J Soils Sediments (2017) 17:2742–2751
DOI 10.1007/s11368-017-1709-1
SOILS, SEC 2 • GLOBAL CHANGE, ENVIRON RISK ASSESS, SUSTAINABLE LAND USE • RESEARCH
ARTICLE
Long-term leaching prediction of constituents in coal bottom ash
used as a structural fill material
Hosub Lee 1 & Gihyeon Yu 1 & Yongju Choi 1 & Eun Hea Jho 2 & Kyoungphile Nam 1
Received: 23 May 2016 / Accepted: 2 April 2017 / Published online: 8 April 2017
# Springer-Verlag Berlin Heidelberg 2017
Abstract
Purpose This study is aimed to assess the long-term leaching
of inorganic constituents from structural fills composed of
reused coal bottom ash in Korea and identify key parameters
that affect the amount of the constituents leached.
Materials and methods A model for the prediction of long-
term leaching by percolation of stormwater through a struc-
tural fill is adopted and used. The long-term leaching model is
applied to five field sites in Korea using site-specific parame-
ters obtained for each site and coal bottom ash specific param-
eters determined using column studies for two coal bottom ash
samples collected from coal-fired power plants.
Results and discussion The long-term leaching of trace inor-
ganic constituents, As, Cu, Sb, and Zn, is variable among the
sites primarily due to the variation in the total amount of
leachable constituents and application depth of a structural fill.
First-order leaching rate constant is also one of the key param-
eters when the leaching rate is relatively small. Because of the
significant variability in the leaching rate constants and appli-
cation depths, the time for the leachate constituent concentra-
tion to reach half the initial value, t50%, ranges from less than a
year to more than hundreds of years for the studied sites and
constituents.
Conclusions The long-term leaching characteristics of the
trace inorganic constituents are predicted to significantly vary
Responsible editor: Fanghua Hao
* Kyoungphile Nam
kpnam@snu.ac.kr
1
Department of Civil and Environmental Engineering, Seoul National
University, Seoul, Republic of Korea
2
Department of Environmental Science, Hankuk University of
Foreign Studies, Yongin, Gyeonggi-do, Republic of Korea
by the type of reused bottom ash and the site conditions, sug-
gesting the need to determine the model parameters in a case-
specific manner.
Keywords Application depth . Coal bottom ash . Leaching
rate . Long-term leaching . Structural fill
1 Introduction
Coal ash from power plants is one of the largest industrial
byproduct streams generated in Korea. In 2013, 2 million tons
of coal ash were generated at four major power plants in Korea
with bottom ash accounting for approximately 15% of the
total (KSEPC 2013). Since coal bottom ash has suitable phys-
ical properties for use as a public work material such as struc-
tural fill, embankment, land reclamation, road base material,
and flowable fill application (Kim et al. 2005; Benson and
Bradshaw 2011; Jayaranjan et al. 2014), approximately 10
million tons of bottom ash were reused for such applications
between 2009 and 2011 in Korea (KSEPC 2013).
For sites where coal bottom ash is applied as a structural
fill, a carefully designed site management strategy is required
to protect human health and maintain environmental sound-
ness. The reused material for structural fill is applied at a
massive amount substituting the indigenous soil. The exoge-
nous material is expected to be in contact with the surrounding
environment for almost an infinite period of time. Once a
construction project is completed, it is difficult and costly to
take measures to prevent the contaminant leaching from the
structural fill materials applied. Short-term leaching tests,
which are often employed to screen the potential hazard of
waste materials (e.g., toxicity characteristic leaching proce-
dure) may over- or under-estimate the potential leachability
of constituents in wastes and result in misled decisions for
J Soils Sediments (2017) 17:2742–2751
their beneficial use (Kosson et al. 2002). Therefore, the long-
term effect by the application of coal bottom ash as a structural
fill should be evaluated in lieu of the screening assessment by
short-term leaching tests.
Recently, long-term leaching prediction programs such as
Leach Expert System (LeachXS™) and Industrial Waste
Management Evaluation Model (IWEM) have been devel-
oped to support decisions for the reuse of industrial wastes
as landfill, surface impoundment, or structural fill. Both
modeling programs are relatively complicated as they employ
sub-models to simulate geochemical speciation of chemicals
and mass transport processes (e.g., ORCHESTRA), and apply
probabilistic methods (e.g., Monte Carlo). A range of input
parameters should be determined for the application of such
models, resulting in significant time and cost requirements to
obtain case-specific values, or the use of default values (Van
der Sloot et al. 2008; USEPA 2015) which may be unrealistic.
This calls for the establishment of a simpler model with input
parameters easily available from routinely measured data set
or from relatively simple laboratory tests.
In this study, long-term (e.g., 100 years) leaching of trace
constituents from coal bottom ash used as a structural fill
material is predicted for five study sites in Korea using two
different coal bottom ash samples obtained from coal-fired
power plants. A simple model for the long-term leaching pre-
diction available in the literature is adopted with coal bottom
ash and site-specific parameters determined in this study. By
comprehensive analysis of the model and the case study re-
sults, the sensitivity and variability of the predicted results
according to the changes in each input parameter are studied.
2 Materials and methods
2.1 Coal bottom ash samples
Coal bottom ashes were collected from two coal-fired power
plants, YD and YH, in Korea. The collected ashes were air
dried, homogenized, sieved with a 2-mm-size mesh, and kept
in air-tight containers. Major constituents of the two coal bot-
tom ashes were analyzed by X-ray fluorescence (XRF; S4
Pioneer, Bruker AXS, Germany). Total contents of trace inor-
ganic constituents in the ashes, heavy metals and metalloids,
were analyzed by extracting the samples using microwave-
assisted acid digestion following U.S. Environmental
Protection Agency (USEPA) method 3052 and analyzing the
extract using ICP-OES (iCAP 7400 Duo, Thermo Scientific,
Waltham, MA, USA).
2.2 Long-term leaching scenario and the prediction model
For prediction of long-term contaminant leaching from the
coal bottom ash structural fill, it was assumed that the
2743
structural fill itself is permeable and is capped with a layer
that allows partial infiltration of the precipitation that falls on
the surface. In this situation, percolation of stormwater is the
dominant process for long-term contaminant leaching
(Kosson et al. 2002). The contaminant concentration in the
leachate released at the bottom of the structural fill was as-
sumed to decrease exponentially with a leaching rate constant,
κ (kg L−1), which can be determined by laboratory column
studies:
C ðL=SÞ ¼ C ð0Þ∙e−κ∙ðL=SÞ ð1Þ
where C is the concentration in the leachate and L/S (L kg−1)
is the cumulative liquid to solid (i.e., percolated water volume
to structural fill dry mass) ratio.
Reports issued by National Institute for Public Health and
the Environment of the Netherlands (RIVM) in 1996 (Aalbers
et al. 1996) and 2007 (Verschoor et al. 2007) provides a solu-
tion for this scenario with parameters describing the charac-
teristics of the structural fill material (i.e., coal bottom ash in
this study) and site conditions. The cumulative contaminant
mass released over time t (year) at the bottom of the structural
fill, It (mg m−2), can be calculated by (Aalbers et al. 1996;
Verschoor et al. 2007)


