Densities, Viscosities, and Refractive Indices of Binary Mixtures of 1,2

Article pubs.acs.org/jced

Densities, Viscosities, and Refractive Indices of Binary Mixtures of 1,2,3,4-Tetrahydronaphthalene with Some n‑Alkanes at T = (293.15 to 313.15) K Xianjie Gong, Yongsheng Guo,* Juan Xiao, Yuzhong Yang, and Wenjun Fang* Department of Chemistry, Zhejiang University, Hangzhou 310058, China ABSTRACT: Densities, viscosities, and refractive indices are investigated for binary mixtures of 1,2,3,4-tetrahydronaphthalene with several n-alkanes, namely, octane, nonane, and decane, at different temperatures (293.15 K, 298.15 K, 303.15 K, and 313.15 K) and atmospheric pressure. The values of density (ρ) of the compounds were used to compute excess molar volume (VmE) of the solution. The refractive indices of these binary systems were also determined over the whole concentration range at 293.15 K and 303.15 K.

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INTRODUCTION The thermal stability at high temperatures of hydrocarbon fuel plays a crucial role in the design and development of hypersonic aircraft, in which the fuel temperature is expected to be high enough for the cleavage of carbon−carbon bonds, then leading to the rapid degradation of hydrocarbons and carbon deposition.1,2 1,2,3,4-Tetrahydronaphthalene can significantly retard the formation of carbonaceous materials in hydrocarbon fuels. It has been ascertained that tetralin acts as a hydrogen donor, capping aliphatic radicals formed at high temperatures while transforming into relatively stable products.3−5 At the same time, as a high-density naphthene compound, tetralin can be added into n-alkanes (major components of commercial petroleum based fuel6,7) to enhance its poor performance in energy density, which is directly dependent on the volumetric properties of fuels. In the present work, the physical properties (densities, viscosities, and refractive index) of the binary mixtures of octane, nonane, and decane + 1,2,3,4-tetrahydronaphthalene were measured in detail at T = (293.15 to 313.15) K and atmospheric pressure over the whole composition range. The excess molar volumes (VmE) of these binary mixtures were calculated based on the experimental data. The results may provide important information for the blending of hydrocarbon fuels.

were obtained from J&K Chemical Reagent Company, Shanghai, China. All reagents were used without further purification. Detailed information of samples is listed in Table 1. Table 1. Samples Used in This Work source

initial mass fraction purity

purification method

1,2,3,4-tetrahydronaphthalene octane nonane decane

Aladdin J&K J&K J&K

0.99 0.99 0.99 0.99

none none none none

Apparatus and Procedure. The densities (ρ) of pure sample and their binary mixtures at (293.15 K, 298.15 K, 303.15 K, and 313.15 K) were determined using a DMA 5000 M density meter, Anton Paar. The apparatus has a built-in thermometer with an accuracy of ± 0.01 K, and the uncertainty in measuring density is ± 5·10−5 g·cm−3. The viscosities (η) of pure compounds and their binary mixtures at different temperatures were measured by an AMVn viscometer (Anton Paar). The constant-temperature system is controlled within ± 0.01 K, and the accuracy of the efflux time measurement is ± 0.001 s for the apparatus. The uncertainty of the viscosity measurements in the present work is within ± 0.005 mPa·s. Refractive index (nD) measurements were carried out using a WAY-2S refractometer at temperatures (293.15 K and 303.15

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EXPERIMENTAL SECTION Materials. The sample of 1,2,3,4-tetrahydronaphthalene (CAS No. 119-64-2, mass fraction purity > 99 %) was supplied by Aladdin Chemistry Co., Ltd., Shanghai, China. Octane (CAS No. 111-65-9), nonane (CAS No. 111-84-2), and decane (CAS No. 124-18-5) with mass fraction purities of better than 99 % © 2012 American Chemical Society

chemical name

Received: August 14, 2012 Accepted: October 18, 2012 Published: October 25, 2012 3278

dx.doi.org/10.1021/je300899n | J. Chem. Eng. Data 2012, 57, 3278−3282

Journal of Chemical & Engineering Data

Article

Table 2. Densities (ρ), Viscosities (η), and Refractive Indices (nD) at T = 298.15 K and 1 atm of Pure Compounds Used in This Work ρ/g·cm−3

a

η/mPa·s

nD

compound

exptl

lit.

exptl

lit.

exptl

lit.

octane nonane decane 1,2,3,4-tetrahydronaphthalene

0.6987 0.7146 0.7273 0.9649

0.6986a 0.7139b 0.7272c 0.9651d

0.5289 0.6813 0.8600 2.0205

0.5184e 0.6715f 0.8590g 1.9800h

1.3950 1.4041 1.4102 1.5388

1.3959i 1.4041i 1.4099i 1.5392j

Reference 8. bReference 9. cReference 10. dReference 11. eReference 12. fReference 13. gReference 14. hReference 15. iReference 16. jReference 17.

