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International Biodeterioration & Biodegradation 128 (2018) 134e140

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International Biodeterioration & Biodegradation


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

Vegetation recovery and groundwater pollution control of coal gangue


field in a semi-arid area for a field application
Baiwei Liu a, b, Zhonghua Tang a, Shaogang Dong c, *, Lixin Wang c, Dongwei Liu c
a
School of Environmental Studies, China University of Geosciences, Wuhan 430074, China
b
Social Sciences Department of Inner Mongolia University, Hohhot, 010021, China
c
School of Ecology and Environment, Inner Mongolia University, Hohhot, 010021, China

a r t i c l e i n f o a b s t r a c t

Article history: This paper studied the impact of a gully-type gangue dump in the Daliuta mine area, Shaanxi, China on
Received 25 October 2016 the groundwater environment and its contamination control. Multiple methods including eco-
Received in revised form hydrogeological survey, soil column leaching test, field test and groundwater flow analysis were
10 January 2017
applied in the study. According to the field survey, the stack of gangue had changed the original feature of
Accepted 16 January 2017
Available online 24 January 2017
groundwater flow system, with the groundwater level of the gangue field raising about 1e3 m compared
with the condition before the establishment of gangue dump. The long-term immersion of gangue had
released various harmful substance into the groundwater and affected the downstream areas. The
Keywords:
Coal gangue
leaching test showed that the loess could significantly purify the mine wastewater by increasing pH
Groundwater pollution value from 4.5 to 6.2e6.7 and absorbing heavy metals. Based on the loess column test, two loess
Leaching test permeable reactive barriers (LPRBs) were established in situ to improve the groundwater environment of
Loess gangue field. Besides, the vegetation restoration had been successfully carried out by covering a 30 cm-
Loess permeable reactive barrier (LPRB) thick loess layer on the coal gangues and planting Alfalfa and Artemisica ordosica to improve the
Vegetation recovery ecological environment, and the vegetation coverage had increased from 10% in 2008 to about 65% in
2013.
© 2017 Elsevier Ltd. All rights reserved.

1. Introduction produces large amounts of mine wastewater and gangue leachate,


which can be acidic and contain high concentrations of sulfide and
The migration and transformation of pollutants in groundwater heavy metals (Gibert et al., 2011; Miao et al., 2012); the uncon-
are affected by the water-rock interaction (Olaka et al., 2016), mi- trolled discharge of mine water could degrade the water quality of
crobial action (Maizel et al., 2016; Cesar and Ros, 2013; Li et al., the receiving water body (Nordstrom, 2011). Ao and Huang (2005)
2014; Da Silva and Corseuil, 2012; Souza et al., 2009), and human found that the Wuda mining gangue dump of Inner Mongolia has
activities (Da Silva and Bonotto, 2015; Fabro et al., 2015) among been heavily polluted as evidenced by the lower pH value and high
others. The coal resource is rich in China and has been the main concentration of SO2 4 in the surface water around the gangue
energy for a long time. However, coal mining can cause negative dump. The coal mine wastewater and coal gangue leachate can
impacts on the regional environment. The change in coal mine geo- discharge harmful heavy metals, radioactive elements, polycyclic
ecological environment is a result of human activities that destroy aromatic hydrocarbons and other organic pollutants, which may
the system construction and function (Davis et al., 2010; Cherry cause hydrogeochemical reactions and consequently significant
et al., 2001; Moldovan et al., 2008; Sasamoto et al., 2004). There increase of TDS and hardness in groundwater, pollution of soil and
are three main impacts of coal mine development on the envi- deterioration of ecological environment (Sydnor and Redente,
ronment, including changing the groundwater flow system, dis- 2002; Gomo and Vermeulen, 2014; Khalil et al., 2013). High level
turbing the soil and causing ecological degradation. Coal mining of acidity and heavy metals in coal gangue field are regarded as key
factors limiting plant growth and vegetation restoration (Chadwick,
1973). Currently, CaO or CaCO3 are commonly used to regulate the
* Corresponding author. School of Ecology and Environment, Inner Mongolia
pH of the mine water and soak solution of coal gangue, and
University, Hohhot, No.235 West College Road, Hohhot, 010021, China. appropriate plants are known to be able to stabilize or extract
E-mail address: groundwater@163.com (S. Dong). heavy metals in soils (Marseille et al., 2000). Therefore, how to

