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Environmental Technology

ISSN: 0959-3330 (Print) 1479-487X (Online) Journal homepage: http://www.tandfonline.com/loi/tent20

Elimination of nitrogen present in swine manure


using a high-efficiency biotrickling filter
Karine Raby , Antonio Avalos Ramirez & Michle Heitz
To cite this article: Karine Raby , Antonio Avalos Ramirez & Michle Heitz (2013) Elimination
of nitrogen present in swine manure using a high-efficiency biotrickling filter, Environmental
Technology, 34:7, 813-824, DOI: 10.1080/09593330.2012.720615
To link to this article: http://dx.doi.org/10.1080/09593330.2012.720615

Accepted author version posted online: 13


Sep 2012.
Published online: 19 Sep 2012.
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Date: 27 September 2016, At: 13:53

Environmental Technology, 2013


Vol. 34, No. 7, 813824, http://dx.doi.org/10.1080/09593330.2012.720615

Elimination of nitrogen present in swine manure using a high-eciency biotrickling lter


Karine Rabya , Antonio Avalos Ramireza,b and Michle Heitza
a Department

of Chemical Engineering and Biotechnological Engineering, Faculty of Engineering, Universit de Sherbrooke,


Sherbrooke, Canada; b Institut de Recherche et de Dveloppement en Agroenvironnement (IRDA), Qubec, Canada
(Received 5 April 2012; nal version received 1 August 2012 )

Experiments were performed to remove nitrogen as ammonium in biotrickling lters (BTFs) treating synthetic swine manure.
Two BTFs packed with polypropylene spheres and ceramic beads were used. BTFs were continuously fed, and leachate
obtained was recirculated at dierent ow rates in the range from 0 to 1.5 L min1 . When increasing the recirculation
ow rate, the carbon dioxide (CO2 ) production rate increased from 16.5 to 25.6 g CO2 m3 h1 and nitrogen elimination
decreased from 99% to 86% for the polypropylene spheres, whereas for the ceramic beads the CO2 production rate decreased
from 20.3 to 15.0 g CO2 m3 h1 and nitrogen removal from 99% to 90%. The increase of recirculation ow rates also
promoted the production of nitrite (NO
2 ) in the leachate. For both packing types, when increasing nitrogen loads from 60 to
240 g N m3 day1 without recirculation of leachate, the BTFs achieved nitrogen removals of more than 99%. For the same
nitrogen loads, nitrogen removal increased from 90% to 99% for the BTF packed with ceramic beads at a recirculation ow
rate of 0.6 L min1 . Operating the BTFs with continuous purge was optimal for biomass production with a maximum level
of 71.3 g m3 day1 .
Keywords: biotrickling lter; synthetic swine manure; nitrogen elimination; CO2 production; nitrication; denitrication

Introduction
Pig industry and manure production
Between 1986 and 2006, the pig industry in Canada, in
terms of hogs marketed, has shown a growth of approximately 205%. In the province of Quebec, for the same
period of time, this growth has been approximately 153%
[1]. The pig industry is the second most important industry
in the province of Quebec and with about 7.3 million hogs
produced annually, it has generated incomes of more than
1.5 billion dollars in 2007 [1,2].
In Canada, between 1981 and 2006, total manure production from animal breeding has increased by 16%, the
equivalent of 25 million tons of manure. In this, total
production of swine manure rose by 5 million tons. In
the province of Quebec, an estimated 14 million tons of
manure is produced annually and about 4 million tons
of swine manure specically [3,4]. Nowadays, average
manure production across all sub-sub-drainage areas in
Canada (Quebec included) is about 1070 kg of manure per
hectare of cultured land [5].
Benets and environmental impacts of manure
Manure is the main by-product of animal breeding. It is
a mix of urine and faeces to which is added water from
piggery cleaning, rain and many wastes (food, straw, litter,
Corresponding

