Adsorptive Separation of Acetic Acid from Dilute Aqueous Solutions

Nov 20, 2015 - ZSM-5 (Zeolite Scony Moblie-5) (SiO2/Al2O3 = 360, 470), NaY, 13X (pellet, powder) and coconut shell activated carbon (YK-AC) are employ...
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Adsorptive Separation of Acetic Acid from Dilute Aqueous Solutions: Adsorption Kinetic, Isotherms, and Thermodynamic Studies Huanhuan Zhang, Yuming Wang, Peng Bai, Xianghai Guo,* and Xiuxiu Ni Key Laboratory of Systems Bioengineering, Ministry of Education, Tianjin 300072, China Department of Pharmaceutical Engineering, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China ABSTRACT: ZSM-5 (Zeolite Scony Moblie-5) (SiO2/Al2O3 = 360, 470), NaY, 13X (pellet, powder) and coconut shell activated carbon (YK-AC) are employed for acetic acid separation from dilute aqueous solutions via adsorption. Zeolite 13X exhibits a much higher adsorption capacity than other zeolites and activated carbon. The effects of adsorption time and different initial acetic acid concentrations were studied. At 71.77 g·kg−1, the initial acetic acid concentration, 13X in pellet exhibited the highest uptake capacity of 354.03 mg·g−1 at 318 K. Meanwhile, adsorption equilibrium, kinetics, and thermodynamics of an acetic acid aqueous solution on zeolite 13X in pellet were studied in batch experiments. Kinetic models such as pseudo-first-order, pseudo-second-order, and Elovich have been used to describe the adsorption behavior of zeolite 13X in pellet. Pseudo-second-order was found the most suitable for this system. Langmuir and Freundlich isotherm models were applied to experimental data depending on temperature. The Freundlich isotherm fitted the experimental data better than the Langmuir isotherm for adsorption of acetic acid. Using the thermodynamic equilibrium coefficients obtained at different temperatures, the thermodynamic constants (ΔG, ΔH, and ΔS) of adsorption were also calculated, and the results indicated that the adsorption process of acetic acid on zeolite 13X in pellet was spontaneously endothermic. extraction,3−5 pervaporation,6−8 membrane filtration,9 and bipolar membrane electrodialysis (BMED)10,11 have been used for this process. Although these methods show good separation selectivity, high cost and energy consumption limited their applications in industry.12,13 Compared with the methods above, the adsorption process allows flexibility in terms of both design and operation. After adsorption they can be easily regenerated, thereby resulting in significant cost savings. Although some kinds of adsorbents have been tried for adsorption of acetic acid, there is still lack of suitable adsorbents effectively for acetic acid recovery from dilute aqueous solutions.14−18 As part of the process for selection of the adsorbents, the following information is necessary on the characteristics of the adsorbents: (1) the equilibrium capacity of the adsorbent, (2) the selectivity of the adsorbent, (3) physical and chemical characteristics of the adsorbent, (4) the regeneration characteristic of the adsorbent. To test the suitability of adsorbents such as zeolites ZSM-5, NaY, 13X, coconut shell activated carbon (YK-AC), we have undertaken a study on adsorption of acetic acid solutions on these materials. This paper focuses specially on acetic acid adsorption process from dilute aqueous solutions and evaluates equilibrium, kinetic

1. INTRODUCTION Acetic acid is an important raw material in industry and has been widely used as solvent in food, pharmaceutical, chemical, and dyes industries. Understandably, with the rapid increasing demand of acetic acid, a large number of wastewaters containing acetic acid at different concentrations emerged from those industries, including the production of acrylic acid, cellulose acetate, terephthalic acid, poly(vinyl alcohol), and acetaldehyde by the Wacker process, destructive distillation of wood, and reactions involving acetic anhydride, etc. These wastewaters show strong acidities and the chemical oxidation demands (CODs) usually reach as high as 10 000 mg·L−1 to 100 000 mg·L−1, making it very difficult to biodegrade and impossible to be discharged directly.1 On the other hand, acetic acid is mainly produced by the fermentation processes employing anaerobic microorganisms, which is characterized by lower feedstock cost, low energy consumption, and low temperature and pressure. However, the common problem of the process is to extract acetic acid from solutions, because of the low concerntration values of acetic acid (∼ 10 %) and intensive energy by distillation.2 Unfortunately, separation of acetic acid from dilute aqueous solutions, especially below 5 % (weight percentage, as follows), is very difficult, even implausible because of the close boiling point of two compounds. To improve the efficiency of separation of acetic acid from water solution and reduce energy consumption, reactive © XXXX American Chemical Society

