Post-Treatment of Anaerobically

Treated Medium-Age Landll

Leachate
Ebru Akkaya, Ahmet Demir, Dogan Karadag, Gamze Varank, M. Sinan Bilgili, and Bestamin Ozkaya
Department of Environmental Engineering, Yildiz Technical University, Esenler, Istanbul 34220, Turkey; ekoca@yildiz.edu.tr
(for correspondence)

Published online 1 May 2009 in Wiley InterScience (www.interscience.wiley.com). DOI 10.1002/ep.10362

This study focused on the removal of COD and INTRODUCTION

NH41 from medium-age leachate. Experiments were Sanitary landlling is the most widely used method
performed in a laboratory-scale upow anaerobic for the nal treatment of municipal solid wastes
sludge blanket (UASB), a membrane bioreactor (MSW). It is estimated that more than 70% of global
(MBR), and using magnesium ammonium phosphate MSW is disposed in landll sites [1]. Physical, chemi-
(MAP) precipitation. MBR and MAP were used for the cal, and biological processes occur within a landll
post-treatment steps for anaerobically treated leachate site to promote degradation on MSW. These proc-
to increase the removal of organics and ammonium. esses result in the production of leachate for a very
The UASB reactor removed nearly all biodegradable long time [2]. Leachate is a high-strength wastewater
organics and supplied constant efuent COD for all due to high content of organic and inorganic com-
concentration ranges of inuent leachate. Ammo- pounds such as COD, BOD5, and ammonium, and
nium removal efciency in the UASB reactor was rel- discharging leachate without efcient treatment may
atively low and the average value was 7.9%. Inte- result in serious environmental problems for receiv-
gration of MBR to the efuent of UASB reactor ing water bodies.
increased the average COD removal efciency from Ammonium and organics are the most signicant
51.8 to 65.6% and maximum removal efciency pollutants of leachate in the long term and these
increased to 74.3%. MAP precipitation was applied as components should be treated efciently before dis-
a nal step to decrease the ammonium concentration charging. In the technical literature, many biological,
in the efuent of UASB1MBR reactors. The effect of chemical, and physiochemical technologies have
pH and the molar ratio of MAP constituents on the been used for the removal of organics and nitrogen
removal of ammonium were evaluated. At optimal from leachate. Among biological technologies, anaer-
conditions (pH: 9.0 and Mg/NH4/PO4: 1/1.2/1.2), obic treatment methods are more suitable due to
96.6% of ammonium was removed and MAP pro- advantages of higher organic loading rates (OLRs),
vided additional COD and turbidity treatment. lower operating costs, and production of usable bio-
Consequently, the combined system of MBR and MAP gas [3]. In spite of these advantages, anaerobic treat-
precipitation could be used as an appropriate post ment does not generally produce efuent quality that
treatment option for the anaerobically treated meets strict discharge limits. Therefore, the efuents
medium-age landll leachate. 2009 American Institute from anaerobic reactors usually require a post-treat-
of Chemical Engineers Environ Prog, 29: 7884, 2010
ment before discharging into water bodies [4].
Keywords: ammonium, leachate, magnesium am- The membrane bioreactor (MBR) is a compact sys-
monium phosphate precipitation, membrane bioreac- tem that combines biological treatment with mem-
tor, upow anaerobic sludge blanket reactor brane ltration. Recently, MBR-based systems have
been increasingly used for wastewater treatment [5
7]. Among alternative treatment methods, magnesium
ammonium phosphate (MAP) precipitation has been
2009 American Institute of Chemical Engineers proven as an excellent treatment process to eliminate

78 April 2010 Environmental Progress & Sustainable Energy (Vol.29, No.1) DOI 10.1002/ep
high levels of ammonium ions in leachate [8]. Addi-
tionally, MAP sludge is accepted as a valuable fertil-
izer because of its nitrogen, phosphorus, and magne-
sium constituents and low solubility [9, 10].
In the light of the above evaluations, it can be
seen that the applications of cascaded treatment
methods are a crucial and necessity for leachate treat-
ment. Hence, the aims of the present work were to
perform an experimental study investigating MBR sys-
tem and MAP precipitation as a post-treatment of
anaerobically treated landll leachate. Pretreatment of
raw leachate was carried out in an upow anaerobic
sludge blanket (UASB) reactor in the lab scale. Raw
leachate samples were obtained from the Odayeri
Sanitary Landll Site. The landll site receives munici-
pal waste from a population of about 10 million and
is a medium-age landll (12 yr). To our knowledge,
many researchers have generally been focused on the
treatment of young leachate of Odayeri landll [11,
12], but there is no study for leachate having me-
dium-age characteristics. Furthermore, with the
implementation of the mentioned post treatment
methods, the changes in COD and ammonium re-
moval of pretreated leachate samples were observed.
The effects of each method on the treatment perform- Figure 1. Simplied UASB/MBR/MAP system layout
ance are determined and discussed in detail. for leachate treatment.