1−e−κ∙ d∙h
t∙inf
I t ¼ E L=Slab ∙d∙h∙ ð2Þ
ð1−e−κ∙L=Slab Þ
where EL=Slab (mg kg−1) is the total cumulative contaminant
mass leached in laboratory column studies; L/Slab (L kg−1) is
the total liquid to solid ratio applied for the laboratory column
studies; d (kg m−3) and h (m) are the bulk density and depth of
the structural fill, respectively; and inf (mm year−1) is the
stormwater infiltration rate at the site.
From Eq. (2), the mathematical expression for the leachate
contaminant concentration at time t, Ct (mg m−3), is obtained
as
e−κ∙ð d∙h Þ
t∙inf
C t ¼ EL=Slab ∙κ∙ ð3Þ
1−e−κ∙L=Slab
From Eq. (3), the time for the leachate contaminant con-
centration to reach half the initial value, t50% (in years), can be
derived for a specific fill material and for a specific site con-
dition. The t50% is expressed as
1 d∙h
t 50% ¼ ∙ ∙ln2 ð4Þ
κ t∙inf
2.2.1 Coal bottom ash specific parameters
The parameters describing the characteristics of coal bottom
ash, i.e., coal bottom ash specific parameters, are the total
2744
contaminant mass leached from the material in laboratory col-
 
