Density, Speed of Sound, and Viscosity of Diethylene Glycol

Article pubs.acs.org/jced

Cite This: J. Chem. Eng. Data XXXX, XXX, XXX−XXX

Density, Speed of Sound, and Viscosity of Diethylene Glycol Monoethyl Ether + N,N‑Dimethylformamide (Ethanol, Water) at T = 288.15−318.15 K Seyyedeh Narjes Mirheydari,† Mohammad Barzegar-Jalali,‡ Behrang Golmohamadi,§ Hemayat Shekaari,§ Fleming Martinez,∥ and Abolghasem Jouyban*,⊥,# †

Drug Applied Research Center, Tabriz University of Medical Sciences, Tabriz, Iran Research Center for Pharmaceutical Nanotechnology and Faculty of Pharmacy, Tabriz University of Medical Sciences, Tabriz, Iran § Department of Physical Chemistry, Faculty of Chemistry, University of Tabriz, Tabriz, Iran ∥ Grupo de Investigaciones Farmacéutico-Fisicoquímicas, Departamento de Farmacia, Facultad de Ciencias, Universidad Nacional de Colombia − Sede Bogotá, Cra. 30 No. 45-03, Bogotá, D.C. Colombia ⊥ Pharmaceutical Analysis Research Center and Faculty of Pharmacy, Tabriz University of Medical Sciences, Tabriz, Iran # Kimia Idea Pardaz Azarbayjan (KIPA) Science-Based Company, Tabriz University of Medical Sciences, Tabriz, Iran

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‡

ABSTRACT: The density (ρ), speed of sound (u), and viscosity (η) of the binary mixtures of (diethylene glycol monoethyl ether (carbitol) and water, ethanol, N,N-dimethylformamide) have been measured in full concentration range at T = 288.15, 298.15, 308.15, and 318.15 K and p = 0.0868 MPa. Using the experimental data, the molar volume (Vm ), excess molar volume (VmE ), isentropic E ), compressibility (κs), excess molar isentropic compressibility (κs,m and viscosity deviation (Δη) were calculated. The most negative E values of VmE and κs,m and positive values of Δη obtained for the carbitol + water mixture are indicative of the strong interactions between different components relative to two other systems. The values of ρ, Vm , and κs for the studied mixtures were correlated E , and Δη were described by using the Jouyban−Acree model with high accuracy. Furthermore, the obtained values of VmE , κs,m the Redlich−Kister equation and reasonable standard deviations were obtained. organic solvents. It is used in printing and dyeing of fiber and fabrics as well as cosmetic and perfumery industries. Carbitol prevents the gel formation in detergent and cleaner formulation. In addition, it is used as a solubilizer in drilling and cutting coolants.2 Thermophysical property data and the mixing deviation from ideality of the systems containing carbitol are required to study the presence of molecular interactions and arrangements.7 Despite the wide application range of the carbitol, the studies on its physicochemical properties are limited to the binary mixture of carbitol + water at a limited temperature.2,8,9 Therefore, in the present work, the physicochemical properties of three binary mixtures of carbitol with water, ethanol and N,N-dimethylformamide (DMF) were investigated. For this purpose, the density (ρ), speed of sound (u), and viscosity (η) were measured at T = 288.15, 298.15, 308.15, and 318.15 K and p = 0.0868 MPa. The obtained data were used to calculate the molar volume (Vm ),

1. INTRODUCTION Glycol ethers are found to be able to dissolve different compounds by having etheric and alcoholic groups as well as hydrocarbon chain in their structures.1,2 They are very much important solvents in various industries specially pharmaceutical processing. Glycol ethers are known as scrubbing liquids for absorption of acid gases exhausting from industrial plants due to their attractive properties such as low vapor pressure, low toxicity, low viscosity, high chemical stability, and low melting point.1,2 They are also applied as octane number enhancer because of their pollution-reducing properties. Moreover, hydroxyethers with nonionic amphiphilic properties are effective surfactants with a large number of applications.3 Short chain polyethylene glycol monoalkyl ethers are used in biomedical processes including a simple model of biological systems.4 In recent years, the systems containing ethylene glycol ethers are used in pumps and chillers as heat absorbents.5,6 Moreover, they were also used as the polar additive in anionic polymerization and automotive brake fluid.5,6 Diethylene glycol monoethyl ether (carbitol), as a member of glycol ethers family is miscible with water and most of the © XXXX American Chemical Society

Received: November 1, 2018 Accepted: March 11, 2019

A

DOI: 10.1021/acs.jced.8b01012 J. Chem. Eng. Data XXXX, XXX, XXX−XXX

Journal of Chemical & Engineering Data

Article

excess molar volume (VmE ), isentropic compressibility (κs), E excess molar isentropic compressibility (κs,m ), and viscosity deviation (Δη), which were considered in terms of the interaction between different components. The obtained values E of (ρ, Vm, and κs) and (VmE , κs,m , and Δη) were described by the Jouyban−Acree and Redlich−Kister models, respectively.

3. RESULTS AND DISCUSSION 3.1. Density and Speed of Sound and Viscosity Data. The experimental values of ρ, u, and η data for the binary mixtures of carbitol + water, carbitol + ethanol, and carbitol + DMF are given in Tables 3−5. The values of ρ and u at T = 298.15 were compared with those reported in the literature and shown in Figure 1. As can be seen in this figure, the measured data are in agreement with the reported data.8,9 Figures 2−4 display the values of ρ, u, and η for the studied binary systems as a function of carbitol mole fractions. As can be seen in Figure 2, the values of ρ for the binary system of carbitol + water increase up to carbitol mole fraction (x1 = 0.1) and then decrease with an increase in the carbitol content which was similar to those presented by Li et al.,2 who reported the densities of this system at the other temperatures. In the two other systems, the ρ values of the mixtures increase with an increase in the carbitol content. Also, there is an inverse relationship between density and temperature (T). The densities of all mixtures were increased by decreasing the temperature. This phenomenon suggests that, with an increase in the temperature, the molecules give sufficient energy to move and increase the distance between the molecules and therefore the densities are decreased. According to the values of excess molar volumes given in Table 3, the strong polar−polar interactions are found between water and carbitol. With addition of 0.1 mol fraction of carbitol to water, the structure of water (hydrogen bond structure) is not changed and is maintained but addition of more than 0.1 mol fraction can change this structure gradually and the densities are reduced as a result of the increase in the distance between water molecules. Figure 3 shows the speed of sound for the binary mixtures versus carbitol mole fraction of the carbitol + water mixture. A similar trend with density is observed for this system, increasing the speed of sound up to carbitol mole fraction (x1 = 0.1) and after this point decreasing with an increase in the carbitol content. This trend was also observed in the reported data by Douhéreta and co-workers.9 In the mixture of carbitol and ethanol, the speed of sound increases with addition of the carbitol to the mixture, while the vice versa trend is observed for the carbitol + DMF mixture. Moreover, by increasing the temperature, the speed of sound of the mixture decreases while the inverse trend is observed for the density of carbitol in water (Figure 2a). The viscosities of the studied systems were also plotted against the carbitol mole fraction in Figure 4. By looking at this figure, it is observed that the viscosity of the mixture of carbitol and water increases quickly up to the carbitol mole fraction (x1 = 0.3) and then gradually decreases with the addition of carbitol to the mixture. This trend can be interpreted with help the results from excess molar volume (next section), which has the most negative value of VmE in this mole fraction. The viscosities of the carbitol + ethanol and carbitol + DMF systems increase with an increase in the carbitol mole fraction. By increasing the temperature, the viscosities of all studied systems decrease, which means that the mixtures flow better at higher temperatures. 3.2. Excess Molar Volumes. The values of VmE of the binary mixture were calculated using the following equation25,26

