Evaluation of Pulsed Corona Discharge Plasma For The Treatment of Petroleum-Contaminated Soil

Download as pdf or txt
Download as pdf or txt
You are on page 1of 9

Environ Sci Pollut Res

DOI 10.1007/s11356-016-7929-x

RESEARCH ARTICLE

Evaluation of pulsed corona discharge plasma for the treatment


of petroleum-contaminated soil
Rui Li 1 & Yanan Liu 1,2 & Ruiwen Mu 1 & Wenyan Cheng 1 & Stéphanie Ognier 3

Received: 12 August 2016 / Accepted: 16 October 2016


# Springer-Verlag Berlin Heidelberg 2016

Abstract Petroleum hydrocarbons released to the environment species attached petroleum hydrocarbons and degradation oc-
caused by leakage or illegal dumping pose a threat to human curred. This technique reported herein demonstrated significant
health and the natural environment. In this study, the potential potential for the remediation of heavily petroleum-polluted soil,
of a pulsed corona discharge plasma system for treating as well as for the treatment of organic-polluted soils.
petroleum-polluted soils was evaluated. This system removed
76.93 % of the petroleum from the soil in 60 min with an energy Keywords Discharge plasma . Soil remediation .
efficiency of 0.20 mg/kJ. Furthermore, the energy and degrada- Petroleum hydrocarbons . Effectiveness . Energy
tion efficiencies for the remediation of soil contaminated by efficiency . Degrading mechanism
single polyaromatic hydrocarbons, such as phenanthrene and
pyrene, were also compared, and the results showed that this
technology had potential in organic-polluted soil remediation. Acronym
In addition, the role of water molecules was investigated for PAHs Polycyclic aromatic hydrocarbons
their direct involvement in the formation and transportation of AOPs Advanced oxidation processes
active species. The increase of soil moisture to a certain extent PCD Pulsed corona discharge
clearly benefitted degradation efficiency. Then, treated soils PHE Phenanthrene
were analyzed by FTIR and GC-MS for proposing the degra- SI Supporting information
dation mechanism of petroleum. During the plasma discharging DC Direct current
processes, the change of functional group and the detection of EE Energy efficiency
small aromatic hydrocarbons indicated that the plasma active HPLC High-performance liquid chromatography
TOC Total organic carbon
Responsible editor: Bingcai Pan GC-MS Gas chromatography-mass spectrometry
FTIR Fourier transform infrared spectroscopy
Electronic supplementary material The online version of this article
(doi:10.1007/s11356-016-7929-x) contains supplementary material,
which is available to authorized users.
Introduction
* Yanan Liu
liuyanan@dhu.edu.cn Soil is a vital part of the natural environment. Unfortunately,
because of the leakage of underground storage tanks and pipe-
1
School of Environmental Science and Engineering, Dong Hua
lines, accidental spills, and illegal dumping, a significant
University, Shanghai, China amount of petroleum is released into soil and groundwater,
2
State Environmental Protection Engineering Center for Pollution
which poses a considerable threat to human health (Yen et al.
Treatment and Control in Textile Industry, Shanghai, China 2011). Polycyclic aromatic hydrocarbons (PAHs) account for a
3
Laboratoire de Génie des Procédés et Traitements de Surface, UPMC
significant portion of the total petroleum hydrocarbon content
Univirsity of Paris 06, EA 3492, 11 rue Pierre et Marie Curie, (Labud et al. 2007). In addition, soil contamination is usually
75005 Paris, France associated with underground water pollution and air pollution.
Environ Sci Pollut Res

