Journal of Environmental Management 110 (2012) 267e275

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Journal of Environmental Management

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Seasonal variation in chemical properties and degradability by anaerobic

digestion of landll leachate at Benowo in Surabaya, Indonesia
M. Kawai a, *, I.F. Purwanti b, N. Nagao c, A. Slamet b, J. Hermana b, T. Toda a
a
Department of Environmental Engineering for Symbiosis, Faculty of Engineering, Soka University, 1-236 Tangi-cho, Hachioji, Tokyo 192-8577, Japan
b
Department of Civil Engineering, Faculty of Engineering, Institut Teknologi Sepuluh Nopember, Surabaya, Indonesia
c
Institute of Bioscience, Universiti Putra Malaysia, Serdang, Malaysia

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

Article history: Seasonal variations in the physical and chemical characteristics of leachate taken from Benowo landll in
Received 12 April 2011 Indonesia, including factors likely to inhibit anaerobic digestion, were investigated to determine the
Received in revised form impacts on the stability of anaerobic treatment. To evaluate the biodegradability of the leachate,
10 April 2012
a continuous experiment was conducted by changing the organic loading rate (OLR). Chemical oxygen
Accepted 18 June 2012
Available online 17 July 2012
demand (COD) ranged between 2621 and 16,832 mg L
1, and COD in the dry season was twice the level
in the rainy season owing to reduced rainwater input and signicant evaporation. COD, pH, and the
concentrations of ammonium ion, and metals in the leachate were within acceptable ranges for
Keywords:
Anaerobic digestion
decomposition by anaerobic digestion. However, the Na and Cl
in the leachate are high enough to
Annual chemical variation inhibit anaerobic digestion. From chemical investigation of leachate at six monitoring wells in Benowo,
Asia food waste accumulation and seawater intrusion might cause high salinity in the leachate. In the
Landll leachate continuous experiment, COD removal efciency was maintained at 40% regardless of OLR, suggesting
Refractory substances that at least 40% of the leachate contained biodegradable substances. Based on these results, issues
Salinity of wastes surrounding the biological treatment of saline and refractory substances in landll leachate were dis-
cussed. It is suggested that high salinity and refractory substances in the leachate are common issues
during the leachate treatment by anaerobic digestion as the implications for similar landlls in other
countries around the world.
Crown Copyright 2012 Published by Elsevier Ltd. All rights reserved.

1. Introduction used in developed countries, such as coagulation, occulation, and

Landlling, which is an unsustainable way for waste manage-
ment is still a conventional method that is employed worldwide
(Wiszniowski et al., 2006). In emerging countries with rapidly
increasing populations, such as Indonesia, the dumping of solid
waste in landlls has increased greatly (World Bank, 1999). Most of
the landlls are open dumps where waste is discarded in an
uncontrolled manner (Mangimbulude et al., 2009; Visvanathan
et al., 2003). There has been concern that these open dumps
pollute surrounding aquatic environments, including both
groundwater and surface water such as river and coastal areas, with
their leachates owing to a lack of adequate management systems
for the wastes and their leachate (Abu-Rukah and Al-Kofahi, 2001;
El-Fadel et al., 1997).
Leachate should be treated to prevent the contamination of
water resources. The conventional leachate treatment methods
* Corresponding author. Tel.: 81 42 691 5176; fax: 81 42 691 4086.
E-mail address: lotus_375@soka.gr.jp (M. Kawai).
settling, are costly in terms of the capital outlay for plant equip-
ment, the energy requirements, and the frequent use of a range of
chemicals (Wiszniowski et al., 2006). It is therefore difcult to
install such treatment plants in emerging countries, and leachate
treatment in such areas tends to rely on simple methods such as the
use of aeration lagoons and attenuation by means of natural
processes such as dilution by river water and rainfall (Christensen
et al., 2001; Mangimbulude et al., 2009).
In recent years, anaerobic digestion has received increased
attention because it can be employed at relatively low cost and it
produces an energy rich biogas as a by-product. The anaerobic
process is mediated by sequential fermentation reactions driven by
a diverse range of microbes that convert hydrocarbons into simpler
molecules and ultimately into CO2 or CH4 (Appels et al., 2008;
Speece, 1996). In principle, anaerobic digestion is a low-cost
treatment for leachate, and should be an appropriate method for
use in emerging countries. However, the leachate often contains
components such as ammonium ion and heavy metals which
inhibit anaerobic digestion (Alkalay et al., 1998). In addition, the
leachate may have high salinity, which inhibits the activity of