2. EXPERIMENTAL SECTION 2.1. Materials. The purity levels and sources of the chemicals used in this study are listed in Table 1. Double distilled water was used to prepare the aqueous systems. Table 1. Sample Description of the Chemicals Used chem name

CAS Registry No.

source

mass fraction purity

carbitol ethanol DMF

111-90-0 64-17-5 68-12-2

Merck (Germany) Scharlau Chemie (Spain) Merck (Germany)

>0.980 0.992 ≥0.998

2.2. Apparatus and Procedure. The solutions were provided in glass vials and mole fraction concentration by weighing using an analytical balance (Shimadzu, 321-34553, Shimadzu Co., Japan) with an uncertainty ±1 × 10−7 kg and closed firmly with parafilm. The densities and speeds of sound of the mixtures or pure components were measured with a vibrating tube densimeter (Anton Paar, DSA 5000 densimeter and speed of sound analyzer). The instrument was calibrated with doubly distilled deionized and degassed water and dry air at p = 0.0868 MPa. The speed of sound is measured by applying a propagation time technique. One transducer emits sound waves via the sample-filled cavity at a frequency of approximately 3 MHz; the second transducer takes these waves. Thus, u is obtained by dividing the known distance between transmitter and receiver by the measured propagation time of the sound wave.10 The temperature stability during measurements of densities and speeds of sound was kept fixed within ±10−3 K applying the Peltier device built in densimeter. The experimental uncertainties of ρ and u measurements were less than 0.2 kg m−3 and 0.5 m s−1, respectively. The viscosities were measured using an Ubbelohde-type viscometer, which was calibrated with absolute ethanol. The viscosities of the solutions (η) were obtained by the following equation10 η B = At − ρ t

(1)

where ρ is the density, t is the solution flow time, and A and B are the viscometer constants. A digital stopwatch with a resolution 0.01 s has been used for the measurement of the flow time. The estimated uncertainty of the experimental viscosity was ±0.025 mPa s. The experimental values of ρ, u, and η for the pure components were tabulated in Table 2; they were also compared with the available literature data3,9,11−32 and are almost in agreement with the literature data except the reported viscosities of DMF. The deviation in the viscosity of pure DMF in our work with reported data in the literature may be related to the difference in purity, source of DMF, experimental error, and difference in viscometer type used in this work.

ij x M + x M yz 2 2z zz Vm/(m 3 mol−1) = jjjj 1 1 z ρ m k {

B

(2)



Article

Table 2. Experimental Density (ρ), Speed of Sound (u), and Viscosity (η) of the Pure Liquids at Specified Temperatures and p = 0.0868 MPaa 10−3 ρ/(kg m−3)

u/(m s−1)

η/(mPa s)

component

T/K

exptl

lit.

exptl

lit.

exptl

carbitol

288.15 293.15

0.992168 0.987854

1410.40 1392.25

1410.0911 1392.2711

4.855 4.280

298.15

0.983111

1374.42

1374.6211

3.672

303.15

0.978781

1358.02

1356.9811

3.178

308.15 313.15 318.15 288.15

0.974184 0.969699 0.965330 0.953295

0.99227111 0.98784511 0.9878763 0.98341311 0.9835899 0.9833363 0.97898911 0.9787883 0.97451811 0.97004111 0.96554511 0.9541714

1338.93 1321.41 1304.08 1496.93

1339.5111 1322.2411 1305.1311

2.851 2.503 2.264 0.940

293.15

0.948537

1477.13

1477.118

0.892

298.15

0.943773

1457.70

1457.618

0.844

303.15

0.938996

1437.98

1438.018

0.809

308.15

0.934208

0.9493914 0.9487917 0.9446014 0.9438717 0.94291519 0.9398314 0.9389817 0.93396419 0.934221

1418.40

1418.718

0.773

313.15

0.929408

0.92954919

1398.92

1399.318

0.742

318.15

0.924591

0.92467419 0.9240417

1379.40

1380.018

0.713

288.15 293.15

0.795170 0.791017

1181.85 1164.82

1161.9724

1.332 1.207

298.15

0.786468

0.785626 0.785823

1148.28

1145.4424

1.105

303.15

0.782337

0.782226 0.781523

1130.61

1128.7724

1.016

308.15

0.777826

1113.11

1112.1424

0.932

313.15 318.15

0.773470 0.768977

0.777826 0.777223 0.773426 0.769026

288.15 293.15 298.15 303.15 308.15 313.15 318.15

0.999094 0.998210 0.997045 0.995610 0.994039 0.992301 0.990210

0.9982030 0.9970530 0.9956530 0.994031 0.994031 0.9902029

DMF

ethanol

0.790123

1096.21 1079.48

0.860 0.787

lit.

