J Am Oil Chem Soc (2014) 91:10651075
DOI 10.1007/s11746-014-2450-1
ORIGINAL PAPER
Investigation of Some Physicochemical Properties of Mixtures
of Morama Seed Oil with (C6C9) n-Alkanes at 298.15
and Atmospheric Pressure
S. O. Yeboah I. Oathotse W. A. A. Ddamba
Received: 25 October 2013 / Revised: 21 February 2014 / Accepted: 4 March 2014 / Published online: 2 April 2014
AOCS 2014
Abstract Densities q, ultrasonic speeds u and dynamic
viscosities g, of mixtures of morama, Tylosema esculen-
tum, seed oil with n-hexane, n-heptane, n-octane and
n-nonane were determined over the entire composition
range at 298.15 K and atmospheric pressure. Excess molar
volumes, VmE , excess molar free volumes VfE , deviations in
isentropic compressibility, Djs, deviations in ultrasonic
speed, Du, deviations in viscosity, Dg, and the excess free
energy of activation of viscous flow, DG*E, were calcu-
lated therefrom and correlated by the RedlichKister
equation for each of the [morama seed oil ? (n-hexane or
n-heptane or n-octane or n-nonane)] mixtures. The results
have been discussed in terms of possible intermolecular
interactions and structural effects.
Keywords n-Alkanes  Excess molar volume  Excess
molar free volume  Dynamic viscosity  Isentropic
compressibility  Excess free energy of activation of
viscous flow  Morama  Tylosema esculentum
Introduction
The morama, Tylosema esculentum, seed oil is light
yellowish oil, which is much acclaimed due to its fine
organoleptic properties and its good oxidative stability
at ambient temperatures. The oil is highly cherished by
S. O. Yeboah (&)  I. Oathotse  W. A. A. Ddamba (&)
Department of Chemistry, University of Botswana, Gaborone,
Botswana
e-mail: yeboahso@mopipi.ub.bw
W. A. A. Ddamba
e-mail: ddambawa@mopipi.ub.bw
the communities in the Kalahari region of southern
Africa where it is extracted from the morama bean by
traditional methods, e.g., by boiling the pounded seeds
in water and skimming the oil at the top. The oil is
widely used for cooking and also for making butter.
Reported physicochemical parameters of the morama oil
such as iodine value (IV), acid value (AV), and
saponification value (SV), peroxide value (PV), refrac-
tive index and density collectively described morama oil
as composed of medium chain-length fatty acids (C16/
C18) with medium unsaturation and favourable oxida-
tive and hydrolytic stability [13]. Analysis of the lipid
classes showed the morama seed oil to be mainly made
up of non-polar lipids, with triacylglycerol (TAG) being
the predominant lipid class [1]. GCMS determination
of the fatty acid composition of morama oil showed
morama oil to be typically oleic, with oleic acid content
in the range 4553 %. Other major fatty acid compo-
nents are linoleic acid (2125 %), palmitic acid
(1216 %) and stearic acid (79 %) [1, 3, 4]. This fatty
acid composition of morama oil closely resembles that
of olive oil, both of which contain small but measurable
amounts of long chain fatty acids like C20:0, C22:0 and
C22:1. Analysis with a high resolution MS technique,
ESI-FTICR-MS, indicated that morama oil is made up
of seven major triacylglycerol classes, chief among
which are C54:4, C54:3 and C52:3. The 13C NMR ana-
lysis revealed that the sn-2 position of the glycerol
backbone is 100 % occupied by oleoyl and linoleoyl
acyl chains [1, 2]. Thus, triacylglycerol molecules such
as triolein (OOO) will be predominantly present in the
morama oil. This makes morama oil nutritionally a good
monounsaturated oil, as the structure of the triacyl-
glycerol molecules makes the unsaturated fatty acids
readily available for metabolism.
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The socio-economic importance of the morama seed oil
has attracted attention in the southern African region.
Currently a number of agricultural research groups are
working on the domestication of the morama plant for
possible large scale production, whilst the quality, stability
and the chemistry of the morama seed oil is under intense
investigation in our laboratories. Oil yield from the mora-
ma bean has been reported to be 3648 % [1, 3], which is
about two-fold higher than the oil output from soybean and,
thus, makes morama oil an attractive candidate for com-
mercial exploitation.
Morama oil contains modest amounts of phytosterols
and tocopherols, both being higher in morama oil than
in olive oil [2]. The total phytosterol content of the
morama oil has been reported to be 150 lg/g, with
b-sitosterol, stigmasterol and campesterol being the
major phytosterols [2]. It is worth noting that these
phytosterols have been attributed with favourable bio-
active properties such as prevention of cancer and
lowering of total plasma cholesterol [4, 5]. Total tocol
content of the morama oil has been reported as about
200 lg/g, which is mainly made up of c-tocopherol and
a-tocopherol, both being strong antioxidants [2, 4].
Thus, overall, morama oil is nutritionally and health-
wise wholesome and, hence, the keen interest in trying
to develop it into a commercial commodity.
Edible oil processing widely applies organic solvents
for different purification and treatment procedures such
as de-acidification and winterization. Despite their
application in various industrial scale purification pro-
cedures, experimental data on the physico-chemical and
thermodynamic properties of edible oil mixtures with
potential separation solvents using environmentally
friendly procedures of extraction are rare in the litera-
ture. In our systematic investigation of the thermody-
namic, acoustic and transport properties, we measured
density, q, ultrasonic speed u and dynamic viscosity g,
of binary systems of the morama seed oil with n-hexane,
n-heptane, n-octane and n-nonane at 298.15 K over the
entire mole fraction range of the mixtures investigated.
These experimental data have been used to calculate the
excess molar volumes, VmE , excess molar free volume,
VfE , deviations in ultrasonic speed, Du, deviations in
isentropic compressibility, Djs, deviations in viscosity,
Dg, and the excess free energy of activation of viscous
flow, DG*E. The calculated excess or deviation func-
tions: (VmE , VfE , Djs, Du, Dg, DG*E), have been fitted to
the RedlichKister polynomial equation [6]. The varia-
tion of these functions with composition at 298.15 K are
discussed in terms of non-specific molecular interaction
in the [morama seed oil ? (C6C9) n-alkane] binary
systems.
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J Am Oil Chem Soc (2014) 91:10651075
Materials and Methods
Materials
Analytical reagent grades of n-hexane, n-heptane,
n-octane and n-nonane were used, and were purchased
from Aldrich Chemicals. The n-alkanes were fractionally
distilled and stored over 0.4 nm molecular sieves for
60 h to remove any water content. The mass fraction
purities that were tested by gas chromatography were: n-
hexane ([99 %), n-heptane ([99 %), n-octane
([99.6 %) and n-nonane ([98.5). The purity of the four
n-alkanes was tested by comparing their densities q,
speeds of sound, u, and dynamic viscosities, g at
298.15 K, with reported literature data in Table 1, which
also includes our measured values of these quantities. It
can be observed from Table 1 that the measured values
of q, u and g were in good agreement with the literature
data [712]. Benzene (Aldrich Chemicals, p.a.) used for
the densimeter calibration was purified as reported
elsewhere [7]. Water was first de-ionized by means of
ion exchange resins and then triply distilled over KMnO4
under nitrogen. Its conductivity was always less than
1.0 9 10-6 S cm-1. All purified organic solvents were
stored in brown glass bottles and fractionally distilled
and degassed immediately before preparation of binary
mixtures. The morama seed oils used in this investiga-
tion were obtained by solvent extraction [2], and were
analyzed by means of a gas chromatograph Thermo-
Quest Voyager capillary GCMS model coupled to a
ThermoQuest Trace GC 2000 SERIES detector (San
Jose, California, USA). The details of the procedure for
the chromatographic analysis were described in previous
works [1]. The fatty acid composition obtained: oleic
acid, 47.27 %; linoleic acid, 23.40 %; palmitic acid,
12.93 %; stearic acid, 8.82 %; arachidic acid, 3.31 %;
erucic acid, 2.63 %; behenic acid, 1.03 % and arachi-
donic acid, 0.61 %; the uncertainty in mol % for these
analyses were better than 0.06. The calculated average
molar mass of the morama seed oil used in this study
was 850.34 g mol-1. The variation in the composition
between different oil samples affects mainly the mono-
unsaturated and polyunsaturated fatty acids, the change
in molar mass being lower than 3 g mol-1.
Measurement of Physicochemical Properties
Solution Density
Density measurements were performed at atmospheric
pressure with an Anton Parr DMA 4500 vibrating-tube
precision densimeter, thermostated at 298.15 K. The
J Am Oil Chem Soc (2014) 91:10651075 1067

