Journal of Industrial and Engineering Chemistry 28 (2015) 241–246

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Journal of Industrial and Engineering Chemistry

journal homepage: www.elsevier.com/locate/jiec

Application of Langmuir and Freundlich isotherms to predict

adsorbate removal efficiency or required amount of adsorbent
Hyung-Keun Chung, Woon-Hoe Kim, Jeongwon Park, Jinwoo Cho, Tae-Young Jeong,
Pyung-Kyu Park *
Department of Environmental Engineering, Yonsei University, 1 Yonseidae-gil, Wonju 220-710, Gangwon-do, Republic of Korea

A R T I C L E I N F O A B S T R A C T

Article history: The aim of this study was to investigate how basic adsorption isotherms could be applied to predict
Received 20 January 2015 removal efficiency or required adsorbent mass under given sets of initial conditions. The intrinsic
Received in revised form 23 February 2015 parameters of the Langmuir and Freundlich adsorption isotherms were experimentally obtained and
Accepted 23 February 2015
subsequently utilized to predict removal efficiencies for other sets of initial solute concentrations,
Available online 28 February 2015
solution volumes, and adsorbent masses, or to estimate the adsorbent mass required to remove solute at
a desired removal efficiency. This was accomplished by combining the isotherms with mass balance of
Keywords:
solutes between liquid solution and solid adsorbent phases.
Activated carbon
Adsorption isotherm
ß 2015 The Korean Society of Industrial and Engineering Chemistry. Published by Elsevier B.V. All rights
Oyster shell reserved.
Prediction

Introduction appropriate adsorption model was selected, the adsorption

Adsorption technology has been widely utilized in water and
wastewater treatment processes because it is a fast, effective, and
relatively inexpensive method [1]. Organic and inorganic con-
stituents in the water phase are effectively removed by adsorption
technology [2–8]. Activated carbon such as granular and powdered
activated carbon (GAC and PAC) have been widely used as
adsorbent for water treatment [9–12], but because of considerable
operating costs associated with regeneration and/or repeated
injection, various alternative adsorbents have been studied [13–
15]. Oyster shell powder containing calcium carbonate is one such
alternative. Large amounts of waste oyster shells are continuously
generated in some countries, which offers a reliable source for
them to be used as a cheap adsorbent material [16,17]. It was
reported that the removal of orthophosphate by adsorption onto
oyster shell powder was comparable to that onto calcium
carbonate [18].
In most adsorption studies, adsorption models such as
Langmuir and Freundlich isotherms have been widely used to
evaluate adsorption phenomena [10,19]. Generally, experimental
data were fitted to adsorption isotherm models, and the best-fitted
model was used to characterize equilibrium adsorption. As the
* Corresponding author. Tel.:+82 33 760 2890.
E-mail address: pkpark@yonsei.ac.kr (P.-K. Park).
parameters of the model were obtained and used to describe
the adsorption characteristics. Langmuir-type adsorption is
considered to be a monolayer process. The maximum adsorption
capacity per unit adsorbent mass is determined along with the
Langmuir constant showing the solute affinity to the adsorbent.
Freundlich-type adsorption is considered to be a multi-layer
process in which the amount of adsorbed solute per unit adsorbent
mass increases gradually. Freundlich parameters were also used to
characterize the adsorption process.
It should be pointed out that, in the adsorption isotherms, the
amount of adsorbed solute per unit adsorbent mass (dependent
variable) is expressed as a function of the solute concentration at
equilibrium (independent variable), not a function of initial
concentration. This implies that the model equation would only
be utilized when the solute concentration at equilibrium is known.
However, in many practical adsorption studies and industrial
applications, it might be more desirable to predict the removal
efficiency for the given initial set of experimental conditions
(initial solute concentration, solution volume, and adsorbent
mass), or to estimate the adsorbent mass required to remove
the solute for a desired removal efficiency. Najm et al. [20] reported
the effect of initial di- and trichlorophenol concentration on
adsorption isotherm. Knappe et al. [21] developed a method to
predict PAC capacity for trace organic compounds from initial
solute concentration at a given adsorbent dose. Bolster [22]
predicted adsorbed solute concentration as a function of initial

