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INTERNATIONAL JOURNAL OF ENVIRONMENTAL SCIENCES

Volume 6, No 1, 2015

© Copyright by the authors - Licensee IPA- Under Creative Commons license 3.0

Research article

ISSN

0976 – 4402

Pseudo second order kinetic model for the sorption of U (VI) onto soil: A comparison of linear and non-linear methods

Sabyasachi Rout, Ajay Kumar, Pazhayath Mana Ravi, Raj Mangal Tripathi Health Physics Division, Bhabha Atomic Research Centre, Mumbai, India-400085 srout.barc@gmail.com

doi:10.6088/ijes.6017

India-400085 srout.barc@gmail.com doi:10.6088/ijes.6017 ABSTRACT Batch kinetic experiments were carried out for the

ABSTRACT

Batch kinetic experiments were carried out for the sorption of U(VI) onto three types of soil. The experimental kinetics were fitted to the pseudo second-order kinetics by linear and a non- linear method. The four different types of Ho pseudo second-order expression have been discussed. A comparison of linear least-squares method and a trial and error non-linear method of estimating the pseudo second-order rate kinetic parameters were examined. The sorption process was found to follow pseudo second-order kinetic model. Present investigation showed that it is appropriate to use a linear model-1 pseudo second-order expressions as proposed by Ho for predicting the kinetic rate constants and the initial sorption rate for the studied system. And the transformation of nonlinear form to linear model-1 changed the conditions in a positive way leads to minimization of error structure and that caused that the linear model-1 give very similar or better fits than other models. Different linear models predicts different reaction rate , hence to avoid this ambiguity it is better to use nonlinear model if the process designer is unable to study the experimental data using all the models.

Keywords: Kinetics, Pseudo first order, Pseudo second order, linear, non linear

1. Introduction

Adsorption is the most important process which predicts the fate of contaminants at soil- water interface in the environment and it is the most commonly used technique for the treatment of industrial waste waters. For practical applications of adsorption such as process design and control, it is important to model the adsorption rate and to establish the time dependence of adsorption systems under various process conditions. The rate at which sorption takes place is of the utmost importance when designing batch sorption systems, accordingly it is important to establish the time dependence of such systems under various process conditions. Kinetics explain how fast the rate of chemical reaction occurs and also on the factors affecting it. Many mechanistic models have been suggested to describe the adsorption kinetics such as; film-solid model (McKay G et al, 1991) the film-pore model (Al- Duri B et al 1992) and the branched pore model (Peel RG et al, 1981) etc. give detailed analysis of the adsorption dynamics. However, these models are presented as partial differential equations and their solution needs dedicated computer programs and extensive computer time. Therefore, it is impractical to use these models in practice as it is preferred to have more simple relations that can be solved quickly and easily. Even in the area of research, most researchers prefer to use simple lumped kinetic models to analyze their experimental results. Literature survey shows that Boyd's film-diffusion (Boyd GE et al, 1947) and Weber's intra particle-diffusion (Weber Jr et al, 1947) are the two most widely used models for studying the mechanism of adsorption. However, in spite of their apparent simplicity, the use

Received on January 2015 Published on July 2015

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Pseudo second order kinetic model for the sorption of U (VI) onto soil: A comparison of linear and non-linear methods