MATERIALS AND METHODS

Leachate Sample 5500 and12,070 mg/L, and BOD5 values ranged from
Leachate used in this study was obtained from 1250 to 5830 mg/L.
Odayeri Sanitary Landll Site located in the European
side of Istanbul, Turkey. Leachate was being col- Membrane Bioreactor
lected in a pond within a landll site. Samples were The MBR was used as a rst post-treatment step
transferred to the laboratory once a week and kept at following anaerobic treatment in order to remove the
48C in a refrigerator before usage. The leachate was residual organics and ammonium ion. The efuent
treated by using UASB, MBR, and MAP precipitation from UASB was fed simultaneously to the MBR and
methods. Raw leachate was pumped to the UASB re- these two systems were operated in continuous
actor without pretreatment applications such as pH mode. MBR consisted of an activated sludge bioreac-
adjustment, particle separation, etc. A diagram of tor, which was lled with biomass-supported material
treatment system is shown schematically in Figure 1. supplied from a domestic wastewater treatment plant
(Pasakoy), and a membrane unit submerged into the
Leachate Treatment System bioreactor. The reactor was made of a cylindrical
Plexiglas vessel with an internal diameter of 20.0 cm
Upow Anaerobic Sludge Blanket Reactor and a height of 50.0 cm. Therefore, its working vol-
The UASB reactor was made of Plexiglas with an ume was 9.0 L. A circular air diffuser, which was
internal diameter of 10 cm and a height of 125 cm. placed under the membrane module, maintained aer-
The working volume of UASB reactor was 9.0 L. The obic conditions and homogeneous distribution in
raw leachate was fed continuously through the bot- order to avoid membrane fouling. A cartridge lter
tom of the reactor using peristaltic pump and the gas membrane module made of polypropylene with a
liquid separator was equipped at the top of the reac- pore size of 1.0 lm and a ltration area of 0.5 m2
tor. The temperature of the reactor was maintained at was used. The efuent was withdrawn by a pump.
mesophilic conditions (358C) by pumping water from During the experimental studies, MBR reactor has the
an external thermostat through a water jacket sur- same ow rate with the UASB reactor and HRT was
rounding the reactor. The UASB reactor was seeded constant at 3 days. Inuent COD of MBR reactor was
with anaerobic sludge supplied from a full-scale an- ranged from 3675 to 7056 mg/L in the rst 30 days of
aerobic reactor treating brewery wastewater. During operation and average value was 4250 mg/L during
the 120 operational days, hydraulic retention time the experimental course.
(HRT) was kept constant as 3 days and OLR changed
in the range of 1.844.03 kg COD/m3-day due to the MAP Precipitation
uctuations in COD content of the leachate. The Treatment performance of MAP process depends
COD concentration of raw leachate varied between primarily on the pH and ratio of magnesium, ammo-

