Environ Sci Pollut Res (2014) 21:774–780
DOI 10.1007/s11356-013-2138-3
SHORT RESEARCH AND DISCUSSION ARTICLE
Amelioration of acidic soil using various renewable
waste resources
Deok Hyun Moon & Yoon-Young Chang & Yong Sik Ok &
Kyung Hoon Cheong & Agamemnon Koutsospyros &
Jeong-Hun Park
Received: 30 December 2012 / Accepted: 6 September 2013 / Published online: 28 September 2013
# Springer-Verlag Berlin Heidelberg 2013
Abstract In this study, improvement of acidic soil with re-
spect to soil pH and exchangeable cations was attempted for
sample with an initial pH of approximately 5. Acidic soil was
amended with various waste resources in the range of 1 to
5 wt.% including waste oyster shells (WOS), calcined oyster
shells (COS), Class C fly ash (FA), and cement kiln dust
(CKD) to improve soil pH and exchangeable cations. Upon
treatment, the soil pH was monitored for periods up to
3 months. The exchangeable cations were measured after
1 month of curing. After a curing period of 1 month, a maize
growth experiment was conducted with selected-treated sam-
ples to evaluate the effectiveness of treatment. The treatment
results indicate that in order to increase the soil pH to a value
of 7, 1 wt.% of WOS, 3 wt.% of FA, and 1 wt.% of CKD are
required. In the case of COS, 1 wt.% was more than enough to
increase the soil pH value to 7 because of COS's strong
Responsible editor: Zhihong Xu
D. H. Moon (*) : K. H. Cheong
Department of Environmental Engineering, Chosun University,
Gwangju 501-759, Republic of Korea
e-mail: dmoon10@hotmail.com
Y.<Y. Chang
Department of Environmental Engineering, Kwangwoon University,
Seoul 139-701, Republic of Korea
Y. S. Ok
Department of Biological Environment, Kangwon National
University, Chuncheon 200-701, Republic of Korea
A. Koutsospyros
Mechanical, Civil and Environmental Engineering,
University of New Haven, West Haven, CT 06516, USA
J.<H. Park
Department of Environmental Engineering, Chonnam National
University, Gwangju 500-757, Republic of Korea
alkalinity. Moreover, the soil pH increases after a curing
period of 7 days and remains virtually unchanged thereafter
up to 1 month of curing. Upon treatment, the summation of
cations (Ca, Mg, K, and Na) significantly increased. The
growth of maize is superior in the treated samples rather than
the untreated one, indicating that the amelioration of acidic
soil is beneficial to plant growth, since soil pH was improved
and nutrients were replenished.
Keywords Acidic soil . Soil pH . Exchangeable cations .
Oyster shells . Fly ash . Cement kiln dust
Introduction
Soil acidity is a serious problem in Korea with well-
documented adverse effects on soil productivity and plant
growth. Reportedly, low soil pH is responsible for poor plant
growth yields due to the deficiencies and toxicities associated
with a number of elements (Blamey and Chapman 1982; Ok
et al. 2007). Atmospheric deposition containing SOx and NOx
is one of the major reasons for soil acidification. Heavy
industrialization has caused a gradual increase in acid deposi-
tion since the late 1970s (Kim 2005). The annual mean rain
pH near Seoul, Korea has ranged between 4.2 and 4.8 for the
past two decades. The wet deposition of the total acid ions
including H+, SO42−, NO3−, and Cl− is 2.9 keq ha−1 year−1,
with SO42− representing 60 % of the total acid ions (Kim
2005; Rhyu and Kim 1994; Yang et al. 2009). Furthermore,
most soils in Korea derive from parent materials mainly
consisting of granite and granite gneiss which are likely to
be more acidic than the soil generated from calcareous shale or
limestone.
Various renewable waste resources such as waste oyster
shells (WOS), calcined oyster shells (COS), Class C fly ash
(FA), and cement kiln dust (CKD), are used in this study as
Environ Sci Pollut Res (2014) 21:774–780 775