of both the intraparticle-diffusion and the film-diffusion models often suffers from uncertainties due to their multi-linear nature (Ho YS et al, 1998). At the present time pseudo kinetics models such as; Pseudo first order kinetics (PFO) and pseudo second-order (PSO) are more frequently used to explain the adsorption kinetics of solid/liquid system (Ho YS et al, 1998; Kumar KV et al, 2005; Fu Y et al, 2000). In some literature multiple first order kinetics has been reported for adsorption on protein/silica system also (Sarkar D et al, 1993). Previously researchers (Ho YS et al, 1998; Kumar KV et al, 2005) found that the experimental kinetic data well fit to Lagergren pseudo first-order kinetics, where the probable adsorbate interactions were assumed to be negligible. It was also observed that though the Lagergren pseudo first-order kinetics provide excellent fit with the experimental kinetic data, it failed to predict the equilibrium adsorption capacity (qe) theoretically thus differing from the theory (Allen SJ et al, 2005). In recent years, Ho (Ho YS, 1995) described sorption, which included chemisorption and provided a different idea to the second-order equation called a pseudo-second-order rate expression. PSO was found to explain the sorption kinetics of the most of systems very well for the entire range of period. And it was found that it exhibits a better fit towards the sorption of heavy metals (Hui KS et al, 2005). Linearization of pseudo second-order expression proposed by Blanchard et al. (1984) with ideas similar to Ho expression was also found to explain the sorption kinetics better than PFO model. In the present study an extensive analysis of pseudo second-order expression was made using the experimental kinetic data of U(VI) onto different soil types. The objectives of this paper were to demonstrate the differences in estimated PSO parameters arising from the application of linear and non-linear regression methods to kinetic adsorption data and to assess the accuracy of predictions from different regression methods. This will help to fix the model suitable to study kinetics of the sorption.

2. Material and methods

2.1 Selection of soil and characterization

Soil of different origin, chemical compositions and texture were used as adsorbent such as Soil A (Metamorphic Rock), Soil B (Sedimentary Rock), Soil C (Igneous Basalt). Soil particle size distribution was carried out using CILAS Particle Size Analyzer 1109 (Range:

40nm-2500µm) in liquid mode and mineralogical characterization was carried out using GNR, APD 2000 PRO X-ray diffract meter (Cu-Kα1 X-rays:1.54 A0) over the range of 5– 50, 2-theta for processed soil samples. The natural organic content (NOM) was estimated using CHNO-S Analyzer (Flash EA-112, Thermo-Fischer), Fe and Mn content in soil was estimated using AAS (GBC, Avanta). Physicochemical properties with mineralogical compositions of all the soils are presented in the Table 1.

2.2 Chemical regents and experimental setup

All the chemicals were analytical grade and used without any further purification. Working solution [U(VI)= 0.1, 0.5, 1.0, 10.0, 100.0mg/L] was prepared by appropriate dilution of the stock solutions (10000mg/L of Uranyl Nitrate, SEPEX Ltd.). Adsorption of U(VI) on the different soil was carried out in a batch system. 4 g of soil added to 40 ml of known concentration of U(VI) solution. The mixture was agitated at160 rpm in a rotary shaker (SK- 300,JIOTECH, Korea) at ambient temperature for 7days. For kinetics study the samples were withdrawn at pre-determined time (1 h, 2, 3, 6, 10, 24, 48…168 h) intervals until adsorption equilibrium was achieved. Then, the U(VI) solution was separated from the soil by centrifugation (Eppendorf Centrifuge 5430R, Germany) at 7000 rpm for 15min. The

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Pseudo second order kinetic model for the sorption of U (VI) onto soil: A comparison of linear and non-linear methods

supernatants were then filtered using Millipore filter paper (0.45µm) to ensure the solutions were free from particles before measuring the residual U(VI) concentration followed by analysis using differential pulse striping voltammetry (Metrohm, Switzerland). All experiments were carried out in duplicate, and the average values were taken to minimize random error.

Table 1: Physical and chemical properties of Natural Soil

Soil

Type

Sand

Silt

Clay

Max

Distribution

NOM

(%)

Fe

(%)

Mn

(mg/Kg)

CEC

(meq/100g)

Mineralogy

Data Generated

(µm)

Using XRD

                 

Ilite, Chlorite,

A 56.16

42.25

1.59

80

0.058

2.6

245

5.60

Quartz, K-

Feldspar,

Dolomite

                 

Ilite, Chlorite,

B 53.93

39.78

6.29

90

0.15

2.2

196

22.12

Kaoline, K-

Calcite,fedspar

                 

