Density and Viscosity for Binary Mixtures of Diethylene Glycol

Article pubs.acs.org/jced

Density and Viscosity for Binary Mixtures of Diethylene Glycol Monobutyl Ether with Monoethanolamine, Diethanolamine, and Triethanolamine from (293.15 to 333.15) K Xin-Xue Li,*,† Gui-Chen Fan,† Zai-Liang Zhang,‡ Yan-Wei Wang,† and Yi-Qiang Lu† †

Department of Chemistry and Chemical Engineering, University of Science and Technology Beijing, Beijing 100083, People’s Republic of China ‡ China Petroleum Engineering & Construction Corp., Beijing 100120, People’s Republic of China ABSTRACT: Density and viscosity for binary mixtures of diethylene glycol monobutyl ether (DEGMBE) with monoethanolamine (MEA), diethanolamine (DEA), and triethanolamine (TEA) have been measured as a function of composition from (293.15 to 333.15) K at intervals of 10 K under ambient pressure. Densities were measured with a capillary pycnometer. Viscosities were determined using capillary viscometers of the Ubbelohde type. Excess molar volumes VE and viscosity deviations Δη were calculated from the experimental results and correlated by the Redlich−Kister type equations to derive the coefficients and standard deviations. The values of VE and Δη are both negative over the entire range of mole fraction which indicates that molecular interaction of MEA, DEA, and TEA through the hydrogen bond become weaker in the presence of DEGMBE.

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flexibility, negligible vapor pressure, chemical and thermal stability, and nontoxicity.9 The combination of physical and chemical solvents has been proposed for selective absorption processes in order to possess the advantages of both physical solvents and chemical solvents. It is shown that mixtures of triethylene glycol monomethyl ether (TEGMME) + MDEA and methanol + MDEA absorb more CO2 than pure TEGMME or methanol alone.10 Higher absorption capacity would help to reduce absorbent flows that need to be circulated. With this in mind, the present work was undertaken to measure the densities and viscosities for binary mixtures of diethylene glycol monobutyl ether (DEGMBE) with MEA, DEA, and TEA. These properties are essential for the analysis and evaluation of mass transfer and CO2 capture capacity which is an important step for designing gas liquid absorption processes. On the other hand, the macroscopic properties of liquid and liquid mixtures can supply helpful information for understanding the types of molecular interactions involved in the solutions. As far as we know, there is no literature report on the thermodynamic properties for the three mixtures mentioned.

INTRODUCTION The removal of acid gas impurities such as CO2 and H2S from natural, refinery, and synthesis gas streams is an important operation in gas processing.1 Aqueous solutions of alkanolamine as chemical absorbents have been used in the removal of acid gases for quite a long time, and they are still widely used nowadays. Industrially important alkanolamines are monoethanolamine (MEA), diethanolamine (DEA), and methyldiethanolamine (MDEA). Other amines, such as bis (2-hydroxypropyl) amine (DIPA), 1-amino-2-propanol (MIPA), or 3-amino-1propanol (AP), have also been used. Lately, much more attention has been focused on the blends of amine using the synergetic effects of each component during the absorption and regeneration operation. By varying the composition of amines, an optimum solvent formulation with high absorption capacity and selectivity toward acid gases may be designed for a specific application.2−5 In recent years, the process for removing CO2 has changed from industrial streams purification to postcombustion emission reduction, which is one possible solution to fight against global warning.6,7 Apart from solvents of amines, ionic liquids (ILs), and polyether (PEG) have also been investigated to use as solvents for capturing CO2. The application of ionic liquids combined with molecular solvents leads to mixtures with low viscosity, which is useful for mass transfer.8 PEG, physical solvent, does not have the drawbacks of high energy consumption and degradation as does amine-based solvents, and it can be regenerated by pressure or temperature swings, leading to lower energy consumption. In addition, PEG with varied molecular weight has excellent properties such as operational © 2013 American Chemical Society

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EXPERIMENTAL SECTION Materials. Diethylene glycol monobutyl ether (DEGMBE, CAS 112-34-5 Fluka, mass fraction GC > 99 %),

