Solubility of N2O in and Density and Viscosity of Aqueous Solutions of

Jul 19, 2012 - Solubilities of N2O in and densities and viscosities of aqueous solutions of ammonia, piperazine (PZ), and their aqueous blends were ...
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Solubility of N2O in and Density and Viscosity of Aqueous Solutions of Piperazine, Ammonia, and Their Mixtures from (283.15 to 323.15) K Jinzhao Liu,† Shujuan Wang,† Ardi Hartono,‡ Hallvard F. Svendsen,*,‡ and Changhe Chen† †

Department of Thermal Engineering, Key Laboratory for Thermal Science and Power Engineering of Ministry of Education, Tsinghua University, 10084 Beijing, China ‡ Department of Chemical Engineering, Norwegian University of Science and Technology, NO-7491 Trondheim, Norway

ABSTRACT: Solubilities of N2O in and densities and viscosities of aqueous solutions of ammonia, piperazine (PZ), and their aqueous blends were measured at (283.15, 293.15, 303.15, 313.15, and 323.15) K. The experiments cover the mass fraction ranges: (1 to 30) mol % ammonia, (0.1 to 2) mol % PZ, and (1 to 11) mol % ammonia + (0.18 to 2) mol % PZ in the blended solutions. The results are compared with available data in the literature. The experimental density and viscosity data were correlated using two semiempirical correlations as a function of temperature and concentration of ammonia and PZ.

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INTRODUCTION The absorption of CO2 with amine-based absorbents (i.e., monoethanolamine (MEA), methyl diethanolamine (MDEA)) is an established and proven technology.1 However, drawbacks of normal alkanolamines are still high energy requirements and capital cost. The overall challenge is to bring these two factors down with new and environmentally acceptable solvents. Aqueous ammonia has recently been considered to have potential as an effective and economic solvent for CO2 capture based on low corrosion potential, low regeneration energy requirement, low cost, and low degradation rates.2−6 However, ammonia as an absorbent has two important issues to face. First, the reaction rate of CO2 absorption into aqueous ammonia is low compared with MEA, ethylenediamine (EDA), and other organic amine solutions.7 Second, aqueous ammonia at concentrations higher than 15 % has a high volatility.8 Organic amine solutions are considered as additives to aqueous ammonia. Piperazine (PZ) was found to be a very active promoter compared to other amines. Several studies report on the characteristics and performance of PZ activated blends such as PZ-activated aqueous MDEA, 2-amino-2-methyl1-propanol (AMP), and K2CO3. The patent of Alstom9 mentions the use of PZ as a promoter to the chilled ammonia absorbent. Therefore, using PZ-blended ammonia solution is considered to be a possible route to improve the absorption characteristics of © 2012 American Chemical Society

ammonia. The density and viscosity of aqueous absorbents are essential for the measurement of other physicochemical properties such as diffusivity, gas solubility, and reaction rate constants. As the kinetics are typically derived by the experiments based on mass transfer process, data of physical diffusivity and solubility of CO2 in aqueous ammonia and PZ solutions are required. However, due to the chemical reactions between CO2 and NH3/ PZ solutions, these properties are not possible to determine directly.10 It is suggested to use an “N2O analogy” to estimate the aforementioned physicochemical properties, since N2O resembles CO2 in molecular volume, configuration, and electronic structure, and it is a nonreactive gas in amine conditions.11−13 The density of aqueous ammonia solutions can be found in Perry’s Chemical Engineering handbook,14 but the temperature range is only from (−15 to 25) °C, which does not cover the important range for CO2. The viscosity of ammonia was studied by Frank et al.15 from (20 to 60) °C, but the experimental points are not numerous enough to fit an accurate correlation. The solubility of N2O in ammonia was only obtained by Qin16 from (20 to 50) °C using the same experimental system as this work. Received: January 3, 2012 Accepted: June 15, 2012 Published: July 19, 2012 2387

