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Investigation of the isothermal (vapour + liquid) equilibria of aqueous2-amino-2-methyl-1-propanol (AMP),
 
-benzylethanolamine, or3-dimethylamino-1-propanol solutions at several temperatures
Aouicha Belabbaci
a
, Nouria Chiali-Baba Ahmed
a
, Ilham Mokbel
b
, Latifa Negadi
a,
*
a
University Abou Bekr Belkaid of Tlemcen, Faculty of Sciences, Department of Chemistry, P.O. Box 119, Tlemcen 13000, Algeria
b
LSA, Laboratoire des Sciences Analytiques, CNRS-UMR 5180, Université Claude Bernard – Lyon I, 43, Bd du 11 Novembre 1918, Villeurbanne Cedex 69622, France
a r t i c l e i n f o
 Article history:
Received 14 February 2010Received in revised form 24 March 2010Accepted 20 April 2010Available online 28 April 2010
Keywords:
(Vapour+liquid) equilibriaIsoteniscopeAminesWaterExcess Gibbs free energy
a b s t r a c t
The vapour pressures of (2-amino-2-methyl-1-propanol (AMP)+water), (
-benzylethanol-amine+water), or (3-dimethylamino-1-propanol+water) binary mixtures, and of pure AMP and 3-dimethylamino-1-propanol components were measured by means of two static devices at temperaturesbetween 283K and 363K. The data were correlated with the Antoine equation. From these data, excessGibbs functions (
G
) were calculated for several constant temperatures and fitted to a fourth-order Red-lich–Kister equation using the Barker’s method. The {2-amino-2-methyl-1-propanol (AMP)+water} bin-ary mixture exhibits negative deviations in
 G
(at
 
 <353.15K) and a sinusoidal shape for
 G
for thehigher temperatures over the wholecompositionrange. For theaqueous
 N 
-benzylethanolaminesolution,a S shape is observed for the
 G
for all investigated temperatures over the whole composition range. The(3-dimethylamino-1-propanol +water) binary mixture exhibits negative deviations in
 G
(at
 <293.15K), positive deviations in
 G
(for 293.15K<
 <353.15K) and a sinusoidal shape for
 G
forthe higher temperatures over the whole composition range.
 2010 Elsevier Ltd. All rights reserved.
1. Introduction
Aqueous alkanolamine solutions are widely used for theremovaloftheacidgases(CO
2
 andH
2
S)fromgasmixtures.Inaddi-tion to the well-established industrial uses of experimental datafor these completely miscible (alkanolamine+water) systems,there is a general scientific interest in using such experimentaldata in combination with theories or mathematical models toimprove our understanding of molecular interactions in non-idealliquid systems. (Vapour+liquid) equilibria (VLE) data for(alkanolamine+water) systems are rarely available in theliterature.The present paper is part of a research program on (VLE) inaqueous mixtures of alkanolamines. VLE data for binary mixturescontaining {methylethanolamine (MEA)+water}, or (4-methyl-morpholine+water) have been reported previously [1]. Thepurpose of the present work is to investigate VLE of {2-amino-2-methyl-1-propanol (AMP) (
CAS #
 124-68-5)+water},{
-benzylethanolamine (
CAS #
 104-63-2)+water}, or {3-dimeth-ylamino-1-propanol (
CAS #
 3179-63-3)+water} binary mixtureswith a viewto use the results to determine interaction parametersfor predictive group contribution methods. A survey of the litera-ture shows that there is only one data set available for the(AMP+ water) system [2].
2. Experimental
The alkanolamines were supplied by Aldrich Chem. (Milwau-kee, WI, USA). They were used without further purification. Thepurities, tested by GLC, were better than mass fraction purity0.99. Aqueous solutions were prepared from distilled and deion-ised water.For the pure AMP and 3-dimethylamino-1-propanol compo-nents, the vapour pressure measurements were carried out usinga static apparatus. The description of the apparatus and the exper-imental procedure can be found elsewhere [3–6], so only the mostsalientinformationisgivenhere.Theapparatuswasequippedwitha differential manometer from MKS, type 670, model 616A. Thepressure measurement consisted of applying the vapour pressureof thesampleonthemeasurementsideof thegauge. Thereferenceside was submitted to a permanent-dynamic pumping. The resid-ual pressure was 10
4
Pa and therefore can be neglected. Temper-ature measurements were carried out using a copper-constantanthermocouple calibrated against a 25
X
platinum resistance stan-dard thermometer (±0.001K, IPTS 90) and a Leeds and Northrup
0021-9614/$ - see front matter
 2010 Elsevier Ltd. All rights reserved.doi:10.1016/j.jct.2010.04.015
*
 Corresponding author. Tel./fax: +213 43 28 65 30.
E-mail address:
 latifanegadi@yahoo.fr (L. Negadi). J. Chem. Thermodynamics 42 (2010) 1158–1162
Contents lists available at ScienceDirect
 J. Chem. Thermodynamics
 
