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16 =6 K 3? & K

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( #+H :

Experimental Study of Effects of pH, Temperature and H2O2 on Gasoline

Removal from Contaminated Water Using Granular Activated Carbon
Hasti Hasheminejad 1
Naser Taleb Beydokhty 3
(Received Dec. 8, 2007

Ayoub Karimi- Jashni 2

4
Parviz Monajemi
Accepted Apr. 23, 2008)

Abstract

Contamination of water with petroleum compounds is a serious environmental problem in Iran. Old fuel storage
tanks, gasoline stations, and oil refineries are the main sources of gasoline leakage into water resources. In this
study, the batch adsorption technique was used to investigate adsorption of petroleum compounds (gasoline) on
granular activated carbon. Experiments showed that the adsorption capacity of activated carbon is a function of
pH, temperature, and H2O2 concentration in solution. Maximum adsorption of petroleum compounds was
obtained at pH of 8. Adsorption of petroleum compounds was increased by decreasing temperature (due to
decreasing van der Waals forces between the adsorbent and the adsorbate) and H2O2 concentration in solution
(due to the decrease in the initial concentration of the adsorbate by oxidation) . In this experiment, the maximum
equilibrium capacity of granular activated carbon was 129.05 mg COD/g GAC at pH 8 and at an ambient
temperature of 10^C. The experimental adsorption data were fitted to the Freundlich and Langmuir adsorption
model. The correlation coefficients calculated indicate that the Freundlich model was best fitted. Also, the
regression analysis was used with a correlation coefficient of 0.981 to develop a model for describing the
relationship between absorption variation in equilibrium state, pH, temperature, and H2O2. On the whole, the
correlation coefficient calculated by the proposed model was found to be higher than Freundlichs.

Keywords: Granular Activated Carbon, Adsorption, Gasoline, Contaminated Water, Isotherm,

Hydrogen Peroxide.
1. Assist. Prof., Dept. of Civil Eng., Isfahan University of Technology,
(Corresponding Author) (+98 311) 3913833 hhasheminejad@cc.iut.ac.ir
2. Assist. Prof., Dept. of Civil and Environmental Engineering, Shiraz
University
3. Prof., Dept. of Civil and Environmental Engineering, Shiraz University

43

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44

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45

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46

8; . ) L $ *r ; * L $ QP ;*
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1 %D = )
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1; 5 . ;
W
QP
P
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# (#

Shukla et al.

Hyperconjugation
(>#)
pH=5

130
120

pH=7

pH=8

pH=9

1600

110
100

1400
1200
1000
800

90

600

80

400

2 8$ * ! G V
V
;pH COD

50

100
(

pH

47

pH=6

1800

COD(mg /L)

qe (mg of COD/gr of adsorbent)

(,)

;pH
G (qe)

COD [

150
)0

x$(VR ) 7D+
3$ /R G
QP [ x$ ( )

200

250

300

h
G +
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& DM ; 8
R S & ^/^^ i/ii =p O
2
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. WT = )Q& g R G
% B
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gB
COD [ x$ =VR n 6 )
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*r
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Snoyeink
3
Zogorski and Faust
2

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5 L $ W
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3$ / R G
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5 I
5 8 / R G qe[ x$ /# +
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5
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9
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1; = 1 %D % 3R @
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5
0 I
3D
L $ : ) S A [ 3R @ * $
8 * E ./ )Q&
(>#)
t=15

t=20

t=30

1800

140

1600

130
COD(mg /L)

qe (mg COD/gr of adsorbent)

(,)

t=10

120
110

1400
1200
1000
800

100

600

90

400

10

15
(

20

25

30

50

100
(

= )

2 8$ * !
V
;

G V
COD

;
G (qe)

150
)0

200

250

300

COD [

x$ (VR ) 9 7D+
3$ /R G
QP [ x$ ( )

48

(>#)
C=0 mg/L

140

1800

130

1600

120

1400

COD (mg /L)

qe (mg COD/gr of adsorbent)

(,)

110
100

1000
800

80

600

70

400
2

4
C H2O2 (mg/L)

2 8$ * !
*r ;

50

100
(

G *r ;
(V
gB

(V

gB
G (qe)

COD

C=3.33mg/L

1200

90

C=6.66mg/L

150
)0

200

250

300

COD [

x$ (VR ) F 7D+
3$ /R G
QP [ x$ ( )

pH=8,Temp.=15C, Con. Of H2O2=0 mg/L

pH=8,Temp.=15C, Con. Of H2O2=6.66mg/L
pH=8,Temp.=15C, Con. Of H2O2=3.33mg/L

1800

COD (mg/L)

1750
1700
1650
1600
1550
1500
0

2 8$ * !