3.82812 3.8513

0.936015 0.969316 0.86414 0.912116 0.80920 0.825015 0.860516 0.76020 0.71020 0.736015 0.771216 0.68422 0.67320 0.665015 0.697516 1.201625 1.20426 1.209727 1.10426 1.099528 1.99027 1.01326 0.994425 0.997127 0.93326 0.969828 0.85926 0.79226 0.764225

water

a

1466.56 1481.54 1496.93 1509.01 1520.12 1529.25 1536.22

−3

1466.5629 1496.9129 1520.0029 1536.6329

1.089 0.970 0.879 0.807 0.747 0.702 0.657

1.13029 1.003028 0.891428 0.798228 0.720228 0.66732 0.596428

−1

Standard uncertainties (u) for each variables are u(ρ) = 0.2 kg m ; u(u) = 0.5 m s ; u(η) = 0.025 mPa s; u(T) = 0.02 K; u(p) = 0.5 kPa.

ij x M + x M yz ij M yz ij M yz 2 2z zz − x1jjj 1 zzz − x 2jjj 2 zzz VmE/(m 3 mol−1) = jjjj 1 1 z j z j ρ z ρm k { k ρ1 { k 2{

volume of the mixtures. The excess molar volumes of the binary mixtures were reported in Tables 3−5 and shown in Figure 5. As can be seen in Figure 5a, VmE of the carbitol + water mixture are negative and become less negative by increasing the temperature, which is in agreement with those reported for this system at other temperatures.2 The minimum value of the

(3)

where Mi and ρi are the molar mass and density of the pure components, respectively, and ρ and Vm are density and molar C



Article

Table 3. Experimental Density (ρ), Molar Volume (Vm ), Excess Molar Volume (VmE ), Speed of Sound (u), Isentropic E ), Viscosity (η), and Viscosity Deviation (Δη) of the Binary Compressibility (κs), Excess Molar Isentropic Compressibility (κs,m Mixture of Carbitol (1) + Water (2) at the Experimental Temperatures and p = 0.0868 MPaa x1

10−3ρ/(kg m−3)

106Vm /(m3 mol−1)

0.0000 0.1148 0.1990 0.3006 0.3979 0.5002 0.5934 0.6888 0.7914 0.9010 1.0000

0.99909 1.03220 1.02584 1.01905 1.01302 1.00740 1.00339 0.99968 0.99695 0.99408 0.99217

18.016 30.359 40.084 51.942 63.405 75.564 86.655 98.067 110.298 123.428 135.259

0.0000 0.1148 0.1990 0.3006 0.3979 0.5002 0.5934 0.6888 0.7914 0.9010 1.0000

0.99705 1.02210 1.01731 1.01029 1.00418 0.99890 0.99444 0.99106 0.98809 0.98520 0.98308

18.053 30.659 40.420 52.392 63.963 76.207 87.435 98.920 111.286 124.539 136.509

0.0000 0.1148 0.1990 0.3006 0.3979 0.5002 0.5934 0.6888 0.7914 0.9010 1.0000

0.99404 1.01552 1.00873 1.00151 0.99536 0.98995 0.98573 0.98230 0.97912 0.97633 0.97427

18.108 30.858 40.764 52.852 64.530 76.896 88.208 99.802 112.306 125.671 137.744

0.0000 0.1148 0.1990 0.3006 0.3979 0.5002 0.5934 0.6888 0.7914 0.9010 1.0000

0.99021 1.00475 0.99996 0.99255 0.98642 0.98042 0.97679 0.97337 0.97030 0.96738 0.96533

18.178 31.189 41.122 53.329 65.115 77.643 89.015 100.718 113.327 126.834 139.019

106VmE /(m3 mol−1)

u/(m s−1)

Carbitol (1) + Water (2) T/K = 288.15 1466.56 −1.114 1690.35 −1.260 1628.79 −1.319 1568.45 −1.257 1525.91 −1.098 1492.69 −0.929 1467.79 −0.703 1449.32 −0.505 1433.90 −0.225 1420.16 1410.40 T/K = 298.15 1496.91 −0.990 1665.00 −1.202 1596.50 −1.271 1534.70 −1.218 1491.49 −1.099 1457.73 −0.906 1432.89 −0.723 1414.17 −0.514 1398.62 −0.244 1384.53 1374.42 T/K = 308.15 1519.73 −0.981 1638.62 −1.147 1563.46 −1.220 1499.96 −1.175 1456.78 −1.054 1422.74 −0.888 1398.14 −0.708 1379.45 −0.482 1363.63 −0.229 1349.44 1339.93 T/K = 318.15 1536.22 −0.859 1611.31 −1.100 1530.71 −1.176 1466.28 −1.141 1422.53 −0.980 1388.53 −0.866 1369.79 −0.693 1351.88 −0.485 1333.97 −0.223 1316.47 1304.08

κs/TPa−1

κEs,m/(TPa−1)

η/(mPa s)

Δη/(mPa s)

465.365 339.064 367.442 398.901 423.961 445.510 462.598 476.224 487.855 498.774 506.676

−146.678 −124.814 −98.002 −75.785 −56.314 −40.622 −28.107 −17.419 −7.306

1.089 5.923 8.569 9.241 9.050 8.089 7.182 6.478 5.945 5.356 4.855

4.402 6.731 7.020 6.463 5.116 3.858 2.795 1.876 0.874

447.604 352.922 385.664 420.249 447.660 471.110 489.774 504.542 517.372 529.505 538.484

−139.673 −121.245 −96.852 −75.668 −56.767 −41.158 −28.817 −18.051 −7.678

0.879 3.913 5.663 6.064 5.870 5.464 5.040 4.656 4.322 3.984 3.672

2.713 4.228 4.346 3.880 3.188 2.503 1.854 1.232 0.589

435.576 366.737 405.557 443.799 473.405 499.039 518.970 534.986 549.251 562.465 571.683

−136.422 −119.02 −96.006 −75.692 −56.842 −41.465 −29.066 −17.875 −7.280

0.747 2.299 3.849 4.241 4.132 3.943 3.687 3.482 3.233 2.989 2.851

1.311 2.684 2.861 2.547 2.144 1.692 1.286 0.822 0.347

427.923 383.340 426.809 468.614 500.972 529.024 545.620 562.141 579.167 596.458 609.136

−134.806 −119.831 −98.254 −78.227 −59.172 −48.614 −36.886 −23.931 −10.112

0.657 1.219 2.597 3.104 3.052 2.959 2.836 2.648 2.512 2.385 2.264

0.379 1.621 1.964 1.756 1.499 1.226 0.884 0.584 0.281

Standard uncertainties (u) for each variables are u(ρ) = 0.2 kg m−3; u(u) = 0.5 m s−1; u(η) = 0.025 mPa s; u(T) = 0.02 K; u(p) = 0.5 kPa; u(x1) = E 0.0002; u(106VmE ) = 0.1 m3 mol −1; u(κs) = 1 TPa−1; u(κs,m ) = 0.1 TPa−1.