http://dx.doi.org/10.1016/j.ibiod.2017.01.032
0964-8305/© 2017 Elsevier Ltd. All rights reserved.
B. Liu et al. / International Biodeterioration & Biodegradation 128 (2018) 134e140 135

remove heavy metals and select suitable species for ecological Quatz, one of the main mineral compositions of the loess accounts
restoration has been one of the hot issues in ecological restoration for more than 50%, followed by mica, amphibole and feldspar. SiO2,
research and practice in coal gangue fields. the dominant chemical composition in loess accounts for more
This study analyzed the effect of the establishment of loess than 50%, followed by Al2O3, CaO, Fe2O3, MgO, K2O, Na2O, FeO, TiO2,
permeable reactive barriers (LPRB) and the pavement of a loess etc. The studied loess are characterized by small particles with large
layer for vegetation recovery in the Daliuta mine area, Shaanxi, specific surface area, and a large amount of clay minerals with
China. Multiple methods, such as eco-hydrogeological survey, lab- negative charges to absorb positive ions. Therefore, the loess strata
oratory and field experiments as well as groundwater pollution have large adsorption capacity for heavy metal pollutants.
treatment were applied.

2. Materials and methods


2.5. The loess column experiments of absorbing heavy metals
2.1. Sites information
Considering the unavailability of massive soak solution of
gangue and the similar chemical compositions of the gangue soak
Daliuta coal mine is located on the north of Shaanxi province.
solution and coal mine wastewater, the wastewater from Daliuta
This area is a transition zone of Maowusu sandland and loess hill,
coal mining was applied as the input solution of the loess column
which belongs to Yanhe stratum of Erdos section of North China
experiment. The loess was taken from the north hills of the coal
formation. The studied gangue field is surrounded by active, fixed
mine. The grain size of experimental loess was 0.05e0.10 mm, the
and semi-fixed sand dunes and is located in a valley 4.8 km away
porosity was 0.32 and the volume weight was 1.54  103 kg/m3.
from the Wulanmulun River in the east. The unconfined aquifer of
The column experimental setup was an organic glass column
this area consists of Quaternary residual sand, aeolian sand and
with a diameter of 8 cm and length of 100 cm. The loess sample was
lacustrine silty-fine sand (Fig. 1). The mean annual rainfall is
air dried, sorted and then packed into the organic glass column high
440.8 mm, 71% of which falls from June to September every year.
up to 70 cm with the nature density (Fig. 4). In order to avoid the
The total evaporation is 2163 mm per year.
disturbance of loess and blocking of the outlet, 1 cm-thick pebble
layer were laid on both ends of the loess column when filling the
2.2. The investigation of the gangue field
column. Unpolluted groundwater from upstream of gangue field
was injected into the loess column from the bottom for water
The Gangue field is surrounded by 10e40 m high sand dunes.
saturation to record the pore volume (PV). After the loess was
The Neogene mudstone aquiclude is under Quaternary aeolian
saturated, 3e5 PVs water was injected from the top of the loess
sand. The gangue field has been stacked since April 2003. The field
column to wash way desorbed ions. At last, the coal mine waste-
has been piled up with 2.5  106 m3 gangue reaching the height of
water was added into the loess column and kept at a certain level
20 m on average until February 2007. The characteristics of
for the leaching test. Each PV leachate from the loess column was
groundwater flow have been changed by the gangue dumps in the
collected and numbered before filter. Soluble metals such as Cu,
valley. The valley as the local discharge channel of unconfined
Mn, and Cr were measured using filtered and acidified samples also
water before the gangue being stacked, receives recharge in rainy
by inductively coupled plasma mass spectrometry.
seasons and phreatic water occasionally. Since waste rocks were
piled, the evaporation receded greatly, and the discharge of
groundwater into the valley from sides stored in pores of coal
gangue. At the same time, precipitation was capable of recharging 2.6. Remediation projection
the aquifer quickly through the loose pores of the gangue pile.
Therefore, the phreatic water level of the gangue field has risen According to the previous experience and the local conditions of
1e3 m after four-year stack according to the observation at probe climate, soil texture and precipitation, artemisia ordosica and al-
holes in June 2008 (Fig. 2). The long-term soak of coal gangue at the falfa were selected as the optimal vegetation for ecological recovery
bottom of the gangue pile produced a large number of leachate of the mine. Both of the species are indigenous species, which can
under water-rock interactions, and caused water pollution. survive easily, keep the characteristics of local species, and more-
over prevent invasive species to reduce the risk of biodiversity
2.3. Water pollution survey decrease and extinction of local species as well as the other
ecological disasters.
According to the hydrogeological setting surrounding the The first stage of the project of the coal gangue plant started in
gangue field, two samples from surface water and four samples April 2003 and ended in February 2007 with the volume of gangue
from groundwater in the study area were collected in March of stacks as 2.5  106 m3. Based on further exploitation of coal in 2010,
2008. Sample L2 and L3 were collected from the stream in the the second stage of the project was set up in June of 2011 to pile up
valley. Sample L1 was collected from the spring vent upstream the gangues along the downstream of the valley.
study area, sample L4 and L5 from the wells, while sample L6 from A 30 cm-thick loess layer was covered on the top of the gangue
the soaking solution of the coal gangue (Fig. 3). The concentrations field after the first-stage project had ended in March, 2008. Arte-
of Zn, Cu, Ni, Cr, Hg, Mn, As in water samples were measured using misia ordosica were planted in drilling way in early April, based on
inductively coupled plasma mass spectrometry (ICP-MS, Agilent 13.5e16.5 kg/ha. Three months later, 2-or-3-year artificial re-
7500a, Santa Clara, CA, USA). The concentrations of NO 3 and F

