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298 to 573 K and at pressures up to 40 MPa

I.M. Abdulagatova,∗ , A. Zeinalovab , N.D. Azizovb

a Institute for Geothermal Problems of the Dagestan Scientiﬁc Center of the Russian Academy of Sciences,

367003 Makhachkala, Shamilya Str. 39-A, Dagestan, Russia

b Azerbaijan State Oil Academy, Baku 370601, Azerbaijan

Received 24 August 2004; received in revised form 20 October 2004; accepted 21 October 2004

Abstract

Viscosities of nine (1.5, 3, 5, 7, 10, 15, 20, 23, and 26) mass% of aqueous Na2 SO4 solutions have been measured in the liquid phase with a

capillary flow technique. Measurements were made at five isobars 0.1, 10, 20, 30, and 40 MPa. The range of temperatures was from 298.15

to 573.5 K. The total uncertainty of viscosity, pressure, temperature, and concentration measurements was estimated to be less than 1.5%,

0.05%, 15 mK, and 0.015%, respectively. The reliability and accuracy of the experimental method was confirmed with measurements on pure

water for four selected isobars 5, 10, 20, and 40 MPa and at temperatures between 296.7 and 573.7 K. The experimental and calculated values

from IAPWS (International Association for the Properties of Water and Steam) formulation for the viscosity of pure water show excellent

agreement within their experimental uncertainty (AAD = 0.41%). The temperature, pressure, and concentration dependences of the relative

viscosity (η/η0 ) where η0 is the viscosity of pure water are studied. The values of the viscosity A-, B-, and D-coefficients of the extended

Jones–Dole equation for the relative viscosity (η/η0 ) of aqueous Na2 SO4 solutions as a function of temperature are studied. The maximum of

the B-coefficient near the 323 K isotherm has been found. The behavior of the concentration dependence of the relative viscosity of aqueous

Na2 SO4 solutions is discussed in terms of the modern theory of transport phenomena in electrolyte solutions. The derived values of the

viscosity A- and B-coefficients were compared with the results predicted by Falkenhagen–Dole theory of electrolyte solutions and calculated

with the ionic B-coefficient data. Different theoretical models for the viscosity of electrolyte solutions were stringently tested with new accurate

measurements on aqueous Na2 SO4 . The quality and predictive capability of the various models was studied. The measured values of viscosity

were directly compared with the data reported in the literature by other authors.

© 2004 Elsevier B.V. All rights reserved.

Keywords: Aqueous solutions; B-coefficient; Capillary viscometer; Sodium sulfate; Viscosity; Water

tion by supercritical water oxidation. Aqueous Na2 SO4 is

The association and hydrolysis of the sodium sulfate in also an important constituent of natural subsurface brines and

aqueous solutions is important in many industrial processes sea floor vent fluids. In addition, aqueous Na2 SO4 is a prime

such as material transport, solid deposition, corrosion in representative of 1:2 charge-type electrolytes. Knowledge of

steam generators, and electrical power boilers [1,2]. Sodium the pressure, temperature, and composition dependence of

viscosity of aqueous salt solutions is essential to understand

a variety of problems in a number of technological and en-

∗ Corresponding author. Present address: Physical and Chemical Proper-

gineering applications such as environmental applications,

ties Division, National Institute of Standards and Technology, 325 Broadway,

Boulder, Colorado 80305, USA. Tel.: +1 303 497 4027;

treatment of wastewater, geothermal power, and hydrother-

fax: +1 303 497 5224. mal formation of minerals. Characterization of the mass and

E-mail address: ilmutdin@boulder.nist.gov (I.M. Abdulagatov). heat transfer phenomena in the hydrothermal environments,

0378-3812/$ – see front matter © 2004 Elsevier B.V. All rights reserved.

doi:10.1016/j.fluid.2004.10.028

58 I.M. Abdulagatov et al. / Fluid Phase Equilibria 227 (2005) 57–70

design calculation, and flue and vent gases often requires to test the quality of previous studies by comprehensive com-

modeling of electrolyte solutions. The viscosity of aqueous parisons all of the available data sets; (3) to test the predictive

electrolyte solutions is of importance in many industrial and capability of the various theoretical models for the viscosity

scientific applications because the long-range electrostatic of electrolyte solutions with new accurate measurements on

interactions (coulombic forces between ions) present cause aqueous Na2 SO4 . The present results considerably expand

difficulty in describing ionic solutions [3–10]. Electrostatic the temperature, pressure, and concentration ranges in which

interactions determine thermodynamic and transport proper- viscosity data for aqueous Na2 SO4 solutions are available.

ties of ionic electrolyte solutions. A brief analysis some of the correlations of the viscosity of

In this paper, we report new precise viscosity measure- H2 O + Na2 SO4 solutions is given below.

ments for aqueous Na2 SO4 solutions over wide ranges of Korosi and Fabuss [23] represented measured values of

temperature, pressure, and composition using a capillary flow viscosity for H2 O + Na2 SO4 solutions as a linear function of

technique, which allows accurate measurements at high tem- the logarithm of the viscosity of water η0 (mPa s)

peratures and high pressures [11–16]. The research presented η

in this paper is part of a continuing series of measurements of log10 = A0 + B0 log10 η0 , (1)

η0

transport properties of aqueous solutions at high temperatures

and high pressures [11–13,15,16]. where the temperature independent constants A0 and B0 were

expressed as a function of ionic strength.