Received: January 8, 2013 Accepted: March 22, 2013 Published: April 4, 2013 1229

dx.doi.org/10.1021/je4000372 | J. Chem. Eng. Data 2013, 58, 1229−1235

Journal of Chemical & Engineering Data

Article

monoethanolamine (MEA, CAS 141-43-−5 Fluka, mass fraction GC > 99 %), diethanolamine (DEA, CAS 111-42-2 Sigma, mass fraction GC > 99.5 %), triethanolamine (TEA, CAS 102-71-6 Sigma, mass fraction GC > 99 %) were used as received. They were dried over 0.4 nm molecular sieves and partially degassed under vacuum before measurement. Bidistilled water with its conductivity lower than 10−7 Ω−1·cm−1 was used. Apparatus and Procedure. The methods for density and viscosity measurements have been described elsewhere.11 The binary mixtures were prepared by mass, using an electronic analytical balance (HANGPING FA2104, Shanghai, China) with a precision of ± 0.0001 g. The uncertainty of the mole fraction for a binary mixture was estimated to be ± 0.0001. The experimental temperature for density and viscosity measurement was controlled to ± 0.01 K by using a water bath. The densities of the pure liquids and the mixtures were measured with a 10 cm3 capillary pycnometer, with the internal diameter of the capillary less than 1 mm. Degassed doubly distilled water was used as a calibrating substance. The uncertainty in density measurement was estimated to be better than 0.1 %. The viscosities were determined by using of two capillary viscometers of Ubbelohde type with the capillary diameter around 0.5 and 1.0 mm, respectively. Doubly distilled water and high-purity ethylene glycol were used as calibrating substances. The flow time measurements were made using an accurate stopwatch with uncertainty of ± 0.01 s. The average of five sets of flow times for each fluid was taken for the purpose of the calculation of viscosity. The uncertainties of the viscosity measurements were estimated to be better than 3 %.

Table 1. Comparison of Measured Densities (ρ) and Viscosities (η) of Pure Compounds with Literature Values at Temperatures from (293.15 to 333.15) K ρ/g·cm−3

x1M1 + x 2M 2 xM xM − 1 1 − 2 2 ρM ρ1 ρ2

Δη = ηM − (x1η1 + x 2η2)

T/K

this work

lit

this work

DEGMBE

293.15

0.9529

0.9522a 0.95281b 0.952196c

5.84

5.8597d

4.98 4.23 3.22 2.51

5.052e 4.3229d 3.2955d 2.5805d

24.14 18.89

24.10i 18.95j 18.98i 14.05j 15.0k 15.1088l 15.1940m 9.95j 9.94k 10.0209l 10.0283m 6.87k 6.9715l 6.9463m 5.006j 5.0473l 5.0454m 890.5i 566.3i 379.3o 383.9i 186.4o 188.2i 98.85o 119.5i 57.69i

DEA

RESULTS AND DISCUSSION A comparison of our measurements of density and viscosity of pure compounds with the data in the literature was presented in Table 1. The agreement between our experimental density value and those in the literature is fairly good. There exist differences in previously published viscosity values which may be caused by material purity and measurement method. The relative difference in viscosity value between this work and literature is low, within limitations of available information. The experimental results of the densities and viscosities for binary mixtures of DEGMBE with MEA, DEA, and TEA from (293.15 to 333.15) K at various mole fractions are listed in Table 2. Excess molar volumes VE and viscosity deviations Δη were calculated from the experimental results according to the following equations, respectively, VE =

compound

MEA

■

TEA

(1) (2)

η/mPa·s

298.15 303.15 313.15 323.15 333.15 293.15 298.15

0.9435 0.9359 0.9266 0.9184 1.0161 1.0121

303.15

1.0084

313.15

1.0001

1.0000h 1.00001g 1.000037f

9.93

323.15

0.9919

0.9920h 992.014f

6.89

333.15

0.9836

0.9839h 0.9839g

4.97

293.15 298.15 303.15

1.0929 1.0898

313.15

1.0837

323.15

1.0774

333.15

1.0707

293.15 298.15

1.1243 1.1213

1.0937g 1.0904n 1.09048g 1.0838n 1.08401g 1.0774n 1.07732g 1.0708n 1.07074g 1.12342p 1.12131g 1.12082f

