Article pubs.acs.org/jced
Physicochemical Properties of Aqueous Solutions of Sodium L‑Prolinate as an Absorbent for CO2 Removal M. S. Shaikh, A. M. Shariff,* M. A. Bustam, and Ghulam Murshid Research Center for CO2 Capture (RCCO2C), Department of Chemical Engineering, Universiti Teknologi PETRONAS, 31750 Tronoh, Perak, Malaysia ABSTRACT: The physicochemical properties such as density, viscosity, and refractive index of aqueous solutions of sodium L-prolinate (SP) as a solvent for CO2 capture was measured. These properties were measured at different temperatures from (298.15 to 343.15) K. The mass fractions of SP were 0.05, 0.10, 0.20, 0.30, and 0.40. The coefficient of thermal expansion was calculated from the experimental density values in the same temperature range. The analysis of experimental results shows that the densities, viscosities, and refractive indices of the aqueous solutions of SP increase with an increase in the mass fraction in the solution, and decrease with increasing temperature. The thermal expansion coefficient slightly increases with increasing temperature and concentration. The experimental data of density, viscosity, and refractive index were correlated by the least-squares method as a function of temperature. The predicted data were estimated from correlation coefficients for all measured properties and reported with standard deviations.
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INTRODUCTION An uncontrolled global environmental problem is global warming caused by excessive emissions of carbon dioxide (CO2) from a variety of sources such as the combustion of fossil fuels for electricity generation, and other industrial as well as human activities.1,2 Currently, CO2 concentration in the atmosphere is 396.80 ppm and expected to grow beyond 400 ppm by 2015.2 According to the various climate estimation models; by the year 2100, the average rise in global temperature may reach to about (1.4 to 5.8) °C owing to the effect of global warming.3 Therefore, it has become a global challenge to mitigate the CO2 emissions by establishing effective technologies for the reduction of bulk emissions of CO2 from different sources.4 Chemical absorption is one of the most efficient technologies for removal of CO2 from various industrial gas streams. This technology employs the chemical solvents which are reactive with CO2.5−7 The conventional chemical solvents used for this purpose are monoethanolamine (MEA), diethanolamine (DEA), diisopropanolamine (DIPA), triethanolamine (TEA), and methyldiethanolamine (MDEA).8−10 These are amine-based solvents, which have been extensively used for years to capture CO2 effectively at the commercial level. Despite the widespread use of amines in CO2 removal processes, these solvents suffer from various practical problems, which have been identified after extensive investigations of amines usage in industrial applications. The practical issues associated with the use of amine solvents include the thermal and oxidative degradation caused during the cyclic absorption−desorption process.11,12 Corrosion of process equipment and flow lines has also been reported when amine solvents are used. Solvent loss due to volatilization, highenergy consumption during regeneration, and a toxic nature are the additional negative aspects of these usual solvents.13−16 © XXXX American Chemical Society
These demerits of amine-based solvents restrict their use for CO2 removal processes. Recently, amino acids salts have been investigated widely as a prospective candidate for CO2 capture from various gas streams owing to different advantages over the amines. Amino acids have the same functional group like amines and behave in a similar way in the CO2 capture process, but there are various positive aspects in their use as CO2 capture agents. The potential benefits of amino acids are their better resistance toward thermal and oxidative degradation and the low vapor pressure due to the ionic structure of amino acids salts, which prevents the vapor loss even at elevated temperatures.12,17−19 In addition to this, amino acids