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 nonlinear methods
Sabyasachi Rout, Ajay Kumar, Pazhayath Mana Ravi, Raj Mangal Tripathi Health Physics Division, Bhabha Atomic Research Centre, Mumbai, India400085 srout.barc@gmail.com
doi:10.6088/ijes.6017
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 secondorder kinetics by linear and a non linear method. The four different types of Ho pseudo secondorder expression have been discussed. A comparison of linear leastsquares method and a trial and error nonlinear method of estimating the pseudo secondorder rate kinetic parameters were examined. The sorption process was found to follow pseudo secondorder kinetic model. Present investigation showed that it is appropriate to use a linear model1 pseudo secondorder 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 model1 changed the conditions in a positive way leads to minimization of error structure and that caused that the linear model1 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; filmsolid model (McKay G et al, 1991) the filmpore 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 filmdiffusion (Boyd GE et al, 1947) and Weber's intra particlediffusion (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 nonlinear methods
of both the intraparticlediffusion and the filmdiffusion models often suffers from uncertainties due to their multilinear nature (Ho YS et al, 1998). At the present time pseudo kinetics models such as; Pseudo first order kinetics (PFO) and pseudo secondorder (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 firstorder kinetics, where the probable adsorbate interactions were assumed to be negligible. It was also observed that though the Lagergren pseudo firstorder 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 secondorder equation called a pseudosecondorder 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 secondorder 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 secondorder 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 nonlinear 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:
40nm2500µm) in liquid mode and mineralogical characterization was carried out using GNR, APD 2000 PRO Xray diffract meter (CuKα1 Xrays:1.54 A0) over the range of 5– 50◦, 2theta for processed soil samples. The natural organic content (NOM) was estimated using CHNOS Analyzer (Flash EA112, ThermoFischer), 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 predetermined 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 nonlinear 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 secondorder kinetics can be represented as (1)
dq
=
k
2 (
q
e
−
q
t
)
2
(1)
Where k _{2} is the rate constant of pseudosecondorder 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 nonlinear form of Eq. (2). Linear model1, 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 nonlinear pseudo secondorder kinetic model and its linearized expressions with effect of linearization were given in Table 1. The pseudo secondorder kinetic constant and the theoretical qe by a type 1 pseudo secondorder expression can be calculated from the plots of t/qt versus t as shown in Figure 1. Similarly the pseudo secondorder 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 secondorder 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 nonlinear methods
(a)
(b)
(c)
(d)
(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 nonlinear 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 secondorder 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 model1 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 secondorder model was getting valid for a linear model1 pseudo secondorder expression and the theory of pseudo secondorder 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 model4 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 nonlinear 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 secondorder expression to linear model1 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 model2 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 model3 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 model4, 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 nonlinear 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 secondorder kinetics using nonlinear 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 nonlinear 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 nonlinear regression analysis
To compare model fits between the different linearization and the nonlinear pseudosecond order kinetic model equation, the bestfit lines for each linearization were transformed back to sorbed concentrations (qe) and error analysis were using for comparison goodnessoffit 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 model1 give very similar or better fits than the nonlinear models in all the cases and other linear model 2, 3 and 4 in some specific cases.
Table 2: Pseudo secondorder kinetics and their linear forms
NonLinear 
Parameters S: Slope & I: Intercept 

Type 
Form 
Linear Form 
Plot 

t 
1 
1 
qe = 1/S 

Linear Model1 
= 
+ 
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 Model2 
q 
t 
^{=} q e 1 + 
kt q e 
t 
1
q
t

=
1
2
k q 2 e 
e 
1
q
t

vs 
1 t 
k _{2} =I ^{2} /S h =1/S 

qe = I 

Linear Model3 
q 
t 
= 
q e 
−
1
2
k q e t q 
q 
t 
vs 
q
t
t

k _{2} = 1/(I×S) h= I/S 

qe = I/S 

Linear 
q
t
t

= k q 2 2 
k q q 2 e t 
q
t
t

_{2} =S ^{2} /I h = I 

Model4 
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 nonlinear methods
Table 3: Pseudo secondorder 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 
5.38E01 
11.09 
1.000 
4.471 
6.56E01 
13.11 
0.93 