/ B 1 % D
\
W
! : 9+ :
[ WG 60
/B1 %D
3D 5

G *r

;
:
.
^

49

(V

gB

& : ; I =/
W
R / B = \ *r ;
(
R /B 1;
$ $5 .
1;
g+~ W P
;: 9+ \
*%
[ T5
&
= )
~P
L $ W
QP * % =*r ;
(
.
1; %
,T

100

*$@.#

F 9

6 8E \@
QPe
;
G
5 ./ :Y / 8;
QP S $ % 5 3$
:Y
g C 8
3$ /R G
~ P QP / D
9+ :
QP
~ P 6 8$ @ [ T <0 ,
QP S $ %
5 3$ B .[Z]] & * = )
&: W
8, 9 R D ? 3
! 3R @ 5
@ [ T *+ @0 S D _ @ [ T 8, 9
:/ * 6 >

)0

200

~ P > D : R+ + ; 8

300

COD [

x$ I 7D+

1; ; 8 *r ;
( /B
3D 5 L $ W
QP / D I O
3$ /R G
) *r ;
( >D ; 8
@ )
5 [ x$ * % . + /
Zb]/p mg COD/g GAC
3D 5 L $ 5 % QP O 5 I 5 8
P M D 5 =1 !+ [ ; I
. T by/p^
= \
3D 5 *r ;
( * %8; FG
1; A
W
R /B
x$ P
D M 1 !+ = M D 5 * ) 5)
. )
QP \
) S A ~ P > D : R+ + 8 *r ;
(* 8
= 85
P $ . ) : ; I 6 >_6 )
T )
WT 8 *r ;
( /B
@ )
? : P
QP
#$ 6 R ; 8 /B 1;
( / B 1 % D ./ T Z/
8 G
L $*
S A 6 R * % 5 = ; 8 *r ;
5
.
1 %D T Zb/_^ * % $ *r ;
(
>
*r ;
( 5
P$
$$

S $%
;
* I (R2) j5 3$ M O
, #8; 3D 5 L $ W [ # $ QP O R D
@ : ; * I R D QP S $ %
.
g
./ =: W
3D 5 /0
,T

S
*
5
:

2 # 6 pO*

qe= x/m= (b.qmax.Ce)/(1+b.Ce)

Ce/(x/m) = 1/(b.qmax) + (1/qmax)Ce

:*+
=S & S &
G
R 3$ /B
~ P QP / D qe
S & ) COD G
3$ /R G
W : /B Ce
~ P *! G
W [ # $ O 5 I qmax =( R
~ P @
6 h 9 $
6 I$ B
O
/
/ C (S &
R) b (S & S & )
8, 9 R 3 -9 83 . )
@
QP r
5 1
: 5 ,8; -.
~ P @
@ )
.[b_]
/ % QP
; R
qL [ T
$ $ *+ @0 S D R D
:/ * 6 > y
(1/n)
qe= Kf.Ce
(q)
Log qe= Log Kf+(1/n) log Ce
(y)
:L 5
a
QP/ D : ; * I $ $
)
/ C n Kf
8, 9
!: W
B .[b_] /
Q P[ )
^6 ). 8 : W
@0 L ! * $ R
D
=y ; 8 pH
@ )
Ce
G qe [ x$
WT
*r
;
( /B 2
P Zp L \
: 8; R D
8, 9
g C. ; * I = )
./ : ) : + Z P R2 O

I 9

Ce =qe

O 5 @ 5 3$ B
P
@0
@0
bybi ! 3R @ 5
& 6 \$ S A
Table Curve
8; ; %D
I
L 5 !
3$ ! . & : W
) : + g# M 5
O : 8;
5 3$
M O
:/

R2= 0.949
R2= 0.946
R2= 0.926
R2= 0.926
R2= 0.926

qe=a ce+b log pH+c log T

qe=a ce+b pH+c T
qe=a log ce+b log pH/ log T
log qe=a log ce+b log pH+c log T
qe=a log ce+b log pH+c log T