Received: June 11, 2015 Accepted: November 9, 2015

A

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were recorded by an X-ray diffractometer (D8, Bruker) using Cu Kα radiation. 2.3. Batch Adsorption Procedure. The required solutions of different acetic acid concentrations were prepared by dissolving some amount of acetic acid into deionized water. The adsorption experiments were performed at batch scale. A weighed amount (5.00 ± 0.01 g) of adsorbent was added into a 250 mL round-bottom flask containing 100 mL of acetic acid solution with known concentrations. The bottle was shaken for 6 h on magnetic stirrers at 200 rpm. After mixing, the solutions were centrifuged for 20 min with 5000 rpm, and the supernatant was kept for determination of the remaining acetic acid concentration. Samples were measured in triplicate, and the average value was used in subsequent analysis. The acetic acid adsorbed by 13X in pellet zeolite was calculated from the initial and final concentrations according to the following equation:

and thermodynamic parameters of the system, which are significant for design of waste dilute acetic acid recovery system.

2. MATERIALS AND EXPERIMENT METHODS 2.1. Materials. Acetic acid (purity, > 0.99), and sodium hydroxide (NaOH, purity, > 0.96) are of analytical grade and used without further purification. Deionized water was used throughout the experiments. The adsorbents for acetic acid adsorption included ZSM-5 (SiO2/Al2O3 = 360, 470), NaY, YK-AC, 13X (pellet, powder), which were purchased from Nankai University, except YK-AC which came from a wastewater treatment plant. The characteristics of these materials were shown in Table 1. Table 1. Characteristics of Adsorbent Used in the Study adsorbent

type

SiO2/Al2O3

ABET(m2/g)

ZSM-5(I) ZSM-5(II) NaY YK-AC 13X(I) 13X(II)

strip strip pellet granular pellet powder

360 470 4.8 to 5.6

340 340 720 1000 680 740

< 3.0 < 3.0

Qe =

ABET, specific surface area determined by nitrogen adsorption at 77 K

V (C0 − Ce) m

(1)

where Qe (mg/g) is the amount of acetic acid adsorbed, C0 is the initial concentration (g/L), Ce is the equilibrium concentration (g/L), V the volume of the solution (mL) and m is the amount of 13X in pellet added (g). The acetic acid removal efficiency R (%) is calculated by following equation:

2.2. Instruments. The acetic acid concentration was determined by titrated with NaOH solutions, and phenolphthalein was used as an indicator. Field emission scanning electron microscope (FESEM, SU8010) was used to characterize the surface morphology of the zeolite 13X and acetic acidadsorbed 13X samples. The X-ray diffraction (XRD) patterns

R=

C0 − Ce 100 C0

(2)

Figure 1. Characterization of zeolite 13X: (a) SEM image of 13X before adsorption; (b) SEM image of 13X after adsorption; (c) comparison of XRD pattern of 13X before and after adsorption. B

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Table 2. Influence of Different Adsorbentsa

a

adsorbent

type

initial concn C0 (g·L−1)

equil concn Ce (g·L−1)

Qe (mg·g−1)

ZSM-5(I) ZSM-5(II) NaY YK-AC 13X 13X

strip strip pellet granula pellet powder

31.68 31.68 31.68 31.68 31.68 31.68

27.74 27.35 27.27 23.85 19.75 15.89

78.80 86.60 88.20 156.60 238.60 315.80

Standard uncertainties u are u(Ce) = 0.01 Ce, and the combined expanded uncertainty Uc is Uc(Qt) = 0.001 Qt