soil conditioning additives in order to ameliorate the acidic Table 1 Physicochemical and mineralogical properties of the acidic soil
soil. WOS are generated at an annual rate of approximately Soil properties Acidic soil
250,000 t/year in Ton-young, Keoje, and Kosung, Korea.
Fifty percent of the WOS are used to seed oyster beds and Soil pH 5.2±0.21
10 % are recycled as fertilizers. Moreover, 40 % of the WOS Organic matter content (%)a 7.6
are discarded in coastal areas causing both serious odor prob- Cation exchange capacity (meq/100 mg)b 8.82
lems and environmental degradation (Lim et al. 2013; Ok Composition (%)c
et al. 2010). The beneficial reuse of WOS as a soil conditioner Sand 97.5
provides a sustainable solution for two environmental prob- Silt 1.6
lems simultaneously. The COS are generated by the calcina- Clay 0.9
tion process of WOS at 900 °C for 2 h. The main phase in the Textured Sand
WOS is calcite (CaCO3) transformed into quicklime (CaO) Mineral compositions Quartz
upon calcination. Lime has been frequently used to ameliorate Kaolinite
acidic soil to increase crop yields (Adams 1984). Muscovite
FA and CKD are widely used as amendments to immobi- Microcline
lize heavy metals in contaminated soils (Moon and Dermatas Cristobalite
2007; Moon et al. 2008). Moreover, it has been reported that
a
FA is beneficial in improving soil structure and water holding Organic matter content (%) was calculated from measured loss-on-
ignition (Ball 1964; FitzPatrick 1983)
capacity (Chang et al. 1977; Khan and Khan 1996). FA has b
Cation exchange capacity (CEC) measured by USEPA method
also been reported to enhance soil fertility (Elseewi et al.
9081(USEPA 1986)
1980; Ghodrati et al. 1995). FA and CKD may be used to c
Sand, 50–2,000 μm; silt, 2–50 μm; clay, <2 μm
increase soil pH as they are alkaline materials known to d
Soil texture suggested by the United States Department of Agriculture
contain alkaline (K) and alkaline earth (Ca and Mg) metals (USDA)
which are essential elements for plant growth (Kumpiene et al.
2007).
Following the amelioration of the acidic soil using various Amelioration agents
renewable waste resources, maize growth experiments were
performed to assess the potential benefit of the ameliorated WOS were collected from Tong-young, Korea and pulverized
acidic soil to plant growth. Maize, a very important feedstock to pass through a #20-sieve (0.853 mm). The WOS calcination
for humans and animals, has been reported to grow well in the process was conducted at 900 °C for 2 h to activate the
pH range of 6.5∼8 (IITA 1982). Therefore, any soil pH quicklime in the calcite and create the COS. FA and CKD
outside of this range may adversely affect its growth.
The objective of this study is to investigate the effective-
ness of the ameliorated acidic soil with various renewable Table 2 Physicochemical properties of the acidic soil and various waste
waste resources. The effectiveness of amelioration of the resources
acidic soil is evaluated in terms of soil pH, exchangeable
Chemical properties Soil WOS COS FA CKD
cations, and maize growth upon treatment.
SiO2 61.0 3.51 2.59 38.2 18.8
Al2O3 19.8 1.36 0.96 19.8 6.06
TiO2 0.72 0.07 0.05 – –
Experimental methodology Fe2O3 4.56 0.53 0.40 5.11 2.66
MnO 0.07 0.04 0.04 – –
Acidic soil MgO 0.70 0.71 0.86 3.86 3.78
CaO 0.21 88.1 87.7 21.4 55.5
Acidic soil was obtained from a fruit garden in the Na2O 0.22 0.86 0.73 2.04 0.67
Chungcheongnam-do Province, Korea at a depth of 0–30 cm K2O 4.67 0.27 0.13 0.65 3.78
below the ground surface. The collected acidic soil was sieved P2O5 0.24 0.28 0.25 – –
through a #10-mesh (2 mm) to remove large particles and to SO3 0.04 0.69 0.65 2.2 8.88
provide homogeneous fractions of the soil. Physicochemical LOI 7.6 2.9 5.1 2.2 0.9
and mineralogical characterization information of the acidic pH (1:5) 5.02 10.5 12.4 11.9 12.8
soil is presented in Table 1. The bulk chemistry of the acidic
soil measured using x-ray fluorescence (XRF) is presented in Oxide values expressed in percentages by mass
Table 2. LOI loss on ignition
776 Environ Sci Pollut Res (2014) 21:774–780

