl)sulfonyl]imide [24]
[C1OC2mpyrr][Tf2N] 1-(2-methoxyethyl)-1-methylpyrrolidinium bis[(trifluoromethyl)sulfonyl]imide [24]
[N4,1,1,1][Tf2N] butyltrimethylammonium bis(trifluoromethylsulfonyl)imide [26]

[26] reported viscosity values of butyltrimethylammonium and 1-butyl-
3-methylpyridinium bis(trifluoromethylsulfonyl)imide at high pres­
sures. They utilized the equation proposed by Comuñas et al. [27]
which is a modified VFT equation. Recently, Sequeira et al. [28] have
measured and analysed the viscosities of 1-ethyl-3-methylimidazolium
trifluoromethanesulfonate at pressures up to 50 MPa.
There is still a need to develop reliable and simple models for the
correlation of viscosities of ionic liquids within wide ranges of tem­
perature and pressure. It should be emphasized that the complete
pressure and temperature dependence of the viscosity is very compli­
cated, and any single correlation is unlikely to be within the experi­
mental accuracy over a broad range of temperature and pressure. In this
work, we propose a new simple linear equation to describe the viscosity
of ionic liquids with pressure. Also, there is a need to develop reliable
and simple models for the correlation of viscosities of ionic liquids over
observed in Table 1, the imidazolium-, pyridinium-, pyrrolidinium-, and
ammonium-based ILs with different alkyl chain lengths and various
anions are studied. Impurities has a remarkable effect on the viscosity
of ILs. The presence of halide generally increases the viscosity values of
the ILs and the presence of water results into a lower viscosity [22,29].
Thus, the water and halide contents of the ILs samples must be con­
sidered in the evaluation of literature experimental viscosity data. A
detailed list of the viscosity measurement methods, standard un­
certainties of the methods, and water and halide contents is provided in
the Supplementary Material (Table S1).
The temperature dependence of the viscosity (η) of liquids is rea­
sonably well described by the Arrhenius equation [31,32]:
= 'exp(E /RT ) (1)
where is a pre-exponential factor, E is the activation energy, R is the
'

wide ranges of temperature and pressure. It should be emphasized that
the complete pressure and temperature dependence of the viscosity is
very complicated, and any single correlation is unlikely to be within the
experimental accuracy over a broad range of temperatures and pres­
sures. The development of a new equation is also outlined in which
both temperature and pressure dependence of the viscosity of ionic li­
quids can be incorporated. The viscosity data of various ILs including
imidazolium, pyridinium, pyrrolidinium, and ammonium with a variety
of anions are considered to warrant generality of the proposed equa­
tions. The accuracy of the proposed equation is compared with litera­
ture models on ionic liquid viscosities. The proposed equations combine
simplicity and accuracy. The pressure-viscosity coefficient ( ) is also
calculated for the studied ILs using the proposed correlation.
2. Data and methods
In the literature, most of the published studies on the ILs viscosity
have been carried out at ambient pressure, where numerous combina­
tions of cations and anions are involved. However, there are very few
studies addressing the viscosity of ILs at elevated pressures [22,29].
High-pressure viscosity data of 26 ILs are examined to verify the pro­
posed equations. The list of ILs, abbreviations, and sources of the ex­
perimental viscosity data can be observed in Table 1. As can be
universal gas constant and T is the absolute temperature. However, it
has been known that the viscosity of ILs increases sharply with de­
creasing temperature and deviates from the Arrhenius equation
[33,34]. In the case of non-Arrhenius liquids, the Litovitz equation
[35]:
= A'exp(B'/ RT 3) (2)
and the Vogel– Fulcher–Tammann (VFT) equation [36–38]:
= A'' exp(B''/(T To)) (3)
are often used, where A′ and A″ are pre-exponential factors and B′, B″
and To are specific substance-dependent parameters. In recent years,
the viscosity of ILs has been reasonably well represented by the Litovitz
and VFT equations [16,17,24,25,39,40]. In 2010, we have shown that
the temperature dependence of the viscosity of ILs can be described on
the basis of fluidity (i.e. 1/η) by the following simple linear equation
[41,42]:
1
= a + bT
(4)
where a and b are specific adjustable parameters of ILs and ϕ is a
characteristic exponent. This three-parameter equation describes the
temperature dependence of the viscosity of a wide variety of ILs

2
L. Darabi and M. Zare
Fig. 1. (a) Plots of η0.3 versus pressure at different temperatures for [C2mim]
[C2H5SO4]: (■) 313.15 K, (▲) 343.15 K, (●) 363.15 K. The solid lines are the
fits of Eq. (8) with ϕ = 0.3. (b) Plots of η0.3 versus pressure at 323.15 K for
several ILs: (□) [C2mim][Tf2N], (Δ) [C6mim][Tf2N], (○) [C10mim][Tf2N], (■)
[C3py][BF4], (▲) [C4py][BF4].
including imidazolium-, pyridinium-, pyrrolidinium-, ammonium-, and
nicotinium-based and a broad range of anions (such as halides, [PF6]–,
[BF4]–, [(CN)2N]–, [Tf2N]–, [CH3COO]–, [CF3SO3]–, [CH3SO4]–,
[C2H5SO4]–) with high accuracy. The fluidity equation (Eq. (4)) has
been successfully applied as a two-parameter equation with a universal
exponent (ϕ = 0.3) [42,43]. This equation has attracted considerable
attention in recent years [44–54]. Ghatee and Zare [43] showed that
the parameters (a and b) of Eq. (4) are related to fragile-strong cross­
over temperature. The viscosity of two ionic liquids based on benzyli­
midazolium cation has been satisfactorily correlated using the fluidity
equation [44]. Yu et al. [45] utilized Eq. (4) to describe the dependence
of viscosity on temperature for 696 ILs. Seoane et al. [46] correlated the
viscosity of the imidazolium-, pyridinium-, and pyrrolidinium-based ILs
by using Eq. (4). Moosavi et al. [48] reported that the fluidity equation
can describe the temperature dependent viscosity of three imidazolium-
based dicationic ILs quite accurately. The temperature dependence of
3
Chemical Physics 539 (2020) 110933
viscosity of a set of nine waste lubricant oils has been accurately de­
scribed by Eq. (4). It is also applied to a series of normal aliphatic al­
cohols, methanol through n-dodecanol [50]. Ghaedi et al. [51] utilized
the fluidity equation to represent the temperature dependence of the
viscosity of several phosphonium-based deep eutectic solvents. The
temperature dependence of viscosity of five quaternary ammonium-
based ionic liquids with [Tf2N]– anion can be accurately described by
Eq. (4) [52]. The fluidity equation was also applied for the temperature
dependence of viscosity of ether-, alcohol-, carboxylic-, and nitrile-
functionalized ILs [54].
The major effort in the literature has been focused on the variation
of ILs viscosity with temperature, while the number of high-pressure
studies is limited. Harris et al. [16,18] modified both Litovitz and VFT
equations in order to provide reliable descriptions of the viscosity–­
temperature–pressure behavior as follows:
= exp(a + bp + (c + dp + ep2 )/T 3), modified Litovitz (5)
= exp(a' + b'p + (c ' + d'p + e 'p2 )/(T To)), modified VFT (6)
Comuñas et al. [27] suggested the following equation to correlate
the viscosity as a function of pressure and temperature:
B p + E (T )
= Aexp exp D ln
T C 0.1 + E (T ) (7)
where A, B and C are obtained by fitting viscosity data at the reference
pressure of 0.1 MPa as a function of temperature. Coefficient D is as­
sumed to be temperature independent and E(T) is a second-order
polynomial function of temperature: E(T) = E0 + E1T + E2T2. These
equations (Eqs. (5)–(7)) have been applied to the correlation of visc­
osities of ILs [17–19,23–26,55].
Generally, when pressure is applied to a liquid, the molecules are
forced together, holes and defects vanish, and the viscosity of the liquid
increases [56]. At a given temperature, increasing the pressure leads to
a non-linear smooth augmentation of the viscosity of ILs. Herein, we
propose a relationship between the viscosity of ionic liquids and pres­
sure as follows:
= A + Bp (8)
where A and B are specific adjustable parameters and ϕ is a char­
acteristic exponent. We employ two different approaches in using this
equation. First, we use the Eq. (8) as a two-parameter equation by fixing
the exponent ϕ at 0.3, and next as a three-parameter equation by op­
timizing ϕ as an adjustable parameter.
As shown in the next section, the parameters of Eq. (8) with ϕ = 0.3
(A and B) decrease with increasing temperature. The parameters A and
B can be described by second-order polynomial functions of tempera­
ture (Figs. S1 and S2 of the Supplementary data):
A = A0 + A1 T + A2 T 2 (9)
B = B0 + B1 T + B2 T 2 (10)
In order to find a relation for representing the viscosity as a simulta­
neous function of both pressure and temperature, Eqs. (9) and (10) are
substituted into Eq. (8) to construct an equation to fit the data set as a
whole:
=
(A0 + A1 T + A2 T 2) + (B0 + B1 T + B2 T 2) p, (with = 0.3) (11)
Here, we utilize Eq. (11) for the temperature and pressure depen­
dence of viscosity data for ILs. The experimental p–η–T data for each IL
are fitted to Eq. (11) and the best-fitted parameters (A0, A1, A2, B0, B1,
and B2) are calculated using the linear least-squares method using the
SigmaPlot 8.0 software.
The effect of pressure on the viscosity can also be analyzed by the
pressure–viscosity coefficient, , defined by Dowson and Higginson
[57]:
L. Darabi and M. Zare Chemical Physics 539 (2020) 110933