Table 3. Density ρ and Viscosities η at Temperature T and Mole Fraction x for the System n-Alkanes + 1,2,3,4Tetrahydronaphthalene at 1 atma ρ/g·cm−3 xn‑alkane

293.15 K

298.15 K

0.0000 0.0997 0.2011 0.3013 0.3997 0.5003 0.5995 0.7001 0.8014 0.8955 1.0000

0.96890 0.93921 0.90975 0.88140 0.85429 0.82722 0.80123 0.77554 0.75033 0.72750 0.70276

0.96495 0.93511 0.90565 0.87730 0.85027 0.82312 0.79713 0.77144 0.74623 0.72340 0.69873

0.0000 0.1063 0.2018 0.3066 0.4057 0.5014 0.6005 0.7040 0.7942 0.8898 1.0000

0.96890 0.93616 0.90822 0.87893 0.85264 0.82844 0.80451 0.78071 0.76084 0.74066 0.71844

0.96495 0.93218 0.90428 0.87497 0.84870 0.82450 0.80058 0.77678 0.75693 0.73675 0.71456

0.0000 0.1001 0.2044 0.2961 0.3964 0.4994 0.6017 0.6964 0.7971 0.8894 1.0000

0.96890 0.93694 0.90607 0.88081 0.85493 0.83023 0.80735 0.78750 0.76765 0.75044 0.73106

0.96495 0.93307 0.90222 0.87699 0.85113 0.82644 0.80358 0.78375 0.76391 0.74672 0.72729

η/mPa·s 303.15 K

313.15 K

293.15 K

Octane (1) + 1,2,3,4-Tetrahydronaphthalene (2) 0.96099 0.95306 2.229 0.93120 0.92327 1.831 0.90173 0.89377 1.527 0.87337 0.86539 1.303 0.84632 0.83834 1.143 0.81917 0.81114 0.976 0.79317 0.78512 0.850 0.76747 0.75939 0.747 0.74225 0.73414 0.673 0.71941 0.71126 0.612 0.69469 0.68652 0.556 Nonane (1) + 1,2,3,4-Tetrahydronaphthalene (2) 0.96099 0.95306 2.229 0.92819 0.92039 1.814 0.90029 0.89250 1.585 0.87102 0.86322 1.352 0.84475 0.83695 1.198 0.82057 0.81277 1.082 0.79665 0.78885 0.976 0.77286 0.76506 0.890 0.75301 0.74521 0.826 0.73284 0.72504 0.784 0.71060 0.70281 0.727 Decane (1) + 1,2,3,4-Tetrahydronaphthalene (2) 0.96099 0.95306 2.229 0.92911 0.92124 1.873 0.89829 0.89047 1.629 0.87311 0.86531 1.471 0.84724 0.83948 1.345 0.82258 0.81484 1.226 0.79973 0.79202 1.143 0.77992 0.77223 1.071 0.76009 0.75243 1.015 0.74291 0.73528 0.968 0.72350 0.71589 0.925

298.15 K

303.15 K

313.15 K

2.021 1.675 1.405 1.207 1.063 0.918 0.811 0.702 0.635 0.580 0.529

1.840 1.533 1.294 1.118 0.989 0.857 0.762 0.662 0.599 0.550 0.501

1.549 1.308 1.117 0.971 0.866 0.757 0.675 0.592 0.539 0.496 0.456

2.021 1.653 1.450 1.254 1.111 1.006 0.908 0.833 0.775 0.735 0.681

1.840 1.518 1.334 1.151 1.034 0.937 0.848 0.777 0.728 0.690 0.641

1.549 1.308 1.148 0.997 0.905 0.821 0.749 0.690 0.649 0.615 0.572

2.021 1.703 1.486 1.349 1.238 1.134 1.060 0.993 0.942 0.900 0.860

1.840 1.560 1.368 1.245 1.148 1.053 0.986 0.925 0.878 0.838 0.802

1.549 1.328 1.175 1.073 0.995 0.917 0.862 0.809 0.770 0.737 0.705

a

xn‑alkane is the mole fraction of solutions. Standard uncertainties u are u(T) = 0.01 K, u(x) = 0.0001, and the combined expanded uncertainties Uc are Uc(ρ) = 0.00005 g·cm−3, and Uc(η) = 0.005 mPa·s (level of confidence = 0.95).

literature data and shown in Table 2. It can be clearly seen that the experimental data of all measured properties are in good agreement with those reported in literature.8−17 Experimental values of densities and viscosities of all binary mixtures at 293.15 K, 298.15 K, 303.15 K, and 313.15 K are shown in Table 3. It is clearly shown that the densities and viscosities of the 1,2,3,4-tetrahydronaphthalene are much higher than those of n-alkanes (octane, nonane, and decane);

K). The measurement temperatures were maintained constant by circulating water with a precision of ± 0.01 K. Each refractive index value reported in this work was an average of three measurements, with an uncertainty of ± 0.004.

