Viscosities Of Pure And Aqueous Solutions Of .

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ANNUAL TRANSACTIONS OF THE NORDIC RHEOLOGY SOCIETY, VOL. 21, 2013Viscosities of Pure and Aqueous Solutions of Monoethanolamine (MEA),Diethanolamine (DEA) and N-Methyldiethanolamine (MDEA)Udara S. P. R. Arachchige1,a, Neelakantha Aryal1, Dag A. Eimer1, and Morten C. Melaaen11 Telemark University College, Porsgrunn, 3901, anolamine and methyldiethanolaminesolutions were examined at a temperaturerange from (293.15 to 423.15) K for pureamines and (293.15 to 353.15) K foraqueous amines at different compositions.The experimental viscosities measured inthis work are in good agreement with thosereported in the literature.INTRODUCTIONAlkanolamines have been used for theacid gas absorption process for a longperiod. The physical properties of thosealkanolamines are important for processdesign. The main objective of this paper isto provide values for viscosities of differentaqueous amines at different temperatureswhich are needed for the acid gas absorptionprocess. Acid gas absorption process takesplace at 313 K temperature. However,different operating temperatures areinterested for high performance. Therefore,physical properties like viscosity of aminesare important to calculate for differenttemperature range to perform mathematicalcalculations. The physical properties such asdensity, viscosity and solubility data ofsolvents are important for the acid gasabsorption and regeneration process.Different types of amines are available, suchas primary amines (MEA, DGA), secondaryamines (DEA), tertiary amines (MDEA,299TEA), hindered amines (AMP) and cyclicamines(Piperazine).Importantalkanolamines for industrial application aremonoethanolamine (MEA), diethanolamine(DEA), di-2-propanolamine (DIPA) and Nmethyldiethanolamine(MDEA)[1].Aqueous MEA solutions are widely used forgas treating processes due to high reactivity,low operating cost and ease of reclamation[2]. However, the possibilities of using othersolvents like DEA and MDEA have to beanalyzed in order to lower the cost of CO2capturing. This work has been carried out todetermine the effect of temperature on theviscosity of different types of amines atdifferent concentration levels at atmosphericpressure. The experiments were performedtochecktheviscositiesofmonoethanolamine (MEA), diethanolamine(DEA) and methyldiethanolamine (MDEA).Thepurealkanolamineviscositymeasurements were carried out for thetemperature range (293.15 to 423.15) K andalkanolamine solution viscosity weremeasured in the range of (293.15 to 353.15)K. This represents an extension ofpreviously reported data.The measured data for the different kindof amines are compared with those availablefrom the literature. The pure viscosity datafor MEA, DEA and MDEA solutions arecompared with data from Li and Lie1,DiGuilio et al. [3] and Mandal et al. [4] Thedata given by Amundsen et al. [5], Rinker et

al. [6] and Li and Lie [1] are used tocompare the aqueous viscosity data forMEA, DEA and MDEA solutions.Agreement between the measurement dataand literature values were found to besatisfactory.The obtained results were used toproduce correlations for amine viscosity atdifferent temperatures. A number ofcorrelations for computation of viscosity ofliquids are presented in the literature. Vogel[7] has reported the simple three constantcorrelation for pure liquid viscosity andViswanath and Natarajan [8] utilized asimilar form for both dynamic andkinematic viscosities.The equation presented by Vogel wasmodified by Goletz and Tassios [9] toinclude the boiling point of the substance.Dutt [10] described a similar idea to Goletzand has derived a correlation using densityand boiling point of the component. Pureliquid viscosity can be represented bypolynomial type equation mentioned byGirifalco [11] which was extended byThorpe and Rodger [12].Digullio et al. [3] have reported a threeconstant equation which is closer to Vogel’sequation for pure amines’ viscosity. Amongthose, Digullio’s equation is selected forcalculation of pure amines’ viscosity due toless deviation when fitting experimentalvalues.The aqueous amine viscosities measuredin this work are used to regress thepolynomial for representation of amineviscosities. Teng et al. [13] and Chowdhuryet al. [14] have reported the correlations foraqueous amine viscosity variation withmolar concentration for specific temperaturevalues. The correlation from Teng et al. [13]is selected for this study because of lessdeviation when fitted to experimentalvalues.300EXPERIMENTAL SECTIONDynamic viscosity was measured usingMCR 101 Anton Paar double-gaprheometer. The viscometer was calibratedagainst the petroleum distillate and mineraloil calibration fluid from Paragon Scientificltd. The calibration factor was decidedaccording to the given temperature for thecalibration liquid and experimental viscosityachieved during the calibration. The lowtemperature measurements were achievedby applying cooling water supply to therheometer setup at (293.15, 298.15 and303.15) K. The MEA was purchased fromMerck KGaA, DEA and the MDEA fromMerck Schuchardt OHG. The purity of thechemicals in mass basis are 99.5%, 99% and98% respectively for MEA, DEA andMDEA. The information about chemicalsare given in Table 1. Without furtherpurification, all these amines were used forexperimental studies. De-gassed distilledwater was used for preparation of aqueousamine solutions. All the experiments areperformed at 1.01 bar operating pressure.Table 1. Purity of the amines used tOHGRESULTS AND DISCUSSIONThe results from the experimental workhave been sub-divided into two sections:viscosities of pure amines and viscosities ofaqueous amines.