Table 2
Temperature, pressure range, number of viscosity data points, fitting parameters of Eq. (8) with ϕ = 0.3, R2 and AARD for studied ILs.
Ionic liquid T/K Δp/MPa No. of data points A B.102 R2 %AARDa

[C2mim][C2H5SO4] 313.15 10–150 8 0.4045 0.109 0.99879 1.17

343.15 10–150 8 0.3039 0.062 1.00000 0.13
363.15 10–150 8 0.2682 0.050 0.99994 0.21
[C2mim][CF3SO3] 298.22 0.21–50.35 70 0.3898 0.108 0.99904 0.35
313.24 0.22–49.79 63 0.3351 0.083 0.99747 0.46
328.18 0.19–50.07 75 0.2956 0.066 0.99755 0.45
343.19 0.21–50.08 79 0.2654 0.055 0.99927 0.23
358.29 0.22–49.85 66 0.2411 0.048 0.99904 0.25
[C2mim][Tf2N] 303.15 0.1–70.72 9 0.3367 0.101 0.99775 0.94
313.15 0.1–66.81 9 0.3065 0.094 0.99912 0.55
323.15 0.1–71.11 9 0.2864 0.091 0.99954 0.47
333.15 0.1–70.05 9 0.2681 0.078 0.99973 0.32
343.15 0.1–66.69 9 0.2486 0.068 0.99606 0.81
353.15 0.1–70.84 9 0.2332 0.060 0.99912 0.41
[C4mim][Tf2N]b 303.15 0.1–66.83 9 0.3839 0.144 0.99974 0.41
313.15 0.1–64.15 9 0.3436 0.118 0.99988 0.25
323.15 0.1–68.29 9 0.3118 0.100 0.99994 0.20
333.15 0.1–67.98 9 0.2862 0.086 0.99996 0.17
343.15 0.1–62.76 9 0.2654 0.075 0.99969 0.23
353.15 0.1–73.31 9 0.2475 0.067 0.99986 0.19
[C4mim][Tf2N]c 283.15 0.1–74.1 4 0.5079 0.233 0.99907 1.12
298.15 0.1–126.4 6 0.4057 0.171 0.99852 1.64
323.15 0.1–249.6 14 0.3031 0.116 0.99657 3.48
348.15 0.1–200.6 11 0.2550 0.073 0.99957 0.93
[C6mim][Tf2N] 298.15 0.1–124 11 0.4450 0.183 0.99715 2.17
323.15 0.1–124 11 0.3299 0.112 0.99993 0.33
343.15 0.1–124 11 0.2760 0.080 0.99928 0.78
[C10mim][Tf2N] 298.15 0.1–122.57 11 0.5098 0.228 0.99956 0.95
323.15 0.1–122.57 11 0.3695 0.133 0.99986 0.37
343.15 0.1–122.57 11 0.2991 0.101 0.99978 0.53
[C4mim][BF4] 283.15 0.1–100.6 7 0.6672 0.287 0.99898 1.29
298.15 0.1–200.9 11 0.5032 0.208 0.99596 3.79
323.15 0.1–250.13 13 0.3624 0.118 0.99694 3.35
348.15 0.1–300 14 0.2850 0.076 0.99778 2.50
[C6mim][BF4] 298.15 0.1–117.85 11 0.6145 0.270 0.99616 2.80
323.15 0.1–121.81 11 0.4258 0.128 0.99976 0.48
343.15 0.1–121.81 11 0.3371 0.085 0.99962 0.59
[C8mim][BF4] 298.15 0.1–117.5 10 0.7166 0.321 0.99866 1.56
308.15 0.1–200.1 12 0.5996 0.257 0.99686 3.31
323.15 0.1–199.8 11 0.4794 0.180 0.99828 2.45
333.15 25–175.1 7 0.4185 0.147 0.99917 1.12
348.15 0.1–224.2 15 0.3567 0.111 0.99920 1.52
[C4mim][PF6]b 303.15 0.1–64.97 9 0.6212 0.285 0.99912 0.86
313.15 0.1–62.17 9 0.5273 0.215 0.99907 0.76
323.15 0.1–71.1 9 0.4571 0.171 0.99913 0.76
333.15 0.1–68.96 9 0.4054 0.140 0.99944 0.56
343.15 0.1–67.53 9 0.3647 0.120 0.99938 0.54
353.15 0.1–75.7 9 0.3316 0.106 0.99894 0.71
[C4mim][PF6]d 298.15 0.1–174.1 11 0.6573 0.376 0.99383 4.94
308.15 0.1–151 10 0.5664 0.282 0.99703 3.47
323.15 0.1–249.3 15 0.4455 0.209 0.99326 6.67
333.15 0.1–100.1 7 0.4050 0.147 0.99955 0.71
343.15 0.1–172.9 11 0.3629 0.130 0.99858 1.84
[C4mmim][(C2F5)3PF3] 313.15 10–150 8 0.4186 0.361 0.99169 7.15
343.15 10–150 8 0.3066 0.183 0.99311 5.01
[C6mim][PF6]e 298.15 0.1–60.3 9 0.8088 0.398 0.99900 0.85
323.15 0.1–126 11 0.5279 0.211 0.99784 1.47
343.15 0.1–126 11 0.4011 0.136 0.99970 0.56
[C6mim][PF6]c 293.15 0.1–100.1 6 0.8001 0.432 0.99757 2.14
313.15 0.1–150 8 0.6056 0.300 0.99701 3.20
323.15 0.1–174.8 9 0.5123 0.245 0.99722 3.26
333.15 0.1–200.1 8 0.4539 0.195 0.99692 3.94
348.15 0.1–238.5 8 0.3783 0.150 0.99701 3.90
[C8mim][PF6] 293.15 0.1–20 5 1.0133 0.484 0.99705 0.51
313.15 0.1–20 5 0.6762 0.274 0.99736 0.42
333.15 0.1–20 5 0.4945 0.182 0.99681 0.38
353.15 0.1–20 5 0.3863 0.139 0.99842 0.29
[C4mpyrr][CF3SO3] 303.15 10–150 8 0.5296 0.249 0.99788 2.31
313.15 10–150 8 0.4611 0.199 0.99872 1.69
323.15 10–150 8 0.4098 0.162 0.99944 1.07
333.15 10–150 8 0.3702 0.133 0.99900 1.32
343.15 10–150 8 0.3359 0.115 0.99937 0.94
353.15 10–150 8 0.3109 0.095 0.99997 0.18
[C4mpyrr][Tf2N] 313.15 10–150 8 0.3789 0.166 0.99856 1.81
(continued on next page)

