Physical Properties of Aqueous Blends of Sodium Glycinate (SG) and

Feb 7, 2013 - (13-15) Originally, the use of various conventional solvents based on alkanoamines like MEA, ... (20-23) In addition, flooding and entra...
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Physical Properties of Aqueous Blends of Sodium Glycinate (SG) and Piperazine (PZ) as a Solvent for CO2 Capture 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 physical properties including the density, viscosity, and refractive index of aqueous blends of sodium glycinate (SG) and piperazine (PZ) as a solvent for CO2 absorption were measured under the wide temperature range (298.15 to 343.15) K. Different concentrations (mole fraction) of sodium glycinate and piperazine (SG + PZ) blends were (0.0348/0.0089, 0.0263/ 0.0177, 0.0177/0.0263, and 0.0089/0.0348), respectively. From the observations, it was found that the densities of the aqueous blends decrease when the piperazine concentration in the blend increases. It was noticed that the viscosity of the blend decreases initially by increasing the concentration of piperazine from 0.0089 to 0.0177 mole fraction; however, on further increasing the piperazine and decreasing the sodium glycinate concentration in the blend, the viscosity tends to increase. The refractive indices of the aqueous blend of sodium glycinate and piperazine decrease with increasing the concentration of piperazine in the blend. The density, viscosity, and refractive index of an aqueous blend of (SG + PZ) decreases with increasing temperature. The measured values of density, viscosity, and refractive index were correlated as a function of temperature by using standard equations of the least-squares method. All of the correlation parameters were reported together with the standard deviation.

1. INTRODUCTION The climate change issues due to the emissions of carbon dioxide (CO2) from various sources have become a challenge for many years because of the various deleterious effects of climate change on social, economic, and environmental agents. The major sources of CO2 emissions are the power plants, industries, transportation, agriculture, residential buildings, and energy sectors.1−8 The aim of CO2 capture is to be safe from its enormous effects results after climate change.10 The interest in the development of CO2 capture technology has increased due to the rising effects of global warming.11 In this regard, some techniques have been established for the removal and minimization of CO2 emissions from various sources, while others have been proposed to optimize the removal process. The techniques presently in operation include the absorption, adsorption, membrane, and cryogenic processes.8 The most commonly applied technique is absorption by chemical solvents. The absorption by chemical solvents is mature technology, and many advancements and successful alteration in the selection of the solvents have been made by various researchers.7−9 The most widely used solvents in industrial applications are alkanoamines like monoethanolamine (MEA), diethanolamine (DEA), and methyldiethanolamine (MDEA).13−15 Originally, the use of various conventional solvents based on alkanoamines like MEA, DEA, and MDEA © 2013 American Chemical Society

have been preferred for several benefits such as that the alcohol group minimizes drastically the vapor pressure of amine which results in almost no contamination of the treated gas by the amine. They also allow tunable amine reactivity to be in adequation with the gas acidity.17 After the long time use of amine-based solvents, it is identified that there are various potential drawbacks of the amine-based solvents used for the absorption of CO2. The identified potential drawbacks include inadequate lifetime due to amine oxidation degradation and as a result corrosion occurrence in pipelines and equipment which causes unplanned downtime, reduced equipment life, production losses, and management expenses to restore a corroded system.16,18,19 The energy cost is too high during desorption in combination with a high loss of liquid due to the evaporation of the solvent because of solvent’s high volatility in the stripper.20−23 In addition, flooding and entrainment of the absorption liquid limit the process, and the liquid gas stream cannot be controlled independently.12 Chemical solvents based on amino acids have been proposed in place of the amine-based solvents due to the various benefits. The various positive properties of amino acid based solvents including a higher Received: October 7, 2012 Accepted: January 24, 2013 Published: February 7, 2013 634

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repeatedly after completing each measurement. The reported data are the average of three readings with an accuracy of ± 0.00005 nD.

resistance to degradation, low volatility, and a smaller amount of oxidative degradation products encourage the researchers to work more on these solvents for commercial implementation.12,17,22 These amino acids can be made nonvolatile by adding salt functionality which lowers the liquid loss and consumption of energy associated with the process which ultimately affect positively on the process economics.13 Furthermore, interest is also raised to impart more suitable characteristics in amino acid based solvents by mixing the promoters and other compounds to enhance the absorption properties of the solvent blend. This has motivated us to prepare the new blend of solvent based on amino acid and promoter-like piperazine. For the practical implementation of the blend solvent prepared by sodium glycinate and piperazine in this study, it is very important to study the physical properties such as density and viscosity of the blend at various ratios and temperatures. The refractive index also helps to determine the composition of the liquid mixtures, and it has wide applications in chemical analysis and industries.28 In this paper, the physical properties including the density, viscosity, and refractive index of the aqueous blends of sodium glycinate and piperazine (SG + PZ) as a solvent for CO2 capture have been studied and reported.