were obtained from the American Fly Ash Company
(Naperville, IL, USA) and Lafarge North America
(Whitehall, PA), respectively. These materials were also used
as amelioration agents since these agents were widely used for
the stabilization of contaminated soil; the physicochemical
properties of WOS, COS, FA, and CKD are presented in
Table 2.
Treatment
The acidic soil was treated with the sole addition of WOS,
COS, FA, and CKD in the range of 1 to 5 wt.%. All treatments
were cured for 7, 14, 21 days, 1, and 3 months. A liquid to
solid ratio of 0.2 was used to ensure full hydration. A specific
treatment matrix is presented in Table 3.
accordance with the Korean Standard Test (KST) meth-
od with a L/S ratio of 5:1. The bulk chemistry of the
acidic soil and various waste resources was measured
using XRF (ZSX100e, Rigaku). The exchangeable cat-
ions were measured in accordance with the KST method
and the extracted solutions were analyzed by inductively
coupled plasma mass spectrometry (Agilent 7500ce,
USA). All sample analyses were performed in triplicate
and the averaged values were reported only if the indi-
vidual measurements were within an error of 10 %. Two
different quality control standards and recovery spikes
were used to monitor the accuracy and performance of
the equipment.
X-ray powder diffraction analyses

Maize growth experiment
Following 1 month of curing, after the treatment of the acidic
soil, three maize seeds (Miniheukchal, Lot no. 124201)
obtained from the Jinheung nursery company (Korea) were
sown in a small pot containing the following samples: control,
3 wt.% WOS, 1 wt.% COS, 3 wt.% FA, and 2 wt.% CKD. The
soil pH varied in the range of 7 to 8 for all sample variants
except for the sample treated with 1 wt.% COS that resulted in
a soil pH higher than 8. The pot had three holes (diameter
about 7 mm) on the bottom and a plastic screen was placed on
the bottom of the pot to prevent the soil loss. In addition, the
pot had the following dimensions: height of 7 cm, top inner
diameter of 5 cm, and bottom diameter of 4.8 cm.
The mineralogy of the acidic soil was analyzed by x-ray
powder diffraction (XRPD) analyses. The acidic soil was
air-dried and pulverized to pass through a #200-sieve.
Step-scanned x-ray diffraction patterns were collected
using a PANalytical XRD instrument (X'Pert PRO
MPD). XRPD analyses were conducted at 40 kV and
30 mA using a diffracted beam graphite-monochromator
with Cu radiation. The XRPD patterns were collected at
2θ values in the range of 5 to 70 °, with a 2θ step size
of 0.03 ° and a count time of 3 s per step. The qualitative
analyses of the XRPD patterns were performed using the
Jade software version 7.1 (MDI 2005) with reference to
the patterns present in the International Centre for
Diffraction Data database (ICDD 2002).

Physicochemical analyses

The pH values of the acidic soil treated with various Results and discussion
renewable waste resources were obtained after curing in
Characteristics of the acidic soil and amelioration agents

Table 3 Test matrix for control and treated samples The initial soil pH was 5.2. This soil was classified as
sand in accordance with the United States Department of
Sample Waste oyster Calcined oyster Fly ash Cement kiln L/S
Agriculture (USDA) (Table 1). The results of the major
ID shells (wt.%) shells (wt.%) (wt.%) dust (wt.%) ratio
chemical composition of the acidic soil and the various
Control – – – – 0.2 waste resources performed by XRF analyses are listed in
1WOS 1 – – – 0.2 Table 2. The acidic soil is mainly composed of 61 wt.%
3WOS 3 – – – 0.2 SiO2 and 19.8 wt.% Al2O3. The WOS and COS additives
5WOS 5 – – – 0.2 mainly consisted of approximately 88 wt.% CaO. FA is
1COS – 1 – – 0.2 mainly composed of 38.2 wt.% SiO2 and 21.4 wt.% CaO,
1FA – – 1 – 0.2 while CKD is mainly composed of 55.5 wt.% CaO and
2FA – – 2 – 0.2 18.8 wt.% SiO2. XRPD results showed that the main
3FA – – 3 – 0.2 phases in the acidic soil are quartz (SiO2, PDF# 46–
1CKD – – – 1 0.2 1045), kaolinite (Al2Si2O5(OH)4, PDF# 29–1488), musco-
2CKD – – – 2 0.2 vite (KAl2Si3AlO10(OH)2, PDF# 07–0025), microcline
3CKD – – – 3 0.2 (KAlSi3O8, PDF# 19–0932), and cristobalite (SiO2, PDF#
39–1425) (Table 1; Fig. 1).
Environ Sci Pollut Res (2014) 21:774–780 777