4
L. Darabi and M. Zare Chemical Physics 539 (2020) 110933

Table 2 (continued)

Ionic liquid T/K Δp/MPa No. of data points A B.102 R2 %AARDa

343.15 10–150 8 0.2886 0.101 0.99812 1.82

363.15 10–150 8 0.2587 0.079 0.99998 0.21
[C1OC2mpyrr][Tf2N] 313.15 10–150 8 0.3445 0.138 0.99904 1.33
343.15 10–150 8 0.2729 0.086 0.99913 1.14
363.15 10–150 8 0.2452 0.070 0.99977 0.53
[C3py][BF4] 283.15 0.16–65.24 8 0.6842 0.273 0.99870 0.81
293.15 0.09–65.91 8 0.5639 0.183 0.99896 0.67
303.15 0.1–65.2 8 0.4725 0.142 0.99838 0.73
313.15 0.41–65.47 8 0.4094 0.107 0.99826 0.70
323.15 0.58–64.9 8 0.3558 0.104 0.99592 0.91
333.15 0.29–65.07 8 0.3234 0.068 0.99609 0.74
[C4py][BF4] 283.15 0.06–64.73 8 0.7992 0.333 0.99950 0.58
293.15 0.06–65.85 8 0.6383 0.228 0.99713 1.15
303.15 0.11–65.02 8 0.5328 0.165 0.99851 0.73
313.15 0.1–64.71 8 0.4524 0.132 0.99904 0.51
323.15 0.1–64.61 8 0.3927 0.108 0.99956 0.32
333.15 0.1–64.51 8 0.3476 0.087 0.99921 0.38
[C42mpy][BF4] 298.15 0.14–65.69 8 0.6583 0.281 0.99192 2.08
303.15 0.13–65.29 8 0.5999 0.232 0.99565 1.38
313.15 0.13–65.16 8 0.5052 0.173 0.99830 0.86
323.15 0.13–65.15 8 0.4347 0.134 0.99777 0.89
333.15 0.1–64.73 8 0.3766 0.118 0.99835 0.74
[C43mpy][BF4] 283.15 0.13–59.81 8 0.8347 0.398 0.99883 0.87
293.15 0.16–64.56 8 0.6621 0.291 0.99698 1.31
303.15 0.07–65.05 8 0.5476 0.208 0.99858 0.87
313.15 0.12–64.7 8 0.4622 0.161 0.99877 0.73
323.15 0.15–64.74 8 0.3992 0.129 0.99896 0.59
333.15 0.11–64.75 8 0.3516 0.104 0.99846 0.73
[C44mpy][BF4] 283.15 0.1–64.79 8 0.8671 0.460 0.99843 1.18
293.15 0.1–64.96 8 0.6719 0.331 0.99533 1.92
303.15 0.1–64.87 8 0.5509 0.230 0.99840 0.90
313.15 0.1–64.87 8 0.4644 0.173 0.99866 0.74
323.15 0.1–64.7 8 0.3990 0.141 0.99888 0.62
333.15 0.1–64.65 8 0.3499 0.111 0.99976 0.27
[C83mpy][BF4] 283.15 0.1–30.32 5 1.1358 0.502 0.99696 0.84
293.15 0.08–64.8 8 0.8868 0.414 0.99990 0.26
303.15 0.11–64.33 8 0.7097 0.314 0.99872 0.96
313.15 0.09–64.15 8 0.5918 0.222 0.99887 0.72
323.15 0.1–64.08 8 0.5035 0.176 0.99887 0.67
333.15 0.09–64.28 8 0.4346 0.143 0.99744 1.25
[C4py][CF3SO3] 308.15 0.09–64.88 8 0.4786 0.168 0.98746 2.10
313.15 0.15–64.26 8 0.4427 0.157 0.99576 1.32
323.15 0.1–64.69 8 0.3872 0.116 0.99845 0.72
333.15 0.09–64.31 8 0.3443 0.105 0.99431 1.32
[C43mpy][N)CN(2] 288.15 0.14–59.25 8 0.4067 0.113 0.99922 0.42
298.15 0.1–61.47 8 0.3565 0.085 0.99802 0.51
308.15 0.11–59.4 8 0.3172 0.069 0.99643 0.72
318.15 0.14–59.96 8 0.2880 0.055 0.99947 0.31
328.15 0.11–59.92 8 0.2651 0.048 0.99672 0.58
338.15 0.11–60.03 8 0.2448 0.041 0.99766 0.46
348.15 0.1–60.17 8 0.2275 0.036 0.99691 0.54
[C43mpy][Tf2N] 303.15 10–75 5 0.4092 0.170 0.99965 0.49
313.15 10–100 6 0.3654 0.141 0.99885 1.08
323.15 10–100 6 0.3264 0.120 0.99957 0.63
333.15 10–100 6 0.2979 0.099 0.99924 0.80
343.15 10–100 6 0.2746 0.085 0.99951 0.58
353.15 10–100 6 0.2543 0.075 0.99977 0.37
[N4,1,1,1][Tf2N] 303.15 10–150 8 0.4583 0.248 0.99564 3.71
313.15 10–150 8 0.4063 0.192 0.99821 2.11
323.15 10–150 8 0.3624 0.156 0.99827 1.99
333.15 10–150 8 0.3277 0.129 0.99865 1.62
343.15 10–150 8 0.2998 0.111 0.99752 2.11
353.15 10–150 8 0.2772 0.95 0.99973 0.69
Overall 0.06–300 1477 1.24

a
× 100.
1
%AARD = m
| exp t . calc . / exp t .|
m
b
Ref. [22].
c
Ref. [17].
d
Ref. [18].
e
Ref. [20].

5
L. Darabi and M. Zare Chemical Physics 539 (2020) 110933

Table 3
Temperature, fitting parameters of Eq. (8) (A, B, and ϕ), R2 and AARD for
studied ILs. Pressure range and number of viscosity data points are the same as
in Table 2.
Ionic liquids T/K A B.102 ϕ R2 %AARD

