Removal of Polycyclic Aromatic Hydrocarbons from Sediments using

Chemical Oxidation Processes

Chiu-Wen Chen, Nguyen Thanh Binh, Chang-Mao Hung, Chih-Feng Chen, Cheng-Di Dong*
Department of Marine Environmental Engineering, National Kaohsiung Marine University, 142 Haijhuan Road,
Nanzih District, Kaohsiung City 81157, Taiwan

Abstract:
The presence of polycyclic aromatic hydrocarbons (PAHs) in sediments is a major concern of risks associated
with the aquatic ecosystems through bioaccumulation in food chains. To minimize the ecological risks due to
contaminated sediments, processes that can degrade the sorbed PAHs are urgently needed. The present study
aims at assessing the treatment efficiency of several chemical oxidation processes using potassium permanganate
(KMnO4), sodium persulfate (Na2S2O8), conventional Fenton, and modified Fenton. Efforts were focused on
identifying the most effective liquid oxidant to obtain the maximum acceptable concentration for a total of 16
PAH compounds (1000 ng/g) and on assessing the optimal reactant doses. The concentration of PAHs in the un-
treated sediment was around 4226 ng/g (2-ring at 273 ng/g, 3-ring at 1285 ng/g, 4-ring at 1508 ng/g, 5-ring at
789 ng/g, and 6-ring at 369 ng/g) and 76% of degradation was required to meet the remediation goals. The
removal efficiency was 5.3–72.8%, 10.7–39.1%, 0–30.9% and 31.5–68.3% by KMnO4, Na2S2O8, conventional
Fenton and modified Fenton, respectively. Results demonstrated a medium reduction of a mixture of 16 PAHs in
sediments; only in case of using KMnO4 that showed the highest removal efficiency (72.8%) using a considerably
large amount of oxidizer. Modified Fenton showed remarkable improvement in removal efficiency compared
with the conventional Fenton method. Sodium citrate resulted in the maximum contaminant removal through
H2O2 activation at near neutral pH environment. Sodium pyrophosphate and sodium oxalate at higher dosages
could cause negative effect on the removal efficiency. In general, the degradation of PAHs in slurry system was
limited, which could be attributed to the availability and reactivity of PAHs and physical-chemical composition
of the sediment.

Keywords: Sediment, Polycyclic aromatic hydrocarbons, Chemical oxidation, Chelating agent, Fenton reaction

Introduction presence of PAH in sediments, sediment quality

Polycyclic aromatic hydrocarbons (PAHs) are a
ubiquitous group of several hundred chemically-
related, environmentally persistent organic compounds
of various structures and varied toxicity. PAHs tend to
persist in the environment and are found widespread
in natural media such as soils, sediments, water, and
air and in particular, due to their hydrophobic nature
and low water solubility, they can become rapidly
associated with sediments (1-4). Their presence in
environmental matrices is a great concern due to their
high toxicity, carcinogenic effects and environmental
persistence. Such contamination may pose an indirect
exposure threat to humans exposed to PAHs through
the consumption of foods (5-6). Around 130 PAHs
have been identified but the most studies are the 16
PAHs listed by the US Environmental Protection
Agency (US EPA) as priority contaminants. For the
*Corresponding author; E-mail: cddong@mail.nkmu.edu.tw
guideline of 1000 ng/g total PAHs to protect estuarine
fish suggested that practical activities are urgently
need to prevent adverse environmental effects from
PAH-contaminated sediments if the concentration of
total PAHs exceeds 1000 ng/g (7).
Among the various remediation techniques for
PAHs removal, chemical oxidation is considered a
promising technique and can overcome many
limitations of other methods for the remediation of
aquatic matrices contaminated by recalcitrant PAHs,
namely, strong sorption to the solid phase reduces
their availability for microbial attack and high-
molecular weight PAHs (five or six aromatic rings)
are more recalcitrant to biological degradation (8-11).
The oxidants most commonly used for chemical
remediation are hydrogen peroxide, permanganate and
persulfate. In addition, Fenton oxidation using
hydrogen peroxide and iron catalyst has emerged as a
viable remediation technique that is classified under
AOPs (Advanced Oxidation Processes). However, the