Table 1 Values of density q, ultrasonic velocities u, and dynamic viscosities g for pure liquids at T = 298.15 K
Liquid qexp (kg m-3) qlit (kg m-3) uexp (m s-1) ulit (m s-1) gexp (mPa s) glit (mPa s)

n-C6H14 655.07 654.84a 1,081.7 1,077.7b 0.3113 0.2942a

b,c
655.07 0.3130b
0.2950c
n-C7H16 679.57 679.46a 1,135.1 1,130e 0.3950 0.3967a
d f
679.55 1,129.8 0.3950c
a d
n-C8H18 698.62 698.62 1,174.4 1,172.2 0.5145 0.5151a
c
698.59 0.5150c
a d
n-C9H20 713.99 713.75 1,210.7 1,207 0.6695 0.6690a
714.01c 0.6650c
MO 909.32 1,459.5 78.1916
a
Ref. [7]
b
Ref. [8]
c
Ref. [9]
d
Ref. [10]
e
Ref. [11]
f
Ref [12]

densimeter was first calibrated with ultra pure water and
benzene [1315] as reference liquids. The [morama seed
oil ? (n-hexane or n-heptane, or n-octane or n-nonane)]
binary mixtures were prepared by weighing appropriate
amounts of the purified morama seed oil and n-alkane on
a Sartorius Supermicro balance (Fabr.-Nr., Dm = 10-6
g) by syringing each component into Teflon stoppered
flasks in order to minimize preferential evaporation of the
alkane. Pure components were separately degassed by
ultrasound shortly before sample preparations. This pro-
cedure eliminated possible changes in mixture composi-
tion that could occur during the degassing of already
prepared binary mixtures. The uncertainty in solution
composition expressed as mole fraction was found to be
less than 8 9 10-5. A sample volume of not more than
1.0 cm3 was needed to fill the densimeter cell, and ther-
mal equilibrium was attained quickly at each temperature.
The temperature of the sample was controlled electrically
by means of a built-in thermostat (a semiconductor Peltier
element and a resistance thermometer temperature control
system) and was measured with an accuracy of 0.01 K.
The densimeter was calibrated after each set of four
sample measurements to offset any problem of instrument
drift. There was, however, no noticeable drift in the
density of the reference fluid and a linear relation between
the density of the fluid and the square of the vibrating
period s, (q = A ? Bs2), was assumed. Buoyancy cor-
rections to the weight were made by taking into account
the air density, the barometric pressure, and the relative
humidity. Under such conditions quadruplet density
measurements of each sample were reproducible to
within 0.01 kg m-3.
Ultrasonic Speeds
The ultrasonic speeds were measured with an uncertainty
of 0.3 % using a single-crystal variable-path ultrasonic
interferometer (Mittal Enterprises, New Delhi, India),
which was first calibrated with triply distilled water
(Table 1). The temperature was maintained to with-
in 0.01 K by circulating thermostated water around a
steel cell fitted with a quartz crystal of 1 MHz. In order to
minimize the uncertainty in the wavelength measurements,
the number of measured maxima, n, was recorded against
the total distance, d, covered by the reflector. Each maxi-
mum was recorded with the highest swing of the needle on
the micrometer scale for maximum sensitivity. The total
distance, d, is given by:
d nk=2; 1
where k is the wavelength. All plots of d vs n generated
were linear (r2 = 1) with a slope of k/2. The frequency of
the cell single-crystal, m being accurately known (1 MHz),
the speed of sound, u, is calculated by using the relation:
u km: 2
Each ultrasonic speed value presented in Tables 1 and 2
represents an average of u values deduced from four
independently determined k/2 values for pure components
and [MO ? n-alkane] binary compositions.
Dynamic Viscosity
Dynamic viscosity, g-values of the pure liquids and their
binary mixtures were measured at 298.15 K using an