O
5 3$
:

gA
M =*
& 6 \$
;
M O 5D & B
. ) { I 5 3$ M
& * ! [ T [ Cf$ 5 *
@ 5 g

qe=0.377Ce+0.163Ce.pH+0.008Ce.T- 2.71pH. T0.00011Ce2-3.093T2 -0.011pH2.Ce . + 0.802T2.

pH-0.003CH2O22Ce- 0.043pH2.T2-264.32

Correlation Coefficient

Monolayer

P Zp

pH

COD

R2

O : 8; R

> ($ M *$@.#
2

p/]y^

p/_y]

8, 9 QP S $ %

"( *$@.#
(1/n)

Kf [(mg/g)(L/mg)

b (L/mg)

qmax
(mg/g)

p/yZZ

p/pppb

Zppp

p/ppi

g C

O % $

1. -

# 6

COD

1200

qe (m g CO D/gr G AC)

(m)
(^)

1000
800
600
400
200
0
0

P Zp

500

y pH : ,I !+ : )

1000
Ce (mg/L)

&:!

COD 2

1500

Ce

2000

G (qe)

3$ /R G

QP [ x$ N 7D+

50

COD

y
Z_
^/^^

y
Z_
i/ii

y
ip
p

y
bp
p

R2

O : 8; R

y
Zp
p

]
Z_
p

y
Z_
p

D QP S $ %
q
Z_
p

g C

^
Z_
p

_
Z_
p

$
pH

p/pppZ p/pppZi p/ppZ^ p/ppbb p/ppi p/pppyy p/ppby p/ppZ^ p/pppyq

p/pppZ^

p/i

p/^_

p/_^b p/_p p/_y]

p/_ip

p/_qq p/__]

p/_ip

p/qq

Kf
[(mg/g)(L/mg)(1/n)]
n

p/]__

p/]p

p/]_y p/]_y p/]y^

p/]Z

p/]qb p/]^q

p/]_]

p/]bp

R2

(,)
2: #

> ($ M

1200
1000
800
600
400
200

2: #

> ($ M

1200
1000
800
600
400
200
0

0
0

pH=_ (VR

500

1000
Ce (mg/L)

D QP S $ %

1500

2000

500

1000

1500

2000

Ce (mg/L)

g I (*

&
Zp C

= ; ,I !+
pH=y ( Z_ C

(
/B
=pH 8; ;
./D & >
(*r ;
()
pH
3D 5 L $ 3$ G
QP I / D
O
2
P Zp
L )
y
* I 5 . +/
Zb]/p_ mg COD/g of GAC
@ )
3D 5 L $ W
QP [ > 1 %D : ;
:%
S D ; R
/ $ T
8 pH /
* I [ 3R @ 5
, ? !.
> 0
/ E ) 8
1 %D
3D 5
QP [ >
1 % D ( ~ P @ : 9+ 5 cR
1;
1; 5 % *
/ E ) *r
;
( /B
/ gP : 9+
\
1; A
*+ /B
.
1; ( 3D 5 [ WG 60 ~ W
5
: +/
; ,I !+ ;:
,
!
) : e!
8, 9 R D ? 3
3R @
*
! / G =: + / 5 3$
M O
6 \$ % * ( ./) 8, 9
O R D
Q P * % [ x$ : \ g V T $
R =* &
/B
=pH ;
( [ Cf$ 5 D & B
3$ /R G
gI(
. & 7
\ *r ;
(
./ R D
O
$9 5 3$ M

51

S$%
R D

(>#)

qe (mg COD/gr adsorbent)

qe (mg COD/gr adsorbent)

L )
; ,I !+

(C
)
H2O2 (mg/L)/B

Ce

G (qe)

3$ /R G

QP

O g 7D+

R2=p/]yZ

5
: + / 5 3$ M O
;/B ; =pH qe Ce O [ 3R @
./
5 3$ : ,I !+
\ *r ;
([ W
.(b P) ) : e! R D
/
;:
Ce
G qe O = VR q 6 )
@ )* &
! : +/
;: =: ,I !+ : +
5 ?. 0 5 I 5 8
@ ) R D
(]
5 3$
M
O . ;
*I
5 3$ ; M
5 , q 6 ) : ) : * I : 8; : + /
)
I
: ) 5 3$ *
&
/
@
2
P Zp g +
y ; 8 pH
RG z
./
0 R D
O
# /> ! ( )
$$
gI(
: +/
@0 6> G z G
/
R G 5 . )
T p/pb T q^/bp
$ $ R D
: +/
@0 6> G z G
. )
T p/bZ T ^Z/Z