303.15

1.1185

1.11859g 1.118061f

404.7

313.15

1.1128

1.11282g 1.112402f

203.9

323.15

1.1071

1.106778f

108.3

333.15

1.1015

1.10156g

64.17

a

0.9438 0.9353a 0.9266a 0.9178a 1.015977f 1.0118g 1.01202f 1.0080h 1.00795g 1.008002f

14.88

890.9 569.5 382.2 187.6 99.11 58.12

604.8

lit

605.95q 607j 666.88o 405.9j 405.6r 460.48o 201.7j 236.09o 208.6r 99.76o 116.2r 64.6j 64.55r

a

From ref 12. bFrom ref 13. cFrom ref 14. dFrom ref 15. eFrom ref 16. From ref 17. gFrom ref 18. hFrom ref 19. iFrom ref 20. jFrom ref 21. k From ref 22. lFrom ref 23. mFrom ref 24. nFrom ref 25. oFrom ref 26. p From ref 27. qFrom ref 1. rFrom ref 28. f

where x1 and x2 are the mole fractions; M1 and M2 are molar masses; ρ1 and ρ2 are the densities; and η1 and η2 are the viscosities of pure components 1 and 2, respectively. The subscript M represents mixture properties. The values calculated for VE and Δη are shown in Table 3. The values of VE and Δη were fitted by a Redlich−Kister-type polynomial29

m

Y = x1x 2 ∑ Ak (x1 − x 2)k k=0

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Table 2. Densities ρ and Viscosities η for the Mixtures of DEGMBE with MEA, DEA, and TEA at Temperatures from (293.15 to 333.15) Ka ρ/g·cm−3 x1

T/K = 293.15

303.15

313.15

0.0000 0.04025 0.08607 0.1392 0.2008 0.2732 0.3602 0.4111 0.4671 0.4977 0.6007 0.7204 0.7699 0.8163 0.9331 1.0000

1.0161 1.0103 1.0045 0.9985 0.9925 0.9864 0.9802 0.9769 0.9738 0.9721 0.9671 0.962 0.9602 0.9585 0.9548 0.9529

1.0084 1.0025 0.9966 0.9905 0.9842 0.9779 0.9715 0.9682 0.9649 0.9633 0.9581 0.9529 0.9511 0.9493 0.9455 0.9435

1.0001 0.9943 0.9885 0.9825 0.9764 0.9701 0.9637 0.9604 0.9572 0.9555 0.9503 0.9452 0.9433 0.9416 0.9377 0.9357

0.0000 0.03299 0.06718 0.1026 0.1394 0.2174 0.3018 0.3933 0.4929 0.6019 0.7008 0.7558 0.8059 0.8537 0.9031 1.0000

1.0961 1.0883 1.0807 1.0732 1.0658 1.0509 1.0363 1.0219 1.0077 0.9938 0.9823 0.9764 0.9712 0.9664 0.9616 0.9529

1.0898 1.0818 1.0742 1.0665 1.0589 1.0437 1.0287 1.014 0.9995 0.9852 0.9735 0.9675 0.9622 0.9573 0.9524 0.9435

1.0837 1.0758 1.068 1.0603 1.0525 1.0371 1.0219 1.007 0.9923 0.9779 0.9661 0.96 0.9547 0.9497 0.9448 0.9357