Quartz, Calcite,

5.55

C 77.13

17.31

4.0

2.04

4.9

502

62.04

Dolomite, Ca-

Mont.,Chlorite,

Amphibole

2.3 Kinetics models of sorption

For adsorption system following the pseudo second kinetics, the adsorbate was assumed to get adsorbed onto two surface sites. Thus the sorption kinetics following pseudo second-order kinetics can be represented as (1)

dt
dt

dq

=

k

2 (

q

e

q

t

)

2

(1)

Where k 2 is the rate constant of pseudo-second-order adsorption (g µg 1 h 1 ), qe is the amount of solute adsorbed at equilibrium (µg g 1 ) and qt is the amount of solute adsorbed at time t (µg g 1 ). Integrating Eq. (1) for boundary conditions t=0 to t=t and qt=0 to qt=qt gives:

q

t

=

q

2

e

k

2

t

1 +

k

2

q

e

t

(2)

And the initial rate of adsorption, h, is: h = k 2 q 2 e Eq. (2) can be linearized to at least four more different linear forms as shown in Table 1. Table 1 also shows the non-linear form of Eq. (2). Linear model-1, expression as shown in Table 1 was previously reported by Ho (Ho YS, 1995) for the sorption of divalent metal ions onto peat particles. The non-linear pseudo second-order kinetic model and its linearized expressions with effect of linearization were given in Table 1. The pseudo second-order kinetic constant and the theoretical qe by a type 1 pseudo second-order expression can be calculated from the plots of t/qt versus t as shown in Figure 1. Similarly the pseudo second-order kinetic constant K 2 and the theoretical qe can be obtained from the plot of 1/q versus 1/t, q versus qt/t and qt/t versus q for a linear model 2, linear model 3, and linear model 4 of pseudo second-order expressions respectively. The way to obtain the kinetic rate constant K 2 (g/µg h), initial sorption rate h (µg/g h) and the amount of U (VI) adsorbed at equilibrium qe (µg/g) are explained in Table 1.

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Pseudo second order kinetic model for the sorption of U (VI) onto soil: A comparison of linear and non-linear methods

onto soil: A comparison of linear and non-linear methods (a) (b) (c) (d) (e) Figure 1:

(a)

(b)

soil: A comparison of linear and non-linear methods (a) (b) (c) (d) (e) Figure 1: Fitting

(c)

(d)

comparison of linear and non-linear methods (a) (b) (c) (d) (e) Figure 1: Fitting of sorption

(e)

Figure 1: Fitting of sorption data to PSO (Linear Model -1) kinetics for all the three types of

soil at initial concentration of a) 0.100µg/L(1); b) 500µg/L c) 1000µg/L d) 10000 µg/L and e) 100000 µg/L.

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Pseudo second order kinetic model for the sorption of U (VI) onto soil: A comparison of linear and non-linear methods

3. Results and discussion

The calculated kinetic parameters using PSO kinetic model at different levels of U(VI) were presented in Table 2. Table 2 reveals that the K2, h and qe values obtained from the four linear forms of pseudo second-order expressions were different. In addition to above, it was also observed that the theoretically predicted qe values using all the linear models increases with increasing initial U(VI) concentration which is in line with actual adsorption process i.e., In the surface phenomenon, the amount of U(VI) adsorbed should increase with increasing initial concentrations. Very higher r2 values (>0.99 in most of the cases) for linear model-1 at all initial U(VI) concentration studied suggests pseudo second order kinetic model was the optimum kinetic expression to explain the sorption of U(VI) uptake by all soil types. Thus the theory behind the pseudo second-order model was getting valid for a linear model-1 pseudo second-order expression and the theory of pseudo second-order kinetics and the adsorption theory were found to getting violated for other linear models on the basis of r2. However the comparison of experimentally derived qe value with theoretically predicted values of qe using different linear models revealed that linear model-4 is also valid. This indicates, rejection of models based upon the good ness of fitting (high r2 value) is not the correct approach. Based upon these observations it can be assumed that, the linear methods instead of verifying the theory of adsorption kinetics just verify the hypothesis of linear regression. These different observations and predictions by linear method show the complexities in predicting the optimum sorption kinetics. Different outcomes from linear models for different initial U(VI) concentrations and different soil show the real complexities and problems in estimating the kinetic parameters by linearization technique.