Glass and Madgin [19] reported the relative viscosity data

2. Literature review of the experimental viscosity for aqueous Na2 SO4 at atmospheric pressure in the temper-

data and correlations for H2 O + Na2 SO4 solutions ature range from 298 to 313 K for the compositions between

0.018 and 3.28 mol kg−1 . The Jones and Dole equation has

Table 1 shows the available viscosity data sets for been applied to dilute Na2 SO4 solution and the values of

H2 O + Na2 SO4 solutions. In this table, the first author, the A = 0.0155 and B = 0.357 coefficients has been found.

year published, and uncertainty are given together with Correla and Kestin [28] used the linear function of pres-

the method employed the temperature, pressure, and con- sure along the isotherm to correlate the measured values of

centration ranges. The available viscosity data sets for viscosity of aqueous Na2 SO4

H2 O + Na2 SO4 solutions included the measurements with η(P, t, c) = η0 (T, c)[1 + β(T, c)P], (2)

various techniques such as capillary flow, oscillating-disk vis-

cometer, and falling-body. Most of the data were obtained by where η0 (T, c) and β(T, c) are the hypothetical zero-pressure

the capillary technique. Most of the data sets cover very lim- viscosity (mPa s) and pressure coefficients (in GPa), respec-

ited ranges of temperature, pressure, and concentration. A tively, were correlated in term of temperature and concentra-

literature survey revealed that all previous reported viscosity tion.

data for aqueous Na2 SO4 solutions were performed at atmo- Millero et al. [24] reported the precision measurements of

spheric pressure except the data reported by Pepinov et al. the relative viscosity of dilute aqueous Na2 SO4 solutions. The

[26,27] and Correla and Kestin [28]. Thus, the main objec- results have been used to calculate viscosity B-coefficient in

tives of this work are: (1) to provide reliable experimental the Jones and Dole equation at temperatures 293.15, 298.15,

viscosity data for aqueous Na2 SO4 solutions at high temper- 303.15, 308.15, and 313.15 K. The derived results are 0.375,

atures (up to 573 K) and high pressures (up to 40 MPa); (2) 0.392, 0.398, 0.405, and 0.409 dm3 mol−1 , respectively. They

Table 1

Summary of the viscosity measurements for aqueous Na2 SO4 solutions

First author Year Uncertainty (%) Method Temperature range (K) Pressure range (MPa) Concentration range (molality)

ITC [17] 1928 0.3 CF 283–313 0.1 0.1–1.0

Herz [18] 1929 n.a. CF 293–363 0.1 0.5–4.0

Glass [19] 1934 n.a. OTV 298–313 0.1 0.018–3.28

Ezrokhi [20] 1953 n.a. CF 283–353 0.1 0.248–2.970

Kaminsky [21] 1956 n.a. CF 285–316 0.1 Up to 0.1

Chesnokov [22] 1962 0.05 CF 293.15 0.1 0.25–1.0

Korosi [23] 1968 0.1–0.2 GC 298–423 0.1 0.033–1.203

Millero [24] 1968 n.a. CUSLV 293–313 0.1 Dilute

Puchkov [25] 1974 1.5 FB 298–573 0.1–2 0.486–2.274

Pepinov [26,27] 1978, 1992 1.0 CF 293–573 2–30 0.1–0.782

Correla [28] 1981 1.0 ODV 293–363 0.1–30 0.56–1.104

Maksimova [29] 1987 0.5 CF 293–363 0.1 0.1–2.87

This work 2004 1.5 CF 298–573 Up to 40 0.107–2.473

CF: capillary flow; FB: falling-body; GC: glass capillary; ODV: oscillating-disk viscometer; OTV: Ostwald type viscometer; CUSLV: Cannon–Ubbelohde type

suspended level viscometer; n.a.: no uncertainty given in source reference.

I.M. Abdulagatov et al. / Fluid Phase Equilibria 227 (2005) 57–70 59

found that the B-coefficient goes through a maximum near The final working equations for this method is

318–323 K. Kaminsky [21] reported viscosity B-coefficients

ρ ρc ρc

0.375, 0.381, 0.399, 0.398, and 409 dm3 mol−1 for the η = Uτ 1− (1 + α t)3 − W ,

Na2 SO4 solutions at temperatures 293.15, 298.15, 303.15, ρc ρHg τ

308.15, and 313.15 K, respectively. The B-coefficients ob- gπR4 H0 ρ0,Hg mVc

tained by Kaminsky [21] increase linearly with temperature. U= and W= , (5)

8LVC 8πL

Moulik and Rakshit [30] correlated the relative viscos-

ity data for H2 O + Na2 SO4 solutions with the B-coefficients. where R = 0.15091 ± 0.0005 mm is the inner radius of the

They proposed a general polynomial form to represent the capillary, L = 540.324 ± 0.005 mm the capillary tube length,

experimental viscosity data for electrolyte solutions in the τ the time of flow, α the linear expansion coefficient of the

concentration range of 0.1–1 m capillary material, t the temperature difference between

experimental temperature and room temperature, m = 1.12 a

η n constant, ρ(P, T) the density of the fluid under study at the

= 1 + Bc + (B2 ) c(1+l) , (3)

η0 experimental conditions (P, T), VC = 1.2182 cm3 the volume

of the unmovable (measuring) cylinder, ρc the density of the

where B is the viscosity B-coefficient in the Jones and Dole fluid under study at room temperature and experimental pres-

equation, l a constant whose values are restricted within sure, (H0 = (H1 –H2 )/ln(H1 /H2 )), where H1 and H2 are the

the limits 1 ≤ l ≤ 2, and c is the concentration in m. For mercury levels at the beginning and ending of fluid flow, re-

H2 O + Na2 SO4 solutions, the values of the constants n and l spectively, at room temperature and atmospheric pressure,

are equal 1. Moulik and Rakshit [30] reported the values of ρHg the density of mercury at room temperature and exper-

the B-coefficient for H2 O + Na2 SO4 solutions at five temper- imental pressure, ρ0,Hg is the density of mercury at room

atures between 298 and 333 K. temperature and atmospheric pressure.