author. Email: michele.heitz@usherbrooke.ca

2013 Taylor & Francis

etc.). Manure is mainly composed of water, organic matter


and fertilizing minerals such as nitrogen and phosphorus
[6]. Table 1 shows the characteristics of swine manure in
terms of biological oxygen demand (BOD5 ), total Kjeldahl nitrogen (TKN), total suspended solids (TSS) and total
phosphorus concentrations, which are 60100 times higher
than those of domestic wastewater [68].
Manure is a source of organic matter which, when
spread, helps to reduce soil erosion and improves soils
water-holding capacity. Manure is also a source of phosphorus and nitrogen, which are essential nutrients for crop
growth. On the other hand, pig industry and manure production induce several adverse environmental impacts.
Gaseous emissions of ammonia (NH3 ), methane (CH4 ), carbon dioxide (CO2 ) and volatile organic compounds (VOCs)
represent a real problem of atmospheric pollution. The content of liquid manure is also a problem: phosphorus can x
to the soil; ground-water can be polluted by nitrates (NO3 ),
pesticides and pathogens; and surface waters can be polluted
by nitrogen, phosphorus, suspended solids, antibiotics and
organic matter as BOD5 [3].
A pig produces from 15.5 kg of manure per day
[3,4]. Some of the manure produced may be spread for
agricultural purposes but the soils phosphorus saturation
level is quickly reached and the excess manure trickles
to surrounding surface waters and underground waters

814
Table 1.

K. Raby et al.
Comparison of the composition of crude pig manure and typical domestic wastewater.
Parameters

Mean concentration (Variation) (mg/L)

Composition of crude pig manure

Biological Oxygen Demand (BOD5 )


Total Suspended Solids (TSS)
Total Kjeldahl Nitrogen (TKN)
Total Phosphorus

13,000 (10,00020,000)
16,000 (10,00020,000)
2300 (20003800)
650 (500900)

Composition of typical domestic wastewater

Biological Oxygen Demand (BOD5 )


Total Suspended Solids (TSS)
Total Kjeldahl Nitrogen (TKN)
Total Phosphorus

200 (120290)
240 (160350)
40 (2565)
8 (412)

[9]. Baril [3] performed a mass balance to determine the


required agricultural area to spread the manure coming from
the pig industry in Quebec and in Canada. A pig produces
the equivalent of 5 kg of phosphorus per year. Knowing that
an average agricultural site requires about 38 kg of phosphorus per hectare and that, in 2008, total pigs on farms were
about 4 million in Quebec and 13 million in Canada [1],
areas of 0.5 and 1.7 million hectares of land would be necessary to run o the manure coming from this production in
Quebec and Canada, respectively. These quantities represented 27% in Quebec and 4.8% in Canada of the available
cultured lands in 2006 [10].
Manure management
In a sociological context where sustainable development
is a priority, management of liquid and gaseous euents
coming from breeding pigs represents a big challenge. The
spreading of manure is now strongly restricted by Canadian
government in order to bypass the environmental problems
associated with this practice. New guidelines based on a
crops phosphorus needs have lowered the quantities of
manure that can be applied on land and have restricted
manure spreading during certain periods of the year. In
Canada, transformations that have taken place in the agrifood industry in the last 50 years have reduced the area of
cultivated lands by 44%. As a result, producers nd themselves with large excesses of manure that they cannot spread
and must transport long distances to spread it in farming
areas [5,11].
Environmental impact of nitrogen
Nitrogen is one of the main components of manure, representing up to 3.9% of dry weight [9]. Ammonium (NH4 + ) is
the main form of nitrogen in manure. Oxidation of NH4 + to
NO3 (the process of nitrication) consumes oxygen (O2 )
and then contributes to reduce O2 in rivers and lakes, to
the detriment of many animal species. Depending on the
pH and temperature of the environment, NH4 + transforms
to free NH3 which is toxic to sh at low concentrations
(<1 ppm). In combination with phosphorus, nitrogen can
lead to eutrophication of water sources, producing growth
of undesirable algae [6].

Nitrogen removal
Nitrication is a series of biological reactions where
NH4 + is converted to hydroxylamine (NH2 OH), then to
nitrite (NO2 ) and nally to NO3 . Some gaseous byproducts (nitrogen monoxide (NO), nitrogen dioxide (N2 )
and nitrous oxide (N2 O)) can be released from this reaction
as follows [6]:
NO, N2O
NH4+

NH2OH

NO2-

NO3-

NO, N2O, N2

(1)

This process is done by autotrophic bacteria, strictly aerobic. These bacteria use CO2 or bicarbonate (HCO3 ) as a
carbon source and NH4 + as an energy source. Denitrication is an anoxic process where heterotrophic bacteria use
oxidized forms of nitrogen (NO2 and NO3 ) as electron
donors instead of molecular nitrogen. The denitrication
process is as follows [6]:
NO3-