3. RESULTS AND DISCUSSION 3.1. Characterization of Zeolite 13X in Pellet. The SEM and XRD of zeolite 13X before and after adsorption were shown in Figure 1. SEM shows that the morphology and particle size of zeolite 13X did not change visibly. Moreover, no obvious change in XRD patterns of zeolite 13X was observed after adsorbing acetic acid. The results verify that zeolite 13X was stable when exposed to dilute acetic acid solution. 3.2. Influence of Different Adsorbents. The adsorbents, including ZSM-5 (SiO2/Al2O3 = 360, 470), NaY, 13X (pellet, powder), YK-AC were used for acetic acid adsorption. The amount of adsorbed acetic acid per gram adsorbent was listed in Table 2. It is observed that the quantities of adsorbed acetic acid over 13X is much higher than other zeolites and activated carbon. This may be due to the two possible reasons as follows: (1) the pore size of 13X is 10 Å which is larger than acetic acid with 4.5 Å and allows the acetic acid to move across the pore smoothly; (2) the higher adsorption percentage may be attributed to the presence of Na+.19,20 It is well-known that 13X belongs to faujasite aluminosilicates which are hydrophilic adsorbents due to extra-framework charge cations and frameworks that are electrostatically charged.21 So type X zeolites are highly selective for acetic acid from dilute solutions. Though NaY zeolite has a 10 Å pore size and the presence of Na+, the adsorption capacity of NaY is much lower than 13X, which is probably due to the higher silica−alumina ratio than 13X.20 13X in powder shows more considerable adsorption capacity than 13X in pellet because of a larger surface area. In practical application, the pellet is more mechanically stable and easily disposed and operated, therefore this paper studied the kinetic and thermodynamic parameters of 13X in pellet for the design on industry. 3.3. Effect of Contact Time and Adsorption Kinetics Model. The influence of the contact time is another essential parameter in practical applications. The effect of adsorption time for acetic acid by 13X in pellet has been investigated for the determination of equilibrium time. The results of the effect of contact time are shown in Figure 2. The consequence indicated that the adsorption efficiency increased as time passed, until the equilibrium concentration of acetic acid approximately reached constant. The equilibrium time is about 4.5 h for 31.50 g·L−1 initial acetic acid concentration at 298 K. After equilibrium time, there is no significant decrease in equilibrium concentration of acetic acid, so 6 h was chosen as the optimum time to ensure that the equilibrium was really achieved for subsequent isotherm studies. Meanwhile, to identify the adsorption kinetics of acetic acid on the solid surface of 13X in pellet, three kinetics models, the pseudo-firstorder, pseudo-second-order, and Elovich models, were applied to investigate the kinetics as given in the following text. Pseudo-first-order Model. The pseudo-first-order rate expression based on capacity is generally expressed as follows:22

Figure 2. Effect of contact time on the adsorption of acetic acid on 13X in pellet.

dQ t dt

= k1,ad(Q e − Q t ) −1

(3)

−1

where k1,ad (g·mg ·h ) is the pseudo-first-order rate constant. Qe (mg·g−1) and Qt (mg·g−1) are the amount of acetic acid adsorbed per unit weight of the adsorbent at equilibrium and time t. The linear form of eq 3 can be given as23 log(Q e − Q t ) = log Q e −

k1,ad 2.303

t

(4)

If first-order kinetic model is applicable, the plot of log(Qe − Qt) against t of eq 4 should give a liner relationship, from which k1,ad can be obtained from the slope and intercept. The correlation of pseudo-first-order model is presented in Figure 3,

Figure 3. Pseudo-first-order kinetic of acetic acid-13X in pellet zeolite.

which shows the correlation coefficient R2 of 0.9658. Actually, in most cases the first-order kinetic model does not fit well for the whole range of contact time and is generally applicable over the initial 20−30 min of sorption process. Pseudo-second-order Model. The pseudo-second-order model assumes that the adsorption rate is determined by the square of vacant sites on the surface and adsorption process is controlled by the chemical adsorption, and the chemical C

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adsorption is related to the share or transport of electrons between adsorbate and adsorbent. The pseudo-second-order equation is also based on the sorption capacity, which is expressed as24 dQ t dt

= k 2,ad(Q e − Q t )2 −1

(5)

−1

where k2,ad (g·mg ·h ) is the rate constant of second-order adsorption. For the same boundary conditions the integrated form of eq 5 becomes t 1 1 = + t 2 Q Qe k 2,adQ e (6)

Figure 5. Elovich model of acetic acid-13X in pellet zeolite.