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C-W. Chen et al.
low pH (pH 2-4) involved in conventional Fenton
oxidation often hinders practical application at natural
matrices pH, which is approximately neutral as iron
catalyst is easily precipitated to iron oxy hydroxides
(Fe(OH)3). Additionally, replicating the acidic pH in
the field application is impractical due to the enormous
buffering capacity associated with most native
matrices (12-13). Hence, Fenton reaction has been
modified to extend its applicability to native matrices
pH, which is at approximately neutral. For the sake of
facilitating practical application, modified Fenton
based treatments encompass the addition of chelating
agent (CA) have recently received much attention.
Chelating agents such as sodium pyrophosphate (SP),
potassium dihydrogen phosphate (PP), ethylene-
diaminetetraacetic acid (EDTA), oxalic acid (OA),
sodium oxalate (SO), sodium citrate (SC), are able to
prevent iron precipitation even at neutral pH
conditions by forming complexes (14-18).
This study was to investigate the effectiveness of
chemical oxidation for the remediation of PAH-
contaminated sediments. Four liquid oxidants were
used tests: potassium permanganate, sodium persulfate,
conventional Fenton and modified Fenton (MF).
Additionally, it was to identify the above-mentioned
chelating agents suitable for Fe(II)-mediated activation
of H2O2 at neutral pH condition and to assess the
optimal chelating agent dose.
Materials and Methods
Sediment Samples
The contaminated sediments were obtained from
an industrial port area of southern Kaohsiung with an
Ekman Dredge Grab aboard a fishing boat. The
samples were immediately scooped into glass bottles
which had been pre-washed with n-hexane. The
collected sediments were kept frozen during trans-
portation. In the laboratory, the samples were free-
dried for 72 h before being homogenized with a mortar
and sieved (at 0.5 mm). Properties of the sediment and
initial concentrations of PAHs are presented in Table
1. Due to the high organic carbon content in the
sediment, PAHs strongly sorbed to sediment organic
carbon which can render the sediment remediation
process more difficult and the availability of oxidant
at adequate concentration for PAHs oxidation.
Chemicals
Potassium permanganate (KMnO 4, 99%), sodium
persulfate (Na2S2O8, 99%) and hydrogen peroxide
(H2O2, 35%) were purchased from Merck. Ferrous
sulfate (FeSO4.7H2O, 99%), potassium iodide (KI,
99%) and sodium thiosulfate (Na 2S2O3.5H2O, 99%)
were from Sigma-Aldrich. EDTA, SP, SO, PP, OA
16 J. Adv. Oxid. Technol. Vol. 18, No. 1, 2015
and SC (≥99%) were purchased from Fisher Scientific.
Acetone, methanol and n-hexane (99.8%, HPLC
grade) were purchased from Merck. Standards of 16
PAHs in a 80-mg/L mixture solution were obtained
from AccuStandard Chem. Co. (New Haven, CT,
USA). Deuterated PAH internal standard solutions
(naphthalene-d8, acenaphthene-d10, phenanthrene-d10,
chrysene-d12, and perylene-d12) at 4000 mg/L and
surrogate standard solutions (2-fluorobiphenyl and 4-
terphenyl-d14) at 2000 mg/L were obtained from
AccuStandard Chem. Co.
PAHs Oxidation by Permanganate and
Persulfate
For each test, 1 g sample of sediment was
transferred into a 40-mL borosilicate glass vial
reactor. Then, 25 mL of oxidizer solution with various
concentrations were added in each vial to reach
weight ratio of oxidizer to PAHs of 10 2 : 1, 103 : 1,
104 : 1, 105 : 1 and 106 : 1. All sample vials were
hand-shaken for ~30s and placed in a water bath
shaker (SB-9D) set at 200 rpm. The temperature of the
reaction process was controlled automatically at
ambient level (25 ± 1 oC). Reaction time was fixed at
24-hperiod. All batch experiments were conducted in
duplicate. Besides, controls examining the behavior of
contaminants alone in a slurry system were also
conducted in parallel. At the end of each experiment,
sodium thiosulfate (Na2S2O3) was added into the
reactor to terminate the potassium permanganate
oxidation (25), and persulfate degradation reactions
were quenched by the addition of an excess of
potassium iodide (KI) (26) to obtain representative
PAHs concentrations. To detect the contaminant in the
sediment as well as to assess the PAHs removal
efficiency of chemical oxidation, the solid and liquid
phases were extracted together by sonication and
solvent addition (acetone:n-hexane). PAH concen-
trations were detected by GC-MS, so as to take into
account all PAHs in the sample.
Conventional Fenton
Sediment sample (1 g) was put in contact with a
ferrous solution in 40-mL borosilicate glass vial. The
Fenton oxidation was initiated upon the addition of
H2O2 solution with different concentrations, giving a
final weight ratio of Fe2+ to PAHs of 100:1. The pH
values of all slurry systems were adjusted to 3. A
sudden addition of the entire reactant dose was avoided
because it would have resulted in the consumption of
the hydroxyl radicals for undesired side reactions
(oxidant scavengers) such as a significant amount of
radicals can be consumed by the dosed reactants (27-28).
C-W. Chen et al.