[C2mim][C2H5SO4] 313.15 0.7784 0.051 0.0837 0.99996 0.17

343.15 0.3540 0.062 0.2617 0.99999 0.09
363.15 0.2158 0.048 0.3492 0.99996 0.16
[C2mim][CF3SO3] 298.22 0.3000 0.108 0.3833 0.99899 0.36
313.24 0.1988 0.075 0.4432 0.99751 0.46
328.18 0.2900 0.066 0.3047 0.99753 0.45
343.19 0.1447 0.045 0.4372 0.99930 0.24
358.29 0.2412 0.048 0.2999 0.99904 0.25
[C2mim][Tf2N] 303.15 0.7973 0.046 0.0625 0.99933 0.51
313.15 0.7519 0.052 0.0724 0.99992 0.22
323.15 0.6809 0.062 0.0923 0.99997 0.26
333.15 0.5302 0.071 0.1447 0.99993 0.20
343.15 0.4841 0.066 0.1564 0.99665 0.77
353.15 0.1512 0.052 0.3891 0.99916 0.44
[C4mim][Tf2N]a 303.15 0.6334 0.107 0.1433 0.99999 0.11
313.15 0.5092 0.106 0.1897 0.99999 0.11
323.15 0.4041 0.098 0.2333 0.99998 0.11
333.15 0.3399 0.087 0.2588 0.99997 0.15
343.15 0.1917 0.069 0.3734 0.99972 0.22
353.15 0.1812 0.061 0.3668 0.99993 0.27
[C4mim][Tf2N]b 283.15 0.8246 0.097 0.0859 0.99999 0.06
298.15 0.7217 0.096 0.1096 0.99999 0.16
323.15 0.6662 0.068 0.1049 0.99991 0.63
348.15 0.4032 0.071 0.2001 0.99997 0.22
[C6mim][Tf2N] 298.15 0.8311 0.067 0.0691 0.99945 0.91
323.15 0.3843 0.110 0.2589 0.99997 0.17
343.15 0.4965 0.073 0.1634 0.99957 0.59
[C10mim][Tf2N] 298.15 0.6484 0.173 0.1939 0.99994 0.31
323.15 0.3883 0.132 0.2851 0.99986 0.39
343.15 0.3940 0.098 0.2317 0.99988 0.48
[C4mim][BF4] 283.15 0.8766 0.110 0.0987 0.99999 0.16
298.15 0.8567 0.064 0.0695 0.99999 0.16
323.15 0.7268 0.061 0.0959 0.99997 0.46
348.15 0.5959 0.055 0.1255 0.99995 0.34
[C6mim][BF4] 298.15 0.8131 0.136 0.1287 0.99709 2.30
323.15 0.5411 0.113 0.2161 0.99988 0.39
343.15 0.4284 0.082 0.2340 0.99967 0.54
[C8mim][BF4] 298.15 0.8787 0.136 0.1201 0.99999 0.11
308.15 0.8312 0.108 0.1110 0.99997 0.40
323.15 0.7112 0.107 0.1408 0.99995 0.27
333.15 0.6576 0.096 0.1473 0.99999 0.38
348.15 0.5485 0.090 0.1756 0.99999 0.33
[C4mim][PF6]a 303.15 0.9099 0.075 0.0599 0.99999 0.12
313.15 0.9579 0.024 0.0202 0.99998 0.39
323.15 0.9018 0.040 0.0398 1.00000 0.17
333.15 0.8240 0.056 0.0645 0.99996 0.16
Fig. 2. (a) Relative deviations between experimental viscosities ηexpt and pre­
343.15 0.7281 0.070 0.0945 0.99994 0.27
dicted viscosities ηcalc by using Eq. (8) with ϕ = 0.3 (b). The correlation be­ 353.15 0.8536 0.036 0.0431 0.99992 0.21
tween ηcalc and ηexpt (1477 data points). [C4mim][PF6]c 298.15 0.9526 0.049 0.0377 0.99991 0.64
308.15 0.8871 0.075 0.0649 0.99998 0.54
323.15 0.8586 0.057 0.0585 0.99987 1.12
1 333.15 0.6669 0.099 0.1350 0.99997 0.24
=
p T (12) 343.15 0.6884 0.078 0.1115 0.99999 0.38
[C4mmim][(C2F5)3PF3] 313.15 0.9323 0.044 0.0260 0.99999 1.26
Substitution of Eq. (11) into Eq. (12) yields: 343.15 0.9677 0.012 0.0086 0.99993 3.37
[C6mim][PF6]d 298.15 0.7715 0.476 0.3653 0.99905 0.90
10 (B0 + B1 T + B2 T 2) 323.15 0.7305 0.130 0.1486 0.99931 0.90
=
3 (A0 + A1 T + A2 T 2) + (B0 + B1 T + B2 T 2) p (13) 343.15 0.5328 0.118 0.2074 0.99994 0.29
[C6mim][PF6]b 293.15 0.9538 0.096 0.0672 0.99999 0.06
By using Eq. (13), we calculate and analyze the pressure–viscosity 313.15 0.8634 0.105 0.0903 0.99999 0.30
coefficients for the studied ILs. 323.15 0.7292 0.141 0.1448 0.99910 1.61
333.15 0.7639 0.092 0.1038 0.99998 0.32
348.15 0.6738 0.089 0.1241 0.99998 0.29
3. Results and discussion [C8mim][PF6] 293.15 1.0021 0.073 0.0476 0.99802 0.39
313.15 0.6185 0.312 0.3680 0.99704 0.44
3.1. Pressure dependencies 333.15 0.3375 0.196 0.4626 0.99672 0.37
353.15 0.4131 0.138 0.2787 0.99846 0.28

The experimental viscosity data at high pressures are fitted to Eq. (continued on next page)
(8) with ϕ = 0.3 for each isotherm. The result is shown in Fig. 1, where
the values of η0.3 are plotted against p for several ILs. The values of the
fitting parameters, pressure ranges, number of viscosity data points, the
squared correlation coefficient (R2), and average absolute relative

6
L. Darabi and M. Zare Chemical Physics 539 (2020) 110933

Table 3 (continued)