1.0 
A 
9.20 
10.00 
1.06E01 
10.60 
1.000 
8.916 
8.22E01 
65.32 
0.56 

10.0 
77.75 
83.30 
3.27E03 
22.69 
0.998 
70.472 
1.76E02 
87.48 
0.77 

100.0 
466.50 
476.20 
7.23E04 
163.95 
0.999 
480.769 
8.27E04 
191.21 
0.96 

0.1 
0.96 
0.98 
7.28E01 
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 
2.70E01 
20.42 
1.000 
8.581 
6.63E01 
48.83 
0.95 

10.0 
67.36 
71.43 
5.44E03 
27.76 
0.999 
63.052 
2.43E02 
96.62 
0.82 

100.0 
399.54 
500.00 
6.67E05 
16.68 
0.866 
483.092 
1.07E04 
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 
8.37E01 
19.72 
1.000 
4.827 
1.11E+00 
25.95 
0.96 

1.0 
C 9.76 
9.80 
2.77E01 
26.60 
1.000 
9.652 
8.11E01 
75.53 
0.75 

10.0 
90.00 
90.90 
2.02E02 
166.91 
1.000 
88.968 
4.36E02 
344.83 
0.94 

100.0 
797.46 
1000.00 
5.00E05 
50.00 
0.923 
478.469 
1.14E03 
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 
6.53E01 
13.06 
0.66 
4.49 
6.01E01 
12.12 
0.92 

1.0 
A 9.20 
8.93 
8.00E01 
63.77 
0.54 
9.07 
4.51E01 
37.07 
0.54 

10.0 
77.75 
72.10 
1.54E02 
79.98 
0.92 
75.31 
1.01E02 
57.56 
0.66 

100.0 
466.50 
461.5 
1.08E03 
229.57 
0.90 
475.07 
8.88E04 
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 
6.21E01 
45.93 
0.94 

10.0 
67.36 
99.62 
1.14E+00 
11346.5 
0.90 
65.31 
1.69E02 
72.12 
0.75 

100.0 
399.54 
957.2 
1.72E04 
157.84 
0.71 
457.42 
1.31E04 
27.38 
0.33 

0.1 
0.94 
0.91 
2.78E01 
3.01 
0.30 
4.84 
1.05E+00 
24.59 
0.62 

0.5 
4.84 
4.83 
9.10E01 
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 
6.10E01 
57.55 
0.75 

10.0 
90.00 
89.05 
2.33E+01 
340.80 
0.96 
89.30 
3.98E02 
317.74 
0.92 

100.0 
797.46 
615.0 
1.74E+03 
217.27 
0.62 
614.77 
5.74E04 
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 nonlinear methods
(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 nonlinear methods
Table 4: Comparison of theoretically derived kinetic parameters using nonlinear 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 
NonLinear 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 
6.25E01 
12.55 
0.92 

1.0 
A 
9.20 
8.94 
7.46E01 
59.60 
0.54 

10.0 
77.75 
73.70 
1.14E02 
61.93 
0.67 

100.0 
466.50 
462.78 
1.09E03 
232.55 
0.86 

0.1 
0.96 
1.11 
2.29E+00 
2.82 
0.71 

0.5 
4.56 
4.56 
1.99E01 
4.15 
0.91 

1.0 
B 
8.64 
8.58 
6.51E01 
47.93 
0.94 

10.0 
67.36 
64.58 
1.83E02 
76.43 
0.75 

100.0 
399.54 
529.97 
4.76E05 
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 
6.74E02 
6.68 
0.89 

10.0 
99.71 
99.62 
1.14E+00 
11294.78 
0.73 

100.0 
957.06 
1042.49 
1.52E04 
165.47 
0.39 
Table 5: Statistic parameters for the nonlinear and linearized pseudosecond order kinetic equations for three soil types.
Non 

Soil 
Parameters 
linear 
Linear1 
Linear2 
Linear3 
Linear4 

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 secondorder kinetic model. The present study confirms that, kinetics of U(VI) uptake by different soil types best expressed by linear model1. 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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