Hence, the remediation of petroleum-contaminated soil for attention in recent years. Wang et al. have utilized pulsed corona
achieving sustainable development is of considerable concern discharge (PCD) plasma for the degradation of pentachlorophe-
for the government, public, and researchers. nol and p-nitrophenol at atmospheric pressure and temperature,
Significant efforts have been devoted toward the reme- followed by applying this catalyst for plasma soil remediation
diation of petroleum-contaminated soil, and researchers in their sequent studies (Wang et al. 2011; Wang et al. 2010).
have reported methods for in situ and ex situ technolo- Redolfi has reported that the abatement of the total kerosene
gies. Bioremediation is clearly the method of choice for components can reach 90 % in 22 min (Redolfi et al. 2010).
treating petroleum-contaminated soil in situ (Liu et al. From our previous studies, dielectric barrier discharge (DBD)
2008; Sanscartier et al. 2009). Maddela et al. have suc- plasma successfully removed 63.2 % of p-nitrophenol, 87.3 %
cessfully isolated microorganisms, such as bacteria and of phenanthrene (PHE), and 67.9 % of pyrene in soil (Li et al.
fungi, for removing petroleum hydrocarbons from crude 2016a; Li et al. 2015; Mu et al. 2016).
oil in solids (Maddela et al. 2016). However, the use of In this study, to the best of our knowledge, we report for the
microorganisms is limited, caused by drawbacks. Their first time the application of PCD plasma for the remediation of
use is time-consuming, as well as they have fastidious petroleum-contaminated soil; we aim at evaluating the poten-
environmental requirements (Plaza et al. 2005). Even tial of PCD plasma for treating petroleum hydrocarbon-
though a number of studies have been conducted on this contaminated soil. In this study, heavily polluted soil was
topic, the bioremediation of petroleum-contaminated soils treated by using a PCD plasma system for achieving rapid,
is still a significant challenge. Hence, studies focus on effective degradation. Degradation efficiency and energy effi-
chemical oxidation for directly destroying these pollutants ciency, as well as the possible mechanism, were investigated
or their conversion into more biodegradable products. In for evaluating the possible applications of this technology for
this regard, advanced oxidation processes (AOPs) (Ayoub treating organic-polluted soils.
et al. 2010) are drawing considerable attention as an en-
vironment-friendly, effective soil remediation technology
(Ayoub et al. 2010). Basically, AOPs depend on highly Experimental
oxidizing species, such as ozone, hydroxyl radicals, or
persulfate (Cheng et al. 2016). Yen’s group has reported Materials
that persulfate oxidation can be utilized for diesel and fuel
oil-contaminated soil (Yen et al. 2011), and Sherwood has Petroleum was purchased from a gas station in Shanghai,
reported that their modified Fenton oxidation effectively China (no. 93 gasoline). All other organic and inorganic
treated aged diesel fuel in three artic soils having a high reagents of analytical grade (Sinopharm Chemical
content of soil organic matter and Fe oxides (Sherwood Reagent Co., Ltd., China) were used as purchased without
and Cassidy 2014). Ozonation was also investigated for further purification. Table 1 summarizes the properties of
its potential to treat diesel–fuel-polluted sediments (Li soil samples collected from the campus of Donghua
et al. 2014). University in Shanghai, China. For eliminating the effect
On the other hand, non-thermal plasma is one of the AOP of organic matter on the results obtained from degrada-
technologies; for years, it has been successfully applied for tion, soil was washed with organic solvents before use. S1
treating contaminated water and air at atmospheric pressure and S2 of Supporting Information (SI) summarize the
and room temperature (Cadorin et al. 2015; Stasiulaitiene procedures of washing and preparation of petroleum-
et al. 2016). Non-thermal plasma aims at the in situ generation contaminated soil, respectively.
of active species (e.g., radicals and molecules such as hydroxyl
radicals and ozone) during discharging (Lukes et al. 2004). As Experimental setup
this technique has been proven to be a rapid, effective, and clean
method and as non-thermal plasma can non-selectively react Figure 1 shows the experimental setup; this system consisted
with various pollutants (Magureanu et al. 2010), its application of a high-voltage direct current (DC) power supply (P60KV-
for the remediation of organic-polluted soil has been attracting D-RSG-11, China) and a needle–plate corona discharge

Table 1 Main properties of soil


sample Bulk pH Organic Moisture Particle size distribution %
density (g/m3) matter (%) content (%)
Sand (>20 μm) Silt (2–20 μm) Clay (<2 μm)