0.0000 0.09279 0.1871 0.2841 0.3804 0.4787 0.5789 0.6816 0.7855 0.8923 1.0000

1.1243 1.1051 1.0863 1.0679 1.0504 1.0333 1.0165 0.9999 0.9839 0.9681 0.9529

1.1185 1.0989 1.0799 1.0610 1.0431 1.0256 1.0085 0.9917 0.9752 0.9591 0.9435

1.1128 1.0931 1.0739 1.0548 1.0367 1.0189 1.0016 0.9846 0.9679 0.9515 0.9357

η/mPa·s 323.15

333.15

293.15

DEGMBE (1) + MEA (2) 0.9919 0.9836 24.14 0.9862 0.9782 23.11 0.9804 0.9725 21.86 0.9743 0.9664 20.39 0.9681 0.9601 18.81 0.9617 0.9537 17.01 0.9551 0.9471 15.02 0.9518 0.9437 13.86 0.9484 0.9404 12.72 0.9467 0.9387 12.16 0.9415 0.9335 10.46 0.9363 0.9283 8.65 0.9344 0.9264 8.02 0.9327 0.9247 7.42 0.9287 0.9207 6.34 0.9266 0.9185 5.84 DEGMBE (1) + DEA (2) 1.0774 1.0707 890.9 1.0694 1.0628 681.3 1.0615 1.0549 550.2 1.0536 1.0469 425.1 1.0457 1.0388 321.3 1.0299 1.0228 191.6 1.0145 1.0073 114.4 0.9992 0.9918 65.16 0.9842 0.9767 38.57 0.9696 0.9619 23.75 0.9576 0.9498 15.75 0.9514 0.9435 12.19 0.946 0.9381 10.43 0.9409 0.933 8.982 0.9359 0.9279 7.858 0.9266 0.9185 5.84 DEGMBE (1) + TEA (2) 1.1071 1.1015 917.6 1.0872 1.0814 491.9 1.0675 1.0616 269.8 1.0481 1.0418 153.2 1.0295 1.0229 85.31 1.0114 1.0045 50.08 0.9937 0.9866 30.52 0.9764 0.9690 18.81 0.9595 0.9519 12.36 0.9427 0.9349 8.49 0.9266 0.9185 5.84

303.15

313.15

323.15

333.15

14.88 14.27 13.61 12.86 11.99 11.01 9.83 9.16 8.51 8.17 7.18 6.21 5.82 5.47 4.62 4.23

9.93 9.52 9.10 8.62 8.08 7.47 6.76 6.37 5.97 5.77 5.12 4.42 4.17 3.96 3.48 3.22

6.89 6.64 6.37 6.07 5.73 5.33 4.88 4.63 4.37 4.23 3.79 3.34 3.17 3.02 2.69 2.51

4.97 4.82 4.65 4.43 4.19 3.91 3.61 3.45 3.28 3.19 2.91 2.59 2.48 2.37 2.11 2.00

382.2 290.7 231.6 189.9 150.1 96.21 59.95 37.05 22.76 14.92 10.43 8.762 7.305 6.312 5.501 4.23

187.6 156.2 122.5 98.20 81.15 53.26 34.51 22.29 14.83 10.02 7.262 6.011 5.293 4.629 4.032 3.22

99.11 80.04 66.29 53.87 43.18 30.37 20.74 14.26 9.416 7.041 5.199 4.251 3.759 3.407 3.028 2.51

58.12 46.73 38.49 31.99 26.71 19.13 13.22 9.429 6.995 5.178 3.927 3.358 3.035 2.756 2.463 2.00

404.7 228.3 126.6 69.69 41.88 26.39 17.51 10.74 8.16 6.01 4.23

203.9 112.6 67.74 40.77 25.92 16.38 10.81 7.41 5.23 4.01 3.22

108.3 69.65 44.43 28.48 17.59 12.82 8.79 5.83 4.35 3.39 2.51

64.2 43.5 28.3 18.4 12.6 8.97 6.52 4.71 3.54 2.67 2.00

a The standard uncertainties u are u(T) = 0.01 K, u(x1) = 0.0001 and the relative expanded uncertainties Ur are Ur(ρ) = 0.001, Ur(η) = 0.03 (level of confidence = 0.95).

where Y = VE/cm3·mol−1 or Δη/mPa·s, and the coefficients of

⎡ ∑ (Y − Y )2 ⎤1/2 cal ⎥ σ (Y ) = ⎢ n−p ⎦ ⎣

Ak are parameters that were obtained by fitting the equations to the experimental values with a least-squares method, which

(4)

−1

where Y refers to V /cm ·mol or Δη/mPa·s; n is the number of data points; and p is the number of coefficients. The subscript cal represents calculated value. E

were given in Table 4. The tabulated standard deviation σ(Y) was defined as 1231

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Table 3. Excess Molar Volumes VE, and Viscosity Deviations Δη for the Mixture of DEGMBE with MEA, DEA, and TEA at Temperatures from (293.15 to 333.15) K VE/cm3·mol−1 x1

T/K = 293.15

303.15

313.15

0.0000 0.04025 0.08607 0.1392 0.2008 0.2732 0.3602 0.4111 0.4671 0.4977 0.6007 0.7204 0.7699 0.8163 0.9331 1.0000