umn studies E L=Slab and the leaching rate constant (κ) for
contaminants of potential concern (COPCs), and the bulk den-
sity of coal bottom ashes (d). As will be discussed in the Results
and discussion section, arsenic (As), antimony (Sb), copper
(Cu), and zinc (Zn) are selected as COPCs in this study.
Column tests were conducted following ISO/TS 21268-3
Bup-flow percolation test^ procedure (ISO 2007) to determine
E L=Slab and κ for YD and YH coal bottom ashes. Triplicate
column runs were conducted for each bottom ash sample.
Columns with a length of 250 mm and an inner diameter of
50 mm were used. Filter discs with a pore size of 47 mm were
placed at both ends of the packed material. Deionized water
was introduced at a flow rate of 0.2 mL min−1 using a peri-
staltic pump connected to the column inlet. After 96 h of
equilibration period, the column eluates were sampled at
L/Slab (ratio of eluate volume to packed coal bottom ash mass)
intervals of 0–0.1, 0.1–0.2, 0.2–0.5, 0.5–1, 1–2, 2–5, 5–10,
10–20, and 20–40 L kg−1. The collected eluates were filtered
using 0.45 μm GHP syringe filter and kept at 4 °C prior to
analysis. The samples were analyzed using ICP-MS (Varian
820-MS, Varian, Australia).
E L=Slab for each COPC was calculated by summing up the
COPC mass in all eluate samples collected up to an L/Slab of
40 L kg−1. The κ value was determined as the best-fit value of
the following equation:
h i
E L=S ¼ E L=Slab 1−e−κ∙ðL=SÞ ð5Þ
where EL/S (mg kg−1) is the cumulative contaminant mass
leached for the L/S at the end of each sampling interval.
Bulk densities of YD and YH coal bottom ash were calculated
by dividing the mass of the ashes by packing volume for the
triplicate columns.
2.3 Case study sites and site-specific parameters
Five sites in Korea where coal ash has been or will be applied
as a structural fill, Yeosu, Namhae, Mockpo, Busan, and
Gunsan (Lee 2011; DEC 2014), were studied for long-term
leaching of the COPCs.
The parameters describing the characteristics of site condi-
tions, i.e., site-specific parameters, are infiltration rate (inf)
and depth of application (h). Application depths of structural
fills for construction projects in Korea show significant varia-
tion and were not available for any of the study sites. As a
conservative estimate, application depths were assumed to be
equal to the depth of local groundwater table available in
MOLIT and K-Water (2014) for each site. USEPA (2015)
specified that the depth of a structural fill should be above
the local groundwater table to protect groundwater from fill
material leachate. Year-averaged precipitation data were
J Soils Sediments (2017) 17:2742–2751
obtained for each study site, and the infiltration rate was cal-
culated as 14.44% of the local precipitation rate following
MOLIT (2012) which suggested the default value of ground-
water recharging rate in Korea from nationwide survey results.
The infiltration rate and depth of application determined for
the study sites are listed in Table 1.
It should be noted that applying 14.44% as the infiltration-
to-precipitation ratio to obtain the local infiltration rate is a
very rough estimation. The actual infiltration-to-precipitation
ratio should widely vary from site to site. A bottom ash-based
structural fill without any cover is expected to have an
infiltration-to-precipitation ratio in the range of 40–70% con-
sidering the suggested runoff coefficient range of 0.30–0.60
for a bare packed soil with a smooth surface in the literature
(Goldman et al. 1986). This study used a much smaller ratio
than the expected value for an uncovered structural fill by
assuming the presence of a low permeability cap or an instal-
lation of an overlying structure. For decision-making pur-
poses, a site-specific determination of an infiltration rate ac-
counting for the presence and characteristics of an overlying
structure or a cap, surface slope, permeability of the structural
fill, and the local precipitation patterns (e.g., intensity and
duration of a storm event) is required.
2.4 Sensitivity and variability analysis
Sensitivity of the cumulative contaminant mass released over
100 years at the bottom of the structural fill (I100yr) to the coal
bottom ash and site-specific parameters was studied. Default
parameters used for the sensitivity analysis were the average
values of EL=Slab , κ, and d determined for the YD and YH coal
bottom ashes, and nationwide average values of groundwater
table depth and precipitation rate in Korea. The sensitivity
index (S(Xi); %) of I100yr to each parameter Xi was obtained
by (Webster et al. 1998; Dalla Valle et al. 2007)
∂I 100yr X i
S ðX i Þ ¼ ∙ ∙100 ð6Þ
I 100yr ∂X i
The variability of I100yr due to the range of the parameters
obtained for the study sites and the YD and YH coal bottom
ashes was also studied. In this case, the average values of
Table 1 Depth of application and infiltration rate determined for the
five study sites for the prediction of long-term leaching
Sites Depth of application (m) Infiltration rate (mm year−1)
Namhae 8.5 266
Busan 4.5 219
Yeosu 3.4 208
Gunsan 2.6 174
Mockpo 2.3 168
J Soils Sediments (2017) 17:2742–2751 2745