Figure 4 showed the linear plot of the pseudo-second-order model. The high correlation coefficient R2 of 0.9986 suggested

acetic acid from aqueous to the adsorbent surface. Results of various initial concentrations of acetic acid were listed in Table 3 with respect to temperature. It can be observed that increasing the initial acid concentration from 12.03 g·L−1 to 71.93 g·L−1 at 298 K, the efficiency of removal decreased from 61.47 % to 21.26 % and the uptake of acetic acid by 13X in pellet increased from 138.8 to 321.1 mg·g−1. This may be explained by the saturation of accessible exchangeable sites of the adsorbent and the important driving force to overcome the mass transfer resistance of acetic acid between aqueous and adsorbent. In addition, to help to explain the adsorption mechanism and heterogeneity of the adsorbate surface, and establish the most appropriate isotherm to optimize the design of the sorption system, Langmuir and Freundlich isotherm models were used to fit experimental data. Langmuir Isotherm. Langmuir model supposes that the surface of adsorbent is uniform; there is no interaction between adsorbates; adsorption is monolayer and adsorption happens outside the surface.26 Therefore, this model is stricted by the experimental conditions and the parameters should be adjusted once the conditions change. So Langmuir model applies to monolayer chemical adsorption. The saturation monolayer can be represented by the following expression:

Figure 4. Pseudo-second-order kinetic of acetic acid-13X in pellet zeolite.

that the adsorption data of acetic acid fit well with the pseudosecond-order model. The Elovich Kinetic Model. The Elovich equation describes the process of series of reaction mechanism, such as diffusion of solute in solution phase or interface, surface activation, and deactivation. It is suitable to the process with significant activation energy changes. Moreover, the Elovich equation can also reveal the irregularity of data that other dynamic equations have ignored. The Elovich model equation can be written as25 dQ = α exp( −βQ ) dt −1

Qe =

KAQ 0Ce 1 + KACe

(9)

−1

where Qe (mg·g ) is the equilibrium amount of adsorbate adsorbed by the solid, Ce (g·L−1) is the equilibrium concentration of adsorbate, and Q0 (mg·g−1) and KA (L·g−1) are Langmuir constants representing the monolayer adsorption capacity and the adsorption ability of the adsorbent, respectively. The linearized form of Langmuir model is given as27

(7)

−1

where α (mg·g ·h ) is known as the rate of adsorption. β (g· mg−1) is known as coefficient of desorption. In fact, eq 7 can be written as 1 1 Q t = ln(αβ) + ln(t ) β β (8)

Ce = −

which is a simplified form of the Elovich equation when the adsorbed Qt is zero at time t = 0 and αβt ≫ 1. If acetic acid adsorption on 13X in pellet obeys the Elovich kinetic model, Qt vs ln(t) must give a line with a slope of values of 1/β and intercept of ln(αβ). Figure 5 shows a plot of the Elovich equation for adsorption of acetic acid on 13X in pellet, and the correlation coefficient R2 is 0.9890, which implies the Elovich model is less suitable for the acetic acid adsorption process on 13X in pellet zeolite than pseudo-second-order model. 3.4. Effect of Initial Concentration of Acetic Acid and Adsorption Isotherm. the initial concentration of acetic acid should be considered during the acetic acid adsorption process, because it provides the driving force to promote the transfer of

Q 1 + Ce 0 KA Qe

(10)

The values of KA and Q0 are determined from the intercept and slope of the straight line in Figure 6. The parameters of the Langmuir equation are presented in Table 4. Freundlich Isotherm. The Freundlich equation is suitable to both monolayer adsorption and ununiform surface adsorption. Freundlich model describes the adsorption mechanism on the heterogeneous surface and is fit for the adsorption of low concentation. It can also explain the experimental results in a wide range. However, the Freundlich isotherm provides no information on the monolayer adsorption capacity. The Freundlich model is applicable to a heterogeneous surface and is given as28 D