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268 M. Kawai et al. / Journal of Environmental Management 110 (2012) 267e275

anaerobic microorganisms. Moreover, in a large part of Asia, landll
characteristics are inuenced by the monsoon climate, which is
characterized by great differences between the rainy and dry
seasons. Large amounts of leachate with low concentration are
produced by dilution of the heavy downpour during last several
months in the rainy season. While, in the dry season leachate is
concentrated due to evaporation (Trankler et al., 2005; Visvanathan
et al., 2003). This seasonal variation in leachate quality is an
important constraint for successful treatment of landll leachate
(Mangimbulude et al., 2009; Tatsi and Zouboulis, 2002), and its
effect (variations in leachate characteristics) must thus be
accounted for to permit efcient operation of leachate treatment.
The characteristics of leachate change not only depend on the
season but also on the landll age (Chen, 1996; Christensen et al.,
2001; Fan et al., 2006). The following ve phases are typical of
a landlls lifecycle: the aerobic phase (Phase I), the anaerobic acidic
phase (Phase II), the intermediate methanogenic phase (Phase III),
the stabilized methanogenic phase (Phase IV), and the nal aerobic
phase (Phase V) (Kjeldsen et al., 2002; Tchobanoglous et al., 1993).
The pH decreases during Phase II due to the produced organic acids
and then increases to 7.5e9.2 by consumption of the organic acids
during Phase III (Chiemchaisri et al., 2009; Kjeldsen et al., 2002).
Biodegradability of leachate also decreases with increasing landll
age (Kjeldsen et al., 2002; Renou et al., 2008). Furthermore, periods
of these phases are changed depending on region and landll
management, such as landll with leachate recirculation.
Emerging countries are in dire need of cost effective treatment
of relatively matured leachate and the potential application of
treatment by anaerobic digestion should be evaluated. However,
leachates from landll bioreactors or relatively young landlls were
used in most of the previous researches (Castillo et al., 2007; Chen
et al., 2008a; He et al., 2007; Thabet et al., 2009).
In the present study, the seasonal variation in the physical and
chemical characteristics of the leachate from Benowo landll in
Indonesia was examined and the factors capable of inhibiting
anaerobic digestion were studied. Moreover, a continuous anaer-
obic digestion experiment to determine the biodegradability of the
leachate was also performed.
2. Materials and methods
2.1. Benowo landll
The Benowo landll is located in northwest Surabaya, East Java,
Indonesia, approximately 3.4 km southeast of the coast (Fig. 1A).
The landll is at an elevation of 0e3 m above sea level. Established

A
112o 36 18 112o 39 54 112o 43 30
7o 09 54 7o 09 54
Surabaya City, Java Island

7o 11 6 7o 11 6
Madura Strait

Benowo Landfill
7o 12 18 7o 12 18

7o 14 6 7o 14 6
112o 30 18 112o 39 54 112o 43 30

B
112o 37 26 112o 37 45 112o 38 06
7o 12 57 7o 12 57
Surabaya city N

A
3
1 2
4 L

6
5

0 100 200 300 400 500 m

7o 13 20 7o 13 20
112o 37 26 112o 37 45 112o 38 06

Fig. 1. (A) The location of Benowo landll near Surabaya, which is located in the eastern part of Indonesias Java Island. (B) Sampling stations at Benowo landll. A, articial pond; L,
seepage pond; 1e6, monitoring wells.
 M. Kawai et al. / Journal of Environmental Management 110 (2012) 267e275 269

Table 1 Fe (200 mg L-1)*1

Operational parameters for the continuous treatment experiment using an upow
anaerobic sludge blanket reactor. OLR, organic loading rate; HRT, hydraulic retention
time. Zn m L-1)*2
Ni (20 mg
g L-1)*2
(10 mg
Operation Phase Substrate OLR Inuent HRT Current
period (g-COD COD (days) velocity
(days) L
1 d
1) (mg L
1) (m d
1)
100
0e16 Start-up 1 Synthetic 2.50 5000 2 0.35 80
17e23 Start-up 2 Synthetic 0.71 5000 7 0.10 60
40
4 0
24e34 OP1 Leachate 0.25 1770 7 0.10 20
0
35e64 OP2 Leachate 0.44 1770 4 0.18 Cu Cd
65e72 OP3 Leachate 0.89 1770 2 0.35 (5.0 mg L-1)*3 ((10 mg L-1)*3
73e91 OP4 Leachate 0.44 1770 4 0.18
92e108 OP5 Leachate 0.25 1770 7 0.10
109e180 OP6 Synthetic 0.71 5000 7 0.10

