Environmental Engineering and Management Journal August 2012, Vol.11, No.

8, 1467-1474
http://omicron.ch.tuiasi.ro/EEMJ/

“Gheorghe Asachi” Technical University of Iasi, Romania

COLOR AND COD REMOVAL FROM POULTRY LITTER

LEACHATE USING AN OZONATION PROCESS

Muhammad Saif Ur Rehman1,2, Azeem Khalid1, Sadaf Liaquat1,

Ch. Tahir Mehmood1, Tariq Mahmood1, Sajid Mehmood3
1
Department of Environmental Sciences, PMAS Arid Agriculture University, Rawalpindi, Pakistan
2
Department of Environmental Sciences, University of Gujrat, Gujrat, Pakistan
3
Department of Biochemistry and Molecular Biology, University of Gujrat, Gujrat, Pakistan

Abstract

Effectiveness of ozone oxidation reaction for removal of color and chemical oxygen demand (COD) from poultry litter leachate
was investigated. The poultry litter leachate (PLL) was prepared using a locally fabricated triple bed arrangement. The leachate
was ozonated at its original pH for different periods in order to examine the effect of ozone dose on color and COD reduction.
After 54 minutes of ozonation of PPL at its original pH 7.86, 73% of color and 50% of COD were reduced. The effect of initial
pH was studied by adjusting pH of the leachate at 5, 7 and 9. Ozonation at an initial pH 7 removed 77% of color and 58% of
COD after 54 minutes of ozonation. Statistical analysis revealed that decolorization of the leachate was independent of initial pH
while COD reduction was a function of an initial pH value. An acidic pH of 5 decarbonated the leachate and molecular ozone
reaction mechanism resulted in the higher removal efficiency. On the other hand, a basic pH of 9 was confronted with high
alkalinity and increased self decomposition resulted in the loss of oxidant. The process was optimized at 18 minutes of ozonation
time with a sequential pH adjustment.

Key words: alkalinity, color, COD, ozonation, poultry litter leachate

Received: July, 2010; Revised final: September, 2011; Accepted: September, 2011

1. Introduction bedding. The composition of poultry waste depends

Poultry industry is an important pillar of the
economy of Pakistan. Pakistan has observed a rapid
growth in poultry sector during the last decade. The
recent livestock census report showed that 73.6
million poultry birds were raised per year (ACO,
2006). Besides significant development in the poultry
sector, many environmental problems have emerged
regarding safe disposal of poultry waste.
A poultry bird takes seven weeks for its full
growth and produces around 12 kg of manure (Gupta
et al., 1997). In this way, poultry industry produces a
total waste of 883 million kg per year in Pakistan.
Poultry litter is usually composed of bird
excreta, leftover feed, feathers and material used for
on the materials used such as feed, bedding material
and vaccine practices (Gupta et al., 1997; Van der
Watt et al., 1994; Yetilmezsoy et al., 2011). Poultry
litter leachate is a toxic biowaste that has
demonstrated toxicity against a number of indicator
organisms and it has been found considerably toxic
than other livestock wastes (Gupta and Kelly, 1992).
Various sources contribute to litter toxicity which
include feed additives, antibiotics, hormones,
pathogens and heavy metals (Gerber, 2008; Pohontu
et al., 2010; Schiopu and Gavrilescu, 2010;
Yetilmezsoy et al., 2011).
A higher value for pollution parameters like
COD, BOD (biological oxygen demand), VFA
(volatile fatty acid), alkalinity and sulfate in poultry