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1068 J Am Oil Chem Soc (2014) 91:10651075

Table 2 Densities, speeds of sound, deviation in speed of sound, of viscous flow and molar free volume for [(C6C9) n-alkane
deviation in isentropic compressibility, excess molar volumes, (1) ? MO (2)] binary systems at 298.15 K
deviation in dynamic viscosity, excess Gibbs free energy of activation
X2 q (kg m-3) u (m s-1) Du (m s-1) 1010 9 Djs (m2 N-1) 106 9 VmE (m3 mol-1) Dg (mPa s) DG*E (J mol-1) 106 9 VfE (m3 mol-1)

MO ? n-hexane
0.0040 662.71 1,093.8 10.59 -0.403 -0.1182 -0.1266 1,139 -0.0134
0.0062 667.11 1,100.0 15.95 -0.609 -0.2457 -0.1915 1,617 -0.0175
0.0081 670.70 1,106.2 21.45 -0.799 -0.3545 -0.2458 1,950 -0.0255
0.0106 675.48 1,112.2 26.50 -0.995 -0.5047 -0.3203 2,336 -0.0305
0.0142 681.57 1,117.0 29.93 -1.175 -0.6035 -0.4286 2,796 -0.0615
0.0164 685.31 1,124.2 36.31 -1.372 -0.7025 -0.4943 3,031 -0.0752
0.0211 692.68 1,129.8 41.26 -1.570 -0.8101 -0.6396 3,470 -0.0862
0.0252 698.92 1,132.8 43.11 -1.698 -0.9585 -0.7646 3,780 -0.0976
0.0313 707.60 1,147.5 53.98 -2.067 -1.1175 -0.9563 4,172 -0.1100
0.0359 713.88 1,152.5 57.22 -2.217 -1.2455 -1.1039 4,423 -0.1200
0.0407 720.10 1,158.4 61.33 -2.377 -1.3985 -1.2560 4,646 -0.1409
0.0499 730.95 1,182.0 81.45 -2.861 -1.5876 -1.5552 5,009 -0.1576
0.0601 741.84 1,192.9 88.48 -3.100 -1.7628 -1.8925 5,332 -0.1679
0.0714 752.77 1,205.4 96.71 -3.341 -1.9598 -2.2691 5,616 -0.1818
0.0807 760.92 1,212.6 100.42 -3.473 -2.1113 -2.5785 5,805 -0.1972
0.0899 768.39 1,228.7 113.02 -3.717 -2.2288 -2.8909 5,966 -0.2037
0.1021 777.24 1,242.7 122.42 -3.910 -2.3413 -3.3004 6,140 -0.2124
0.1526 805.81 1,274.3 134.96 -4.201 -2.5267 -4.9651 6,569 -0.2355
0.2025 826.06 1,310.9 152.69 -4.406 -2.6293 -6.4795 6,712 -0.2447
0.3004 852.35 1,354.2 158.99 -4.280 -2.5217 -8.7823 6,581 -0.2363
0.3993 869.33 1,390.4 157.84 -3.948 -2.3011 -9.9674 6,126 -0.2128
0.5088 882.19 1,411.4 137.47 -3.345 -2.0046 -9.9031 5,374 -0.1727
0.6013 890.05 1,422.3 113.44 -2.752 -1.6726 -8.8925 4,579 -0.1401
0.6991 896.50 1,431.8 85.98 -2.094 -1.3145 -7.1504 3,607 -0.1024
0.8046 902.01 1,439.0 53.31 -1.349 -0.9415 -4.8390 2,432 -0.0704
0.9023 906.02 1,448.7 26.11 -0.674 -0.4869 -2.5495 1,249 -0.0394
MO ? n-heptane
0.0041 685.99 1,137.8 1.36 -0.135 -0.1159 -0.0652 1,206 -0.0113
0.0062 689.01 1,141.5 4.39 -0.244 -0.1548 -0.0986 1,635 -0.0148
0.0081 691.68 1,145.9 8.19 -0.360 -0.1897 -0.1292 1,962 -0.0216
0.0105 695.01 1,149.4 10.89 -0.464 -0.2143 -0.1699 2,330 -0.0258
0.0142 699.88 1,153.5 13.78 -0.593 -0.2313 -0.2339 2,798 -0.0520
0.0162 702.54 1,155.7 15.34 -0.662 -0.2792 -0.2682 3,008 -0.0637
0.0183 705.43 1,159.8 18.76 -0.768 -0.3592 -0.3050 3,209 -0.0729
0.0211 708.92 1,163.3 21.34 -0.865 -0.3873 -0.3557 3,455 -0.0826
0.0304 719.97 1,186.8 41.84 -1.369 -0.5496 -0.5271 4,094 -0.0931
0.0352 725.31 1,192.5 45.98 -1.505 -0.6194 -0.6197 4,356 -0.1015
0.0403 730.61 1,196.6 48.44 -1.610 -0.6758 -0.7192 4,596 -0.1192
0.0506 740.56 1,208.5 56.97 -1.858 -0.7371 -0.9297 5,000 -0.1333
0.0601 749.03 1,217.9 63.30 -2.044 -0.8243 -1.1284 5,291 -0.1590
0.0702 757.43 1,227.6 69.66 -2.220 -0.9197 -1.3474 5,545 -0.1608
0.0803 765.08 1,240.1 78.94 -2.419 -0.9908 -1.5706 5,753 -0.1722
0.0901 771.96 1,253.7 89.36 -2.615 -1.0598 -1.7907 5,920 -0.1820
0.1035 780.90 1,272.7 104.01 -2.867 -1.2291 -2.0967 6,104 -0.1921
0.2013 825.04 1,321.5 121.11 -3.221 -1.5394 -4.3000 6,621 -0.2116
0.2964 850.20 1,356.5 125.23 -3.174 -1.5421 -6.0009 6,467 -0.2078
0.4012 868.22 1,387.6 122.35 -2.928 -1.4243 -6.9852 5,958 -0.1823
0.5020 880.20 1,410.4 112.47 -2.568 -1.2148 -6.9629 5,260 -0.1539
0.6029 889.19 1,423.8 93.10 -2.100 -1.0371 -6.1099 4,407 -0.1200
0.7004 895.86 1,434.7 72.39 -1.615 -0.8224 -4.7391 3,463 -0.0909
0.8002 901.26 1,443.7 49.01 -1.090 -0.4936 -3.0759 2,394 -0.0624
0.9001 905.66 1,448.7 21.61 -0.527 -0.2758 -1.4316 1,234 -0.0332