This may arise due to the variation in the error structure which will vary upon linearizing the non-linear equation. The error distribution may vary the better or worse depending on the way of linearization. This is because of the problem with the linear method as they cause some of the assumptions behind linear regression getting violated. Transformation of non- linear pseudo second-order expression to linear model-1 leads to reversal of relative weights of data points because of 1/q in the dependent variable and‘t’ in both dependent and independent variables, leading to spurious correlation. Similarly linearization to model-2 leads to reversal of relative weights of data points because of 1/q in dependent variable and independent variable (1/t) leads to distortion of error distribution. q in both dependent and independent variables, leading to spurious correlation in linear model-3 and the presence of q in the independent variable (q/t) introduces experimental error, violating a basic assumption in the method of least squares as well as 1/t in independent variable, leading to distortion of error distribution. In case of linear model-4, q in both dependent and independent variables, leading to spurious correlation and the presence of q in the independent variable introduces experimental error, violating a basic assumption in the method of least squares. In a nutshell various outcomes for the linearized models are due to the different axial settings that would alter the result of linear regression and influence the determination process (Ho YS et al, 2004). The linear method does not check whether the kinetic trend is linear or not, instead it assumes the experimental data or the transformed experimental data are linear.

For non-linear method, a trial and error procedure, which is applicable to computer operation, was developed and used to determine the kinetic parameters by minimizing the respective the coefficient of determination between experimental data and predicted values using OriginPro 8. Figure 2 shows experimental data and the predicted pseudo second-order kinetics using non-linear method and Table 4 presents the theoretically derived kinetic parameters with

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Pseudo second order kinetic model for the sorption of U (VI) onto soil: A comparison of linear and non-linear methods

experimental equilibrium adsorption capacity of soil for U(VI). Study of good ness of fit using r2, reduced χ2 and SSE value presented in Table 5 nonlinear model well explained the kinetics of U(VI) sorption.

3.1 Comparison of linear and non-linear regression analysis

To compare model fits between the different linearization and the nonlinear pseudo-second order kinetic model equation, the best-fit lines for each linearization were transformed back to sorbed concentrations (qe) and error analysis were using for comparison goodness-of-fit measure using reduced χ2, SSE and regression coefficient r2. The statistical parameters are presented in Table- 5. From the statistical analysis we can conclude, that the linearized models -1 is more suitable than the nonlinear model based upon the reduced χ2, SSE values for all the soil types.

And the Linear model 4 is more suitable for Soil B and gives us very similar fits to the non- linear model in case of Soil C and A. Linear model 2 and 3 are not comparable with nonlinear model. This fact can be described in the following way: If we want to use the linear forms of the kinetic equations of the pseudo second order the data from the measurement must be transformed. The transformation probably changed the conditions in a positive way, and that caused that the linear model-1 give very similar or better fits than the non-linear models in all the cases and other linear model- 2, 3 and 4 in some specific cases.

Table 2: Pseudo second-order kinetics and their linear forms

   

Non-Linear

   

Parameters S: Slope & I: Intercept

Type

 

Form

 

Linear Form

   

Plot

 
   

t

1

1

 

qe = 1/S

Linear

Model-1

 

=

 

+

t

 

t

 

q

t

k q

2

e

2

q

e

q

vs t

 

k 2 = S 2 /I

   

t

H = 1/I

   

2

 

  1 t

+

1

q

   

qe = 1/I

Linear

Model-2

q

t

=

q

e

1 +

kt

q

e

t

1 q t
1
q
t

=

1 2
1
2

k q

2

e

e

1 q t
1
q
t

vs

1

t

k 2 =I 2 /S

h =1/S

       

qe = I

Linear

Model-3

 

q

t

=

q

e

1 2
1
2

k q

e

t

q

 

q

t

vs

q t t
q
t
t

k 2 = -1/(I×S)

h= -I/S

         

qe = -I/S

Linear

 
q t t
q
t
t

=

k q

2

2

 

k q q

2

e

t

 
q t t
q
t
t
 

2 =S 2 /I h = I

Model-4

e

vs

q

t

k

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Pseudo second order kinetic model for the sorption of U (VI) onto soil: A comparison of linear and non-linear methods

Table 3: Pseudo second-order rate constants by linear method for the sorption of U(VI) on to soil A, B and C (Co: mg/L; qe, µg/g; h: µg/g h; K 2 : g/µg h.)