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Table 3. Effect of Initial Concentrations and Temperature on Acetic Acid Adsorptiona T (K)

initial concn C0 (g·L‑1)

amount of 13X in pellet (g)

equil concn Ce(g·L‑1)

adsorbed acid Qe (mg·g‑1)

298

12.03 21.35 31.59 52.92 71.93 11.76 21.16 31.94 53.78 71.77 11.76 21.16 31.94 53.78 71.77

5.00 5.00 5.00 5.00 5.00 5.00 5.00 5.00 5.00 5.00 5.00 5.00 5.00 5.00 5.00

5.26 12.28 20.20 38.46 55.95 4.75 11.94 20.37 38.28 54.85 4.59 11.63 20.18 37.71 54.13

134.83 181.00 227.91 289.37 321.17 140.02 184.12 231.15 310.43 339.14 142.58 189.93 234.92 321.79 354.03

308

318

a

Standard uncertainties u are u(Ce) = 0.01 Ce, u(T) = 0.02 K, and the combined expanded uncertainty Uc is Uc(Qt) = 0.001 Qt

Figure 7. Freundlich isotherms of acetic acid-13X in pellet adsorption at different temperatures: blue ◆, 298 K; red ■, 308 K; green ▲, 318 K.

Figure 6. Langmuir isotherms of acetic acid-13X in pellet adsorption at different temperature: blue ◆, 298 K; red ■, 308 K; green ▲, 318 K.

Table 5. Freundlich Isotherm Parameters for Adsorption of Acetic Acid on 13X in Pellet Zeolite

Table 4. Langmuir Isotherm Parameters for Adsorption of Acetic Acid on 13X in Pellet Zeolite

Freundlich isotherm

Langmuir isotherm T (K)

Q0 (mg·g‑1)

KA (L·g‑1)

R2

298 308 318

383.87 405.48 426.77

4.69 4.79 4.94

0.9898 0.9810 0.9755

Q e = KFCe1/ n

1 log Ce n

KF (mg·g−1)

n (L·g−1)

R2

298 308 318

72.04 72.79 74.37

2.66 2.58 2.55

0.9957 0.9924 0.9918

of 0.9957 at 298 K, which indicates that acetic acid adsorption on 13X in pellet fits well with the Freundlich isotherm and the heterogeneous distribution of adsorption sites over the adsorbent surface. The best-fit Freundlich parameters n at 298 K is 2.66. The n value of more than 1 indicates that the attractive force to promote the adsorption exists between the adsorbent surface and adsorbate, an indication of a favorable adsorption process.28 3.5. Effect of Temperature on Acetic Acid Adsorption. The equilibrium uptake of acetic acid was also affected by temperature and increased slightly with increasing temperature up to 318 K, which was also shown in Table 3 as well. At 71.77 g·kg−1 initial acetic acid concentration, the equilibrium uptake capacity of 13X in pellet increased from 339.1 mg·g−1 to 354.0 mg·g−1 acetic acid with increasing temperature from 308 K to 318 K. Acetic acid adsorption was endothermic thus the uptake of adsorption increased with increasing temperature, which implied that acetic acid adsorption may involve not only physical and chemical interactions. This may be attributed to

(11)

where KF (mg·g−1) and 1/n (L·g−1) are the constants that are characteristics of the system, which indicate the adsorption capacity of the adsorbent and the intensity of the adsorption, respectively. A logarithmic plot linearizes the equation enabling the exponent n and the constant KF to be determined:29 log Q e = log KF +

T(K)

(12)

From eq 12, the Freundlich coefficients can be determined from the plot of log Qe versus log Ce. Freundlich isotherms for 298 K, 308 K, and 318 K are shown in Figure 7. Results of the Freundlich isotherm are summarized briefly in Table 5. On the basis of Figure 5 and Table 4, the Langmuir plot was found to be linear (R2 = 0.9898) and the value of Q0 was 383.87 mg·g−1 at 298 K. The regression coefficients of the Freundlich model are better than those of the Langmuir model, R2 values E

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due to a stronger interaction between the preadsorbed water and the adsorbent than interaction between the acetic acid and the adsorbent. The positive standard entropy change ΔS (24.29 J·mol−1·K−1) confirms the increased randomness at the solidsolution interface during adsorption because the number of desorbed water molecules is larger than that of the adsorbed acetic acid. This positive ΔS is easily understandable considering the molecular size of water and acetic acid.