Mn Cr
as a controlled dump site since 2001, it has been in operation for (5.6 mg L-1)*4 (10 mg L-1)*3
over 9 years at the time of our study and was considered
a relatively old landll. The landll covers an area of 34 ha and Pd (500 mg L-1)*3
receives 6064 t of municipal solid waste (MSW) per day from
Surabaya city (Ferita, 2006). The composition of the MSW (by Fig. 3. Maximum metal and heavy metal concentrations in the Benowos leachate.
Values after the element names represent the level at which each element causes
weight) is 65.6% organic matter, 13.3% paper, 4.9% cardboard, 9.0% inhibition of for anaerobic digestion. Sources: *1Yang and Shen (2006); *2Zayed and
plastic and rubber, 1.0% metal, 1.0% glass, 1.8% fabric, and 3.4% dust Winter (2000); *3Lin and Chen (1999); *4Ginter and Grobicki (1997).
(Kementrian Lingkungan Hidup, 2006).

2.2. Annual variation in leachate characteristics at Benowo landll
From December 2007 to December 2008, samples were collected
twice a month from eight sampling stations in the landll (Fig. 1B).
Leachate ows through ditches and gathers in an articial pond
(Fig. 1B, location A). A number of other ponds form as a result of
leachate seepage from the nearby wastes, and one of these was
selected (Fig. 1B, location L) as a representative sampling station for
seepage. The Benowo landll also has six monitoring wells
(161e325 cm in depth) (Fig. 1B, location 1e6). All samples taken
from the articial pond, the seepage pond, and the six monitoring
wells were measured for the following characteristics: chemical
oxygen demand (COD), salinity, pH, and the concentrations of
several ions and heavy metals.
COD was measured according to standard methods (APHA,
1998). The pH was determined using a pH meter (F-22, Horiba,
Kyoto, Japan). Salinity was measured by a conductivity meter
equipped with a SevenGo metro SG3 combined electrode (Mettler
Toledo International Inc., Tokyo, Japan). Cations (Na, K, NH4 ,
Mg2, Ca2), an anion (Cl
), and various elements (Fe, Zn, Ni, Cd,
Mn, Cu, Cr) were measured after ltering the samples through
a 0.45-mm glass-ber lter (GC-50, Advantec, Tokyo, Japan). Cation
and anion concentrations were determined using an SSC-600 ion
chromatograph (Senshu Kagaku Co. Ltd., Tokyo, Japan). Samples for
detecting the elemental concentrations were measured by using an
ICPS-7000 inductively coupled plasma-atomic emission spec-
trometer (Shimadzu, Tokyo, Japan). Both the chromatograph and
the spectrometer were calibrated before and after the series of
analyses for each element using standard solutions. The resulting
measurement errors averaged 1% and 0.1%, respectively.
Precipitation data in Surabaya from December 2007 to December
2008 was obtained from the website of the NOAA Satellite and
Information Service, U.S. National Climatic Data Center which
provides the climate database at http://www.ncdc.noaa.gov/oa/
ncdc.html.
2.3. Anaerobic digestion of leachate
2.3.1. Seed sludge and substrate
The seed sludge for inoculation was collected from the Hokubu
Sludge Treatment Center in Yokohama, Japan, following treatment
in an anaerobic digester. In the laboratory, the sludge was left for 3
days to allow sedimentation to increase microorganism cell density
in the seed sludge bed. The total COD was 42 g L
1, soluble COD was

20 rainy dry rainy 100 10

COD concentration ( 103 mg L-1)

COD 90
pH 9
80
Precipitation (mm day-1)