NO2-

NO

N2O

N2

(2)

This process can lead to a nal product of gaseous nitrogen (N2 ), which is environmentally acceptable. However,
denitrication can be stopped at any step and releases intermediate compounds such as NO and N2 O, which are gas
pollutants [6,12,13].
Bioltration of swine manure
Bioltration can be used to treat manure. A biolter (BF)
can be described as a three-phase bioreactor. The liquid
phase is the manure containing nutrients for microorganisms, the gaseous phase is the air fed part, and the solid phase
is the biolm covering the packing material. The biolm is a
microbial population where physical, chemical and biological processes occur. The immobilization of microorganisms
on the packing material allows a more stable operation by
improving the retention time of the microorganisms. Fixedlm bioreactors are widely used for removal of organic
matter and nitrogen (by nitrication and denitrication) in
wastewater treatment [14]. BFs can be divided into two

Environmental Technology
categories: 1) BFs with discontinuous feeding of the liquid
phase; and 2) biotrickling lters (BTFs) with continuous
feeding of the liquid phase.
In the literature, it is reported that organic packing BTFs
treating pig manure have shown organic matter removal
(evaluated as BOD5 ) of 9599%. BFs achieved an incomplete removal of around 75% of TKN by transforming
NH4 + by nitrication and denitrication processes [12].
Other studies on BFs treating manure and packed with
organic materials have shown that after the start-up period,
the BF totally oxidizes NH4 + to NO3 but partially reduces
NO3 in N2 . It was hypothesized that a simultaneous
nitrication and denitrication (SND) occurred. The SND
process usually occurs in anoxic micro-zones inside ocks
of biomass or deep in the biolm [6,12].
BTFs have been used in wastewater treatment for over
40 years [15]. More recently, BTFs have been used in odour
control and air pollution treatment. In BTFs, synthetic packing materials such as polypropylene or polystyrene are used
as growth media to attach microorganisms [15].
This study aims to treat swine manure in a BTF packed
with synthetic media. The research was divided into three
experimental phases. In the rst phase, the inuence of the
purging method on the CO2 and the biomass production

Figure 1.

Schematic representation of biotrickling lter setup.

815

rates (PCO2 and PB) was evaluated. In the second phase,


the inuence of the following parameters on ammonium
(NH4 + ) conversion and PCO2 was studied: (a) kind of packing material; (b) recirculation ow rate of the leachate; and
(c) total carbon and nitrogen inlet loads. In the third and last
phase, the removal of organic matter (total carbon) present
in the synthetic swine manure was evaluated.
Material and methods
Biotrickling lters
Two BTFs called, respectively, BK1 and BK2 were constructed from Plexiglas cylinders with an internal diameter of 0.15 m and a total packed-bed height of 1 m divided
into three sections of 0.33 m. Figure 1 shows the schematic
representation of the BTF setup. For the experiments, two
dierent inert packing materials were tested. BK1 was
packed with ceramic beads (Hydroton , kotau GmbH,
Germany) with an average diameter of 0.012 m, a specic surface of 310 m2 m3 and 40% void space [16]. BK2
was packed with non-porous polypropylene spheres (Jaeger
Tri-Packs , Fabco Plastics, Canada) of 0.025 m diameter,
280 m2 m3 specic surface and a void space of 90%. For
both BTFs, the empty bed volume (V) was about 0.018 m3 .

816
Table 2.

Biolter

K. Raby et al.
Summary of the operational parameters tested in biotrickling lters BK1 and BK2.
Packing
media

BK1

Ceramic beads

BK2

Polypropylene spheres

Recirculation
ow rates tested
(L min1 )

Carbon loads
Nitrogen loads
tested
tested
(gC m3 day1 ) (gN m3 day1 )