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Table 1. Densities and Viscosities of Standard Solution N1.0 and S3 for Calibration, at (293.15 to 323.15) K and 1 atm (1.01325·105 Pa)a density ρ/g·mL−1

viscosity η/mPa·s standard

T/K

meas.

ref.

deviation

meas.

ref.

deviation

N1.0

293.15 298.15 313.15 323.15 293.15 203.15 313.15 323.15

0.9968 0.9237 0.7540 0.6675 3.7033 3.2604 2.3233 1.9114

1.0010 0.9277 0.7531 0.6642 3.7090 3.2610 2.3160 1.9030

0.42 % 0.43 % −0.12 % −0.49 % 0.15 % 0.02 % −0.31 % −0.44 %

0.78268 0.77879 0.76723 0.75952

0.7827 0.7789 0.7674 0.7596

−0.002 % −0.014 % −0.022 % −0.011 %

S3

a

“meas.” stands for measured experimental values and “ref.” for the reference values.

Figure 1. Experimental setup of N2O solubility (Hartono et al.19).

Density and Viscosity. The densities of aqueous solutions were measured by using a DMA 4500 density meter in this work. The measuring range for density is (0 to 3) g·cm−3, for temperature (0 to 90) °C, and for pressure (0 to 10) bar. The accuracy in the density measurements was ± 0.00005 g·cm−3 and for temperature ± 0.03 °C. The repeatability standard deviation of density is 0.00001 g·cm−3 and for temperature 0.01 °C. The viscosities of aqueous solutions were measured by using an Anton Paar PHYSICA MCR 100 rheometer with a DG26.7/ Q1-SN18602 measuring system in this work. DG26.7/Q1 is a double gap cylinder measuring system (Standard: DIN 54453) with a cup length of 42 mm and measuring gap internal and external diameters of 0.417 mm and 0.471 mm. The procedure was done by filling the space of the cylinder with 3.8 mL of solution at a specific temperature. The temperature of the sample was controlled by means of a water circulation unit with the range of (5 to 80) °C and an accuracy of ± 0.01 °C. The total accuracy of viscosity given by the manufacturer is ± 0.1 %. Calibrations were done by measuring the density and the viscosity of standard solutions N1.0 and S3 (ISO 17025 Viscosity and Density Reference Standard, UKAS) in the temperature range between (293.15 and 323.15) K. The data for the calibration are given in Table 1. It can be seen that both density and viscosity from the measurements agree very well with the reference values for the

The solubility of N2O in and density and viscosity of PZ solutions were measured by Derks et al.,10 Sun et al.,17 and Samanta and Bandyopadhyay.18 However, their data do not cover the entire temperature and concentration range of this work, and comparisons have been made between the results of theirs and this work under the same conditions. The solubility of N2O in and density and viscosity of NH3/PZ mixtures have not been presented until now. In this study, the solubilities of N2O in and densities and viscosities of aqueous solutions of ammonia, PZ, and aqueous blends of ammonia and PZ have been measured at (283.15, 293.15, 303.15, 313.15, and 323.15) K, covering (1 to 30) mol % ammonia, (0.1 to 2) mol % PZ, and some of their mixtures. The results are compared with available data in the literature. The experimental density and viscosity data were correlated using two semiempirical correlations as a function of temperature and concentration of ammonia and PZ.

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EXPERIMENTAL SECTION Piperazine (> 99 % pure) and ammonia (≥ 25 wt %) were obtained from Sigma-Aldrich. Distilled water was used for preparing experimental solutions. The ammonia and PZ concentrations were determined by titration against 0.2 N H2SO4 using a Metrohm 809 Titrando auto titrator. The N2O gas (99.9991 vol % pure) was supplied by AGA Gas GmbH. 2388

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Table 2. Solubility of N2O (Mass Fraction w kg·kg−1) and the Distribution Coefficient m of N2O in Water, (293.15 to 323.15) K T/K PN2O/kPa

293.15 80.3

solubility of N2O wa/% distribution coefficient m a

298.15 70.9

0.0988 0.668

303.15 78.3

0.0743 0.580

313.15 88.7

0.0727 0.523

0.0643 0.423

323.15 92.7 0.0551 0.360

The uncertainty of the w measurement is ± 3 %.