3. RESULTS AND DISCUSSION The physical properties such as the density, viscosity, and refractive index of aqueous blends of sodium glycinate and piperazine (SG + PZ) were experimentally measured over the wide range of temperature and for various concentrations of SG and PZ. All of the equipment was calibrated before any measurement to validate the experimental data. The calibration was made with aqueous solutions of sodium glycinate with mass fractions of 0.1 and 0.2 at various temperatures, and the data were compared with the literature. The refractive index of Milipore quality water was also measured and compared with literature as presented in Table 1 as no data of RI on SG are Table 1. Comparison of Experimental data of Densities (ρ, in g·cm−3) and Viscosities (η, in mPa·s) of Aqueous Sodium Glycinate (SG) Solution and Refractive Index (nD) of Millipore Water with Literature Dataa density (ρ, in g·cm−3) SG mass fraction 0.1

2. EXPERIMENTAL SECTION The chemicals i-e glycine (≥ 99 % pure) and sodium hydroxide (≥ 99 % pure) were obtained from Merck Sdn. Bhd, Malaysia. Piperazine with purity (≥ 99 %) was purchased from Acros Chemicals Sdn. Bhd, Malaysia. Different blends of (SG + PZ) were prepared using double-distilled water. The different concentrations (mole fraction) of (SG + PZ) blends were (0.0348/0.0089, 0.0263/0.0177, 0.0177/0.0263, and 0.0089/ 0.0348), respectively, with a concentration accuracy of ± 0.001. The total blend concentration was kept at 0.0348 mole fraction, as amino acids form precipitates at higher concentrations and the properties were measured over the wide range of temperature. Measurement of Density. Densities of aqueous blends of (SG + PZ) of different concentrations were mearured using a digital Anton Par density meter (DMA-4500 M) with a measuring accuracy of ± 0.00003 g·cm−3 and temperature control accuracy of ± 0.01 K. The equipment was calibrated repeatedly after completing each measurement with standard water of Millipore quality. The data reported are the average of three measurements. Measurement of Viscosity. A digital Anton Par microviscometer (Lovis-2000 M) was used with suitable capillary tube to measure the viscosities in mPa·s of aqueous blends of sodium glycinate and piperazine (SG + PZ) of different concentrations. All of the reported values of viscosity are the average of three measurements with the accuracy of ± 0.002 mPa·s. The equipment was calibrated repeatedly after completing each measurement by standard water of Millipore quality, and the data were compared with literature. Before each measurement, the sample was kept inside the viscometer until the set temperature was reached at equilibrium conditions, and the temperature accuracy was ± 0.02 K. Measurement of Refractive Index. The refractive indices of aqueous blends of (SG + PZ) of various concentrations were evaluated under a wide range of temperature with the accuracy of ± 0.05 K. A digital Anton Par refractometer (Abbemet) was used to measure the refractive index nD. Standard water of Millipore quality was used to calibrate the equipment

0.2

T/K

exp.

303.15 313.15 323.15 333.15

1.0334 1.0299 1.0254 1.0203

T/K

exp.

ref 26

% AAD

303.15 313.15 323.15 333.15

1.2613 1.1839 1.1374 0.9572

1.261 1.184 1.137 0.957

0.0040

ref 26

% AAD

exp.

1.0332 0.0054 1.0803 1.0296 1.0765 1.0252 1.0719 1.0201 1.0668 viscosity (η, in mPa·s) SG mass 0.1

ref 26

% AAD

1.0800 1.0763 1.0718 1.0665 fraction

0.0052

0.2 exp.

ref 26

% AAD

1.3315 1.331 1.2481 1.248 1.2072 1.207 1.1670 1.165 refractive index (nD)

0.0140

Millipore water T/K

exp.

ref 29

% AAD

303.15 313.15

1.33229 1.33045

1.33221 1.33048

0.0009

a Experimental uncertainties (u) for u(conc. mass fraction) = ± 0.001, for density: u(T) = ± 0.01 K, u(ρ) = ± 0.00003 g·cm−3; for viscosity: u(T) = ± 0.02 K, u(η) = ± 0.002 mPa·s, for refractive index: u(T) = ± 0.05 K, u(nD) = ± 0.00005.

found in literature. There is a good agreement found between literature and the present work as indicated by the percent average absolute deviation (% AAD) values presented in Table 1. The percent average absolute deviation (% AAD) presented in Table 1 was calculated by the following equation.27 %AAD =

1 n

∑

Xexptl − Ylit. Ylit.