Precipitation
15
70
8
60
pH

10 50 7
40
30 6
5 20
5
10

0 0 4
Dec. Jan. Feb. Mar. Apr. May June July Aug. Sep. Oct. Nov. Dec.
2007 2008

Fig. 2. Seasonal dynamics of precipitation, COD, and pH of samples obtained from the articial pond (Fig. 1B) from December 2007 to December 2008.
270 M. Kawai et al. / Journal of Environmental Management 110 (2012) 267e275

3000
rainy dry rainy

Concentration of NH4+ (mg L-1)

2500

2000

1500

1000

500

0
Dec. Jan. Feb. Mar. Apr. May June July Aug. Sep. Oct. Nov. Dec.
2007 2008

Fig. 4. Seasonal variations in the ammonium ion concentration from December 2007 to December 2008.

0.52 g L
1, total solids (TS) content was 30 g L
1, and volatile solids
(VS) content was 20 g L
1.
In the continuous experiment, the synthetic wastewater described
by Sekiguchi et al. (1998) was used. This substrate comprised the
following ingredients (all values in mg L
1): sucrose, 2000; sodium
acetate, 1500; sodium propionate, 750; peptone, 500; NH4Cl, 500;
Na2SO4, 120; KH2PO4, 150; KCl, 300; CaCl2$2H2O, 130; MgCl2$2H2O,
400; NaHCO3, 2000; FeCl3$6H2O, 4.46; ZnSO4$7H2O, 0.15; CoCl2$6H2O,
0.17; H3BO3, 0.06; MnCl2$4H2O, 0.5; NiCl$6H2O, 0.04; CuCl2$2H2O,
0.03; and NaMoO4$2H2O, 0.03. The Benowos leachate was also used as
the substrate. The 200 L of leachate as a substrate in the continuous
experiment was obtained from the articial pond at the Benowo
landll in June 2009. COD of the leachate was 5044 mg L
1, the pH was
7.9, EC was 29 mS cm
1, TS was 2.2 g L
1, and salinity was 1.7%. The
substrate leachate salinity was kept constant at 0.5% by dilution in
order to evaluate the biodegradability of organic compounds without
the inhibition of anaerobic digestion due to high salinity.
2.3.2. Experimental parameters and analytical methods
A 5 L upow anaerobic sludge blanket (UASB) reactor was used
in this study. The reactor was installed in a constant temperature
room (37  1  C) and the substrate tank was placed in a refrigerator
(4  C). Synthetic wastewater and leachate were supplied to the
reactor by a peristaltic pump. At start-up, the reactor was fed
synthetic wastewater for 23 days (Table 1). After start-up, leachate
was fed to the reactor by increasing and decreasing the organic
loading rate (OLR) in a stepwise manner. After day 109, synthetic
wastewater was again fed to the reactor. Treated water, sludge, and
biogas samples were taken at the end of each period. Next, the TS,
COD, and ammonium ion content of the treated efuent water were
analyzed. The cell density in the sludge sample was measured.
Biogas production was also measured by collecting the gas
produced into an aluminum gas bag.
Samples used for determining the bacterial cell density were
xed in 4% paraformaldehyde in phosphate-buffered saline
immediately after sampling. The xed samples were stored at 4  C
and stained with 40 ,6-diamidino-2-phenylindole for 5 min at room
temperature (Shibata et al., 2006). The stained samples were then
immediately viewed under an Axioskop 2 plus microscope (Carl
Zeiss International, Hamburg, Germany). Biogas was analyzed using
a GC-2014AT biogas chromatograph (Shimadzu). The methane
content of the biogas was analyzed and was expressed as the
methane ratio (the proportion of the total biogas accounted for by
methane).

rainy dry rainy

20

Na+
Cl-
Concentration of ions (g L-1)

15 K+
Ca2+
Mg2+

10

0
Dec Jan
2007 2008 Feb Mar Apr May June July Aug Sep Oct Nov Dec

Fig. 5. Seasonal variations in the concentrations chloride ions, sodium ions, potassium ions, calcium ions, and magnesium ions from December 2007 to December 2008.
 M. Kawai et al. / Journal of Environmental Management 110 (2012) 267e275 271