0.78 7.54 3.22 1.44 14.0 57.2 28.8


Environ Sci Pollut Res

Fig. 1 Schematic diagram of


experimental setup system

reactor, which had a high-voltage electrode comprising


dVm
98 stainless steel needles; the needles were uniformly I ¼ CM ð1Þ
distributed in a multi-pore plate. The reactor was a cu- dt
boid made of polymethyl methacrylate with a length of Z T Z T Z
1 CM dV M
40 cm, a width of 40 cm and a height of 25 cm. The P¼ VIdt ¼ V dt ¼ f C M VdV ð2Þ
discharging gap between needle and ground electron was T O T O dt
14 cm. where I is the discharge current, CM is the capacitance, VM is
Pulse voltage and current were measured by using a the discharge power, and f is the supplied power frequency.
Tektronix TDS 2012B digital oscilloscope equipped with With the use of voltage signals generated by using a voltage
a high-voltage probe and current probe. Figure 2 shows the divider, a closed curve was observed. Moreover, when VM and
typical applied voltage and current signals in one pulse CM were plotted on the x and y axes, respectively, the area
from the oscilloscope during system operation. The peak- within the closed curve was proportional to the energy con-
to-peak voltage in our application was 30 kV with a pulsed sumed during discharge in the period T.
frequency of 50 Hz. Figure S3 in SI shows the multiple Energy efficiency (EE; mg/kJ) is defined as follows:
pulses.
Discharge power (P) is calculated by the Lissajous figure mpetroleum
EE ¼ ð3Þ
method, and the integration formulae are as follows: Pt

0.7

Before treatment
0.6 20min
Voltage 40min
0.5 60min
Absorbance (Abs)
9ROWDJH(kV)

Degradation efficiency (%)


&XUUHQW(A)

80
0.4
60

0.3 40

20

Current 0.2 0
0 20 40 60
Time (min)
0.1

0.0
200 220 240 260 280 300 320 340
7LPH (us) Wavelength (nm)
Fig. 2 Typical voltage and current waveforms obtained from the Fig. 3 The UV absorption curve of petroleum aromatics at different time
oscillography of PCD treatment
Environ Sci Pollut Res

25 0.40
Soil moisture was measured by the gravimetric method.
Mineralization was determined by using a total organic carbon
20 Energy efficiency 0.36
(TOC) analyzer (Shimadzu). The components of petroleum

Energy efficiency (mg/kJ)


TOC removal rate (%)

hydrocarbons were analyzed by a gas chromatography-mass


0.32
15 spectrometry (GC-MS, QP-2010Ultra) system. Fourier trans-
form infrared spectroscopy (FTIR, NEXUS-670) was
0.28
10 employed for the characterization of the chemical bonds of
the soil samples. S3 of SI shows the details of all analysis
TOC removal rate 0.24
5
methods. All experiments were conducted in triplicate under
identical conditions, and the results were obtained as the av-
0.20
erage value.
0
0 10 20 30 40 50 60
Time (min)
Fig. 4 Evolution of TOC removal rate and energy efficiency with Results and discussions
treatment time

Evaluation of the effectiveness of plasma treatment


Here, mpetroleum denotes the average of the mass of petro-
Figure 3 shows the UV absorption spectrum of petroleum
leum removed, and t denotes the treatment time of the
aromatics at different times of treatment with the following
petroleum-contaminated soil.
operating parameters: peak-to-peak voltage of 30 kV, a pulsed
frequency of 50 Hz, a discharging gap distance of 14 cm, a soil
Extraction and analysis
moisture content of 1.44 %, and an initial concentration of
5000 mg/kg. Later experiments were conducted under these
First, the treated soil was immediately extracted by using 20 mL
conditions unless otherwise noted. With treatment time, ab-
of petroleum ether. After sonication at 30 °C for 30 min, mixing
sorption decreased, while degradation efficiency increased.
at 250 rpm for 60 min, and centrifugation at 5000×g for 20 min,
Moreover, in 60 min, the degradation efficiency reached
the supernatant was then pipetted for analysis. The recovery of
76.93 %. The increasing treatment time resulted in the forma-
petroleum hydrocarbon was greater than 88 %. UV–Vis spec-
tion of active species, which react violently with the PAH
troscopy (TU-1810) was employed for measuring the concen-
molecules in petroleum, resulting in the degradation of these
tration of the total petroleum hydrocarbon at a wavelength of
target pollutants.
223 nm, and S3 of SI shows the related supporting materials for
For further evaluating the effectiveness of PCD plasma
proving the effectiveness of the UV method. Degradation effi-
technology for treating petroleum-polluted soil, the TOC re-
ciency was calculated as follows:
moval rate and EE were calculated, and Fig. 4 shows the
results. After 60 min, 21.07 % of the petroleum components
Degradationefficiency ð4Þ were mineralized into H2O and CO2 with an EE of 0.20 mg/
½UV223 absorbancebefore treatment‐ ½UV223 absorbance
aftertreatment kJ. Table 2 lists the comparison of different remediation
¼ h methods for treating petroleum hydrocarbon-contaminated
UV223 absorvancebeforetreatment
soil. Bioremediation and AOPs such as Fenton-like processes,