0.000 −0.0581 −0.118 −0.170 −0.222 −0.264 −0.299 −0.299 −0.315 −0.307 −0.286 −0.215 −0.191 −0.148 −0.0579 0.000

0.000 −0.0652 −0.133 −0.194 −0.238 −0.279 −0.313 −0.322 −0.326 −0.335 −0.304 −0.236 −0.218 −0.165 −0.0698 0.000

0.000 −0.0694 −0.142 −0.208 −0.266 −0.307 −0.339 −0.346 −0.360 −0.356 −0.322 −0.264 −0.229 −0.190 −0.0732 0.000

0.0000 0.03299 0.06718 0.1026 0.1394 0.2174 0.3018 0.3933 0.4929 0.6019 0.7008 0.7558 0.8059 0.8537 0.9031 1.0000

0.000 −0.0340 −0.0775 −0.121 −0.167 −0.223 −0.270 −0.296 −0.296 −0.286 −0.246 −0.225 −0.191 −0.147 −0.0910 0.000

0.000 −0.0353 −0.0985 −0.143 −0.189 −0.254 −0.297 −0.326 −0.329 −0.303 −0.265 −0.246 −0.210 −0.163 −0.102 0.000

0.000 −0.0559 −0.113 −0.169 −0.207 −0.274 −0.317 −0.345 −0.343 −0.325 −0.290 −0.264 −0.236 −0.179 −0.126 0.000

0.0000 0.09279 0.1871 0.2841 0.3804 0.4787 0.5789 0.6816 0.7855 0.8923 1.0000

0.000 −0.0842 −0.138 −0.192 −0.227 −0.249 −0.241 −0.198 −0.152 −0.0793 0.000

0.000 −0.0979 −0.188 −0.235 −0.272 −0.291 −0.289 −0.266 −0.186 −0.108 0.000

0.000 −0.125 −0.227 −0.284 −0.328 −0.336 −0.336 −0.311 −0.226 −0.121 0.000

Δη/mPa·s 323.15

333.15

293.15

DEGMBE (1) + MEA (2) 0.000 0.000 0.000 −0.0843 −0.105 −0.293 −0.167 −0.196 −0.705 −0.236 −0.267 −1.20 −0.297 −0.322 −1.66 −0.340 −0.366 −2.13 −0.364 −0.390 −2.53 −0.378 −0.393 −2.76 −0.375 −0.401 −2.87 −0.373 −0.400 −2.87 −0.348 −0.374 −2.69 −0.284 −0.309 −2.31 −0.253 −0.277 −2.03 −0.217 −0.240 −1.78 −0.0891 −0.110 −0.724 0.000 0.000 0.000 DEGMBE (1) + DEA (2) 0.000 0.000 0.000 −0.0653 −0.0853 −180.4 −0.131 −0.162 −281.2 −0.187 −0.219 −375.0 −0.234 −0.256 −446.2 −0.295 −0.317 −506.9 −0.354 −0.384 −509.4 −0.370 −0.395 −477.6 −0.364 −0.395 −416.1 −0.354 −0.375 −334.4 −0.319 −0.339 −254.9 −0.293 −0.304 −209.8 −0.263 −0.280 −167.2 −0.200 −0.223 −126.3 −0.142 −0.152 −83.7 0.000 0.000 0.000 DEGMBE (1) + TEA (2) 0.000 0.000 0.000 −341.1 −0.162 −0.185 −0.260 −0.316 −477.2 −0.335 −0.382 −505.4 −0.363 −0.409 −485.5 −0.380 −0.421 −431.1 −0.368 −0.415 −359.3 −0.343 −0.377 −277.3 −0.269 −0.302 −189.1 −0.137 −0.165 −95.55 0.000 0.000 0.000

303.15

313.15

323.15

333.15

0.000 −0.0737 −0.143 −0.210 −0.281 −0.363 −0.432 −0.459 −0.474 −0.480 −0.469 −0.395 −0.348 −0.295 −0.113 0.000

0.000 −0.0305 −0.0644 −0.127 −0.184 −0.249 −0.290 −0.299 −0.303 −0.302 −0.276 −0.240 −0.203 −0.176 −0.0887 0.000