Table 3. Densities of Aqueous NH3 (x1), PZ (x2) Solution, and NH3/PZ Blended Solution from (283.15 to 323.15) K and 1 atm (1.01325·105 Pa) Density ρa (g·mL−1) 100x1 (mol·mol−1) T/K

a

14

0

2.68

283.15 293.15 303.15 313.15 323.15

0.99970 0.99820 0.99565 0.99222 0.98804

0.98873 0.98679 0.98398 0.98032 0.97598

T/K

014

0.181

283.15 293.15 303.15 313.15 323.15

0.99970 0.99820 0.99565 0.99222 0.98804

1.00015 0.99863 0.99610 0.99266 0.98851

5.05

11.24

0.97982 0.95785 0.97750 0.95452 0.97443 0.95065 0.97059 0.94614 0.96609 0.94098 100x2 (mol·mol−1) 0.367

0.741

1.00051 1.00134 0.99898 0.99975 0.99642 0.99715 0.99299 0.99368 0.98881 0.98947 100x1/100x2 (mol·mol−1)

14.80

30.43

0.94497 0.94101 0.93667 0.93170 0.92612

0.89590 0.88982

1.119

1.938

1.00224 1.00058 0.99791 0.99437 0.99014

1.00470 1.00252 0.99969 0.99604 0.99164

T/K

1.08/0.182

2.52/0.183

5.00/0.185

7.98/0.187

5.89/0.373

7.79/0.376

283.15 293.15 303.15 313.15 323.15

0.99568 0.99400 0.99135 0.98782 0.98254 5.92/0.565

0.98992 0.98800 0.98519 0.98153 0.97717 10.84/0.575

0.98065 0.97834 0.97522 0.97141 0.96696 0.694/0.743

0.96931 0.96636 0.96289 0.95843 0.95379 2.82/0.745

0.97846 0.97593 0.97270 0.96825 0.96403 5.04/0.751

0.97108 0.96823 0.96472 0.96047 0.95562 10.96/0.766

283.15 293.15 303.15 313.15 323.15

0.97883 0.97627 0.97295 0.96894 0.96420

0.96034 0.95682 0.95281 0.94808 0.94289

0.99864 0.99692 0.99424 0.99070 0.98643

0.99037 0.98828 0.98531 0.98154 0.97710

0.98273 0.98029 0.97706 0.97303 0.96850

0.96249 0.95901 0.95485 0.94992 0.94495

The uncertainty of the ρ measurement is ± 0.01 %.

the compressibility factor. The amount of N2O in the liquid phase (nlN2O) can be calculated by the difference between total N2O added and the increasing of N2O in gas phase, and then the concentration of N2O (nlN2O) could be calculated. The solubility of N2O at different pressures and temperatures have been expressed as mass fraction w (kg·kg−1) in this paper and are also calculated as the distribution coefficient (m) to compare with other literature results.

standard solutions. The probable uncertainty in the measured density is about 0.01 %, and the estimated uncertainty in viscosity measurement is 0.3 %. Solubility of N2O. The N2O solubility apparatus contains a jacketed stirred glass vessel for which the volume is 7.76·10−4 m3 and a gas holding vessel made by stainless steel for which the volume is 1.17·10−3 m3. The amount of solvent added (around half of reactor) into the glass vessel was calculated by measuring the weight of solvent before and after transfer. The solution was degassed by vacuum to around 2 kPa at room temperature until vapor−liquid equilibrium in the reactor was reached. The experimental setup is shown in Figure 1. The details of the experimental apparatus and method are described by Hartono et al.19 The amount of N2O added (nN2O) was obtained by the difference of pressure before and after feeding N2O in supply vessel. In the gas phase, the amount of N2O (ngN2O) could be calculated by temperature (T), partial pressure of N2O (PN2O), and compressibility factor z of N2O after reaching equilibrium, respectively. The Peng−Robinson equation was used to calculate