3. Results and discussion
3.1. Investigation of seasonal leachate variation
3.1.1. Seasonal range of COD and pH in the articial pond
During our sampling period, the rainy season was from
December 2007 to March 2008 and from November to December
2008, and the dry season was from April to October 2008 (Fig. 2).
COD of the leachate in the articial pond ranged from 2621 to
16,832 mg L
1, and averaged 4539  800 mg L
1 during the rainy
season and 9004  4480 mg L
1 during the dry season. CODs in the
dry season were therefore nearly two times the value in the rainy
season. In the rainy season, a large volume of leachate is produced
by the heavy rain, whereas in the dry season, a smaller volume of
more concentrated leachate is produced because of the reduced
rainfall and increased evaporation (Mangimbulude et al., 2009;
Tatsi and Zouboulis, 2002). Speece (1996) reported that a substrate
requires at least 1000 mg-COD L
1 to be effective for anaerobic
digestion because anaerobic microorganisms require high nutrient
levels. As the average COD of the Benowo leachate even during the
rainy season was more than 4500 mg L
1, it would be suitable for
anaerobic digestion in terms of COD.
Benowo had been operating for 9 years at the time of our study,
and the pH value during the sampling period was relatively stable,
ranging from 7.7 to 8.7. This suggests that the Benowo landll was
a Phase III landll (Chiemchaisri et al., 2009). Such a pH range is
optimal for anaerobic digestion (Chiemchaisri et al., 2009; Kjeldsen
et al., 2002).
During pre- and post-dry season such as May and November, the high
ion concentrations may have been caused by evaporation. Na and
Cl
ions were frequently present at high concentrations (maximum
values of 10,930 mg L
1 and 19,121 mg L
1, respectively). Salinity is
a known factor that is capable of inhibiting biological processes.
Speece (1996) reported a 50% inhibition at a concentration of
12,000 mg-Na L
1 for occulated sludge; Lim et al. (2008) reported
that methane production decreased to 1/4 at salinity levels over 1.0%.
The maximum salinity in the Benowo leachate was about 2.5 times
higher than these inhibitive levels. The high salinity values suggest
that a considerable inhibition of biodegradation occurs during the
anaerobic treatment of leachate from the Benowo landll.
3.1.4. COD and salinity at each sampling site at Benowo
Cluster analysis on the annual COD and salinity data from the
eight sampling stations were performed to identify groups of
sampling stations based on similarities in their leachate charac-
teristics (Fig. 6). In the analysis, the stations roughly divided into
(Salinity)
Well 6
Well 5
Group 1
Seepage pond
Artificial pond

3.1.2. Heavy metals in the leachate at the articial pond

Well 3
Metals and heavy metals (Al, Fe, Zn, Ni, Cd, Mn, Pb, Cu and Cr)
were detected in the leachate. The presence of metals in the
leachate shows the effect of leaching in unsegregated solid waste Well 4
Group 2
that is likely derived from items such as scrap steel, lead batteries,
tins, and other metal wastes like metal containers (Mor et al., Well 2
2006). Most of Al in the waste stream comes from beverage cans
80%
(Diaz and Warith, 2006), and Al was also detected in the samples at Well 1
this study site. Detection of Fe in the samples indicates that iron,
steel products were dumped in the landll (Rowe et al., 1995). Pb in 70 75 80 85 90 95 100
the leachate might come from batteries, photographic chemicals,
Similarity (%)
old lead-based paints and lead pipes. The wastes delivered from
Surabaya city contained 13% paper (the ink content of this paper
(COD)
can also be a source of heavy metals) and 1.0% metal. Well 6
According to previous studies of the inhibition of anaerobic
digestion by metals, inhibition would occur at levels exceeding Well 5
200 mg L
1 Fe, 20 mg L
1 Ni, 10 mg L
1 Cd, 10 mg L
1 Cr,
500 mg L
1 Pb, 5.6 mg L
1 Mn, 5.0 mg L
1 Cu, and 10 mg L
1 Zn Group 1
Seepage pond
(Ginter and Grobicki, 1997; Lin and Chen, 1999; Yang and Shen,
2006; Zayed and Winter, 2000). Each metal in the leachate from
the Benowo landll was detected at values less than these critical Artificial pond
levels (Fig. 3). Because none of the metals or heavy metals in the
leachate reached 50% of the inhibition level, their concentrations Well 4
would not inhibit anaerobic digestion.
Well 3
3.1.3. Seasonal ion concentrations in the leachate at the articial Group 2
pond
Well 2
Ammonium ion is another factor that can inhibit anaerobic
digestion (Chen et al., 2008b). During our sampling period, the
ammonium ion concentration in the leachate decreased over time. Well 1
50%
In all months, concentrations of ammonium ions at Benowo were
under the recognized inhibition level of 4000e5000 mg L
1 (Li and 0 20 40 60 80 100
Zhao, 2001) (Fig. 4).
Similarity (%)
The concentration of all ions except ammonium ion uctuated
during the sampling period (Fig. 5). Ion concentrations may have Fig. 6. Results of cluster analysis based on salinity and COD values at the eight
been diluted by heavy rainfall especially during the rainy season. sampling stations in Benowo landll (Fig. 1B) using SPSS.
272 M. Kawai et al. / Journal of Environmental Management 110 (2012) 267e275