Table 1. Properties of the sediment and initial concentrations of PAHs.

Analytical items Value Method

Organic carbon % (w/w) 8.5 Loring and Rantala (19)
pH 7.2 ASTM D4972(20)
Total grease (mg/kg) 360 APHA (21)
Total nitrogen (mg/kg) 2680 USEPA Method 351.1 (22)
Total phosphorus (mg/kg) 673 USEPA Method 365.2 (22)
Sand (<2μm) (%) 13.2
Silt (2-63μm) (%) 84 Chen et al.(23)
Clay (>63μm) (%) 2.8
PAHs (ng/g) Dong et al. (24)
2-ring
1. Napthalene (NA) 273
3-ring
2. Acenaphthalene (ACY) 160
3. Acenaphthene (ACE) 265
4. Fluorene (FL) 238
5. Phenanthrene (PH) 392
6. Anthracene (AN) 230
4-ring
7. Fluoranthene (FLU) 503
8. Pyrene (PY) 525
9. Benzo[a]anthracene (BaA) 235
10. Chysene (CH) 245
5-ring
11. Benzo[b]fluoranthene (BbF) 224
12. Benzo[k]fluoranthene (BkF) 197
13. Benzo[a]pyrene (BaP) 273
14. Dibenzo[a,h]anthracene (DA) 95
6-ring
15. Indeno [1,2,3-cd]pyrene (IP) 193
16. Benzo[g,h,i]perylene (BP) 176
∑LPAHs: Total Light PAHs (1-7) 1559
∑HPAHs:Total Heavy PAHs (8-16) 2667
∑PAHs: Total PAHs 4226

All sample vials were hand-shaken for ~ 30s and
the reactions took place in a water bath shaker (SB-
9D) set at 200 rpm. The oxidation processes were
conducted at 25 ± 1oC. All batch experiments were
conducted in duplicate. Besides, controls examining
the behavior of contaminants alone in a slurry system
were also conducted in parallel. At the end of the
chosen time (24 h), methanol was added to quench
radicals and then extraction process by sonication and
solvent addition (acetone:n-hexane). The extracts were
further concentrated, and then analyzed by GC-MS.
Modified Fenton
Sediment sample (1 g) was slurries in 40-mL glass
vial containing a specific amount of chelated ferrous
ion. Two different weight ratios of chelated Fe2+ to
PAHs as 102:1 and 103:1, were performed. In both
cases ferrous ion and chelating agent were dosed at a
weight ratio of 1:1. Then the hydrogen peroxide
solution was slowly added to achieve the catalyst to
oxidant weight rato of 1:10. Other experimental
conditions were similar to those of the conventional
Fenton process.
Gas Chromatography-Mass Spectrometry (GC-
MS) Analysis
The PAHs from both sediment and slurry extracts
were analyzed using a GC (HP Agilent Technologies
6890 Gas Chromatography, USA), equipped with an
Agilent 5975 mass selective detector (MSD). The GC