PN2O = HN2OC Nl 2O

(1)

The relationship between the distribution coefficient and the Henry’s law constant can be expressed as in eq 2. m=

C Nl 2O C Ng 2O

=

C Nl 2O PN2O/RT

=

RT HN2O

(2)

Calibrations were done by measuring the solubility of N2O in water at different temperatures from (293.15 to 323.15) K and comparing the data to the literature. The data of solubility of N2O and the distribution coefficient in water are shown in Table 2389

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2, whereas the comparison of distribution coefficient mN2O with several literature references is shown in Figure 2.

Figure 4. Densities of PZ solution measured by this work compared with literature data.10,17,18,22 Colors: orange, 283.15 K; green, 293.15 K; purple, 303.15 K; red, 313.15 K; blue, 323.15 K. Symbols: ◆, this work; ◇, Derks et al. (2005); □, Sun et al. (2005); △, Samanta et al. (2006); ○, Muhammad et a. (2009). Figure 2. Distribution coefficient m of N2O in water: this work comparing with literature data:10,17,20,21 , Verteeg and van Swaiij (1988); △, Derks et al. (2005); □, Samanta et al. (2007); ○, Sun et al. (2005); ◆, this work.

Figure 5. Viscosities of NH3(aq) measured by this work compared with literature data.15 Colors: black, this work; blue, Frank et al. (1996). Symbols: ◆, 283.15 K; ■, □, 293.15 K; ▲, △, 303.15 K; ●, ○, 313.15 K; ×, 323.15 K.

Figure 3. Densities of NH3 (aq) measured by this work compared with literature data.14 This work: ■, 283.15 K; ◆, 293.15 K; ▲, 303.15 K; ●, 313.15 K; ∗, 323.15 K. Perry's Handbook: □, 283.15 K; ◇, 293.15 K.

It can be seen that the solubility of N2O in water measured by this work agrees very well with the literature data. The uncertainty is within 3 %.

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RESULTS AND DISCUSSION Density. The measured densities for the solutions of NH3(aq), PZ, and NH3/PZ blends are presented in Table 3. For the NH3(aq) and PZ solutions, the deviations are less than 0.05 % when compared with Perry’s handbook14 and other researchers' results10,17,18,22 under the same conditions, as shown in Figures 3 and 4. The densities of the binary and ternary mixtures decrease with increasing mole fraction of NH3, decreasing mole fraction of PZ, and increasing temperature in the mixture. The experimental density data for the binary and ternary mixtures can be fitted as functions of temperature and concentration of amine and ammonia. The principle chosen to select the form of correlation for fitting the density data is a combination of lowest average

Figure 6. Viscosities of PZ solution measured by this work compared with literature data.17,18 Colors: black, this work; blue, Sun et al. (2005); red, Samanta et al. (2006). Symbols: ◆, 283.15 K; ■, 293.15 K; ▲, △, 303.15 K; ●, ○, 313.15 K; ∗, ×, 323.15 K.

absolute deviation (AAD) and few parameters. Based on these principles, the form of correlation used in this work is given as eq 3. 2390

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Table 4. Parameters, Standard Deviations, and AADs for the Density for NH3, PZ, and NH3/PZ Blended Solutions k1 NH3 PZ NH3+PZ a

0.6475 0.6475 0.6475

δk1

k2

0.01 0.003 0.01

45.01 47.67 45.01

δk2 4 5 4

k3 0 1 −0.4923

δk3

k4

0 0 0.04

−1.3741·10 −1.3741·104 −1.3741·104 4

δk4

k5

δk5

k6

δk6

AADa

290 78 290

210.0557 210.0557 210.0557

10 3 10

−0.70402 −0.1047 −0.70402

0.02 0.04 0.02

6·10−4 1·10−4 7·10−4

AAD = (1/N)∑Ni=1(|ρcal,i − ρexp,i|)/(ρexp,i).