two groups: group 1 had high values of both parameters (articial
pond, seepage pond, well 5, and well 6); group 2 had low values of
both parameters (wells 1e4). The average COD and salinity for
group 1 were 4601 mg L
1 and 1.7%, respectively, which were
more than 25 and 3 times the corresponding values in group 2
(183 mg L
1 and 0.5%, respectively).
Group 1 stations were located near the working area of the
landll, whereas group 2 stations were located near inactive areas.
From Fig. 7, there were signicant correlations between COD and
salinity at all four stations in group 1, but in group 2, the correlation
was only signicant at well 4. In group 1, the COD increased with
increasing salinity, suggesting that salt had accumulated from the
food waste, which accounts for 65.6% of the MSW from Surabaya
city. Moreover, salinity in the leachate might be also concentrated
by strong evaporation which is caused by a considerable amount of
solar radiation in low latitude countries.
A 8.0
Group 1
6.0
The Benowo landll is at an elevation of 0e3 m above the sea
level. Seawater intrusion into the aquifer below the coastal area
has been reported at depths as shallow as 1e2.5 m (Al-Hogaraty
et al., 2008). Because the depth to water in our sampling sites
ranged from 0.7 to 2.4 m, seawater could have contaminated the
water collected at many of the sampling sites. It is also possible
that high salinity seawater penetrates the groundwater and soil of
the landll. In the case of seawater intrusion, the COD would
decrease with increasing saline concentration. At some of the
stations in group 2, the COD was low and the salinity was high.
This suggests that seawater might have permeated the landll.
Furthermore, Nativ et al. (1997) reported that soluble salts such as
NaCl, NaNO3, CaSO4, and CaCl2 in groundwater are often deposited
by signicant evaporation in arid regions where the maximum
evapotranspiration rate exceeds the precipitation rate. In coastal
areas where the groundwater has a high salt content as a result of
seawater inltration, precipitation of salts can also occur. There-
fore, it is possible that salts dissolved in the groundwater accu-
mulate, and are then transferred into the leachate during periods
of heavy rainfall.
Artificial pond
Seepage pond
well 5
well 6
3.0 300 up
start 1 2 3 4 5 6 A 2.5
Organic loading rate(g-COD L-1 day-1)

Cell density (109 cells mL-1)

Ammonium ion
Salinity (%)

2.5 250
Cell density 2.0
Ammonium ion (mg L-1)
OLR
2.0 200
4.0 r = 0.467* 1.5
r = 0.773 *** 1.5 150
r = 0.527**
1.0
1.0 100
r = 0.506**
2.0 0.5
0.5 50

0 0 0
start
120 up
1 2 3 4 5 6 B 1200
0

Biogas production (mL day-1)

0 5000 10000 15000 20000
COD removal efficiency (%)

100 1000

COD concentration (mg L-1) 80 800

B
COD removal efficiency
2.0 60 Biogas production 600
well 1
Group 2
well 2 40 400
well 3
20 200
well 4
1.5
0 0
start
100 up
1 2 3 4 5 6 C
Salinity (%)

1200
Biogas production (mL day-1)

1.0 Methane ratio 1000

r = 0.503** 80 Biogas production
Methane ratio (%)