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Table 2 continued
X2 q (kg m-3) u (m s-1) Du (m s-1) 1010 9 Djs (m2 N-1) 106 9 VmE (m3 mol-1) Dg (mPa s) DG*E (J mol-1) 106 9 VfE (m3 mol-1)

MO ? n-octane
0.0042 704.02 1,179.3 3.69 -0.143 -0.0902 -0.0491 1,080 -0.0077
0.0060 706.14 1,183.0 6.88 -0.228 -0.1082 -0.0701 1,417 -0.0101
0.0080 708.47 1,185.9 9.21 -0.300 -0.1251 -0.0941 1,744 -0.0147
0.0102 710.99 1,190.3 12.98 -0.398 -0.1436 -0.1207 2,058 -0.0176
0.0141 715.22 1,193.0 14.59 -0.481 -0.1681 -0.1679 2,514 -0.0355
0.0168 718.24 1,195.7 16.50 -0.552 -0.2061 -0.2023 2,790 -0.0434
0.0184 719.99 1,198.3 18.64 -0.610 -0.2272 -0.2229 2,938 -0.0497
0.0202 721.87 1,201.5 21.34 -0.677 -0.2505 -0.2455 3,088 -0.0563
0.0302 731.93 1,214.1 31.08 -0.952 -0.3647 -0.3773 3,773 -0.0635
0.0355 736.81 1,220.0 35.49 -1.075 -0.4100 -0.4485 4,053 -0.0692
0.0406 741.51 1,228.2 42.22 -1.226 -0.4740 -0.5204 4,291 -0.0813
0.0506 749.89 1,234.9 46.09 -1.370 -0.5617 -0.6623 4,672 -0.0909
0.0603 757.38 1,240.9 49.31 -1.489 -0.6071 -0.8061 4,972 -0.1084
0.0699 764.31 1,248.5 54.17 -1.620 -0.6655 -0.9517 5,214 -0.1164
0.0800 771.15 1,264.4 67.18 -1.850 -0.7392 -1.1083 5,425 -0.1311
0.0901 777.35 1,270.2 70.12 -1.935 -0.7714 -1.2668 5,600 -0.1477
0.1008 783.59 1,276.2 73.07 -2.017 -0.8219 -1.4389 5,755 -0.1554
0.1501 807.25 1,301.3 84.12 -2.280 -0.9580 -2.2486 6,188 -0.1687
0.2003 825.45 1,331.0 99.48 -2.495 -1.0534 -3.0634 6,337 -0.1758
0.3020 851.03 1,365.2 104.71 -2.499 -1.0991 -4.4730 6,176 -0.1652
0.4016 867.71 1,391.6 102.69 -2.333 -1.0551 -5.3094 5,691 -0.1458
0.5061 880.13 1,412.6 93.91 -2.045 -0.9584 -5.4352 4,978 -0.1227
0.6006 888.59 1,423.8 78.16 -1.694 -0.8574 -4.8731 4,207 -0.0993
0.7023 895.64 1,433.3 58.67 -1.280 -0.6758 -3.6789 3,271 -0.0728
0.8054 901.25 1,442.7 38.69 -0.847 -0.4109 -2.1305 2,224 -0.0495
0.9011 905.55 1,445.5 14.21 -0.394 -0.1887 -0.7799 1,170 -0.0268
MO ? n-nonane
0.0046 718.74 1,213.0 1.17 -0.079 -0.0527 -0.0545 852 -0.0051
0.0064 720.62 1,214.0 1.72 -0.111 -0.0857 -0.0763 1,118 -0.0067
0.0080 722.33 1,215.9 3.21 -0.156 -0.1169 -0.0964 1,337 -0.0098
0.0107 724.97 1,218.8 5.44 -0.222 -0.1468 -0.1292 1,652 -0.0117
0.0141 728.15 1,223.0 8.79 -0.311 -0.1590 -0.1712 1,998 -0.0237
0.0162 730.02 1,225.7 10.98 -0.366 -0.1707 -0.1963 2,180 -0.0289
0.0181 731.81 1,228.3 13.09 -0.418 -0.1843 -0.2208 2,342 -0.0331
0.0206 733.98 1,230.1 14.27 -0.461 -0.1878 -0.2518 2,530 -0.0376
0.0300 741.93 1,235.7 17.53 -0.596 -0.2296 -0.3706 3,116 -0.0423
0.0354 746.31 1,240.0 20.48 -0.685 -0.2659 -0.4399 3,387 -0.0461
0.0408 750.47 1,245.9 25.05 -0.792 -0.2971 -0.5093 3,621 -0.0542
0.0503 757.49 1,252.9 29.68 -0.924 -0.3664 -0.6331 3,969 -0.0606
0.0601 764.22 1,260.0 34.35 -1.049 -0.4287 -0.7619 4,262 -0.0723
0.0702 770.7 1,266.0 37.84 -1.151 -0.4845 -0.8961 4,512 -0.0776
0.0808 777.06 1,274.0 43.20 -1.271 -0.5411 -1.0378 4,730 -0.0874
0.0900 782.22 1,280.2 47.10 -1.359 -0.5812 -1.1613 4,891 -0.0978
0.1006 787.92 1,287.0 51.26 -1.451 -0.6596 -1.3036 5,048 -0.1059
0.1504 809.85 1,309.8 61.69 -1.697 -0.7941 -1.9613 5,514 -0.1238
0.1999 826.61 1,330.2 69.77 -1.840 -0.8803 -2.5751 5,700 -0.1372
0.3016 851.09 1,363.1 77.37 -1.907 -0.9158 -3.5906 5,627 -0.1321
0.4041 867.72 1,386.6 75.37 -1.786 -0.8507 -4.1383 5,207 -0.1172
0.5001 879.03 1,405.6 70.47 -1.600 -0.7449 -4.1435 4,626 -0.0988
0.6042 888.4 1,423.3 62.27 -1.345 -0.6518 -3.6109 3,853 -0.0816
0.7024 895.22 1,433.8 48.34 -1.036 -0.4798 -2.7044 3,018 -0.0638
0.8514 903.22 1,442.5 19.97 -0.495 -0.2157 -1.0404 1,592 -0.0355