E L=Slab , κ, and d for the two bottom ash samples, and the Table 3 Composition of trace inorganic compounds in YD and YH
coal bottom ash samples. Values are shown as mean ± standard deviation
average values of inf and h for the five study sites were used of triplicate measurements
to constitute a default case. By variation of the parameters
from a minimum to a maximum value, the range of I100yr Contaminants Total concentration (mg kg−1)
according to the changes in the parameters was obtained.
YD YH

Antimony 15 ± 9.1 18 ± 1.9

Arsenic 8.4 ± 12 17 ± 0.91
3 Results and discussions
Beryllium 4.1 ± 0.11 N.D.
Cadmium 0.67 ± 0.29 5.0 ± 0.35
3.1 Chemical composition of coal bottom ash samples
Chromium VI N.D. N.D.
The chemical composition of YD and YH coal bottoms ash Cobalt 35 ± 0.91 48 ± 1.6
samples analyzed in this study is similar to those reported in Copper 160 ± 130 44 ± 4.0
previous studies as shown in Table 2. SiO2, Al2O3, Fe2O3, and Fluoride N.D. N.D.
CaO are identified as major constituents, accounting for 80% Lead 29 ± 0.96 24 ± 0.93
of the total by weight. Some trace inorganics are detected in Mercury N.D. N.D.
the bottom ash samples as shown in Table 3. Of those, arsenic Molybdenum 120 ± 6.3 N.D.
(As), antimony (Sb), copper (Cu), and zinc (Zn) are selected Selenium N.D. N.D.
as study COPCs. The selection of the study COPCs is based Vanadium 140 ± 4.2 170 ± 2.8
on the following criteria: (i) the exceedance of the screening Zinc 29 ± 5.8 35 ± 0.56
level for coal combustion waste landfill suggested by USEPA
N.D. not detected
(2015), (ii) representation of both anionic and cationic trace
constituents in the samples, which may exhibit differential
long-term leaching behavior (Cornelis et al. 2008; Neupane and Donahoe 2013), and (iii) ensuring the detectability in the
column studies.
Table 2 Major chemical constituents and their composition (in weight)
for YD and YH coal bottom ash samples
3.2 COPC leaching characteristics from coal bottom ash
Constituents Contents (%)
The cumulative COPC mass leached from YD and YH coal
YD YH Literature value
bottom ashes in column studies is plotted against L/S in Fig. 1.
SiO2 51 52 39–70a,b,c,d,e,f,g,h,i,j,k,l The COPCs in cationic form, Cu and Zn, generally exhibited
Al2O3 24 23 11–28a,b,c,d,e,f,g,h,i,j,k,l faster leaching behavior than those in anionic form, As and
Fe2O3 15 12 4.7–25a,b,c,d,e,f,g,h,i,j,k,l Sb. For example, 39 and 65% of total Zn leached in the entire
CaO 5.2 4.7 1.1–18a,b,c,d,e,f,g,h,i,j,k,l column run (L/S = 40 L kg−1) are leached within an L/S of
TiO2 1.6 1.8 0.44–1.5a,b,c,d,e,g,h,i 0.1 L kg−1 for YD and YH coal bottom ashes, respectively. On
K2O 1.4 1.5 0.20–5.3a,b,c,d,e,g,h,i,j,k,l the other hand, only 1.6 and 0.070% of As are leached within
MgO 0.85 1.3 0.38–5.2a,b,c,d,e,f,g,h,i,j,k,l an L/S of 0.1 L kg−1 for YD and YH coal bottom ashes,
Na2O 0.48 1.6 0.10–1.3a,b,c,d,e,f,g,h,i,j,k,l respectively. As a result, the leaching rate constants (κ) for
the cationic compounds are greater than those for the anionic
a
Liu et al. (2004) compounds by an order of magnitude or greater. One excep-
b
Depoi et al. (2008) tion is the leaching rate constant for Cu in YH coal bottom ash,
c
Wang et al. (2008) which is comparable to those for anionic compounds in both
d
Durgun and Genc (2009) coal bottom ashes.
e
Levandowski and Kalkreuth (2009) The total cumulative COPC mass leached from the column
f
 
