Ye 2019

Accepted Manuscript
Emerging Sustainable Technologies for Remediation of Soils and Groundwater in

a Municipal Solid Waste Landfill Site -- A Review
Jianshe Ye, Xiao Chen, Chao Chen, Bate Bate
PII: S0045-6535(19)30701-5
DOI: 10.1016/j.chemosphere.2019.04.053
Reference: CHEM 23561
To appear in: Chemosphere
Received Date: 01 February 2019
Accepted Date: 06 April 2019
Please cite this article as: Jianshe Ye, Xiao Chen, Chao Chen, Bate Bate, Emerging Sustainable
Technologies for Remediation of Soils and Groundwater in a Municipal Solid Waste Landfill Site --
A Review, Chemosphere (2019), doi: 10.1016/j.chemosphere.2019.04.053
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ACCEPTED MANUSCRIPT
1 Emerging Sustainable Technologies for Remediation of Soils and Groundwater in a
2 Municipal Solid Waste Landfill Site -- A Review
3 1Jianshe Ye, 1Xiao Chen, 1Chao Chen, 2*Bate Bate
5 1Graduate Research Assistant, Institute of Geotechnical Engineering, College of Civil

6 Engineering and Architecture, MOE Key Laboratory of Soft Soils
7 and Geoenvironmental Engineering, Zhejiang University, China
8
9 2“100-TalentsProgram” Professor, Institute of Geotechnical Engineering, College of Civil
10 Engineering and Architecture, Zhejiang University, Hangzhou, China.
11 E-mail: batebate@zju.edu.cn (Corresponding author)
12
13
14
15
16 A revised manuscript submitted to
17 Chemosphere
18 Special Issue on
19 Green and Sustainable Land Remediation
20
21 April 5, 2019
22
23
24 'Declarations of interest: none'
1
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25 Emerging Sustainable Technologies for Remediation of Soils and Groundwater in A
26 Municipal Solid Wastes Landfill Site -- A Review
27 Ye, J., Chen, X., Chen, C., Bate, B.*
28 Abstract
29 Remediation of soils and groundwater in a municipal solid wastes (MSW) landfill site
30 emerges as a global challenge to the living environment on earth with significant market
31 potential. Unlike contaminants in an industry or agricultural site, contaminants from MSW
32 landfills are diverse, primarily consisting of chemical oxygen demand (COD), inorganic matter
33 (ammonia-nitrogen, nitrate-nitrogen, total phosphorus) and heavy metals. This renders new
34 challenges to remediation contaminants of different characters altogether. A status quo of
35 existing technologies, including permeable reactive barriers, electrokinetic remediation,
36 microbial remediation, and injection of either solubilizing agents or micro or nanobubbles were
37 thoroughly reviewed, with an emphasis on removal efficiency based on existing projects at lab,
38 pilot or field scales. A design chart tailored for the remediation of a landfill contaminated site
39 was developed, verified by a few case studies, which supplement the chart. Future trends of
40 technical innovation (such as multi-layer permeable reactive barriers (PRBs)) and challenges
41 (such as flow pattern) were identified.
42 Introduction
43 Soil and groundwater pollution are a global challenge. More than 5 million contaminated
44 sites need to be remediated, among which 20 million hectares of sites are contaminated by heavy
45 metals (Wuana and Okieimen, 2011). Many municipal solid waste (MSW) landfills are either
46 historically unregulated (unlined), poorly constructed, or aged, which makes them a major source
47 of pollution. Due to degradation of wastes, microbial metabolism, rainfall, and groundwater
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48 intrusion in landfills, leachate is generated, but is often not contained, diverted, collected, or
49 treated. This leads to contamination of the soil, groundwater, air and the vadose zone
50 surrounding landfills (Liu et al. 2018). Such negligence subsequently poses severe risks to
51 human health (sometimes even carcinogenic, leukemic, or leading to abortion), and to agriculture
52 and the ecological system.
53 Such risks have raised increasing worldwide attention over the past decades and have given
54 rise to a booming global market for site remediation. In China, 1.01 million square kilometers of
55 sites exceed environmental quality standard for soils (GB15618-1995) (MEP-PRC and
56 MLR-PRC, 2014). Moreover, about 1600 MSW landfills and 27000 simple landfills are prone to
57 leachate leakage (MHURD-PRC, 2018); Among the 188 solid waste landfills surveyed (1351
58 survey sites), 21.3% exceeded the GB15618-1995 standard (MEP-PRC and MLR-PRC, 2014).
59 The Forward Industrial Research Institute (Qin et al., 2018) predicted that Chinese market of
60 contaminated sites remediation reached 682.1 billion Chinese yuan, among which 21.6 billion
61 Chinese yuan was for solid waste landfills. Europe had identified 80,000 contaminated sites by
62 2007 (EEA, 2007) and 2.5 million potentially contaminated sites (PCS) by 2013, among which
63 38% were caused by MSW landfills (Panagos et al., 2013). The remediation market was
64 estimated to be 6 billion Euro annually (Panagos et al., 2013). In United States, it was estimated
65 that about 294,000 contaminated sites require treatment from 2004 to 2033, which will cost 209
66 billion USD (USEPA, 2004) and cost a total of 650 billion USD is expected in the next 30-35
67 years (Naidu and Birke, 2014). Australia has more than 50,000 confirmed contaminated sites and
68 160,000 PCS. The annual treatment cost is estimated to exceed 3 billion USD (He et al., 2015;
69 Naidu and Birke, 2014). Japan has over 500,000 PCS, and their annual treatment cost is about 3
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70 billion USD by 2010 (Naidu and Birke, 2014). A summary of the worldwide status quo of
71 contaminated sites and the remediation market is summarized in Table 1.
72 Table 1 Status quo of global polluted sites and remediation markets
Identified and potential Value of Current Future Market

Country Reference
contaminated sites Market Potential
>5 million sites, 20 million ha of land are Wuana and Okieimen
Globally - -
contaminated by heavy metal (2011)
*MEP-PRC and
1.01 million square kilometers of soil $101.6 billion Unassessed MLR-PRC. (2014);
China Qin et al. (2018)
1600 MSW landfills and 27000 simple
- - *MHURD-PRC (2018)
landfills
>80000 pollution sites - - He et al. (2015)
Europe 342,000 identified contaminated areas
$6.7 billion annually - Panagos et al. (2013)
and 2.5 million PCS*
209 billion USD
United 294000 contaminated sites (including
- from 2004 to *US EPA (2004)
States identified sites and PCS)
2033
>50000 pollution sites - - He et al. (2015)
Australia >$3 billion per
160,000 PCS Unassessed Naidu and Birke (2014)
annum
$1.2 billion+, Estimated to grow
Japan 500,000+ PCS timeframe to $3 billion by Naidu and Birke (2014)
unspecified 2010
Brazil 5942 identified contaminated areas - - Thomé et al. (2018)
73 *MEP-PRC, Ministry of Environmental Protection of the People’s Republic of China; MLR-PRC, Ministry of Land and
74 Resources of the People’s Republic of China; MHURD-PRC, Ministry of Housing and Urban-Rural Development-People’s
75 Republic of China; PCS, potentially contaminated sites; US EPA (U.S. Environmental Protection Agency)
76
77 The complicated and spatiotemporally heterogeneous contaminants from MSW landfill
78 leachates can be grouped into four major categories, namely, dissolved organic matter
79 (quantified by COD), inorganic contaminants (including ammonium-nitrogen, nitrate-nitrogen,
80 total phosphorus), heavy metals (Fe2+, Mn2+, Cd2+, Cr (VI), Cu2+, Pb2+, Ni2+ and Zn2+), and the
81 broad range of xenobiotic organic compounds (Kjeldsen et al., 2002; Han et al., 2016).
82 Features of young MSW landfills leachate (< 10 years old) differ from old MSW landfills
83 (Renou et al., 2008). The young landfills are divided into two phases: aerobic degradation of
84 microorganisms (typically short duration) and anaerobic degradation of microorganisms (acid
85 production); while an old landfill is divided into two phases: the methanogenic phase (microbial
86 anaerobic degradation) and the stabilization phase (Kjeldsen et al., 2002; Renou et al., 2008).
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87 Generally, pH value increases and the COD concentration decreases while the ammonia
88 concentration usually does not decrease in the leachate as landfill ages, which is the long-term
89 contaminant component in the leachate (Kjeldsen et al., 2002). Metal solubility decreases as pH
90 increases, so the concentration of heavy metals is generally very low for old landfills (Ehrig,
91 1983; Kjeldsen et al., 2002; Kulikowska and Klimiuk, 2008). On the other hand, concentrations
92 of total phosphorus, calcium, magnesium, heavy metal, BTEX are influenced by season of the
93 year, rather than landfill age (Kulikowska and Klimiuk, 2008).
94 Features of the leachate components from six countries or regions are summarized in Fig. 1,
95 which provide the following information: 1) Concentrations of COD and inorganic pollutants in
96 leachates are high, while the concentration of heavy metals is generally low (expect in Beijing).
97 2) The COD concentration of the new landfill is much higher than that of the old landfill.
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98
99 Figure 1. Statistics on chemical characteristics of landfill leachate from selected countries and
100 regions. All landfills are old landfills, except for those in Hong Kong SAR (young landfills) and
101 in Beijing (including both young and old landfills). The height of the histogram represents the
102 average concentration value, and the upper and lower points correspond to the maximum and
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103 minimum concentration values, respectively. Note: the primary and secondary ordinates are
104 logarithmic coordinates.
105 The objective of this paper is to identify existing technologies that are suitable for
106 sustainable remediation of solid waste sites, to provide guidance for future work, and to identify
107 challenges. In the following sections, Part 1 summarizes existing and emerging remediation
108 methods for landfills contaminated sites; Part 2 provides a design chart, which suggests the
109 proper remediation technology for a specific hydrogeological condition, and a few case studies
110 as examples; Part 3 identifies challenges to sustainable remediation methods. Then a summary is
111 given. The layout of the content is as follows:
112 Part 1. Remediation Technologies for Contaminated MSW Sites
113 1.1. Permeable reactive barrier (PRB)
114 1.2. Electrokinetic (EK) Remediation
115 1.2.1. EK+PRB
116 1.2.2. BioEK
117 1.3. Microbial Remediation
118 1.4. In-Situ Injection Treatment
119 1.4.1. Nano zero-valent iron
120 1.4.2. Micro and nanobubble
121 1.5 Phytoremediation
122 Part 2. Design chart for sustainable remediation and Case studies
123 Part 3. Challenges
124 3.1. Flow pattern
125 3.2. Multi-layer PRB
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126 Part 4. Summary
127 Part 1. Remediation Technologies for Contaminated MSW Sites
128 Several remediation technologies have been developed over the past decades to remediate
129 soil and groundwater contaminated by practices of chemical engineering, petroleum engineering,
130 agriculture or mining operations. These remediation technologies include permeable reactive
131 barriers (PRBs), electrokinetic (EK) technology, biologically enhanced degradation, solubilizing
132 agents, micro bubbles, and nanobubbles. A detailed examination of these technologies is
133 provided below, which can be used to assist in identifying techniques suitable for sustainable
134 remediation of contaminated municipal solid waste sites.
135 1.1. Permeable Reactive Barrier
136 A permeable reactive barrier (PRB), as defined by the U.S. Environmental Protection
137 Agency (US EPA, 1998; Powell et al., 1998), is “an emplacement of reactive materials in the
138 subsurface designed to intercept a contaminant plume, provide a flow path through the reactive
139 media, and transform the contaminant(s) into environmentally acceptable forms to attain
140 remediation concentration goals down gradient of the barrier.” Approximately 200 PRB
141 applications were constructed in Europe, North American and Australia from 1994 to 2005,
142 among which 120 were zero valence iron-based (with 83 applications in full-scale) (ITRC, 2005;
143 Gillham et al., 2010; Liu et al., 2015). The annual number of published articles on PRB increases
144 steadily from 2000 to 2018 (Fig. 2). In China, most PRB research is still at lab scale, with a few
145 pilot PRB applications reported in Shenyang (Hou et al., 2014; Li et al., 2014), Baotou, Jiaozuo
146 and Changsha.
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147
148 Figure 2. Number of articles under the topic of “permeable reactive barrier” and “zero valence
149 iron permeable reactive barrier” from 2000 to 2018 (Data retrieved from Web of Science)
150
151 Commonly-used reactive materials in a PRB are zero valence iron, activated carbon and
152 zeolite, while other reactive materials include steel slag, scrap rubber, sponge iron, and medical
153 stone (Tables 2-5). Reversible absorption and irreversible redox reaction are the primary
154 remediation mechanisms in a PRB (Lu et al., 2005). Replacement of the reactive medium is
155 required at intervals to counter performance degradation, saturation, or depletion of materials.
156 Most existing PRBs contain only one type of reactive material, which also targets removing
157 contaminants of the same group (such as those leaked from a gas station). Recently, multi-layer
158 PRB has been the research focus for remediation of complex contaminants in solid waste
159 landfills and in wastes from pharmaceutical industries. (Yang et al., 2013; Pawluk and Fronczyk,
160 2015; Poloński et al., 2017; Kumarasinghe et al., 2018; Pawluk et al., 2019).
161 The efficiencies of PRB reactive materials on removing COD, ammonia nitrogen,
162 nitrate-nitrogen, total phosphorus and heavy metals from different studies are summarized in
163 Tables 2-6 and analyzed as follows.
164 The removal rate of COD in contaminated water of a landfill ranges from 44.3% to 90%
165 (Table 2), with the highest removal rate (90%) obtained with reactive materials of a mixture of
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166 activated carbon and zero valence iron (Dong et al., 2003). Other notable reactive materials for
167 COD removal are a mixture of anthracite, steel slag, and zeolite (85.78% removal efficiency via
168 adsorption by intermolecular force) (Di et al., 2013b), and clinoptilolite (84% removal efficiency
169 via adsorption by the strong dispersive force and electrostatic attraction of the surface) (Song et
170 al., 2011).
10
171 Table 2 Removal rates of COD
Initial
Removal
Removal Condition of Type of concentration Removal
Remover Contaminant efficiency Reference
mechanism removal experiment of time
(%)
contaminant
pump rate 0.8