0.000 −0.181 −0.353 −0.538 −0.751 −0.960 −1.21 −1.34 −1.40 −1.41 −1.30 −0.998 −0.861 −0.716 −0.322 0.000

0.000 −0.140 −0.252 −0.376 −0.503 −0.627 −0.753 −0.802 −0.826 −0.820 −0.779 −0.676 −0.594 −0.493 −0.189 0.000

0.000 −79.0 −125.2 −153.5 −179.4 −203.8 −208.2 −196.5 −173.1 −139.8 −106.9 −87.8 −70.3 −53.2 −35.4 0.000

0.000 −25.3 −52.7 −70.5 −80.7 −94.3 −97.4 −92.8 −81.9 −66.6 −51.1 −42.2 −33.7 −25.6 −17.1 0.000

0.000 −15.9 −26.3 −35.3 −42.5 −47.7 −49.2 −46.9 −42.1 −33.9 −26.2 −21.8 −17.5 −13.2 −8.84 0.000

0.000 −9.54 −15.9 −20.4 −23.6 −26.8 −28.0 −26.6 −23.5 −19.2 −14.9 −12.3 −9.86 −7.45 −4.98 0.000

0.000 −139.2 −203.2 −221.2 −210.5 −186.6 −155.4 −121.0 −82.0 −41.4 0.000

0.000 −72.7 −98.6 −106.1 −101.6 −91.5 −76.9 −59.7 −41.0 −20.8 0.000

0.000 −29.7 −44.9 −50.5 −51.1 −45.4 −38.7 −30.7 −21.1 −10.6 0.000

0.000 −14.9 −24.3 −28.1 −27.9 −25.5 −21.7 −17.1 −11.8 −6.03 0.000

temperature dependence between V E and Δη. With increasing temperature, the excess molar volumes become more negative while the viscosity deviations become less. The effect of temperature on viscosity is more pronounced than that on density. There exist molecular interactions mainly by hydrogen bonds in pure liquids of MEA, DEA, TEA, and DEGMBE. This kind of interaction is very strong especially in pure DEA and TEA owing

Figures 1 to 3 show that the excess molar volumes are negative over the entire range of composition at the experimental temperature range. The negative VE indicate that there is a volume contraction on mixing. Figures 4 to 6 show that the viscosity deviations are also negative over the entire range of composition within the experimental temperature range. Obviously, the values of VE and Δη are affected by temperature and composition. There exists a difference in 1232



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Table 4. Coefficients of the Redlich−Kister Equation and Standard Deviation for Excess Molar Volume and Viscosity Deviation for DEGMBE with MEA, DEA, and TEA T/K 293.15 303.15 313.15 323.15 333.15

293.15 303.15 313.15 323.15 333.15

293.15 303.15 313.15 323.15 333.15

property Y

A0

VE/cm3·mol−1 Δη/mPa·s VE/cm3·mol−1 Δη/mPa·s VE/ cm3·mol−1 Δη/mPa·s VE/cm3·mol−1 Δη/mPa·s VE/cm3·mol−1 Δη/mPa·s

−1.227 −11.40 −1.302 −5.616 −1.404 −3.306 −1.486 −1.928 −1.574 −1.204


−1.214 −1648 −1.318 −691.1 −1.382 −323.7 −1.487 −165.5 −1.577 −93.84


−0.9784 −1669 −1.178 −721.6 −1.381 −355.2 −1.530 −177.9 −1.701 −98.94

A1

A2

DEGMBE (1) + MEA (2) 0.2294 0.06635 −0.2725 1.110 0.1769 −0.07477 0.02882 4.198 0.2294 −0.1404 −0.2018 0.2699 0.2761 −0.4146 −0.2126 0.1961 0.2404 −0.6651 0.2540 0.00814 DEGMBE (1) + DEA (2) 0.1102 −0.0712 1353 −972.6 0.1783 −0.1903 510.0 −231.6 0.1379 −0.4219 251.5 −179.5 0.1243 −0.5929 121.8 −78.57 0.1328 −0.7718 66.64 −35.80 DEGMBE (1) + TEA (2) −0.00603 0.1859 1321 −894.1 −0.07082 0.03467 595.6 −464.8 −0.05416 −0.04883 260.5 −159.5 −0.03694 −0.2849 127.6 −79.06 0.05862 −0.5140 72.09 −48.23

Figure 1. Excess molar volume VE vs mole fraction x1 for DEGMBE (1) + MEA (2): ■, 293.15 K; •, 303.15 K; ▲, 313.15 K; ∗, 323.15 K; □, 333.15 K. The symbols represent experimental values, and the solid curves represent the values calculated from eq 3 with corresponding parameters listed in Table 4.