Geetha and Ramamurthy (2010) studies E L=Slab is determined for each COPC and coal bot-
g
Arenas et al. (2011) tom ash as shown in Table 4. The E L=Slab values are 1.0 and
h
Skousen et al. (2012) 1.5% of total contents for As, 0.14 and 1.4% for Cu, 3.0 and
i
Menendez et al. (2013) 3.7% for Sb, and 0.43 and 7.9% for Zn for YD and YH coal
j
Tiwari et al. (2014) bottom ashes, respectively. These results suggest that most of
k
Arenas et al. (2015) the COPCs are strongly bound to the coal bottom ashes such
l
Asokbunyarat et al. (2015) that only small fractions are leachable by percolation of water.
2746
Fig. 1 Cumulative mass of
COPCs leached from YD and YH
coal bottom ashes in column
studies plotted against L/S for a
As, b Cu, c Sb, and d Zn. The
error bars represent standard de-
viation of triplicate measurements
The EL=Slab and κ values for the two bottoms ash
samples are significantly different from each other. Up
to two orders of difference in the parameter values are
found for the same COPC in YD and YH coal bottom
ashes. Coals used in the two power plants are obtained
from different sources (actual sources of coals for each
plant cannot be listed in this paper due to confidential-
ity reasons), which should result in different contents
and leaching behavior of the COPCs. Even for the same
type of coal obtained from the same location, bottom
ash with different physicochemical properties can be
obtained according to the boiler design and operating
conditions (Ratafia-Brown 1994; Meij and Winkel
2007). The substantial variations of the EL=Slab and κ
values for different coal bottom ashes indicate that ac-
tual laboratory measurements are needed to determine
the values for each sample.
 