Environmental Progress & Sustainable Energy (Vol.29, No.1) DOI 10.1002/ep April 2010 79
nium, and phosphate ions in solution. In the litera- Table 1. Characteristics of raw leachate used in the
ture, there are some articles dealing with the opti- study period.
mum pH for MAP precipitation. Zhang et al. studied
in the pH range of 8.511.0 for the treatment of land- Mean
ll leachate and maximum ammonium removal was Parameter Value range value Unit
obtained at pH 9.5, whereas Gunay and coworkers
COD 5,50012,070 9,134 mg/L
[12, 13] achieved the lowest residual ammonium con-
BOD5 1,2505,830 3,510 mg/L
centration in the efuent at pH 8.5. Ozturk et al. [14]
BOD5/COD 0.230.48 0.38
applied MAP precipitation to anaerobically pretreated
TKN 2,2183,260 2,280 mg/L
efuent and the highest removal efciency was
NH4 2,0832,980 2,514 mg/L
observed at pH 9.2. Similarly, Li et al. [15] indicated
Alkalinity 14,40017,120 15,920 mg CaCO3/L
that pH 8.59.0 is the optimum range for ammonium
Color 3,0205,540 4,013 Hazen
removal by chemical precipitation. According to these
Turbidity 1,3203,840 2,428 NTU
results, the effect of pH on the MAP process was
pH 7.88.4 8
studied in the range of 8 to 10 at the stoichiometric
molar ratio (Mg:NH4:PO4:1/1/1). Furthermore, the
effect of the molar ratios of MAP constituents was
investigated while pH was kept constant as pH 9.0. are characterized with high amounts of readily biode-
MAP experiments were performed in batch mode gradable organics and ratio of BOD5/COD is over 0.5
using the efuent of MBR reactor. Experimental stud- in the literature [1719]. However, the biodegradabil-
ies were carried out in 500 mL beakers using analyti- ity of the leachate reduces and ammonium concentra-
cal grade magnesium chloride (MgCl2
6H2O) and so- tion in leachate increases along with landll age. The
dium hydrogen phosphate (Na2HPO4
12H2O) as the medium-aged leachate usually contains COD ranging
magnesium and phosphate source. The leachate solu- from 5000 to 10,000 mg/L and BOD5/COD is
tion was mixed for 3 min rapidly after adding the between 0.1 and 0.5 [7, 2022].
magnesium and phosphate chemicals and pH adjust- Values in Table 1 indicated that the leachate was
ment was made using 10.0 M NaOH. Following the relatively stable and well buffered with alkaline pH.
slow mixing for 10 min, the solution was precipitated High concentrations of nitrogen compounds in leach-
for 30 min to separate the MAP sludge from the bulk ate ranged from 2083 to 2980 mg/L for NH1 4 and
liquid. Results of ammonium, phosphate, magnesium, 2217 to 3260 mg/L for total Kjeldahl nitrogen (TKN),
color and turbidity measurements, and settled sludge respectively. NH1 4 was dominant among the nitrogen
volume were used to evaluate the efciency of the concentrations and small differences between NH1 4
MAP process. and TKN designate the scarcity of organic nitrogen
content in the raw leachate. These concentrations are
typical values given in the technical literature for the
Analytical Methods characteristics of medium-aged leachate [6, 23, 24].
The performance of each system was monitored
using the experimental analysis of COD, ammonium Anaerobic Treatment of Leachate
(NH14 ), phosphorus, and turbidity. Measurement of
Raw leachate was anaerobically treated in the
pH was carried out with Jenway Ion Electrode
UASB reactor. The operation duration of 120 days
(Model 3040). Biogas production was measured volu- during the treatment process was taken into account
metrically using a wet-type Ritter 14724 Gerate-
in this study for evaluation. Inuent and efuent
nummer gas ow meter. Magnesium analyses were
COD concentrations of UASB reactor and the OLR as
performed using a Unicam Atomic Absorption Spec- a function of COD content of the raw leachate are
trophotometer (Unicam, Model No. 929A). All mea-
given in Figure 2. It is seen from this gure that dur-
surements were conducted according to Standard
ing the rst 50 days, organic loadings rates are rela-
Methods [16].
tively high and variable. This situation can be
explained with variable COD concentrations which
RESULTS AND DISCUSSION resulted from raw leachate characterizations and cli-
mate conditions within those times.
Characteristics of the Leachate During the rst 30 days, COD removal rates of
The leachate used throughout the study was col- UASB reactor remained relatively low due to the high
lected from the Odayeri Sanitary Landll located on organic loadings. However, performance of subse-
the European side of Istanbul. Table 1 shows the quent days was not adversely affected by variation of
composition of raw leachate used during the experi- organic loading, and COD removal rates changed lin-
mental period. The COD concentration varied early with the variation of inuent COD. This circum-
between 5500 and 12,070 mg/L, and BOD5 values stance is clearly observed in Figure 3. For example,
ranged from 1250 to 5830 mg/L. The BOD5/COD the lowest removal efciency obtained was 32% for
ratios ranging from 0.23 to 0.48 values indicate the the inuent COD of 5500 mg/L and as the COD of
biodegradability for the medium-aged samples. When raw leachate increased to 12,070 mg/L, the removal
comparing these values with those of young leachate, efciency of COD in the UASB reactor reached a
it is seen that BOD5/COD ratios of the medium-aged maximum value of 71%. During the last 90-day pe-
samples are lower. In fact, young landll leachates riod for the performance of UASB reactor, the efuent