Aseyev [31] represented available experimental viscosity The values of the parameters U and W can be also deter-

data from the literature for H2 O + Na2 SO4 solutions by fol- mined by means of a calibration technique. The volume of

lowing correlation equation: the unmovable cylinder VC was determined using a weighing

technique [11]. Eq. (5) takes into account the acceleration of

log10 η = log10 η0 + (1.418 + 0.00099t)x, (4) a fluid at the inlet and outlet, the variation of the geometrical

sizes of the capillary with T and P, the mercury and sam-

where η0 (mPa s) is the viscosity of pure water, x the com- ple densities at the experimental conditions were varied with

position (mass fraction) and t is the temperature (◦ C). The temperature and pressure.

absolute uncertainty of the calculated values of the viscosity The time period for fluid flow through the capillary, τ, was

of H2 O + Na2 SO4 is 0.0855 Pa s. measured with a stopwatch with an uncertainty of less than

0.1 s (0.5%). All values of τ are averages of at least 5–10

measurements. At a temperature of 573 K, the minimal value

3. Experimental apparatus and procedures of τ was 40 s.

At the maximum measured temperature (573 K), the val-

The apparatus for the determination of the viscosity of ues of the root-mean-square deviations in the viscosity mea-

a aqueous Na2 SO4 was the same as that used to measure surements was δη = 2 × 10−5 g cm−1 c−1 . Based on the de-

the viscosity of aqueous LiNO3 , BaNO3 , Ca(NO3 )2 , MgCl2 , tailed analysis of all sources of uncertainties likely to affect

and BaCl2 in earlier studies [11–13,15,16]. The details of the determination of viscosity with the present apparatus, the

the apparatus, procedures and uncertainties of the measured combined maximum relative uncertainty δη/η in measuring

quantities have been provided in previous papers [11–13]. the viscosity was 1.5% (see [11]). The experimental uncer-

Only essential information will be given here. The measure- tainty in the concentration is estimated to be 0.015%.

ments were made using a capillary flow method, which gives To maintain laminar flow in the capillary the Reynolds

an uncertainty of 1.5% for the viscosity. The main parts of (Re) number was less that the critical value (Rec = 300) during

the apparatus consisted of a working capillary, a high tem- all measurements.

perature and high-pressure autoclave, movable and unmov- As one can see from Eq. (5), the values of density ρc (T0 ,

able cylinders, electrical heaters, and solid red copper block. P) of the solution under study at room temperature and exper-

The capillary and extension tubes were located in the high imental pressure, and density at the experimental conditions

temperature and high-pressure autoclave. The autoclave was ρ(P, T) are needed to calculate the dynamic viscosity from

placed in a solid red copper block. Two electrical heaters measured quantities. For this aim we used the density data

were wound around the surface of the copper block. To cre- measured in our previous paper [32] for aqueous Na2 SO4 so-

ate and measure the pressure, the autoclave was connected lutions at high temperatures (up to 573 K) and high pressures

with a dead-weight pressure gauge (MP-600) by means of (up to 40 MPa).

separating vessel. The uncertainty in pressure measurements As a check of the method and procedure of the measure-

was 0.05%. ments, the viscosity of pure water was measured from 296

60 I.M. Abdulagatov et al. / Fluid Phase Equilibria 227 (2005) 57–70

Table 2

Experimental viscosities, pressures, and temperatures of pure water

P (MPa) η (mPa s)

296.70 (K) 338.30 (K) 372.40 (K) 413.62 (K) 469.40 (K) 500.22 (K) 544.23 (K) 573.70 (K)

5 0.918 0.431 0.286 0.196 – – – –

10 0.917 0.434 0.287 0.197 0.138 0.120 0.0983 0.0860

20 0.915 0.435 0.288 0.201 0.141 0.123 0.1012 0.0891

40 0.914 0.440 0.293 0.205 0.145 0.127 0.1060 0.0950

to 574 K at pressures up to 40 MPa. Table 2 provides the viscosity is little affected (up to 5%) at high temperatures

present experimental viscosity data for pure water measured (573 K) and up to 1% at low temperatures (298 K) by pres-

using the same experimental apparatus. These data were com- sure changes between 0.1 and 40 MPa along the isotherms

pared with values calculated from the IAPWS [33] formula- (see Fig. 3). Fig. 5 shows the temperature dependence of

tion (see Fig. 2a). The agreement between IAPWS [33] calcu- the experimental values of the viscosity pressure coefficient

lations and the present results along the isobars 5, 10, 20, and αP = −1 (∂η/∂P)TX for two H2 O + Na2 SO4 solutions (5 and

40 MPa is good. Deviation statistics for the present viscosity 10 mass%) at fixed pressure of 10 MPa together with values

data for pure water and values calculated with IAPWS [33] for pure water. From the data obtained, it can be concluded

formulation are as follows: AAD = 0.41%, Bias = −0.18%, that the pressure coefficients αP is always positive and almost

S.D. = 0.48%, S.E. = 0.10%, and Max. Dev. = 0.89% (N = 23). independent of the concentration.

This good agreement between the present viscosity results The experimental values of the viscosity for H2 O +

and IAPWS [33] calculations for pure water is confirms Na2 SO4 solutions reported here were directly compared

the reliability and high accuracy of the measurements for with the data reported by other authors in the literature.