Table 4 The total cumulative COPC mass leached E L=Slab and the leaching rate (κ) of each COPC for YD and YH coal bottom ashes determined by
−1
the column studies with a total L/S of 40 L kg . Values are shown as mean ± standard deviation of triplicate measurements
COPCs Total cumulative mass leached, E L=Slab (mg kg−1)
YD
As 0.085 ± 0.005
Cu 2.2 ± 0.8
Sb 0.56 ± 0.09
Zn 2.3 ± 0.2
J Soils Sediments (2017) 17:2742–2751
3.3 Sensitivity of COPC leaching to model parameters
The sensitivity indices of the cumulative mass of 100 year
COPC leaching (I100yr) to the model parameters are shown
in Table 5. For all COPCs, the sensitivity indices are 100%
for E L=Slab , indicating the significance of this parameter for
the estimation of long-term leaching from coal bottom ash.
A sensitivity index of 100% indicates that I100yr is linearly
proportional to a given parameter. It is not surprising that
the sensitivity index for E L=Slab is 100% since Eq. (2) shows
that the cumulative mass of COPC leaching (i.e., It) should
be linearly proportional to E L=Slab when other parameters
are fixed.
The sensitivity indices for other parameters, leaching rate
constant, bulk density, application depth, and infiltration rate,
are variable for different COPCs. Cationic compounds, Cu
and Zn, show very low sensitivity to the leaching rate constant
Leaching rate constant, κ (kg L−1)
YH YD YH
0.25 ± 0.10 0.16 ± 0.01 0.020 ± 0.001
0.060 ± 0.044 4.9 ± 2.5 0.054 ± 0.047
0.54 ± 0.07 0.36 ± 0.02 0.079 ± 0.008
0.15 ± 0.07 4.5 ± 0.2 11 ± 6
J Soils Sediments (2017) 17:2742–2751
Table 5 Sensitivity index (%) of cumulative COPC mass leached from a coal bottom ash structural fill in 100 years (I100yr) for long-term leaching
model parameters
Parameter (Xi) Sensitivity index, S (%)
As
Total mass leached, E L=Slab 100
Leaching rate constant, κ 66
Dry bulk density, d 23
Application depth, h 23
Infiltration rate, inf 77
and the infiltration rate. Because of the relatively high
leaching rate constants for these compounds, most of the com-
pounds leachable from coal bottom ash are released from a
structural fill within 100 years. As a result, leaching kinetics
does not play a significant role in the I100yr values for Cu and
Zn. The I100yr values for these compounds are highly depen-
dent on the total amount of leachable COPCs from a structural
fill, which is determined by E L=Slab , bulk density, and applica-
tion depth of the coal bottom ash. The sensitivity indices for
Cu and Zn are 100% not only for E L=Slab but also for bulk
density and application depth as shown in Table 5.
However, for anionic compounds As and Sb, kinetics also
play a significant role in long-term leaching. The sensitivity
indices for leaching rate constant and the infiltration rate are
50% or greater for these compounds. Other parameters, bulk
density and application depth, still significantly contribute to
the I100yr values for As and Sb, although the sensitivity indices
are smaller than those for Cu and Zn.
In sum, sensitivity of long-term leaching from a coal bot-
tom ash structural fill to each parameter depends on the
leaching characteristics of COPCs. For compounds showing
relatively rapid leaching characteristics, long-term leaching is
almost completely governed by the total COPC leachable from
a structural fill. In this case, bulk density and application depth
of a coal bottom ash are significant for the long-term leaching.
For compounds with relatively slow leaching characteristics,
parameters relevant to leaching kinetics, leaching rate constant
and infiltration rate, should be considered in addition to bulk
density and application depth. For any cases, the total cumu-
lative mass leached in laboratory studies, EL=Slab , acts as a key
parameter for long-term leaching of COPCs.
3.4 Long-term leaching prediction for case study sites
3.4.1 Long-term COPC leaching behavior
The long-term cumulative COPC masses leached from a
structural fill significantly vary for each site because of
the differences in site-specific parameters, i.e., infiltration
rate and depth of application. The predicted It for YD coal
2747
Cu Sb Zn
100 100 100
0.001 50 0.000
100 50 100
100 50 100
0.001 50 0.000
bottom ash applied at the four study sites is plotted
against time in Fig. 2.
For Cu and Zn which exhibit relatively high leaching rates,
the It value reaches a plateau after 20 years or shorter, indicating
negligible leaching of the COPCs from a structural fill after
20 years. In case when the same coal bottom ash is applied
(i.e., fixed EL=Slab , κ, and d), the plateau value of It should
depend solely on the application depth. Thus, the variation in
It among different sites after 20 years or longer for Cu and Zn in
Fig. 2 represents the difference in the application depth.
Namhae has the greatest application depth of 8.5 m, resulting
in the greatest value of It for Cu and Zn in the long term.
For As and Sb which show relatively low leaching rates,
kinetics play a role in the long-term leaching behavior for all
study sites. As can be seen from Eq. (2), following parameter
determines the kinetic state of leaching at time t for each site
when the same coal bottom ash is applied (i.e., fixed value of
κ) (Hjelmar 1990; Kosson et al. 2002):
inf ∙t
L=Sfield ¼ ð7Þ
d∙h
where L/Sfield (L kg−1) is the cumulative volume of leachate
percolated through a structural fill at t (year). The L/Sfield
value is the smallest for Namhae (4.8 L kg−1 for t = 100 years)
and the greatest for Mockpo (11 L kg−1 for t = 100 years). As a
result, it is seen from Fig. 2 that the It value reaches a plateau
for Sb in Mockpo within 100 years, while the result for Sb in
Namhae shows a continuous increase with time even after
100 years.
The long-term cumulative COPC masses released is also
variable for the different coal bottom ashes because of the
significant variation in the coal bottom ash specific parame-
ters, E L=Slab and κ, observed in the column studies. The pre-
dicted It values for YD and YH coal bottom ashes are plotted
against time for Namhae site in Fig. 3. For Zn which exhibits
relatively high leaching rate constants for both coal bottom
ash samples, the I100yr value for YD is a factor of 37 greater
than that for YH as E L=Slab is a factor of 37 greater for YD. For
Cu, the It reaches a plateau after approximately 20 years for
2748 J Soils Sediments (2017) 17:2742–2751