bridge (±10
4
X
). During measurements the stability of the tem-perature is ±0.02K. The differential pressure gauge was calibratedagainst a U-manometer filledwithmercuryor Apiezonoil depend-ing on pressure range. The levels in both arms of the U-shapedmanometer were read by a cathetometer (reference 70298, fromBouty France) to the nearest 0.001mm. The calibration was thenchecked by measuring the vapour and the sublimation pressuresof water and naphthalene [4]. The uncertainty of the measure-ments is estimated to be:
 r
(
 P)
 =0.03(
/Pa) for
 
 <600Pa;
r
(
P)
 =0.01(
/Pa) for
 
 in the range (600 to 1300)Pa,
r
(P)
 =0.03(
/Pa) for
 
 over 1300Pa, and
 r
(T 
)=0.02K for thetemperature range 203
6
/K
6
463.Forthethreebinarysystems,theexperimentalvapourpressure,
, data were obtained with an apparatus described in detail byBlondel-Telouk
 et al
. [7,8], as a function of the temperature,
 T 
, forconstant mole fraction composition,
 x
i
. The apparatus allows mea-surements at pressures from 27Pa to 200
10
3
Pa and at tempera-turesfrom(258.15to468.15)K.Thepressurewasmeasuredwithapressure gauge (Rosemount, Model 1151 DPE 22S2, Minneapolis,MN, USA), separated from the working fluid by a differential pres-sure indicator (MKS, Model 615D, MKS Instruments, USA). Thepressure gauges were periodically checked against a Hg or oilmanometer and a Bouty (Paris, France) Type 70298 cathetometer,which when combined provide pressures with an uncertainty of 1Pa. The temperature of the oil-filled thermostat was maintainedconstant to ±0.01K. The temperature was measured by means of a copper-constantan thermocouple calibrated against a Leeds andNorthrup standard platinum resistance thermometer 8163-B, cali-brated by the National Bureau of Standards (NIST) (Washington,DC, USA) and connected to Mueller type G2 bridge (with a preci-sion 10
4
X
). All temperatures are reported on ITS-90. The esti-mated uncertainties in pressure, temperature and mole fractionare:
 r
(
)=0.15(
/Pa) for
 P 
 <13.3Pa,
 r
(
)=0.05(
/Pa) at pressurebetween (13.3 and 200)Pa,
 r
(
)=0.005(
/Pa) in the range (200to 1000)Pa,
 r
(
)=0.002(
/Pa) for the range (1000 to200
10
3
)Pa,
 r
(
)=0.01K and
 r
(
 x
i
)=0.0002. Mixtures were pre-paredbymassandthoroughlydegassedbydistillationasdescribedby Blondel-Tellouk
 et al
3. Results and discussion
The experimental vapour pressure data were fitted to the Antoine equation:
lg
10
=
Torr
 ¼
 A
 B
 þ
=
ð
C
Þ
:
 ð
1
Þ
The objective function
 Q 
 was the sumof the squared relative deviations in pressure:
 ¼
X
 