·100 (1)

The experimentally measured values of the physical properties including densities, viscosities, and refractive indices of aqueous blends of (SG + PZ) of different concentration (mole fraction) ratios (0.0348/0.0089, 0.0263/0.0177, 0.0177/0.0263, and 0.0089/0.0348) at different temperatures (298.15, 303.15, 308.15, 313.15, 318.15, 323.15, 328.15, 333.15, 338.15, and 635

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343.15) K are presented in Tables 2, 3, and 4, respectively. The temperature dependence of density, viscosity, and refractive Table 2. Densities (ρ, in g·cm−3) of Different Concentrations (Mole Fraction) of Aqueous Blends of (SG + PZ)a mole fraction of (SG + PZ) aqueous blends T/K

0.0348 SG + 0.0089 PZ

0.0263 SG + 0.0177 PZ

0.0177 SG + 0.0263 PZ

0.0089 SG + 0.0348 PZ

298.15 303.15 308.15 313.15 318.15 323.15 328.15 333.15 338.15 343.15

1.04997 1.04808 1.04603 1.04439 1.04157 1.03916 1.03663 1.03398 1.03123 1.02839

1.03497 1.03320 1.03125 1.02915 1.02690 1.02454 1.02204 1.01942 1.01669 1.01384

1.02571 1.02399 1.02209 1.02002 1.01780 1.01545 1.01296 1.01034 1.00761 1.00477

1.01413 1.01251 1.01069 1.00869 1.00654 1.00424 1.00178 0.99919 0.99647 0.99363

Figure 1. Densities of different concentrations (mole fraction) of aqueous blends of (SG + PZ) as a function of temperature: ◆, 0.0348 SG + 0.0089 PZ; △, 0.0263 SG + 0.0177 PZ; ■, 0.0177 SG + 0.0263 PZ; ○, 0.0089 SG + 0.0348 PZ.

Experimental uncertainties (u) for parameters are u(T) = ± 0.01 K, u(ρ) = ± 0.00003 g·cm−3, and u(conc. mole fraction) = ± 0.001. a

Table 3. Viscosities (η, in mPa·s) of Different Concentrations (Mole Fraction) of Aqueous Blends of (SG + PZ)a mole fraction of (SG + PZ) aqueous blends T/K

0.0348 SG + 0.0089 PZ

0.0263 SG + 0.0177 PZ

0.0177 SG + 0.0263 PZ

0.0089 SG + 0.0348 PZ

298.15 303.15 308.15 313.15 318.15 323.15 328.15 333.15 338.15 343.15

1.4410 1.2830 1.1520 1.0400 0.9466 0.8684 0.7989 0.7391 0.6848 0.6404

1.2990 1.1550 1.0340 0.9330 0.8491 0.7757 0.7135 0.6585 0.6092 0.5655

1.3660 1.2100 1.0790 0.9721 0.8820 0.8058 0.7411 0.6869 0.6369 0.5892

1.3980 1.2410 1.1140 1.0060 0.9146 0.8397 0.7793 0.7222 0.6679 0.6142

Figure 2. Viscosities of different concentrations (mole fraction) of aqueous blends of (SG + PZ) as a function of temperature: ◆, 0.0348 SG + 0.0089 PZ; △, 0.0263 SG + 0.0177 PZ; ■, 0.0177 SG + 0.0263 PZ; ○, 0.0089 SG + 0.0348 PZ.

a Experimental uncertainties (u) for parameters are u(T) = ± 0.02 K, u(η) = ± 0.002 mPa·s, and u(conc. mole fraction) = ± 0.001.

Table 4. Refractive Indices (nD) of Different Concentrations (Mole Fraction) of Aqueous Blends of (SG + PZ)a mole fraction of (SG + PZ) aqueous blends T/K

0.0348 SG + 0.0089 PZ

0.0263 SG + 0.0177 PZ

0.0177 SG + 0.0263 PZ

0.0089 SG + 0.0348 PZ

298.15 303.15 308.15 313.15 318.15 323.15 328.15 333.15 338.15 343.15

1.3513 1.3506 1.3499 1.3491 1.3485 1.3479 1.3476 1.3472 1.3470 1.3466

1.3502 1.3495 1.3488 1.3481 1.3472 1.3465 1.3459 1.3453 1.3448 1.3444

1.3500 1.3502 1.3496 1.3488 1.3481 1.3474 1.3468 1.3463 1.3458 1.3452

1.3484 1.3478 1.3470 1.3463 1.3456 1.3450 1.3442 1.3437 1.3433 1.3430

Figure 3. Refractive indices of different concentrations (M) of aqueous blends of (SG + PZ) as a function of temperature: ◆, 0.0348 SG + 0.0089 PZ; △, 0.0263 SG + 0.0177 PZ; ■, 0.0177 SG + 0.0263 PZ; ○, 0.0089 SG + 0.0348 PZ.

a function of temperature by using eq 2 and coefficients are reported in Tables 5 and 7, respectively, whereas the viscosity values measured experimentally were correlated by using eq 3 and coefficients are presented in Table 6. For all properties, the standard deviation was calculated using eq 4. (2)

Experimental uncertainties (u) for parameters are u(T) = ± 0.05 K, u(nD) = ± 0.00005, and u(conc. mole fraction) = ± 0.001.