are able to regenerate, environmentally friendly, and easily available at the commercial scale.20,21 These potential benefits of amino acids make them interesting and make it essential to carry out extensive investigations of these solvents for CO2 removal. Various studies on amino acids and their types such as potassium and lithium salts of L-proline, sarcosine, L-phenylalanine, L-arginine, etc. have been carried out and provide the evidence that these solvents have potential to capture CO2 from industrial gases.22,23 This has encouraged us to study another amino acid salt system, namely, the sodium salt of L-proline as a CO2 capture agent. For the commercial implementation of the solvent such as the design of gas treatment processes, modeling and simulation, and operation of the equipment, the study of physical properties of the solvent, such as density, and viscosity, is very essential.24−27 Refractive index data are also essential for Received: September 12, 2013 Accepted: December 12, 2013
A
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Table 1. Specifications of Chemicals name of chemical
chemical formula
purity
method of purification
source
C5H9NO2 NaOH C2H7NO H2O
≥ 98 % pure ≥ 99 % pure ≥ 99 % pure 99 pure
none none none double distilled water distillation
Merck Merck Merck
L-proline
sodium hydroxide monoethanolamine double distilled water
Table 2. Comparison of Experimental Data of Density (ρ/g·cm−3), Viscosity (η/mPa·s) and Refractive Index (nD) of Pure MEA with Published Work at Pressure p = 0.1 MPa density (ρ/g·cm−3)
a
viscosity (η/mPa·s)
T/K
present work
published work
% AAD
present work
298.15
1.01238
1.013039 1.012140 1.0120242 1.0118043
0.030a 0.025b 0.008c 0.033d 0.038g 0.040h 0.051i
18.8870
18.8940 18.9541 18.9845
303.15
1.00935
15.10583
313.15
1.00216
323.15
0.99440
333.15
0.98624
1.009534 1.009838 1.0097039 1.008440 1.00800242 1.0079543 1.008044 1.001334 1.000938 1.0024739 1.000140 1.00003742 1.0000143 1.000044 0.992434 0.992938 0.9948039 0.991940 0.99201442 0.992044 0.9867539 0.983640 0.9839543 0.983944
15.10934 15.108838 14.8840 14.0541 15.046 15.108847 15.194048 10.02134 10.020938 9.9340 9.9541 9.9446 10.020947 10.028348 6.97034 6.971538 6.8940 6.8746 6.971547 6.946348 4.9740 5.00641 5.047347 5.045448
published work
10.02841
6.98330
4.97240
refractive index (nD) % AAD
present work
published work
% AAD
0.018a 0.016b 0.150d 0.540e 0.489j 0.322k 0.039l 0.083m
1.45406
1.4543239 1.452129
0.003c 0.070f
1.45241
1.4527339 1.450329
1.449
1.4491339
1.44522
1.4456139
1.44198
1.4421339
% AAD with ref 34. b% AAD with ref 38. c% AAD with ref 39. d% AAD with ref 40. e% AAD with ref 41. f% AAD with ref 29. g% AAD with ref 42. % AAD with ref 43. i% AAD with ref 44. j% AAD with ref 45. k% AAD with ref 46. l% AAD with ref 47. m% AAD with ref 48.
h
dissolved in double distilled water, with an equimolar amount of sodium hydroxide. An electronic analytical balance (Sartorius, model BSA-224S-CW) was used for all weight measurements with the measurement accuracy of ± 1·10−4 g. Different mass fractions (0.05, 0.10, 0.20, 0.30, and 0.40) were prepared. The uncertainty in concentration was determined to be ± 1·10−3. All the properties were measured within the temperature range of (298.15 to 343.15) K. The maximum mass fraction in the solution was kept at 0.40, as per the commercial suitability of solvent usage. Density Measurement. The density of different aqueous solutions of SP was measured using a digital oscillating tube densimeter (Anton Par, model, DMA- 4500M) having stated accuracy of ± 5·10−5 g·cm−3. The calibration of the apparatus cell was carried out every day and each time before the measurement in order to minimize the error in results. The
the calculation of molar refraction, which is helpful in the detailed understanding of the molecular interaction of the solvent.28−30 To the best of our knowledge, the data on physical properties of sodium L-prolinate (SP) is unavailable in open literature. Therefore, in the present work, density, viscosity, and refractive index of aqueous solutions of SP have been studied and reported.