Fig. 2 Predicted changes in the

cumulative COPC masses
leached (It) over 100 years and for
the five study sites for a As, b Cu,
c Sb, and d Zn

YD while it continuously increases for the entire time of sim-
ulation for YH because of the much higher leaching rate con-
stant for YD than that for YH. These results indicate that the
difference in EL=Slab and κ significantly affects the long-term
COPC leaching characteristics from a structural fill, and thus,
these parameters should be assessed for the specific type of
coal bottom ash used at a site.
3.4.2 Time scale for COPC leaching from a structural fill
The time for the leachate contaminant concentration to reach
half the initial value, t50%, obtained for the COPCs and the two
coal bottom ashes is shown in Table 6. In some cases, the t50%
values are in the order of years or shorter. In these cases, the
leachate concentration approaches close to zero after a few

Fig. 3 Predicted changes in the

cumulative COPC masses
leached (It) over 100 years for YD
and YH coal bottom ashes for a
As, b Cu, c Sb, and d Zn at
Namhae site
J Soils Sediments (2017) 17:2742–2751 2749

Table 6 Time for the leachate

contaminant concentration to COPCs t50% (years)
reach half the initial value, t50%,
determined for the COPCs and for Namhae Busan Yeosu Gunsan Mockpo
YD and YH coal bottom ashes
YD YH YD YH YD YH YD YH YD YH

As 89 644 57 410 45 326 41 297 39 280

Cu 4.0 >700 2.0 >700 2.0 >700 2.0 >700 2.0 >700
Sb 39 168 25 107 20 85 18 78 17 73
Zn 3.0 1.0 2.0 <1.0 2.0 <1.0 1.0 <1.0 1.0 <1.0

years to 20 years at most and no significant leaching of the 1 d∙h 100%

COPCs is expected afterwards. In other cases, the t50% values
are in the order hundreds of years or longer. In these cases, the
COPCs are released steadily from a structural fill without sub-
stantial reduction in the leachate concentration for decades or
even longer.
Both the coal bottom ash and site-specific parameters de-
termine t50%. As can be seen from Eq. (4), t50% is proportional
to the site-specific parameters d and h, and inversely propor-
tional to the coal bottom ash specific parameter κ and the site-
specific parameter inf. The t50% value is an integrative param-
eter for kinetics of leaching from a structural fill. Actually, a
tp% value can be determined for any p% reduction of the
leachate concentration from the initial value as
t p% ¼ ∙ ∙ln ð5Þ
κ t∙inf ð100−pÞ%
and used as a reference to determine (i) the time span re-
quired for the site monitoring program and (ii) the design
period for the leachate mitigation measures at the site, when
such measure are taken.
3.4.3 Effect of model parameters on long-term leaching
The variation of the I100yr value for the range of coal bottom
ash and site-specific parameter values obtained in this study is
shown in Fig. 4. In general, E L=Slab , κ, and h are identified as

1.0.E-01 1.0.E+00 1.0.E+01 1.0.E-01 1.0.E+00 1.0.E+01

(a) (b)
Rate constant ( ) Rate constant ( )

Total mass Total mass

leached ( ) leached ( )

Bulk density ( ) Bulk density ( )

Depth of application ( ) Depth of application ( )

Infiltration rate ( ) Infiltration rate ( )