80 April 2010 Environmental Progress & Sustainable Energy (Vol.29, No.1) DOI 10.1002/ep
Figure 2. COD removal in the UASB reactor.
Figure 4. Effect of membrane fouling on the COD
removal of MBR.

the MBR occurred in two different stages. The data in

Figure 3 shows that the MBR was very effective for
COD removal during the rst 30 days of operation.
After that the COD removal decreased. A higher re-
moval efciency in the earlier stage could be due to
the higher COD content of UASB efuent. The sec-
ond stage started after the 30 operational days, and
the COD removal efciency of the MBR decreased
gradually. Although the inuent COD of the MBR
remained constant in the second stage, the treatment
performance decreased linearly with the reduction
Figure 3. Comparing the COD removal performances of permeate ux caused by membrane fouling (see
of reactors. Figure 4).
Membrane fouling is the major obstacle for
decreasing of treatment efciency, and the phenom-
enon of the fouling mechanism is very complex and
COD values were very similar although the inuent difcult to understand because the MBR system
COD values varied widely. A possible explanation for includes living microorganism and their metabolites.
these observations may be related to the degradation Several investigators have reported that membrane
of biodegradable organics by anaerobic microorgan- fouling occurring in MBR-activated sludge is attribut-
isms. Similar results were observed for the anaerobi- able to three aspects such as sludge particle deposi-
cal treatment of leachate elsewhere [24]. Over the tion, adhesion of macromolecules to the membrane
course of the experiment, COD removal efciencies surface, and pore clogging by small molecules. How-
of UASB were changed between 32.2 and 71.0% and ever, some agreement has been reached on the fact
average value occurred as 51.8%. This low COD re- that sludge particle deposition makes signicant
moval with the UASB reactor was due to the lower effect on membrane fouling in MBR system using
rate of biodegradable material in the leachate, but it activated sludge [2730].
is comparable with those reported for medium-age Comparing the performance of treatment systems
leachate [23]. in terms of the individual and combined performan-
It can be seen in Figure 4 that the removal of am- ces of the MBR indicates that the major part of the
monium ion in the UASB reactor ranged from 3.8 to COD was removed by the UASB reactor and integra-
14.2%, and the average efciency was  7.9%. In a tion of the MBR reduced variations and improved the
study, Kettunen et al. [25] observed low ammonium quality of the UASB efuent (see Figure 3). It is
reduction in the UASB reactor. In the same study, observed that the COD removal efciency of both
they stated that this situation could be attributed to systems varied between 39.5 and 82.1%, with an aver-
utilization of NH1 4 through assimilation of anaerobic age value of 65.6%. Moreover, our results obtained in
bacteria. Further, Tuyluoglu [26] obtained 20% for this study show good performance comparable to
NH1 4 removal in the UASB reactor. Similarly, Agdag previous studies for the combined treatment of leach-
and Sponza [24] obtained 1327% NH1 4 removal in ate [31, 32]. The NH14 removal efciency of the MBR
the UASB reactor, which was in good agreement with alone remained 35.0% for the entire duration of the
the other studies. experiment (see Figure 5). Integration of the MBR
increased total NH1 4 removal to between 32.7 and
Effect of MBR 50.4%, with an average value of 41.1%. The main
The efuent of the UASB reactor was fed to the mechanism for NH1 4 removal was nitrication and a
MBR for the rst post treatment. The COD removal in slight reduction was maintained by stripping of

Environmental Progress & Sustainable Energy (Vol.29, No.1) DOI 10.1002/ep April 2010 81
Figure 5. Ammonium removal in the UASB and MBR Figure 7. Effect of molar ratios on the performance of
reactors. MAP.