Table 2 Comparisons of
different remediation methods for Method Pollutant Initial Quality (g) Time Degradation Literatures
petroleum hydrocarbon- concentration efficiency (%)
contaminated soil
Ozonation Diesel 25,000 mg/kg 15 20 h 92 Li et al. (2014)
Persulfate Diesel 5040 mg/kg 2.5 12 h 38 Do et al. (2010)
Fenton process Diesel 1000 mg/kg 5 8h 75 Pardo
et al. (2014)
Biotreatment Diesel 10 % (v/v) 10 2 weeks 86.94 Singh
et al. (2008)
Biotreatment Petroleum 60,600 mg/kg 50 35 days 47 Mancera-Lopez
et al. (2008)
This study Petroleum 5000 mg/kg 5 60 min 76.93 –
Environ Sci Pollut Res

1.4%
80 2500mg/kg 80 9.2%
5000mg/kg
18.8%
7000mg/kg

Degradation efficiency (%)


10000mg/kg
Degradation efficiency (%)

60 60

40 40

20 20

0 0
0 10 20 30 40 50 60 0 10 20 30 40 50 60
Time (min) Time (min)
Fig. 5 Petroleum degradation at different initial concentrations Fig. 6 Petroleum degradation at different soil moisture contents

ozonation, and persulfate oxidation have demonstrated prom- shows the energy efficiencies at the four concentrations: EE
ise for treating petroleum hydrocarbon-polluted sediments. increased from 0.11 to 0.30 mg/kJ, while the initial concen-
Nevertheless, considering the degradation efficiency, treat- tration increased from 2500 to 10,000 mg/kg. Under the same
ment time, and EE, this technology can remediate discharging conditions, the same amount of the active species
petroleum-polluted soil (a degradation efficiency of was generated. High petroleum concentrations imply that
76.93 %) in a short period of time (60 min) and consume more pollutant molecules exist, which would compete with
limited input energy for per unit of contaminates (0.20 mg/ each other for active species, leading to a low degradation
kJ), suggesting that the PCD plasma system demonstrates sig- efficiency for 10,000 mg/kg soil. This result was consistent
nificant potential for the remediation of petroleum- with that reported previously (Lou et al. 2012). The trend for
contaminated soil. EE was opposite to that of degradation efficiency because
most active species, such as hydroxyl radicals, were short-
Comparison of treatment using single and heavy lived. High petroleum hydrocarbon concentration provides
contaminants more chances for pollutant molecules to react with these spe-
cies before disappearing in air. Considering both degradation
The ability to degrade high concentrations of petroleum- efficiency and EE, there is a chance that the PCD plasma
polluted soils was assessed by comparing the degradation ef- system can be applied for treating heavily polluted soils.
ficiencies of 2500, 5000, 7500, and 10,000 mg/kg polluted Petroleum hydrocarbon contains a significant amount of
soil. From Fig. 5, the higher the pollutant concentration, the PAHs. In this study, for investigating the ability to treat single
lower the degradation efficiency. After 60 min of treatment, and mixed pollutants, as well as different concentrations, two
petroleum hydrocarbon was degraded by 81 % from an initial typical PAHs were chosen for the comparison of degradation
concentration of 2500 mg/kg. However, with increasing initial and energy efficiencies. As shown in Table 3, single PAHs,
concentrations to 5000, 7500, and 10,000 mg/kg, the removal such as PHE and pyrene, were degraded by using PCD plasma
efficiencies were 77, 67, and 57 %, respectively. Table 4 at degradation efficiency of 91 and 51 %, respectively. This
result indicated that PCD plasma reacts non-selectively with
Table 3 Degradation and energy efficiency of individual PAHs and
petroleum
Table 4 Soil moisture content after different treatment time
Pollutant Initial Degradation Energy
concentration efficiency efficiency Treatment Moisture content Moisture content
(mg/kg) (%) (mg/kJ) time (min) before treatment (%) after treatment (%)