http://dx.doi.org/10.1016/j.jiec.2015.02.021
1226-086X/ß 2015 The Korean Society of Industrial and Engineering Chemistry. Published by Elsevier B.V. All rights reserved.
242 H.-K. Chung et al. / Journal of Industrial and Engineering Chemistry 28 (2015) 241–246

solute concentration. However, few studies have sought to Substituting Eq. (4) into Eq. (1) gives the second order function
directly predict removal efficiencies of adsorption processes as in which Ce is a one argument variable as follows:
functions of both initial solute concentration and adsorbent  
K L  qmax  M
mass—information that could be conveniently applied to real K L  Ce2 þ 1 þ  K L  C0  Ce  C0 ¼ 0 (5)
V
adsorption processes.
The objective of this study was to demonstrate how basic
Note that the resulting equation shown above is a form of
adsorption isotherms combined with simple mass balance can be
quadratic equation if all variables other than Ce are treated as
applied to predict removal efficiency or required adsorbent mass
constants, and thus Ce can be explicitly and simply solved by using
under given sets of initial conditions. The intrinsic parameters of
the following quadratic formula [22,23]:
Langmuir and Freundlich adsorption isotherms were first obtained
by fitting experimental data for the adsorption of orthophosphate ð1 þ ðK L  qmax  M=V Þ  K L  C 0 Þþ
and methylene blue onto oyster shell powder and PAC, respec- qffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
ffi
tively. Even though only one isotherm for each adsorption ð1 þ ðK L  qmax  M=V Þ  K L  C 0 Þ2 þ 4K L  C 0
Ce ¼ (6)
experiment need be determined for the predictions, experimental 2K L
data for different sets of initial adsorption conditions were
obtained to be compared to the predicted values. Finally, contour The resulting Ce is a function of C0 and M for a specific V with
plots of predicted removal efficiencies were generated using both parameters KL and qmax. Therefore, once KL and qmax are obtained
initial solute concentration and adsorbent mass as independent from a set of adsorption experiments, equilibrium solute
variables. concentrations can be estimated for the given initial solute
concentration and the adsorbent mass in a fixed volume, which
Model development can differ from the conditions in the experimental set used for
determining KL and qmax. If the removal efficiency by adsorption for
Langmuir isotherm water treatment is set to R, it can be expressed as
C0  Ce
R¼ (7)
The Langmuir isotherm, which assumes monolayer adsorption C0
onto an adsorbent surface, can be expressed by the following
equation [10]: and thus R is also a function of C0 and M (R = R(C0, M)) for a specific
V.
  For the given initial solute concentration and target removal
K L  Ce
qe  qmax (1) efficiency, the model equation to predict the adsorbent concen-
1 þ K L  Ce tration can also be obtained. Substituting Eqs. (4) and (7) into
where Ce is the solute, or so-called adsorbate, concentration in the Eq. (1) and arranging for M gives:
solution at equilibrium (mg/L), qe the solute mass adsorbed per
V R V R
unit adsorbent mass at equilibrium (mg/g), KL the constant of the M¼ þ  C0 (8)
K L  qmax  ð1  RÞ qmax
Langmuir isotherm (L/mg), and qmax relates to the maximum
adsorption capacity (mg/g). The above equation may be reformu-
Note that the resulting Eq. (8) is an explicit equation in which M
lated in the form of the following linear equation:
is a function of C0 and R for a specific V with parameters KL and qmax
(M = M(C0, R)), and thus the required adsorbent mass can be simply
 
1 1 1 1 predicted from a set of an initial solute concentration and a desired
¼  þ (2)
qe K L  qmax C e qmax removal efficiency (Fig. 1).