Table 5. Viscosities of Aqueous NH3 (x1), PZ (x2) Solution, and NH3/PZ Blended Solution from (283.15 to 323.15) K and 1 atm (1.01325·105 Pa) Viscosity μa/(mPa·s) 100x1 (mol·mol−1) T/K

a

23

0

11.47

17.60

283.15 293.15 303.15 313.15 323.15

1.3070 1.0020 0.7977 0.6532 0.5470

1.3128 1.0249 0.8106 0.6720 0.5645

1.11

1.3515 1.4282 1.0465 1.0738 0.8278 0.8450 0.6922 0.7124 0.5795 0.5945 100x2 (mol·mol−1)

2.79

5.62

1.5593 1.1569 0.9025 0.7653 0.6297

1.7129 1.2888 0.9955 0.8467 0.6829

T/K

023

0.0906

0.182

0.366

0.553

0.742

283.15 293.15 303.15 313.15 323.15

1.3070 1.0020 0.7977 0.6532 0.5470

1.3302 1.0121 0.8241 0.6757 0.5816

1.3615 1.3928 1.0429 1.0921 0.8339 0.8791 0.6868 0.7176 0.5923 0.6210 100x1/100x2 (mol·mol−1)

1.4622 1.1189 0.8894 0.7531 0.6448

1.5328 1.1743 0.9414 0.7800 0.6604

T/K

1.08/0.182

2.52/0.183

5.00/0.185

7.98/0.187

5.89/0.373

7.79/0.376

283.15 293.15 303.15 313.15

1.3661 1.0767 0.8538 0.7072 5.92/0.565

1.4264 1.1141 0.8988 0.7355 10.84/0.575

1.4819 1.1330 0.9491 0.7549 6.94/0.743

1.5217 1.1525 0.9968 0.7763 2.82/0.745

1.5435 1.1799 1.0174 0.7938 5.04/0.751

1.5843 1.2055 1.0287 0.8199 10.96/0.766

283.15 293.15 303.15 313.15

1.5994 1.2269 1.0488 0.8642

1.7136 1.3055 1.1094 0.9170

1.5417 1.1701 0.9758 0.8222

1.6309 1.2170 1.0098 0.8496

1.6598 1.2841 1.0640 0.8778

1.7727 1.3606 1.1383 0.9346

The uncertainty of the μ measurement is ± 0.3 %.

⎛ k ⎞ k ρNH + PZ = ⎜k1 + 2 ·(x NH3 + k 3·x PZ) + 42 ⎟ · 3 ⎝ T T ⎠ ⎛ k5 ⎞ exp⎜ + k6·(x NH3 + k 3·x PZ)⎟ ⎝T ⎠

The viscosities of the binary and ternary mixtures increase with an increasing mole fraction of NH3 or PZ and decrease with increasing temperature. The experimental viscosity data for the binary and ternary mixtures can also be fitted as functions of temperature and concentration of amine and ammonia. The principles for choosing the form of correlation for fitting the viscosity data are the same as for the density data. The form of correlation used in this work is given in eq 4.

(3)

where ρ is the density of the mixture, T is the temperature, and x is the mole fraction of PZ or NH3. k1 to k6 are the correlation parameters, where k3 is especially used to describe the interaction between the ammonia and amine in the mixed solution. The calculated parameters k, standard deviation of the parameters δk, and the average absolute deviations (AADs) are listed in Table 4. The calculated densities from the correlation eq 3 are in good agreement with the experimental data of this work; the AADs between the correlated and experimental data for NH3 (aq), PZ solution and NH3/PZ blended solution are about 0.0006, 0.0001 and 0.0007, respectively. Viscosity. The measurements of viscosities in this work also comprise the solutions of NH3(aq), PZ, and the NH3/PZ blend. The experimental data are presented in Table 5. For the aqueous NH3 and PZ solutions, the experimental data of this work are compared with literature data15,17,18 in Figures 5 and 6 for the same conditions.

