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Energy Procedia 90 (2016) 316 – 325

5th International Conference on Advances in Energy Research, ICAER 2015, 15-17 December
2015, Mumbai, India

Comparative Studies on CO2 Adsorption Kinetics by Solid

Adsorbents
Vinod Kumar Singha, E. Anil Kumara,*
a
Discipline of Mechanical Engineering, Indian Institute of Technology Indore, Indore-453552, India

Abstract

Adsorption kinetics of carbon dioxide (CO2) on activated carbon (Norit RB3 type steam activated rod) and zeolite 5A
(Si/Al = 1.33) are compared at various temperatures (298, 308, 318 and 338 K) and supply pressures (1, 5, 10 and 20 bar).
Sievert’s type experimental setup is used for adsorption kinetics measurement. The experimental data is subsequently modelled
using pseudo first and second order kinetics models, which revealed that the pseudo second order kinetics model well fitted the
CO2 adsorption kinetics data than pseudo first order kinetics model. The rate constants and activation energies of CO2 adsorption
on activated carbon and zeolite 5A are estimated. It is found that at 1 bar supply pressure, the rate of CO2 adsorption on zeolite
5A is more than that of the activated carbon, while at higher pressure, the rate of CO2 adsorption on the activated carbon is
greater than the zeolite 5A due to large surface area and pore volume. Activation energies are calculated at different pressures by
fitting the Arrhenius equation to the adsorption kinetics data. It is observed that the activation energies of activated carbon are
slightly more than that of the zeolite 5A.
© 2016 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND license
© 2016 The Authors. Published by Elsevier Ltd.
(http://creativecommons.org/licenses/by-nc-nd/4.0/).
Peer-reviewunder
Peer-review under responsibility
responsibility of organizing
of the the organizing committee
committee of ICAER
of ICAER 2015 2015.

Keywords: Activation energy; Activated carbon; Adsorption kinetics; Carbon dioxide; Zeolite 5A

* Corresponding author. Tel.: +91-7879779188; fax: +91-7312-438-710.

E-mail address: anil@iiti.ac.in

1876-6102 © 2016 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND license
(http://creativecommons.org/licenses/by-nc-nd/4.0/).
Peer-review under responsibility of the organizing committee of ICAER 2015
doi:10.1016/j.egypro.2016.11.199
 Vinod Kumar Singh and E. Anil Kumar / Energy Procedia 90 (2016) 316 – 325 317

Nomenclature

A Arrhenius factor
Ea Activation energy (J/mol)

1 Pseudo-first order rate constant (1/min)

2 Pseudo-second order rate constant (g/mg min)

m 1' Amount of CO2 available in supply volume before adsorption (g)
m 2' Amount of CO2 available in supply volume after adsorption at any time (g)
mad,t Amount of CO2 adsorbed at any time (g of CO2/g)
Ps Supply pressure (N/m2)
qe Equilibrium adsorption capacity (g of CO2/g)
qt Adsorption capacity at any time (g of CO2/g)
R Universal gas constant (8.314 J/mol K)
RCO2 Characteristic gas constant (J/mol K)
T Absolute temperature (K)
t Time (sec)
V Volume (m3)
Z Compressibility factor

Subscripts

ad Adsorption
i Initial

1. Introduction

At present, the world is facing two major problems in the form of global warming and climate change.
Carbon capture and sequestration is suggested as one of the options to reduce the greenhouse gas emissions. Physical
adsorption on porous solid adsorbents is widely used for different applications like water treatment, adsorption based
cooling system, gas storage and purification and separation of flue gases [1]. Published data [2-6] on CO2 adsorption
isotherms of various solid adsorbents at different temperatures reveals that the amount of CO2 adsorbed decreases
significantly with increase in adsorption temperature owing to low binding forces between the adsorbate-adsorbent
interactions. Shen et al. [7] measured CO2 adsorption isotherms and kinetics on pitch-based activated carbon beads
at different temperatures (303 to 423 K) with a pressure range of 0-1 bar. They have suggested that the designing of
any gas storage system requires the knowledge of adsorption isotherms and kinetics data for increasing the
adsorption capacity. Balsamo et al. [8] reported that the adsorption rate increases with increasing CO2 gas pressure,
but with increasing temperature the adsorption rate decreases. Zhang et al. [9] measured the adsorption isotherms
and kinetics of CO2 on activated carbon and zeolite 13X at different temperatures (298, 308, 318 and 328 K) and
pressures up to 30 bar. They have observed that the adsorption rate of CO2 on zeolite 13X is more at lower pressure
than activated carbon whereas at high pressure the adsorption capacity is higher in activated carbon than that of
zeolite 13X.