a

VmE (−1.29) is placed in the carbitol mole fraction (x1 = 0.3). The negative VmE values indicate the volume contraction in the mixing process. With addition of carbitol to water, the network structure of water molecules is changed and the new interactions are formed between carbitol and water. In fact, the newly formed

interactions may lead to the decrease in self-association between the carbitol molecules and water which causes a decrease of the possible cavities in the systems. The maximum value of the viscosity of the mixture is also observed at x1 = 0.3, which confirms the strongest interactions at this composition. In the D



Article

Table 4. Experimental Density (ρ), Molar Volume (Vm ), Excess Molar Volume (VmE ), Speed of Sound (u), Isentropic E ), Viscosity (η), and Viscosity Deviation (Δη) of the Binary Compressibility (κs), Excess Molar Isentropic Compressibility (κs,m Mixture of Carbitol (1) + Ethanol (2) at the Experimental Temperatures and p = 0.0868 MPaa x1

10−3ρ/(kg m−3)

106Vm /(m3 mol−1)

0.0000 0.1002 0.2006 0.3007 0.4078 0.5035 0.6057 0.7040 0.8031 0.8958 1.0000

0.79517 0.83791 0.87090 0.89732 0.91999 0.93640 0.95144 0.96382 0.97475 0.98335 0.99217

57.975 65.553 73.230 80.903 89.158 96.602 104.536 112.184 119.884 127.139 135.259

0.0000 0.1002 0.2006 0.3007 0.4078 0.5035 0.6057 0.7040 0.8031 0.8958 1.0000

0.78647 0.82915 0.86200 0.88835 0.91094 0.92745 0.94255 0.95488 0.96562 0.97443 0.98311

58.616 66.245 73.986 81.719 90.044 97.533 105.522 113.235 121.017 128.304 136.505

0.0000 0.1002 0.2006 0.3007 0.4078 0.5035 0.6057 0.7040 0.8031 0.8958 1.0000

0.77783 0.82062 0.85345 0.87955 0.90229 0.91882 0.93382 0.94604 0.95688 0.96563 0.97418

59.268 66.934 74.728 82.537 90.907 98.450 106.509 114.293 122.123 129.474 137.756

0.0000 0.1002 0.2006 0.3007 0.4078 0.5035 0.6057 0.7040 0.8031 0.8958 1.0000

0.76898 0.81180 0.84472 0.87067 0.89340 0.90998 0.92513 0.93710 0.94790 0.95668 0.96533

59.949 67.661 75.500 83.379 91.812 99.407 107.510 115.383 123.280 130.685 139.020

106VmE /(m3 mol−1)

u/(m s−1)

Carbitol (1) + Ethanol (2) T/K = 288.15 1181.85 −0.166 1228.95 −0.251 1266.65 −0.315 1297.58 −0.331 1324.53 −0.286 1344.10 −0.248 1362.22 −0.202 1377.04 −0.162 1390.58 −0.069 1400.66 1410.78 T/K = 298.15 1148.28 −0.176 1194.26 −0.258 1231.88 −0.322 1262.64 −0.333 1289.12 −0.300 1308.74 −0.270 1326.74 −0.218 1341.43 −0.155 1354.27 −0.088 1364.78 1374.42 T/K = 308.15 1113.11 −0.198 1160.69 −0.288 1198.03 −0.336 1228.27 −0.366 1254.95 −0.336 1274.30 −0.298 1292.19 −0.234 1306.56 −0.182 1319.39 −0.107 1329.69 1338.93 T/K = 318.15 1079.48 −0.211 1126.89 −0.314 1164.37 −0.351 1194.27 −0.379 1220.91 −0.354 1240.08 −0.331 1257.70 −0.235 1278.81 −0.174 1284.49 −0.099 1294.70 1304.97

κs/(TPa−1)

κEs,m/(TPa−1)

η/(mPa s)

Δη/(mPa s)

900.358 790.197 715.679 661.889 619.574 591.120 566.401 547.156 530.535 518.354 506.403

−28.922 −39.183 −41.155 −37.978 −32.327 −25.952 −19.395 −13.322 −6.750

1.332 1.564 1.856 2.208 2.641 3.054 3.458 3.849 4.247 4.540 4.855

−0.120 −0.183 −0.184 −0.128 −0.051 −0.008 0.037 0.086 0.053

964.325 845.606 764.458 706.083 660.578 629.507 602.729 581.991 564.653 550.966 538.484

−31.030 −42.774 −45.149 −41.471 −35.653 −28.793 −21.609 −14.383 −7.768

1.105 1.302 1.526 1.823 2.124 2.391 2.716 2.999 3.269 3.472 3.672

−0.060 −0.093 −0.054 −0.028 −0.007 0.057 0.087 0.102 0.068

1037.627 904.539 816.370 753.619 703.722 670.234 641.334 619.201 600.340 585.720 572.538

−37.472 −49.907 −51.514 −47.681 −40.856 −32.980 −24.577 −16.568 −8.977

0.932 1.089 1.260 1.490 1.717 1.915 2.153 2.376 2.596 2.751 2.851

−0.035 −0.057 −0.019 0.002 0.017 0.059 0.093 0.123 0.100

1115.983 970.040 873.188 805.270 750.908 714.613 683.354 652.530 639.408 623.583 608.306

−41.755 −56.017 −57.212 −52.909 −45.168 −36.24 −33.686 −17.429 −8.962

0.787 0.926 1.059 1.228 1.417 1.602 1.769 1.948 2.114 2.219 2.264

−0.009 −0.023 −0.002 0.028 0.072 0.088 0.121 0.141 0.110

Standard uncertainties (u) for each variable are u(ρ) = 0.2 kg m−3; u(u) = 0.5 m s−1; u(η) = 0.035 mPa s; u(T) = 0.02 K; u(p) = 0.5 kPa; u(x1) = E 0.0002; u(VmE × 106) = 0.1 m3 mol −1; u(κs) = 1 TPa−1; u(κs,m ) = 0.1 TPa−1. a

other system, carbitol + ethanol, the VmE values are negative and the minimum value is located around −0.37 in the carbitol mole fraction (x1 = 0.4). The more negative values of VmE for carbitol + water relative to the carbitol + ethanol system indicate that the mixing proceeds with the more contraction in the volume. The

stronger hydrogen bond interactions formed between carbitol and water can be because of this phenomenon which relates to the higher affinity for change in the water molecular structure. Moreover, the VmE values of the carbitol + ethanol mixture become more negative with the rise in temperature, which E