In any adsorption experiments, Ce can be measured and qe can Freundlich isotherm

be calculated for a series of different conditions. Then 1/qe can be
plotted as a function of 1/Ce. Note that most of the adsorption The Freundlich isotherm, which was originally developed as an
experiments have utilized the above linear form of the equation to empirical model, may be written as follows [10,19]:
evaluate whether or not the adsorption process satisfies the
Langmuir isotherm. If the resulting plot shows appreciable qe ¼ K F  Ce
1=n
(9)
linearity, the adsorption process may be deemed to follow the
Langmuir adsorption isotherm. Consequently two parameters (KL where KF is the constant of the Freundlich isotherm (L1/n mg(11/n)/
and qmax) can be obtained by using the slope and the intercept to g), and 1/n is the Freundlich exponent. The linear form of the
characterize the adsorption process.
In this study, the isotherm equation was combined with a mass
balance, which has been generally used in modelling studies on
adsorption [10,19]. In a batch system at the given solution volume,
the following mass balance should be satisfied:

C 0 ¼ C e þ CeS (3)

where C0 is the initial concentration of solute in the solution, and CeS

is the concentration of solute adsorbed onto the adsorbent at
equilibrium. The qe in Eq. (1) can also be expressed in terms of
solution volume, V, and adsorbent mass, M, with C0 and Ce as
follows:

V  CeS V ðC 0  C e Þ Fig. 1. Simplified flowcharts for the application of adsorption isotherms combined
qe ¼ ¼ (4)
M M with mass balances to predict removal efficiency or required adsorbent mass.
 H.-K. Chung et al. / Journal of Industrial and Engineering Chemistry 28 (2015) 241–246 243

Freundlich isotherm can also be formulated as follows: analysis, and it was found that adsorption for 3 h was sufficient to
reach equilibrium. To test the validity of the developed model,
1
log qe ¼ log C e þ log K F (10) additional adsorption tests were carried out by changing the mass
n
of the oyster shell powder separately added to 0.050 L of 10, 30, 60
Similar to the Langmuir adsorption isotherm, the above linear and 90 mg/L orthophosphate solutions. The oyster shell powder in
form of the equation can be used to evaluate whether the each sample was filtered out using 0.45-mm syringe filters.
adsorption process satisfies the Freundlich isotherm and to A total of 0.20 g of PAC was added to 0.40 L of each 25 to
identify the constants. If the experimental results show appreci- 450 mg/L methylene blue solution. Again, to verify the validity,
able linearity according to the equation, the adsorption process additional adsorption tests were conducted under different initial
may be deemed to follow the Freundlich adsorption isotherm. conditions. The mixtures were well agitated at 25 8C for 24 h using
The Freundlich isotherm was reformulated with mass balance. a mechanical shaker. The PAC was filtered from each sample using
Substituting Eq. (4) into Eq. (9) gives a 0.45-mm syringe before measuring absorbance in order to
evaluate the equilibrium concentration of methylene blue.
K F  M 1=n
Ce þ C e  C 0 ¼ 0 (11)
V
Parameter determination and model calculation
in which Ce is the one argument variable. Even though Eq. (11) is
not an explicit one and should be solved by using the numerical The isotherms were fitted to experimental data for orthophos-
analysis method, Ce is a function of C0 and M for a specific V with phate with linearized Eqs. (2) and (10) to determine isotherm
parameters KF and 1/n. Therefore, with Eq. (7), R = R(C0, M) again. parameters. Those for methylene blue were fitted by non-linear
The mass of the adsorbent necessary for the desired removal regression using Eqs. (1) and (9) with a software program
efficiency can also be derived as follows: (Datafit1, Oakdale Engineering, USA). Eq. (11) was solved by
V R numerical analysis based on the Newton-Rahphson method [26]
ð11=nÞ
M¼ C (12) utilizing a spreadsheet program (Excel1 with visual basic
K F ð1  RÞ1=n 0
applications, Microsoft, USA). Menu-driven software using the
in which M = M(C0, R) for a fixed V (Fig. 1). visual basic userform of the program was exclusively created,
In summary, we have shown that mathematical expressions which allowed input of the pre-determined parameters and the set
were derived from both Langmuir and Freundlich adsorption
isotherms combined with the basic mass balance of the solute
concentration in the system. Once isotherm parameters are
determined from an isotherm consisting of a set of experimental
data, (i) the final solute concentration in the solution and the
removal efficiency, or (ii) required adsorbent mass in a fixed
volume for a desired removal efficiency can be estimated from an
initial set of conditions. Fig. 1 shows simplified flowcharts for
prediction under two different sets of initial conditions: left- and
right-side flowcharts correspond to the (i) and (ii) cases,
respectively.