Author to whom all correspondence should be addressed: E-mail: sajid.mehmood@uog.edu.pk; Phone: +92 53 3643375 (ext 119);
Fax: +92 (53) 3642167
 Rehman et al./Environmental Engineering and Management Journal 11 (2012), 8, 1467-1474
leachate has been observed (Rao et al., 2008). The
use of poultry litter as soil amendment may cause the
transfer of toxic agents in the food web via plants,
animals, and humans. It has been reported that areas
in the vicinity of poultry farmhouses are concentrated
with elevated levels of nitrogen and phosphorus and
excessive eutrophication of water bodies occurs
(Fisher et al., 2000).
Some metals such as arsenic, cobalt, copper,
iron, manganese, selenium and zinc are applied as
feed additives to prevent diseases in poultry and
improve production (Bolan et al., 2004; Jackson et
al., 2003). Only 5–15 % of these metals can be
ingested and the rest is released in manure. Upon
application to soil or in case of runoff, these heavy
metals end up in water bodies where they become
more concentrated (Gerber, 2008). Similar to heavy
metals, most quantity of the antimicrobial agents
administrated to poultry birds is excreted to the
environment where they may produce antimicrobial-
resistant bacterial strains (Chee-Stanford et al.,
2001). Steroid hormones have also been found in
poultry litter which is considered endocrine
disrupting chemicals (EDCs). These hormones
include estrogen (17-ß-estradiol), estrone and
testosterone (Fisher et al., 2005). These EDCs pose
the risks associated with reproductive health in
humans and wildlife (Samir et al., 2006; Schiopu and
Gavrilescu, 2010).
Besides all these risks to the environment,
local poultry houses are least interested in safe
disposal of poultry litter. It is simply thrown outside
the poultry farmhouses. This waste enters into water
bodies through leaching/runoff and poses a serious
threat to underground and surface water quality. This
situation triggers when natives use water from such
contaminated reservoirs for drinking purpose. There
is a need to install effective subsequent waste
treatment facilities for poultry litter leachate (PLL).
Biological treatment for PLL management is
rapidly growing because of its low operating cost and
environment friendly nature compared with other
treatment options (Tabrizi and Mehrvar, 2004).
However, biological processes show limited
perfromance for complete mineralization (Li et al.,
2010). Thus, an efficient treatment is required to
handle such type of wastewater. Advanced oxidation
processes (AOPs) are extensively used for leachate
treatment due to their high performance against
complex organic matter (Derco et al., 2010; Pohontu
et al., 2010; Wu et al., 2004).
Among AOPs, ozonation is a process which
involves the application of ozone to water for the
removal of pollutants. Ozone possesses an oxidizing
potential of 2.08 eV which makes it a powerful
oxidizing agent. Ozone can react with organic matter
either directly as O3 or indirectly through OH.
radicals (Gottschalk et al., 2000; Masten and Davies,
1994). Application of ozone for wastewater treatment
has increased tremendously due to its various
advantages. These advantages include high oxidation
potential of ozone, its high efficiency to remove color
1468
and degrade organic matter in one step, the addition
of oxygen to water, easy installation, requires little
space, no chemical sludge and residual ozone can be
converted into oxygen (Cu and Ma, 2000;
Siminiceanu et al., 2012; Soares et al., 2006; de
Souza et al., 2010). Ozone molecule selectively
targets color containing compounds. This results in
fast decolorization but low mineralization by the use
of ozone (Soares et al., 2006).
The solution pH has an important relationship
with ozone reactivity. Ozone decomposes at elevated
pH to generate non selective hydroxyl radicals and
these radicals govern the oxidation of pollutnats,
whereas at acidic pH, the molecular ozone leads the
oxidation process (Cu and Ma, 2000). Ozone can be
applied either as pre or post-treatment option
depending upon strength of wastewater. Pre-
ozonation step converts recalcitrant organic matter
into intermediates (Goel et al., 1995; Volk et al.,
1993). These intermediate compounds may escape