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1070
Ubbelohde viscometer. The viscometer was thoroughly
cleaned, perfectly dried and filled with sample liquid and
its limbs closed to minimize partial evaporation of the n-
alkane. The apparatus was submerged in a transparent
walled thermostatic water-bath at 298.15 K with a resolu-
tion of 0.05 K and allowed to stand for about 25 min to
attain thermal equilibrium. The viscometer was calibrated
to determine the two viscometer constants A and B in the
equation g qAt  B/t, by measuring efflux time t with
triply distilled water and cyclohexane. The efflux time for
the flow of a finite volume of liquid through the capillary of
the viscometer was measured with an electronic digital
stopwatch with a precision of 0.1 s. Four repetitions of
readings for the efflux time were measured for each pure
liquid or binary liquid mixture and the results were aver-
aged. The obtained parameters were: A = 4.7706 m2 s-2
and B = -1.9625 m2. The dynamic viscosity was repro-
ducible to within 2.0 9 10-3 mPa s.
Results and Discussion
Experimental density, q, ultrasonic speed, u, and
dynamic viscosity, g, for pure n-hexane, n-heptane,
n-octane, n-nonane and the morama seed oil (MO) at
298.15 K are listed in Table 1, together with the liter-
ature data. The agreement, within the experimental
uncertainties, between the measured and the literature
values confirmed the purity of the chemicals used as
well as the accuracy of the equipment and the experi-
mental procedure. The experimental values of q, u, and
g, with respect to the mole fraction x2 for the MO at
298.15 K and atmospheric pressure are listed in Table 2.
To the best of our knowledge, no data have been
reported previously for the density, ultrasonic speeds or
dynamic viscosity for any of the binary systems in the
present investigations.
Excess molar volumes, VmE , were calculated for each
[MO ? (C6C9) n-alkane] binary composition at 298.15 K
from density measurements using the following equation:
X n
VmE Vm  Vmid M=q  xi Mi =qi ; 3 wE x1 x2 R Ak 1  2x2 k ;
where M is the molar mass of the mixture, which is the
mole fraction weighted adduct of the molar masses of the
two pure components in each binary mixture. Vmid is the
ideal molar volume, q is the density of the mixture, and xi,
Mi and qi are, respectively, the mole fraction, the molar
mass and the density of the pure liquid component i.
The values of the deviations in isentropic compress-
ibility, Djs, for each binary system were calculated by
using the following standard relation:
123
J Am Oil Chem Soc (2014) 91:10651075
 
Djs js  x1 js;1 x2 js;2 4
where the subscripts 1 and 2 stand for the pure n-alkane
and MO, respectively. Assuming the absorption of the
acoustic wave is negligible, the value of js is calculated
from the NewtonLaplace equation:
 1
jS q  u2 : 5
The deviations of speed of sound, Du, were calculated
using the relation:
Du u  x1 u1 x2 u2 : 6
The deviations in dynamic viscosity, Dg, from linear
dependence and excess free molar volume, VfE , were cal-
culated by using the following relations:
Dg g  x1 g1 x2 g2 ; 7
 