Most of the researchers studied adsorption capacity of solid adsorbents by measuring adsorption isotherms
and a few researchers studied the CO2 adsorption kinetics on solid adsorbent. Studying adsorption kinetics is useful
for better understanding the phenomenons involved during adsorbent-adsorbate reaction and also to estimate the
time required to complete the adsorption process. Adsorption process time is one of the criteria to select the solid
adsorbents used in gas storage and adsorption based cooling system. The motivation of the present work is to
compare the adsorption kinetics of CO2 on activated carbon and zeolite 5A at different temperatures (298, 308, 318
and 338 K) and supply pressures (1, 5, 10 and 20 bar). The rate constants and activation energies of CO2 adsorption
process on activated carbon and zeolite 5A at different supply pressures and temperatures are also estimated.
318 Vinod Kumar Singh and E. Anil Kumar / Energy Procedia 90 (2016) 316 – 325

2. Experimental Measurements

CO2 adsorption kinetics is measured at supply pressures of 1, 5, 10 and 20 bar and at different temperatures (298,
308, 318 and 338 K). The schematic of experimental setup for adsorption kinetics measurement is illustrated in Fig.
1. The experimental set up is divided into four volumes (V1, V2, V3 and V4). All the volumes are calculated at the
time of installation using high pure argon gas (99.999%). The adsorption cell is made of stainless steel (SS-316) with
a functioning length of 100 mm, inner diameter and wall thickness of 16 and 2 mm respectively is used for
adsorption kinetics measurements. Before starting of adsorption kinetics measurements, activation of solid
adsorbents is required for the removal of unwanted gaseous substances present in the surface of adsorbent. After
activation, the adsorbent was degassed at 10-3 mbar pressure using a vacuum pump at 373 K for 4 hours then cooled
to the required temperature and maintained at that temperature throughout the adsorption experiment.

At the beginning of adsorption kinetics measurement, valves v3 and v6 are closed and CO2 is supplied to the
supply volume V2 and V3 at a fixed pressure through opening a valve v1. After attaining equilibrium the pressure and
temperature of CO2 in the supply volume is recorded and valves v1 and v4 are closed. Then valve v6 is opened and
CO2 is allowed to pass into the adsorption cell. CO2 is supplied to the adsorbent from a known volume (supply
volume). The amount of CO2 adsorbed with time is calculated by mass balance of CO2 in the supply volume. The
amount of CO2 adsorbed as a function of time is calculated using mass balance by measuring pressure reduction in
the supply volume. The pressure and temperature data is recorded continuously till the end of adsorption process.

The total amount of CO2 available in the supply volume (V2 and V3) at the beginning of the experiment is calculated
as follows:

⎛3 pi Vi ⎞
m1 ' = ⎜ ∑ ⎟ (1)
⎜ i = 2 Z ( pi ,Ti ) R CO Ti ⎟
⎝ 2 ⎠

Total amount of CO2 available in the volumes V2-V4 at any time t is calculated as follows:

⎛ 4 pi,t Vi ⎞
m2 ' = ⎜ ∑ ⎟ (2)
⎜ i = 2 Z ( pi,t , Ti,t ) R CO Ti,t ⎟
⎝ 2 ⎠

At any time (t), the amount of CO2 adsorbed in the adsorbent is estimated by the following equation.

mad,t = m1 '− m2 ' (3)

3. Data Reduction of Adsorption Kinetics Modelling

The experimental CO2 adsorption kinetics data is examined by fitting it to pseudo first order and pseudo
second order kinetics models which are given in Table 1.