1.0.E-01 1.0.E+00 1.0.E+01 1.0.E-01 1.0.E+00 1.0.E+01

(c) (d)
Rate constant ( ) Rate constant ( )

Total mass Total mass

leached ( ) leached ( )

Bulk density ( ) Bulk density ( )

Depth of application ( ) Depth of application ( )

Infiltration rate ( ) Infiltration rate ( )

Fig. 4 Variation of I100yr for a As, b Cu, c Sb, and d Zn due to the change in each parameter from the average value to the maximum or minimum value
obtained in this study
2750
key parameters for long-term COPC leaching from a coal
bottom ash applied structural fill.
E L=Slab is a key parameter for most cases because of the large
variability of the value for the two coal bottom ashes studied
and high sensitivity of I100yr to the parameter. The κ value is
also a key parameter as long as the value is sufficiently small
such that the kinetics of leaching affect I100yr. When the long-
term leaching is not governed by kinetics because of the large κ
value, as in the case of Zn (Fig. 4d) and the upper end of Cu
(Fig. 4b), the parameter does not affect the I100yr value at all.
Depth of application, h, is also identified as a key parameter
for the long-term leaching because of its significant variation
among study sites and its influence on both total leachable
COPC mass and leaching kinetics. Actually this is a parameter
that can be controlled or regulated for a certain coal bottom ash
and for a certain site. Once a quantitative criterion for long-term
COPC leaching from a coal bottom ash structural fill is deter-
mined, the limiting value of the depth of application can be
derived for a specific case of application. For example, RIVM
of the Netherlands regulates that the increment in I100yr due to
the replacement of the natural soil with construction materials
should not exceed 1% of the total amount of a COPC in 1 m
soil layer underneath the materials applied (Verschoor et al.
2007). From this criterion, the maximum depth allowed as a
structural fill can be calculated from Eq. (2) with parameters
determined for a specific coal bottom ash and site conditions.
The effects of coal bottom ash bulk density and infiltration
rate on the I100yr value are not as pronounced as those of other
parameters. Bulk density is not likely to significantly vary for
different coal bottom ashes. The relative insignificance of in-
filtration rate to the I100yr value is due to the use of a uniform
infiltration-to-precipitation ratio of 14.44% and a relatively
small variation in precipitation rates among the study sites
(within 30% of the average value). Although not taken into
account in this study, the infiltration-to-precipitation ratio de-
pends on many site-specific factors including the presence and
characteristics of an overlying structure or a cap, surface slope,
permeability of the structural fill, and the local precipitation
patterns (e.g., intensity and duration of a storm event), and
may widely vary from site to site. Because long-term leaching
exhibits high sensitivity to infiltration rate for COPCs with
relatively slow releasing characteristics (e.g., As and Sb in
the current study), infiltration rate should still be considered
as a key parameter for those bottom ash constituents.
4 Conclusions
Long-term leaching characteristics of As, Cu, Sb, and Zn from
structural fill composed of reused coal bottom ash are studied.
For the two bottom ash samples analyzed, the cationic trace
constituents studied, Zn and Cu, generally exhibited faster
J Soils Sediments (2017) 17:2742–2751
leaching rates than the anionic constituents, As and Sb. The
leaching parameters for the study COPCs from the bottom ash
samples vary by up to two orders of magnitude, suggesting the
need to experimentally determine the leaching characteristics
for each coal bottom ash to be applied. Prediction of long-term
leaching of the study COPCs at five sites in Korea show sig-
nificant variation in cumulative amount of COPC leaching
depending primarily on the total amount of leachable COPC
in coal bottom ash and application depth of a structural fill.
Leaching rate constant is also a significant factor when the
value is relatively small that the long-term leaching is kineti-
cally controlled. The time for the leachate COPC concentra-
tion to reach half the initial value, ranges from less than a few
years to more than a hundred years due to the significant
variation in the leaching rate constants and application depths.
Acknowledgements This study received financial support from the
Geo-Advanced Innovative Action (GAIA) project of the Korea
Environmental Industry and Technology Institute. We thank the
Integrated Research Institute of Construction and Environmental
Engineering, Seoul National University, and Water/Environment
Research Team of Hyundai Engineering and Construction Co., LTD.
for technical assistance.
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