VfE Vf;m  x1 Vf;1 x2 Vf;2 ; 8
where g is the dynamic viscosity of the binary mixture and
gi is the viscosity of pure component i, Vf,m and Vf,i rep-
resent molar free volume of the mixture and pure compo-
nent i, respectively.
The molar free volume can be estimated using the
relation:
Vf; Mu = kg3=2 ; 9
9
where k is a constant equal to 4.28 9 10 [16].
On the basis of the theory of absolute reaction rates [17],
the excess free energy of activation of viscous flow, DG*E,
was calculated by using the following equation:
DGE RT lngV  x1 lng1 V1  x2 lng2 V2 ; 10
where R is the universal constant of gases, T is the absolute
temperature, V and Vi are molar volumes of the binary
mixtures and pure component i, respectively.
The values of the functions: VmE , VfE , Djs, Du, Dg and
DG*E (Table 2) for each of the [MO ? (C6C9) n-alkane]
binary systems were least-squares fitted to the Redlich
Kister polynomial regressions [6]:
11
k0
where WE = VmE , VfE , Djs, Du, Dg and DG*E.
All points in the polynomial were weighted equally and
the regression coefficients Ak in Eq. (11) were evaluated by
the least-squares method. The estimated values of Ak
regression coefficients for the excess or deviation proper-
ties: (VmE , VfE , Djs, Du, Dg or DG*E) for each of the
[MO ? (C6C9) n-alkane] binary mixtures at 298.15 K are
listed in Table 3 along with the corresponding standard
deviations r(WE) defined by Eq. (12).
J Am Oil Chem Soc (2014) 91:10651075 1071

Table 3 Least squares fitted Ak coefficients of the RedlichKister polynomial Eq. 11 and corresponding standard deviations of the fits, r (WE),
for the [(C6C9) n-alkane (1) ? MO (2)] binary systems at 298.15 K
Excess property A0 A1 A2 A3 A4 A5 A6 r (WE)

MO ? n-hexane
106 9 VmE (m3 mol-1) -8.122 6.765 -4.295 -0.203 -11.466 14.459 0.027
1010 9 DjS (m2 N-1) -13.403 12.523 -16.287 0.247 31.793 22.178 -54.860 0.080
Du (m s-1) 557.14 -443.08 193.88 39.92 -159.22 -503.96 686.63 3.32
Dg (mPa s) -39.823 11.430 12.014 -9.966 1.336 -1.760 -3.135 0.004
*E -1
DG (kJ mol ) 21.37 -20.08 47.40 118.81 -359.02 -953.21 113.83 0.15
106 9 VfE (m3 mol-1) -0.704 0.781 -0.764 -0.135 0.757 1.230 -2.008 0.006
MO ? n-heptane
106 9 VmE (m3 mol-1) -4.862 3.846 -6.919 3.067 12.104 0.607 -13.794 0.030
10 2 -1
10 9 DjS (m N ) -10.302 8.115 -4.813 5.404 -11.700 9.239 0.054
Du (m s-1) 455.18 -273.60 -206.33 -221.62 1,879.48 -244.32 -1,696.69 3.49
Dg (mPa s) -27.888 9.013 13.638 -7.762 0.003
DG*E (kJ mol-1) 20.61 -21.17 52.88 143.89 -416.91 -1,114.2 1,344.44 0.15
6 3 -1
10 9 VfE (m mol ) -0.613 0.666 -0.612 -0.104 0.316 1.180 -1.380 0.006
MO ? n-octane
106 9 VmE (m3 mol-1) -3.874 1.911 -2.786 3.578 4.412 0.378 -6.659 0.013
10 2 -1
10 9 DjS (m N ) -8.278 7.125 -3.259 -1.973 -7.410 13.327 0.030
Du (m s-1) 376.10 -268.29 54.02 71.84 303.52 -436.59 -195.58 2.03
Dg (mPa s) -21.800 4.400 14.800 0.009
DG*E (kJ mol-1) 19.74 -19.17 434.05 104.87 -308.19 -836.02 971.85 0.12
106 9 VfE (m3 mol-1) -0.495 0.448 -0.380 0.607 -0.585 0.005
MO ? n-nonane
106 9 VmE (m3 mol-1) -3.044 2.302 -1.576 1.855 -0.464 0.025
1010 9 DjS (m2 N-1) -6.427 4.558 -3.092 2.515 -2.984 4.160 0.016
Du (m s-1) 282.81 -129.32 113.35 -222.12 -56.10 1.23
Dg (mPa s) -16.575 5.050 9.725 0.002
DG*E (kJ mol-1) 185.78 -8.07 6.66 -96.91 52.84 318.91 -62.82 0.14
106 9 VfE (m3 mol-1) -0.769 0.219 -4.254 6.380 21.880 -10.003 -30.861 0.003