0
0
0
0.5
0.5
0.5
1
1.5
0
0
0
0.5
1
1.5
0.8
0.8
0.8

The BTFs were inoculated with a leachate from a BF that


had been treating swine manure [17].
Inlet air, dry and particle free, was bubbled in a humidication column before entering the bottom of the lter at a
rate of 8 L min1 for an empty bed residence time (EBRT) of
130 s and at an average temperature of 24 C. The treated liquid coming out of the BTF (leachate) was collected in a 12 L
holding tank and recirculated at the top of the BTF using a
centrifugal pump (model 1212-2AA-121, SHURo, UK).
Table 2 shows a summary of the operational parameters tested in both BTFs for this study. For the rst
phase of the study, BK2 was operated for about 200 days
under a recirculation ow rate of 0.8 L min1 with carbon
and nitrogen loads of, respectively, 137 g C m3 day1 and
60 g N m3 day1 . During 95 days of operation, leachate
was not purged from the holding tank and continuously
recirculated. For 55 days, BK2 was then operated using
discontinuous purge which consisted of collecting manually an amount of leachate of 0.45 L day1 . Finally, for 50
days, BK2 was operated using continuous purge which consisted of collecting continuously, with a peristaltic pump,
the same amount of leachate as the manure fed. The continuous purge was performed by a peristaltic pump (Masterex,
Cole-Parmer, USA), pumping 1820 mL of leachate from
the holding tank each hour (24 times a day) for a total purge
rate of 0.45 L day1 . For each of the purging methods, 12
measurements of PCO2 and three measurements of PB were
performed. For the rest of the experiments, both BTFs were
operated using continuous purge.

Synthetic manure feed


The synthetic manure used in this study had a constant
carbon:nitrogen ratio of 2.4:1 throughout the experiments.

137
275
550
137
275
550
137
137
137
275
550
137
137
137
137
137
137

60
120
240
60
120
240
60
60
60
120
240
60
60
60
60
60
60

Table 3.

Purging
method

Duration of the
experiment
(days)

Continuous purge
Continuous purge
Continuous purge
Continuous purge
Continuous purge
Continuous purge
Continuous purge
Continuous purge
Continuous purge
Continuous purge
Continuous purge
Continuous purge
Continuous purge
Continuous purge
No purge
Discontinuous purge
Continuous purge

27
12
21
24
22
18
15
12
24
12
15
22
22
12
95
55
50

Synthetic manure recipe used.

Chemical compound
Sodium propionate
Sodium acetate
Lactic acid
Butyric acid
Ethanol
Ammonium bicarbonate
Potassium phosphate
Potassium sulfate

Chemical
formula

[Compound]
g L1 manure

C2 H5 CO2 Na
C2 H2 O2 Na
C 3 H6 O3
C 4 H8 O2
C 2 H6 O
NH4 HCO3
KH2 PO4
K2 SO4

2
2
3.3
0.07
1.7
13
0.366
4.15

For the basic recipe, the carbon loading rate of the BF


was 137 g C m3 day1 for an equivalent BOD5 load of
144 g O2 m3 day1 [6,7,18]. The detailed recipe is shown
in Table 3. The BTFs were fed continuously with synthetic
manure at a ow rate of 0.45 L day1 by using a peristaltic
pump (Masterex, Cole-Parmer, USA).
For the second phase of the study, BK1 and BK2
were rst fed at four dierent recirculation ow rates:
0, 0.5, 1 and 1.5 L min1 under a carbon load of
137 g C m3 day1 . Then, three dierent carbon loads (137,
275 and 550 g C m3 h1 ) and nitrogen loads (60, 120 and
240 g N m3 h1 ) were tested in the BTFs by concentrating the basic recipe two or three times. Carbon inlet loads
to the whole system were kept constant by means of adjusting the ow rate and the concentration of the synthetic
manure. The three dierent loads were tested at recirculation
ow rates of 0 and 0.5 L min1 with BK1, and at 0 L min1
with BK2. The duration of each experiment varied from
1227 days depending of the length before stabilization of
the BTF after changing one parameter. For both BTFs, for
each parameter tested, 48 measurements of PCO2 were
performed and two samples, taken on dierent days (two

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replicates for each sample), were analyzed to determine
NH4 + conversion and distribution of nitrogen species in
the leachate.
For the third phase of the study, carbon elimination was
tested in BK1 with no recirculation and at a carbon load
of 550 g C m3 h1 . The duration of the experiment was
21 days and two samples, taken on dierent days (two replicates for each sample), were analyzed to determine carbon
elimination.
Performance and characterization of the biotrickling
lters
BTF performance was analyzed in terms of biomass production rate (PB), NH4 + conversion (X) and carbon dioxide production rate (PCO2 ). The variables are dened as
follows:


PB =

 Dry Biomass
 Number of Days

Ci Co
100
Ci
Q(CO2o CO2i )
PCO2 =
V
X =

(3)
(4)
(5)

PB and PCO2 have units of g m3 h1 , while X is


expressed as a percentage. Q is the air ow rate (m3 h1 ),
V is the empty bed volume (m3 ), C is the concentration
of NH4 + (g m3 ), CO2 is the carbon dioxide concentration
and subscripts i and o indicate, respectively, inlet and outlet. The concentrations of CO2 were measured with a CO2
analyzer (Ultramat 22P, Siemens AG, Germany). The  dry

817

biomass is the biomass accumulation in the biolters and


was calculated according to a method reported by Avalos
Ramirez et al. [16].
Global mass balances were made on the process using
the feed of synthetic manure and the leachate purge. The
concentrations of NH4 + , NO2 and NO3 in the leachate
purge or in the synthetic manure feed were determined
with an ion-exchange chromatography system (ICS-1000,
Dionex Corporation, USA). Total organic carbon (TOC) in
liquid was measured with a total carbon analyzer (TOC-VE ,
Shimadzu Corporation, Japan).
Liquid samples taken for analysis were collected at the
outlet, ltered and acidied with sulphuric acid to a pH
lower than 2 in order to conserve them for a maximum
period of 28 days at 4 C in plastic Falcon tubes [19].

Results and discussion


Eect of purging method on CO2 and biomass
production rates
Figure 2 shows the eect of the purging method on
PB and PCO2 for the BTF packed with polypropylene spheres. The experiment was carried out at an
inlet carbon load of 137 g C m3 day1 , an inlet nitrogen
load of 60 g N m3 day1 and a recirculation ow rate
of 0.8 L min1 . Each value of PB and PCO2 presented
in Figure 2 is the average data over 7 weeks of operation. Figure 2 shows that the method of purging the
leachate aected the PB drastically. The PB was 3.0
1.5 g m3 day1 without purge, 42.1 9.6 g m3 day1
with discontinuous purge and 71.3 39.9 g m3 day1 with
continuous purge, and PCO2 was, respectively, 15.1 7.3,

Figure 2. Eect of purging method on CO2 production rate ( PCO2 ) and biomass production rate ( PB). The biotrickling lter was packed with polypropylene spheres and operated under an inlet carbon load of 137 g C m3 day1 , an inlet nitrogen load of
60 g N m3 day1 and a recirculation ow rate of 0.8 L min1 .

818

K. Raby et al.

Figure 3. Eect of recirculation ow rate on CO2 production rate. The biotrickling lters (BTFs) were operated under an inlet carbon
load of 137 g C m3 day1 and an inlet nitrogen load of 60 g N m3 day1 . The BTFs were packed with () polypropylene spheres and
() ceramic beads.

17.2 6.2 and 19.1 4.4 g m3 h1 for the same conditions. Both PB and PCO2 presented the highest values when
leachate was continuously purged. Chou and Wang [20]
observed that in a BTF treating ammonia (NH3 ), a fraction of the leachate must be purged and replaced by the
same volume of liquid every day to avoid the accumulation of metabolites in the system, such as NO2 and
NO3 . Without purge, these toxic metabolites accumulated in the recirculated leachate and decreased the biomass
growth.
The high variations of PB show that the biomass can
detach easily from the polypropylene surface. However, it
did not aect the microbial activity because PCO2 was stable and, according to Yang et al. [21], the biomass that
detached is mainly the inactive fraction. Since PB and
PCO2 , when using the continuous purge, were respectively
70% and 11% higher than the levels obtained with a discontinuous purge, the continuous purge was selected to carry
out the rest of the experiments.
Eect of ow rate on PCO2
Figure 3 shows the eect of the recirculation ow rate
and the packing material on PCO2 . For the polypropylene spheres, the PCO2 increased with the recirculation
ow rate from 16.5 3.7 to 25.6 3.7 g m3 h1 in the
range of recirculation ow rate from 01.5 L min1 . For
the ceramic beads, the PCO2 decreased from 20.3 4.8 g
to 15.0 1.0 g m3 h1 . PCO2 was also determined in the
three stages of each BTF as shown in Figure 1. For both
packing materials, PCO2 increased with the recirculation