biological treatment so these compounds can be
removed by post-ozonation process (Arslan and
Balcioglu, 2001; Karrer et al., 1997).
The aim of present study was to treat PLL by
ozonation to check its efficacy for color and COD
removal. The ozonation was carried out at original
pH of the leachate and at adjusted initial pH levels in
order to understand its effect on the leachate
treatment. The role of ozonation time, initial pH and
alkalinity was studied to search for process
performance.
2. Materials and methods
2.1. Poultry litter source and leachate preparation
Poultry litter was collected from commercial
poultry farms located in sub urban areas of
Islamabad. The broken egg shells, hair or feathers
were removed from litter to avoid clogging. The litter
was then arranged in a three bed table. These beds
were connected with Teflon tubes. The bottom bed
was fitted with an outlet to collect poultry litter
leachate. The tap water was poured in first bed which
leached through the beds.
The poultry litter leachate obtained was
homogenized using magnetic stirrer and then stored
as stock solution in the refrigerator at 4 °C to
minimize substrate decomposition before the
experiment. The stock leachate was diluted 20 times
to assume practical concentration and then used for
ozonation experiment.
2.2. Leachate characterization
The leachate was analyzed before and after
ozonation treatment. Color reduction was measured
as described by Mohajeri et al. (2010).
The pH, DO, COD, alkalinity (measured as
CaCO3) and total dissolved solids (TDS) were
determined according to the standard methods
(APHA, 2005).
 Color and COD removal from poultry litter leachate using an ozonation process
Characteristics of the raw PLL samples are
presented in Table 1.
Table 1. Characteristics of poultry litter leachate with five
replicates (at 95% significance level)
Poultry Litter
Parameters Unit
Leachate
pH 7.86 ± 0.14
COD mg/L 734 ± 100
Color (at 465nm) a.u. 0.28 ± 0.05
DO mg/L 0.33 ± 0.24
TDS mg/L 422 ± 16
Alkalinity as CaCO3 mg/L 170 ± 30
2.3. Ozonation process
Ozonation was carried out in a bubble column
reactor in semi batch mode. The reactor was made of
boro-silicate glass with internal diameter of 5 cm and
50 cm in length. A corona discharge ozone generator
(Model OZX-B300T) was employed to produce
ozone from ambient air at the rate of 200 mg h-1.
The ozone-air mixture was fed to the reactor
at a flow rate of 2 L min-1 through diffusing stone
placed at the bottom of the reactor. Teflon tubing was
used for all connections from the ozone generator to
the reactor (Pachhade et al., 2009). Two 250 cm3 gas
washing bottles containing 200 cm3 of 4 percent KI
solution were connected in series with the reactor to
collect all the unreacted ozone gas passing through
the leachate being treated (Selcuk and Meric, 2006).
Ozonation was initially carried out at room
temperature and at original pH (7.86) of the leachate
which was not controlled during the process. The
effect of pH on ozonation was studied adjusting
initial pH level of the leachate at 5, 7 and 9. The pH
of the PLL samples was adjusted using 1.0 to 6.0 N
solutions of NaOH and H2SO4. Sample aliquots were
taken from the reactor at 18, 36 and 54 minutes and
were analyzed for pH, color, DO, alkalinity and COD
to check the process efficiency. Five replicates were
used for characterization while duplication was
carried out to calculate COD reduction after
ozonation.
2.4. Statistical analysis
Experimental design was two factorial; the
source of leachate and ozonation time. Analysis of
variance (ANOVA) was carried out to determine the
significance of main effects and their interaction. The
treatment means were compared by least significant
difference (LSD). The data was statistically analyzed
using Microsoft Excel 2007.
3. Results and discussion
The results shown in Figs. 1 and 2 revealed
that 73% color and 50% COD were removed when
leachate was ozonated for 54 minutes. The most of
decolorization and COD reduction occurred during
first 18 minutes of ozonation and a trivial
improvement in both parameters was observed for
the rest of ozonation period (18-54 minutes).
This observation demonstrated two distinct
stages of the ozonation process as reported in the