⎛ (x NH3 + k 2·x PZ) μ NH + PZ = ⎜⎜1 + k1· 3 T ⎝ (x NH3 + k 2·x PZ)2 ⎞ ⎟· + k 3· ⎟ T2 ⎠ ⎛k ⎞ k exp⎜ 4 + 52 + k6·(x NH3 + k 2·x PZ)2 ⎟ ⎝T ⎠ T

(4)

where μ is the mixture viscosity, T is the temperature, and x is the mole fraction of PZ or NH3. k1 to k6 are the correlation parameters, where k2 is especially used to describe the interaction between ammonia and amine. The calculated parameters, 2391

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Table 6. Parameters, Standard Deviations, and AADs for Viscosity for NH3, PZ, and NH3/PZ Blends NH3 Pz NH3+PZ

k1

δk1

k2

δk2

k3

δk3

k4

δk4

k5

δk5

k6

δk6

AAD

255.8 6370 499.6

78 846 37

0 1 15.85

0 0 0.7

1.37·106 −1.247·108 −4.48·105

3.2·105 1.0·108 1.56·105

−2110.41 −2041.96 −2044.64

20 19 21

6.19·105 5.99·105 5.99·105

5.8·103 5.4·103 6.2·103

−8.263 1478.7 3.86

1.26 1.1·103 1.6

1.2·10−2 9.9·10−3 2.2·10−2

Table 7. Solubility of N2O (Mass Fraction w kg·kg−1) in Aqueous PZ (x2) Solution and NH3/PZ (x1/x2) Blended Solution from (293.15 to 323.15) K 100x2 (mol·mol−1) 0

0.182 a

T/K

PN2O/kPa

w /%

PN2O/kPa

w/%

293.15 298.15 303.15 313.15 323.15

80.3 70.9 78.3 88.7 92.7

0.0988 0.0743 0.0727 0.0643 0.0551

48.9 64.0 86.3 97.1 88.8

0.0597 0.0669 0.0779 0.0693 0.0503

2.69/0.182

a

0.744

2.73/0.748

PN2O/kPa

1.30 w/%

59.4 0.0734 61.2 0.0633 80.8 0.0729 78.3 0.0572 92.7 0.0546 100x1/100x2 (mol·mol−1)

5.45/0.188

2.11

PN2O/kPa

w/%

PN2O/kPa

w/%

151.3

0.1812

167.2 182.3 196.4

0.1551 0.1331 0.1149

70.6 79.1 78.9 89.7 94.3

0.0836 0.0818 0.0704 0.0628 0.0534

5.64/1.348

8.33/0.758

8.71/1.99

T/K

PN2O/kPa

w/%

PN2O/kPa

w/%

PN2O/kPa

w/%

PN2O/kPa

w/%

PN2O/kPa

w/%

PN2O/kPa

w/%

293.15 303.15 313.15 323.15

107.2 118.6 129.3 139.4

0.1282 0.1103 0.0953 0.0828

110.8 122.3 133.3 143.9

0.1324 0.1138 0.0980 0.0843

108.0 119.3 129.8 139.8

0.1285 0.1103 0.0952 0.0824

104.9 116.2 126.7 136.8

0.1238 0.1068 0.0927 0.0807

104.0 114.6 124.4 133.5

0.1205 0.1039 0.0904 0.0794

101.7 112.0 121.5 130.3

0.1142 0.0995 0.0878 0.0782

The uncertainty of the w measurement is ± 3 %.