Table 3. Comparison of the Viscosities η of Pure DEA Measuredin This Work with Literature Values from Temperature T (293.15 to 423.15) KPure Amine ViscositiesViscosities of pure MEA, DEA andMDEA from temperature range (293.15 to423.15) K are tabulated in Tables 2, 3 and 4,respectively. The experimental viscosityresults for pure amines, tabulated in Tables3 to 5, are plotted in Fig. 1 as viscosity vs.temperature. As shown in the Fig. 1,viscosities of pure amines are decreasingwith the increase of temperature. Theviscosities of pure MEA, DEA and MDEAmeasured in this work agree well with theliterature values taken from Li and Lie1,DiGuilio et al. [3] and Mandal et al. [4],respectively.Theaverageabsolutedeviations between the literature values andour data are (0.019, 1.21, 0.39) mPa·s forpure MEA, DEA and MDEA respectively.The deviations are in the range ofexperimental uncertainties which is givenunder the each table.Standard uncertainties u are u(T) 0.3 K and the combinedexpanded uncertainties Uc are Uc(η) 0.843 mPa·sTable 2. Comparison of the Viscosities η of Pure MEA Measuredin This Work with Literature Values from Temperature T (293.15 to 423.15) KTable 4. Comparison of the Viscosities η of Pure MDEA Measuredin This Work with Literature Values from Temperature T (293.15 to 423.15) KT/KThisworkLi andLie1DiGuilio etT/KDiGuilioMandal etet his work566.3119.535.0923.410.535.67ThisLi andworket al.422.43Lie [1]DiGuilio et al. [3]al. 62393.152.65618.98323.152.912Mandal andard uncertainties u are u(T) 0.3 K and the combinedexpanded uncertainties Uc are Uc(η) 0.015 6714.314.385969.9877.1513.9872.5047.088

mPa sStandard uncertainties u are u(T) 0.3 K and the combinedexpanded uncertainties Uc are Uc(η) 0.122 mPa·s10001510η /mPa 5413.15T/KFigure 1. Pure amines’ viscosity variationwith temperature at (293.15 to 423.15) K: ,MEA; , MDEA; , DEA.Aqueous Amine ViscositiesThe viscosity data for aqueous MEA,DEA and MDEA solutions are presented inTables 5, 6 and 7, respectively. Theexperiments were performed to measureviscosities of amines with concentrations inthe range from mass fraction (0.1 to 0.9) forthe temperature range (293.15 to 353.15) K.The aqueous MEA, DEA and MDEAviscosity data of Amundsen et al. [5],Rinker et al. [6] and Li and Lie [1] arecompared with our experimental data(Figures 2, 3 and 4). The average absolutedeviations are (0.08, 0.02, 0.02) mPa·s foraqueous MEA, DEA and MDEA,respectively and the maximum deviation is0.25 mPa·s when compared against theliterature sources. Hence, aqueous amineviscosities measured in this work are ingood agreement with those reported byAmundsen et al. [6], Edward et al.5, Li andLie [1].The dynamic viscosities of aqueousMEA, DEA and MDEA are plotted versustemperature in Figures 2, 3 and 4.302Figure 2. Comparison of aqueous MEAviscosity as a function of temperature. Linesare experimental data: , 20%; ---, 30%;, 40%;, 50%;, 70%;,90%. Symbols refer to literature data [5]: ,20%; , 30%; x, 40%; , 50%; Δ, 70%; ,90%.43η/mPa s0293.15210293.15313.15333.15353.15T/KFigure 3. Comparison of aqueous DEAviscosity variation with temperature. Lines, 20%;are experimental data: , 10%;, 30%. Symbols refer to literaturedata6: , 10%; , 20%; , 30%.