Materials and methods

Materials and analytical methods

Oyster shell powder for the adsorption of orthophosphate

was prepared by thoroughly washing, drying, and grinding
oyster shells with a bench grinder [24]. Large particles were
removed by using a 50-mesh sieve. Orthophosphate solution
was prepared by dissolving Na2HPO4 (Sigma-Aldrich Korea,
Republic of Korea) in deionized water. The concentration of
orthophosphate was measured by using the ascorbic acid
method [25].
PAC (Duksan Pure Chemicals Co. Ltd., Republic of Korea) were
used as adsorbent. Methylene blue (Samchun Pure Chemicals Co.
Ltd., Republic of Korea) was used as solute to be adsorbed onto the
PAC, and its concentration was determined by measuring
absorbance at 664 nm with a spectrophotometer (8453 UV–vis,
Agilent Technologies, USA) after preparing a calibration curve
obtained with methylene blue solutions of known concentrations.

Adsorption experiments

Batch adsorption tests were conducted to determine param-

eters in isotherm equations. For orthophosphate adsorption, 1.0 g
of oyster shell powder was placed in 0.050 L of solution containing
orthophosphate ions in the range of 0 to 600 mg/L as P. The
mixtures were then shaken vigorously in a mechanical shaker at
25 8C. Adsorption was allowed to proceed up to 12 h with periodic
Fig. 2. Experimental data of orthophosphate adsorption onto oyster shell powder
fitted to linearized forms of (a) Langmuir and (b) Freundlich isotherms (1.0-g oyster
shell powder in 0.050 L) where Ce is orthophosphate concentration in the solution at
equilibrium (mg/L) and qe is orthophosphate mass adsorbed per unit oyster shell
powder mass at equilibrium (mg/g).
244 H.-K. Chung et al. / Journal of Industrial and Engineering Chemistry 28 (2015) 241–246

Table 1
Adsorption isotherm parameters determined from experimental data plotted in Figs. 2 and 4.

Orthophosphate onto oyster shell powder Methylene blue onto PAC

Langmuir isotherm KL (L/mg) 0.345 50.6

qmax (mg/g) 1.82 (R2 = 0.896) 298 (RSS1 = 5.71  104)
Freundlich isotherm KF (L1/n mg(11/n)/g) 0.500 214.50
1/n () 0.328 (R2 = 0.994) 0.0690 (RSS = 6.13  104)
1
Residual sum of squares.