Phenanthrene 200 91 0.25 20 18.8 2.79


Pyrene 200 51 0.19 40 18.8 1.51
Petroleum 2500 81 0.11 60 18.8 1.22
Petroleum 5000 77 0.20 20 9.2 1.86
Petroleum 7500 67 0.26 40 9.2 1.17
Petroleum 10,000 57 0.30 60 9.2 0.84
Environ Sci Pollut Res

Role of soil moisture for the formation and performance


3097 before treatment
of active species
1412
2853
836 720
2961 873 800 During the application of voltage to a plasma system, the
2925 1324
1013
presence of water molecules directly affects the formation
1579 and distribution of active species. In addition, water molecules
1486 1243 1106
T (%)

1152
can also affect mass transfer between soil and air (Wang et al.
1773
2014a). Hence, soils with different moisture contents are treat-
3069 1710
1012 ed by using the PCD plasma system, and Fig. 6 shows the
2853 after treatment 1073 837
2956 873 720 results. The increase of soil moisture to a certain extent clearly
2925
benefitted degradation efficiency. In the first 20 min, the deg-
1579 1107 radation efficiencies at moisture contents of 1.4 and 9.2 %
1486 1243 1152 were 42.58 and 50.69 %, respectively, indicating an increase
3500 3000 2500 2000 1500 1000 of 20 %. At 40 min, an additional enhancement of 28 % with
-1 respect to the degradation efficiency was observed. H2O
Wavelength (cm )
played an important role in the formation of oxygen and hy-
Fig. 7 The FTIR spectra of petroleum pollutant before and after PCD
plasma treatment
drogen active species, as well as in the interaction of these
reactive species; water can be excited and ionized by energetic
electrons. Hence, slight increase in the moisture content en-
hances degradation. Our previous study has discussed the for-
target pollutants, opening avenues for its future application for mation of hydroxyl radicals from water molecules (Li et al.
treating other organic-polluted soils. By comparing the EEs of 2016b), and the following pathways also show the possible
PHE, pyrene, and petroleum at different concentrations, PHE reactions of water molecules (Du et al. 2008; Wang et al.
exhibited an EE of 0.25 mg/kJ, while pyrene exhibited an EE 2014a):
of 0.19 mg/kJ. Meanwhile, EE was higher for petroleum
hydrocarbon-polluted soil, indicating that this technique is 2H2 O þ e− →H2 O2 þ H2 ð5Þ
suitable for treating polluted soil with high contaminant con- −
H2 O þ e →⋅O þ ⋅OH ð6Þ
centrations and complex components, as well as promising for − þ −
the treatment of PAHs and other types of organic- H2 O þ e →H2 O þ 2e ⋅ ð7Þ
contaminated soil. H2 O þ ⋅O→2⋅OH ð8Þ

Fig. 8 The GC-MS data of 5.699


petroleum-polluted soil before 200000 before treatment
6.602 7.667 8.201
and after PCD plasma treatment 7.084
160000 8.907