J. Adv. Oxid. Technol. Vol. 18, No. 1, 2015 17

C-W. Chen et al.
5000
KMnO4: ∑PAHs
(w:w)
PAHs Concentration (ng/g)
4000
3000
2000
1000
0 0
ΣLPAHs
Figure 1. PAH removal achieved with different weight ratios of KMnO 4 to PAHs. Experimental conditions: [PAHs] ≈ 4200 ng/g;
ambient pH; reaction time = 24 h; temperature = 25 ± 1 oC. Control experiments were also carried out under the same condition without
KMnO4, the volume of KMnO4 was substituted by deionized water.
was equipped with an Agilent 7683B split/splitless
injector (splitless time: 1 min; flow: 60 mL/min);
injector temperature was maintained at 300oC. The
transfer line and ion source temperature were 280oC
and 230oC. Column being used to separate the PAH
compounds was HP-5MS capillary column (Hewlett-
Packard, Palo Alto, CA, USA) with 30 m x 0.25 mm
i.d x 0.25 μm film thickness. The carrier gas was
helium at a constant flow rate of 1 mL/min. The
column temperature was initially kept at 40oC for 1
min, gradually raised to 120oC at the rate of 25oC/min,
then increased to 160oC at the rate of 10oC/min and
finally elevated to 300 oC (final temperature was held
for 15 min) at the rate of 5 oC/min. Mass spectrometer
was operated in Selected Ion Monitoring (SIM) mode
in the electron impact mode at 70 eV. The concen-
tration of individual PAH in the solvent was quantified
using the internal standard calibration method with 5-
point standard curves (all r2>0.98).
Results and Discussion
Potassium Permanganate
The concentration of permanganate was varied for
each experiment while the initial concentration of
PAHs fluctuated in the range of 4100-4300 ng/g.
Applying chemical oxidation in remediation of PAHs
contaminated sediment as well as contaminant in soil,
the amount of oxidant will be consumed by naturally
occurring sediment oxidizable matters instead of
target compounds (29). To overcome this major
drawback, the concentration of permanganate was
increased gradually from 0.017 to 170 g/L. The
increase of oxidant decreased the PAHs concentration
significantly, with the removal efficiency ranging
from 5.3 to 72.8% (Figure 1). The greatest reduction
18 J. Adv. Oxid. Technol. Vol. 18, No. 1, 2015
Control 102:1 103:1 104:1 105:1 106:1 C/Co
1
0.9
0.8
0.7
0.6
C/Co
0.5
0.4
0.3
0.2
0.1
ΣHPAHs ΣPAHs
in PAH concentration was observed at weight ratio of
oxidant to PAHs as high as 106:1. As seen from Figure
2, remarkable degradation rate of 3-rings and 4-rings
PAH compounds occurred when oxidant was added at
high dose to reaction vial. This can be attributed to
the strong reactivity of 3 and 4 rings sorbed PAH
compounds toward permanganate in addition to the
higher initial concentration of these compounds in
sediment (3-rings accounted for 30.4% total 16 PAHs;
4-rings accounted for 35.7% total 16 PAHs), which
enhanced the contact between PAHs and oxidant
during chemical oxidation. In general, permanganate
may cause a considerable removal of PAHs from the
contaminated sediment. Furthermore, permanganate
did not require lower pH condition, which makes the
process promising for field operation. However, a
large amount of MnO2 precipitate was formed, which
is a drawback for the process (30).
Sodium Persulfate
Experimental condition with sodium persufate as
oxidant was similar to that of permanganate oxidation.
The dose of persulfate varied between 0.017 and 170
g/L. Results in Figure 3 shows that high degree of
PAHs oxidation took place at higher persulfate con-
centrations. At the highest dose of persulfate of 170
g/L only led to PAHs removal efficiency of 39.1%.
The results indicate that permanganate had better PAH
removal performance than persulfate. Our results are
in agreement with results of other researchers (27, 31).
Persulfate is a strong oxidant with a redox potential of
2.01 V in comparison with permanganate (1.7 V) but
achieved PAHs removal efficiency lower than
permanganate due to strong consumption by non-target
compounds in sediments. Based on above results it is
C-W. Chen et al.

1600

1400 2-ring 3-ring 4-ring 5-ring 6 -ring

PAHs Concentration (ng/g)

1200

1000

800

600

400

200

0
Control 102:1 103:1 104:1 105:1 106:1

Figure 2. Degradation of PAH compounds with different weight ratios of KMnO4 to PAHs.