waste landfill
filtration and mL/min; Chung et
Atomized slag leachate in column 642 mg/L 40
absorption 10 pore al. (2007)
Korea
volumes
Colloidal
Laboratory particles
prepared 0.5g/200mL,
chemical Jiao et al.
Waste rubber groundwater oscillation lab 250 mg/L 44.3 36h
adsorption (2016)
contaminated frequency
by leachate 150 r/min，
pH7
Landfill
different ratios chemical leachate from flow rate 0.5 Zhou et
column 108.72 mg/L 55.8 576h
of ZVI/Zeo/AC adsorption Guangdong, mL/min al. (2014)
China
strong
adsorption electrical
capacity and 40-year-old conductivity
van
contains Belgian 51±4 mS/cm, 389±36 mg
Clinoptilolite column 51-72 127d Nooten et
exchangeable landfill (1967) flow rate N/L
al. (2008)
cations with leachate 10mL 0.16-1.05
ion exchange m/d
characteristics
Laboratory
high porosity prepared
Steel slag and flow rate Di et al.
and adsorption groundwater column 250 mg/L 61.2 48d
zeolite 40-100 cm/d (2014)
capacity contaminated
by leachate
11
Laboratory
prepared flow rate
chemical Di et al.
Waste rubber groundwater 0.45-0.85 column 250 mg/L 73.2
adsorption (2013a)
contaminated m/d
by leachate
Anaerobic
absorb the old-fashioned stirred at a
Bentonite and
complex garbage speed of 200
activated
components of simulation r/min, stirred Ji et al.
carbon (3%) batch 1100 mg/L 77.3 3h
various column for for 2 h, and (2012)
sample/solution
organic leachate let stand for 1
ratio=3g/50ml
molecules recirculation h
treatment
Leachate from
quartz 34.78%,
high porosity Shibeiling
ZVI 43.48% Dong et
and adsorption Landfill, lab 1027.1 mg/L 80.5
and zeolite al. (2009)
capacity Changchun,
21.74%
China
(1) zeolite (2)
ceramsite (3)
activated
Landfill
carbon (4) fly
Leachate
ash (5) Fe0 reduction;
diluted 45 flow rate Cui et al.
anthracite (6) adsorption; column 42.70 mg/L 82.22-88.11 40d
times 80-150 cm/d (2010)
80% slag and biodegradation
(Shijiazhuang,
20% ZVI (7)
China)
80% activated
carbon and 20%
ZVI
12
(1) zeolite (2)
ceramsite (3)
Landfill
activated
Leachate
carbon (4) slag Fe0 reduction;
diluted 50 flow rate Cui et al.
50% and ZVI adsorption; column 45.5 mg/L 82.36-88.17 65d
times 90-150 cm/d (2010)
50% (5) 50% biodegradation
(Shijiazhuang,
activated
China)
carbon and 50%
ZVI
strong
adsorption and
pH8,
contains
Clinoptilolite Pig farm hydraulic Song et
exchangeable column 1011 mg/L 84 24h
(SiO4/AlO4) wastewater load 375 al. (2011)
cations with
mL/h
ion exchange
characteristics
1-4 sand box:
8h，
average flow
(1) steel slag rate 0.76L/h,
(2) zeolite (3) hydraulic
anthracite (4) load 0.0704
steel slag, Coal mine pit m3/(m2d);
zeolite, high porosity water from 16h, average
Di et al.
anthracite and adsorption Inner flow rate lab 15 mg /L 85.78
(2013b)
mixed filler (5) capacity Mongolia, 0.38L/h;
steel slag, China 5 sand box:
zeolite, 8h, average
anthracite flow rate 0.86
combined filler L/h,
hydraulic
load 0.239
m3/(m2d)
13
(1) sand 40%
and ZVI 60%;
Leachate
(2) sand
formed by
34.78%, ZVI
Fe0 reduction; soaking seepage
43.48% and 90 Dong et
adsorption; garbage velocity column 1000.6 mg/L
activated （80,90,70） al. (2003)
biodegradation (Shibeiling, 45-85 cm/d
carbon 21.74%;
Changchun,
(3) sand 40%,
China)
ZVI 40% and
zeolite 20%;
172
173
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174 Removal rate of ammonia nitrogen ranges from 70.8% to 99% (Table. 3). In the laboratory,
175 a mixture of zeolite and zero-valence iron yielded the highest removal rate of 97.4% (Dong et al.,
176 2009). Zeolite adsorbs NH4+ ― N, while ZVI react with NH4+ ― N by redox reaction. Other
177 notable reactive materials for NH4+ ― N removal include clinoptilolite (96% removal efficiency
178 via the strong dispersive force and electrostatic attraction of the surface) (Song et al., 2011), and
179 mixtures of zero-valence iron, zeolite and activated carbon at different proportions (89.2%
180 removal efficiency via adsorption by intermolecular force) (Zhou et al., 2014).
181
15
182 Table 3 Removal rate of ammonia-nitrogen
Initial
Removal
Removal Condition of Type of concentration Removal
Remover Contaminant efficiency reference
mechanism removal experiment of time
(%)
contaminant
Landfill
ZVI/Zeolite/AC leachate Zhou et
chemical flow rate 0.5 TN
at different from column 70.8 al.
adsorption mL/min 35.47mg/L
ratios Guangdong, (2014)
China
(1) sand 40%
and ZVI 60%;
Leachate
(2) sand
formed by
34.78%, ZVI
Fe0 reduction; soaking Dong et
43.48% and seepage velocity
adsorption; garbage column 45.41mg/L 78-91 al.
activated 45-85 cm/d
biodegradation (Shishiling, (2003)
carbon 21.74%;
Changchun,
(3) sand 40%,
China)
ZVI 40% and
zeolite 20%
Leachate
(1) quartz sand
formed by
44.4% and
Fe0 reduction; soaking Dong et
ZVI55.6%; (2) flow rate 70-80
adsorption; garbage lab 60.35mg/L 85 al.
quartz sand cm/d
biodegradation (Shishiling, (2004)
75% and ORC
Changchun,
25%
China)
16
1st-4th sand box：
(1) steel slag 8h, average flow
(2) zeolite (3) rate 0.76L/h，
anthracite (4) hydraulic load
steel slag, Coal mine 0.0704m3/(m2d);
zeolite, high porosity pit water, 16h，average Di et al.
anthracite and adsorption Inner flow rate lab 200 mg /L 88.8
(2013b)
mixed filler (5) capacity Mongolia, 0.38L/h;
steel slag, China 5th sand box;
zeolite, 8h, average flow
anthracite rate 0.86 L/h,
combined filler hydraulic load
0.239 m3/(m2d)
Landfill
ZVI/Zeolite/AC leachate Zhou et
chemical flow rate 0.5
mixtures at from column 29.77mg/L 89.2 al.
adsorption mL/min
different ratio Guangdong, (2014)
China
The particle
size, dosage and
oscillation
frequency of
high porosity Laboratory
Steel slag and zeolite and steel Di et al.
and adsorption prepared batch 50mg/L 91.7 2h
zeolite slag are: (2013c)
capacity wastewater
0.297~0.595
mm, 10
g/100mL, 150
r/min
strong
adsorption and
contains Song et
Clinoptilolite Pig farm pH8, hydraulic
exchangeable column 700 mg/L 96 24h al.
(SiO4/AlO4) wastewater load 375 mL/h
cations with (2011)
ion exchange
characteristics
17
Laboratory
high porosity
Steel slag and prepared flow rate 40 Di et al.
and adsorption column 25 mg/L 96.3 48d
zeolite contaminated -100 cm/d (2014)
capacity
groundwater
Leachate
quartz 34.78%, from
high porosity Dong et
ZVI 43.48% Shibeiling
and adsorption lab 60.4 mg/L 97.4 al.
and zeolite Landfill,
capacity (2009)
21.74% Changchun,
China
strong
adsorption
capacity and
Huang et
contains Synthesized flow rate 15 5.29-10.80
Clinoptilolite pilot-scale 99 al.
exchangeable groundwater mL/min mg/L
(2015)
cations with
ion exchange
characteristics
the Hun hydraulic Hou et

sorption and
zeolite River in conductivity 7× pilot-scale 2-10mg/L 90 al.
ion exchange
Shenyang 10-3 m/s (2014)
sequential River water