Article

Table 5. Experimental Density (ρ), Molar Volume (Vm ), Excess Molar Volume (VmE ), Speed of Sound (u), Isentropic E ), Viscosity (η), and Viscosity Deviation (Δη) for the Binary Compressibility (κs), Excess Molar Isentropic Compressibility (κs,m Mixture of Carbitol (1) + DMF (2) at the Experimental Temperatures and p = 0.0868 MPaa x1

10−3ρ/(kg m−3)

106Vm /(m3 mol−1)

0.0000 0.1001 0.2007 0.2956 0.4013 0.5005 0.5857 0.7004 0.7999 0.8976 1.0000

0.95330 0.96095 0.96701 0.97205 0.97667 0.98030 0.98293 0.98605 0.98837 0.99033 0.99217

76.681 82.434 88.277 93.785 99.954 105.764 110.775 117.534 123.407 129.192 135.259

0.0000 0.1001 0.2007 0.2956 0.4013 0.5005 0.5857 0.7004 0.7999 0.8976 1.0000

0.94377 0.95143 0.95774 0.96274 0.96742 0.97117 0.97394 0.97720 0.97935 0.98133 0.98311

77.455 83.259 89.131 94.691 100.910 106.758 111.797 118.598 124.543 130.376 136.505

0.0000 0.1001 0.2007 0.2956 0.4013 0.5005 0.5857 0.7004 0.7999 0.8976 1.0000

0.93421 0.94201 0.94836 0.95359 0.95830 0.96210 0.96493 0.96811 0.97044 0.97244 0.97427

78.248 84.092 90.013 95.601 101.870 107.765 112.841 119.712 125.687 131.569 137.744

0.0000 0.1001 0.2007 0.2956 0.4013 0.5005 0.5857 0.7004 0.7999 0.8976 1.0000

0.92459 0.93262 0.93908 0.94424 0.94900 0.95288 0.95580 0.95898 0.96141 0.96345 0.96533

79.062 84.938 90.902 96.547 102.869 108.808 113.920 120.852 126.866 132.796 139.019

106VmE /(m3 mol−1)

u/(m s−1)

Carbitol (1) + DMF (2) T/K = 288.15 1496.93 −0.110 1488.74 −0.163 1480.35 −0.215 1472.15 −0.237 1462.98 −0.236 1454.19 −0.214 1446.65 −0.175 1436.51 −0.128 1427.97 −0.068 1419.33 1410.40 T/K = 298.15 1457.70 −0.106 1449.81 −0.177 1441.60 −0.221 1433.75 −0.245 1424.96 −0.251 1416.60 −0.241 1409.60 −0.215 1399.65 −0.144 1391.46 −0.082 1383.08 1374.42 T/K = 308.15 1418.40 −0.111 1411.11 −0.178 1403.20 −0.237 1396.21 −0.256 1387.81 −0.261 1379.85 −0.252 1373.23 −0.206 1363.70 −0.149 1355.68 −0.082 1347.55 1338.93 T/K = 318.15 1379.40 −0.125 1373.18 −0.195 1365.75 −0.241 1358.56 −0.257 1350.46 −0.263 1343.02 −0.257 1336.85 −0.204 1327.53 −0.153 1320.07 −0.083 1312.21 1304.08

κs/(TPa−1)

κEs,m/(TPa−1)

η/(mPa s)

Δη/(mPa s)

468.133 469.527 471.889 474.687 478.384 482.39 486.126 491.456 496.186 501.249 506.676

−4.928 −8.077 −9.843 −10.632 −10.358 −9.516 −7.697 −5.702 −3.085

0.940 1.147 1.489 1.836 2.256 2.663 3.033 3.538 3.963 4.426 4.855

−0.185 −0.236 −0.261 −0.255 −0.236 −0.199 −0.143 −0.108 −0.028

498.650 500.034 502.414 505.294 509.071 513.109 516.745 522.369 527.376 532.708 538.466

−5.142 −8.453 −10.286 −11.144 −10.962 −10.317 −8.320 −6.140 −3.337

0.844 1.047 1.315 1.578 1.876 2.175 2.444 2.798 3.102 3.387 3.672

−0.080 −0.097 −0.102 −0.103 −0.085 −0.056 −0.027 −0.003 0.005

532.058 533.117 535.536 537.947 541.799 545.903 549.561 555.443 560.684 566.303 572.538

−5.568 −8.932 −11.312 −12.172 −11.989 −11.372 −9.181 −6.816 −3.771

0.773 0.952 1.149 1.348 1.577 1.793 1.974 2.227 2.445 2.647 2.851

−0.029 −0.041 −0.04 −0.030 −0.020 −0.016 −0.001 0.010 0.009

568.421 568.641 570.892 573.799 577.792 581.833 585.422 591.703 596.892 602.787 609.136

−6.439 −10.001 −11.909 −12.658 −12.561 −12.033 −9.466 −7.172 −3.868

0.713 0.853 0.999 1.149 1.319 1.481 1.619 1.815 1.978 2.126 2.264

−0.015 −0.025 −0.022 −0.016 −0.008 −0.003 0.015 0.024 0.021

Standard uncertainties (u) for each variable are u(ρ) = 0.2 kg m−3; u(u) = 0.5 m s−1; u(η) = 0.025 mPa s; u(T) = 0.02 K; u(p) = 0.5 kPa; u(x1) = E 0.0002; u(VmE × 106) = 0.1 m3 mol −1; u(κs) = 1 TPa−1; u(κs,m ) = 0.1 TPa−1. a

mixtures of carbitol is larger than those for carbitol + ethanol and carbitol + DMF mixtures and the order of the negative VmE values is carbitol + water > carbitol + ethanol > carbitol + DMF. This trend shows that the interaction between carbitol and water is stronger than the two other system, while the weakest

suggests that the interaction between carbitol and ethanol needs energy to form and therefore more contraction occurs in the volume. For the binary system of carbitol + water, the values of VmE are also negative and become more negative with an increase in the temperature. The extent of the VmE values for aqueous F



Article

Figure 1. Comparison of the density and speed of sound for carbitol in water at T = 298.15 K in our work (●), ref 8 (Δ), and ref 9 (○).

Figure 3. Speed of sound (u) of the binary mixtures (a) carbitol (1) + water (2), (b) carbitol (1) + ethanol (2), and (c) carbitol (1) + DMF (2) at the experimental temperatures 288.15 (■), 298.15 (▲), 308.15 (⧫), and 318.15 K (•).