X 2 1=2 molecules of the larger component, due to differences in

 E E E
r W Yexp  Ycalc = Nn ; 12
where N is the number of experimental data points and
n the number of the regression coefficients.
The variation of the excess molar volume, VmE , with
mole fraction of the MO, x2, for each of the [MO ? (C6
C9) n-alkane] binary systems are presented graphically in
Fig. 1. For each isotherm the solid line represents the fitted
curve calculated from the smoothing Eq. (11). It is
observed that the VmE values are negative over the entire x2-
range for all investigated [MO ? (C6C9) n-alkane] binary
systems, which in general indicates completely miscible
systems. The negative VmE values observed in each of the
[MO ? (C6C9) n-alkane] binary systems may partly be
resulting from structural effects. Structural effects result
from the geometrical interstitial accommodation of mole-
cules of the smaller component into cavities created by
molar masses, shape and molar free volumes of unlike pure
components. The molar volumes of n-hexane, n-heptane,
n-octane and n-nonane at 298.15 K are 1.3155 9 10-4,
1.4746 9 10-4, 1.6351 9 10-4 and 1.7963 9 10-4
m3 mol-1, respectively, compared with 9.3514 9 10-4
m3 mol-1 for MO. The corresponding differences in molar
volumes between MO and the n-alkanes at 298.15 K are:
n-hexane; 8.0359 9 10-4, n-heptane; 7.8768 9 10-4,
n-octane; 7.7163 9 10-4 and n-nonane; 7.5551 9 10-4
m3 mol-1, respectively. Thus, for each of the [MO ? (C6
C9)n-alkane] binary systems, the large molar volume dif-
ference between the mixing components would result in a
more efficient geometrical interstitial accommodation of
the smaller n-alkane molecules into voids created by larger
MO molecules. This leads to a contraction in volume,
resulting in negative VmE values for each of the
[MO ? (C6C9) n-alkane] binary systems. It is further

123
1072
106V Em / (m mol )
-1
3
X2
Fig. 1 Excess molar volume, VmE vs X2 for the [(C6C9) n-alkane
(1) ? MO (2)] binary mixtures: (open diamond) n-hexane; (filled
diamond) n-heptane; (open triangle) n-octane and (filled triangle) n-
nonane; at 298.15 K. The solid lines are from the appropriate
RedlichKister fitting Eq. 11
observed for all VmE vs x2 isotherms that the n-alkane rich
region (0.00 \ x2 \ 0.1) is characterized by a steep nega-
tive variation in VmE values, which supports the possibility
of enhanced structural effects in low x2. It is also noticeable
that the sequence of the algebraic value of the functions,
VmE (min), increases with the chain-length of n-alkane
molecules in the order: n-nonane [ n-octane [ n-hep-
tane [ n-hexane, with minimum values of isotherms shif-
ted towards the n-alkane-rich mole fractions.
Quantitative information on solutesolvent intermolec-
ular interactions can be obtained from the limiting excess
partial molar volumes, (ViE;1 ), of each component in the
mixture [1820]. We have, thus, used the RedlichKister
least squares fitting correlation coefficients, Ak, (Table 3)
to obtain values of the limiting excess partial molar vol-
umes for n-alkane, (V1E;1 ) and MO, (V2E;1 ) components in
each binary system using the relations below [1820];
X X
V1E;1 Ak  Ak x1 ! 0; 13
neven nodd
X nonane)] binary systems are highly negative over the entire
V2E;1 Ak x2 ! 0: 14
k
Negative ViE;1 values for both components in each of
the [MO ? (C6C9) n-alkane] binary systems were
obtained (Table 4). An explanation based on the hard-
sphere approach [21, 22] is that the negative ViE;1 values
result from the enhancement of the packing efficiencies and
geometric fits arising from the cage effects. Thus, the
solutesolvent interactions, either in the case of the solvent
123
J Am Oil Chem Soc (2014) 91:10651075
Table 4 Limiting excess molar volumes ViE;1 (m3 mol-1) for the
components in [(C6C9) n-alkane (1) ? MO (2)] binary systems at
298.15 K
n-hexane n-heptane n-octane n-nonane
106 9 V1E;1 -2.861 -6.027 -3.040 -1.776
(m3 mol-1)
106 9 V2E;1 -44.904 -21.206 -14.773 -9.200
(m3 mol-1)
being the n-alkane or MO, are stronger than the intermo-
lecular interactions in the pure components. The unusually
large negative V2E;1 values may be ascribed to the complete
rupture of both the intra-molecular and intermolecular
dipoledipole associations in the MO triglyceride molecules
in the infinite dilute solutions. The magnitude of negative
values of V2E;1 follow the order: MO ? n-hexane [ MO ?
n-heptane [ MO ? n-octane [ MO ? n-nonane, which
E
supports the observed trend in the Vm data.
Figures 2 and 3 display the experimental Djs vs x2 and
Du vs x2 for each of the [MO ? (C6C9) n-alkane] binary
systems investigated. The Djs values were negative over
the entire x2-range for all the binary mixtures and there is a
parallel in the qualitative trend of Djs curves with VmE
isotherms (Figs. 1, 2). The Du data, however, shows a
similar trend observed in Djs data but with opposite sign
for each binary system. Negative values of Djs and positive
values of Du suggest that each of the four [MO ? (C6
C9)n-alkane] binary systems is less compressible than the
corresponding ideal mixture, due to formation of a denser
molecular packing. Thus, the magnitude of negative Djs
values follow the order: MO ? n-hexane [ MO ? n-hep-
tane [ MO ? n-octane [ MO ? n-nonane with the
[MO ? n-hexane] system exhibiting least compressible
liquid compositions over the entire x2-range. A plausible
qualitative interpretation of the behaviour of these mixtures
with respect to composition has been suggested. Thus, for
each of the binary systems, the negative Djs values result
from geometrical interstitial accommodation of the small
n-alkane molecules into voids in larger MO molecules.
Figure 4 indicates that Dg vs x2 curves for each of the
four [MO ? (n-hexane or n-heptane, or n-octane or n-
x2-range at 298.15 K, in which the trend of changes in Dg
values is similar to that of VmE and Djs data (Figs. 1, 2). The
strongly negative Dg values for the four [MO ? (C6C9) n-
alkane] binary systems would imply that in each case the
mixture is less viscous than the corresponding ideal mix-
ture. The viscosity of MO is 251, 198, 152 and 117 times
larger than n-hexane, n-heptane, n-octane and n-nonane,
respectively. This is due to the stronger dipoledipole
intermolecular association in the triglyceride MO
J Am Oil Chem Soc (2014) 91:10651075
u / (ms )
-1
X2
Fig. 2 Deviations of speed of sound, Du vs X2 for the [(C6C9)
n-alkane (1) ? MO (2)] binary mixtures at 298.15 K. Symbols are
same as in Fig. 1
1010 k s / (m .N )
-1
2
X2
Fig. 3 Deviations in isentropic compressibility, Djs vs X2 for the
[(C6C9) n-alkane (1) ? MO (2)] binary mixtures at 298.15 K.
Symbols are same as in Fig. 1
molecules. When the n-alkane molecules are added, the
dipoledipole intermolecular associations in MO molecules
are broken resulting in loss of cohesive energy [23, 24].
Thus, the unlike interactions are weak compared to the like
interactions which result in a decrease in the g-values for
the binary mixtures. Large negative Dg values are also
observed for mixtures containing unlike components with a
big difference in their molecular sizes [24] in the case
between MO and each of the (C6C7) n-alkane molecules.
Large and positive DG*E values are observed over
the entire x2-range for each of the four [MO ? (C6C9)
1073
(mPa.s)
x2
Fig. 4 Deviations in dynamic viscosity, Dg vs X2 for the [(C6C9)
n-alkane (1) ? MO (2)] binary mixtures at 298.15 K. Symbols are
same as in Fig. 1
n-alkane] binary systems (Fig. 5). It can also be noticed
that the magnitude of the positive deviations increases with
decrease in chain length of the n-alkane molecules. Large
positive values of DG*E are attributed to the considerable
size and cohesive energy differences between the two
unlike components [25, 26] in the mixture. Thus, for
[MO ? (C6- C9) n-alkane] binary systems, the expected
negative values of DG*E are masked by the positive con-
tribution to DG*E which arises from the large size differ-
ence between MO and each of the (C6C9) n-alkane. This
observation illustrates the importance of free volume
effects in these binary systems. The positive magnitude of
DGEmax has been reported to be an increasing function of the
h i2
1=2 1=2
size difference function; V1  V2 [25]. Similar
results were reported for [monoalkylamine (butyl to
dodecyl) ? cyclohexane] [27] and [trialkylamine (butyl to
dodecyl) ? cyclohexane] [28].
Figure 6 represents the composition dependence of
excess molar free volumes, VfE , for the four [MO ? (C6
C9) n-alkane)] binary mixtures at 298.15 K. All the four VfE
vs x2 plots are negative over the entire x2-range and show a
trend which is similar to VmE , Djs and Dg data. A com-
parison of VmE and VfE data (Figs. 1, 6,) however, indicates
that the magnitudes of the two functions for each binary
system are different although the sign and sequence are the
same. Thus, the magnitude of the negative VfE -values
decrease as the size of n-alkane molecule increases. For
each binary mixture, negative VfE -values indicate closer
molecular packing due to the geometrical effects that result
in a more efficient interstitial accommodation of the
smaller n-alkane molecules in voids of the MO liquid
structure.
123
1074 J Am Oil Chem Soc (2014) 91:10651075