nitrification, from Hun
0.3-36.6 Li et al.
zeolite adsorption, River, flow rate 1 m/d pilot-scale 90 382d
mg/L (2014)
and Shenyang,
denitrification China
183
184
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185 Removal rate of nitrate-nitrogen, primarily obtained at lab scale, ranges from 76.1% to
186 99.87% (Table 4). The highest removal rate of NO3― ― N (99.87%) was achieved by loading
187 modified nano-iron onto activated carbon to constitute SM-nano iron/carbon, which both
188 enhanced adsorption onto AC and expanded the reaction area of nZVI (due to its attachment onto
189 the AC surface) (Gao et al., 2016). Other effective reactive materials for nitrate-nitrogen removal
190 are the combination of sponge iron and activated carbon (94.4% removal efficiency via
191 adsorption) (Zhu et al., 2017) and the combination of medical stone (adsorption) and iron filings
192 (97.34% removal efficiency via adsorption and chemical denitrification) (Di et al., 2016).
193
194
195
196
197
19
198 Table 4 Removal rate of nitrate-nitrogen
Initial
Removal
Condition of Type of concentration Removal
Remover Removal mechanism Contaminant efficiency reference
removal experiment of time
(%)
contaminant
(1) sand 40% and
ZVI 60%; (2) sand
Leachate from
34.78%, ZVI
Fe0 reduction; Shibeiling hydraulic Dong et
43.48% and
adsorption; Landfill, conductivity column 48.24mg/L 85 al.
activated carbon
biodegradation Changchun, 45-85 cm/d (2003)
21.74%; (3) sand
China
40%, ZVI 40% and
zeolite 20%
(1) ZVI+ medium
coarse sand (2)
AC+ medium
coarse sand (3)
sawdust + medium Laboratory
coarse sand (4) preparation of Liu et al.
Adsorption column 80 mg/L 76.1 10d
ZVI + AC + groundwater (2017)
medium coarse contaminated
sand (3:1:6) (5)
ZVI + sawdust +
medium coarse
sand
13 groups of tests,
sawdust + iron Laboratory
Wang et
powder > sawdust preparation of
column 80 al.
after composting > groundwater
(2008)
sawdust > iron contaminated
powder
(1) quartz sand Leachate from
44.4% and Fe0 reduction; Shibeiling hydraulic Dong et
ZVI55.6%; adsorption; Landfill, conductivity lab 48.24mg/L 80 al.
(2) quartz sand biodegradation Changchun, 70-80 cm/d (2004)
75% and ORC China
20
25%
Fe0 reduction; Rotating speed Li et al.
nZVI 0.5g lab 125 mg/L 90
adsorption 250 r/min (2006)
Laboratory
Straw compost Yang et
prepared T = 25C, pH= 7～
humus soil: fine Anaerobic respiration lab 150 mg /L 91.8 15d al.
contaminated 8
sand 1:10 or 1:50 (2016)
groundwater
Laboratory
Tang et
n-ZVI and carbon preparation of Stirring speed 500
Adsorption lab 60 mg/L 94.3 al.
composite 5:2 groundwater r/min
(2016)
contaminated
After the reaction,
(1) sponge iron (2)
many oxides and
sponge iron + AC
hydroxides were
single layer
formed on the surface
medium 1:1 (3)
of the sponge iron, Laboratory
sponge iron + AC Zhu et
and the micropores prepared 91.1，94.4，
+ Zeo single layer flow rate 2.6 cm/h column 30 mg/L 8d al.
were severely contaminated 87.9，91.0
medium 1:1:1 (4) (2017)
blocked, which groundwater
sponge iron +
hindered the further
AC1:1 mixing and
reaction of the sponge
Zeo double layer
iron with NO-3-N.
media 2:1
Oxidation
0.15-0.42 mm simulate Meng et
Fe0 reduction; pH6.9-7.1, flow
ZVI+0.15 mm contaminated lab 20 mg /L 95 al.
adsorption rate 50-80 cm/d
AC1:1 groundwater (2012)
Medical stone adsorbs
Laboratory
and the role of Iron
Medical stone, iron prepared Flow rate 0.18 Di et al.
filings are adsorption column 20 mg /L 97.3 40d
filings contaminated L/d (2016)
and chemical
groundwater
denitrification
Laboratory
Modified nano Gao et
prepared flow rate
iron/carbon 5:2 Adsorption column 40 mg/mL 99.9 100min al.
contaminated 1mL/min, pH7
(1.5g) (2016)
groundwater
21
using cotton as a
Laboratory
cotton as carbon carbon source and
prepared Jin et al.
source and reaction reaction medium to T = 25±1C lab 22.6 mg /L 100
contaminated (2004)
medium remove nitrate from
groundwater
groundwater
reactors were
sealed with
siliconlined,
gray-butyl septa,
acid-washed waste convert NO3- to NO2-, leachate and aluminum Oh et al.
batch 10 mg/L 100 7h
steel scrap NH3, and NH4+ simulant crimps. Reactors (2007)
were shaken on a
reciprocating
shaker (150 rpm,
25C)
199
200
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201 Relatively few studies have been conducted on total phosphorus (TP) contaminants (Table
202 5). The notable reactive materials for nitrate-nitrogen removal are a combined packing of
203 anthracite, steel slag, and zeolite (96.08% removal efficiency via adsorption by intermolecular
204 force) (Di et al., 2013b), and clinoptilolite (97% removal efficiency via adsorption) (Song et al.,
205 2011). Other reactive materials reported for removing total phosphorus include acid-treated basic
206 oxygen furnace slag (98% removal efficiency via adsorption and chemical precipitation for
207 PO43-(Xue et al., 2009) and modified steel slag (99% removal efficiency via chemical
208 precipitation and ligand exchange) (Duan et al., 2012).
209
210
211
212
213
23
214 Table 5 The removal rate of total phosphorus
Initial
Removal
Removal Type of concentration Removal
Remover Contaminant Condition of removal efficiency Reference
mechanism experiment of time
(%)
contaminant
1st-4th sand box: 8h,

average flow rate
(1) steel slag (2)
0.76 L/h, hydraulic
zeolite (3) anthracite
Coal mine load 0.0704
(4) steel slag,
pit water, m3/(m2d); 16h,
zeolite, anthracite high porosity and Di et al.
Inner average flow rate lab 50 mg /L 96.1
mixed filler (5) steel adsorption capacity (2013b)
Mongolia, 0.38 L/h;
slag, zeolite,
China 5th sand box: 8h,
anthracite combined
average flow rate
filler
0.86 L/h, hydraulic
load 0.239 m3/(m2d)
strong adsorption
and contains
Clinoptilolite exchangeable Pig farm pH8, hydraulic load Song et
column 50 mg/L 97 24h
(SiO4/AlO4) cations with ion wastewater 375 mL/h al. (2011)
exchange
characteristics
24
chemical and
geometrical
heterogeneities;
abundant calcium
and aluminum ions synthesized
aid treated Basic Xue et al.
which enhance the Artificial pH=7.0-7.2, 20C batch 10 mg/L 98 1h
oxygen furnace slag (2009)
processes of wastewater
adsorption and
chemical
precipitation for
PO43-
Modified steel slag

obtained by mixing
steel slag and Chemical Laboratory
Duan et
aluminum hydroxide precipitation and prepared pH=4-8, 30C batch 2 mg/L 99 2h
al. (2012)
in a mass ratio of ligand exchange wastewater
4:3 and calcined at
700°C for 2 h
reacted (formation
reactors were sealed
of precipitate) with
with siliconlined,
metal cations (Al3+,
gray-butyl septa, and
Fe2+, Fe3+, Ca2+
leachate aluminum crimps. Oh et al.
Converter slag etc.), which are batch 10 mg/L 100 20min
simulant Reactors were shaken (2007)
common
on a reciprocating
components of
shaker (150 rpm,
converter slag in
25C)
solution
215
25
ACCEPTED MANUSCRIPT
216
217 The removal rates of heavy metals are usually high, exceeding 95% in many instances
218 (Table 6). Steel slag and zeolite were used to remove iron from leachate-contaminated
219 groundwater at a removal rate of 99.8% (Di et al., 2014). ZVI and zeolite were used to remove
220 Mn, Zn, Cd and Cr(VI) in leachate from the Shibeiling Landfill, Changchun, China with removal
221 rates of 99.6%, 97.2%, 95.2% and 70.7%, respectively (Dong et al., 2009). Acid-washed
222 ZVI/ZVAl was used to remove Cr(VI), Zn and Ni in heavy metal wastewater with a removal rate
223 of 99% (Han et al., 2016). Pumice, perlite and lime were also used to remove Pb with a removal
224 rate of 99% (Ranjbar et al., 2017).
225
226
227
228
229
230
231
232
233
234
26
235 Table 6 Removal rates of heavy metals
Initial
Remo Re
concent
Type of val mo
Condition of ration
Remover Removal mechanism Contaminant experim efficie val Reference
removal of
ent ncy tim
contam
(%) e
inant
Laboratory prepared
flow rate 50 Di et al.
Waste rubber chemical adsorption contaminated column 95.2 30d
0.45~0.85 m/d mg/L (2013a)
groundwater
Colloidal particles
Laboratory prepared 0.5g/200mL,
50 Jiao et al.
Waste rubber chemical adsorption contaminated oscillation lab 96.2 36h
mg/L (2016)
groundwater frequency 150
r/min，pH7
The particle size,
Fe dosage and
oscillation
frequency of
Steel slag and high porosity and Laboratory prepared 40 Di et al.
zeolite and steel batch 98.5 2h
zeolite adsorption capacity wastewater mg/L (2013c)
slag are:
0.297~0.595 mm,
10 g/100mL, 150
r/min.
Laboratory prepared
Steel slag and high porosity and flow rate 40-100 40 Di et al.
contaminated column 99.8 48d
zeolite adsorption capacity cm/d mg/L (2014)
groundwater
Colloidal particles
Laboratory prepared 0.5g/200mL,
30 Jiao et al.
Mn Waste rubber chemical adsorption contaminated oscillation lab 86.2 36h
mg/L (2016)
groundwater frequency
150r/min，pH7
27
Leachate formed by
sand 40%, ZVI Fe0 reduction;
soaking garbage in seepage velocity 60.89 Dong et al.
40% and zeolite adsorption; column 90
Shishiling, 45-85 cm/d mg/L (2003)
20% biodegradation
Changchun, China
Laboratory prepared
Steel slag and high porosity and flow rate 40-100 30 Di et al.
contaminated column 97.4 48d
zeolite adsorption capacity cm/d mg/L (2014)
groundwater
The particle size,
dosage and
oscillation
frequency of
Steel slag and high porosity and Laboratory prepared 15 Di et al.
zeolite and steel batch 93.1 2h
zeolite adsorption capacity wastewater mg/L (2013c)
slag are:
0.297-0.595 mm,
10 g/100mL, 150
r/min
1st-4th sand box:
8h, average flow
(1) steel slag (2) rate 0.76L/h,
zeolite (3) hydraulic load
anthracite (4) steel 0.0704 m3/(m2d);
slag, zeolite, high porosity and Inner Mongolia coal 16h, average flow 1.5 Di et al.
lab 98.98
anthracite mixed adsorption capacity mine pit water rate 0.38L/h; mg/L (2013b)
filler (5) steel slag, 5th sand box: 8h,
zeolite, anthracite average flow rate
combined filler 0.86 L/h, hydraulic
load 0.239
m3/(m2d)
quartz 34.78%, Leachate from
high porosity and 13.8 Dong et al.
ZVI 43.48% and Shibeiling Landfill, lab 99.6
adsorption capacity mg/L (2009)
zeolite 21.74% Changchun, China
Leachate formed by
sand 40%, ZVI Fe0 reduction;
soaking garbage in seepage velocity 70.35 Dong et al.
Zn 40% and zeolite adsorption; column 80
Shishiling, 45-85cm/d mg/L (2003)
20%; biodegradation
Changchun, China
28
Calcite was used to
calcite, vegetal raise pH and Groundwater
hydraulic
compost and precipitate contaminated with 15 Gibert et al.
conductivity: field 95
sewage sludge and metals as acid mine drainage, mg/L (2013)
10-400 m/day
Fe0 (oxy)hydroxides and Spain
carbonates
reactors were
sealed with
siliconlined,
adsorption of heavy
gray-butyl septa,
metals by iron oxide
acid-washed waste and aluminum 10.2 Oh et al.
on the acid-washed Leachate simulant 98 6h
steel scrap crimps. Reactors mg/L (2007)
waste steel scrap
were shaken on a
surface
reciprocating
shaker (150 rpm,
25C)
aluminum is an
effective electron
acid-washed
donor, acting wastewater containing pH=5.4; flow 20 300 Han et al.
ZVI/ZVAl=80 column 99.5
as a strong reductant heavy metal rates=1.0 mL/min mg/L h (2016)
g/40 g
to remove heavy
metal ions
Medical stone
adsorbs and the role
Laboratory prepared KCr2O7
Medical stone, of Iron filings are Di et al.
contaminated flow rate 0.18 L/d column 10 97.7 40d
Iron filings adsorption and (2016)
groundwater mg/L
chemical
Cr denitrification
(VI) 0.15-0.42mm ZVI Fe0 reduction; Contaminated pH 6.9-7.1, flow 10 Meng et al.
lab 96
+ 0.15mm AC1:1 adsorption groundwater simulant rate 50-80 cm/d mg/L (2013)
29
13X zeolite and 50 Silva et al.
adsorption 78.2
vermiculite mg/L (2017)
Medical stone
adsorbs and the role
Laboratory prepared
Medical stone, of Iron filings are 10 Di et al.
contaminated flow rate 0.18 L/d column 97.7 40d
Iron filings adsorption and mg/L (2016)
groundwater
chemical
denitrification
aluminum is an
effective electron
acid-washed
g/40 g
to remove heavy
metal ions
adsorption (van der
Waals force,
Adding hexavalent
Sulfuric acid chemical bond force, Huang et al.
chromium to pH=2, 25C batch 5 mg/L 99 3h
modified fly ash hydrogen bond force (2012)
groundwater
and electrostatic
attraction)
ZVI/Zeolite/AC at Landfill leachate from flow rate 0.015 576 Zhou et al.
chemical adsorption column 70.7
different ratios Guangdong, China 0.5mL/min mg/L h (2014)
ZVI/Pumice flow rate 0.5 324 Calabrò et