Fig. 1 The XRD pattern for

acidic soil Q
Q: Quartz, K: Kaolinite,

Relative intensity (%)

M: Muscovite,
Mi:Microcline,
C: Cristobalite

Q
Mi
M Q Q
K K C K Mi K Q Q Q Q Q Q
M Q

5 10 15 20 25 30 35 40 45 50 55 60 65 70
2 theta

pH Improvement of the acidic soil
The results of the pH improvement of the acidic soil are
presented in Fig. 2. The WOS treatment was beneficial in
increasing soil pH. The soil pH was approximately 5.2 in the
control sample and increased in the range of 7 to 8 upon WOS
treatment at 1, 3, and 5 wt.%. Similar results have been
reported in the literature in two different studies. Agricultural
lime treatment at an application rate of 2,400 kg/ha produced a
significant soil pH increase from 3.8 to 5.2 (Blamey and
Chapman 1982). This study indicated that precipitated
CaCO3 which is main phase of WOS had an influence on
changing the soil pH. The detailed mechanism behind the pH
improvement of soil using CaCO3 was detailed in a study by
Lim et al. (2013) and Ok et al. (2011). Moreover, soil pH was
significantly increased from 5.21 to 6.64 with oyster shell ash
treatments at a rate of 8 t/ha (Onwuka et al. 2009). Treatments
of the acidic soils with 3 and 5 wt.% WOS did not achieve a
marked pH change above the pH levels attained with 1 %
WOS indicating a sole treatment of 1 wt.% WOS is sufficient
for a soil pH increase of 2 units.
For the FA treatment, 3 wt.% FA was required to increase
the soil pH value in the range between 7 and 8. These results
are in agreement with literature values reported for a control
soil sample with a pH of 4.7 and a similar clay content of
about 16 %, where pH increases to 7.5 and 7.7 upon 2 and
5 wt.% fly ash treatments, respectively, were observed (Matsi
and Keramidas 1999). This study concluded that an increase
in soil pH mainly depends on the buffering capacity which is
strongly linked to clay content. It implies that a high dosage of
fly ash may be needed for the treatment of acidic soils with
high clay content. Moreover, field applications to ameliorate
an acidic soil with Class C fly ash were successful in neutral-
izing the acidity in the soil (Schlossberg et al. 2006).
In the case of the COS treatment, the 1 wt.% COS treatment
was sufficient in increasing the soil pH by 3 units. The pH
improvement of soil is mainly induced by the dissociation of
Ca(OH)2. Therefore, for a soil pH in the range of 7 to 8
(beneficial for plant growth), less than 1 wt.% COS can be
sufficient.
For the CKD treatment, a similar soil pH increase in
the range of 7 to 8 was observed upon 1 and 2 wt.%

Fig. 2 Soil pH improvement 10

upon treatment using waste 9
resources
8

6 7 days
Soi pH

14 days
5
21 days
4
1 month
3 3 months
2

0
Control 1WOS 3WOS 5WOS 1COS 1FA 2FA 3FA 1CKD 2CKD 3CKD
778 Environ Sci Pollut Res (2014) 21:774–780

CKD treatments. However, treatment with 3 wt.% CKD Table 4 Maize plant growth results
resulted in a soil pH higher than 8. Therefore, 1 wt.% Sample ID Germination rate (%) Height (cm)
was sufficient to increase the soil pH in the desired
level of 7 to 8. The soil pH values remained virtually Control 66.7 10.5
unchanged with increasing curing times up to 3 months 3WOS 66.7 17.4
for all samples, indicating that a curing period of 7 days 1COS 100 18.3±1.61
is sufficient. 3FA 66.7 18.25
2CKD 100 16.5±0.5