5000
Na2 S2O 8: ∑PAHs
(w:w ) 2
Control 10 : 1
3
10 :1
4 5
10 :1 10 :1 10 :1
6
C/C o

1
PAHs Concentration (ng/g)

4000
0.9
0.8
3000
0.7
0.6

C/Co
2000 0.5
0.4
0.3
1000
0.2
0.1
0 0
ΣLPAHs ΣHPAHs ΣPAHs
Figure 3. PAH removal achieved with different weight ratios of Na 2S2O8 to PAHs. Experimental conditions: [PAH] ≈ 4200 ng/g;
ambient pH; reaction time = 24 h; temperature = 25 ± 1 oC. Control experiments were also carried out under the same condition without
Na2S2O8, the volume of Na2S2O8 was substituted by deionized water.

possible to achieve higher removal efficiency of Conventional Fenton

PAHs using higher amount of MnO 2. Hence, the The OH radical yielded in conventional Fenton
sequential application of permanganate and persulfate, reaction is the second most reactive chemical species
using persulfate to satisfy a majority of the non-target known next to fluorine atom, with a relative redox
compounds, followed by using permanganate to potential of 2.06 V. It acts as the primary radical
degrade target compounds could be applied (32). With which oxidizes contaminants. However, hydroxyl
regard to degradation of individual PAH compounds radicals is very reactive and nonspecific in attacking
(Figure 4), there are also similarities between organic molecules (33); so removal efficiency can not
persulfate and permanganate, namely there were be high when applying this reagent in the remediation
considerable degradation rate of 3-rings and 4-rings of PAHs contaminated sediments.
PAH compounds when higher dose of oxidant was For the lowest concentration of hydrogen peroxide,
used. Sodium persulfate at the highest dose of 170 g/L the results indicateed that total PAH concentration
could only remove 3-rings PAHs compounds at the after treatment did not change significantly comparing
maximum efficiency of 30.8% and 4-rings PAH to the original concentration. The most noticeable
compounds of 50.2%. observation is that there was the apparent increase in

J. Adv. Oxid. Technol. Vol. 18, No. 1, 2015 19

C-W. Chen et al.

1600

1400 2-ring 3-ring 4-ring 5-ring 6 -ring

PAHs Concentration (ng/g)

1200

1000

800

600

400

200

0
Control 102:1 103:1 104:1 105:1 106:1
Figure 4. Degradation of PAH compounds with different weight ratios of Na 2S2O8 to PAHs.

5000
H 2O2 : ∑PAHs
(w: w) 2
Control 10 :1
3
10 :1 10 4:1 105 :1 C/C o
PAHs Concentration (ng/g)

4000 1.2
1.1
1
3000 0.9
0.8
0.7

C/Co
2000 0.6
0.5
0.4
1000 0.3
0.2
0.1
0 0
ΣLPAHs ΣHPAHs ΣPAHs
Figure 5. PAH removal achieved with different weight ratio of H2O2 to PAH. Experimental conditions: [PAH]≈ 4200 ng/g; pH ≈ 3;
reaction time = 24 h; temperature = 25 ± 1 oC. Control experiments were also carried out under the same condition without the Fenton’s
reagent, the volume of the Fenton’s reagent (H2O2 and Fe2+) was substituted by deionized water. All of the conventional Fenton
experiments were performed using Fe2+ : PAHs weight ratio of 100:1.

some extractable-PAH compounds concentration after deplete OH in the reactions. The highest removal
one day exposure to Fenton’s reagent (Figure 6). efficiency of 30.9% with oxidant dose of 1.7 g/L (104:
According to Kawahara et al. (34), this considerable 102: 1, w/w/w, H2O2: Fe2+: PAHs) can be clearly seen
increase is probably due to the iron ions complexing from Figure 5. This ratio was chosen for modified
with the PAHs and weakening the adsorptive bonds of Fenton process in the presence of chelating agents
the PAHs-complex formed with matrices surface. later.
In all experiments performed with conventional
Fenton’s reagent, the removal efficiency was dependent Modified Fenton
on the oxidant dosage. The removal efficiency When chelating agents are added to the Fenton
increased with the oxidant dose if the dosage was low, reagent, they can maintain adequate dissolved transition
while if the oxidant dose was increased above a metal concentration in near-neutral pH condition as
certain level, the removal efficiency might decrease. well as can improve the persistence of H2O2 in
This effect originated from the strong and rapid chemical oxidation process (7). As a result of above-
quenching reaction caused by the high oxidant mentioned characteristics, the addition of chelating
dosages (H2O2 + OH → H2O + HO2 ), which may agents produced an increase of PAH degradation by

20 J. Adv. Oxid. Technol. Vol. 18, No. 1, 2015

C-W. Chen et al.