800
60
600
0.5 40
400

20 200

0 0 0
0 20 40 60 80 100 120 140 160 180 200
0 200 400 600 800 1000 1200
Operation time (day)
COD concentration (mg L-1)
Fig. 8. Measurement parameters in the continuous treatment experiment using the
Fig. 7. Relationships between salinity and COD at each sampling station in the two upow anaerobic sludge bed reactor. (A) Concentration of ammonium ion, and the cell
groups (Fig. 7) of stations at Benowo landll. (A) Group 1. (B) Group 2. Signicance density and organic loading rate (OLR). (B) COD and gas production. (C) Biogas
levels: *p < 0.05; **p < 0.01; ***p < 0.001. production and the methane ratio.
 M. Kawai et al. / Journal of Environmental Management 110 (2012) 267e275
3.2. Continuous anaerobic digestion of the landll leachate
Table 1 summarizes the operational conditions in the contin-
uous experiment. Synthetic wastewater was fed to the reactor with
a high hydraulic retention time (HRT), such as 2 days during start-
up period 1. During start-up period 2, synthetic wastewater was
also fed to the reactor, but with HRT 7 days. Thereafter, the
substrate was switched to leachate and fed to the reactor with HRT
ranging from 2 to 7 days during operation periods 1e5 (OP1eOP5).
Finally, the substrate was reverted to the synthetic wastewater
during OP6, with HRT 7 days.
During start-up period 1 and 2, when the synthetic wastewater
was fed to the UASB reactor, the ammonium ion concentration in the
treated efuent water was generally less than 120 mg L
1 (Fig. 8A)
and COD removal efciency was greater than 95% (Fig. 8B). In
addition, biogas production averaged 317 mL day
1 and the methane
ratio was 60% (Fig. 8C). These results suggest stable operation of the
Fig. 9. COD and salinity values in leachate from the present study (articial pond) and in studies of other landlls around the world. Circles show landlls which are within 5 km
from the sea.
273
anaerobic digestion process. The cell density decreased with HRT 2
days during the initial phase. This might have been caused by
washout of the microorganisms from the reactor.
After switching from the synthetic wastewater to the leachate
during OP1, the ammonium ion concentration increased to
237 mg L
1. However, the maximum level was still lower than the
inhibition level of 4000e5000 mg L
1 (Li and Zhao, 2001). In
addition, cell density, COD removal efciency, and biogas produc-
tion decreased gradually. Although the biogas composition was
more than 60% methane at start-up, methane was 0.2% by the end
of OP1 and biogas composition was as follows: 57.1% CO2, 31.6% N2,
0.2% CH4, and 11.1% others.
From OP2 to OP5, when the reactor continued to be supplied
with leachate, the cell density was maintained at
0.5  109 cells mL
1 regardless of the different OLRs (Fig. 8A). The
COD removal efciency was also maintained around 40% even when
biogas was scarce (Fig. 8B). One of the reasons for the detection of
274 M. Kawai et al. / Journal of Environmental Management 110 (2012) 267e275
almost no biogas even when COD reduction took place is that the
CO2 produced may have immediately dissolved in the water dis-
charged from the reactor owing to the high solubility of CO2.
The reduced 40% COD in the leachate indicates the proportion of
degradable materials. However, inhibitors and toxic materials in the
leachate, such as humic substances and aromatic compounds, are
reported to affect anaerobic microbial activities (Alkalay et al., 1998;
Chen et al., 2008b; Renou et al., 2008). Calace et al. (2001) reported
that the proportion of refractory dissolved organic matter in
leachate, such as humic materials, increase with increasing landll
age. Benowo which was categorized as Phase III had been opera-
tional for 9 years at the time of our study, and its leachate may be
relatively old. Humic substrates are sufciently resistant to biolog-
ical treatment that they are considered to be non-biodegradable
compounds (Lou and Zhao, 2007). These facts raise the possibility
that biodegradable material reduction was limited to 40% in the
leachate because of other factors. In our subsequent experiment, the
conrmation of whether this is the case, and to identify the domi-
nant humic substrates in the leachate will be attempted.
During OP6, when the substrate reverted to the synthetic
wastewater, COD removal efciency rapidly increased. Although
biogas production recovered to 200 mL day
1, maximum methane
composition was only 40% (Fig. 8C) which was lower than the value
during start up. It is suggested that the sludge condition may have
changed owing to the prolonged constant loading of leachate (84
days) which will reduce the methane productive potential of
microbes. The low methane ratio did not recover until OP6 at 60
days of operation. It is indicated that microbial activity might not be
recovered for 60 days after switching the leachate to synthetic
wastewater.