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EXPERIMENTAL SECTION L-Proline (≥ 98 % pure), sodium hydroxide (≥ 99 % pure), and monoethanolamine (≥ 99 % pure), were purchased from Merck Sdn. Bhd, Malaysia. The additional information about the chemicals used in this study is specified in Table 1. All the chemicals were used without further purification. The double distilled water was used to prepare all the solutions. The aqueous solutions of SP were prepared by neutralizing L-proline B
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suppliers of chemicals, as well as the different measurement apparatus. These deviation values between our experimental results and those published in literature show fairly good agreement. The measured values of the density of aqueous solutions of SP at various temperatures from (298.15 to 343.15) K are presented in Table 3, and the density versus temperature is
standard water of Millipore quality was used in the calibration process. The temperature was regulated with a built-in solidstate thermostat. The measurements were performed in triplicate to report the data in average. The density and temperature uncertainty was ± 6·10−5 g·cm−3 and ± 0.01 K, respectively. Viscosity Measurement. A digital rolling ball microviscometer (Anton Par, model, Lovis- 2000M/ME) with the accuracy up to 0.5 % was used to measure the viscosity of SP aqueous solutions. Before filling the sample in a suitable capillary, the capillary was properly washed with acetone and air-dried to avoid any inaccuracy in the reading. Before and after each measurement, the viscometer was carefully calibrated with Millipore water. For the measurement, the capillary was filled with the sample by the help of 1 mL syringe, kept inside the viscometer until the temperature equilibration was achieved, and finally, the measurement was started. The temperature was controlled by the solid-state built-in thermostat. Triplicate measurements were carried out to report the viscosity data in average. The uncertainty of the viscosity and temperature was estimated to be ± 7·10−3 mPa·s and ± 0.02 K, respectively. Refractive Index Measurement. For measuring the refractive index of aqueous SP solutions, a fully automatic Abbemat refractometer (Anton Par, model WR) was used with the accuracy of ± 4·10 −5 nD. To get accurate results, the refractometer was calibrated with water of Millipore quality each time after changing the sample. Before pouring the sample into the sample holder, the prism face was carefully cleaned with acetone and dried to prevent the disturbance in results caused by the minute sediments on the prism face. Measurement was started after pouring the sample into the sample holder and setting the required temperature. The temperature was controlled by the internal thermostat. Each experiment was conducted thrice to present the data in average. The uncertainty in refractive index and temperature was ± 5·10 −5 nD and ± 0.03 K, respectively.
Table 3. Densities (ρ/g·cm−3) of Aqueous Solutions of SP at Mass Fractions of 0.05, 0.10, 0.20, 0.30 and 0.40 and at Pressure p = 0.1 MPaa density (ρ/g·cm−3) T/K
0.05
0.10
0.20
0.30
0.40
298.15 303.15 308.15 313.15 318.15 323.15 328.15 333.15 338.15 343.15
1.01528 1.01373 1.01198 1.01005 1.00796 1.00572 1.00332 1.00079 0.99813 0.99535
1.03390 1.03218 1.03028 1.02822 1.02601 1.02366 1.02118 1.01858 1.01587 1.01304
1.07161 1.06951 1.06729 1.06494 1.06247 1.05989 1.05721 1.05442 1.05156 1.04861
1.10981 1.10673 1.10408 1.10195 1.09931 1.09670 1.09278 1.09033 1.08820 1.08534
1.14869 1.14579 1.14283 1.13980 1.13671 1.13356 1.13034 1.12709 1.12380 1.12046
a Experimental uncertainties (u) for parameters are, u(T) = ± 0.01 K, u(ρ) = ± 6·10−5 g·cm−3, u(concn) = ± 0.001.
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RESULTS AND DISCUSSION Validation of the experimental methods and results were carried out in order to ensure the validity of the experimental data. For this purpose, experimental measurement of density, viscosity, and refractive index of pure monoethanolamine (MEA) were carried out at temperatures ranging from (298.15 to 333.15) K. The results obtained were compared in Table 2 with those of literature, and the validity of the results were evaluated based on the percent average absolute deviation between experimental and literature values published by various authors. The percent average absolute deviation (% AAD) was calculated using eq 1 as in the literature.31 1 %AAD = n
∑
Xexp − Ylit Ylit
Figure 1. Plot of experimental values of density versus temperature for different mass fractions of aqueous solutions of SP: ◇, 0.05; ○, 0.10; ▲, 0.20; ●, 0.30; △, 0.40.