column 5 mg/L
granular cm³/min 99.9 0h al. (2012)
aluminum is an
Ni effective electron
acid-washed
g/40 g
to remove heavy
metal ions
(1) ZVI 240g (2) Benchm
flow velocity 50 Madaffari et
lapillus 1289g (3) ark 99
0.4m/d mg/L al. (2017)
ZVI+lapillus column
30
aluminum is an
effective electron
acid-washed
g/40 g
Cd to remove heavy
metal ions
ZVI/Zeolite/AC at Landfill leachate from flow rate 0.5 0.006 576 Zhou et al.
chemical adsorption column 92.7
different ratios Guangdong, China mL/min mg/L h (2014)
Pb
pumice, perlite and flow rate 2.4 200 Ranjbar et
adsorption 99.9 50d
lime2:1:2 mL/min mg/L al. (2017)
236
31
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237 1.2. Electrokinetic Remediation
238 Electrokinetic (EK) remediation, a technology of running electrical current through pairs of
239 electrodes across a contaminated soil body to remove heavy metals and organic contaminants,
240 has steadily received growing attention in countries including United States and Korea since the
241 mid-1990s (Fig. 3) (Acar and Alshawabkeh, 1996). Electrokinetic remediation is especially
242 suitable for soils of low permeability and strong adsorption capacity, i.e., clay or silt, where other
243 remediating agents have difficulty reaching the interaggregate space.
244
245 Figure 3. Number of articles under the topic of “electrokinetic” from 2000 to 2018 (Data
246 retrieved from Web of Science)
247
248 The fundamental operating principles of electrokinetic remediation are summarized as
249 follows. Under external electric current, the cathode produces hydroxide ions (4𝐻2𝑂 +4𝑒 ― = 4
250 OH ― + 2𝐻2↑), which then form hydroxide precipitates with heavy metal ions; the anode
251 produces oxygen and free radicals (4OH ― ―4𝑒 ― = 2𝐻2𝑂 + 𝑂2↑), which in theory could oxidize
252 COD and nitrate-nitrogen due to the electrochemically produced strongly oxidizing hydroxyl
253 radicals (Zhang et al., 2001; Virkutyte et al., 2002; Qiao et al., 2004).
32
ACCEPTED MANUSCRIPT
254 However, limited studies have been reported on EK removal of COD and ammonia nitrogen.
255 Li et al. (2016) reported that the removal efficiencies of the EK method for COD and ammonia
256 nitrogen from a landfill leachate are 83.7% and 100%, respectively. More complicated
257 mechanisms were reported: (1) Al3 + ions were released from aluminum cathode, dissolved in
258 the solution, and produced sludges, which had a coagulation effect on COD and ammonia
259 nitrogen, and (2) On Ti/RuO2 ― IrO2 anode, there are direct oxidation (by transferring electrons
260 directly, 4𝐻2𝑂 +4𝑒 ― = 4OH ― + 2𝐻2↑) and indirect oxidation, both of which can remove COD
261 and ammonia nitrogen.
262 The removal efficiency by the EK method depends on many factors, including electrode
263 material, pH, voltage gradient, and current density. Anode materials are usually inert to chemical
264 reactions and high electrical conductivity, including titanium, graphite, platinum, or sometimes
265 sacrifice electrode such as aluminum; while cathode materials are usually corrosive-resistant in
266 basic environments, including aluminum and iron (Alshawabkeh et al., 1999). Mahmad et al.
267 (2015) reported that the highest iron removal efficiencies are 96.81% (pH 5, voltage 2.5V,
268 aluminum electrodes) and 94.3% (pH 4, voltage 2.5V, stainless steel electrodes), respectively.
269 The dissolution of the stainless-steel electrode was postulated to attribute to the slightly lower
270 removal rate. Kim et al. (2011) reported EK-solar cell remediation for a soil contaminated with
271 Cd, Cu, and Pb, and found that the maximal removal efficiencies of Pb and Cd were achieved at
272 90% with addition of 50mM of citric acid.
273 Many innovative techniques were developed over the past decades to improve the removal
274 efficiency of EK. Placing iron-loaded activated carbon in Cr(VI)-contaminated soils improved
275 removal efficiency due to adsorption of Cr(VI) on AC and reduction of Cr(VI) by Fe2 + (Cr6 +
276 + 3Fe2 + +AC→Cr3 + +3Fe3 + +AC). The highest removal efficiency (80.2%) was achieved at
33
ACCEPTED MANUSCRIPT
277 an AC-Fe ratio of 5%, with graphite and stainless-steel plates as the anode and cathode,
278 respectively (Yan et al., 2018). A hexagonal unit cell, with six anodes at corners and one cathode
279 at the center, was constructed to increase the hydroxyl production at the cathode. This enhanced
280 formation of metal hydroxide to remove heavy metals (Liu, 2013). To prevent the precipitates
281 from clogging the pores near the cathode and from depositing directly onto the cathode, the
282 cathode was replaced every 120 h. Average removal efficiencies of Cd (89.9%) and Pb (69.3%)
283 were achieved after 480 h (Liu, 2013) (Table 7). Colantonio et al. (2016) reported that the
284 removal rate of Pb2 + is 83% in the anode chamber, open circuit and 62% in the cathode
285 chamber, open circuit, using lab-scale microbial electrolysis cells (MECs) with an anion
286 exchange membrane (AEM) (Colantonio et al., 2016). Furthermore, alternating electrical field
287 was used to neutralize pH near electrodes, thereby improving the removal efficiencies of metal
288 ions.
289 The electrokinetic (EK) technique was also used in conjunction with other remediation
290 techniques, such as permeable reactive barrier and microbes to further increase efficiency and
291 tackle soil and groundwater with complex contaminants. Wastewater containing both COD and P
292 b2 + was treated with both EK and PRB (Hu, 2013). During the migration of contaminants from
293 anode to cathode under an external electric field, COD was oxidized near the anode, while Pb
294 was precipitated near the cathode and was then adsorbed by PRB. The removal efficiencies of
295 COD and Pb were 57.03% and 81.62% in the anode zone, and were 90.4% and 94.6% in the
296 cathode zone, respectively (Hu, 2013). The molecular sieve, which is commonly composed of
297 zeolite, was installed adjacent to the cathode and can prolong the life of cathode and adsorb
298 heavy metals. Meanwhile a ZVI layer installed near the anode can reduce heavy metals. The
299 combination of the zeolite molecular sieve near the cathode and the ZVI layer near the anode
34
ACCEPTED MANUSCRIPT
300 yielded removal efficiencies for lead, cadmium, nickel and copper of 49.4%, 47.1%, 39.2% and
301 36.7%, respectively (Fu et al.2012). Adikesavan et al. (2018) reported that bioleaching enhanced
302 electrokinetic remediation (BEER) technology improved the removal efficiency of zinc
303 (93.08%), where the anode optimized the pH to produce acidophilic bacteria, and the acidic
304 environment created by acidophilic bacteria increased the solubility of heavy metals attached to
305 the soil, thereby promoting its electromigration.
35
306 Table 7 Removal rate of contaminant using EK
Initial Rem
Type
concentrati oval Rem
of
Removal Electrode types Contaminant Condition of removal on of effici oval Reference
experi
contaminan ency time
ment
t (%)
current density: 0.1
The cathode: Al A/cm2, pH 6.37,
The anode: Ti / landfill leachate, Conductivity 12.05– 3640-4296 150m Li et al.
COD lab 83.93
RuO2-IrO3 Changsha, China 13.08 mS/cm, chloride mg/L in (2016)
Oxidation, precipitation ion concentration 6.5
g/L
current density: 0.1
Amm The cathode: Al A/cm2, pH 6.37,
onia The anode: Ti / landfill leachate, Conductivity 12.05– 1840–2042 150m Li et al.
lab 100
nitro RuO2-IrO3 Changsha, China 13.08 mS/cm, chloride mg/L in (2016)
gen Oxidation, precipitation ion concentration 6.5
g/L
The cathode: Al Mahmad
EK Pulau Burung 60mi
Oxidation, precipitation pH5; 2.5V lab 96.81 et al.
Landfill, Malaysia n
Fe + 2H+→ Fe2+ +H2 (2015)
Fe The cathode: stainless
Mahmad
steel Pulau Burung 60mi
pH4; 2.5V lab 94.3 et al.
Oxidation, precipitation Landfill, Malaysia n
(2015)
Fe + 2H+→ Fe2+ +H2
The cathode: Al Mahmad
Pulau Burung 60mi
Oxidation, precipitation pH3; 2.5V lab . 72.65 et al.
Landfill, Malaysia n
Fe + 2H+→ Fe2+ +H2 (2015)
Cr(Ⅵ) The cathode: stainless
Mahmad
steel Pulau Burung 60mi
lab 88.35 et al.
Oxidation, precipitation Landfill, Malaysia pH7; 2.5V n
(2015)
Fe + 2H+→ Fe2+ +H2
36
Natural saline-sodic Hydraulic
soil, spiked with conductivity 6.91×
contaminant mixture 10−9 cm/s, Electrical Lukman et
EK+GAC lab 75.9 21d
(kerosene, phenol, conductivity 8.62 al. (2013)
Cr, Cd, Cu, Zn, Pb, dS/m, voltage gradient
and Hg) 1 V/cm
the synthetic AC-Fe
particles are in soil 1V/cm; Na2SO4 0.1
Yan et al.
The anode: Graphite plate from industrial site mol/L, Conductivity lab 39.4 mg/L 80.2 10d
(2018)
The cathode: 51.1 mS/cm
Stainless-steel plate
leachate from
The cathode: current density 1A; 1.39 ± 0.42 60mi Rabbani et
Kahrizak landfill, batch 84
precipitation initial pH=7 mg/L n al. (2012)
Tehran, Iran
The anode/The cathode:
Fe/Fe
Pt Ti/Fe Mouedhen
Na2SO4 1 g/L and 1000 60mi
Al / Al lab 100 et al.
NaCl 0.5 g/L mg/mL n
Pt Ti / Al (2009)
The cathode: Aluminum
hydroxide precipitation
Natural saline-sodic
Hydraulic
soil, spiked with
conductivity 6.91×
contaminant mixture
10−9 cm/s, Electrical Lukman et
EK+GAC Adsorption (kerosene, phenol, lab 26.8 21d
conductivity 8.62 al. (2013)
Cr, Cd, Cu, Zn, Pb,
dS/m, voltage gradient
Zn and Hg)
1 V/cm
100mg/kg
Voltage gradient
The anode andtThe Artificial soil (60%
1.5(v/cm), Saberi et
cathode were reticular kaolin, 40%sand); lab 18 mg/kg 63 15d
Brij35 1%, EDTA al. (2018)
stainless steel Kaolin
0.1M, Na2SO4 0.1M
37
Electrolyte refreshed
at a rate of 40 rpm,
Two square titanium Zhou et al.
red soil the catholyte pH was lab 265 mg/kg 65 554h
alloy electrodes (2005)
controlled by lactic
acid and CaCl2
Voltage gradient
The anode and The Artificial soil (60%
1.5(v/cm), Saberi et
cathode were reticular kaolin, 40%sand); lab 33 mg/kg 54 15d
Brij35 1%, EDTA al. (2018)
stainless steel Kaolin
0.1M, Na2SO4 0.1M
soil, spiked with conductivity 6.91 ×
contaminant mixture 10-9 cm/s
Lukman et
EK+GAC (kerosene, phenol, Electrical conductivity lab 55.8 21d
al. (2013)
Cr, Cd, Cu, Zn, Pb, 8.62 dS/m
and Hg) voltage gradient 1
100mg/kg V/cm
Acar and
pilot 109.3 2950
EK kaolinite 133 μA/cm2 0.55 Alshawab
scale mg/kg h
keh (1996)
Pb Anode (oxidation) Fe --> the electrical current
Fe2++ 2e- ratio between reacting
Cathode (reduction) surface area Thaveema
landfill leachate
2H2O + 2e- —>H2 + volume of reactor batch 30 mg/L 99 itree et al.
samples (Thailand)
2OH- operation time (2003)
Fe + 2H2O —> Fe(OH)2 following a first-order
+ H2 reaction.
Non-uniform
Electrokinetic
permeable reactive
composite electrode
electrokinetic voltage gradient 1.7 109.2
soil lab 69.3 480h Liu (2013)
(PRCE-EK) remediation V/cm mg/kg
The anode：Graphite
electrode
The cathode：PRCE
38
Hydraulic
Natural saline-sodic
conductivity 6.91 ×
soil, spiked with
10−9 cm/s
contaminant mixture Lukman et
EK+GAC Adsorption Electrical conductivity lab 34.4 21d
(kerosene, phenol, al. (2013)
8.62 dS/m
Cr, Cd, Cu, Zn, Pb,
voltage gradient 1
and Hg)
V/cm
Non-uniform
Cd
electrokinetic
permeable reactive
composite electrode