Figure 4. Comparison of aqueous MDEAviscosity variation with temperature: Linesare experimental data: , 20%; ---, 30%;, 40%;, 50%. Symbols refer toliterature data1: , 20%; , 30%; , 40%;o, 50%.1210η/mPa KTable 5. Viscosities of Aqueous MEA Solutions Measured in This Work from Temperature T (293.15 to 353.15) K as a function of massfraction.Temp10 %20 %30 %40 %50 %60 %70 %80 %90 150.4490.5890.7790.9771.2911.774Standard uncertainties u are u(T) 0.3 K and the combined expanded uncertainties Uc are Uc(η) 0.015 mPa·sTable 6. Viscosities of aqueous DEA solutions measured in this work from T (293.15 to 353.15) K as a function of mass fraction.Temp10 %20 %30 %40 %50 %T/K60 %70 %80 %90 00.8331.0991.6852.6594.21607.1113.03580 %90 %Standard uncertainties u are u(T) 0.3 K and the combined expanded uncertainties Uc are Uc(η) 0.843 mPa·sTable 7. Viscosities of aqueous MDEA solutions measured in this work from T (293.15 to 353.15) K as a function of mass fraction.TempT/K10 %20 %30 %40 %50 %60 %70 029.03058.28781.670303

44.9166.674Standard uncertainties u are u(T) 0.3 K and the combined expanded uncertainties Uc are Uc(η) 0.121 mPa·smln η/(mPa.s) ln 0 a kCorrelation for Pure Amine Viscositiesb2T / ( K ) b3where η represents the viscosity of thebinary solution while ηo is the viscosity ofpure water, and x the mole fraction of theamines. Pure water viscosity is taken fromLi and Lie [1].Calculatedpolynomialcoefficientsindicated by ak are tabulated in Table 9.Deviation of calculated versus measuredaqueous amines’ viscosities are calculatedas AAD and tabulated for differenttemperature values in the same table. ForMEA, AAD values vary from 0.01 to 0.07and similarly for DEA and MDEA thevalues vary from 0.01 to 0.08 and 0.002 to0.05 mPa·s, respectively.(1)The b1, b2 and b3 are constants. Averageabsolute deviation (AAD), (η-ηreg), is 0.05,2.85 and 0.35 mPa·s respectively for pureMEA, DEA and MDEA.EVALUATION OFUNCERTAINTIESTable 8. Constants for viscositycorrelation (eq. 1).Substanc(2)0The eq 1 can be used to correlate thepure amines’ viscosities as a function oftemperature [3]. Table 8 lists thecoefficients of Eq 1 obtained by regressionand also include the average absolutedeviation between the experimental dataand regression value.ln[ / (mPa s )] b1 33430.35EXPERIMENTALViscosity measurement uncertainties arearising as a combination of the nties and instrument uncertainties.The MCR rheometer has itself specifiedtemperature accuracy of 0.3K. Thesamples were measured using an analyticalbalance which has accuracy of 0.0001g(0.1mg). The estimated uncertainty in massfraction of MEA, DEA and MDEA are0.5%, 0.4% and 0.4% respectively.Rheometer accuracy is mentioned as 0.002 mPa·s for viscosity measurements upto 453K temperature level. Total value ofuncertainties for experimental viscositiescalculated using combination of allmentioned uncertainties with root sum ofeCorrelation for Aqueous Amine ViscositiesAqueous amine viscosities measured inthis work are used to generate thepolynomial for representation of amineviscosities using regression. The followingpolynomial (Eq 2) which is taken from theTeng et al. [13] is used for the regression.304