3.1 Pseudo-first Order Kinetics Model

Pseudo-first order kinetics model assumes that the rate of adsorption is proportional to the number of
available free active sites on the adsorbent surface. The pseudo-first order kinetics model basically used for liquid-
solid phase is given in Table 1 [10]. The value of k1 and qe are obtained from the slope and intercept of the plots,
which are given in Table 1.
 Vinod Kumar Singh and E. Anil Kumar / Energy Procedia 90 (2016) 316 – 325 319

V1 = 20.80 ml = Volume between valve v1, v2, v3 and v4

V2 = 312.90 ml = Volume between valve C1 and valve v5
V3 = 6.95 ml = Volume between valve v4, v5 and v6
V4 = 75.83 ml = Free volume in reactor up to valve v6
Fig. 1 Schematic of experimental setup for CO2 adsorption kinetics measurement

3.2 Pseudo-second Order Kinetics Model

An assumption of pseudo-second order kinetics model is the rate of adsorption is proportional to the square
of the number of free available sites on the adsorbent surface. Many researchers [11-13] have used this model to fit
the experimental kinetics data of CO2 adsorption. The value of qe and k2 are estimated from the slope and intercepts
of the plots, which are given in Table 1.

Table 1 Adsorption kinetics models

Nonlinear
Kinetics model Linear equation Plot Slope and Intercept Ref.
equation
κ1
dq t ⎛ κ ⎞ Slope =
Pseudo-first order = κ1 ( q e − q t ) log ( q e − q t ) = log ( q e ) − ⎜ 1 ⎟ t log ( q e − q t ) vs t 2.303 [10]
dt ⎝ 2.303 ⎠ Intercept = log ( q e )

1
Slope =
dq t 2 t 1 t t qe
Pseudo-second order = κ2 ( qe − q t ) = + vs t [13]
dt q t κ2q e 2 q e qt 1
Intercept =
κ2q e 2

3.3 Validity of Adsorption Kinetics Models

The experimental data of adsorption kinetics is fitted with the kinetics models to describe the adsorption
process. The validation criterion of these models is based on the value of coefficient of correlation (R2) and the
average relative error (ARE), which is given by Eq. (4) defined as [14]:
100 n q e exp − q e mod
ARE(%) = ∑ (4)
N i=1 q e exp
where qe and q e are the amount of CO2 adsorbed obtained from experimental and kinetics model data
exp mod

respectively and N is the number of adsorption kinetics data points.

320 Vinod Kumar Singh and E. Anil Kumar / Energy Procedia 90 (2016) 316 – 325

4. Results and Discussion

Figs. 2(a-d) and 3(a-d) show the adsorption kinetics of CO2 on the activated carbon and zeolite 5A at
different temperatures (298, 308, 318 and 338 K) and supply pressures (1, 5, 10 and 20 bar). The amount of CO2
adsorbed on adsorbents increased with increase in CO2 supply pressure. It is observed that at the beginning, the
amount of CO2 adsorbed on the adsorbents is fast and it gradually decreases as the adsorption progresses till it
reaches equilibrium state. These figures demonstrate that the adsorption process reached equilibrium in about an
average time of 120 sec. It is found that in the initial stage, CO2 molecules come into direct contact of adsorbent
causing a stronger binding force. After all the pores get occupied by the adsorbate no more CO2 molecules are
adsorbed. Figs. 2(a) and 3(a) shows at supply pressure of 1 bar the amount of CO2 adsorbed on zeolite 5A is higher
than that of activated carbon which is due to availability of more active sites to adsorb more CO2 molecules on
zeolite 5A as compare to activated carbon. With the increase of supply pressures (5, 10 and 20 bar), Fig. 2(b-d) and
3(b-d) show that the amount of CO2 adsorbed on activated carbon increased significantly than that of zeolite 5A,
owing to the large surface area and pore volume. It is also observed that the amount of CO2 adsorbed on the
adsorbents decrease with increase in adsorption temperature due to decrease in adsorbent density during the
adsorbate-adsorbent interactions. The amount of CO2 adsorbed on the activated carbon and zeolite 5A are compared
with other available activated carbons and zeolites cited in the literature and summarized in Table 2 [9,15,16]. It
shows that the reported values of amount of CO2 adsorbed on activated carbon and zeolite 5A are quite similar to
that of measured values in this study. The maximum uncertainty in the estimation of amount of CO2 adsorbed in
kinetics measurements on activated carbon and zeolite 5A are 2.81 and 3.21 mg of CO2/g respectively.