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RESULTS AND DISCUSSION The density and viscosity of all of the pure solvents are measured at T = 298.15 K and 1 atm compared with the 3279



Article

In the equation, Mi, xi, and ρi (i = 1, 2) are the molar masses (g·mol−1), the mole fractions, and the densities (g·cm−3) of pure component, respectively. Component 1 is octane, nonane, or decane, and component 2 is 1,2,3,4-tetrahydronaphthalene. ρm is the density of the binary system. The uncertainty of the excess volume, VmE, is ± 1·10−3 cm3·mol−1. Figure 3 shows that the excess molar volumes of all binary systems are negative over the whole concentration range at each temperature, and the values of VmE decrease with increasing temperature. When compared with other researchers' results,18−20 It can be seen that the present experimental data are in good agreement with some of reported data but not

as for the binary mixtures, these values decrease continuously with increasing molality of n-alkane or temperature. The density values of octane + 1,2,3,4-tetrahydronaphthalene binary mixtures varying with temperature are presented in Figure 1,

Figure 1. Densities of the system octane (1) + 1,2,3,4tetrahydronaphthalene (2) for different mole fraction xoctane at each temperature: ■, 0.0000; ●, 0.0997; ▲, 0.2011; ▼, 0.3013; ⧫, 0.3997; ◀, 0.5003; ▶, 0.5995; △, 0.7001; ○, 0.8014; ◇, 0.8955; □, 1.0000.

and the viscosities against the mole fraction xoctane are shown in Figure 2. We can see a linear behavior for density versus

Figure 2. Viscosities for the system octane (1) + 1,2,3,4tetrahydronaphthalene (2) as a function of mole fraction xoctane at different temperatures: ■, 293.15 K; ●, 298.15 K; ▲, 303.15 K; ▼, 313.15 K.

temperature from Figure 1 and an exponential decay for viscosity versus mole fraction xoctane from Figure 2. The same trend also is observed in the system of nonane or decane + 1,2,3,4-tetrahydronaphthalene. Excess molar volumes VmE of the binary mixtures are calculated using the equation below. Vm E =

M1x1 + M 2x 2 ⎛ M1x1 Mx ⎞ − ⎜⎜ + 2 2 ⎟⎟ ρm ρ2 ⎠ ⎝ ρ1

Figure 3. Excess molar volumes (VmE) variation with mole fraction for the systems n-alkane (a, octane; b, nonane; c, decane) + 1,2,3,4tetrahydronaphthalene at different temperatures. This work: ■, 293.15 K; ●, 298.15 K; ▲, 303.15 K; ▼, 313.15 K; ref 18: ◊, 298.15 K; ref 19: □, 293.15 K; ○, 298.15 K; △, 303.15 K; ▽, 313.15 K; ref 20: ☆, 293.15 K; ∗, 303.15 K; +, 313.15 K.

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Article

all. The variations of VmE as a function of xn‑alkane for three binary mixtures at T = 298.15 K are shown in Figure 4. It can

listed in Table 4. It shows that the refractive indices vary little while passing from octane to decane. Figure 5 shows the

Figure 4. Excess molar volume (VmE) as a function of xn‑alkane at T = 298.15 K: ■, octane; ●, nonane; ▲, decane.

Figure 5. Refractive index of decane + 1,2,3,4-tetrahydronaphthalene against the mole fraction xdecane at two temperatures. This work: ■, 293.15 K; ●, 303.15 K; ref 20: □, 293.15 K; ○, 303.15 K.

be seen that values of VmE decrease with the increment of nalkane concentration up to the mole fraction x1 of 0.4 to 0.5 and then increase with x1. Obviously, the values of VmE are sensitive to the alkyl length of the n-alkane. The absolute values of VmE decrease with increased carbon number of the n-alkane and follow the order: octane > nonane > decane. For the nonpolar systems of n-alkanes + 1,2,3,4-tetrahydronaphthalene, the physical intermolecular forces are very weak. The variations of VmE can be mainly attributed to molecular structural factors. 1,2,3,4-Tetrahydronaphthalene is a cyclic component, while octane, nonane, and docane are chain alkanes. Therefore, small alkane molecules can get the chance to enter the space of cyclic tetralin and cause intermolecular bundling or intertwining. As a result, the molecular distance between two components becomes smaller. That is the reason that the excess molar volumes of all binary systems studied are negative. The refractive indices of binary mixtures of n-alkanes + 1,2,3,4-tetrahydronaphthalene at 293.15 K and 303.15 K are

experimental behaviors of refractive indices for decane + 1,2,3,4-tetrahydronaphthalene, which agrees well with the reported data.20 A decrease in refractive index with increasing decane concentration is observed. The same trend also is found in the system of octane or nonane + 1,2,3,4-tetrahydronaphthalene.