shown in Figure 1. It was found that, with increasing the mass fraction of the SP in the solution, the density increases; however, the density decreases with the rise of temperature. This can be due to the wider spaces between the blend molecules at high temperature.31 This density trend is similar to previously reported work.32,33 The measured viscosity data of different concentrations of aqueous SP at different temperatures are listed in Table 4, and the viscosity versus temperature is shown in Figure 2. After analysis of the results, it was noticed that the viscosity decreases with an increase in temperature. This can occur because with the rise in temperature the internal resistance of molecules decreases, which allows the solution molecules to flow easily, thereby reducing the viscosity.
100 (1)
where n is the number of experimental data points, Xexp and Ylit are experimental and literature values, respectively. It was found that the minimum values of (% AAD) are 0.008 %, 0.016 %, and 0.003 % for density, viscosity, and refractive index respectively. Whereas, the maximum percent average absolute deviation is 0.051 % for density, 0.540 % for viscosity, and 0.070 % for refractive index, respectively. The deviation between experimental and literature values could be due to the difference in purities of chemicals used, the different C
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Table 4. Viscosities (η/mPa·s) of Aqueous Solutions of SP at Mass Fractions of 0.05, 0.10, 0.20, 0.30 and 0.40 and at Pressure p = 0.1 MPaa
Table 5. Refractive Indices (nD) of Aqueous Solutions of SP at Mass Fractions of 0.05, 0.10, 0.20, 0.30 and 0.40 and at Pressure p = 0.1 MPaa
viscosities (η/mPa·s)
refractive index (nD)
T/K
0.05
0.10
0.20
0.30
0.40
T/K
0.05
0.10
0.20
0.30
0.40
298.15 303.15 308.15 313.15 318.15 323.15 328.15 333.15 338.15 343.15
1.16030 1.01990 0.90282 0.80621 0.72447 0.65559 0.59830 0.54542 0.50077 0.46168
1.45620 1.26700 1.11360 0.98398 0.87844 0.78743 0.71178 0.64713 0.59299 0.54260
2.29210 1.96680 1.70220 1.48220 1.30950 1.16360 1.03770 0.92208 0.83454 0.75245
3.78667 3.32650 2.92330 2.50920 2.19330 1.94030 1.69040 1.51860 1.36090 1.20320
5.56010 4.80150 4.21030 3.53010 2.99670 2.58090 2.24140 1.96020 1.72850 1.53610
298.15 303.15 308.15 313.15 318.15 323.15 328.15 333.15 338.15 343.15
1.34005 1.33942 1.33879 1.33802 1.33724 1.33642 1.33569 1.33497 1.33424 1.33349
1.34767 1.34706 1.34633 1.34560 1.34502 1.34433 1.34373 1.34306 1.34256 1.34213
1.36337 1.36278 1.36201 1.36125 1.36042 1.35984 1.35931 1.35882 1.35866 1.35842
1.37937 1.37869 1.37768 1.37678 1.37586 1.37526 1.37439 1.37364 1.37322 1.37279
1.39604 1.39498 1.39387 1.39268 1.39154 1.39048 1.38912 1.38795 1.38677 1.38566
a Experimental uncertainties (u) for parameters are u(T) = ± 0.02 K, u(η) = ± 7·10−3 mPa·s, u(concn) = ± 0.001.
a Experimental uncertainties (u) for parameters are u(T) = ± 0.03 K, u(nD) = ± 5.0·10−5 nD, u(concn) = ± 0.001.
Figure 2. Plot of experimental values of viscosity versus temperature for different mass fractions of aqueous solutions of SP: ◇, 0.05; ○, 0.10; ▲, 0.20; ●, 0.30; △, 0.40.
Figure 3. Plot of experimental values of refractive index versus temperature for different mass fractions of aqueous solutions of SP: ◇, 0.05; ○, 0.10; ▲, 0.20; ●, 0.30; △, 0.40.