H2 O + Na2 SO4 solutions and correct operation of the present Figs. 1(a and b)–4 contains the values of viscosity reported by

instrument. various authors from the literature together with the present

Chemically pure Na2 SO4 and distilled water were used to results. As one can see from these figures, the agreement be-

prepare the solutions. The solutions at the desired concentra- tween various data sets is good. Figs. 1(a and b)–4 illustrate

tion were prepared by the gravimetric method, and the con- that our data are consistent with literature values at atmo-

centration was checked using the density at 20 ◦ C by means spheric and high pressures and various temperatures. The ac-

of pycnometers with reference data. ceptable agreement within ±1.5% was found between present

measurements and the data reported by Pepinov et al. [26,27]

at high pressures (10 and 30 MPa) and concentration of 5 and

4. Results and discussion 10 mass%, while at low pressures the deviations are within

0.65%. Excellent agreement within ±0.75% was found be-

The viscosity, η, measurements for aqueous Na2 SO4 so- tween present results and the data reported by Phuchkov and

lutions has been made in the temperature range from 298 to Sargaev [25] at concentrations 15 and 20 mass% and at tem-

573 K at pressures up to 40 MPa for nine compositions 1.5, peratures up to 348 K, while at low temperatures (298.15 K)

3, 5, 7, 10, 15, 20, 23, and 26 mass%. All experimental vis- an outlying data point shows the deviation up to 2%. The data

cosity data were obtained as a function of temperature at five reported by Maksimova et al. [29] at atmospheric pressure

isobars 0.1, 10, 20, 30, and 40 MPa. The experimental tem- and concentrations 10 and 15 mass% are systematically lower

perature, viscosity, pressure, and composition values for the (up to 3–4%) than the present results and other viscosity data,

aqueous Na2 SO4 solutions are presented in Table 3. Some although at low concentrations (5 mass%) the deviations are

selected experimental viscosity data for H2 O + Na2 SO4 so- within their experimental uncertainty (0.85%). Good agree-

lutions as an example of the present results are shown in ment within 0.5 to 1.3% is observed between present data and

Figs. 1(a and b)–4 in the η–T, η–P, and η–m projections to- the data reported by Glass and Madgin [19] and the data by

gether with values calculated from the IAPWS [33] formu- Korosi and Fabuss [23]. Differences between our measure-

lation for pure water (x = 0). To check the reproducibility of ments and the values calculated with the correlation of Eq.

the experimental data, the measurements of the viscosity re- (3) within (1.0–1.5%), which is less than their experimental

peated 5–10 times at the same selected temperature and pres- uncertainty. The deviation plots between present data and the

sure. The scattering of the experimental data is within of ±0.2 values calculated with correlations (2) and (4) are given in

to 0.4%. Figs. 1(a and b)–4 contains also the data reported by Figs. 6 and 7. Table 4 provides the deviation statistics for

other authors and calculated with correlation Eqs. (2) and (4) correlation (2). Maximum deviations of up to 3–4% were ob-

by Correla and Kestin [28] and Aseyev [31], respectively. As served at high temperatures and high concentrations (extrap-

one can see from Fig. 3, the viscosity of the solution at con- olated values) where the correlation (2) is not valid. At low

stant composition (x = 5 mass%) and selected temperatures concentrations (<3 mass%) the agreement between present

is slightly increases linearly as the pressure increases. The data and the correlation (2) extrapolated to high temperatures

I.M. Abdulagatov et al. / Fluid Phase Equilibria 227 (2005) 57–70 61

Experimental viscosities, pressures, temperatures, and concentrations of

T (K) η (mPa s)

H2 O + Na2 SO4 solutions

T (K) η (mPa s) 0.1 (MPa) 10 (MPa) 20 (MPa) 30 (MPa) 40 (MPa)

421.40 – 0.2535 0.2565 0.2596 0.2635

0.1 (MPa) 10 (MPa) 20 (MPa) 30 (MPa) 40 (MPa)

447.20 – 0.2125 0.2163 0.2189 0.2219

x = 1.5 (mass%) 471.31 – 0.1847 0.1878 0.1904 0.1941

298.15 0.9330 0.9335 0.9365 0.9399 0.9420 498.22 – 0.1618 0.1641 0.1786 0.1711

323.70 0.5669 0.5741 0.5795 0.5821 0.5835 525.40 – 0.1430 0.1469 0.1493 0.1524

348.15 0.3950 0.3977 0.4006 0.4038 0.4087 547.90 – 0.1296 0.1329 0.1360 0.1399

373.80 – 0.2947 0.2994 0.3034 0.3065 573.20 – 0.1143 0.1178 0.1204 0.1266

399.01 – 0.2321 0.2367 0.2398 0.2412

422.61 – 0.1927 0.1968 0.1999 0.2022 x = 15 (mass%)

447.60 – 0.1633 0.1684 0.1700 0.1724 298.15 1.5450 1.5480 1.5500 1.5510 1.5540

470.70 – 0.1432 0.1468 0.1499 0.1508 323.40 0.9286 0.9316 0.9354 0.9401 0.9450

498.30 – 0.1248 0.1286 0.1307 0.1325 348.70 0.6292 0.6336 0.6367 0.6418 0.6473

520.64 – 0.1128 0.1165 0.1191 0.1209 372.80 – 0.4705 0.4743 0.4795 0.4840

547.90 – 0.1000 0.1025 0.1068 0.1089 395.40 – 0.3731 0.3767 0.3810 0.3860

421.30 – 0.2998 0.3027 0.3087 0.3114

x = 3 (mass%) 447.60 – 0.2493 0.2551 0.2575 0.2603

298.15 0.9746 0.9759 0.9769 0.9799 0.9812 473.93 – 0.2133 0.2169 0.2991 0.2240

323.15 0.5972 0.5991 0.6012 0.6054 0.6090 497.80 – 0.1892 0.1945 0.1978 0.2001

348.35 0.4107 0.4134 0.4169 0.4200 0.4225 522.40 – 0.1686 0.1709 0.1748 0.1790

372.90 – 0.3096 0.3124 0.3164 0.3186 547.70 – 0.1510 0.1548 0.1589 0.1634

398.40 – 0.2422 0.2468 0.2494 0.2510 570.50 – 0.1354 0.1399 0.1463 0.1496

421.50 – 0.2013 0.2035 0.2068 0.2090

447.81 – 0.1686 0.1705 0.1734 0.1761 x = 20 (mass%)