of initial experimental conditions. Once the program was executed
after the desired variables were input, the outputs of typical
adsorption isotherm curve data and related plots were exported
into the spreadsheet. The removal efficiency and/or the required
adsorbent mass for a particular level of target efficiency were
calculated, yielding the results in the userform.
Results and discussion
Adsorption of orthophosphate onto oyster shell powder
Experimental data from tests of orthophosphate adsorption
onto oyster shell powder were fitted to the linear forms of
isotherms (Eqs. (2) and (9)), which are graphically represented in
Fig. 2. The results indicate that the Freundlich equation, rather than
the Langmuir equation, provided a good mathematical model to
describe the adsorption equilibrium. From the slope and intercept
of the plot of log qe against log Ce in Fig. 2(b), the KF and 1/n values
were obtained as listed in Table 1.
Once the isotherm parameters were determined, the removal
efficiencies for any set of experimental conditions could be
predicted. Calculations using Eqs. (6) and (11) were executed to
obtain the predicted removal efficiencies as a function of the mass
of oyster shell powder for the different initial concentrations of
orthophosphates in the range of 10 to 90 mg/L. At the same time,
the predicted data were compared to the experimental data. Fig. 3
shows that the predicted data were consistent with the
experimental data. This indicates that the required adsorbent
mass for any initial conditions could be pre-estimated prior to the
actual adsorption process. Although the plots of removal efficiency
as a function of the initial orthophosphate concentration for a fixed
adsorbent mass are not shown in this paper, the findings were
similar.
Adsorption of methylene blue onto PAC
Overall the adsorption capacity of oyster shell powder was very
low. Thus PAC adsorption of methylene blue, which is typically
used as a model adsorbate, was tested to further validate the
prediction method using an isotherm with mass balance. Fig. 4
shows the experimental data of qe vs. Ce and the best-fitting
isotherms (Eqs. (1) and (8)). Resulting parameters of the isotherms
are listed in Table 1. Based on the residual sum of squares (RSSs)
calculated by summing squared errors between data points and
predicted values, the data were slightly better fitted to the
Langmuir isotherm in this case. Considering qmax of the Langmuir
isotherm and KF of the Freundlich isotherm, PAC capacity for
adsorbing methylene blue was much greater than that of oyster
shell powder for adsorbing orthophosphate. The determined
parameters were used as constants in the isotherms with mass
balance to predict removal efficiency or required adsorbent mass
for conditions other than those of the experiments described
above.
The prediction was compared to experimental data for
validation (Table 2). When C0 = 313 mg/L for methylene blue
and M = 0.41 g for PAC in 0.4 L, removal efficiencies were predicted
to be 96.9% and 89.2% by the models based on the Langmuir and
Freundlich isotherms, respectively (Table 2(a)). The experimental-
ly determined value was 88.8%, and thus the prediction error was
9.12% and 0.45%. When C0 = 54.3 mg/L and M = 0.05 g in 0.5 L, the
errors were 3.78% and 6.24%, respectively. These findings
demonstrate that once constants in the isotherm equations are
determined with an experimental set under specific conditions, the
removal efficiency at different initial concentrations of solute and
adsorbent can be predicted without significant error by utilizing
the model.
In sequence, model verification was carried out in terms of
required adsorbent concentration (Table 2(b)). When C0 = 50 mg/L
and target R = 95%, the required M was predicted to be around
0.1 g/L for both models. For comparison, a batch adsorption test
was conducted with C0 = 50 mg/L for methylene blue and M = 0.1 g
for PAC in V = 0.5 L. The experimental removal efficiency was
95.6%. Therefore, calculations were repeated for C0 = 50 mg/L and
target R = 95.6%, and the results are presented in Table 2(b). The
error was 19.1% and 6.00% for each model, respectively. Similarly,
when the verification was tried once more for target R = 99.1% with

Table 2
Comparison of (a) removal efficiency, R, and (b) required adsorbent mass, M, predicted by Freundlich isotherm with mass balance to experimental data points obtained from
adsorption of methylene blue onto PAC (a) R prediction.

Initial conditions Experimental R (%) Predicted R (%)

C0 (mg/L) M (g) Langmuir isotherm1 Error (%) Freundlich Error (%)

isotherm2

313 0.41 (in 0.4 L) 88.8 96.9 9.12 89.2 0.45

54.3 0.05 (in 0.5 L) 52.9 54.9 3.78 49.6 6.24

(b) M prediction

Initial conditions Experimental M (g) Predicted M (g)

C0 (mg/L) Desired R (%) Langmuir Error (%) Freundlich Error (%)