7000 solvents, which are frequently applied in the refining pro-

cedures of vegetable oils. In this paper the densities, speeds
6000
of sound and dynamic viscosities for the four [MO ? (C6
5000 C9) n-alkane] binary systems have been measured and are
reported over the entire composition range at 298.15 K and
G* / (J.mol )
-1

4000
atmospheric pressure. The excess volume VmE , deviations in
3000
the speed of sound Du, deviations in isentropic compress-
E

ibility Djs, deviations in dynamic viscosity Dg, excess free

2000 energy of activation DG*E for viscous flow and excess
molar free volume VfE were calculated from the experi-
1000
mental data and fitted to the RedlichKister polynomial
0 equation. Since the n-alkanes contain no polar functional
0 0.2 0.4 0.6 0.8 1 groups, the negative magnitudes in VmE and Djs functions
X2
arise from the geometrical interstitial accommodation of
Fig. 5 Excess free energy of activation of viscous flow, DG*E vs X2 the smaller n-alkane molecules into the morama liquid
for the [(C6C9) n-alkane (1) ? MO (2)] binary mixtures at 298.15 K. structure. The location of the minima of the VmE and Djs
Symbols are same as in Fig. 1 isotherms in the high n-alkane mole fraction region for all
binary mixtures suggests a more efficient geometrical
0
effect in the low morama oil compositions. The large
0 0.2 0.4 0.6 0.8 1 negative Dg and large positive DGE* values for each of the
{morama oil ? (C6C9) n-alkane} mixture over the entire
-0.05 composition range suggest that structural effects largely
determined the signs of VmE and Djs data. The results of this
-0.1 investigation have demonstrated good mixing properties of
106. Vf E,m / (m mol )
-1

the morama oil with (C6C9) n-alkane solvents in the

order: n-hexane [ n-heptane [ n-octane [ n-nonane as
3

-0.15 reflected in the attenuation of the negative magnitudes of

VmE and Djs values towards the longer n-alkane chain.
-0.2 Thus, for future possible large scale production and pro-
cessing of morama oil, the n-alkane solvents (especially n-
hexane) hold promise as good candidates for process
-0.25
application.

-0.3
Acknowledgments Financial support from the Office of Research
X2 and Development, University of Botswana, is gratefully acknowledged.

Fig. 6 Excess free molar volume, VfE vs X2 for the [(C6C9) n-alkane
(1) ? MO (2)] binary mixtures at 298.15 K. Symbols are same as in
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