correlations were used to fit theexperimental values for pure and aqueousamines. Finally, calculated the deviation forall fitted correlations and correlation whichgives lowest deviation is selected for thiswork. The deviation of regression valuesand measured values are varied as 0.05,2.85 and 0.35 mPa·s respectively for pureMEA, DEA and MDEA amines and 0.002to 0.08 mPa·s for aqueous amines.Deviations are in the range of expandedexperimental uncertainties except pure DEAand MDEA deviation. Deviation of the pureDEA and MDEA is slightly higher than thecalculated experimental uncertainties.square method. The combined expandeduncertainties for pure amines calculated as 0.015 mPa·s, 0.843 mPa·s and 0.122mPa·s for MEA, DEA and MDEArespectively. The combined expandeduncertainties for aqueous amines calculatedas 0.015 mPa·s, 0.843 mPa·s and 0.121 mPa·s for MEA, DEA and MDEArespectively.CONCLUSIONThe viscosity of MEA, DEA and MDEAwere measured at a temperature range from(293.15 to 423.15) K for pure amines and(293.15 to 353.15) K for aqueous amines.Aqueous amine viscosities were measuredfor a mass fraction range 0.10 to 0.90. Asthe temperature increased, viscosity of pureand aqueous amine solutions decreased.Moreover, the viscosity of aqueous aminesolutions increased as the mass fraction ofamine increased for a given temperature.The measured viscosity data are in goodagreement with literature data to the TThe support of Statoil’s research centerin Porsgrunn, especially Morten Tande,clarifying possible improvements to obtainmore accurate viscosity results andinstructions to the equipment used, isgratefully acknowledged.Table 9. Coefficients of the Polynomial for the binary solutions between MEA, DEA andMDEA and water at different temperatures.T/ 559-472.06671274.50.010.010.02293.15298.15305

100.degree.C", J. Chem. Eng. Data., 39,392-395.REFERENCES1. Li, M. H. and Lie, Y. C. (1994),"Densities and Viscosities of Solutions ofMonoethanolamine Nmethyldiethanolamine Water andMonoethanolamine 2-Amino-2-methyl1-propanol Water", J. Chem. Eng. Data.,, 39, eitsgesetzderViskosität von Flüssigkeiten", Physikz., 22,645-646.8.Viswanath, D. S. and Natarajan, G.(1989), "Databook on Viscosity ofLiquids", Hemisphere, New York.2. Isaacs, E. E., Otto, F. D., and Mather,A. E. (1980), "Solubility of mixtures ofhydrogen sulfide and carbon dioxide in amonoethanolamine solution at low partialpressures", J. Chem. Eng. Data., 25, 118120.9. Goletz, Jr. E., and Tassios, D. (1977),"An Antoine type equation for liquidviscosity dependency to temperature", Ind.Eng. Chem. Proc., 16(1), 75-79.3. DiGuilio, R. M., Lee, R.-J., Schaeffer,S. T., Brasher, L. L., and Teja, A. S.(1992), "Densities and viscosities of theethanolamines", J. Chem. Eng. Data., 37,239-242.10.Dutt, N. V. K. (1990), "A simplemethod of estimating the viscosity ofpetroleum crude oil and fractions", Chem.Eng. J., 45, 83-86.4. Mandal, B. P., Kundu, M., andBandyopadhyay, S. S. (2003), "Densityand Viscosity of Aqueous Solutions of (NMethyldiethanolamine Monoethanolamine),(NMethyldiethanolamine Diethanolamine),(2-Amino-2-methyl-1-propanol Monoethanolamine), and (2-Amino-2methyl-1-propanol Diethanolamine)", J.Chem. Eng. Data., 48, 703-707.11.Girifalco, L. A. (1955), "Temperaturedependence of viscosity and its relation tovapor pressure for associated liquids", J.Chem. Phys., 23(12), 2446-2447.5. Amundsen, T. G., Øi, L. E., and Eimer,D. A. (2009). "Density and Viscosity ofMonoethanolamine Water CarbonDioxide from (25 to 80) C", J. Chem.Eng. Data., 54, 3096-3100.13. Teng, T. T., Maham, Y., Helper, L. G.,and Mather, A. E. (1994), "Viscosity hanolamine", J. Chem. Eng. Data., 39,290-293.12.Thorpe, T. E. & Rodger, J. W. (1895),"Bakerian Lecture: On the relationsbetween the viscosity (internal friction) ofliquids and their chemical nature", Phil.Trans., 185, 397-710.6.Rinker, E. B., Oe

Viscosities of pure MEA, DEA and MDEA from temperature range (293.15 to 423.15) K are tabulated in Tables 2, 3 and 4, respectively. The experimental viscosity results for pure amines, tabulated in Tables 3 to 5, are plotted in Fig. 1 as viscosity vs. temperature. As sh

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