120000 5.181

5.300
80000 10.595
9.956
10.848
40000
Abundance

0
200000 after treatment

160000

120000

80000

40000

0
3 4 5 6 7 8 9 10 11 12 13
Time (min)
Environ Sci Pollut Res

Table 5 Main products detected by GC-MS

Molecular Molecular Molecular CAS


No. Time (min) Compound
formula structure weight number

1 5.181 3-Ethyltoluene C9H12 120 620-14-4

2 5.300 Mesitylene C9H12 120 108-67-8

1,2,3-Trimethylbenz
3 5.699 C9H12 120 526-73-8
ene

4 6.602 1,4-Diethylbenzene C10H14 134 105-05-5

2-ethyl-1,4-dimethyl
5 7.084 C10H14 134 1758-88-9
benzene

1,2,4,5-Tetramethyl
6 7.667 C10H14 134 95-93-2
benzene

1-Allyl-2-methylben
7 8.201 C10H12 132 1587-04-8
zene

8 8.907 Naphthalene C10H8 128 91-20-3

9 9.956 ε-Caprolactam C6H11NO 113 105-60-2

2-Methylnaphthalen
10 10.595 C11H10 142 91-57-6
e

1-Methylnaphthalen
11 10.848 C11H10 142 90-12-0
e

However, at a moisture content of 18.8 %, a low degrada- reactive sites on the soil surface, impeding the reaction of
tion efficiency was observed. In highly moist soils, the soil active species with petroleum hydrocarbons. Similar results
surface is covered by water molecules, which block the have been reported by Wang et al. (2014b). Meanwhile, high
Environ Sci Pollut Res

moisture content decreases soil porosity, hindering the reac- summarizes their retention times as well as compound
tion between pollutants and active species (Choi et al. 2002). information. Aromatic hydrocarbons in the petroleum-
After treatment for 60 min, the soil moisture content decreased contaminated soils were predominantly naphthalene and
in the range from 0.84 to 2.70 % (Table 4), mainly attributed to homologs of benzene. The predominantly detected com-
the reactions of water molecules, as well as the heating of the pounds were 1,2,3-trimethylbenzene, 1,4-diethylbenzene,
PCD plasma reactor. This result also manifested similar deg- 2-ethyl-1,4-dimethylbenzene, 1,2,4,5-tetramethylbenzene,
radation efficiency at 60 min for soils with different moisture 1-allyl-2-methylbenzene, and naphthalene. Most of the
contents. peaks corresponding to individual components decreased
after degradation, indicative of the degradation of pollut-
Degradation mechanism ants. Peaks for the highly detected compounds sharply
decreased, and naphthalene as well as its homologs was
For better understanding degradation, FTIR was adopted barely observed after PCD plasma treatment. However,
for monitoring the change of functional groups before and peak corresponding to ε-caprolactam increased, attributed
after treatment, and Fig. 7 shows the result. Bands were to the ring opening and formation of the carbonyl and
observed at 3100–3000 and 1650–1450 cm−1, correspond- amide groups. These phenomena were consistent with
ing to C–H stretching vibrations and skeletal vibration of degradation efficiency in terms of treatment time as well
the benzene nucleus, respectively. The absorption in these as FTIR analysis. As discharging progresses, active spe-
two regions confirmed the existence of aromatic rings. cies such as ozone and hydroxyl radicals are generated,
Peaks were also observed at 650–900 cm−1, attributed to which then react with aromatic rings. Substitution and
the C–H out-of-plane flexural vibration of aromatic rings. lactonization occur, leading to the opening of rings and