standard deviations of the parameters, and the average absolute deviations (AADs) are listed in Table 6. The calculated viscosities from correlation eq 4 agree well with the experimental data in this paper; the AADs between the correlated and experimental data for NH3(aq), PZ solution, and NH3/PZ blended solution are about 0.012, 0.0099, and 0.022, respectively. Solubility of N2O. The measurements of solubility of N2O in this work comprise the solutions of PZ and the NH3/PZ blend; the data of NH3 (aq) have already been measured by Qin16 using the same apparatus as this work. The experimental data for solubility of N2O w (kg·kg−1) under different PN2O and T are presented in Table 7. For PZ solutions, the experimental data of distribution coefficient mN2O in this work are compared with literature data10,17,21 in Figure 7 for the same conditions. Comparisons between the distribution coefficient mN2O of NH 3 (aq), PZ, and NH3 /PZ blends, as defined in the Experimental Section above, are shown in Figure 8. The distribution coefficient mN2O in NH3(aq) is significantly lower than in water, mN2O in PZ solution is higher than in water, and the mN2O in NH3/PZ blends is between NH3(aq) and PZ solutions. The experimental results also indicated that the values of mN2O in NH3/PZ blends are very close to water data under the full temperature range from (293.15 to 323.15) K. Therefore, the mN2O equation for water could be used to estimate the values of mN2O in NH3/PZ blends if the concentration and temperature conditions are the same or similar to this work.

Figure 7. Distribution coefficient m of N2O in PZ solution measured by this work compared with literature data.10,17,21 Colors: black, this work; red, Derks et al. (2005); green, Samanta et al. (2007); blue, Sun et al. (2005). Symbols: ◆, ◇, 293.15 K; ▲, △, 298.15 K; ×, 303.15 K; ●, ○, 313.15 K; ■, 323.15 K.

range (283.15 to 323.15) K. The experimental results cover the composition range (1 to 28) wt % NH3(aq), (0.1 to 1) M PZ and (1 to 10) wt % NH3/(0.1 to 0.4) M PZ blends. The densities and viscosities of the binary and ternary mixtures were correlated using two semiempirical correlations. The correlated results are in good agreement with the experimental data for all of the temperatures and concentrations studied. The solubilities of N2O in PZ solution and NH3/PZ blends were measured over the temperature range (283.15 to 323.15) K. The experimental results cover the composition range (0.1 to 1) M PZ and (1.48 to 4.4) M NH3/(0.1 to 1) M PZ blends. The distribution coefficient, mN2O, in PZ solution is significantly higher than in water, and mN2O in NH3/PZ blends is between the

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CONCLUSION Densities and viscosities of NH3(aq), PZ, and NH3/PZ blended solution were measured and correlated over the temperature 2392

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Figure 8. Distribution coefficient m of N2O in NH3(aq), PZ, and NH3/ PZ blends from (293.15 to 323.15) K: red ■, 0.1 M PZ; red ▲, 0.4 M PZ; purple ◆, 0.7 M PZ; red ●, 1 M PZ; green □, 1.69 M NH3; green △, 3.44 M NH3; green ◇, 3.92 M NH3; green ○, 5.89 M NH3; blue −, 1.448 M NH3/0.1 M PZ; blue |, 1.48 M NH3/0.4 M PZ; blue -, 2.9 M NH3/0.1 M PZ; blue ∗, 2.9 M NH3/0.7 M PZ; purple ●, 4.4 M NH3/0.4 M PZ; ×, 4.4 M NH3/1 M PZ; , water.

values of mN2O in NH3(aq) and PZ solutions and very close to water results under the full temperature range from (293.15 to 323.15) K.

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AUTHOR INFORMATION

Corresponding Author

*E-mail: [email protected]. Funding

Financial support from project 50876051 of the National Natural Science Foundation of China and from NTNU, Department of Chemical Engineering is greatly appreciated. Notes

The authors declare no competing financial interest.

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REFERENCES

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dx.doi.org/10.1021/je300102d | J. Chem. Eng. Data 2012, 57, 2387−2393