Ionic liquids T/K A B.102 ϕ R2 %AARD

[C4mpyrr][CF3SO3] 303.15 0.8305 0.095 0.0903 0.99999 0.16

313.15 0.7265 0.111 0.1260 0.99999 0.28
323.15 0.5908 0.124 0.1786 0.99998 0.34
333.15 0.6700 0.085 0.1221 0.99999 0.25
343.15 0.5745 0.090 0.1535 0.99999 0.12
353.15 0.3470 0.094 0.2721 0.99998 0.29
[C4mpyrr][Tf2N] 313.15 0.6825 0.100 0.1198 0.99997 0.33
343.15 0.7727 0.047 0.0629 0.99998 0.37
363.15 0.2697 0.079 0.2909 0.99999 0.12
[C1OC2mpyrr][Tf2N] 313.15 0.6106 0.099 0.1403 1.00000 0.25
343.15 0.6041 0.065 0.1171 0.99999 0.14
363.15 0.3950 0.070 0.1988 0.99999 0.23
[C3py][BF4] 283.15 0.8514 0.135 0.1277 0.99913 0.65
293.15 0.5253 0.194 0.3369 0.99897 0.64
303.15 0.3081 0.153 0.4703 0.99852 0.68
313.15 0.4132 0.107 0.2968 0.99827 0.70
323.15 0.4573 0.100 0.2271 0.99608 0.90
333.15 0.2856 0.067 0.3328 0.99651 0.75
[C4py][BF4] 283.15 0.8441 0.259 0.2276 0.99958 0.51
293.15 0.9012 0.069 0.0698 0.99850 0.79
303.15 0.5589 0.160 0.2772 0.99853 0.72
313.15 0.5576 0.117 0.2211 0.99911 0.49
323.15 0.2605 0.106 0.4312 0.99931 0.44
333.15 0.5033 0.080 0.1950 0.99939 0.33
[C42mpy][BF4] 298.15 0.9740 0.024 0.0191 0.99638 1.68
303.15 0.9091 0.060 0.0561 0.99790 1.06
313.15 0.7234 0.112 0.1424 0.99881 0.71
323.15 0.5998 0.110 0.1842 0.99800 0.80
333.15 0.3263 0.119 0.3439 0.99836 0.72
[C43mpy][BF4] 283.15 0.9927 0.017 0.0125 0.99994 0.78
293.15 0.9598 0.038 0.0300 0.99909 0.73
303.15 0.7328 0.136 0.1552 0.99897 0.63
313.15 0.7387 0.095 0.1180 0.99922 0.54
323.15 0.5833 0.107 0.2044 0.99913 0.47
333.15 0.4051 0.102 0.2592 0.99871 0.60
[C44mpy][BF4] 283.15 0.9635 0.123 0.0801 0.99954 0.69
293.15 0.9779 0.024 0.0170 0.99888 1.04
303.15 0.9092 0.055 0.0481 0.99977 0.36
313.15 0.8651 0.056 0.0568 0.99964 0.43
323.15 0.7901 0.067 0.0771 0.99962 0.44
333.15 0.3550 0.111 0.2959 0.99976 0.28
[C83mpy][BF4] 283.15 1.0365 0.123 0.0841 0.99769 0.72
293.15 0.8925 0.393 0.2846 0.99991 0.23
303.15 0.8896 0.125 0.1030 0.99931 0.64
313.15 0.5671 0.232 0.3239 0.99880 0.73
323.15 0.5006 0.177 0.3024 0.99886 0.66
333.15 0.2883 0.149 0.4466 0.99743 1.03
[C4py][CF3SO3] 308.15 0.7424 0.099 0.1213 0.99120 1.88
313.15 0.7061 0.101 0.1283 0.99640 1.19
Fig. 3. Comparisons of the calculated viscosities using Eq. (8) with the ex­
323.15 0.1804 0.104 0.5408 0.99887 0.59
333.15 0.1471 0.087 0.5383 0.99474 1.36 perimental data for considered ILs: (a) Relative deviations versus pressure (b)
[C43mpy][N(CN)2] 288.15 0.5660 0.097 0.1898 0.99932 0.36 Calculated versus experimental viscosities.
298.15 0.4208 0.084 0.2518 0.99807 0.54
308.15 0.3465 0.070 0.2768 0.99646 0.71
318.15 0.1142 0.040 0.5229 0.99961 0.25
deviation (AARD) are listed in Table 2. The values of R2 and AARD of
328.15 0.0110 0.008 1.0198 0.99815 1.54 the correlated data indicate a good fit between the experimental data
338.15 0.3000 0.043 0.2567 0.99773 0.45 and those calculated by Eq. (8). As can be seen, the R2 values for the Eq.
348.15 0.2359 0.037 0.2926 0.99692 0.52 (8) are greater than 0.995 for 130 of the 137 isotherms. For most of the
[C43mpy][Tf2N] 303.15 0.7208 0.100 0.1105 1.00000 0.10
ILs investigated, the AARD values are less than 2%, with an overall
313.15 0.8979 0.032 0.0324 1.00000 0.10
323.15 0.6156 0.089 0.1306 0.99999 0.06 value of 1.24%. Relative deviations between the calculated and ex­
333.15 0.5610 0.082 0.1437 0.99966 0.49 perimental viscosity data are shown in Fig. 2(a), which vary between
343.15 0.3337 0.086 0.2549 0.99954 0.57 –11% and +11%, but the majority of results have relative deviations
353.15 0.4695 0.072 0.1660 0.99996 0.19 less than ± 4%. As shown in Fig. 2(b), the calculated viscosities using
[N4,1,1,1][Tf2N] 303.15 0.9320 0.035 0.0282 1.00000 0.21
313.15 0.7274 0.102 0.1081 0.99999 0.15
Eq. (8) with ϕ = 0.3 are consistent well with the experimental mea­
323.15 0.7253 0.083 0.0964 0.99999 0.10 surements (with R2 = 0.99853). Thus, Eq. (8) can describe the pressure
333.15 0.6715 0.081 0.1083 0.99999 0.15 dependent viscosity of various ILs quite accurately.
343.15 0.9016 0.023 0.0261 1.00000 0.37 As shown in Table 2, the parameters A and B decrease when the
353.15 0.4103 0.091 0.2091 0.99997 0.23
temperature increases for all the studied ILs. Since B is the slope of plots
Overall 0.50
= 0.1888 of 0.3 versus p, its reduction with increasing temperature illustrates that
a the viscosity at higher temperatures is less sensitive to pressure than at
Ref. [22].
b lower temperatures, as can be observed in Fig. 1(a). The comparison of
Ref. [17].
c
Ref. [18].
the viscosity of ILs which differ only in the alkyl side-chain shows that
d
Ref. [20].

7
L. Darabi and M. Zare Chemical Physics 539 (2020) 110933

the viscosity increases when the alkyl chain length increases. The
parameters A and B also increase with increasing number of carbon
atoms in the alkyl chain (Figs. S3–S8 of the Supplementary Material).
The increasing of B indicates that the viscosity of ILs with the longer
alkyl chain is more sensitive to pressure changes.
It should be noted that the experimental viscosity data may have
large discrepancies for some ILs from different literature sources. These
differences can be assigned to the purity of the IL samples and/or dif­
ferent experimental methodologies. Nevertheless, there is a good con­
sistency between the experimental viscosities from different literature
sources used in this work. Therefore, the differences in parameters
between various sources for the same ILs at the same temperatures may
be attributable to the different pressure ranges in which the experi­
ments have been performed.
We also applied Eq. (8) as a three-parameter equation with opti­
mizing ϕ for each IL at different temperatures. The values of the fitting
parameters (A, B, and ϕ), R2 and AARD are listed in Table 3. The values
of ϕ are in the range of 0.0086 to 1.0198 (with the average value of
0.1888). The values of R2 and AARD indicate a good fit between the
calculated and experimental viscosity data. As can be seen, the R2 va­
lues are greater than 0.995 for 135 of the 137 isotherms. The viscosity
data are reproduced with AARDs less than 2% for 135 of the 137
isotherms (with an overall AARD of 0.50%). Relative deviations be­
tween the experimental and calculated viscosities using Eq. (8) are
plotted in Fig. 3(a), which vary from –6 to +7%. However, most of the
viscosity data have relative deviations of less than ± 2%. As shown in
Fig. 3(b), a remarkable agreement is observed between the calculated
and the experimental viscosity data, by using Eq. (8), with
R2 = 0.99990. Using Eq. (8) with an extra adjustable parameter (ϕ)
make significant improvement in the prediction of viscosity for most of
the ionic liquids considered, as expected.
3.2. Temperature and pressure dependencies
The experimental p–η–T data for each IL are fitted to Eq. (11) and
the best-fitted parameters (A0, A1, A2, B0, B1, and B2), R2, and AARD are
listed in Table 4. In Fig. 4, we present the experimental values of η0.3
and correlated η0.3–p–T surfaces for two representative ILs [C2mim]
[C2H5SO4] and [C4py][BF4]. As expected, pressure and temperature act
antagonistically on the viscosity of ILs. As can be seen in Table 4, this
equation reproduces the experimental viscosities with the AARD from
0.54% for [C2mim][C2H5SO4] to 6.65% for [C44mpy][BF4], with an
overall value of 2.69%. Relative deviations between the experimental
and correlated viscosities using Eq. (11) for the studied ILs are

Table 4
Fitting parameters, number of data points, R2 and AARD of Eq. (11) for studied ILs.
Ionic liquid Na A0 -A1.102 A2.105 B0.102 -B1.104 B2.107 R2 %AARD