κs/Pa−1 = (ρu 2)−1

(4)

E κs,m = κs − κsid

(5)

where ρ, u, κs, and κsid are density, speed of sound, the isentropic compressibility of the binary mixture, and the ideal contribution of isentropic compressibility, respectively. The last parameter was calculated by the following equation9.34,35 ÑÉ ÄÅ ÉÑ ÅÄÅ 2 2 2 Ñ 2 ÑÑ ÅÅ αi 2 ÑÑÑÑ ÅÅÅÅ T (∑i = 0 xiVi )(∑i = 0 ϕα ÅÅ i i )Ñ id ÑÑÑ κs = ∑ ϕiÅÅκsi + TVi ÑÑ − ÅÅÅ 2 ÑÑ ÅÅ ÑÑ Å C ∑ x C pi ÑÑ Å Å Ñ i=0 Ç Ö ÅÅÇ i = 0 i pi ÑÖ

(

)

(6)

where ϕi is the ideal state volume fraction, αi is the isobaric thermal expansion coefficient, Cpi is the molar heat capacity of pure components, T is the temperature, and Vi is the molar volume of pure components. The molar heat capacity for chemicals used in this work was obtained from literature and listed in Table 6.36−41 Moreover, on the basis of the density data, the isobaric thermal expansivity can be calculated. At constant mole fraction, the corresponding isobaric thermal expansion coefficients can be calculated using the relation

Figure 2. Density (ρ) of the binary mixtures (a) carbitol (1) + water (2), (b) carbitol (1) + ethanol (2), and (c) carbitol (1) + DMF (2) at the experimental temperatures 288.15 (■), 298.15 (▲), 308.15 (⧫), and 318.15 K (•).

interactions exist between carbitol and DMF. This trend shows that DMF has the lower affinity to form the strong hydrogen bond with water and therefore contraction in the volume is lower. 3.3. Excess Molar Isentropic Compressibility. The isentropic compressibility (κs) of the pure components and binary mixtures and excess molar isentropic compressibility E (κs,m ) were calculated according to the following equations using the measured ρ and u data33

1 i ∂ρ y αi = − jjj zzz ρ k ∂T { P

(7)

Calculated values of αi are given in Table 6 at different temperatures. The ideal state volume fraction was calculated using following relation G



Article

Figure 5. Excess molar volumes (VmE ) for the binary mixtures (a) (carbitol (1) + water (2)) (b) (carbitol (1) + ethanol (2)) and (c) (carbitol (1) + DMF (2)) at the experimental temperatures 288.15 (■), 298.15 (▲), 308.15 (⧫), and 318.15 K (•).

Figure 4. Viscosity (η) of the binary mixtures (a) carbitol (1) + water (2), (b) carbitol (1) + ethanol (2), and (c) carbitol (1) + DMF (2) at the experimental temperatures 288.15 (■), 298.15 (▲), 308.15 (⧫), and 318.15 K (•).

ϕi =

Table 6. Experimental Isobaric Heat Capacities (Cp) and Isobaric Thermal Expansivity (αP) of Pure Components

xiVi 2

∑i = 1 xiVi

(8)

Cp/(J mol−1 K−1)

E For all studied mixtures, the calculated values of κs and κs,m are given in Tables 3−5. As it can be seen in Table 3, the κs values for the mixtures of carbitol + water decrease with addition of carbitol to the mixtures up to carbitol mole fraction (x1 = 0.1) and then increase with an increase in the carbitol content. The decrease in the κs values with the addition of carbitol (x1 = 0.1) indicates obvious change in the water molecule structure which causes the compressibility of the mixture to reduce.42 By the addition of carbitol higher than x1= 0.1, the compressibilities increase again but are not higher than pure water. This trend suggests that the new interaction that occurred between carbitol and water can produce the new cavities in the system, which do not exist to as great an extent in pure water. By looking at Table 3 E and Figure 2a, it is understood that the κs,m values are negative and the minimum value is observed in the carbitol mole fraction (x1 = 0.1); the same trend is observed for κs. The negative values E of κs,m show that the mixture of carbitol + water is more compressible than carbitol or water which may be attributed to the produced new interactions between different components which are not much affected by the temperature. The calculated values of κs given in Table 4 for (carbitol + ethanol) decrease with an increase in the carbitol mole fraction while increasing with the rise in the temperature. Moreover, the E values (given in Table 4) for this system are negative, and κs,m the minimum values (−52 TPa−1) are observed in the carbitol

104αP/K−1

component

T/K

lit.

cald

carbitol

288.15 298.15 308.15 318.15 288.15 298.15 308.15 318.15 288.15 298.15 308.15 318.15 288.15 298.15 308.15 318.15

299.2a 301.7a 304.6a 307.9a 111.72237 115.86637 120.28037 124.98437 141.5738 150.4339 151.7039 152.99b 75.41040 75.29840 75.241 75.341

7.229 10.14 13.11 16.13 3.865 6.705 9.608 1.258 3.566 6.356 9.205 12.11 0.476 2.885 5.308 7.752

ethanol

DMF

water

a

The Cp values were calculated using the Redlich−Kister equation presented in ref 36 for carbitol in terms of temperature. bThe Cp value for this temperature was obtained from extrapolation of data reported in ref 39 at temperature range T = 298.15−313.15 K.

E values are mole fractions (x1 = 0.3 and 0.4). The negative κs,m indicative of the less compressibility of the mixtures compared to E the pure components. The κs,m values become more negative at

H



Article

E Figure 6. Excess molar isentropic compressibility (κs,m ) of the binary mixtures (a) carbitol (1) + water (2), (b) carbitol (1) + ethanol (2), and (c) carbitol (1) + DMF (2) at the experimental temperatures 288.15 (■), 298.15 (▲), 308.15 (⧫), and 318.15 K (•).

Figure 7. Viscosity deviations (Δη) of the binary mixtures (a) carbitol (1) + water (2), (b) carbitol (1) + ethanol (2), and (c) carbitol (1) + DMF (2) at the experimental temperatures 288.15 (■), 298.15 (▲), 308.15 (⧫), and 318.15 K (•).