highly insoluble at alkaline pH [35]. A maximum NH1 4

removal of 93.9% was obtained at pH of 9.0 whereas
the lowest removal efciency was 86.6% at pH of 8.0,
as shown in Figure 6. The optimum pH for ammo-
nium removal obtained in this study was in agree-
ment with other studies in literature [36].
To improve further the performance of MAP pre-
cipitation, the molar ratios of Mg and PO4 were
increased while the pH was kept at pH 9.0. Figure 7
shows the effect of the molar ratios as functions of
NH4, COD, color and turbidity removal, and settled
sludge volume. Increasing the magnesium and phos-
phate concentrations had a slight effect on the re-
moval of NH1 4 from the leachate. Ammonium re-
Figure 6. Effect of pH on the removal of ammonium moval was enhanced in all cases and the maximum
in MAP. efciency obtained was 96.6% at the molar ratio of 1/
1.2/1.2. Following MAP precipitation, the overall am-
monium removal efciency of the combined system
was achieved as 98.0%.
gaseous ammonia due to vigorous aeration. Similar MAP precipitation also provided additional re-
results were reported in the technical literature for moval of color, turbidity, and COD. Leachate color
the treatment of wastewater by MBR reactor [33, 34]. decreased with the increasing of molar ratio and the
removal efciency increased from 18.5% at the stoi-
chiometric ratio to 22.5% at the ratio of 1/1.4/1.4.
MAP Precipitation Increasing of PO4 and Mg amounts slightly decreased
The ammonium level of leachate decreased about the turbidity and COD of the leachate solution. Maxi-
41.1% in the combined treatment of the UASB reactor mum COD and turbidity removals obtained were 25.7
and MBR, and the residual concentration was about and 36.4%, respectively. However, Yangin et al. [37]
1500 mg/L in the efuent. The MBR was inefcient and Ozturk et al. [14] obtained about 50% COD re-
and the necessity of NH1 4 elimination from the leach- moval with MAP precipitation of anaerobically treated
ate entailed application of additional methods. There- leachate [24, 37]. Kapdasli et al. [38] stated that COD
fore, MAP precipitation was used as a nal step to removal in MAP process is due to the adsorption of
decrease the ammonium ion in leachate efuent of organics onto the surface of MAP crystals, so the dif-
the UASB reactor and MBR. ferences in the COD removal efciencies could be
The effect of pH on the MAP process was attributed to the different physical properties of crys-
investigated at the stoichiometric molar ratio tals formed during MAP precipitation.
(Mg:NH4:PO4:1/1/1). It was observed that after add- The effect of magnesium and phosphate addition
ing chemicals, MAP crystals rapidly formed and set- was observed on the volume of the settled MAP
tled quickly to the bottom of beakers. Solution pH sludge. Sludge volume increased from 15.6% at the
decreased from 9.2 to 5.9 and only 50% of the NH1 4 stoichiometric ratio to 38.2% at the maximum ratio
was removed without pH adjustment. To increase the studied. Additional Mg and PO4 increased the sludge
NH1 4 removal, the solution pH was adjusted between volume and lowered NH41removal due to increasing
8 and 10 using 10.0 M NaOH. Visible size of MAP the size of MAP crystals and settling velocity. These
crystals and NH1 4 removal efciency were increased data show that MAP precipitation is very effective for
rapidly after pH adjustment because MAP crystals are eliminating NH1 4 from leachate and provided further

82 April 2010 Environmental Progress & Sustainable Energy (Vol.29, No.1) DOI 10.1002/ep
COD and color removal from the leachate. The main 7. Ahn, Y.T., Kang, S.T., Chae, S.R., Lee, C.Y., Bae,
drawback to this approach is that chemicals used in B.U., & Shin, H.S. (2007). Simultaneous high-
the MAP process are the main cost of the treatment strength organic and nitrogen removal with com-
but economic value of MAP sludge will help to bined anaerobic upow bed lter and aerobic
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CONCLUSION (2007). Enhancing struvite precipitation potential
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centrated leachate, a combined post treatment of ll leachate, Journal of Hazardous Materials, 146,
MBR and MAP precipitation is applied to the anae- 8185.
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treatment, COD removal of 51.8% and NH4 removal tion of suitable pretreatment method for old-in-
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ACKNOWLEDGMENTS ammonium removal from landll leachate by
This research has been supported by the Yildiz chemical precipitation, Journal of Hazardous
Technical University Scientic Research Projects Coor- Materials, in press.
dination Department. Project Number: 26-05-02-02. 14. Ozturk, I., Altinbas, M., Koyuncu, I., Arikan, O.,
The authors would also like to thank the ISTAC, Man- & Yangin, C.G. (2003). Advanced physico-chemi-
agement Ofce of Odayeri Landll site for providing cal treatment experiences on young municipal
the leachate samples. landll leachates, Waste Management, 23, 441
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84 April 2010 Environmental Progress & Sustainable Energy (Vol.29, No.1) DOI 10.1002/ep