voltage gradient 108.9
electrokinetic soil lab 89.9 480h Liu (2013)
1.7V/cm mg/kg
(PRCE-EK) remediation
The anode: Graphite
electrode
The cathode: PRCE
Voltage gradient
Artificial soil (60%
anode and cathode were 1.5(v/cm), Saberi et
Ni kaolin, 40%sand); lab 12 mg/kg 57 15d
reticular stainless steel Brij35 1%, EDTA al. (2018)
Kaolin
0.1M, Na2SO4 0.1M
soil, spiked with conductivity 6.91×
contaminant mixture 10−9 cm/s, Electrical Lukman et
EK+GAC Adsorption lab 41 21d
(kerosene, phenol, conductivity 8.62 al. (2013)
Cr, Cd, Cu, Zn, Pb, dS/m, voltage gradient
and Hg) 1 V/cm
Cu Electrolyte refreshed
at a rate of 40 rpm,
Two square titanium Zhou, et
red soil the catholyte pH was lab 318 mg/kg 63 554h
alloy electrodes al. (2005)
controlled by lactic
acid and CaCl2
leachate from
The cathode：Copper current density 1A, 2.28 ± 0.24 60mi Rabbani et
Kahrizak landfill, batch 95
hydroxide precipitation initial pH=7 mg/L n al. (2012)
Tehran, Iran
39
anod
50ml 0.1mol/L KCl
anode: e:
and 10ml 0.05mol/L
COD was oxidized near Laboratory prepared 71.5 mg/L 40.27
COD Citric acid solution, lab Hu (2013)
the anode contaminated soil cathode: catho
voltage gradient
71.9 mg/L de:
0.35V/cm
90.40
Amm current density 10
ammonia is converted to Mao et al.
onia- mA/cm², flow rate 6 lab 20 mg/L 70
nitrogen (2018)
N mL/min
GAC PRB
Two graphite electrodes carbon to sand
Ghaemini
Nitrat were embedded in the synthetic ratios1:1, flow rate 2.3
lab 135 mg/L 90 111h a et al.
e-N soil layer and under the contaminated water L/min, pH = 6.8,
(2018)
reactive media voltage 30V
respectively
the anode: graphite
electrode + zeolite PRL
EK+ voltage gradient 371.0 Fu et al.
the cathode: iron PRL, soil lab 47.1 15d
PRB 1.5V/cm mg/kg (2012)
zeolite PRL + graphite
electrode
Pb anod
50ml 0.1 mol/L KCl
anode: e:
Pb was precipitated near and 10ml 0.05 mol/L
Laboratory prepared 91.8 mg/L 57.84
the cathode and adsorbed Citric acid solution, lab Hu (2013)
contaminated soil anthode: catho
by PRB voltage gradient
93.2 mg/L de:
0.35V/cm
92.6
the anode: graphite
voltage gradient 500.1 Fu et al.
Cd the cathode: iron PRL, soil lab 49.4 15d
1.5V/cm mg/kg (2012)
electrode
the anode: graphite
Ni the cathode: iron PRL, soil lab 39.2 15d
1.5V/cm mg/kg (2012)
electrode
40
the anode: graphite
Cu the cathode: iron PRL, soil lab 36.7 15d
1.5V/cm mg/kg (2012)
electrode
anod
Cathode: reduction
e:
precipitation Colantoni
83
Pb Anode: Graphite Fiber Industrial waste o et al.
catho
Electrode (2016)
de:
Biosorption
62
EK+ 72.86
BIO (BIO
acidophilic bacteria;
),
Bioleaching, inoculum dosage of 96h Adikesava
1000 56.67
Zn electrokinetic (EK) and contaminated sludge the acclimatized lab 96h n et al.
mg/kg (EK),
BEER technology bacterial strain 4%, 72h (2018)
93.08
pH5
(BBE
R)
41
ACCEPTED MANUSCRIPT
308 1.3. Microbial Remediation
309 Microbial remediation of contaminated sites is economical, sustainable, and has a shorter
310 treatment cycle than phytoremediation. Previous studies focus on the remediation of a single type
311 of heavy metals or xenobiotic organic compounds, or a combination of the two (Liu et al., 2015;
312 Jiang et al., 2015; Chen et al., 2015; Mandal et al., 2016; Gong et al., 2018). Few studies have
313 been performed on microbial remediation of contaminated soils or leachate in municipal solid
314 waste landfill sites, which contain complex components (Table 8).
315 Bacteria, fungi, and actinomycetes are commonly used for remediation of contaminated
316 sites (Liu et al., 2015; Pinedo-Rivilla et al., 2009), and have been known to achieve a high
317 degradation efficiency of COD by intracellular/extracellular enzymes and co-metabolism of
318 microorganisms. Under the optimal growth conditions (pH=7, inoculum size 3%, 25 ℃), the
319 cold-tolerant strain, isolated and screened from the activated sludge of the sewage treatment
320 plant, catalyzed a series of biological redox reactions using the dehydrogenase produced by the
321 strain, and removed 78.8% COD (initial concentration of 800 mg/L) after 96 hours (Gao et al.,
322 2015).
323 Microbial remediation techniques for heavy metal removal are relatively mature with high
324 removal rates, including bioaccumulation (precipitating or chelating heavy metal ions on
325 biopolysaccharides, binding contaminants to the extracellular matrix, or electrostatic adsorption),
326 and biotransformation (methylation, demethylation, or redox), with which heavy metals are
327 either passivated or eliminated (Liu et al., 2015; Ye et al., 2017). Akar et al. (2007) utilized
328 biomass, which produced by Aspergillus parasiticus fungi, to remove Pb(II) from wastewater
329 through ion exchange (mainly) and the organic complexation process. At pH=5, 20 °C, and an
42
ACCEPTED MANUSCRIPT
330 initial concentration of 100 mg/dm3 of Pb(II), a removal rate of APG-Biomass (1.6 g/dm3) was
331 reached at 83.98±2.22% after 70 min. The multi-metal resistant endophytic bacteria L14 (EB
332 L14) increased the removal efficiency of heavy metals in wastewater by inhibiting the ATPase
333 (Guo et al., 2010). After 24 h, the removal rates of Cd(II) and Pb(II) at initial concentration of
334 10 mg/L reached 75.78% and 80.48% (Guo et al., 2010). Contaminated soils can also be
335 remediated by microorganisms. Cui et al. (2017) employed a composite microbial agent to repair
336 tailings contaminated soil. After 49 days, 74.98% of the total Zn (C0=73.2 mg/kg), 85.29% of
337 total Pb (C0=13.55 mg/kg), and 79.41% of total Mn (C0=1070 mg/kg) inside the soil were
338 stabilized. P. ostreatus (macro fungi) took straw as a nutrient and adsorbed 81.25% and 68.86%
339 of Pb and Ni from a contaminated soil taken from an MSW landfill site to its fruiting body after
340 22 days (Bharath et al., 2019).
341 Even though the basic elements for microorganism growth can theoretically be consumed
342 via metabolism, nitrogen and phosphorus have rarely been reported as removed microbially from
343 landfills until recently. With 30 g/L of bamboo charcoal-probiotics EM.1 (3%), 89.5% of
344 ammonia-nitrogen with an initial concentration of 387 mg/L, and 68.29% of total phosphorus
345 with an initial concentration of 20.16 mg/L were removed after 48 h (Jiang et al., 2012).
346 Bioremediation efficiency is restricted by the following factors: (1) a microorganism
347 usually can handle only one group of contaminants; (2) the removal efficiency is sensitive to pH
348 and temperature. If pH or the temperature is away from optimal conditions, enzyme activity will
349 be reduced, the spatial structure of microorganisms will be destroyed (Gao et al., 2015), and
350 binding sites and surface charge will be dissociated (Akar et al., 2007), which results in lower
43
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351 removal ability; and (3) sometimes the microbial activity is inhibited by high concentrations of
352 pollution sources.
353 In order to enable bioremediation technology to remove multiple contaminants
354 simultaneously and improve its efficiency, bio-enhancing agents, which increase the
355 biodiversity, supply electron acceptors, and provide sufficient oxygen and nutrient salts (such as
356 carbon-nitrogen and carbon-phosphorous at ratios of 10:1 and 30:1 in Kensa (2011)) were
357 suggested.
44
358 Table 8 Studies of the treatment of contaminants detected in MSW leachate by microorganisms
Description of the
Description of contaminants Description of the remover/removal method
removal effect
Rem
oval
Initial Type Referenc
Rem rate/r
Type of Contaminan conce Dosage of Condition of of es
Remover Removal mechanism oval emov
pollutant t ntrati remover removal exper
time al
on iment
capac
ity
3% 78.8
biological redox reactions
Simulated Inoculum % Gao et
800 cold-tolerant pH=7.0, catalyzed by
domestic dose batch 96h (71.2 al.
mg/L strain 25C microorganism produced
sewage (volume %, (2015)
DHAase
fraction) 4C)
COD/SO42-
=2.0, Maifan stone has good
100ml
1372 sulfate-reduci adequate adsorption capacity,
Simulated SRB, 475
- ng bacteria carbon dissolution properties and colu 46.70 Di et al.
coal mine cm3 54d
COD 1680 (SRB)-maifan supply, porous structure, and mn % (2014)
wastewater maifan
mg/L Stone hydraulic serves as immobilization
Stone
load= 0.1m3 carrier of microorganism
/( m2·d)
Bamboo charcoal serves as
bamboo a microbial immobilization
4494. Jiang et
Biogas probiotics charcoal pH=7.0-8.0, carrier; synergistic effect 66.30
1mg/ batch 48h al.
slurry EM.1 (30g/L)-E DO=2mg/L of bamboo charcoal %
L (2012)
M.1 (3%) adsorption and microbial
degradation.
bamboo
Inor 1167. a microbial immobilization Jiang et
Biogas probiotics charcoal pH=7.0-8.0, 87.29
gani NH3 25 carrier; synergistic effect batch 48h al.
slurry EM.1 (30g/L)-E DO=2mg/L %
c mg/L of bamboo charcoal (2012)
M.1 (3%)
adsorption and microbial
45
degradation.
Leachate
BWF sample/sol Liu and
pretreated 387m 89.50
microbial ution ratio - - batch 7d Zhang
by A/O g/L %
agent = 8g/10L (2016)
process
bamboo a microbial immobilization
Jiang et
Biogas 20.16 probiotics charcoal pH=7.0-8.0, carrier; synergistic effect 68.29
TP batch 48h al.
slurry mg/L EM.1 (30g/L)-E DO=2mg/L of bamboo charcoal %
(2012)
M.1 (3%) adsorption and microbial
degradation.
Soil Pleurotus Heavy metals were 68.86
Ni straw served Bharath
contaminate ostreatus accumulated onto the %
- - as nutrient batch 22d et al.
d with (mushroom fruiting bodies of 81.25
Pb source (2019)
MSW species) mushrooms %
86.89
Zn(II) 1.2ml pH=7, 26C
%
Heavy metal Monolayer-based ion
20 95.46
Pb(II) stock 1.0ml pH=6, 26C exchange and 24h
mg/L %
solution complexation
92.78
Mn(II) 1.0ml pH=6, 28C
%
Hea
73.2 composite (1) Certain specific 74.98
vy Zn Cui et al.
mg/kg microbial enzymes or extracellular batch %
met (2017)
13.55 agent polymers, which can react 85.29
al Pb
mg/kg with heavy metals, were %
Mine
8–12 g/m2 - secreted by the microbes; 49d
tailings soil
(2) Heavy metals were
1070 79.41
Mn combined with organic
mg/kg %
acids (produced in
metabolic process)
citric acid Klebsiella An iron gel (produced by 100.0
Pb Anoxic Baldi et
leached oxytoca strain BAS-10 using residual 0%
- - environment batch 6d al.
liquid from BAS-10 citrate) that co-precipitates 92.00
Cr , 28C (2007)
contaminate isolated from heavy metals %
46
soil sediments 86.00
Fe
from pyrite %
mine tailings 93.00
Cd
%
80.00
Zn
%
79.00
Cu
%
10 multi-metal 75.78
Cd(II)
Heavy metal mg/L resistant % Guo et
restraining the activities of
stock endophytic - 30C batch 24h al.
10 ATPase 80.48
Pb(II) solution bacteria L14 (2010)
mg/L %
(EB L14)
pH=7-8, 5304
10-2
Cu 25±1C, μmol/
M
under g
extracellular
nitrogen 2509 Comte et
Metal stock 10−2 polymeric
Pb 0.45mg atmosphere, - batch - μmol/ al.
solution M substances
KNO3 g (2008)
(EPS)
served as a
10−3 85μm
Cd supporting
M ol/g
electrolyte
Aspergillus
Ion exchange (primarily);
parasiticus 83.98 Akar et
Metal stock 100m complexation of lead ions 70mi
Pb(II) fungal 1.6 g/dm3 pH=5, 20C batch ±2.22 al.
solution g/dm3 with APF functional n
biomass % (2007)