literature (Rehman et al., 2011; Tizaoui et al., 2007).
First, fast stage lasted for 0-18 minutes while second
slow stage spanned over 18-54 minutes.
During first stage of ozonation, the color
removal efficiency of 66% was achieved besides a
COD reduction of 39%. Color was removed at a rate
of 3.67% per minute while COD observed a
reduction rate of 2% per minute during the first stage.
Ozonation resulted in the cleavage of carbon-carbon
double bonds and other functional groups responsible
for color in the leachate (Saunders et al., 1983).
Higher reduction in color and COD during the first
stage of ozonation process could be attributed to the
increased content of ozone (Derco et al., 2010; Wu et
al., 2004), which possibly increased the rate of
reaction. During the second stage, color and COD
were removed at a rate of 0.2 and 0.3% per minute,
respectively. Similar findings have been reported in
literature (Derco et al., 2010). Lower COD reduction
in the second phase of ozonation process could be
related to very high reactivity of organic compounds
with ozone, followed by the formation of various
intermediates (soluble inert fractions) which require
more oxidant before their final degradation (Derco et
al., 2002; Orhon et al., 2002). Resultantly, a
competition between the parent molecules and
intermediate by-products for ozone started which
made the process less efficient during the second
stage (Sevimli and Sarikaya, 2002). Moreover,
continuous ozonation increased ozone concentration
in the liquid phase. As the ozone concentration
reached saturation level, chemical reaction rate was
driving the process. Further increase in ozone
content, after saturation level, influenced the rate of
reaction negatively (Wu et al., 1998).
In order to investigate the effect of pH on the
ozonation of leachate, the leachate was ozonated at
pH values of 5, 7 and 9 (from acidic to basic
conditions). Ozonation time was also varied to
examine any interactive response for decolorization
and COD reduction. It was evident from Fig. 1 and
Fig. 2 that maximum color removal of 77% was
obtained when leachate was ozonated at an initial pH
of 7 for 54 minutes. The color removal improved as a
function of ozonation time. Statistical analysis
revealed that decolorization was mainly driven by
ozonation time than initial pH of the leachate (Coca
et al., 2005). However, significant difference was
observed among different ozonation timings (P
<0.018). Contrary to decolorization, statistical
analysis showed that COD reduction was
significantly dependent on ozonation time (P <0.022)
while initial pH had a highly significant impact (P
<0.001). The staging was again noticed when
ozonation time and pH varied simultaneously. It was
obvious that almost 60% of color was removed
during first 18 minutes of ozonation for all the
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 Rehman et al./Environmental Engineering and Management Journal 11 (2012), 8, 1467-1474
investigated pH levels, implying that decolorization
occurred at a rate of 3% per minute, whereas during
next 36 minutes of ozonation only 17% of color was
removed at a rate of 0.5% per minute.
Fig. 1. Effect of ozonation time and initial pH on color
reduction of poultry litter leachate at room temperature
Fig. 2. Effect of ozonation time and initial pH on COD
reduction of poultry litter leachate at room temperature
This observation disclosed that decolorization
decreased almost 6 times during second stage of
ozonation (18-54 minutes). Comparing COD
reduction with decolorization, it was noticed that
58% of COD was reduced during first stage while
only 2% improvement was observed during the
second stage. The increase in the ozonation time
applied to the leacahte led to an increase in COD
removal for a given time only. Monje-Ramirez and
Orta de Velasquez (2004) reported that color
reduction was twice as compared to COD removal
when landfill leachate was treated with ozone. The
removal rate of COD was higher initially due to the
presence of easily oxidizable compounds. However,
further increase in reaction time after a certain stage
proved ineffective as reduction rate slowed down due
to inert intermediates produced and/or recalcitrant
molecules (Tizaoui et al., 2007).