producted Alfalfa was planted in points strain method with the
were tested using DXO120 ion chromatography in the laboratory, as spacing of 0.6 m  0.4 m. A LPRB was built on the tertiary mudstone
shown in Table 1. downstream of the gangue field to purify the gangue leachate. The
LPRB was about 5 m high, 1.5 m wide at the bottom and 0.5 m wide
2.4. Loess feature of coal mine area at the top. The same LPRB was built in the second-stage project in
the downstream of the gangue field in June 2012 since the first
Loess is widely distributed in Daliuta coal mine area. It is LPRB and observation hole were covered by the coal gangues
covered by silty sand (50%), clay (15e30%) and silver sand (30%). (Fig. 5).
136 B. Liu et al. / International Biodeterioration & Biodegradation 128 (2018) 134e140

Fig. 1. A sketch hydrogeological map of Daliuta mining area.

3. Result and discussion drinking water standard, with the exceeding rate of 3.5, 308.2,
3.985 and 3.56 (Table 1).
3.1. Water pollution analysis For the surface water samples L2 and L3, the sample L2 located
in the upper reaches of the stream is less affected by the leachate
The water sample L1 was collected from the spring vent up- from the coal gangue than the sample L3, and thus the water quality
stream the coal gangue field, and may not be affected by the is better than the sample L3.
leachate from the coal gangue. Therefore, the ion concentrations of The water sample L4 represents the groundwater in the
sample L1 were applied to represent the background concentration downstream area of the coal gangue, mainly affected by the coal
of the unconfined groundwater in this area. According to the gangue in the northwest Valley. The concentration of As in the
analysis results, all the indexes of sample L1 meet the quality sample L4 is 1.013 mg l1, 148 times higher than the background
standard for drinking water in the People's Republic of China value. NO3-N concentration is 31.2 mg/l, three folders higher than
(GB5749). the background value. The results show that the groundwater
The water sample L6 is from the soaking solution of the coal downstream the coal gangue has been seriously polluted.
gangue, in which the measured concentration can represent the The water quality of the sample L5 from the well in the valley is
concentration of various pollutants released from the coal gangue not only affected by the leachate from the coal gangue in the
during the long-term leaching and soak in natural conditions. The northwest Valley, but also diluted by the groundwater and infil-
measured results showed that all indicators of water sample L6 are trated surface water in the southeast of the Valley. The concen-
significantly higher than the background values. The concentra- trations of all the pollutants were lower than that in the sample L4,
tions of Mn, As, NO3-N, F were significantly higher than of but have also been severely affected by the gangue leachate, with
B. Liu et al. / International Biodeterioration & Biodegradation 128 (2018) 134e140 137