The strong absorption accounted for substitution reactions, formation of small-molecule chemicals. Finally, the re-
and the substituent position was closely related to wave- moval of petroleum hydrocarbons from soil was realized.
lengths: Peaks at 720 cm −1 corresponded to mono-
substitution; those at 837 cm−1 corresponded to para-
substitution; those at 800 cm−1 corresponded to para-
substitution or 1,2,3-tri-substitution; those at 873 cm−1 Conclusions
corresponded to 1,3,5-tri-substitution. Before treatment,
the substituent peaks centralized at 700–800 cm−1, indi- In this study, petroleum-polluted soil was remediated by using
cating that one to four C–H bonds are connected to sub- a PCD plasma system for evaluating the possibility of this
stituent groups. The C–H stretching vibrations of methyl technique for soil remediation. The main findings may be
and methylene were observed at 2960 and 2870 cm−1, summarized as follows:
corresponding to symmetrical and unsymmetrical vibra- 1. The PCD plasma system could degrade 76.93 % of pe-
tions, respectively. In addition, ether exhibited peaks at troleum from contaminated soils in 60 min from an initial
1013 cm−1, and the characteristic absorption of carbonyl concentration of 5000 mg/kg with an EE of 0.20 mg/kJ.
groups was observed at 1579 cm−1, indicating possible This technology was proven to be effective for the remedia-
refractory nitrogen-containing heterocycles. After PCD tion of petroleum-contaminated soils.
plasma processes, the band at 1013 cm−1 significantly de- 2. High initial concentration resulted in low degradation
creased, indicating that the C–O–C structure is destroyed efficiency and high EE. PCD plasma is promising to treat
under the constant attack of active species. The decreasing heavily petroleum-polluted soil, and it is also suitable for
peaks at 3100–3000 and 1650–1450 cm−1 indicated the treating PAH-polluted soils.
reduction of aromatic rings. Beyond that, peak intensities 3. Soil moisture was crucial to the formation of active spe-
decreases at 700–880 cm−1, corresponding to the decrease cies as well as their transfer in air and soil. The slight addition
of C–H connected to the substitution group. Based on the of moisture was beneficial to the degradation efficiency.
fading of these characteristic absorption peaks, the PCD 4. FTIR spectral analysis indicated difference before and
plasma system clearly destroyed the chemical bonds of after treatment, indicative of the degradation of petroleum
pollutants and effectively degraded the components of pe- hydrocarbons.
troleum. This conclusion was further testified by the re- 5. From the results obtained herein, the PCD plasma
sults obtained from GC analysis. system is rapid and effective for the remediation of
For tracking the fate of individual compounds in the petroleum-contaminated soil, and it demonstrates poten-
petroleum-polluted soil, samples were extracted and ana- tial for treating PAHs and other organic-polluted soils.
lyzed by GC-MS before and after treatment. The main Further studies should be performed on a large scale with
products were identified, and Fig. 8 shows the results. In less input energy for laying the foundation for future
total, 11 compounds were identified, and Table 5 applications.
Environ Sci Pollut Res