Ozone showed selective preferential character
towards decolorization process. COD reduction
efficiency was lower than color removal as reported
in the literature (Wu et al., 2004; Kurniawan et al.,
2006). Normally decolorization was associated with
the structural transformation of color containing
compounds whereas the major fragment of parent
1470
molecule was intact or partially oxidized. Thus, COD
reduction was observed lower even for a higher
decolorization (Hao et al., 2000). Partial oxidation of
color causing unsaturated chromophore functional
groups could only transform these functional groups
resulting in wastewater decolorization mainly.
However, these partially oxidized molecules still
demanded oxidant until their final degradation
leading to higher color reduction than lower COD
removal (Tizaoui et al., 2007; Balcioglu et al, 2007).
The pH of the leachate was not controlled
during the ozonation process and was noted on
regular time intervals. Fig. 3 shows the dynamics of
pH during ozonation process. The leachate (at its
original pH7.86) showed an increase in pH. The pH
increased slightly during first stage to 7.91 which
reached a final value of 8.39 after 54 minutes of
ozonation. The high performance of ozone under
alkaline pH conditions due to the generation of
hydroxyl radicals had been well established. Besides
alkaline pH, ozone did not improve color and COD
removal as reported (Glaze et al., 1987, Cortez et al.,
2010).
The hydroxyl radical indirect oxidation was
counter acted by initial high concentration of
alkalinity present in the leachate (170 mg/L as
CaCO3). The adjusted pH values of leachate at 5 and
7 increased as ozonation proceeded. The rise in pH
was notable in case of initial pH 5, which reached to
6.78 accounting for 35% increase in its initial value.
At pH 7, an increase of 6% was observed whereas
14% decrease was observed at pH 9 after 54 minutes
of ozonation. The decrease in pH might be due to
formation of organic acid species like carboxylic
acid. However, increase in pH after ozonation was
not so common. Only few studies have been found
which reported increase in pH after sparging ozone
through wastewater and it was argued that stripping
of CO2 and volatile fatty acids could be responsible
for pH rise (Wu et al., 1998; Wu et al., 2004).
The pH dynamics showed that an increase in
pH could infer the formation of byproducts having
alkaline nature. pH had an important role in
controlling the ozonation kinetics. Ozone was
reported to have two different reaction mechanisms
at acidic and basic pH levels. At acidic pH, ozone
behaved as molecular ozone and observed rate of
reaction was lower due to its selective nature
(Hoigne, 1998) whereas ozone at alkaline pH
decomposed to hydroxyl radical which had high
redox potential than molecular ozone and non
selective in nature (Buxton et al., 1988; Legrini et al.,
1993). The rate of hydroxyl generation decreased
with lowering of pH (Staehelin and Hoigné, 1982).
Contrary to these findings, ozonation at an
initial pH value of 5 resulted in higher color and
COD removal than pH 9 as reported by Coca et al.
(2005) and Cortez et al. (2010). This fact could be
explained by the role of hydroxyl radical scavengers
in the form of alkalinity present in the leachate.
Fig. 4 shows the behavior of alkalinity during
ozonation at different initial pH values. Three times
 Color and COD removal from poultry litter leachate using an ozonation process
lower alkalinity values were found for pH 5 as
compared to pH 9. The acidic pH led to
decarbonation of the leachate which then facilitated
higher removal of color and COD (Beltran et al.,
1997). Coca et al. (2005) suggested that at pH 5,
hydroxide anions competed for ozone with organic
molecules to some extent as compared to pH 7 and 9
which resulted in relatively higher color and COD
reduction by molecular ozone mechanism. Direct
molecular attack of ozone led to formation of
hydrogen peroxide which promoted radical reactions.
Fig. 3. The dynamics of pH during ozonation of poultry
litter leachate at room temperature
Fig. 4. Effect of alkalinity on the ozonation of poultry
leachate at different initial pH levels
Besides lower decolorization, almost no COD
reduction during second stage of ozonation could be