[C2mim][C2H5SO4] 24 4.8181 2.3895 3.1301 2.6269 1.3966 1.8915 0.99984 0.53

[C2mim][CF3SO3] 353 3.4815 1.6965 2.2114 1.9480 1.0504 1.4524 0.99937 1.33
[C2mim][Tf2N] 54 2.4008 1.0925 1.3560 −0.30295 −0.32069 −0.61820 0.99822 1.52
[C4mim][Tf2N]b 54 4.1890 2.1023 2.7932 2.8951 1.5580 2.1446 0.99952 1.04
[C4mim][Tf2N]c 35 6.7058 3.6573 5.1835 3.1575 1.6799 2.2816 0.99778 3.82
[C6mim][Tf2N] 33 5.8818 3.0813 4.2187 3.6517 1.9753 2.7233 0.99946 1.06
[C10mim][Tf2N] 33 6.6616 3.4492 4.6484 6.0016 3.3735 4.8195 0.99991 0.62
[C4mim][BF4] 45 10.038 5.5383 7.8635 5.0516 2.7867 3.8988 0.99722 5.09
[C6mim][BF4] 33 9.5418 5.0603 6.9298 9.4509 5.3962 7.7715 0.99941 1.29
[C8mim][BF4] 55 12.667 6.8324 9.4693 7.1031 3.8651 5.3335 0.99904 2.38
[C4mim][PF6]b 54 10.427 5.5255 7.5536 8.4360 4.7019 6.6371 0.99876 2.75
[C4mim][PF6]d 54 11.462 6.2042 8.6555 10.088 5.6179 7.9136 0.99652 5.89
[C6mim][PF6]e 31 14.652 7.8903 10.891 10.641 5.9159 8.3186 0.99978 0.96
[C6mim][PF6]c 40 10.025 5.1477 6.8227 6.5591 3.4142 4.5179 0.99821 3.92
[C8mim][PF6] 20 18.840 10.276 14.303 12.896 7.2828 10.396 0.99842 4.76
[C4mpyrr][CF3SO3] 48 7.2975 3.7801 5.1029 5.5442 2.9896 4.0983 0.99891 2.27
[C4mpyrr][Tf2N] 24 4.5902 2.2972 3.0413 3.1771 1.6402 2.1672 0.99949 1.23
[C1OC2mpyrr][Tf2N] 24 3.2565 1.5606 2.0142 2.7893 1.4585 1.9541 0.99967 0.97
[C3py][BF4] 48 12.642 7.2093 10.543 8.3856 4.9919 7.4996 0.99816 3.78
[C4py][BF4] 48 16.106 9.2583 13.597 11.370 6.8226 10.319 0.99743 5.05
[C42mpy][BF4] 40 13.162 7.2346 10.197 14.210 8.4476 12.661 0.99906 1.66
[C43mpy][BF4] 48 17.520 10.106 14.873 12.212 7.2367 10.817 0.99802 4.90
[C44mpy][BF4] 48 19.723 11.478 17.007 15.355 9.1569 13.757 0.99687 6.65
[C83mpy][BF4] 45 26.418 15.359 22.700 7.4785 3.9871 5.3508 0.99861 4.09
[C4py][CF3SO3] 32 9.9120 5.3991 7.5859 7.8951 4.5776 6.7199 0.99822 1.47
[C43mpy][N(CN)2] 55 4.4974 2.3557 3.2455 2.5036 1.4179 2.0384 0.99808 2.90
[C43mpy][Tf2N] 35 4.8211 2.4407 3.2502 2.9757 1.5592 2.0891 0.99968 1.04
[N4,1,1,1][Tf2N] 48 5.5778 2.8299 3.7635 6.3244 3.4724 4.8394 0.99839 2.59
Overall 1461 2.69

a
No. of data points.
b
Ref. [22].
c
Ref. [17].
d
Ref. [18].
e
Ref. [20].

8
L. Darabi and M. Zare
Fig. 4. The experimental values of η0.3 (circles) versus temperature and pres­
sure and the present correlation, Eq. (11) (surfaces) for two representative ILs:
(a) [C2mim][C2H5SO4] and (b) [C4py][BF4].
presented in Fig. 5(a), which vary from –14% to +12%. Most of the
viscosity data have relative deviations of less than ± 4%. Comparisons
between experimental and correlated viscosities using Eq. (11) are
shown graphically in Fig. 6(a) (with R2 = 0.99796). Therefore, it seems
that the proposed correlation (Eq. (11)) is successfully applied for the
9
Chemical Physics 539 (2020) 110933
description of ILs viscosity as a function of temperature and pressure. It
is worth mentioning that the differences between the correlations from
different literature sources for the same ILs in Table 4 may be accounted
for based on different temperature and pressure ranges.
As mentioned earlier, very often the modified Litovitz and VFT
equations are used to correlate the experimental p–η–T data of ILs.
Table 5 lists the best-fitted parameters, R2, and AARD of the modified
Litovitz equation. The values of R2 are more than 0.99500 (except
[C2mim]Tf2N and [C6mim][PF6]) and the overall AARD is 1.73%. Re­
lative deviations between the calculated and experimental viscosity
data are shown in Fig. 5(b), which vary between –12% and +14%, but
the majority of results have relative deviations less than ± 4%. As
shown in Fig. 6(b), the calculated viscosities using the modified Litovitz
equation are consistent well with the experimental measurements (with
R2 = 0.99680).
Experimental p–η–T are successfully correlated with the modified
VFT equation (Eq. (6)), with R2 greater than 0.99500 and an overall
AARD of 1.04% (Table 6). Relative deviations between the experi­
mental and calculated viscosity for ILs are presented in Fig. 5(c), which
vary from –9% to +12%. However, the majority of results have relative
deviations less than ± 4%. The linear relationship between the cal­
culated viscosities and the experimental data is shown in Fig. 6(c), with
R2 = 0.99855.
Table 7 lists the best-fitted parameters, R2, and AARD of Eq. (7)
(proposed by Comuñas et al.). The values of R2 are more than 0.99500
and the overall AARD is 1.12%. Relative deviations between the ex­
perimental and calculated viscosity for ILs are presented in Fig. 5(d),
which vary from –9% to +9%. However, the majority of results have
relative deviations less than ± 4%. As shown in Fig. 6(d), the calcu­
lated viscosities using Eq. (7) are consistent well with the experimental
measurements (with R2 = 0.99936).
Comparing the overall AARD of the correlations studied in this work
(Fig. 7) shows that they have similar accuracy, while the modified VFT
equation is generally the most accurate model. The modified VFT model
has the minimum overall AARD of 1.04% and the present correlation
(Eq. (11)) has the maximum overall AARD of 2.69%. Although the
proposed model (Eq. (11)) presents a higher overall deviation than Eqs.
(5)–(7), by comparing the results of Tables 4–7, one can observe that
the AARD values obtained by Eq. (11) are less than the values obtained
by Eqs. (5)–(7) for some of the studied ILs. Therefore, the present
correlation can provide a better description of the viscosity of some
ionic liquids than the other models. It should be noted that the accuracy
of the present correlation (with an overall AARD of 2.69%) is within the
experimental accuracy for the pressure and temperature ranges con­
sidered (Table S1 of the Supplementary Material). Among the studied
equations, the modified Litovitz requires the least number of adjustable
parameters (five parameters). The number of parameters is six for the
modified VFT equation and the proposed model (with ϕ = 0.3), which
is less than seven in the Comunas et al. model. Since ϕ is a constant with
numerical value of 0.3, η0.3 in Eq. (11) is represented as a polynomial
function of temperature and pressure, while Eqs. (5)–(7) are in the form
of exponentials of polynomial and rational functions. Thus Eq. (11) has
a relatively simpler mathematical expression. In summary, the present
correlation is simple, accurate and applicable over a wide range of
temperatures and pressures.
L. Darabi and M. Zare Chemical Physics 539 (2020) 110933

Fig. 5. Relative deviations between experimental and calculated data obtained by using: (a) Eq. (11); (b) modified Litovitz equation (Eq. (5)); (c) modified VFT
equation (Eq. (6)); (d) Comuñas equation (Eq. (7)).