groups
（APF）
359
360
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361 1.4. In-Situ Injection Treatment
362 1.4.1. Nano zero-valence iron
363 Nano zero-valence iron (nZVI), due to its large specific surface area and strong reducing
364 ability, has been widely used in remediation of sites contaminated by chlorinated organic matters,
365 heavy metals and nitrate. Nano-sized ZVI particles are mixed in a slurry, injected through the
366 contaminated area by either natural groundwater flow or pumped to react with the target
367 contaminants (Wang et al., 2018; Wei et al., 2010). Given nZVI particles are prone to
368 agglomerate during migration, which leads to a reduction in specific surface areas, a reduced
369 migration distance, a deterioration of reactivity, and reduced efficiency. To solve these problems,
370 the surface of nZVI is often passivated, loaded, dispersant/stabilizer modified, or coated to form
371 bimetallic composite (Gao et al., 2013).
372 The efficiency of nZVI to remove a variety of heavy metals, such as copper (II), chromium
373 (VI), mercury (II), and lead (II), is often very high (> 90%, Table 9) (Xiao et al., 2011; Wang et
374 al., 2018; Xiong et al., 2009; Zhang et al., 2010). Multiwalled carbon nanotubes loaded with
375 nZVI (MWCNT-nZVI) could convert copper (II) to an Fe/Cu alloy and deposit it on its surface.
376 At pH=4.5, the concentration of copper (II) is 50mg/L; the concentration of MWCNT-nZVI is
377 0.5mg/mL, and the removal rate reaches 94% after a reaction time of 60 minutes (Xiao et al.,
378 2011). Carboxymethyl cellulose with iron sulfide (CMC-FeS) or with nano zero-valence iron
379 (CMC-nZVI), a stabilizer modified nZVI, can reduce contaminants dissociated from polluted
380 soils into groundwater (Xiong et al., 2009; Wang et al., 2018). When the molar mass ratio of
381 CMC (0.2%) FeS to mercury (II) in the soil is 26.5, the removal rate after 7 days reached 97%
382 (leaching to water) and 99% (leaching to TCLP fluid) (Xiong et al., 2009); whereas the leaching
48
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383 removal rate, quantified in the leaching batch experiment (Table 9) is the ratio of the difference
384 of leachate concentration with and without adding nZVI to soil (initial concentration) to initial
385 concentration. Wang et al. (2018) injected 1.5 kg of CMC-nZVI into the injection well, which
386 reduced the chromium (VI) concentration from 2 mg/L to less than 0.1 mg/L in a 6 m  6 m
387 contaminated site. Pilot scale tests of nZVI injection in porous aquifer and fractured bedrock for
388 the removal of Cr(VI), chlorinated aliphatic hydrocarbons, Ni , Pb and nitrate were also reported
389 (Mueller et al., 2012; Müller and Nowack, 2010; Bardos et al., 2014).
390 nZVI can convert nitrate into ammonium, which leads to high removal rate of
391 nitrate-nitrogen but a low removal rate of total nitrogen (Tang et al., 2012). If nZVI is coupled
392 with denitrifying bacteria, most of the final products will be gaseous nitrogen, which reduces the
393 formation of ammonia nitrogen and nitrite and increases the removal rate of total nitrogen (Wang
394 et al., 2015). Wang et al. (2015) reported that 2 g sodium oleate-coated nZVI and 10 mL of
395 activated bacterial solution removed 80.3% nitrate (155 mg) after 6 days and 80% of the final
396 product was gaseous nitrogen.
397 Although nZVI has been extensively adapted for the remediation of contaminated
398 groundwater, many problems remain unsolved: (1) High cost: The Pd-nZVI (bimetallic
399 composite nZVI) is 50 US dollars (Wei et al., 2010) per kilogram. (2) In the presence of oxygen,
400 it is easily oxidized to iron (II) or iron (III). Moreover, the dissolved oxygen or other oxides can
401 easily cause nZVI surface passivation, which interrupts the reaction. (3) In situ injection of nZVI
402 is often accompanied by its agglomeration and sedimentation, resulting in a shorter migration
403 distance and smaller remediation range. (4) The transport process of nZVI in the soil is likely a
404 preferential flow (Shi et al., 2015), so that the contaminated site cannot be uniformly remediated
49
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405 (only the contaminated area near the preferential flow is handled); thus, the nZVI on the end of
406 the preferential flow will accumulate, which adds a secondary pollution to the environment.
50
407 Table 9 Studies of the treatment of contaminants detected in MSW leachate by nZVI
Description of contaminants Description of the remover/removal method Description of the removal effect
Initia Re
Conditi Type
l mo Reference
Type of Contami Remov Dosage of on of of Removal
conce Removal mechanism val Limitation s
pollutant nant er remover remova exper rate
ntrati tim
l iment
on e
15C,
dark
2g sodium
and
sodium oleate coated
anaero
oleate nZVI, 10mL Nano-iron reduces
bic
NaNO3 coated activated nitrate to ammonia
70 enviro
simulate nZVI-d bacteria nitrogen; the sodium Wang et
mg nment, batch 6d 80.30% -
d water enitrify solution, oleate severed as a al. (2015)
N/L dissolv
sample ing 500mL carbon source for
ed
bacteri NaNO3 denitrifying bacteria
Nitrate oxygen
a simulated
=
water sample
0.54mg
/L
1.0
The removal rate
mM
60 ZVI-ra ratio of liquid Nitrate-N converted of nitrate is high,
NaNO3 Fe3+ in Tang et
mg w loess to soil V/W = to ammonium-N by batch 30h 100.0% but the total
solution NaNO3 al. (2012)
N/L soil 5:1 ZVI nitrogen removal
solutio
rate is low
n
Need more
H
studies on using
ea
MWC MWCNT-nZVI
vy Cu CuSO4 50mg [mat]=0.5 pH=4. 60 Xiao et al.
NT-nZ chemical reduction batch 94.0% to remove other
m (II) solution Cu/L mg/mL 5 min (2011)
VI heavy metals,
et
such as Pb(II),
al
Cr(VI), and As
51
(V)
50%
Tot sample/soil leach
83mg pH=9. (leach
al Cr(VI) ratio=0.0012 ing 24h
/kg 0 Degradation of into DI
Cr loaded CMC- g: 1.5g batch Xu et al.
chromium (VI) to water) -
sandy nZVI (2007)
Cr trivalent chromium
loam soil 34mg CCMC-nZVI
(VI - batch 48h 90.0%
/L =0.12g/L
)
97% Further research
(leach in need on how
Mercury
22±0.1 Adsorption and into DI to reduce Hg
spiked CMC( molar ratio of leach
Hg 177m C, co-precipitation, water); methylation, Xiong et
clay 0.2%)- FeS-to-Hg: ing 7d
(II) g/kg pH=7. converting Hg(II) to 99% decrease costs al. (2009)
loam FeS 26.5 batch
0±0.1 HgS (leach and improve
sediment
into environmental
TCLP) friendliness.
K-nZVI has large
specific surface area
electropl sample/soluti and subsequently
Pb ating 12.75 K-nZV on better adsorption and 60 Zhang et
30C batch 98.8% -
(II) wastewa mg/L I(20%n ratio=0.1g/10 reduction properties; min al. (2010)
ter ZVI) ml kaolin prevents
agglomeration of
iron
408
409
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410 1.4.2. Solubilizing agent
411 Solubilizing agents, containing both hydrophobic groups and hydrophilic groups, are
412 water-soluble chemical compounds that can be used to dissolve contaminants adsorbed on the
413 soil. The dissolved contaminants were further collected by seepage induced by either natural
414 hydraulic gradient or by pumping (Strbak, 2000; Paria, 2008; Lee et al., 2007; Mao et al., 2015)
415 during remediation. Common solubilizing agents are surfactant and cosolvent.
416 Due to hydrophobic affinity, solubilizing agents have been widely used to remediate
417 non-polar contaminants, e.g., dense non-aqueous phase liquids (DNAPLs), benzene, toluene,
418 ethylbenzene and xylenes (BTEX) from gasoline spills, and oil from petroleum and chemical
419 industries. The solubilizing agents have achieved good treating effects. Research on this aspect
420 was relatively mature, including lab-scale (Ma et al., 2016; Sun et al., 2013; Taylor et al., 2004;
421 Maire and Fatin-Rouge., 2017), pilot-scale (Tick et al., 2015) and full-scale (Strbak, 2000; Lee et
422 al., 2014) experiments.
423 A p, p’-DDT contaminated soil column with an initial concentration of 990 mg/kg was
424 flushed (flow rate = 6 ml/h) with cosolvent 1-propanol (40%), which reduces the water-p,
425 p’-DDT surface tension and makes the contaminant miscible with water. After 50 hours, 96% p,
426 p’-DDT was desorbed (Juhasz et al., 2003). Sun et al. (2013) utilized 100 g/L methyl
427 β-cyclodextrin (a biosurfactant) in combination with a 50 ℃ water bath and 30 min of 35 kHz
428 ultrasonic fortification to remove PAHs from the soil. After 60 min, 91.3 ± 3.1% of total PAHs
429 (initial concentration = 337.34 ± 9.54 mg/kg) were removed. Maire and Fatin-Rouge (2017)
430 showed that only two pore volumes were needed to reach a DNAPL removal efficiency of 95%
53
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431 when the soil column was preflushed by a synthesized surfactant foam with nitrogen and a
432 dihexyl sulphosuccinate (DHSS) surfactant, and then treated with Tergitol 15S9 (a surfactant).
433 As a comparison, 40 pore volumes were needed to reach a DNAPL removal efficiency of 90%
434 when only treated with Tergitol 15S9. However, few scholars reported treating dissolved organic
435 matter (quantified as COD) in MSW landfills by a solubilizing agent.
436 Surfactants and cheating agents can also remove heavy metals by complexation and ion
437 exchange, which can be enhanced by acidic solutions. At the sample/soil ratio of 0.00375g: 1g,
438 the saponin biosurfactant removed 99% of Ni and 73% of Cr, after 72 hours based on initial
439 concentrations of 151.00±1.98 mg/kg and 70.00±1.12 mg/kg, respectively (Maity et al., 2013).
440 After treating heavy metal-contaminated soil with ethylenediaminetetraacetate acid (EDTA)
441 (0.15 M)-Ammonyx KP (nonionic surfactant) for 48 h, removal rates of Zn, Cu, Pb, and Cd
442 (initial concentrations were respectively 325 mg/kg, 1565 mg/kg, 3245 mg/kg, 59mg/kg) reached
443 99.2%, 100%, 98.7%, and 99.2%. (Slizovskiy et al., 2011).
444 The solubilizing agent is relatively inexpensive, as the synthetic surfactant cost is 1–2 €/kg.
445 However, these issues are noted：(1) Solubilizing agents occasionally adsorbed on the surface of
446 the soil particles due to the strong affinity of the hydrophilic group to soil particles, resulting in
447 reduced efficiency and a second pollution (Mao et al., 2015). (2) After the surfactant is reused
448 three times, its solubilization effect is not obvious (Sun et al., 2013).
449
54
450 Table 10 Studies of the treatment of contaminants detected in MSW leachate by solubilizing agent
Description of the
Description of contaminants Description of the remover/removal method
removal effect Reference
Initial Dosage of Conditi Removal exper Removal s
Type Contaminant Remover time
concentration remover on mechanism iment rate
complexation
Cu clean soils mixed 122.3 mg/kg (0.08 mmol of the saponin 85.7%
EDDS-saponi
with Pb(NO3)2 EDDS + 24mg micelles and Cao et al.
n 25C batch 48h
and CuCl2 saponin): 1g metals; (2013)
Pb 184.4 mg/kg biosurfactant 99.8%
solution soil enhanced by
EDDS
Zn 325 mg/kg 99.2%
Cu 1565 mg/kg EDTA(0.1M) 100.0%