473.70 – 0.1456 0.1486 0.1514 0.1530 298.15 1.9630 1.9650 1.9660 1.9670 1.9680

497.10 – 0.1296 0.1312 0.1360 0.1375 323.15 1.1680 1.1700 1.1760 1.1810 1.1850

523.30 – 0.1150 0.1169 0.1196 0.1219 347.90 0.7892 0.7944 0.8004 0.8053 0.8110

549.90 – 0.1023 0.1065 0.1086 0.1109 374.50 – 0.5699 0.5743 0.5799 0.5875

572.62 – 0.0920 0.0967 0.0992 0.1020 397.21 – 0.4505 0.4540 0.4598 0.4654

420.30 – 0.3686 0.3729 0.3775 0.3826

x = 5 (mass%) 444.81 – 0.3083 0.3129 0.3175 0.3219

298.15 1.0350 1.0400 1.0410 1.0420 1.0440 472.30 – 0.2608 0.2661 0.2699 0.2739

323.80 0.6285 0.6320 0.6330 0.6360 0.6385 497.19 – 0.2292 0.2335 0.2387 0.2425

347.20 0.4434 0.4465 0.4496 0.4530 0.4587 523.80 – 0.2021 0.2076 0.2105 0.2160

371.95 – 0.3317 0.3350 0.3389 0.3430 545.40 – 0.1840 0.1879 0.1923 0.1989

395.62 – 0.2626 0.2668 0.2695 0.2716

424.67 – 0.2079 0.2096 0.2130 0.2164 x = 23 (mass%)

446.24 – 0.1796 0.1820 0.1853 0.1879 303.15 1.9930 1.9930 1.9960 1.9990 2.0020

470.16 – 0.1564 0.1598 0.1629 0.1647 323.15 1.3330 1.3360 1.3400 1.3460 1.3530

499.30 – 0.1352 0.1363 0.1392 0.1430 348.70 0.8925 0.8987 0.9053 0.9128 0.9200

524.70 – 0.1204 0.1231 0.1267 0.1286 370.40 – 0.6799 0.6864 0.6905 0.6997

545.30 – 0.1097 0.1120 0.1143 0.1177 398.80 – 0.5081 0.5124 0.5185 0.5253

572.96 – 0.0965 0.0998 0.1029 0.1066 422.51 – 0.4132 0.4195 0.4254 0.4300

447.90 – 0.3449 0.3498 0.3568 0.3609

x = 7 (mass%) 472.00 – 0.2966 0.3024 0.3086 0.3120

298.15 1.1190 1.1190 1.1190 1.1210 1.1220 496.34 – 0.2620 0.2695 0.2734 0.2776

323.25 0.6825 0.6846 0.6875 0.6902 0.6935 520.51 – 0.2338 0.2387 0.2415 0.2490

347.60 0.4733 0.4764 0.4795 0.4824 0.4875 548.70 – 0.2061 0.2106 0.2186 0.2230

373.90 – 0.3482 0.3508 0.3546 0.3590

397.10 – 0.2772 0.2799 0.2834 0.2870 x = 26 (mass%)

425.60 – 0.2211 0.2267 0.2293 0.2300 303.15 2.2430 2.2450 2.2490 2.2530 2.2590

447.00 – 0.1913 0.1946 0.1975 0.1998 323.15 1.5040 1.5050 1.5090 1.5150 1.5230

472.20 – 0.1656 0.1689 0.1706 0.1739 348.60 1.0100 1.0170 1.0230 1.0290 1.0410

498.70 – 0.1451 0.1489 0.1506 0.1533 375.20 – 0.7321 0.7395 0.7436 0.7535

523.10 – 0.1298 0.1324 0.1367 0.1385 399.40 – 0.5695 0.5739 0.5800 0.5895

546.20 – 0.1171 0.1197 0.1224 0.1267 423.80 – 0.4623 0.4688 0.4726 0.4803

573.50 0.1031 0.1068 0.1092 0.1143 447.60 – 0.3901 0.3981 0.4010 0.4047

473.90 – 0.3308 0.3354 0.3413 0.3476

x = 10 (mass%) 498.70 – 0.2923 0.2976 0.3018 0.3090

298.15 1.2520 1.2550 1.2560 1.2570 1.2580 520.50 – 0.2636 0.2691 0.2746 0.2813

323.05 0.7656 0.7670 0.7710 0.7745 0.7780

348.42 0.5232 0.5267 0.5294 0.5340 0.5399

372.40 – 0.3948 0.3979 0.3998 0.4062

398.72 – 0.3052 0.3094 0.3132 0.3159

62 I.M. Abdulagatov et al. / Fluid Phase Equilibria 227 (2005) 57–70

Fig. 1. (a and b). Measured values of viscosity of H2 O + Na2 SO4 solutions as a function of temperature along the four selected concentrations and at atmospheric

pressure together with values reported by other authors from the literature: (a) 10 mass%; (b) curve 1–20 mass%, curve 2–15 mass% and curve 3–5 mass%.

data still is good (deviations within ± 2%). The deviation example, the A-coefficient of the Jones–Dole equation is

statistics for the correlation (4) at atmospheric pressure are: determined by ion–atmosphere interaction and ionic mo-

AAD = 1.22, Bias = −0.78, S.D. = 1.24, S.E. = 0.3, and Max. bilities and can be calculated from theory [34,35]. Low

Dev. = 2.42. This excellent agreement between present and concentration viscosity measurements for aqueous elec-

published data at atmospheric and high pressures also con- trolyte solutions show good agreement between experi-

firms the reliability of the present measurements and its con- ment and theory [21,36–39]. The second Jones–Dole pa-

sistency with literature data. Good agreement within 1.25% rameter B is related to the size and the shape of the ions

was found also between present data and the values calculated and the solute–solvent interactions [3]. Therefore, viscos-

with correlation (4) at high pressures (see Fig. 2a and b). ity A- and B-coefficients of electrolyte solutions are useful

The measured viscosities were used to calculate viscosity tools in study structural interactions (ion–ion, ion–solvent,

A- and B-coefficients of the Jones–Dole equation for vari- and solvent–solvent) in solutions. An extensive compila-

ous isotherms. The values of viscosity A- and B-coefficients tion of Jones–Dole A- and B-coefficients for aqueous elec-

of an electrolyte provide information on the interaction trolyte solutions is reported by various authors [3,4,21,

between dissolved ions and molecules of a solvent. For 36–49].