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CONCLUSION Densities and viscosities of n-alkanes + 1,2,3,4-tetrahydronaphthalene were measured over the whole concentration range at several temperatures and atmospheric pressure. Based on these measured data, the excess molar volume VmE values were calculated. The VmE values are negative for all of the binary mixtures studied. The values of VmE go through a minimum with increasing the mole fraction of n-alkanes, and the extreme values for the binary systems are all observed at the range of xn‑alkanes from 0.4 to 0.5. It can also be seen that a linear decrease behavior for refractive index is caused by increasing mole

Table 4. Refractive Index nD at Temperature T and Mole Fraction x for the System n-Alkane + 1,2,3,4-Tetrahydronaphthalene at 1 atma nD

nD

nD

xoctane

293.15 K

303.15 K

xnonane

293.15 K

303.15 K

xdecane

293.15 K

303.15 K

0.0000 0.0997 0.2011 0.3013 0.3997 0.5003 0.5995 0.7001 0.8014 0.8955 1.0000

1.540 1.524 1.507 1.495 1.485 1.468 1.460 1.442 1.428 1.412 1.397

1.536 1.520 1.506 1.491 1.483 1.465 1.457 1.440 1.427 1.409 1.392

0.0000 0.1063 0.2018 0.3066 0.4057 0.5014 0.6005 0.7040 0.7942 0.8898 1.0000

1.540 1.522 1.509 1.494 1.483 1.473 1.457 1.446 1.434 1.423 1.407

1.536 1.518 1.505 1.491 1.481 1.470 1.453 1.443 1.430 1.419 1.402

0.0000 0.1001 0.2044 0.2961 0.3964 0.4994 0.6017 0.6964 0.7971 0.8894 1.0000

1.540 1.523 1.506 1.488 1.479 1.463 1.452 1.441 1.430 1.422 1.412

1.536 1.519 1.502 1.487 1.475 1.461 1.448 1.437 1.427 1.418 1.409

a

xn‑alkane is mole fraction of solutions. Standard uncertainties u are u(T) = 0.01 K, u(x) = 0.0001, and the combined expanded uncertainty Uc(nD) = 0.004 (level of confidence = 0.95). 3281



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200 MPa and Temperatures up to 473 K. J. Chem. Eng. Data 2009, 54, 359−366. (16) Aminabhavi, T. M.; Patil, V. B. Density, Refractive Index, Viscosity, and Speed of Sound in Binary Mixtures of Ethenylbenzene with Hexane, Heptane, Octane, Nonane, Decane, and Dodecane. J. Chem. Eng. Data 1997, 42, 641−646. (17) Yu, Z. W.; He, X. H.; Zhou, R.; Liu, Y.; Sun, X. D. Volumetric Properties of Binary Systems between Tetralin and Alkylbenzenes. Fluid Phase Equilib. 1999, 164, 209−216. (18) Letcher, T. M.; Scoones, B. W. H. The Excess Volumes of Tetrahydronaphthalene in n-Alkanes at 10 and 25 °C. J. Solution Chem. 1981, 10, 459−463. (19) Yu, C. H.; Tsai, F. N. Excess Volumes of Binary Mixtures of Tetralin with n-Alkanes from 293.15 to 313.15 K. J. Chem. Eng. Data 1995, 40, 601−604. (20) Paredes, M. L. L.; Reis, R. A.; Silva, A. A.; Santos, R. N. G.; Santos, G. J.; Ribeiro, M. H. A.; Ximango, P. B. Densities, Sound Velocities, and Refractive Indexes of (Tetralin + n-Decane) and Thermodynamic Modeling by Prigogine-Flory-Patterson Model. J. Chem. Thermodyn. 2012, 45, 35−42.

fraction of xn‑alkane. On the whole, it can be explained in terms of the changes of molecular shapes and interactions.

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AUTHOR INFORMATION

Corresponding Author

*Y.G.: Tel.: +86 571 88981416. Fax: +86 571 88981416. Email: [email protected]. W.F.: Tel.: +86 571 88981416. Fax: +86 571 88981416. E-mail: [email protected]. Funding

The authors are grateful for financial support from the National Natural Science Foundation of China (Grant No. 21173191). Notes

The authors declare no competing financial interest.

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Densities, Viscosities, and Refractive Indices of Binary Mixtures of 1,2

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