calc
 
exp
exp
2
:
 ð
2
Þ
The overall mean relative deviation in pressure is:
d
 %
¼
 100
X
 
calc
 
exp
exp
;
 ð
3
Þ
where
 N 
 is the total number of experimental values.Table 1 lists, for the pure AMP and 3-dimethylamino-1-propanol components,the temperaturerange, the coefficients
 A
,
 B
,
 C 
 of theAntoine equation andtheover-all mean relative deviation in pressure. The comparison of the calculated vapour
 TABLE 1
Coefficients
 A
,
 B
,
 
 and overall mean relative deviation in pressure of the Antoineequation (1).
Compound
 
/K
 A B
 100(
d
/
)AMP 3 293.29–373.00 7.73031 1698.90 185.9906 0.673-Dimethylamino-1-propanol283.15–73.10 8.87465 2767.22 262.5195 0.31100
d
=
¼
1
P
i
¼
1
100
 
calc
exp
exp
, where
 
 is the total number of experimentalvalues.
 TABLE 2
Experimental and calculated (with the Antoine equation (1)) vapour pressures of pureAMP and 3-dimethylamino-1-propanol.
/K
 
(experimental)/Pa
 
(from equation (1)/Pa 100
d
/
 AMP 
293.29 41.5 41.0 1.21303.35 97.5 99.3
 
1.87313.24 219.1 219.1
 
0.02323.25 455.6 456.2
 
0.13332.57 874.5 856.0 2.11343.18 1658.6 1657.1 0.09353.17 2933.5 2942.1
 
0.29363.10 4987.5 4993.6
 
0.12373.00 8141.8 8159.0
 
0.21100
d
/
 0.67
 3-Dimethylamino-1-propanol
283.15 7.0 7.0
 
0.04293.14 16.0 16.0
 
0.13303.09 34.6 34.5 0.27313.08 70.7 70.8
 
0.15323.28 141.8 140.8 0.69333.12 260.4 262.3
 
0.72343.12 474.2 475.1
 
0.20363.17 1419.4 1413.0 0.45373.10 2314.6 2318.4
 
0.17100
d
/
 0.31
 TABLE 3
Values of the vapour pressure
 P 
, standard deviations
 d
/
 (%), activity coefficients
 c
1
and
 c
2
 and excess molar Gibbs functions
 G
for the binary system {AMP (1) + water(2)}.
 x
1
 
/kPa
 x
1
 
/kPa
 x
1
 
/kPa
T/K = 293.15
0.0000 2.2838 0.2603 1.6698 0.6692 0.69150.0498 2.1703 0.3598 1.4464 0.8203 0.36270.1001 2.0305 0.5408 1.0027 1.0000 0.04050.1800 1.9769
T/K = 303.15
0.0000 4.1478 0.2603 3.0389 0.6692 1.22690.0498 3.9584 0.3598 2.6179 0.8203 0.70810.1001 3.7225 0.5408 1.7898 1.0000 0.09760.1800 3.5283
T/K = 313.15
0.0000 7.2219 0.2603 5.3265 0.6692 2.10740.0498 6.9120 0.3598 4.5642 0.8203 1.29630.1001 6.5300 0.5408 3.0872 1.0000 0.21760.1800 6.0803
T/K = 323.15
0.0000 12.1071 0.2603 9.0231 0.6692 3.51380.0498 11.6081 0.3598 7.6914 0.8203 2.24460.1001 11.0120 0.5408 5.1605 1.0000 0.45310.1800 10.1488
T/K = 333.15
0.0000 19.6156 0.2603 14.8171 0.6692 5.70090.0498 18.8235 0.3598 12.5658 0.8203 3.70360.1001 17.9239 0.5408 8.3817 1.0000 0.88890.1800 16.4517
T/K = 343.15
0.0000 30.8154 0.2603 23.6497 0.6692 9.01900.0498 29.5745 0.3598 19.9565 0.8203 5.85870.1001 28.2571 0.5408 13.2592 1.0000 1.65440.1800 25.9642
T/K = 353.15
0.0000 47.0737 0.2603 36.7767 0.6692 13.93990.0498 45.1559 0.3598 30.8832 0.8203 8.93060.1001 43.2785 0.5408 20.4713 1.0000 2.93860.1800 39.9802
T/K = 363.15
0.0000 70.1022 0.2603 55.8377 0.6692 21.08630.0498 67.1789 0.3598 46.6687 0.8203 13.17480.1001 64.5689 0.5408 30.9057 1.0000 5.00680.1800 60.1821
 A. Belabbaci et al./J. Chem. Thermodynamics 42 (2010) 1158–1162
 1159
 