ow rate in stages 2 and 3, middle and bottom of the


BTF, respectively, (data not shown). However, total PCO2
(comprising the three stages) increased for the polypropylene spheres and decreased for the ceramic beads. This
means that the stage 1 (top) of the BTF packed with
ceramic beads presented lower microbial activity. Visual
observations showed that biomass growth increased in both
BTFs when the recirculation ow rate increased. In the
BTF packed with ceramic beads, the biomass accumulation clogged the media, particularly in stage 1, producing
channelization of gas and liquid and eventually the total
clogging of stage 1. This could be the reason for the low
microbial activity in this stage. Consequently, frequent
washings of the BTF (every 2 or 3 days) were necessary.
The dierences observed between these two packing materials can be explained by the dierent void space: 90%
for the polypropylene spheres and 40% for the ceramic
beads. The polypropylene spheres provided greater space
for the biolm growth, and the accumulated biomass did
not easily clog up the support media, as was the case
for stage 1 of the BTF packed with ceramic beads (data
not shown).
The literature shows that the concentration of the
biomass at the surface of the bed is much higher in
BFs packed with synthetic media [22]. Verma et al.
[23] showed that high void fraction packing material is
necessary in wastewater bioltration, and Govind [24]
armed that one of the desired features of a good support media to remove contaminants is a void fraction of
more than 80%, as in the polypropylene spheres used in
this study.

Environmental Technology

819

Figure 4. Eect of recirculation ow rate on NH4 + conversion. The biotrickling lters (BTFs) were operated under an inlet carbon load
of 137 g C m3 day1 and an inlet nitrogen load of 60 g N m3 day1 . The BTFs were packed with () polypropylene spheres and ()
ceramic beads.

Eect of ow rate on NH4+ conversion


Figure 4 shows the eect of recirculation ow rate on NH4 +
conversion. A similar trend for both packing materials was
observed: increasing the recirculation ow rate decreased
the NH4 + conversion. Both packing materials achieved
a NH4 + conversion near 100% with no recirculation of
leachate. For the polypropylene spheres, when the recirculation ow rate increased from 0 to 1.5 L min1 , the NH4 +
conversion decreased from 99% to 86%, whereas for the
ceramic beads the NH4 + conversion decreased from 99%
to 89%.
Lee et al. [25] tested gaseous ethylene (C2 H4 ) removal
in BTFs packed with perlite and glass beads. The main
conclusion was that C2 H4 removal eciency was higher
at low trickling ow rates (0.10.2 L min1 ) because this
operating condition provides greater contact of the biolm
with the pollutant, and therefore greater mass transfer. On
the contrary, some studies have shown that increasing the
recirculation ow rate signicantly improves the removal
of water-soluble contaminants (such as ammonia and ethylene) in BTFs [21,25]. In the present study, since NH4 + is
transformed to NO3 consuming O2 , the absorption and diffusion of O2 in the biolm is determinant [16]. O2 has low
solubility in water, and the presence of a liquid layer over
the biolm acts as a barrier to the mass transfer of gases.
The trends observed in Figure 4 suggest that the barrier to
O2 intake by the biolm increased with the recirculation
ow rate.

Eect of carbon load on PCO2


Figure 5 shows the eect of carbon load (Cload ) on
PCO2 . For both packing materials operated under a
recirculation rate of 0 and 0.6 L min1 , the PCO2 was
around 440 g m3 day1 at a Cload of 137 g C m3 day1 .
However, for higher Cload , PCO2 of the BTF packed with
ceramic beads and at a recirculation rate of 0.6 L min1
increased more than both ceramic and polypropylene without recirculation. When leachate was not recirculated, both
BTFs presented similar PCO2 (around 635 g m3 day1 ) at
higher Cloads . Sharvelle et al. [15] showed that increasing
hydraulic loading improves wetting eciency and liquid
biolm interactions. The organic matter is therefore more
available, resulting in higher uptake and biodegradation
rates, which is observed as an increase of PCO2 .
The NH4 + load also increased with Cload when the concentration of the manure recipe was doubled or quadrupled.
For nitrifying autotrophic bacteria, cellular propagation
is dependent on the availability of NH4 + and O2 in the
environment. The bacterial growth rate is a function of
C and NH4 + concentrations, and an increase of NH4 +
load induces greater colonization of the packing media and
consequently increases CO2 production [7,13]. In wastewater treatment, Rocher et al. [13] showed that within a
certain time of operation, biomass in the BF is in equilibrium with NH4 + elimination. This explains the linear
relationship between the PCO2 and the Cload observed in
the present study.