X = A1 + A 2 (T /K) + A3(T /K)2

η /mPa·s = A1 ln(T /K) + A 2

(3)

index of the aqueous (SG + PZ) blend is shown in Figures 1, 2, and 3, respectively. The experimental results of density and refractive index were correlated by the least-squares method as

⎡ ∑n (X − X )2 ⎤0.5 exp calc i ⎥ SD = ⎢ ⎢⎣ ⎥⎦ n

(4)

a

636

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aqueous blend decrease when the piperazine concentration in the blend increases. It was noticed that the viscosity of the blend decreases initially by increasing the concentration (mole fraction) of piperazine to 0.0089; however, on further increasing the piperazine and decreasing the sodium glycinate concentration in the blend, the viscosity tends to increase. The refractive indices of the aqueous blend of sodium glycinate and piperazine decrease with increasing the concentration of piperazine in the blend. The density, viscosity, and refractive index of an aqueous blend of (SG + PZ) decrease with increasing temperature. All experimentally measured values were correlated using the least-squares method. The predicted values obtained from correlation equations are in good agreement with the measured values for all properties of the aqueous (SG + PZ) blend.

Table 5. Correlation Equation Parameters and SD for Densities (ρ, in g·cm−3) of Different Concentrations (Mole Fraction) of Aqueous Blends of (SG + PZ) conc. (mole fraction) SG + PZ 0.0348 SG + 0.0089 PZ 0.0263 SG + 0.0177 PZ 0.0177 SG + 0.0263 PZ 0.0089 SG + 0.0348 PZ

A1

103 A2

106 A3

R2

SD

0.927

1.190

−2.607

0.999

0.037193

0.905

1.216

−2.630

1.000

0.043341

0.881

1.310

−2.771

1.000

0.026891

0.842

1.475

−3.014

1.000

0.009332

Table 6. Correlation Equation Parameters and SD for Viscosities (η, in mPa·s) of Different Concentrations (Mole Fraction) of Aqueous Blends of (SG + PZ) conc. (mole fraction) SG + PZ 0.0348 0.0263 0.0177 0.0089

SG SG SG SG

+ + + +

0.0089 0.0177 0.0263 0.0348

PZ PZ PZ PZ

A1

A2

R2

SD

−5.555 −5.076 −5.351 −5.368

33.006 30.146 31.766 31.899

0.969 0.97 0.966 0.969

0.0442 0.0399 0.0450 0.0429

■

*Tel.: + 60 (17) 5789914. Fax: + 60 (5) 3654090. E-mail: [email protected]. 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.

Table 7. Correlation Equation Parameters and SD for Refractive Index (nD) of Different Concentrations (Mole Fraction) of Aqueous Blends of (SG + PZ) conc. (mole fraction) SG + PZ 0.0348 SG + 0.0089 PZ 0.0263 SG + 0.0177 PZ 0.0177 SG + 0.0263 PZ 0.0089 SG + 0.0348 PZ

AUTHOR INFORMATION

Corresponding Author

Notes

The authors declare no competing financial interest. A1

103 A2

106 A3

R2

SD

1.5344

−1.1000

1.0000

0.9970

0.0640

1.4722

−0.6000

0.8000

0.9980

0.0151

1.4495

−0.5000

0.6000

0.9990

0.0030

1.4789

−0.7000

0.9000

0.9970

0.0017

■

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where X in eq 2 is the density or refractive index, and A1, A2, and A3 are the correlation parameters of eq 2 and 3, respectively. The experimental results of the density measurement show that, with increasing the concentration of piperazine in the blends, density decreases linearly. However, the viscosity of (SG + PZ) blend decreases initially with increasing the concentration of PZ from 0.0089 to 0.0177 mole fraction, while on further increases in PZ concentration in the blend, it increases sharply. The refractive index of the blend decreases slowly with increasing the PZ concentration in the blend. All measured properties were observed to be decreasing with an increase in the temperature. This can be due to the reason that, when temperature of blends or solution mixtures increase, the intermolecular forces of attraction between them decreases. This results in the molecules of liquid mixtures occupying wider space thereby reducing the density and viscosity of the blend. For different solvents, the trend with an increase in temperature is the same.24−27

4. CONCLUSION The physical properties of aqueous blend of sodium glycinate and piperazine as a solvent for CO2 capture were studied in the present work at a temperature range of (298.15 to 343.15) K and concentration ratios of (0.0348/0.0089, 0.0263/0.0177, 0.0177/0.0263, and 0.0089/0.0348). The densities of the 637

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