pressures of AMP or 3-dimethylamino-1-propanol from equation (1) with the mea-suredvaluesisshownintable2. OurvapourpressuredataforpureAMPareingood agreement withthosereported byPappa
et al
. [2] or givenbythe NIST database[9]. For pure 3-dimethylamino-1-propanol, novapour pressure data are available intheliterature. For pure water and
 N 
-benzylethanolamine, the vapour pressures used inthis work have been reported previously [1,10].For the three binary mixtures, the vapour pressures were measured at temper-atures between (283.15 (or 293.15) and 363.15) K and the results fitted to the An-toine equation and the molar excess Gibbs functions
 G
were estimated from theRedlich–Kister equation using the method of Barker [11]:
G
¼
 x
1
ð
1
 x
1
Þ
X
m j
¼
1
RTG
 j
ð
2
 x
1
 
1
Þ
 j
1
;
 ð
4
Þ
where
 x
1
 is the mole fraction for the alkanolamine. The coefficients
 G
 j
 were deter-mined by regression through minimization of the sum of deviations in pressure. Va-pour phase imperfection and variation of the Gibbs function of the pure liquidcomponents with pressure were accounted for in terms of the second molar virialcoefficients,estimatedbythemethodofTsonopoulos[12,13]andthemolarvolumesunder saturation pressure.
 TABLE 4
Values of the vapour pressure
 P 
, standard deviations
 d
/
 (%), activity coefficients
 c
1
and
 c
2
 and excess molar Gibbs functions
 G
for the binary system {
-benzylethanol-amine (1) + water (2)}.
 x
1
 
/kPa
 x
1
 
/kPa
 x
1
 
/kPa
T/K = 283.15
0.0000 1.1995 0.3589 0.9828 0.7546 0.21920.0746 1.1797 0.4879 0.6833 0.8358 0.10870.1798 1.1600 0.6368 0.3759 1.0000 0.00030.2599 1.1242
T/K = 293.15
0.0000 2.2838 0.3589 1.8102 0.7546 0.44340.0746 2.2513 0.4879 1.3596 0.8358 0.21830.1798 2.1784 0.6368 0.7557 1.0000 0.00080.2599 2.0655
T/K = 298.15
0.0000 3.0950 0.3589 2.4174 0.7546 0.61670.0746 3.0538 0.4879 1.8667 0.8358 0.30400.1798 2.9377 0.6368 1.0465 1.0000 0.00130.2599 2.7628
T/K = 303.15
0.0000 4.1478 0.3589 3.1963 0.7546 0.84640.0746 4.0959 0.4879 2.5217 0.8358 0.41870.1798 3.9223 0.6368 1.4287 1.0000 0.00220.2599 3.6646
T/K = 313.15
0.0000 7.2219 0.3589 5.4334 0.7546 1.53590.0746 7.1404 0.4879 4.4051 0.8358 0.77080.1798 6.7991 0.6368 2.5597 1.0000 0.00530.2599 6.2965
T/K = 323.15
0.0000 12.1071 0.3589 8.9249 0.7546 2.66420.0746 11.9800 0.4879 7.3076 0.8358 1.36660.1798 11.3869 0.6368 4.3745 1.0000 0.01250.2599 10.5045
T/K = 333.15
0.0000 19.6156 0.3589 14.2113 0.7546 4.43970.0746 19.4190 0.4879 11.5917 0.8358 2.34140.1798 18.4827 0.6368 7.1709 1.0000 0.02760.2599 17.0558
T/K = 343.15
0.0000 30.8154 0.3589 21.9986 0.7546 7.13760.0746 30.5123 0.4879 17.6823 0.8358 3.88850.1798 29.1565 0.6368 11.3275 1.0000 0.05780.2599 27.0090
T/K = 353.15
0.0000 47.0737 0.3589 33.1874 0.7546 11.11080.0746 46.6090 0.4879 26.0629 0.8358 6.27570.1798 44.8102 0.6368 17.3127 1.0000 0.11590.2599 41.7925
T/K = 363.15
0.0000 70.1022 0.3589 48.9020 0.7546 16.80030.0746 69.3943 0.4879 37.2688 0.8358 9.86640.1798 67.2411 0.6368 25.6896 1.0000 0.22270.2599 63.2972
 TABLE 5
Values of the vapour pressure
 P 
, standard deviations
 d
/
 (%), activity coefficients
 c
1
and
 c
2
 and excess molar Gibbs functions
 G
for the binary system {3-dimethylamino-1-propanol (1) + water (2)}.
 x
1
 