820

K. Raby et al.

Figure 5. Eect of carbon load on CO2 production rate for the BTFs operated under () no recirculation with polypropylene spheres,
( ) no recirculation with ceramic beads and () a recirculation ow rate of 0.5 L min1 with ceramic beads.

Figure 6. Eect of nitrogen load on NH4 + conversion for the biotrickling lters operated under () no recirculation with polypropylene
spheres, ( ) no recirculation with ceramic beads, and () a recirculation ow rate of 0.5 L min1 with ceramic beads.

Eect of nitrogen load on NH4 + conversion


Figure 6 shows the eect of nitrogen load on NH4 +
conversion. For both packing materials tested with no recirculation, the NH4 + conversion ranged between 97100%.
On the other hand, for the BTF packed with ceramic beads
at a recirculation ow rate of 0.6 L min1 , the NH4 + conversion increased with nitrogen loads, going from 90%
to 99% for nitrogen loads of 60 and 240 gN m3 day1 ,
respectively.
The use of higher nitrogen loads could induce the maximal development of the nitrifying capacities of the ceramic
lter media, and NH4 + removal was therefore higher, as

observed in other studies. Rocher et al. [13] analyzed


dierent industrial installations of wastewater treatment
and observed that increasing nitrogen loads from 500 to
1000 gN m3 day1 on a BTF with recirculation caused
NH4 + elimination to increase from 80% to 100%. It was
also shown that nitrication eciencies can be superior
to 90% with NH4 + loads reaching 1200 gN m3 day1 . In
comparison, Dub et al. [26] achieved TKN elimination
performance of 75% with TKN loads of 20003800 ppm
operating traditional BFs packed with organic media when
treating manure at nitrogen loads similar to those tested in
the present study.

Environmental Technology

821

Figure 7. Eect of recirculation ow rate of leachate on nitrogen mass balance distribution (Concentration (% of mol N-species/mol
NH4 + inlet)) in the leachate at a xed nitrogen load of 60 g N m3 day1 for the biotrickling lters packed with (a) Polypropylene spheres
and (b) Ceramic beads. The nitrogen species were () NH4 + , () NO2 , and ( ) NO3 .

Distribution of nitrogen species in the leachate


Eect of recirculation ow rate
Figure 7 shows the eect of recirculation ow rate on nitrogen mass balance in the leachate. Nitrogen species are
shown in terms of leachate content (percentage mole/mole)
of NH4 + , NO2 and NO3 in inlet manure content of NH4 + .
For both packing materials, without recirculation, NO3
was present at a concentration around 22% (mole/mole),
while NH4 + and NO2 presented a concentration near
of 0% (mole/mole). When there was no recirculation of
the leachate, the nitrication process was nearly complete because NH4 + was not detected and the presence of

NO3 at high concentrations in the leachate conrms this


hypothesis.
In this study, BTFs operated with no recirculation
developed a malodorous biolm that changed colour from
yellowish to black, indicating the formation of anaerobic
zones [27]. Denitrication is an anoxic process where denitrifying bacteria use oxygen from the NO3 (coming from
nitrication) to perform cellular respiration [6]. This, as well
as the absence of NO2 in the leachate, led to the hypothesis
that denitrication may have occurred when there was no
recirculation of the leachate. At recirculation rates of 1 and
1.5 L min1 , NO2 was present in leachate. This may suggest an incomplete nitrication according to Equation (1) if

822

K. Raby et al.

Figure 8. Eect of nitrogen load on nitrogen mass balance distribution (Concentration (% of mol N-specie/mol NH4 + inlet)) in the
leachate with no recirculation for the biotrickling lters packed with (a) polypropylene spheres and (b) ceramic beads. The nitrogen
species were () NH4 + , () NO2 , and ( ) NO3 .

the biolm was completely aerobic. However, in the case


of the present study, the presence of anaerobic regions in
the bed allowed us to hypothesize that the nitrogen pathway was part of incomplete denitrication as shown in
Equation (2).
Eect of nitrogen load
Figure 8 shows the eect of nitrogen load on nitrogen
mass balance in the leachate when there was no recirculation of leachate. For both packing materials, it shows
that NO3 , NO2 and NH4 + concentrations in the leachate
for the dierent nitrogen loads presented similar levels

for both packing materials at 60 and 240 gN m3 day1 .