However, with increasing the concentration of SP, viscosity tends to increase. The higher concentrated solutions have high viscosity than lower ones, which may be due to the more molecular resistance in higher concentration solutions. The trend of the variation in viscosity values with change in concentration and temperature is the same as in the published work.33,34 An experimental data for refractive index of aqueous solutions of SP are presented in Table 5 at various temperatures, (298.15 to 343.15) K, and its relationship versus temperature is shown in Figure 3. From measured values, it was observed that, the refractive index increases with increase in concentration; however, with the rise in the temperature, it decreases slightly. The decrease in a refractive index with the increase in temperature can be due to an increase in speed of particles in aqueous SP solution, causing the light to strike fewer molecules thereby reducing the refractive index. In case of concentration, since the additional molecules are added in the solution, the chances of light striking the molecules are more, thereby increasing the refractive index.31,35 The decreasing trend of refractive index with rise in temperature, and increase with increasing the concentration is the same as reported in the literature.31,35
Experimentally measured data for density were converted into the graphical form with respect to temperature; the best fitting was carried out by least-squares method using linear regression software in the Analysis Toolpak of Microsoft Excel. The following fitting equation was developed.
X = A 0 + A 1T
(2)
where, X is the density, A0 and A1 are the fitting parameters, and T is the temperature. These fitting parameters are listed in Table 6 along with standard deviations calculated using eq 3 as also mentioned in literature.27 Table 6. Fitting Parameters of eq 2 and SD for Densities (ρ/ g·cm−3) of Aqueous Solutions of SP
D
SP mass fraction
A0
104 A1
R2
104 SD
0.05 0.10 0.20 0.30 0.40
1.14885 1.17349 1.22506 1.27196 1.33632
−4.4479 −4.6531 −5.1245 −5.4401 6.2816
0.99253 0.99451 0.99720 0.99773 0.99949
5.54 4.96 3.90 3.70 2.03
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⎡ ∑n (X − X )2 ⎤0.5 exp calc i ⎥ SD = ⎢ ⎢⎣ ⎥⎦ n
(3)
where n is the number of experimental data points, Xexp and Xcalc are experimental and calculated values, respectively. Figure 4 shows the comparison between experimental and predicted
Figure 5. Comparison between experimental values versus predicted values of viscosity for aqueous SP.
its relationship versus temperature followed by the series of different concentrations of aqueous solutions of SP. To fit the refractive index data, correlations were established by the leastsquares method in the Analysis Toolpak of Microsoft Excel. The best-fitting equation for this case was a polynomial function described by eq 5 with a value of R2 ≥ 0.99.
Figure 4. Comparison between experimental values versus predicted values of density for aqueous SP.
Z = C0 + C1T + C2T 2
density of aqueous SP system for all temperatures and mass fractions. The values of R2 (≥ 0.99) of fitting eq 2, and standard deviation between experimental and the predicted data show good agreement with each other. Hence, the established correlation for density can be used for predicting the density data of aqueous SP. Measured viscosity data was transformed into a graphical form with respect to the temperature. The fittings were conducted by method of least-squares using regression Analysis Toolpak of Microsoft Excel. The best fit was exponential function. Therefore, following exponential equation was used to fit the viscosity data. Y = B0 exp( −B1·T )
where Z is refractive index, C0, C1, and C2 are equation coefficients, and T denotes the temperature. The parameters of the refractive index fitting equation are listed in Table 8 Table 8. Fitting Parameters of eq 5 and SD for Refractive Index (nD) of Aqueous Solutions of SP SP mass fraction 0.05 0.10 0.20 0.30 0.40
(4)
where Y is the viscosity, B0, and B1 are the correlation coefficients, and T is the temperature. The fitting equation parameters are listed in Table 7 with standard deviations
B0
B1
R2
SD
0.05 0.10 0.20 0.30 0.40