I.M. Abdulagatov et al. / Fluid Phase Equilibria 227 (2005) 57–70 63

Fig. 2. (a and b). Measured values of viscosity of H2 O + Na2 SO4 solutions as a function of temperature at selected concentrations (5 and 10 mass%) and at

pressures (10 and 30) MPa together with data reported by other authors.

The viscosity B-coefficient for aqueous solutions shows correctly explains the rise of viscosity with concentration in

strong temperature dependence, which can be attributed to the limit of very low (dilute solutions) ion concentrations

ion–solvent interactions. However, measurements of the tem- (c < 0.05 mol l−1 ). This model was based on macroscopic

perature dependence of the A- and B-coefficients have so consideration. Therefore, this model is inadequate when in-

far been limited to rather narrow ranges of temperature (up termolecular correlation becomes important. Jones and Dole

to 368 K) with less satisfactory accuracy. We examine the [53] proposed an empirical extension of the Falkenhagen

viscosity A- and B-coefficients values of aqueous Na2 SO4 [35] model to high concentrations as

solutions as a function of temperature in the temperature √

η(P, T, c)

range from 298 to 573 K. We also sufficiently extended the = 1 + A c + Bc, (6)

concentration range of the viscosity measurements to accu- η0 (P, T )

rately determine high degree coefficients (B, D, and F) in the for the viscosity of electrolyte solutions. In Eq. (6), η and

Jones–Dole equation. η0 are the viscosities of an electrolyte solution and pure

Falkenhagen–Onsager–Fuoss [35,50] and Debye– solvent (water), respectively, A an always positive constant,

Hückel–Onsager [51,52] theory predicts a square root

√ and c the electrolyte molarity concentration (mol l−1 ). This

concentration, η(P,T,c)

η0 (P,T ) ∝ c, dependence of the viscosity equation is valid only for concentrations below 0.1 mol l−1

of ionic solutions at infinite dilution (c → 0). This theory and provides a better description of the experimental vis-

64 I.M. Abdulagatov et al. / Fluid Phase Equilibria 227 (2005) 57–70

Fig. 3. Measured values of viscosity of H2 O + Na2 SO4 solutions (open symbols) as a function of pressure at selected concentration (5 mass%) and at various

temperatures together with data reported by other authors. Open symbols are present results and filled symbols are reported by Pepinov et al. [26,27].

∗ Fe2 NA (1 + 2)

long-range coulombic force interactions and the mobilities A = ,

of solute ions and B is the results of interactions between the 12π(ε∗ k)1/2

solvent and ions and ions size. The sign of the B-coefficient z2 (λ∞ ∞

+ + λ− ) 4(λ∞ ∞ 2

+ − λ− )

depends on the degree of solvent structuring introduced by f = √ 1− √ 2 ,

4(2 + 2)(λ∞ ∞

+ λ− ) (1 + 2) (λ∞ ∞ 2

+ + λ− )

the ions. A positive value of the B-coefficient is associ-

(8)

ated with structure-making (ordering) ions, while a negative

value of B-coefficient is associated with structure-breaking

(disordering) ions. Falkenhagen and Dole [54] gave a the- where A* = 1.113 × 10−5 ◦ C2 (m K mol−3 )1/2 ,

oretical derivation of the A- coefficient. Its general form f (λ∞ ∞

+ , λ− , z+ , z− ) is the function of the equivalent con-

is ductance λ∞ ± at infinite dilution of the ions, and z± are the

charges. The value of parameter A depends also on the vis-

A∗ cosity of the solvent η0 , its relative permittivity (dielectric

A= f (λ∞ ∞

+ , λ− , z+ , z− ), (7)

η0 (ε0 T )1/2 constant) ε0 , and the temperature T.

Fig. 4. Measured values of relative viscosity (η/η0 ) of H2 O + Na2 SO4 solutions as a function of concentration m along the isotherms of 298.15 K and at

atmospheric pressure together with values reported by other authors.

I.M. Abdulagatov et al. / Fluid Phase Equilibria 227 (2005) 57–70 65

Fig. 5. The viscosity pressure coefficient, αP = −1 (∂η/∂P)TX , of H2 O + Na2 SO4 solutions and pure water as a function of temperature at two selected concen-

tration (5 and 10 mass%) and at pressures 10 MPa together with values calculated with IAPWS [33] formulation for pure water.

various temperatures together with data reported by other au-

thors at low concentrations were used to calculate A- and B-

coefficients in Jones and Dole [53] Eq. (6). The B-coefficient

can be estimated from experimental viscosity data by extrap-

olating the function

(η/η0 ) − 1 − Ac1/2

B + Dc = , (9)

c

to zero concentration, using theoretical value of A or as slope

of the dependence [(η/η0 )−1 ]/c1/2 on c1/2 (Jones–Dole plot,

see Fig. 8a and b)

(η/η0 ) − 1

= A + Bc1/2 . (10)

c1/2

Fig. 6. Percentage viscosity deviations, δη = ((ηexp − ηcal )/ηexp ) × 100, of The present viscosity data for H2 O + Na2 SO4 solutions

the experimental viscosities for H2 O + Na2 SO4 from the values calculated are presented in Fig. 8(a and b) together with data reported

with correlation Eq. (2) by Correla and Kestin [28]. (䊉) 0.1 MPa; (
)

10 MPa; () 20 MPa; () 30 MPa and (×) 40 MPa.

by other authors at low concentrations in the Jones–Dole plot

[(η/η0 )−1 ]/c1/2 versus c1/2 for the two selected temperatures

of 298.15 and 323.15 K. The coefficients A and B, the

intercept, and the slope, respectively of a Jones–Dole plot,

were calculated using least-squares analysis of the present

data and the data reported in other studies from the literature

Table 4

Deviation statistics between present viscosity results and the values calcu-

lated with Correla and Kestin [28] correlation (2)

x (mass%) AAD Bias S.D. S.E. Max. Dev.