Fig. 2(a-d) Adsorption kinetics curves of CO2 on activated carbon at 1, 5, 10 and 20 bar with different temperatures
 Vinod Kumar Singh and E. Anil Kumar / Energy Procedia 90 (2016) 316 – 325 321

Fig. 3(a-d) Adsorption kinetics curves of CO2 on zeolite 5A at 1, 5, 10 and 20 bar with different temperatures

Table 2 Comparison of amount of CO2 adsorbed and activation energy of different activated carbons and zeolites

Amount of CO2 adsorbed (mg/g) Activation

Pressure P
Adsorbents Temperature T (K) Energy (Ea)
(bar) Ref.
(kJ/mol)
298 308 318 338
1 102.95 91.44 89.85 74.93 23.74
Activated carbon 5 226.61 215.92 203.39 181.06 22.92 This
10 310.85 287.16 258.04 225.26 20.73 study
20 405.20 366.32 341.34 291.26 18.97
1 117.95 106.17 103.11 95.23 12.25
5 145.65 139.43 135.37 125.23 11.42 This
Zeolite 5A
10 158.32 146.46 142.85 132.65 9.27 study
20 160.69 152.62 148.12 142.03 7.23
AC-h 0.5 71.12 59.32 46.43 23.67 - [9]
AC-h 3.0 269.45 224.65 190.32 173.47 - [9]
AC-h 20.0 807.34 656.76 643.34 605.34 - [9]
Zeolite 13X 0.5 91.23 85.45 78.33 73.34 - [9]
Zeolite 13X 3.0 122.23 110.23 105.45 101.78 - [9]
Zeolite 13X 20.0 202.34 189.34 167.34 155.34 - [9]
Corncob-derived AC-h 0.01 (301 K) 116.74 25.50 [15]
Coconut shell - - 17.00 [16]
322 Vinod Kumar Singh and E. Anil Kumar / Energy Procedia 90 (2016) 316 – 325

The CO2 adsorption kinetics data at different supply pressures and temperatures are fitted with pseudo-first
order and pseudo-second order kinetics models. The kinetics parameters at different supply pressures and
temperatures of these models along with coefficient of correlation (R2) and average relative errors (ARE) are
estimated and summarized in Table 3(a) and Table 3(b) for activated carbon and zeolite 5A respectively. The
experimental and calculated amount of CO2 adsorbed showed large deviations in case of pseudo-first order kinetics
model. It is also observed that the pseudo-second order kinetics model well fitted with the adsorption kinetics data at
different pressures and temperatures, with high R2 values as shown in Table 3(a) and Table 3(b). Based on the R2
value and average relative error, the above two kinetics models are found to be suitable for fitting the present
adsorption kinetics data in the following order: pseudo-second order > pseudo-first order kinetics model.
Table 3(a) Pseudo first and second order kinetics model parameters of CO2 adsorption on activated carbon