The group contribution (GC) method and quantitative structure–­
property relationship (QSPR) approach are often used to provide a
reasonable prediction of the viscosity of compounds. In order to de­
velop the GC and QSPR models for the p–η–T behavior of ILs, a suitable
correlation between temperature, pressure, and viscosity needs to be
established. The parameters of the correlation for GC and QSPR ap­
proaches can be adjusted through a linear combination of respective
group contributions and molecular descriptors, respectively. The simple
and accurate p–η–T model proposed in this work can be used for the
estimation of ILs viscosity based on the group contribution method
and/or the quantitative structure–property relationship approach.
3.3. Pressure-viscosity coefficient
The values of pressure–viscosity coefficient, , were calculated
according to Eq. (13) for the studied ILs and are reported in Table S2

10
L. Darabi and M. Zare
Fig. 6. Comparisons of the experimental viscosities with the calculated data using: (a) Eq. (11); (b) modified Litovitz equation (Eq. (5)); (c) modified VFT equation
(Eq. (6)); (d) Comuñas equation (Eq. (7)).
(Supplementary Material). The calculated pressure–viscosity coeffi­
cients are in good agreement with the corresponding literature data
[21–23,25]. Among the studied ILs, [C4mpyrr][Tf2N] and [C6mim]
[PF6] have the highest values of whereas the lowest values are for
[C2mim][C2H5SO4] and [C43mpy][N(CN)2]. Analyzing the values
for the imidazolium-based ILs with different length of the alkyl chain
([Cnmim][Tf2N], [Cnmim][BF4], and [Cnmim][PF6], with n = 4, 6, 8,
11
Chemical Physics 539 (2020) 110933
and 10) shows that the increases with increasing chain length at a
given temperature and pressure. The values are plotted versus
pressure at different temperatures for [C4mpyrr][Tf2N] and [C2mim]
[C2H5SO4] in Fig. 8, as an example, and the others are given in Figs.
S9–S28 (Supplementary Material). This coefficient decreases when the
pressure increases under isothermal conditions, and also decreases
when the temperature increases under isobaric conditions.
L. Darabi and M. Zare Chemical Physics 539 (2020) 110933

Table 5
Fitting parameters, R2 and %AARD of the modified Litovitz equation (Eq. (5)) for studied ILs. The number of viscosity data points is the same as in Table 4.
Ionic liquid a 103.b/MPa−1 10-8.c/K3 10-5.d/K3.MPa−1 e/K3.MPa−2 R2 %AARD

[C2mim][C2H5SO4] 0.027437 1.7075 1.1895 1.9434 −126.96 0.99874 2.27

[C2mim][CF3SO3] 0.0061845 2.9924 1.0000 1.5893 −226.26 0.99974 0.79
[C2mim][Tf2N] 0.0089860 6.1668 0.91620 0.92125 13.566 0.99466 3.02
[C4mim][Tf2N]a −0.25959 3.3395 1.1085 2.3922 −366.10 0.99996 0.27
[C4mim][Tf2N]b −0.29543 2.3664 1.1244 2.5167 −157.02 0.99988 0.81
[C6mim][Tf2N] −0.43751 3.0339 1.2362 2.3791 −182.34 0.99984 0.83
[C10mim][Tf2N] −0.48481 4.3968 1.3690 2.4567 −408.03 0.99985 0.92
[C4mim][BF4] −0.49505 1.6522 1.3767 2.4118 −117.96 0.99993 1.00
[C6mim][BF4] −0.53832 −1.5191 1.5490 3.8183 −261.59 0.99966 1.38
[C8mim][BF4] −0.45509 2.6977 1.6668 2.6695 −210.22 0.99998 0.37
[C4mim][PF6]a −0.38063 2.7745 1.5877 2.9547 −122.67 0.99949 1.54
[C4mim][PF6]c −0.084782 3.2014 1.4977 3.0512 −268.75 0.99641 5.97
[C6mim][PF6]d −0.51926 0.55181 1.7843 3.8741 −265.54 0.99962 1.51
[C6mim][PF6]b 0.26490 0.65190 1.5047 3.9130 −170.07 0.99461 6.18
[C8mim][PF6] −0.55774 6.1968 1.8933 1.8496 1695.0 0.99998 0.40
[C4mpyrr][CF3SO3] −0.089294 2.8683 1.3719 2.8362 −246.02 0.99993 0.59
[C4mpyrr][Tf2N] 0.056927 3.3801 1.1213 2.7166 −236.87 0.99888 5.39
[C1OC2mpyrr][Tf2N] 0.16327 3.2645 0.99069 2.4994 –222.70 0.99943 1.50
[C3py][BF4] −0.90837 0.15021 1.4866 2.7150 −238.97 0.99943 1.87
[C4py][BF4] −1.03659 0.59699 1.6307 2.7129 −200.44 0.99956 1.75
[C42mpy][BF4] −1.03954 1.2517 1.7428 2.8055 155.27 0.99964 1.19
[C43mpy][BF4] −1.17344 1.0043 1.6964 2.9853 −55.038 0.99980 1.27
[C44mpy][BF4] −1.40803 0.38384 1.7739 3.3972 10.757 0.99935 2.53
[C83mpy][BF4] −0.94011 1.8749 1.8753 3.1299 −256.38 0.99982 1.19
[C4py][CF3SO3] −0.81358 3.2490 1.5415 2.1352 29.669 0.99825 1.67
[C43mpy][N(CN)2] −0.54108 0.35650 1.0637 2.0099 −165.96 0.99970 0.85
[C43mpy][Tf2N] −0.38254 2.8580 1.2096 2.6427 −172.51 0.99982 0.70
[N4,1,1,1][Tf2N] −0.31757 2.6232 1.3142 3.0787 −170.39 0.99990 0.65
Overall 1.73

a
Ref. [22].
b
Ref. [17].
c
Ref. [18].
d
Ref. [20].

Table 6
Fitting parameters, R2 and %AARD of the modified VFT equation (Eq. (6)) for studied ILs. The number of viscosity data points is the same as in Table 4.
Ionic liquid a' 103.b' /MPa−1 c ' /K d' /K.MPa−1 103.e' /K.MPa−2 To/K R2 %AARD

[C2mim][C2H5SO4] 0.16975 1.9024 320.51 0.52728 −0.35566 227.48 0.99994 0.45

[C2mim][CF3SO3] −2.0563 −0.053530 924.74 1.4205 −1.1064 139.48 0.99992 0.40
[C2mim][Tf2N] −1.6193 4.4801 752.53 0.76938 0.009191 150.01 0.99536 2.87
[C4mim][Tf2N]a −1.6849 0.58009 728.22 1.5244 −1.7036 168.47 0.99998 0.18
[C4mim][Tf2N]b −1.7021 −1.0035 738.05 1.6895 −0.71284 167.20 0.99994 0.48
[C6mim][Tf2N] −2.5493 −0.67289 980.92 1.8325 −0.96493 153.37 0.99985 0.77
[C10mim][Tf2N] −3.2247 0.42728 1222.0 2.0296 −2.2332 143.54 0.99989 0.80
[C4mim][BF4] −2.0756 −1.5834 865.28 1.5765 −0.47030 170.10 0.99999 0.37
[C6mim][BF4] −2.7852 −6.6271 1100.6 2.6454 −1.2625 162.15 0.99966 1.38
[C8mim][BF4] −3.0715 −0.88392 1247.1 1.8962 −1.0214 158.14 0.99998 0.32
[C4mim][PF6]a −1.2598 1.1342 709.16 1.3133 −0.33726 195.72 0.99996 0.41
[C4mim][PF6]c 0.42529 4.0236 383.84 0.74666 −0.47418 224.47 0.99866 3.53
[C6mim][PF6]d −5.3140 −6.6597 2040.9 3.8182 −2.1001 121.09 0.99986 0.81
[C6mim][PF6]b −4.2695 −7.5933 1897.7 4.2107 −1.2148 112.5 0.9971 4.47
[C8mim][PF6] −3.2431 3.0841 1329.3 1.3772 8.0428 162.87 0.99999 0.37
[C4mpyrr][CF3SO3] −1.9181 −0.39104 920.55 1.8228 −1.1459 166.92 0.99994 0.53
[C4mpyrr][Tf2N] 0.22605 3.7459 294.52 0.71812 −0.65956 228.81 0.99991 0.65
[C1OC2mpyrr][Tf2N] 0.046453 3.0010 319.91 0.80369 −0.68689 217.64 0.99997 0.31
[C3py][BF4] −2.3339 −2.3256 862.69 1.5569 −1.0541 175.24 0.99969 1.35
[C4py][BF4] −2.4924 −1.7314 918.42 1.5130 −0.84930 177.14 0.99989 0.80
[C42mpy][BF4] −3.4896 −2.8340 1215.5 1.9823 0.68515 163.51 0.99965 1.64
[C43mpy][BF4] −3.1064 −2.4343 1066.4 1.8748 −0.13398 169.98 0.99995 0.58
[C44mpy][BF4] −2.5867 −1.8676 897.52 1.7187 0.032606 183.73 0.99992 0.84
[C83mpy][BF4] −4.0079 −3.3775 1445.4 2.4358 −1.3287 155.60 0.99981 1.20
[C4py][CF3SO3] −1.1735 2.7390 581.04 0.80704 0.091387 205.04 0.99847 1.50
[C43mpy][N(CN)2] −1.8763 −2.0779 695.67 1.3004 −0.75463 167.99 0.99979 0.75
[C43mpy][Tf2N] −2.5340 −1.3182 992.44 2.0859 −0.98398 150.22 0.99984 0.67
[N4,1,1,1][Tf2N] −1.8773 −0.71230 822.27 1.8794 −0.76813 172.27 0.99992 0.62
Overall 1.04

a
Ref. [22].
b
Ref. [17].
c
Ref. [18].
d
Ref. [20].