A3 0.1790 −2.140 0.2899 −0.4896 0.2069 0.2936 0.1885 0.2181 0.3543 −0.7717 −0.01697 993.5 −0.04311 480.1 0.06441 148.0 0.1199 88.91 0.2940 57.50 0.1437 830.9 0.2626 242.5 0.3641 196.3 0.4759 30.88 0.3958 0.1091

A4

0.3711 −4.374 −0.1626 −0.08396 0.1972

−736.7 −596.0 −85.79 −74.81 −62.11

−584.4 −14.66 −173.8 0.9534 26.31

σ(Y) 0.0045 0.033 0.0055 0.01 0.0032 0.01 0.0073 0.0032 0.0045 0.0045 0.0071 5.94 0.0078 3.6 0.0045 0.81 0.0063 0.44 0.0078 0.31 0.0045 1.55 0.0063 0.38 0.0063 0.65 0.0063 0.59 0.0055 0.10

Figure 2. Excess molar volume VE vs mole fraction x1 for DEGMBE (1) + DEA (2): ■, 293.15 K; •, 303.15 K; ▲, 313.15 K; ∗, 323.15 K; □, 333.15 K. The symbols represent experimental values, and the solid curves represent the values calculated from eq 3 with corresponding parameters listed in Table 4. 1233



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Figure 5. Viscosity deviation Δη vs mole fraction x1 for DEGMBE (1) + DEA (2): ■, 293.15 K; •, 303.15 K; ▲, 313.15 K; ∗, 323.15 K; □, 333.15 K. The symbols represent experimental values, and the solid curves represent the values calculated from eq 3 with corresponding parameters listed in Table 4.

Figure 3. Excess molar volume VE vs mole fraction x1 for DEGMBE (1) + TEA (2): ■, 293.15K; •, 303.15 K; ▲, 313.15 K; ∗, 323.15 K; □, 333.15 K. The symbols represent experimental values, and the solid curves represent the values calculated from eq 3 with corresponding parameters listed in Table 4.

Figure 6. Viscosity deviation Δη vs mole fraction x1 for DEGMBE (1) + TEA (2): ■, 293.15 K; •, 303.15 K; ▲, 313.15 K; ∗, 323.15 K; □, 333.15 K. The symbols represent experimental values, and the solid curves represent the values calculated from eq 3 with corresponding parameters listed in Table 4.

Figure 4. Viscosity deviation Δη vs mole fraction x1 for DEGMBE (1) + MEA (2): ■, 293.15 K; •, 303.15 K; ▲, 313.15 K; ∗, 323.15 K; □, 333.15 K. The symbols represent experimental values, and the solid curves represent the values calculated from eq 3 with corresponding parameters listed in Table 4.

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to their molecular structure. The large viscosity of DEA and TEA is the macroscopic consequence of their strong molecular interactions. The viscosity of DEA and TEA decreases substantially by adding DEGMBE, which implies that the strong interactions among DEA or TEA molecules become weaker caused by the disturbance of the DEGMBE molecule. Increasing temperature can also weaken the hydrogen bond, which results in the viscosity deviations for binary mixtures of DEGMBE with MEA, DEA, and TEA becoming less negative. On the other hand, molecular voids of the mixtures become easy to be filled due to the weakening of the hydrogen bond at high temperature and the differences in size of different molecules. Thus the excess molar volumes for binary mixtures of DEGMBE with MEA, DEA, and TEA become more negative by increasing temperature.

AUTHOR INFORMATION

Corresponding Author

*Tel.: +86-10-62333871. Fax: +86-10-62332126. E-mail: [email protected]. Funding

The authors are grateful to the financial support provided by the National Science Foundation of China (No. 51274019). Notes

The authors declare no competing financial interest.

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Density and Viscosity for Binary Mixtures of Diethylene Glycol

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