Fig. 2. Hydrogeological section map of valley before and after the stack of gangue.

Cr, Pb was 382 mg l1, 83 mg l1, 921 mg l1, 1.2 mg l1, 3236 mg l1,
19 mg l1, 117 mg l1, and 236 mg l1, respectively. The concentrations
of Cu and Zn meet the drinking water quality standards, while Mn,
Hg, As, Cd, Cr, Pb exceed the standards by 3.82, 1.2, 323, 3.8, 2.34
and 23.6 times, respectively. Table 2 presents the experiment re-
sults. The pH value for coal mine wastewater before leaching was
4.5 and reached to 6.2e6.7 after leaching through the loess column.
The results showed that 98% of Mn, 99% of Cu, 84% of Zn, 79% of Cd
and 99% of Pb in the wastewater were absorbed when the no.21 PV
mine wastewater flowed through the loess column (Table 2). All the
indexes of the leachate meet the drinking water standards. More
than 96% of As was absorbed before the no.8 PV mine wastewater
flowed through the loess column. Ultimately, the absorption of As
almost reached saturation due to high content of As in the waste-
water. The experiment showed the strong absorption capacity of
loess for most heavy metals and the ability of neutralization of the
coal mine wastewater.
The purification of the acid mine wastewater by leaching
through loess column involves many mechanisms, among which
the most important is the neutralization of carbonate minerals and
the decomposition of silicate minerals (Suteerapataranon et al.,
2006; Johnson, 1995).
Calcium and magnesium carbonates are the most common
carbonate minerals in the loess, they can neutralize the infiltrated
acid. The reactive equations were shown as follows:

CaCO3 þ Hþ ¼ Ca2þ þ HCO3  (1)

MgCO3 þ Hþ ¼ Mg2þ þ HCO3  (2)

Fig. 3. Water samples distribution map.


Mg,CaðCO3 Þ2 þ 2Hþ ¼ Mg2þ þ Ca2þ þ 2HCO3  (3)

the concentrations of Mn, As, NO3-N, F and other indicators The layered silicates and allophane with extremely high specific
exceeding the drinking water quality standards. surface in the loess decompose in the acid environment, by which
In summary, the groundwater and surface water were serious consume Hþ and raise the pH value. The equation was shown as
polluted, with coal gangue as the center. follows:

nHþ þ layered silicates ¼ A13þ þ SiðOHÞ4 (4)


3.2. The loess column experiments result
The loess is rich of mica, illite and montmorillonoid. All these
The coal mine wastewater used in the experiment had pH value minerals can decompose by encountering hydrogen ion, taking
of 4.5, and the concentration of heavy metals Mn, Cu, Zn, Hg, As, Cd, sodium feldspar as an example:
138 B. Liu et al. / International Biodeterioration & Biodegradation 128 (2018) 134e140

Table 1
The concentrations of heavy metal ions in water samples (unit: mg l1).

Sample ID Cr Ni Cu Zn Mn Hg As NO3-N F Source

L1 0.003 ND 0.017 0.057 0.24 ND 0.007 9.9 0.013 Spring


L2 0.012 ND 0.016 0.047 0.33 ND 0.008 18.1 0.018 Surface water
L3 0.015 0.016 0.024 0.047 0.034 ND 0.011 16.3 0.021 Surface water
L4 0.081 0.023 0.133 0.079 1.01 ND 1.013 31.2 1.972 Groundwater
L5 0.052 0.011 0.035 0.046 0.25 ND 0.056 25.4 1.155 Groundwater
L6 0.564 0.032 0.426 0.075 2.35 ND 3.082 79.7 3.561 Groundwater
Drinking water standard 0.05 0.05 1 1 0.1 0.001 0.01 20 1 GB5749

Note: ND, below the detection limit.