Acknowledgments This work was completed by the financial support Lou J, Lu N, Li J, Wang T, Wu Y (2012) Remediation of
of the National Natural Science Foundation of China (No. 51578122), the chloramphenicol-contaminated soil by atmospheric pressure dielec-
program for New Century Excellent Talents in University (NCET-12- tric barrier discharge. Chem Eng J 180:99–105
0826), Shanghai Pujiang Program, the Fundamental Research funds for Lukes P, Appleton AT, Locke BR (2004) Hydrogen peroxide and ozone
Central Universities (CUSF-DH-D-2015041), and China Scholarship formation in hybrid gas-liquid electrical discharge reactors. IEEE T
Council. All the financial supports are gratefully acknowledged. Ind Appl 40:60–67
Maddela NR, Burgos R, Kadiyala V, Carrion AR, Bangeppagari M
(2016) Removal of petroleum hydrocarbons from crude oil in solid
and slurry phase by mixed soil microorganisms isolated from
References Ecuadorian oil fields. Int Biodeter Biodegr 108:85–90
Magureanu M, Piroi D, Mandache NB, David V, Medvedovici A,
Ayoub K, van Hullebusch ED, Cassir M, Bermond A (2010) Application Parvulescu VI (2010) Degradation of pharmaceutical compound
of advanced oxidation processes for TNT removal: a review. J pentoxifylline in water by non-thermal plasma treatment. Water
Hazard Mater 178:10–28 Res 44:3445–3453
Cadorin BM, Tralli VD, Ceriani E, de Brito Benetoli LO, Marotta E, Mu R, Liu Y, Li R, Xue G, Ognier S (2016) Remediation of pyrene-
Ceretta C, Debacher NA, Paradisi C (2015) Treatment of methyl contaminated soil by active species generated from flat-plate dielec-
orange by nitrogen non-thermal plasma in a corona reactor: the role tric barrier discharge. Chem Eng J 296:356–365
of reactive nitrogen species. J Hazard Mater 300:754–764 Plaza G, Nalecz-Jawecki G, Ulfig K, Brigmon RL (2005) The application
Cheng M, Zeng G, Huang D, Lai C, Xu P, Zhang C, Liu Y (2016) of bioassays as indicators of petroleum-contaminated soil remedia-
Hydroxyl radicals based advanced oxidation processes (AOPs) for tion. Chemosphere 59:289–296
remediation of soils contaminated with organic compounds: a re- Redolfi M, Makhloufi C, Ognier S, Cavadias S (2010) Oxidation of
view. Chem Eng J 284:582–598 kerosene components in a soil matrix by a dielectric barrier dis-
charge reactor. Process Saf Environ Prot 88:207–212
Choi H, Lim HN, Kim J, Hwang TM, Kang JW (2002) Transport char-
Sanscartier D, Zeeb B, Koch I, Reimer K (2009) Bioremediation of
acteristics of gas phase ozone in unsaturated porous media for in-situ
diesel-contaminated soil by heated and humidified biopile system
chemical oxidation. J Contam Hydrol 57:81–98
in cold climates. Cold Reg Sci Technol 55:167–173
Du C, Shi T, Sun Y, Zhuang X (2008) Decolorization of acid Orange 7
Sherwood MK, Cassidy DP (2014) Modified Fenton oxidation of diesel
solution by gas-liquid gliding arc discharge plasma. J Hazard Mater
fuel in arctic soils rich in organic matter and iron. Chemosphere 113:
154:1192–1197
56–61
Labud V, Garcia C, Hernandez T (2007) Effect of hydrocarbon pollution Stasiulaitiene I, Martuzevicius D, Abromaitis V, Tichonovas M,
on the microbial properties of a sandy and a clay soil. Chemosphere Baltrusaitis J, Brandenburg R, Pawelec A, Schwock A (2016)
66:1863–1871 Comparative life cycle assessment of plasma-based and traditional
Li R, Liu Y, Sun Y, Zhang W, Mu R, Li X, Chen H, Gao P, Xue G, Ognier exhaust gas treatment technologies. J Clean Prod 112:1804–1812
S (2015) Degradation of p-nitrophenol in soil by dielectric barrier Wang T, Lu N, Li J, Wu Y, Su Y (2011) Enhanced degradation of p-
discharge plasma. Water Air Soil Poll 226 nitrophenol in soil in a pulsed discharge plasma-catalytic system. J
Li R, Liu Y, Cheng W, Zhang W, Xue G, Ognier S (2016a) Study on Hazard Mater 195:276–280
remediation of phenanthrene contaminated soil by pulsed dielectric Wang TC, Lu N, Li J, Wu Y (2010) Evaluation of the potential of penta-
barrier discharge plasma: the role of active species. Chem Eng J 296: chlorophenol degradation in soil by pulsed corona discharge plasma
132–140 from soil characteristics. Environ Sci Technol 44:3105–3110
Li R, Liu YA, Cheng WY, Zhang WJ, Xue G, Ognier S (2016b) Study on Wang TC, Qu G, Li J, Liang D (2014a) Evaluation of the potential of soil
remediation of phenanthrene contaminated soil by pulsed dielectric remediation by direct multi-channel pulsed corona discharge in soil.
barrier discharge plasma: the role of active species. Chem Eng J 296: J Hazard Mater 264:169–175
132–140 Wang TC, Qu G, Li J, Lu N (2014b) Transport characteristics of gas
Li X, Cao X, Wu G, Temple T, Coulon F, Sui H (2014) Ozonation of phase ozone in soil during soil remediation by pulsed discharge
diesel-fuel contaminated sand and the implications for remediation plasma. Vacuum 101:86–91
end-points. Chemosphere 109:71–76 Yen C-H, Chen K-F, Kao C-M, Liang S-H, Chen T-Y (2011) Application
Liu P-WG, Whang L-M, Yang M-C, Cheng S-S (2008) Biodegradation of persulfate to remediate petroleum hydrocarbon-contaminated
of diesel-contaminated soil: a soil column study. J Chin Inst Chem soil: feasibility and comparison with common oxidants. J Hazard
Eng 39:419–428 Mater 186:2097–2102

You might also like