481.555 931.184 3347.728 7817.272 32901.15
−0.02034 −0.02181 −0.02458 −0.02564 −0.02917
0.99449 0.99394 0.99567 0.99817 0.99758
0.018 0.024 0.037 0.034 0.081
C0 1.36925 1.43585 1.55425 1.54067 1.44074
C1
C2 −5
−5.388·10 −4.428·10−4 −1.094·10−3 −8.7793·10−4 −7.754·10−5
−7
1.50·10 4.90·10−7 1.53·10−6 1.13·10−6 2.40·10−7
R2
104 SD
0.99938 0.99923 0.99565 0.99769 0.99973
3.17 4.12 4.52 2.20 2.56
together with standard deviations estimated using eq 3, and the comparison of experimental and predicted values of refractive index are shown in Figure 6. The analysis of predicted data for refractive index also shows good consistency with experimental data. The developed correlation can be used to predict the refractive index data for the present aqueous system. The density data were used to calculate another property, termed as the thermal expansion coefficient (α). The thermal expansion coefficient of the aqueous SP was calculated using eq 6 as also mentioned in the literature.36,37
Table 7. Fitting Parameters of eq 4 and SD for Viscosity (η/ mPa·s) of Aqueous Solutions of SP SP mass fraction
(5)
calculated by eq 3, and the comparison of experimental and predicted viscosity values are shown in Figure 5. After the analysis of the predicted viscosity data obtained from the exponential fitting equation with an R2 value ≥ 0.99, it was noticed that the predicted data are in good relation with the experimental data, therefore, can be used for viscosity prediction of the studied system. Likewise, the refractive index data measured experimentally were plotted in the form of
αp = −
A1 1 ⎛ ∂ρ ⎞ ⎜ ⎟ = − ⎝ ⎠ ρ ∂T p A 0 + A1T
(6)
where αp is the coefficient of thermal expansion, ρ is the density, T is the temperature, and, from eq 2, A0 and A1 are the fitting parameters. The values of thermal expansion coefficients at various temperatures are listed in Table 9. The thermal expansion coefficient slightly increases with increasing temperE
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Funding
The authors are thankful to CO2 Management (MOR) research cluster of Universiti Teknologi PETRONAS for providing their financial and technical support to complete the present research work. Notes
The authors declare no competing financial interest.
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Figure 6. Comparison between experimental values versus predicted values of refractive index for aqueous SP.
Table 9. Coefficients of Thermal Expansion (α) of Aqueous Solutions of SP at Mass Fractions of 0.05, 0.10, 0.20, 0.30, and 0.40 α·104/(K−1) T/K
0.05
0.10
0.20
0.30
0.40
298.15 303.15 308.15 313.15 318.15 323.15 328.15 333.15 338.15 343.15
4.37 4.38 4.39 4.40 4.41 4.42 4.43 4.44 4.45 4.46
4.49 4.50 4.51 4.52 4.53 4.54 4.55 4.56 4.57 4.58
4.77 4.79 4.80 4.81 4.82 4.83 4.84 4.86 4.87 4.88
4.90 4.91 4.92 4.93 4.95 4.96 4.97 4.98 5.00 5.01
5.46 5.48 5.49 5.51 5.52 5.54 5.55 5.57 5.58 5.60
ature and concentration. This behavior is a general phenomenon and commonly reported for various aqueous systems.36,37
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CONCLUSION The physicochemical properties of aqueous SP solutions such as density, viscosity, and refractive index were measured at a range of temperatures from (298.15 to 343.15) K. Thermal expansion coefficient was calculated from density data. The measured properties were observed to be increasing with an increase in the mass fraction of SP in the solution. However, all properties tend to decrease with the increase in temperature. The same trend has been reported in the available literature. A little change was observed in the coefficient of thermal expansion values with an increase in temperature and concentration. All experimental data were correlated by mathematical fitting equations of least-squares in order to calculate the predicted data. On the basis of the deviations calculated between experimental and predicted data, there is a good agreement between both data. Hence, the developed correlations can be used satisfactorily in future CO2 removal system design calculations.
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REFERENCES
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dx.doi.org/10.1021/je400830w | J. Chem. Eng. Data XXXX, XXX, XXX−XXX