EDTA served
- Ammonyx
as a chelating
KP (nonionic
Pb 3245 mg/kg agent 98.7%
Soils heavily surfactant)
contaminated
Cd 59 mg/kg 25±1 99.2%
(more than 80 sample/soil Slizovskiy
C,
years) with ratio=0.02ml: batch 48h et al.
pH=6.
Zn sulfuric acid and 325 mg/kg 10g 52.6% (2011)
2
metals deposited Stable metallic
in the air I¯ (0.15M)- complexes
Cu 1565 mg/kg 71.1%
Ammonyx were formed
KP (nonionic with iodide and
Pb 3245 mg/kg surfactant) some heavy 76.8%
metals
Cd 59 mg/kg 67.3%
contaminated saponin sample/soil 26– Maity et

Ni 151.00 mg/kg - batch 72h 99.0%
soil from an biosurfactant ratio=0.00375: 29°C, al. (2013)
55
Cr industrial park 70.00 mg/kg 1g pH=5 73.0%
56
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452 1.4.3. Micro and nanobubbles
453 Micro and nanobubbles (MNBs) are tiny bubbles with a radius in the range of 0.05 μm to
454 25 μm and can be produced by decompression method, gas-water circulation method,
455 electrolysis, gas flotation pump method, micro-pipeline, high-temperature technology, ultrasonic
456 technology (Agarwal et al., 2011; Deng et al., 2014; Wang et al., 2017), or a combination of
457 above-mentioned methods (Li et al., 2013; Agarwal et al., 2011). The mechanisms of
458 contaminants removal by MNBs are as follows. (1) Due to their high surface charge, large
459 specific surface area and long life in water, MNBs adhere to flocs and suspended matter in the
460 pore fluid efficiently (Wang et al., 2017). Under buoyancy or seepage effects, bubbles and the
461 adhered contaminants gradually migrate upward to the water surface (2) The high gas-liquid
462 mass transfer rate of MNBs makes the dissolved oxygen supersaturated in water, thereby
463 promoting the degradation of pollutants by aerobic microorganisms. (3) Due to the high charge
464 density of the electric double layer of MNBs near the water-air interface, at the moment the
465 MNB collapses, the energy accumulated from the densely-packed positive and negative ions is
466 released and excites the generation of many hydroxyl radicals with a strong oxidizing ability
467 (Xiong et al., 2016). (4) Due to the strong oxidizing ability of the ozone, a variety of organic
468 matters, which are hard to be decomposed otherwise, can be oxidized by ozone MNBs.
469 MNBs have been widely used in industrial wastewater treatment and in situ remediation of
470 contaminated groundwater. After raw dyeing wastewater was treated by the coagulation
471 (coagulant dosages = 100 mg/L)-air micro bubble flotation processes for 5 min, the removal rate
472 of COD (initial concentration = 5051.1 mg/L) reached 89% (Liu et al., 2010). The coagulation
473 (coagulant dosages = 100 mg/L)-ozone microbubble flotation process achieved a 64% removal
57
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474 rate of ammonia from raw coke wastewater after 2 min flotation time (Liu et al., 2012).
475 Groundwater containing multiple persistent organic contaminants was treated by ozone
476 microbubbles, with a removal rate of over 95% of benzene (initial concentration= 30.5 ± 5.1
477 mg/L) and chlorobenzene (initial concentration = 14.8±2.5 mg/L), and 67% of nitrobenzene
478 (initial concentration = 502.8 ± 57.5 mg/L) after 30 minutes (Xia and Hu, 2019).
479 Ozone bubbles have been used to conduct in situ remediation of groundwater contaminated
480 by methyl orange using column scale tests with removal rate of 98% (Hu et al., 2018). Ozone
481 bubbles have also been used for field scale tests on trichloroethylene (TCE) with removal
482 rate of 99% (Hu et al., 2018) and on methyl-t-butyl ether (MTBE) with removal rate of 80%
483 (Kerfoot, 2002), and on diesel (Kerfoot, 2003). Oxygen bubbles can promote in situ
484 biodegradation efficacy by supplying the electron acceptor and have been used for the removal
485 of p-xylene (Jenkins, 1993) and phenanthrene (removal rate=51.5%, Choi et al., 2009) under
486 column scale tests. Hu et al. (2015) developed a process for the in situ remediation of
487 contaminated sites by MNBs: MNBs with water containing nutrients were injected upstream of
488 the contaminated area, which decomposed the pollutants and supplied the electron
489 acceptors/donors for the microorganisms in the contaminated area; Monitoring wells enabled
490 real-time monitoring of organic pollutant removal processes; Pumping wells accomplished the
491 secondary utilization of MNBs water and formation of the groundwater flow field. Meegoda et
492 al. (2016; 2017) developed a device consisting of an ozone-nanobubbles water support system
493 and ultrasound probes for decontaminating polycyclic aromatic hydrocarbons (PAHs) from river
494 sediments, with a removal rate that reached 93% under optimal conditions with reasonable time
495 intervals between ultrasound applications.
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496 There are several shortcomings to using MNBs for in situ remediation of contaminated
497 sites: (1) Due to the manufacturing difficulty, energy consumption and maintenance costs of
498 MNB generating device, MNB technology is significantly more expensive than traditional
499 nitriding and ozonation methods in wastewater treatment. (2) MNBs oxidize heavy metals,
500 thereby improving their toxicity and mobility in groundwater, which increases the risk of
501 exposure to the public. For example, ozone micro and nanobubbles would oxidize Cr(III) to
502 Cr(VI) (Meegoda et al., 2016). (3) Most bubbles are generated on microscale (micro bubbles),
503 while generation of nanoscale bubbles is still difficult.
504 Currently, no reports are available on the treatment of landfill leachate or in situ
505 remediation of landfills contaminated sites by MNBs technology. However, it is expected to be
506 applied in this type of treatment based on its successful application to the treatment of COD and
507 ammonia in industrial wastewater and in situ remediation of the petroleum/chemical industry
508 contaminated sites. Nevertheless, more research is warranted.
509 1.5. Phytoremediation
510 Phytoremediation, a means of remediation and rehabilitation for a contaminated land using
511 green plants, has emerged as a viable alternative site remediation method for MSW landfills and
512 dumpsites due to its large treatment area and capability to treat contaminants distributed
513 spatiotemporal variably throughout the shallow soil layers (Nagendran et al., 2006; Pathak et al.,
514 2012; Lamb et al., 2014; Reddy et al., 2017). Mechanisms of phytoremediation include (Pathak
515 et al., 2006; Jones et al., 2006; Nagendran et al., 2006): (1) phytoextraction, where plants (e.g.,
516 Thalaspi, Alyssum and Brassica) take up contaminants from soil or water, then translocate and
517 accumulate them into roots or harvestable shoots; (2) phytofiltration, where plants absorb
59
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518 contaminants from contaminated surface water; (3) phytostabilization, where contaminants
519 (metal and organic) are immobilized in the soil by means of sorption (binding), precipitation, and
520 complexation by the deep or fibrous root systems of the plants; (4) phytovolatilization, where
521 contaminants are converted to volatile form and released into the atmosphere via
522 evapotranspiration process of the plants; (5) phytodegradation, where organic contaminants are
523 converted to less harmful substances by the plants; and (6) Rhizofiltration, where plant roots
524 growing in polluted water precipitate and concentrate metals (Cu, Hg, Pb, Zn).
525 Major categories of contaminants from a solid waste landfill (Kjeldsen et al., 2002; Han et
526 al., 2016) defined in Introduction can all be removed by phytoremediation. COD and NH4+ in
527 landfill leachates can be efficiently reduced by either forestry or grassland treatment system
528 (Jones et al., 2006). COD, nitrogen and phosphorous in an anaerobic MSW landfill in the north
529 of Italy were remediated by sunflower with removing efficiencies of 50%, about 100% and
530 100%, respectively (Garbo et al., 2017). Heavy metals from Kuchyňky landfill leachate were
531 removed by mushroom species (P. ostreatus as a bioaccumulator) (Vaverková et al., 2017). Sites
532 contaminated with both organic and heavy metals were also effectively treated with native
533 species such as Switchgrass and Little Bluestem (Reddy et al., 2017).
534 The major drawback of phytoremediation is the long treatment cycle due to the relative
535 slow growth rate of natural plants, which was also subject to the influence of climate and
536 hydrological conditions.
537 Part 2. Design chart for sustainable remediation (Case studies)
538 To account for the different features of hydrogeological characteristics of contaminated
539 sites, a design chart was compiled for quick adaptation of the suitable technique for remediation
60
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540 of sites contaminated by solid waste landfills (Fig. 4). Three cases were given as follows to show
541 the design procedures.
61
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542 Figure 4. Removal rate of suggested remediation technologies for (a) COD, (b) inorganic
543 contaminants, (c) Fe, Mn, Cr(VI), Cd and (d) Zn, Pb, Cu, Ni
544
545
546
62
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547 2.1 PRB removing COD,𝐹𝑒2 + and 𝐶𝑢2 + in an MSW landfill site
548 Chathuranga et al. (2019) reported a field-scale permeable reactive barrier (PRB) set-up,
549 located in the proposed landfill-site in the Hambantota Municipal Council, where the ground
550 water was contaminated by landfill leachate consisting of COD, nitrogen, Fe2 + , and Cu2 + .
551 Flow rate across the PRB was 100 mL/min (Chathuranga et al., 2019). According to the
552 proposed design chart (Table 11), PRB is a reasonable candidate for remediation. Indeed, a
553 multi-layer PRB was selected, with low-cost and locally available reactive materials, including
554 firewood, charcoal, bio char, saw dust, washed quarry dust, dewatered alum sludge, red soil and
555 washed silica sand. The removal efficiencies of COD, Fe2 + , Cu2 + , and TN (total nitrogen)
556 were 45%, 31%, 53%, and 49%, respectively, primarily through adsorption, ion-exchange
557 reactions, filtration and precipitation mechanisms in the sequential PRB (Chathuranga et al.,
558 2019).
559 2.2 PRB removing 𝐹e2 + and 𝑀n2 +
560 Wang et al. (2016) reported that permeable reactive barrier tests were carried out in the
561 Klondike Landfill, a closed unlined municipal solid waste landfill, located in Florida, USA. The
562 site was contaminated with Fe2 + and Mn2 + , with a hydraulic conductivity of approximately
563 7.93 m/day and a hydraulic gradient of 0.006. This site is most suitable for the PRB method,
564 which is also suggested in the proposed design chart (Table 11). PRB was divided into two equal
565 length sections, filled with different reactive materials for Fe and Mn removal. One reactive
566 material was limestone, achieving an average removal rate of 91% for the first year of operation.
567 Another reactive material was crushed concrete, achieving an average removal rate of 95% for
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568 the first year of operation. The removal rates for both reactive materials in the third year of
569 operation declined to an average of 64% and 61%, respectively (Wang et al., 2016).
570 2.3 EK removing 𝑃𝑏2 +
571 Acar and Alshawabkeh (1996) reported the removal efficiency of lead under electrokinetic
572 remediation at pilot scale in kaolinite spiked with lead nitrate solution. The site was
573 contaminated with Pb2 + , with a hydraulic conductivity of 5 ― 8 × 10 ―8𝑐𝑚/𝑠 and hydraulic
574 gradient of 10 to 20. This site is most suitable for the EK method, also given as an option in the
575 proposed design chart (Table 11). A row of five equally spaced graphite rods that are chemically
576 inert to electrolysis reactions were installed as both the anode and cathode. When a constant
577 direct current density of 133 μA/cm2 is applied, Pb (lead) was transported toward the cathode
578 and produced hydroxide precipitation, with a removal rate of 55% (Acar and Alshawabkeh,
579 1996).
580 2.4 EK+PRB removing Cu2 +
581 Chung (2009) reported an in-situ electrokinetic reactive pile tests (electrokinetic
582 remediation coupled with a permeable reactive barrier) adjacent to a waste landfill site in
583 Incheon, Republic of Korea, which was contaminated with Cu2 + , with a permeability of
584 8.3 × 10 ―4𝑐𝑚/𝑠 (iron powder), 1.2 × 10 ―4𝑐𝑚/𝑠 (zeolite), 2.4 × 10 ―1𝑐𝑚/𝑠 (slag), 3.3 × 1
585 0 ―2𝑐𝑚/𝑠 (tire chip), and 1.8 × 10 ―3𝑐𝑚/𝑠 (sand). This site is most suitable for EK and PRB
586 methods, as suggested in the proposed design chart (Table 11). EK-PRB was chosen as the
587 remediation method. Stainless rods were installed inside both the anode and cathode hollow piles
588 (made of 60 mm diameter PVC pipe, installed vertically to a depth of 2.5 m below the ground
589 surface). The spaces between the rod and pipe were filled with sand (the anode) and reactive
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590 materials (the cathode) respectively. Copper migrated from the anode side towards cathode,
591 where it was adsorbed. The removal rates of Cu were 68–68.7, 93.4–93.7, 74.8–75, 87.3–88.0,
592 and 4.7% in the cases of iron powder, zeolite, slag powder, tire chips, and sand as the reactive
593 material, respectively (Chung, 2009).
594 Part 3. Challenges
595 3.1. Flow Pattern
596 Efficiency of remediation relies on the sufficient contact and reaction time between
597 contaminants and the remediation agents in many instances, such as PRB and the injection of
598 MNBs. Sufficient contact requires uniform flow in a saturated medium, which is more difficult
599 to achieve as the scale of treatment increases (Fig. 5). Batch test usually achieve thorough
600 mixing and contact, and yielded highest remediation efficiency; meanwhile, the column test is
601 subjected to flow patterns (determining contact) and flow rate (reaction time), and is more
602 specific to the applied conditions (Cao et al., 2019). Efficiency of pilot and full-scale
603 experiments is more prone to the influence of the flow pattern and flow rate. Flow pattern is
604 influenced by interfacial surface tension, contact angle, flow rate, and soil matrix network
605 properties (Cao et al., 2016 Sustainability). Therefore, carefully examining the flow pattern is of
606 crucial importance to engineering applications.
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607
608 Figure 5. Flow pattern examples: (a) Fingering patterns observed during water infiltration
609 into the layered sand (Rezanezhad et al., 2006); (b) Distribution of CO2 (yellow) and saline water
610 (blue) in the microfluidic chip after CO2 replacing saline water (Zheng et al., 2017); (c)
611 Displacement pattern produced by injecting glycerin solution into Ottawa F110 sand (Zhang,
612 2012); (d) Non-uniform capillary rise in glass beads (Nie et al., 2019). Inset: directions of flow.
613 3.2. Multi-layer PRB
614 Multiple layers of reactive barriers have gained significant attention during the past few
615 years. Challenges are the membrane effects and inhibition in-between layers. Reactive materials
616 in different layers differ in granular size and gradation (size distribution). At the interface of two
617 layers, two failure mechanisms can occur, namely, clogging and loss of materials (similar to
618 piping failure in an earthen dam). Both mechanisms were referred to as membrane effects.
619 Reactive materials or the products of the reaction of the preceding layer could be the
620 contaminant loading to the latter layer, such as ZVI to zeolite. One logical design of a multi-layer
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621 PRB is that the first layer is for reducing, the second layer is for oxidizing, and the last layer is
622 for adsorption.
623 Part 4 Summary
624 This paper reviewed the technologies suitable for remediation of soil and groundwater
625 contaminated with municipal solid wastes landfills. First, an overview of the market around the
626 globe was given, followed by the features of contaminants in an MSW landfill contaminated site.
627 Then technologies such as permeable reactive barriers, electrokinetic remediation, microbial
628 remediation, and injection of either solubilizing agents or micro or nanobubbles were thoroughly
629 reviewed, with an emphasis on their removal efficiency and on existing projects at lab, pilot or
630 field scale. Furthermore, a design chart was proposed, which is customized for the remediation
631 of a landfill contaminated site, followed by a few case studies implementing the chart. Finally,
632 challenges of existing remediation technologies for MSW landfills were identified, and potential
633 failure mechanisms were elucidated.
634 Acknowledgements
635
636 This work was sponsored by the National Natural Science Foundation of China (Award
637 No.: 51779219). This work was also sponsored by the Ministry of Science and Technology of
638 China (Award No.: 2018YFC1802300). Financial supports by both the One-Thousand Young
639 Talents Program of the Organization Department of the CPC Central Committee and the
640 100-Talents Program of Zhejiang University to the corresponding author are deeply appreciated.
641 MOE Key Laboratory of Soft Soils and Geoenvironmental Engineering is acknowledged.
642
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643
644
645
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Highlights
 Landfills contaminants are grouped into COD, inorganic matter and heavy
metals.
 A status quo of existing technologies were thoroughly reviewed
 A design chart was developed, verified by a few case studies;
 Future trends of technical innovation and challenges were identified.