Fig. 7. Percentage viscosity deviations, δη = ((ηexp − ηcal )/ηexp ) × 100, of 1.5 0.64 −0.21 0.76 0.18 0.86

the experimental viscosities for H2 O + Na2 SO4 from the values calcu- 3.0 1.69 −0.61 1.91 0.39 3.00

lated with correlation Eq. (4) by Aseyev [31] at atmospheric pressure. (䊉) 5.0 0.91 −0.39 1.17 0.31 2.60

1.5 mass%; (
) 3 mass%; (×) 5 mass%; () 7 mass%; () 10 mass% and P = 0.1 MPa 0.73 −0.44 0.86 0.22 2.50

() 15 mass%. All data 1.21 −0.50 1.47 0.20 3.00

66 I.M. Abdulagatov et al. / Fluid Phase Equilibria 227 (2005) 57–70

Fig. 8. (a and b). Jones–Dole plot [(η/η0 )−1]/c1/2 vs. c1/2 for H2 O + Na2 SO4 solutions for isotherm of (a) 298.15 K and (b) 323.15 K at atmospheric pressure.

Table 5

The viscosity A-, B-, D-, and F-coefficients of aqueous Na2 SO4 solutions as a function of temperature

T (K) A (dm3/2 mol−1/2 ) B (dm3 mol−1 ) D (dm6 mol−2 ) F (dm7.5 mol−2.5 )

P = 0.1 (MPa)

298.15 0.0155 0.386 0.030 0.137

323.15 0.0162 0.403 0.020 0.100

348.15 0.0150 0.390 0.015 0.105

P = 10 (MPa)

298.15 0.0155 0.386 0.030 0.137

323.15 0.0160 0.400 0.020 0.100

348.15 0.0150 0.390 0.015 0.104

373.15 0.0142 0.385 0.010 0.105

423.15 0.0140 0.365 0.009 0.110

473.15 0.0140 0.355 0.009 0.120

523.15 0.0140 0.350 0.009 0.140

573.15 0.0140 0.350 0.009 0.230

I.M. Abdulagatov et al. / Fluid Phase Equilibria 227 (2005) 57–70 67

for various temperatures. As Fig. 8(a and b) shows, the data bic interaction, size and shape effects or Einstein effect,

lie on the straight line with negligible scatter in the concen- alignment or orientation of polar molecules by the ionic

tration range c < 0.1 mol l−1 , but this concentration range field, and distortion of the solvent structure [3]). These ef-

might change with temperature. The results are summarized fects govern the viscosity behavior of the aqueous electrolyte

in Table 5 and presented in Fig. 9(a and b) as a function of solutions.

temperature together with values reported by other authors Jones and Talley [38], Kaminsky [21,36], Desnoyers and

and calculated from theory. The agreement between A- and Perron [44], Feakins and Lawrence [66], Desnoyers et al.

B-coefficients derived in present study and calculated with [67], and Robertson and Tyrrell [68], added a quadratic term

theory and ionic B-coefficients data is good (see Fig. 9a (extended Jones–Dole equation)

and b). As one can see from Fig. 9(a and b), both A- and

B-coefficients go through a maximum (dB/dT = 0) near the η(P, T, m) √

= 1 + A c + Bc + Dc2 , (11)

323 K. At temperatures below about 323 K the derivative η0 (P, T )

(temperature coefficient) dB/dT > 0 (structure-breaking ions)

is positive, while above the temperature of 323 K, dB/dT < 0 to extend the Jones–Dole equation for more concentrated

(structure-making ions) [41,55,56]. The B-coefficients, ob- electrolyte solutions (c < 0.1–0.2 m). The new Dc2 term of Eq.

tained by other authors in all previous studies (except [24]), (11) accounts for all solute–solvent and solute–solute

√ struc-

increase almost linearly (see Fig. 9b) with temperature in the tural interactions that were not accounted by the A c and Bc

temperature range up to 313 K. Millero et al. [24] showed terms at high concentrations such as [3,44]: high terms of the

that B-coefficient goes through a maximum near 318–323 K. long-range coulombic forces; high term hydrodynamic ef-

Since B-coefficient is proportional to the partial molar fect; and interactions arising from changes in solute–solvent

volumes of a salt V̄ (see for example, Refs. [41,44,48]), interactions with concentration. The range of the concentra-

or hydration volume, one would expect (dB/dT) to be tion in present study overlaps the range where Dc2 term is

proportional (dV̄ /dT ). As shown by various authors (see for essential. In present study we added an extra term in c2.5 for

example, Refs. [32,57–65]) for aqueous electrolyte solutions application of Eq. (11) to higher concentration

the partial molar volume goes also through maximum within

the same temperature range. Our earlier PVTx and partial η(P, T, m) √

= 1 + A c + Bc + Dc2 + Fc2.5 . (12)

molar measurements [32] for aqueous Na2 SO4 showed η0 (P, T )

that the partial molar volume goes through maximum at

a temperature of 323 K. Therefore, indirect studies of the The relative viscosities for aqueous Na2 SO4 were fitted,

volumetric properties of aqueous Na2 SO4 also confirmed the up to 2.5 m, with the relation (12). The values of the A-, B-,

maximum in temperature dependence of the B-coefficient. D-, and F-coefficients calculated with present viscosity data

Cox and Wolfenden [49] assumed the additivity of the together with data reported by other authors at low concen-

ionic B-coefficients. This additivity, B = 'νi Bi , where the trations are presented in Table 5 for various temperatures. As

summation extends over all the ions present and the ionic one can see from this table the values of the D-coefficient