Kinetics Parameters Activated carbon

Kinetics
Pressure Temperature (K)
Model Parameters
(bar) 298 308 318 338
ƙ1 (1/min) 1.10 1.06 0.91 0.82
(qe)exp (mg/g) 102.95 91.44 89.85 74.93
1 (qe)cal (mg/g) 108.76 94.68 91.27 84.42
R2 0.99 0.98 0.98 0.96
ARE (%) 2.34 3.23 2.75 2.81
ƙ1 (1/min) 1.03 1.01 0.83 0.71
(qe)exp (mg/g) 226.61 215.92 203.39 181.06
5
(qe)cal (mg/g) 193.94 187.66 179.07 133.38
R2 0.99 0.99 0.99 0.99
Pseudo first ARE (%) 2.53 2.75 3.12 3.45
order model ƙ1 (1/min) 1.26 1.22 1.16 1.96
(qe)exp (mg/g) 310.85 287.16 258.04 225.26
10
(qe)cal (mg/g) 265.67 248.24 230.43 204.87
R2 0.99 0.98 0.98 0.97
ARE (%) 3.56 3.25 3.12 2.67
ƙ1 (1/min) 1.03 1.06 1.05 0.98
(qe)exp (mg/g) 405.20 366.32 341.34 291.26
20
(qe)cal (mg/g) 351.69 325.74 292.26 258.21
R2 0.96 0.95 0.95 0.93
ARE (%) 2.12 2.58 2.78 3.12
ƙ2 (g/mg min) 0.04 0.06 0.08 0.13
(qe)exp (mg/g) 102.95 91.44 89.85 74.93
1
(qe)cal (mg/g) 135.14 112.36 105.26 91.74
R2 0.99 0.99 0.99 0.99
ARE (%) 1.23 1.45 1.12 1.35
ƙ2 (g/mg min) 0.03 0.04 0.06 0.08
(qe)exp (mg/g) 226.61 215.92 203.39 181.06
5
(qe)cal (mg/g) 227.27 217.39 204.08 151.52
R2 0.99 0.99 0.99 0.99
Pseudo second ARE (%) 1.12 1.24 1.45 1.21
order model ƙ2 (g/mg min) 0.02 0.03 0.03 0.05
(qe)exp (mg/g) 310.85 287.16 258.04 225.26
10
(qe)cal (mg/g) 322.58 294.12 263.16 232.56
R2 0.99 0.99 0.99 0.99
ARE (%) 1.13 1.01 1.24 1.45
ƙ2 (g/mg min) 0.01 0.02 0.02 0.03
(qe)exp (mg/g) 405.20 366.32 341.34 291.26
20
(qe)cal (mg/g) 416.67 370.37 344.83 294.12
R2 0.99 0.99 0.99 0.99
ARE (%) 1.34 1.02 1.35 1.41
 Vinod Kumar Singh and E. Anil Kumar / Energy Procedia 90 (2016) 316 – 325 323

Table 3(b) Pseudo first and second order kinetics model parameters of CO2 adsorption on zeolite 5A

Kinetics Parameters Zeolite 5A

Kinetics
Pressure Temperature (K)
Model Parameters
(bar) 298 308 318 338
ƙ1 (1/min) 0.93 0.97 0.91 0.87
(qe)exp (mg/g) 117.95 106.17 103.11 95.23
1 (qe)cal (mg/g) 91.95 81.70 78.17 74.82
R2 0.99 0.97 0.98 0.98
ARE (%) 2.45 2.56 2.89 2.87
ƙ1 (1/min) 0.89 0.87 0.88 0.92
(qe)exp (mg/g) 145.65 139.43 135.37 125.23
5
(qe)cal (mg/g) 119.32 113.82 111.36 105.88
R2 0.98 0.98 0.99 0.96
Pseudo first ARE (%) 2.12 2.45 3.56 3.98
order model ƙ1 (1/min) 0.75 0.92 0.99 0.89
(qe)exp (mg/g) 158.32 146.46 142.85 132.65
10
(qe)cal (mg/g) 130.37 125.14 125.00 117.00
R2 0.96 0.97 0.98 0.98
ARE (%) 2.45 2.49 2.54 2.98
ƙ1 (1/min) 0.75 0.76 0.63 0.67
(qe)exp (mg/g) 160.69 152.62 148.12 142.03
20
(qe)cal (mg/g) 138.11 134.43 130.64 126.27
R2 0.95 0.95 0.96 0.94
ARE (%) 2.98 2.89 3.12 3.15
ƙ2 (g/mg min) 0.03 0.03 0.04 0.05
(qe)exp (mg/g) 117.95 106.17 103.11 95.23
1
(qe)cal (mg/g) 121.95 109.89 106.38 98.04
R2 0.99 0.99 0.99 0.99
ARE (%) 1.21 1.75 1.23 1.12
ƙ2 (g/mg min) 0.02 0.03 0.03 0.04
(qe)exp (mg/g) 145.65 139.43 135.37 125.23
5
(qe)cal (mg/g) 149.25 142.88 138.89 128.21
R2 0.99 0.99 0.99 0.99
Pseudo second ARE (%) 1.32 1.34 1.45 1.53
order model ƙ2 (g/mg min) 0.02 0.02 0.02 0.03
(qe)exp (mg/g) 158.32 146.46 142.85 132.65
10
(qe)cal (mg/g) 166.67 135.14 147.06 151.52
R2 0.99 0.99 0.99 0.99
ARE (%) 1.35 1.56 1.12 1.34
ƙ2 (g/mg min) 0.02 0.02 0.02 0.02
(qe)exp (mg/g) 160.69 152.62 148.12 142.03
20
(qe)cal (mg/g) 166.67 156.25 153.85 147.06
R2 0.99 0.99 0.99 0.99
ARE (%) 1.01 1.87 1.61 1.21