attributed to the presence of other inorganic species
like sulfate, chloride, nitrate etc. Though scavenging
behavior of these species was not well known
however they had been found even slower in reacting
with hydroxyl radicals (Liao et al., 2001).
Ammonium was reported to compete for ozone with
color containing molecules leading to lower efficacy
of ozone (Tanaka and Matsumura, 2003). It was
assumed that hydroxyl radicals reacted with
carbonates and bicarbonates preferably than organic
compounds. These bicarbonate radicals appeared as
very selective oxidation species (•CO32- and •HCO3-)
which lower the reaction rate constant than the
hydroxyl radicals. These species inhibited indirect
hydroxyl radical reactions and lowered ozone
efficiency (Gunten, 2003).
It had been reported that bicarbonate ions
produced a scavenging effect to hydroxyl radicals to
produce intermediates which did not lead to a radical
type chain reactions (Coca et al., 2005; Hoigne,
1998).
Another possible reason for lower degradation
during second stage of ozonation might be due to its
increased decomposition into hydroxyl radicals at
alkaline pH (Gilbert, 1982). These hydroxyl radicals
could react with ozone itself and could decompose it
into oxygen and some other less reactive species as
proposed in following Eqs. (1-8) (Gurol and Akata,
1996; Peyton and Glaze, 1985; Tomiyasu et al.,
1985, Westerhoff et al., 1997).
O3 + OH− → HO2− + O2 (1)
HO2− + O3 → O3− + HO2• (2)
O3− → O− + O2 (3)
HO2• → O2− + H+ (4)
O2− + H+ → HO2• (5)
OH• + O3 → O2 + HO2• (6)
2HO2• → H2O2 + O2 (7)
H2O2 + O2•− → OH• + HO− + O2 (8)
The HO2• was not very reactive specie and
could give OH• in two steps, making path too long
(Eqs. 4, 5) and resulting in a slower degradation
process. The self decomposition of ozone into
oxygen was noted with the increase in ozone
concentration into the wastewater (Fig. 5).
Fig. 5. Decomposition of ozone in dissolved oxygen at
various initial pH values
The dissolved oxygen concentration increased
from its initial value of 0.33 mgL-1 to a maximum
concentration 5.75 mgL-1. The dissolved oxygen was
remained almost constant at pH value of 5 and 7 after
first stage of ozonation whereas a linear increase in
DO was observed for leachate which was ozonated at
its orgional pH. The increased DO concentration with
increased ozonation time verifieded ozone
decomposition as described by above mechanism.
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Ozone self decomposition led to greater ozone
requirement due to the loss of oxidant and
counteracted any beneficial increase in reaction rate
(Gilbert, 1982).
4. Conclusions
The ozonation of poultry litter leachate at its
original pH showed improvement in color and COD
removal up to 73 and 50%, respectively. The
ozonation of leachate proved to be a two stage
process. The first stage lasted for 0-18 minutes which
resulted in high oxidation followed by slow second
stage of ozonation which spanned for 18-54 minutes.
The decreased ozone efficiency during second stage
was controlled by increased self decomposition of
ozone. Ozonation time proved statistically significant
factor for both color and COD reduction. The effect
of initial pH on the decolorization and COD
reduction showed that acidic pH 5 removed 70% of
color and 60% of COD from leachate after 54
minutes of ozonation. Statistical analysis showed that
decolorization was independent of initial pH of
leachate while COD was significantly removed as a
function of initial pH. Ozonation under acidic
condition produced better results than basic pH
conditions due to decarbonation of leachate.
Alkalinity played an important role in explaining
ozone behavior under different pH conditions. Higher
concentration of hydroxyl radical scavengers affected
ozone efficiency under different pH conditions. An
ozonation time of 18 minutes at pH 5 was optimized
to treat PPL. Sequential pH adjustments during
ozonation could produce better results for color and
COD reduction.
Acknowledgement
The authors acknowledge financial support provided by
Directorate of Planning and Research, PMAS Arid
Agriculture University, Rawalpindi, Pakistan for this
project (Project No. AUR/DR‐366).
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