   

Experimental

 

Linear Model: 1 (Theoretically derived)

   

Linear Model: 2 (Theoretically derived)

 

C0

Soil

q

e

q

e

K

2

h

R

2

q

e

K

2

h

R

2

0.1

 

0.86

0.86

1.42E+00

1.05

1.000

0.846

3.67E+00

2.62

0.93

0.5

4.48

4.54

5.38E-01

11.09

1.000

4.471

6.56E-01

13.11

0.93

1.0

A

9.20

10.00

1.06E-01

10.60

1.000

8.916

8.22E-01

65.32

0.56

10.0

77.75

83.30

3.27E-03

22.69

0.998

70.472

1.76E-02

87.48

0.77

100.0

466.50

476.20

7.23E-04

163.95

0.999

480.769

8.27E-04

191.21

0.96

0.1

 

0.96

0.98

7.28E-01

0.70

1.000

0.917

2.27E+00

1.91

0.74

0.5

4.56

4.76

1.10E+00

24.94

1.000

4.555

1.35E+00

27.99

0.91

1.0

B 8.64

8.70

2.70E-01

20.42

1.000

8.581

6.63E-01

48.83

0.95

10.0

67.36

71.43

5.44E-03

27.76

0.999

63.052

2.43E-02

96.62

0.82

100.0

399.54

500.00

6.67E-05

16.68

0.866

483.092

1.07E-04

24.95

0.84

0.1

 

0.94

0.94

1.25E+00

1.11

1.000

0.922

2.90E+00

2.47

0.77

0.5

4.84

4.85

8.37E-01

19.72

1.000

4.827

1.11E+00

25.95

0.96

1.0

C 9.76

9.80

2.77E-01

26.60

1.000

9.652

8.11E-01

75.53

0.75

10.0

90.00

90.90

2.02E-02

166.91

1.000

88.968

4.36E-02

344.83

0.94

100.0

797.46

1000.00

5.00E-05

50.00

0.923

478.469

1.14E-03

260.42

0.48

Continued…

Experimental

   

Linear Model: 3 (Theoretically derived)

   

Linear Model: 4 (Theoretically derived)

 

C0

Soil

q

e

q

e

K

2

h

R

2

q

e

K

2

h

R

2

0.1

 

0.86

0.84

3.89E+00

2.77

0.84

0.85

3.53E+00

2.54

0.90

0.5

4.48

4.47

6.53E-01

13.06

0.66

4.49

6.01E-01

12.12

0.92

1.0

A 9.20

8.93

8.00E-01

63.77

0.54

9.07

4.51E-01

37.07

0.54

10.0

77.75

72.10

1.54E-02

79.98

0.92

75.31

1.01E-02

57.56

0.66

100.0

466.50

461.5

1.08E-03

229.57

0.90

475.07

8.88E-04

200.35

0.84

0.1

 

0.96

0.95

5.83E+00

5.32

0.33

0.95

1.54E+00

1.38

0.71

0.5

4.56

4.97

1.28E+01

316.65

0.75

4.57

1.23E+00

25.69

0.90

1.0

B 8.64

9.96

4.47E+00

443.16

0.94

8.60

6.21E-01

45.93

0.94

10.0

67.36

99.62

1.14E+00

11346.5

0.90

65.31

1.69E-02

72.12

0.75

100.0

399.54

957.2

1.72E-04

157.84

0.71

457.42

1.31E-04

27.38

0.33

0.1

 