Table 7. Constants of the Jouyban−Acree Model at T = 288.15−318.15 K and p = 0.0868 MPaa

the higher temperature, which means greater compressibility of the mixture. E Table 5 reports the calculated values of κs and κs,m for carbitol

J0

E values increase with an + DMF. It is observed that the κs and κs,m increase in the carbitol mole fraction as well as temperature. E Figure 6 shows that the κs,m values are negative and the −1 minimum value (−12.2 TPa ) is observed in the carbitol mole E fraction (x1 = 0.4). The κs,m values for the carbitol + ethanol mixture have the most negative values, and those values for carbitol + DMF mixture are the most positive. More negative E values of κs,m for the carbitol + ethanol mixture compared to those for carbitol + water show that the compressibility of the mixture depends on the other factors in addition to the intermolecular interactions. 3.4. Viscosity Deviations. Δη can be calculated from the experimental viscosity according to the following equation43

10−3ρ/(kg m−3) 106Vm/(m3 mol−1) κs/(TPa−1) 10−3ρ/(kg m−3) 106Vm/(m3 mol−1) κs/(TPa−1) 10−3ρ/(kg m−3) 106Vm/(m3 mol−1) κs/(TPa−1)

J1

Carbitol + Water 7.860 −31.985 518.230 −305.102 NSb 273.467 Carbitol + Ethanol 67.384 −28.695 111.977 −10.047 −172.596 65.397 Carbitol + DMF 10.084 −2.740 45.043 NS −12.816 5.371

J2

%ARD

44.166 182.250 −501.155

0.26 1.18 3.52

NS −30.003 NS

0.17 0.40 0.57

NS NS NS

0.04 0.29 0.08

a Standard uncertainties (u) for each variable are u(T) = 0.02 K and u(p) = 0.5 kPa. bNS = nonsignificant correlation coefficient.

ij 2 yz Δη /(mPa s) = η − jjjj∑ xiηi zzzz j i=1 z (9) k { where η and ηi are the viscosity of the mixture and pure components, respectively. The calculated values of the η and Δη for the studied binary mixtures were listed in Tables 3−5, and the Δη values for three binary mixtures were shown in Figure 7. For the systems containing carbitol and water, Δη values are positive, and the maximum value is observed in the carbitol mole fraction (x1 = 0.3) as reported in the literature.2 For this system, the mixture has the higher viscosity relative to the pure

components, while the Δη values of the two other systems, carbitol + ethanol and carbitol + DMF mixtures, are negative. The positive Δη values of the system containing carbitol and water confirm the most negative values of VmE , which may be attributed the strong interactions between different components. The Δη values of carbitol + DMF relative to carbitol + ethanol mixture are more negative, which confirm the more negative values of VmE in the mixture of carbitol + ethanol. This means that the interactions between the different components can increase the viscosity of the mixtures relative the pure components. I



Article

Table 8. Parameters of the Redlich−Kister Equation for the Excess Molar Volume (VmE ), Excess Molar Isentropic Compressibility E ), and Viscosity Deviation (Δη) at the Experimental Temperatures and p = 0.0868 MPaa (κs,m T/K

a0

a1

a2

a3

σ

288.15

Carbitol (1) + Water (2) −4.315 3.153

−3.580

3.381

0.008

298.15 308.15 318.15

−4.282 −4.134 −4.001

3.031 2.734 2.747

−3.031 −2.908 −2.530

2.265 2.806 1.721

0.005 0.006 0.002

κES /(TPa−1)

288.15 298.15 308.15 318.15

−197.886 −201.812 −203.689 −222.419

269.699 270.564 269.206 231.331

−799.792 −752.381 −723.531 −723.198

948.543 873.554 847.145 865.811

2.018 1.841 1.779 1.685

Δη/(mPa s)

288.15 298.15 308.15 318.15

20.853 12.982 9.260 6.198

12.903 8.644 NS NS

NSb NS NS NS

0.046 0.025 0.048 0.042

106VmE /(m3 mol−1)

288.15

−24.993 −14.899 −8.820 −4.603 Carbitol (1) + Ethanol (2) −1.205 0.610

NS

NS

0.003

298.15 308.15 318.15

−1.228 −1.338 −1.448

0.711 0.724 0.709

−0.191 −0.314 NS

−0.379 −0.387 NS

0.001 0.002 0.003

κES /(TPa−1)

288.15 298.15 308.15 318.15

−128.765 −142.004 −161.748 −183.207

135.146 145.625 171.330 184.555

−89.664 −94.022 −120.902 −131.609

NS NS NS NS

0.062 0.092 0.139 0.502

Δη/(mPa s)

288.15 298.15 308.15 318.15

−0.292 0.049 0.153 0.244

NS NS NS 0.375

NS NS NS NS

0.004 0.002 0.004 0.002

106VmE /(m3 mol−1)

288.15

1.351 0.920 0.828 0.809 Carbitol (1) + DMF (2) −0.929 0.229

NS

NS

0.009

298.15 308.15 318.15

−1.008 −1.039 −1.060

0.119 0.162 0.216

NS NS NS

NS NS NS

0.001 0.001 0.001

κES /(TPa−1)

288.15 298.15 308.15 318.15

−41.658 −44.228 −48.438 −51.167

12.658 11.738 11.600 14.634

NS NS NS NS

NS NS NS NS

0.036 0.040 0.044 0.077

Δη/(mPa s)

288.15 298.15 308.15 318.15

−0.927 −0.322 −0.078 −0.026

0.590 0.500 0.162 0.241

−0.294 NS −0.471 0.087

0.517 NS −0.423 NS

0.001 0.001 0.001 0.000

106VmE /(m3 mol−1)

a

Standard uncertainties (u) for each variable are u(T) = 0.02 K and u(p) = 0.5 kPa. bNS = nonsignificant correlation coefficient (p value < 0.05).

3.5. Correlation of the Physicochemical Properties using Jouyban−Acree Model. The physicochemical properties of a binary mixture could be mathematically represented using the Jouyban−Acree model as reported in earlier work.44 This model describes the properties of mixtures as a function of composition and temperature and is expressed as ÄÅ É 2 ÅÅ x x (x − x )i ÑÑÑ 1 2 1 2 Å ÑÑ ln K m, T = x1 ln K1, T + x 2 ln K 2, T + ∑ Ji ÅÅÅ ÑÑ Å ÑÑÖ T Å i=0 Ç

where K m, T , K1, T , and K 2, T are the values of physicochemical properties such as, ρ, Vm, and κs of the mixture and components 1 (carbitol) and 2 (water, ethanol, and DMF) at T and x1 and x2 are the mole fractions of carbitol and (water, ethanol, and DMF) in the binary mixture, respectively. Ji are the model parameters evaluated using no intercept least-squares analysis.27 The accuracy of the model tested on the studied data sets was evaluated by percent average relative deviation (%ARD)

(10) J


Journal of Chemical & Engineering Data %ARD =

K calcd 100 T −1 ∑ m,exptl N K m, T

Article

energy is supplied at the higher temperatures, but the formation of carbitol−water interaction proceeds spontaneously and temperature can change the water molecules’ structure. Furthermore, the Jouyban−Acree and Redlich−Kister equaE tions were used for correlation of (ρ, Vm , and κs) and (VmE , κs,m , and Δη), respectively. The obtained %ARD and σ of the data correlation show that the data for the binary mixture of carbitol + DMF are correlated well by the Jouyban−Acree and Redlich− Kister equations, respectively.