/kPa
 x
1
 
/kPa
 x
1
 
/kPa
T/K = 283.15
0.0000 1.1995 0.2599 0.8687 0.7189 0.33220.0501 1.1288 0.3602 0.7398 0.8119 0.23100.1005 1.0745 0.4998 0.5619 1.0000 0.007
T/K = 293.15
0.0000 2.2838 0.2599 1.6884 0.7189 0.65100.0501 2.1704 0.3602 1.4182 0.8119 0.51630.1005 2.0696 0.4998 1.1314 1.0000 0.0160
T/K = 303.15
0.0000 4.1478 0.2599 3.1272 0.7189 1.21370.0501 3.9719 0.3602 2.6069 0.8119 1.02060.1005 3.7980 0.4998 2.1465 1.0000 0.0346
T/K = 313.15
0.0000 7.2219 0.2599 5.5479 0.7189 2.16370.0501 6.9561 0.3602 4.6130 0.8119 1.83150.1005 6.6752 0.4998 3.8649 1.0000 0.0712
T/K = 323.15
0.0000 12.1070 0.2599 9.4688 0.7189 3.70590.0501 11.7119 0.3602 7.8849 0.8119 3.04160.1005 11.2862 0.4998 6.6449 1.0000 0.1396
T/K = 333.15
0.0000 19.6156 0.2599 15.6059 0.7189 6.12270.0501 19.0343 0.3602 13.0589 0.8119 4.74260.1005 18.4285 0.4998 10.9668 1.0000 0.2627
T/K = 343.15
0.0000 30.8153 0.2599 24.9205 0.7189 9.79210.0501 29.9641 0.3602 21.0130 0.8119 7.02040.1005 29.1571 0.4998 17.4516 1.0000 0.4760
T/K = 353.15
0.0000 47.0737 0.2599 38.6685 0.7189 15.20600.0501 45.8291 0.3602 32.9293 0.8119 9.95120.1005 44.8321 0.4998 26.8798 1.0000 0.8328
T/K = 363.15
0.0000 70.1021 0.2599 58.4529 0.7189 22.98940.0501 68.2833 0.3602 50.3645 0.8119 13.59940.1005 67.1660 0.4998 40.2065 1.0000 1.4116
FIGURE 1.
 Plot of pressure against mole fraction to show the experimental andcalculated
 
 x
(
 y
) behaviour of the system {AMP (1)+water (2)} at differenttemperatures:
 
, 293.15K;
 d
, 323.15K;
 j
, 343.15;
 N
, 363.15K;
 3
, calculatedvalues using Barker’s method.1160
 A. Belabbaci et al./J. Chem. Thermodynamics 42 (2010) 1158–1162

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