0.94

0.91

2.78E-01

3.01

0.30

4.84

1.05E+00

24.59

0.62

0.5

4.84

4.83

9.10E-01

25.62

0.92

0.94

2.30E+00

2.01

0.95

1.0

C 9.76

9.66

1.25E+00

74.69

0.75

9.71

6.10E-01

57.55

0.75

10.0

90.00

89.05

2.33E+01

340.80

0.96

89.30

3.98E-02

317.74

0.92

100.0

797.46

615.0

1.74E+03

217.27

0.62

614.77

5.74E-04

216.84

0.30

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Pseudo second order kinetic model for the sorption of U (VI) onto soil: A comparison of linear and non-linear methods

onto soil: A comparison of linear and non-linear methods (e) Figure 2: Fitting of sorption data

(e)

Figure 2: Fitting of sorption data to PSO (nonlinear) kinetics for all the three types of soil at initial concentration of a) 100µg/L(1); b) 500µg/L c) 1000µg/L d) 10000 µg/L and e) 100000 µg/L

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Pseudo second order kinetic model for the sorption of U (VI) onto soil: A comparison of linear and non-linear methods

Table 4: Comparison of theoretically derived kinetic parameters using non-linear model with experimental equilibrium adsorption capacity of soil for U(VI): (Co: mg/L; qe, µg/g; h: µg/g h; K 2 : g/µg h.)

 

Soil

Experimental

 

Non-Linear Model (Theoretically derived)

 

C0

 

Qe

Qe

K2

h

R

2

0.1

 

0.86

0.84

4.02E+00

2.84

0.90

0.5

4.48

4.48

6.25E-01

12.55

0.92

1.0

A

9.20

8.94

7.46E-01

59.60

0.54

10.0

77.75

73.70

1.14E-02

61.93

0.67

100.0

466.50

462.78

1.09E-03

232.55

0.86

0.1

 

0.96

1.11

2.29E+00

2.82

0.71

0.5

4.56

4.56

1.99E-01

4.15

0.91

1.0

B

8.64

8.58

6.51E-01

47.93

0.94

10.0

67.36

64.58

1.83E-02

76.43

0.75

100.0

399.54

529.97

4.76E-05

13.38

0.33

0.1

 

0.98

1.08

3.40E+02

397.06

0.79

0.5

4.98

4.97

1.27E+01

314.56

0.62

1.0

C

9.97

9.96

6.74E-02

6.68

0.89

10.0

99.71

99.62

1.14E+00

11294.78

0.73

100.0

957.06

1042.49

1.52E-04

165.47

0.39

Table 5: Statistic parameters for the nonlinear and linearized pseudo-second order kinetic equations for three soil types.

   

Non

       

Soil

Parameters

linear

Linear-1

Linear-2

Linear-3

Linear-4

 

Reduced χ 2

3.036

3.861

23.632

6.041

3.745

Soil -A

SSE

9.107

11.584

70.895

18.124

11.235

R

2

1.000

0.999

0.999

0.999

0.999

 

Reduced χ 2

147.248

38.360

81.730

865.457

33.516

Soil -B

SSE

441.743

115.081

245.189

2596.370

100.549

R

2

0.997

0.999

0.998

0.995

0.999

 

Reduced χ 2

114.496

113.739

289.033

91.156

101.41

Soil -C

SSE

343.487

341.218

867.099

273.468

304.22

R

2

0.999

0.999

0.993

0.999

0.999

4. Conclusion

The sorption of U(VI) on to different soil types was found to be well represented by the pseudo second-order kinetic model. The present study confirms that, kinetics of U(VI) uptake by different soil types best expressed by linear model-1. Other linear models 2, 3 and 4 were comparable to nonlinear model and actual q e value in specific cases. This clearly envisages that data transformation can positively or negatively affect the estimate of the regressive model. Therefore, the primary drawback to linearization is not the inability to provide similar parameter estimates as the nonlinear equation but rather the inability to provide poor (or good) model fits when the data don’t (or do) conform to the kinetic model.

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Pseudo second order kinetic model for the sorption of U (VI) onto soil: A comparison of linear and non-linear methods

5. References

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