B-coefficients Bi . The values of Bi are constant at a given are monotonically decreasing with temperature. The temper-

T for given ions in a specific solvent and describe solely the ature dependence of the viscosity D-coefficient for aqueous

ion–solvent interactions. The present results for B-coefficient Na2 SO4 is depicted in Fig. 9(c) together with the values re-

show good agreement with the data estimated from the addi- ported by other authors. Present values of the D-coefficients

tivity principle (see Fig. 9b). are good agreement with the data reported by Kaminsky [21]

For electrolyte solutions like aqueous Na2 SO4 , the viscos- (see Fig. 9c).

ity B-coefficient is positive. At 298.15 K, the B-coefficients Lencka et al. [10] developed the model for multicompo-

values for Na+ are 0.085 and 0.206 for SO4 2− (structure- nent, concentrated electrolyte solutions. They developed the

ordering ion) is positive, typical of ions that are strongly hy- method for calculating viscosity of aqueous systems rang-

drated [48]. The values of the B-coefficients for Na+ and ing from dilute to very concentrated. Chandra and Bagchi

SO4 2− ions become less positive as the temperature is de- [7,8] developed a new microscopic model for the ionic con-

creasing [48]. There are other types of electrolyte solu- tribution to the viscosity of dilute electrolyte solutions on the

tions (for example, H2 O + KNO3 , H2 O + KBr, H2 O + KCl, basis of mode coupling theory. They presented a microscopic

H2 O + KI, H2 O + RbCl, and H2 O + CsCl) for which the vis- study of the concentration dependence of viscosity of an elec-

cosity decreases with concentration at low electrolyte con- trolyte solution. This theory predicts a stronger increase of

centrations reaching a minimum value, then increasing mono- viscosity with concentration than classical theory of Falken-

tonically for higher concentrations. For these type electrolyte hagen [35]. According this theory, at finite concentration the

solutions the B-coefficient is negative. The observed viscos- viscosity increases nonlinearly with square root of concen-

ity changes result from competition between various effects tration contrary to the Falkenhagen [35] equation.

occurring in the ionic neighborhood. At a given concentra- Jiang and Sandler [5] developed a new statistical

tion, the B-coefficient can be interpreted in terms of a com- mechanics-based model for the viscosity of electrolyte so-

petition between specialized viscosity effects as (coulom- lutions. This model based on the combination of liquid-state

68 I.M. Abdulagatov et al. / Fluid Phase Equilibria 227 (2005) 57–70

Fig. 9. (a–c). Experimental viscosity A-, B-, and D-coefficients of the H2 O + Na2 SO4 solutions as a function of temperature together with values reported by

other authors from the literature. The solid curve is to guide the eye.

I.M. Abdulagatov et al. / Fluid Phase Equilibria 227 (2005) 57–70 69

Fig. 10. Comparison of the concentration dependence of the present experimental relative viscosity results for H2 O + Na2 SO4 solutions with values calculated

from various theoretical models and correlations at atmospheric pressure and at two temperatures of 298.15 and 323.15 K.

theory and absolute-rate theory in the liquid phase with a capillary flow technique. Measure-

ments were made at five isobars 0.1, 10, 20, 30, and 40 MPa.

η(P, T, c) √ fEX

= (1 + a c + bc) exp , (13) The range of temperatures was from 298 to 573 K. The total

η0 (P, T ) RT uncertainty of viscosity, pressure, temperature, and concen-

where fEX is the excess contribution of the activation tration measurements was estimated to be less than 1.5%,

Helmholtz energy of the solution with the pure solvent. Jiang 0.05%, 15 mK, and 0.015%, respectively. The reliability and

and Sandler [5] provided the analytical expression for hard- accuracy of the experimental method was confirmed with

sphere and electrostatic contributions fEX = fHS + fEL . The pa- measurements on pure water. The experimental and calcu-

rameters a and b in Eq. (13) have physical meaning. As is the lated values of viscosity for pure water from IAPWS [33]

case for the parameter B in the Jones–Dole Eq. (6), the b formulation show excellent agreement within their experi-

value indicates the degree of order or disorder introduced by mental uncertainties (AAD = 0.41%). The measured viscos-

ions into the solvent structure. The value of the parameter a ity values of solutions at atmospheric and high pressures were

was fixed at 1.6 [5]. Fig. 10 demonstrates the predictive ca- compared with the data reported in the literature by other

pability of the various models and correlation equations for authors. Good agreement (within ±0.5–1.3%) is found be-

the viscosity of electrolyte solutions over a wide concentra- tween the present measurements and the data sets reported

tion range. Different empirical and semi-empirical correla- by other authors in the literature. The temperature, pressure,

tions and microscopic theoretical models were directly fitted and concentration dependences of the relative viscosity (η/η0 )

to present viscosity data for aqueous Na2 SO4 . As Fig. 10 are studied. The values of the viscosity A- and B-, D-, and

shows, the statistical mechanics-based model by Jiang and F-coefficients of the extended Jones–Dole equation for the

Sandler [5] with three physical meaning fitting parameters relative viscosity (η/η0 ) of aqueous Na2 SO4 solutions as a

(σ1 + , ε1 , b) present viscosity data for aqueous Na2 SO4 solu- function of temperature are studied. The quality and predic-

tions as well as multiparametric emperical correlations which tive capability and validity of the various theoretical models

were directly fitted to the experiemntal data. This model can are tested.

reproduce all of the present experimental data with an AAD

that is comparable with empirical correlations.

Acknowledgment

erties Division at the National Institute of Standards and Tech-

Viscosities of nine compositions (1.5, 3, 5, 7, 10, 15, 20, nology for the opportunity to work as a Guest Researcher at

23, and 26) mass% of aqueous Na2 SO4 have been measured NIST during the course of this research.

70 I.M. Abdulagatov et al. / Fluid Phase Equilibria 227 (2005) 57–70

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