In this experiment, though methane could not be produced from
the matured leachate, anaerobic digestion would be useful as
a primary treatment as reduction of energy to the leachate treat-
ment processes might be achieved.
3.3. Relationship between COD and salinity
Fig. 9 indicates the COD and salinity of the leachates in this study
(at the articial pond) and in other landlls around the world. Many
landll leachates have a salinity greater than 1.0%, which results in
signicant inhibition of an anaerobic biodegradation treatment
(Lim et al., 2008; Speece, 1996).
At Benowo, the high-salinity leachate might be caused by
accumulation of salt from food wastes and by the intrusion of
seawater. These phenomena are not unique to this study area.
Several landlls shown in Fig. 9 are located near the sea. Koshy et al.
(2007) reported that many landlls worldwide are located close to
the sea or even at sites that encroach into the sea. Their results
suggest that the number of coastal landll sites has been steadily
increasing. It can be therefore hypothesized that seawater could
intrude into many landll sites in coastal areas, especially those
with insufcient waterproong.
Another possible reason for high salinity could be the accumu-
lation of ash as a result of incineration of wastes in developed
countries. Ash also has high salinity (Ore et al., 2007) and is known
to generate a high-salinity leachate in countries such as Belgium
and France where most of the MSW is incinerated.
Leachate COD decreases over time as landlls age, partly owing
to the build up of humic substances such as humic acid and fulvic
acid which are resistant to further biodegradation (Huo et al.,
2008b). Many landlls have a COD lower than 10,000 mg L
1, and
these leachate may contain many refractory substrates.
When leachate is treated biologically, the high salinity and high
content of refractory substances in the leachate can prove to be
a difcult issue to tackle. Where possible, microorganisms with high
salinity tolerance should be used for leachate treatment (Kimata-
Kino et al., 2011), and research on techniques for the degradation
or absorption of refractory substances should be a priority.
4. Conclusions
In this study, the seasonal patterns in the physical and chemical
characteristics of leachate from a relatively old landll, including
the factors capable of inhibiting anaerobic digestion, were inves-
tigated using a year of sample data from the Benowo landll in
Surabaya city, Indonesia. To provide data that would support the
development of a stable biological treatment process for the
leachate, continuous anaerobic experiment conducted to investi-
gate the biodegradability of the leachate yielded the following main
results:
1. COD reected seasonal variations in the leachate components.
The COD during the dry season was two times the value during
the rainy season owing to reduced rainfall and signicant
evaporation.
2. The COD, pH, and concentrations of ammonium ion and metals
or heavy metals in the leachate were within the range of values
that did not prevent decomposition by anaerobic digestion.
However, the leachate included high concentrations of Na and
Cl
, which are known to inhibit biological processes. Both high
values of these ions and the observed uctuations of salinity in
the leachate must be considered when designing an anaerobic
digestion process for this landll and others with similar
characteristics.
3. In the continuous experiment, regardless of variations in OLR,
the COD removal efciency was maintained at around 40%,
suggesting that the leachate contained at least 40% biode-
gradable substances.
4. High salinity and a high content of refractory materials in the
leachate are common issues when leachates are treated by
anaerobic digestion. Therefore, microorganisms with high
salinity tolerance should be used for treatment of this leachate.
Further investigation should prioritize the development of
methods for the degradation or absorption of refractory
materials.
Acknowledgments
This work was undertaken as part of cooperative research
program, the SEED Project, between the Institute of Technology
Sepuluh Nopember (ITS), Indonesia and the Faculty of Engineering
of Soka University (SU), Japan. We thank Mr. Arie Dipareza Syafei of
ITS and Mr. Yumeto Yamada of SU for their invaluable assistance
during our sampling and analysis. We also thank Professor Yulinah
Trihadiningrum, Ms. Dewi Dwirianti, Mr. Mas Agus Mardyanto of
ITS, and Mr. Chiaki Niwa of SU for their invaluable advice on the
design of our study.
This research was partly funded by a grant from the Center of
Excellence for Private Universities from Japans Ministry of Educa-
tion, Culture, Science and Technology from 2009 to 2013. We are
grateful to the Hokubu Sludge Treatment Center, Yokohama, Japan,
for preparing and providing the seed sludge.
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