( F

W<$ =
( [ T QP
$! : W
K O\$ 5
8
\@
QPe !
&: g 5 % : R+ +
Cf $ 3R @ 5
./ D & > 3R @
3D 5

h #

nd

1- W.H.O. (1996). Benzene in drinking water, Guidelines for Drinking water Quality, 2 Ed., Geneva.
@= (@) *=

M .(4J5

+*#" $ 6! #

+# (BMe ^ 6# 6J[

$ (A

8^ X .(

.% "6= :35

).N

9 R

( 6= () *+

3- ATSDR. (1996). Toxicological profile for methyl tert- butyl ether, Division of Toxicology, Atlanta, GA.
4- ATSDR. (1995). Toxicological profile for benzene, Division of Toxicology, Atlanta, GA.
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groundwater remediation using activated carbon. Applied Energy, 83, 1258-1264.
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EPA 832-F-00-017.U.S.EPA, Washington D.C.
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638-644.
11- Zhang, C., Li, Q., and Kang, C. (2005). Wastewater produced from an oilfield and continuous treatment
with an activated carbon. Process Biochemistry, 40(2), 873-877.

QM @ ! s6@ $ .(@#

+^ AS % ,*& pf9 U+1

8& s#" $ 5"# h 7) "4. C "#

. "+

$ N # U)

s#" $

8& s#" w

# (48*

'FG &
. "+

L $ U6& "| c)

+) 5 6L $ ! M

'

M .(! :3M % h 6V

"+

$ % (4J5
. "+

% "6= UJ5 :3M} sm$

:35

,*& (SX) 'f1 .(

:35

'f1 (

"M U8*

"+

$ EA

.(

]) .' *6# $ .N (5 "

U.M% c6S () *+ ([[g

]) ./.h "&Q!$\ $ .N

68)

U.M% c6S () *+ ([[g QM ! s6 $ .$ "|

) .k

\5(A6 $ $ . S .p.h

:35

"M ( 6= () *+ (A

"6 L . 2 6#

":* s6 +5 . L $

' . (M 6 6= (BM 6& "Mf 6J[ .(

>) .h 2 8)

.% "6= :35

= () *=

4C ) $

() *+

>

16- Karimi- Jashni, A. (1994). Effect of pH on adsorption and desorption equilibria and kinetics of
2- Nitrophenol and phenol onto two activated carbons. M.Sc. Thesis, University of Ottawa, Ontario,
Canada.
17- APHA. (2005). Standard Method for Examination of Water and Wastewater, 21 Ed., Publication Office
American Public health Association, New York, Washington D.C.
18- Smith, M.B., and March, J. (2001). Marchs advanced organic chemistry, 5th Ed., John Wiley and Sons Inc.,
New York.

52

19- Shukla, S.S., Yu. L.J., Dorris, K.L., and Shukla, A. (2005). Removal of Nickel from aqueous solutions by
sawdust. J. Hazard. Mater., 121, 243-246.
20- Zogorski, J. S., and Faust, S.D. (1978). Equilibra of adsorption of phenol by granular activated carbon.
Chemistry of Wastewater Technology, Ann Arbor, Michigan.
21- Hameed, B.H., Chin, L.H., and Rengaraj, S. (2008). Adsorption of 4-Chlorophenol on to activated carbon
prepared from rattan Sawdust. Desalination, 225, 185-198.
22- Cooney, D.O., and Wijaya, J. (1987). Effect of pH and added salts on the adsorption of ionizable organic
species on to activated carbon from aqueous solution. Proc. 2nd Eng. Found., Conf. Fundam. Adsorpt.,
LiAPis New York, 185- 194.
23- Cambiella, A., Ortea, E., Rios, G., Bentio, J.M., Pazos, C., and Coca, J. (2006). Treatment of oil-in-water
emulsions: performance of a sawdust bed filter. J. Hazard. Mater., 131, 195-199.
24- Snoeyink, V.L. (1968). Adsorption of strong acids, phenol and 4-Nitrophenol from aqueous solution. Ph.D
Thesis, Dept. of Civil Eng., University of Michigan, Michigan.
25- AWWA. (1990). Water quality and treatment, 4th Ed., McGraw- Hill Inc., USA.

53