Increase in exchangeable cations upon treatment

Exchangeable cations in the control and treated samples after
1 month of curing are presented in Fig. 3. The exchangeable
cation value for the control sample was 1.44 cmol+/kg, which
is similar to the value for typical sandy soils (Jung et al. 2011).
The values for exchangeable cations increased with increasing
amounts of amended agents. This indicated that once amelio-
ration agents are introduced to the acidic soil, the exchange-
able cations are released into the soil and the occupied soil
exchange sites (Yuan et al. 2011). The difference between the
different amendments was mainly caused by the cation
amounts available in the different waste resources as shown
by the XRF results (Table 2). Moreover, the increase in cation
exchange capacity values was mainly due to the calcium
content which was the main controlling factor when compared
to the other cations (Na, Mg, K) in the waste resources. The
reason why fly ash had a lower cation exchange capacity
values than WOS, COS, and CKD was most probably due
to its lower calcium content. An exchangeable cation value of
more than 5 cmol+/kg, which is similar to the value for fine
sandy loams, was attained for most of the treated samples,
except for the 1 wt.% FA-treated sample. Exchangeable cation
values in the clay loam region (15∼30 cmol+/kg) were also
obtained from the 3 wt.% WOS, 5 wt.% WOS, 2 wt.% CKD,
and 3 wt.% CKD-treated samples. Therefore, the amount of
exchangeable cations could increase significantly through the
addition of agents and this increase can be strongly associated
with soil quality improvements which can be expected to be
beneficial for plant growth.
Maize growth experiment
Maize growth for the following samples: control, 3 wt.% WOS,
1 wt.% COS, 3 wt.% FA, and 2 wt.% CKD, for a growth period
of 7 days after seeding is presented in Table 4 and Fig. 4. In all
of the treated soils, germination varied from 66.7 to 100 %
(Table 4). The height of the maize plants in the control sample
was approximately 10.5 cm, which was lower than all the other
treated samples. The highest maize height (18.3±1.61) was
observed upon 1 wt.% COS treatment (Table 4). In addition,
the plants grown on treated soils appeared to healthier and
richer than the control sample. For amelioration agents with
organic content levels of 0.9–5.1 % and application rates of 1–
5 %, the organic content of the amended soil remained virtually
unchanged. This indicates that pH improvement and the in-
crease of exchangeable cations may contribute to the growth of
maize in ameliorated acidic soil. A similar study has reported
that maize plant height was increased with liming materials
such as oyster shell ash and calcium carbonate (CaCO3), etc.
(Onwuka et al. 2009). Therefore, the optimum use of WOS,
COS, FA, and CKD in acidic soil could be beneficial to the
growth of maize since soil pH improved and essential plant
nutrients were replenished.

Fig. 3 Changes in exchangeable 25

cations upon treatment using
waste resources
20
CEC(cmol+ kg -1)

15

10

0
Control 1WOS 3WOS 5WOS 1COS 1FA 2FA 3FA 1CKD 2CKD 3CKD
Environ Sci Pollut Res (2014) 21:774–780
Fig. 4 Maize growth after 7 days
of seeding in the following
samples: control (a), 3 wt.%
WOS (b), 1 wt.% COS (c),
3 wt.% FA (d), and 2 wt.%
CKD (e)
Conclusions
Acidic soil with an initial pH of approximately 5 was amelio-
rated using renewable waste materials including waste oyster
shell, calcined oyster shell, fly ash, and cement kiln dust. The
soil pH and exchangeable cations were measured upon treat-
ment. Moreover, maize growth was investigated to confirm
whether ameliorated acidic soil is beneficial to plant growth.
779
The results showed that 1 wt.% WOS, 3 wt.% FA, and 1 wt.%
CKD were needed to increase the soil pH value to 7. In the
case of COS, 1 wt.% was more than enough to increase the
soil pH value to 7, due to the strong alkalinity associated with
COS. Moreover, a significant increase in exchangeable cat-
ions including Ca, Mg, K, and Na was observed upon treat-
ment. Improved maize growth was observed in the treated
samples as compared to the control samples. This indicated
780
that waste oyster shell, calcined oyster shell, fly ash, and
cement kiln dust could be used as good amendments for
amelioration of the acidic soil if optimum contents are applied.
Overall, considering the pH, exchangeable cations and maize
growth results, the most effective treatment was 3 wt.% WOS.
Acknowledgments This study was supported by the Korea Ministry of
Environment as The GAIA (Geo-Advanced Innovative Action) Project
(No. 173-111-040).
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