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Accepted Manuscript

Emerging Sustainable Technologies for Remediation of Soils and Groundwater in

Jianshe Ye, Xiao Chen, Chao Chen, Bate Bate

Reference: CHEM 23561

To appear in: Chemosphere

Received Date: 01 February 2019

Accepted Date: 06 April 2019

1 Emerging Sustainable Technologies for Remediation of Soils and Groundwater in a

2 Municipal Solid Waste Landfill Site -- A Review

3 1Jianshe Ye, 1Xiao Chen, 1Chao Chen, 2*Bate Bate

5 1Graduate Research Assistant, Institute of Geotechnical Engineering, College of Civil

25 Emerging Sustainable Technologies for Remediation of Soils and Groundwater in A

26 Municipal Solid Wastes Landfill Site -- A Review

27 Ye, J., Chen, X., Chen, C., Bate, B.*

31 potential. Unlike contaminants in an industry or agricultural site, contaminants from MSW

34 challenges to remediation contaminants of different characters altogether. A status quo of

35 existing technologies, including permeable reactive barriers, electrokinetic remediation,

41 (such as flow pattern) were identified.

47 of pollution. Due to degradation of wastes, microbial metabolism, rainfall, and groundwater

52 and the ecological system.

71 contaminated sites and the remediation market is summarized in Table 1.

72 Table 1 Status quo of global polluted sites and remediation markets

Identified and potential Value of Current Future Market

79 (quantified by COD), inorganic contaminants (including ammonium-nitrogen, nitrate-nitrogen,

84 microorganisms (typically short duration) and anaerobic degradation of microorganisms (acid

93 year, rather than landfill age (Kulikowska and Klimiuk, 2008).

104 logarithmic coordinates.

111 given. The layout of the content is as follows:

112 Part 1. Remediation Technologies for Contaminated MSW Sites

113 1.1. Permeable reactive barrier (PRB)

114 1.2. Electrokinetic (EK) Remediation

115 1.2.1. EK+PRB

116 1.2.2. BioEK

117 1.3. Microbial Remediation

118 1.4. In-Situ Injection Treatment

119 1.4.1. Nano zero-valent iron

120 1.4.2. Micro and nanobubble

121 1.5 Phytoremediation

123 Part 3. Challenges

124 3.1. Flow pattern

125 3.2. Multi-layer PRB

126 Part 4. Summary

127 Part 1. Remediation Technologies for Contaminated MSW Sites

134 remediation of contaminated municipal solid waste sites.

135 1.1. Permeable Reactive Barrier

146 and Changsha.

155 required at intervals to counter performance degradation, saturation, or depletion of materials.

163 Tables 2-6 and analyzed as follows.

170 al., 2011).

pump rate 0.8

the Hun hydraulic Hou et

sequential River water

208 precipitation and ligand exchange) (Duan et al., 2012).

1st-4th sand box: 8h,

Modified steel slag

224 rate of 99% (Ranjbar et al., 2017).

ZVI/Pumice flow rate 0.5 324 Calabrò et

237 1.2. Electrokinetic Remediation

243 remediating agents have difficulty reaching the interaggregate space.

261 and ammonia nitrogen.

272 90% with addition of 50mM of citric acid.

305 the soil, thereby promoting its electromigration.

308 1.3. Microbial Remediation