12
L. Darabi and M. Zare Chemical Physics 539 (2020) 110933

Table 7
Fitting parameters, R2 and %AARD of Eq. (7) for studied ILs. The number of viscosity data points is the same as in Table 4.
Ionic liquid A/mPa.s B/K C/K D E0/MPa E1/MPa 102.E2/MPa R2 %AARD

[C2mim][C2H5SO4] 0.18649 790.62 171.98 3.3020 −9374.1 56.567 −8.1113 0.99892 1.59
[C2mim][CF3SO3] 0.096869 1027.8 129.88 4.8149 −4240 26.758 −3.6039 0.99992 0.41
[C2mim][Tf2N] 0.0049672 2593.5 0.99562 85.867 164,110 −970.57 151.96 0.99870 1.41
[C4mim][Tf2N]a 0.14448 806.57 160.59 4.4137 −1916.7 11.791 −1.4054 0.99997 0.21
[C4mim][Tf2N]b 0.16950 756.63 165.64 8.0853 −295.49 0.79673 0.81177 0.99993 0.54
[C6mim][Tf2N] 0.39259 515.26 198.99 16.131 16,697 −104.98 18.033 0.99963 1.28
[C10mim][Tf2N] 0.020227 1468.0 127.15 4.7677 −2674.2 16.932 −2.2808 0.99994 0.59
[C4mim][BF4] 0.12284 870.95 169.67 10.157 46.229 −2.8442 1.9429 0.99997 0.51
[C6mim][BF4] 0.022166 1448.6 139.27 6.9739 −4441.2 24.197 −2.5168 0.99972 1.07
[C8mim][BF4] 0.041727 1282.4 155.79 7.066 −460.26 2.1196 0.41459 0.99997 0.39
[C4mim][PF6]a 0.182099 830.68 185.1 27.711 −22353 135.1 −18.030 0.99999 0.24
[C4mim][PF6]c 1.3376 411.09 221.15 12.932 −6831.6 41.664 −5.2739 0.99867 3.47
[C6mim][PF6]d 0.0002649 3410.8 61.491 5.3101 −3505.5 20.565 −2.5908 0.99978 0.88
[C6mim][PF6]b 0.0013568 2930.1 65.230 9.8199 7542.7 −47.997 8.3653 0.99870 3.06
[C8mim][PF6] 0.033540 1377.3 160.13 1732.6 −924153 5991.7 −833.64 0.99999 0.37
[C4mpyrr][CF3SO3] 0.14066 938.11 165.73 14.099 −939.94 4.8444 0.66972 0.99983 0.88
[C4mpyrr][Tf2N] 0.16461 820.82 164.83 4.8995 −6148.9 37.324 −5.2603 0.99869 2.16
[C1OC2mpyrr][Tf2N] 0.20204 743.59 165.6 5.6308 −6179.6 38.24 −5.4012 0.99827 2.23
[C3py][BF4] 0.091822 888.27 174.41 4.6284 −1842.0 10.180 −0.83780 0.99969 1.31
[C4py][BF4] 0.074177 938.07 176.38 8.6191 −4398.7 27.388 −3.3194 0.99987 0.85
[C42mpy][BF4] 0.0047457 1825.9 130.18 12.69 −27680 174.84 −26.409 0.99961 1.19
[C43mpy][BF4] 0.035088 1148.7 166.01 34.258 −9573.6 54.431 −4.2920 0.99992 0.59
[C44mpy][BF4] 0.060792 948.65 180.39 19.347 −4781.5 26.857 −2.0147 0.99990 0.88
[C83mpy][BF4] 0.027940 1306.5 163.40 4.0469 2076.9 −13.946 2.6490 0.99974 1.43
[C4py][CF3SO3] 0.57989 448.66 218.38 11.748 4034.0 −26.476 0.054558 0.99833 1.52
[C43mpy][N(CN)2] 0.093612 855.07 151.59 2.9752 −4200.9 25.040 −3.2630 0.99979 0.80
[C43mpy][Tf2N] 0.16273 763.26 170.94 8.9644 2904.0 −18.764 3.8142 0.99978 0.77
[N4,1,1,1][Tf2N] 0.16474 808.69 172.99 16.819 −2629.8 14.118 −0.44610 0.99989 0.70
Overall 1.12

a
Ref. [22].
b
Ref. [17].
c
Ref. [18].
d
Ref. [20].

Fig. 7. Average absolute relative deviations (% AARD) for all correlations
studied in this work.
studied over a wide pressure range. Eq. (8) can be presented as a two-
parameter equation (A and B) with a universal exponent (ϕ = 0.3). A
three-parameter equation is obtained if the ϕ exponent in Eq. (8) is
allowed to float. Eq. (8) can accurately describe the viscosity pressure
dependence of the various ILs over a wide pressure range. In addition, a
new equation (Eq. (11)) has been proposed to incorporate both the
temperature and pressure dependence of the viscosity of ILs. It has been
demonstrated that the proposed η–T–p model can accurately describe
the experimental viscosity data of ILs over a wide range of pressures
and temperatures. The proposed equations combine simplicity and ac­
curacy. It seems that the simple and accurate models proposed in this
work can be used for the estimation of ILs viscosity based on the group
contribution method and/or the quantitative structure–property re­
lationship approach. Finally, the parameters of the proposed equation
(Eq. (11)) were used to determine the pressure–viscosity coefficients of
the studied ILs. The pressure–viscosity coefficient of 1-alkyl-3-methy­
limidazolium ionic liquids increases with increasing alkyl chain length
of the cation.

4. Conclusions
CRediT authorship contribution statement

A new equation (Eq. (8)) has been proposed to represent the pres­
Leila Darabi: Investigation, Data curation, Formal analysis.
sure dependence of the viscosity of ILs. The performance and accuracy
Morteza Zare: Conceptualization, Supervision, Project administration,
of this proposed equation for imidazolium-, pyridinium-, pyrrolidi­
Validation, Methodology, Writing - original draft, Writing - review &
nium-, ammonium-based ILs with a wide variety of anions have been
editing.

13
L. Darabi and M. Zare Chemical Physics 539 (2020) 110933

processing, AIChE J. 47 (2001) 2384–2389.

Fig. 8. Pressure-viscosity coefficient, as a function of pressure at different
temperatures for (a) [C4mpyrr][Tf2N] and (b) [C2mim][C2H5SO4]. (■)
313.15 K, (▲) 343.15 K, (●) 363.15.
Declaration of Competing Interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influ­
ence the work reported in this paper.
Acknowledgments
We are indebted to the Research Council of Shahid Chamran
University of Ahvaz for financial supports in this scientific research
(Grant number: SCU.SC98.202). We thank Prof. M. H. Ghatee and Dr.
M. Bamdad for useful discussions.
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://
doi.org/10.1016/j.chemphys.2020.110933.
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