isotherm3 isotherm4

50.0 95.6 0.100 (for 0.5 L) 0.0809 19.1 0.106 6.00

314 99.1 0.496 (for 0.4 L) 0.420 15.3 0.540 8.87
1 2 3 4
Note: Calculated by using Eq. (6) with Eq. (7), Eq. (11) with Eq. (7), Eq. (8), and Eq. (12).
 H.-K. Chung et al. / Journal of Industrial and Engineering Chemistry 28 (2015) 241–246
Fig. 3. Comparison of removal efficiency, R, predicted by Freundlich isotherm with
mass balance to experimental data points obtained at (a) 10, (b) 30, (c) 60, and (d)
90 mg/L orthophosphate ions as a function of oyster shell powder mass, M, in 0.050 L.
C0 = 314 mg/L, the errors between the predicted and experimental
values were 15.3% and 8.87%, respectively. Even though there were
errors between the predicted and experimental values for some
cases, overall the prediction of required adsorbent mass per known
solution volume without data fitting after parameter determina-
tion was reasonable at different initial concentrations of adsorbate
for target removal.
Practical application of the isotherms
For the oyster shell powder case, the Freundlich isotherm
simulated the experimental data better. Therefore, calculations
were executed with the Freundlich isotherm in order to provide
useful information for the same set of initial experimental
conditions. Fig. 5(a) shows a typical Freundlich isotherm graph,
which gives information only at equilibrium. Plots without initial
concentration or adsorbent mass are less useful in terms of
practical applications because initial conditions are critical in
preparation for injecting adsorbent with the aim of removing
solutes such as pollutants in water and wastewater treatment.
Therefore, it is worth noting that the independent variable is the
Fig. 4. Data obtained from duplicate experiments of methylene blue adsorption
onto PAC non-linearly fitted to Langmuir and Freundlich isotherms (0.20 g PAC in
0.40 L) where Ce is methylene blue concentration in the solution at equilibrium and
qe is methylene blue mass adsorbed per unit PAC mass at equilibrium. The
experiments were duplicated.
245
Fig. 5. Plots of (a) typical Freundlich isotherm calculated with equilibrium
orthophosphate concentration as independent variable and (b) removal efficiency,
R, and equilibrium orthophosphate concentration, Ce, predicted with initial
orthophosphate concentration, C0, as independent variables (1-g oyster shell
powder in 1 L).
initial orthophosphate concentration instead of the concentration
at equilibrium in Fig. 5(b). Specifically, the equilibrium concentra-
tion and removal efficiency by adsorption of 1-g oyster shell
powder in 1 L were predicted as a function of initial orthophos-
phate concentration. Similar to the oyster shell powder case, this
method was also used to predict the expected removal efficiency
from initial methylene blue concentrations, although the data are
not shown here.
Fig. 6(a) was generated by plotting the removal efficiency as a
function of independent variables, the initial methylene blue
concentration and PAC mass per 1 L (R = R(C0, M)). This figure
illustrates the practical application of adsorption isotherms—for
instance, M = 0.4 g results in an estimated 40% removal for
C0 = 308 mg/L (point A in Fig. 6(a)). Furthermore, when 90% and
99% removal efficiencies are required at C0 = 150 mg/L, M values of
0.52 and 0.67 g should be supplied per 1 L (points B and C in
Fig. 6(a)), respectively. In other words, 670 g of PAC should be
prepared to remove 99% of methylene blue from 150 mg/L solution
in a 1-m3 batch adsorption reactor.
Fig. 6(b) shows the orthophosphate case. From the plot, removal
efficiency can be visually estimated with different initial ortho-
phosphate concentrations and oyster shell powder masses. In
addition, the oyster shell mass required to reduce the orthophos-
phate to a desired level in a water treatment setting can be
predicted from the plot. For example, when a reduction in the
concentration from 5 to 0.05 mg/L is required, which corresponds
to 90% removal, it is estimated that an M of 11.3 g should be
supplied per 1 L (point D in Fig. 6(b)). Even though more precise
246 H.-K. Chung et al. / Journal of Industrial and Engineering Chemistry 28 (2015) 241–246
Fig. 6. Contour diagrams of removal efficiency, R, in % as a function of initial solute
concentration, C0, and adsorbent mass, M, (R = R(C0, M)) for adsorption of (a)
methylene blue onto PAC and (b) orthophosphate onto oyster shell powder in 1 L
solution.
values could be calculated by directly using the developed
equations, plots similar to those in Fig. 6 would be practically
useful for determining the trend in removal efficiency as a function
of initial adsorption conditions at a glance.
Conclusions
By combining Langmuir and Freundlich isotherms with mass
balance of solutes between liquid solution and solid adsorbent
phases, the removal efficiency or required adsorbent mass was
successfully predicted using given sets of initial conditions. The
validity of the prediction method was verified by comparing the
predicted values to experimental data of orthophosphate adsorp-
tion onto oyster shell powder and methylene blue adsorption onto
PAC. The isotherm with mass balance enabled prediction of solute
concentration at equilibrium and removal efficiency by adsorption
using initial solute concentration and adsorbent mass per solution
volume. It also allowed estimation of the adsorbent mass required
for a target removal efficiency at an initial solute concentration,
implying that these models would be practically useful in
adsorption processes used for pollutant removal.
Acknowledgements
This work was supported by the Korea Ministry of Environment
as ‘‘The Eco-Innovation project (Global Top Project) (no. GT-SWS-
11-02-007-6).’’
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