the creation of some new active sites on the adsorbent surface or the activation of the adsorbent surface to strengthen the attractive forces between acetic acid and 13X in pellet zeolite. 3.6. Thermodynamic Data. To study the thermodynamics of the acetic acid adsorbed onto 13X in pellet zeolite, the effect of temperatures on adsorption was conducted at 298 K, 308 K, 318 K and the thermodynamic constants such as change in enthalpy (ΔH), Gibbs free energy (ΔG), and entropy (ΔS) were determined. The free energy change of adsorption ΔG was calculated by using the following equation: ΔG = −RT ln KC

4. CONCLUSION ZSM-5 (SiO2/Al2O3 = 360, 470), NaY, 13X (pellet, powder), YK-AC are employed for acetic acid separation from aqueous solutions. The adsorption capacity of zeolite 13X in powder and pellet reached 315.8 mg·g−1 and 238.60 mg·g−1 at 298 K, respectively, which was much greater than other zeolites and activated carbon. Then the research demonstrated that contact time, temperature, and initial acetic acid concentration highly affected the adsorption capacity on 13X in pellet zeolite. The uptake of acetic acid increased with an increase in both acetic acid concentration and temperature. The results found that the kinetics could be well fitted by a pseudo-second-order model and the isotherm could be characterized well by the Freundlich isotherm model. Thermodynamic constants were also evaluated using equilibrium constants changing with temperature. The negative values of ΔG indicated the spontaneity. The positive value of ΔH (1364.62 J·mol−1) and ΔS (33.13 J·mol−1·K−1) showed the endothermic nature and increase in disorder of acetic acid, respectively. We believe that the adsorption of acetic acid by zeolite 13X in pellet can be beneficial for designing wastewater treatment plants through the kinetic and thermodynamic parameters.

(13) −1

−1

where R (8.314 J·mol ·K ) is the universal gas constant; T (K) is Kelvin temperature; KC is the thermodynamic equilibrium constant for adsorption process. KC is obtained by plotting Ce/Qe versus Ce and extrapolating to zero Ce, which shows the linearized form of Langmuir equation.30,31 The other thermodynamic parameters, change in enthalpy (ΔH) and entropy (ΔS) were calculated from the slope and intercept of the plot of ln KC against 1/T according to the equation:32 ΔS ΔH − (14) R RT ΔH and ΔS were obtained by plotting ln KC against 1/T as shown in Figure 8; ΔG values corresponding to each ln K C =

■

AUTHOR INFORMATION

Corresponding Author

*E-mail: [email protected]. Funding

Project supported by the National Natural Science Foundation of China (No. 21202116).

Figure 8. Relationship of KC and T.

Notes

The authors declare no competing financial interest.

■

temperature were also found according to eq 13. The calculated thermodynamic constants derived from the adsorption of acetic acid on 13X in pellet zeolite were given in Table 6. The Table 6. Thermodynamic Parameters for the Acetic Acid Adsorption on 13X in Pellet Zeolite at Different Temperatures (298 K, 308 K, 318 K) temp (K)

ΔG (J·mol‑1)

KC

ΔS (J·mol−1·K−1)

ΔH (J·mol−1)

298 308 318

−8512.41 −8830.07 −9175.61

31.06 31.45 32.15

33.13

1364.62

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negative value of the Gibbs free energy indicates the adsorption of acetic acid on 13X in pellet is thermodynamically spontaneous and the higher negative value reflects a more energetically favorable adsorption. 33 The obtained ΔH (1364.62 J·mol−1) suggests that the adsorption process of acetic acid on 13X in pellet is endothermic and the adsorption process is more favorable at higher temperature in accordance with the increasing adsorption capacity with an increasing adsorption temperature. The endothermic adsorptions may be F

DOI: 10.1021/acs.jced.5b00481 J. Chem. Eng. Data XXXX, XXX, XXX−XXX

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DOI: 10.1021/acs.jced.5b00481 J. Chem. Eng. Data XXXX, XXX, XXX−XXX