The activation energies at different pressures are obtained from the slope (-Ea/R) of the plots of (ln ƙ2)
versus the inverse temperature (1/T) (Arrhenius-type plot) which is given by Eq. (5). The plots of (ln ƙ2) and (1/T)
are fitted with coefficient of correlation (R2) more than 0.95 and showing good linear relations. Fig. 4(a-b) shows
that the activation energy values decreased with increase in supply pressure, which indicates that the adsorbate-
adsorbent interaction is stronger at higher pressure due to increase in adsorbate density. It is found that at supply
pressure of 1 bar, the activation energy is more for both the adsorbents due to more energy requirement for starting
the adsorption process. It is also observed that the activation energies decreased with increase in adsorption
temperature due to heterogeneity of adsorption sites during the adsorbate-adsorbent interactions. In the
physisorption process, the value of activation energy is usually low due to weak Vander Waals forces between
adsorbate-adsorbent interactions. In the present investigation, it is found that the activation energies of activated
carbon and zeolite 5A are 23.74, 22.92, 20.73 and 18.97 kJ/mol and 12.25, 11.42, 9.27 and 7.23 kJ/mol at 1, 5, 10
and 20 bar pressures respectively. The activation energy values for the activated carbon and zeolite 5A are in the
range of that of physisorption processes. The activation energy values obtained in the present study are compared
with other activated carbons and zeolites as shown in Table 2. The maximum uncertainty in the estimation of the
activation energy of CO2 adsorption on activated carbon and zeolite 5A are ±1.55% and ±1.74% respectively.
324 Vinod Kumar Singh and E. Anil Kumar / Energy Procedia 90 (2016) 316 – 325

Ea
ln κ 2 = ln A − (5)
RT

Fig. 4(a-b) ln (ƙ2) versus (1/T) with different temperature and pressures on (a) activated carbon and (b) zeolite 5A

5. Conclusions

Adsorption kinetics of CO2 on activated carbon and zeolite 5A are compared at different temperatures (298,
308, 318 and 338 K) and supply pressures (1, 5, 10 and 20 bar). The amount of CO2 adsorbed on zeolite 5A at 1 bar
supply pressure is more as compared to activated carbon which is due to availability of more active sites on the
surface of adsorbent. At high pressures, the amount of CO2 adsorbed on activated carbon is higher than that of
zeolite 5A due to high surface area and pore volume. CO2 adsorption kinetics data on the adsorbents are described
using the pseudo first and second order kinetics models. It is found that the pseudo second order model is well suited
to the CO2 adsorption kinetics data than pseudo first order model. The rate constants for both the adsorbents
increased with increase in temperatures. Activation energies of CO2 adsorption on activated carbon and zeolite 5A
slightly decreased with increase in CO2 supply pressure.

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