For both BTFs, at 60 gN m3 day1 , a small level of, or
no denitrication occurred since NO3 was present in the
leachate at a concentration greater than 20% (mole/mole).
However, when BTFs were operated at a nitrogen load
of 240 gN m3 day1 , the levels of NO3 or NO2 in
the leachate were nearly zero. This suggests that denitrication probably occurred at higher nitrogen loads.
Rocher et al. [13] showed that nitrogen loads up to 800
1000 gN m3 day1 did not signicantly aect nitrication
performances in BTF. As mentioned above, increasing
the nitrogen load can induce the growth of specialized
microorganisms.

Environmental Technology

823

Table 4. Overall carbon and nitrogen eliminations when the biotrickling lter was packed with ceramic beads and
was operated under an inlet carbon load of 560 g C m3 day1 and an inlet nitrogen load of 240 g N m3 day1 with
a recirculation ow rate of 0.6 L min1 .
Carbon
Inlet ppm
22,240

Nitrogen

Leachate ppm

Removal
eciency %

Inlet
(NH+
4 ) ppm

Leachate (NH+
4,
NO
and
NO
)
ppm
3
2

Removal
eciency %

67

99.7

8778

757

91.4

Overall carbon and nitrogen elimination


Carbon elimination was studied in the BTF packed with
ceramic beads at a recirculation ow rate of 0.6 L min1
and a carbon load of 550 gC m3 day1 (equivalent to
23,360 ppm BOD and 22,250 ppm C). Table 4 shows that
more than 99% of inlet carbon and 91% of inlet nitrogen were removed, with mean carbon concentration of
67 ppm and mean nitrogen concentration (NO3 , NO2 and
NH4 + forms) of 757 ppm at the outlet of the BTF. As a
comparison, Youcai et al. [28] tested BOD and NH4 + elimination in a BF packed with aged refuse from landll. They
obtained 8798% carbon elimination at inlet concentrations
of 5401500 ppm BOD (equivalent to 5151430 ppm C)
and 2030% total nitrogen elimination at inlet concentrations of 500800 ppm NH4 + . This shows that in the present
study, the BTF packed with ceramic beads had very high
nitrogen and carbon removal eciencies. This phase of the
study was performed at the end of all the experiments mentioned previously. This means that the last experiment was
performed after the BTF packed with ceramic beads had
treated synthetic manure for more than 1 year. This conrms
the hypothesis that a high-eciency microbial community
can be developed to treat high loads of manure.
Conclusion
Nitrogen elimination was studied in two BTFs packed with
ceramic beads and polypropylene spheres. It was determined that a continuous purge of leachate was necessary
to improve development of biomass on the media. Increasing leachate recirculation increased CO2 production for the
BTF packed with polypropylene spheres, and decreased
CO2 production for the BTF packed with ceramic beads.
For both packing materials, when increasing carbon and
nitrogen loads in manure, CO2 production increased without recirculating the leachate and the nitrogen removal was
in the range from 9799% of NH4 + feed. The increase
of the recirculation ow rates of the leachate decreased
NH4 + elimination and promoted the production of NO2 in
the leachate. Ceramic beads and polypropylene spheres are
good packing materials for removing carbon and nitrogenNH4 + , with removal eciencies of more than 99% for
both pollutants without recirculating the leachate for nitrogen loads up to 240 gN m3 day1 and 550 gC m3 day1 .
However, with recirculation of the leachate, ceramic beads

packing became clogged due to biomass accumulation,


particularly in the rst stage. The low void fraction of
the packed ceramic beads compared with the polypropylene spheres make it an inappropriate media for BTF with
recirculation of the leachate.

Acknowledgements
Michle Heitz would like to express her sincere thanks to the
Natural Science and Engineering Research Council of Canada
(NSERC-Strategic and Discovery Grants) for the nancial support
of this project.

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