(11)

in which K m, T are the ρ, Vm, and κs values for the mixture and N is the number of data points in each set. The evaluated Jouyban− Acree parameters for mentioned parameters along with their % ARD were listed in Table 7. The data of all systems were correlated well by this model except the viscosity of the carbitol + water mixture, which has the strange trend. This result shows that the density and viscosity data of the systems which have the linear or exponential trend can be correlated by the Jouyban− Acree model with reasonable accuracy. E 3.6. Correlation of the VmE , κs,m , and Δη Values. The

■

Corresponding Author

*E-mail: [email protected].

E , and Δη can be correlated well with the values of VmE , κs,m Redlich−Kister equation18

ORCID

Seyyedeh Narjes Mirheydari: 0000-0002-7666-4976 Hemayat Shekaari: 0000-0002-5134-6330 Fleming Martinez: 0000-0002-4008-7273 Abolghasem Jouyban: 0000-0002-4670-2783

3

A = x1x 2∑ ai(2xi − 1)i i=0

AUTHOR INFORMATION

(12)

E where A represents VmE , κs,m , and Δη fitting parameters based on the least-squares method. The corresponding standard deviations, σ (A) were calculated using the relation ÄÅ ÉÑ2 σ(F(x)) = ÅÅÅÅ∑ Aexptl − Acalcd ÑÑÑÑ /(p − n)]1/2 (13) Ç Ö

Notes

The authors declare no competing financial interest.

■

REFERENCES

(1) Li, X.-X.; Liu, Y.-X.; Wei, X.-H. Hydrolysis of carbonyl sulfide in binary mixture of diethylene glycol diethyl ether and water. Chin. J. Chem. Eng. 2005, 1, 234−238. (2) Li, X.; Xu, G.; Wang, Y.; Hu, Y. Density, viscosity, and excess properties for binary mixture of diethylene glycol monoethyl ether + water from 293.15 to 333.15 K at atmospheric pressure. Chin. J. Chem. Eng. 2009, 17, 1009−1013. (3) Mozo, I.; García de la Fuente, I.; González, J. A.; Cobos, J. C. Thermodynamics of mixtures containing alkoxyethanols. XXIV. Densities, excess molar volumes, and speeds of sound at (293.15, 298.15, and 303.15) K and isothermal compressibilities at 298.15 K for 2-(2-alkoxyethoxy) ethanol + 1-butanol systems. J. Chem. Eng. Data 2007, 52, 2086−2090. (4) Piekarski, H.; Tkaczyk, M.; Góralski, P. Thermochemical properties of electrolyte solutions in {2-(2-methoxyethoxy) ethanol + water} and (2-isopropoxyethanol + water) mixtures at 298.15 K. J. Chem. Thermodyn. 2004, 36, 259−266. (5) Esteve, X.; Conesa, A.; Coronas, A. Liquid densities, kinematic viscosities, and heat capacities of some alkylene glycol dialkyl ethers. J. Chem. Eng. Data 2003, 48, 392−397. (6) Ku, H.-Ch.; Tu, Ch.-H. Densities and viscosities of seven glycol ethers from 288.15 to 343.15 K. J. Chem. Eng. Data 2000, 45, 391−394. (7) Pal, A.; Gaba, R. Densities, excess molar volumes, speeds of sound and isothermal compressibilities for {2-(2-hexyloxyethoxy) ethanol + n-alkanol} systems at temperatures between (288.15 and 308.15) K. J. Chem. Thermodyn. 2008, 40, 750−758. (8) Pal, A.; Singh, Y. P. Excess molar volumes and apparent molar volumes of {xH(CH2)vO(CH2)2O(CH2)2OH + (1-x) H2O} at the temperature 298.15 K. J. Chem. Thermodyn. 1994, 26, 1063−1070. (9) Douhéreta, G.; Salgado, C.; Davis, M. I.; Loya, J. Ultrasonic speeds and isentropic functions of 2-(2-alkoxyethoxy) ethanol + water at 298.15 K. Thermochim. Acta 1992, 207, 313−328. (10) Shekaari, H.; Taghi Zafarani-Moattar, M.; Mirheydari, S. N. Volumetric, ultrasonic and viscometric studies of aspirin in the presence of 1-octyl-3-methylimidazolium bromide ionic liquid in acetonitrile solutions at T=(288.15−318.15) K. Z. Phys. Chem. 2016, 230, 1773− 1799. (11) Pal, A.; Kumar, B. Volumetric, acoustic and spectroscopic studies for binary mixtures of ionic liquid (1-butyl-3-methylimidazolium hexafluorophosphate) with alkoxyalkanols at T= (288.15 to 318.15) K. J. Mol. Liq. 2011, 163, 128−134.

where p is the number of experimental data points and n is the number of parameters. The calculated parameters ai values along with the standard deviations (σ) are given in Table 8. The nonsignificant (NS) correlation coefficients were removed from E reported coefficients. It is found that the VmE , κs,m , and Δη values for carbitol + DMF with lowest σ are correlated well by the Redlich−Kister model, and the highest σ is obtained for the carbitol + water mixture.

4. CONCLUSION The experimental density, speed of sound, and viscosity for the binary mixtures of carbitol + water, carbitol + ethanol, and carbitol + DMF have been reported over the full range of composition and temperatures ranging from 288.15 to 318.15 K. The molar volume (Vm ), excess molar volume (VmE ), isentropic compressibility (κs), excess molar isentropic compressibility E (κs,m ), and viscosity deviation (Δη) of the studied systems were calculated using the experimental data. The calculated values of E the VmE , and κs,m for carbitol + water mixtures are negative and also have the more negative values rather than other systems. It is interesting that the Δη values for this system are positive, while these values for the two other systems, carbitol + ethanol and carbitol + DMF, are negative. This shows that the carbitol molecules tend to form the strong hydrogen bond with water molecules which cause the viscosities of the mixture to become bigger than those for pure components. The order of the E negative VmE and κs,m values is carbitol + water > carbitol + ethanol > carbitol + DMF, which means that more contraction E occurs in the carbitol + water system. The VmE and κs,m values for carbitol + ethanol and carbitol + DMF mixture become more negative with an increase in temperature, while the Δη values become more positive. The observed trend for the carbitol + water mixture is completely vice versa. This trend shows that carbitol needs energy to interact with ethanol and DMF and this K



Article

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