Table 2
The concentration variation of heavy metals in coal mine wastewater (unit: mg l1).

No. of PV pH Mn Cu Zn Hg As Cd Cr Pb

1 6.3 e e e e e e e e
2 6.5 e e e e e e e e
3 6.4 2 e e e e e e 1
4 6.7 e e e e e e e 2
5 6.5 e e 22 e 32 e e e
6 6.3 4 e 34 e 57 e e e
7 6.6 6 e 45 e 56 e e e
8 6.6 3 e e e 123 e e 3
9 6.4 5 5 65 e 107 2 e e
10 6.7 4 3 35 e 335 1 e e
11 6.5 3 6 78 e 893 1 e 3
12 6.5 6 3 109 e 1187 2 e 3
13 6.5 6 5 121 e 1125 3 e 2
14 6.4 8 7 168 e 1367 3 e 2
15 6.3 7 5 156 e 2423 5 e 3
16 6.4 6 6 143 e 1987 2 e 5
17 6.6 11 6 121 e 2356 4 e 4
18 6.4 7 8 154 e 2781 6 e 6
19 6.5 10 10 133 e 2523 7 e 7
20 6.5 8 11 132 e 3012 3 e 5
21 6.2 8 8 145 e 3238 4 e 3

2NaAlSi3 O8 þ 2Hþ þ H2 O ¼ Al2 Si2 O5 ðOHÞ4 þ 2Naþ þ SiO2


(5)
The migration and transformation of heavy metal pollutants in a
water-soil system is also a complex process evolving physical,
chemical and biological reactions (Colin and Villegas, 2012). The
loess is characterized by fine grain, large specific surface and con-
taining a certain amount of clay minerals. When the heavy metal
Fig. 4. Column experimental setup. ions leach though the loess column, they can be removed through

Fig. 5. Site remediation of LPRB.


B. Liu et al. / International Biodeterioration & Biodegradation 128 (2018) 134e140 139

physical and chemical reactions such as the surface adsorption, the Table 4
ion exchange and adsorption, dissolution precipitation, oxidation The second-stage project groundwater monitoring results (unit:mg l1).

reduction, complex chelation, etc. (Adam and Edyvean, 1996; Han Time pH Cr Ni Cu Zn Mn Hg As
et al., 2016). For example, the iron-aluminium oxides in loess can 2012.6 6.1 0.005 e 0.014 0.086 0.35 e 0.007
strongly adsorb As, Cr and other heavy metals (Dugan, 1987). 2013.8 6.0 e e 0.007 0.023 0.17 e e
2014.6 6.7 e e 0.008 0.032 0.15 e e
2015.6 6.5 e e 0.005 0.036 0.13 e 0.003
3.3. Vegetation recovery and groundwater pollution control
effection analysis
layer could satisfy the need of growth of Alfalfa and Artemisia
Every September from 2008 to 2013, the box method was
ordosica. The vegetation of coverage in the gangue field had
adopted to investigate the vegetation and plant species on the
increased from 10% in 2008 to about 65% in 2013. The LPRB can
gangue field.
absorb the most heavy metal ions of gangue leachate and improve
According to the survey results, the artificial cultivated alfalfa
the quality of polluted groundwater.
and artemisia ordosica had grown well and the vegetation coverage
increased yearly. The loess layer could hold enough water for
vegetation growth. The vegetation coverage of the gangue field had Acknowledgments
increased from 10% in 2008 to 65% in 2013. As the soil quality
improved, natural incarvillea sinensis was found in 2009 and other The National Natural Scientific Foundation of China (No.
drought-tolerant plants were found since then, such as Astragalus 41562020, 41571090 and 31560146) supported this research.
adsurgens in 2010, Eragrostis poaeoides in 2011.
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