Table 2. PAHs removal achieved with two different weight ratios of chelated Fe 2+ to PAHs.

PAHs group ∑LPAHs ∑HPAHs ∑PAHs

PAHs (control) (ng/g) 1292 1996 3288
2+ 2 3 2 3 2
Chelated Fe : PAHs 10 10 10 10 10 103
Removal eff. (%)
SPa 34.1 21.2 36.3 38.3 35.4 31.6
SO 29.4 15.3 52.2 47.9 43.2 35.1
EDTA 25.2 33.1 43.9 50.8 36.6 43.9
PP 41.4 43.5 43.9 55.0 42.9 50.5
OA 30.4 43.7 49.3 54.9 41.9 50.5
SC 41.7 69.1 43.8 67.8 43.0 68.3
a
sodium pyrophosphate (SP), sodium oxalate (SO), ethylene diamine tetraacetic acid (EDTA), potassium dihydrogen
phosphate (PP), oxalic acid (OA), and sodium citrate (SC).

1600
2-ring 3- ring 4 -ring 5- ring 6-ring
1400
PAHs Concentration (ng/g)

1200

1000

800

600

400

200

0
Control 102:1 103:1 104:1 105:1
Figure 6. Degradation of PAH compounds with different weight ratios of H2O2 to PAH.

Fenton reaction except for SP or SO as the chelating
agents. Among all the chelating agents studied, SC
resulted in the highest PAH removal efficiency
(68.3%) with the following order: SC > OA > PP >
EDTA > SO > SP (Table 2). This is because the Fe2+ -
SC complex has a stronger bond than others and thus
played an important factor for activation of H 2O2. On
the contrary, SO or SP did not lead to significant
reduction of PAHs because of the scavenging effects
from simultaneous side reaction, which might have
occurred that limited the availability of hydroxyl
radical for PAHs oxidation (8). The stronger scaveng-
ing effect could be clearly seen from Table 2, where
10 times higher removal efficiency by two chelating
agents (SP, SO) were observed. However, the results
were not better as expected; namely; the removal
efficiency of PAHs reduced from 35.4 to 31.6% and
43.2 to 35.1% for SP and SO respectively. The
positive effect of chelating agents was evident of the
increase in PHA removal, for examples, the removal
efficiency increased from 36.6 to 43.9%, 42.9 to
50.4%, 41.9 to 50.5% and 43.0 to 68.3% for EDTA,
PP, OA and SC, respectively. This enhancement
showed that these chelating agents have no strong
reactivity against hydroxyl radical when the optimal
dosages were used. Results showed that iron/chelating
agent complexes (Fe2+ - EDTA, Fe2+ - PP, Fe2+ - OA,
and Fe2+ - SC) were superior to other complexes (Fe2+ -
SP and Fe2+ - SO) in activating H2O2.
Conclusion
This study aimed to evaluate the effectiveness of
chemical oxidation for the remediation of PAH
contaminated sediments. The oxidation of the sorbed
organic compounds as PAHs could be inhibited by the
existence of high content of organic matter in the
sediment. Thus, the remediation of compounds with
hydrophobic characteristics in sediments of high
organic content required the excess amounts of stable
oxidant. Potassium permanganate removed the highest
72.8% of total 16 PAH compounds but only with high
dosages. Sodium persulfate eliminated the highest

J. Adv. Oxid. Technol. Vol. 18, No. 1, 2015 21

C-W. Chen et al.
39.1% of total 16 PAH compounds and persulfate was
strongly consumed by non-target compounds in
sediments. Conventional Fenton process removed the
highest 30.9% of total 16 PAH compounds. Above
results indicated that in the oxidation conditions are
not strong enough, the reactants were consumed by
non-target compounds instead of PAHs. Modified
Fenton process achieved better removal efficiency
than conventional Fenton. Sodium citrate was found
to be the most effective complex agent in activating
H2O2 for the remediation of sediments contaminated
with PAHs. The abundant usage of chelating agents
can have negative effect on PAHs removal efficiency.
In general, the degradation was limited, which can be
explained by several reasons: PAHs availability,
PAHs reactivity, and sediment characteristics. Further
investigations need to be carried out to determine
experimental conditions that would ensure to meet the
remediation goals.
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Received for review April 8, 2014. Revised manuscript
received October 7, 2014. Accepted October 10, 2014.