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Abstract
Although thermophilic treatment systems have recently gained considerable interest, limited information exists on the
comparative performances of membrane-coupled bioreactors (MBR) at thermophilic and conventional conditions. In
this study aerobic MBRs operating at room temperature (20 1C) and at lower thermophilic range (45 1C) were
investigated for the treatment of dissolved air otation (DAF) pretreated pet food wastewater. The particular
wastewater is characterized by oil and grease (O & G) concentrations as high as 6 g/L, COD of 51 g/L, BOD of 16 g/L
and volatile fatty acid (VFA) of 8.3 g/L. The performances of the two systems in terms of COD, BOD and O & G
removal at varying hydraulic retention time (HRT) are compared. COD removal efciencies in the thermophilic MBR
varied from 75% to 98% and remained constant at 94% in the conventional MBR. The O & G removal efciencies
were 6686% and 98% in the thermophilic and conventional MBR, respectively. Interestingly, high concentrations of
VFA were recorded, equivalent to 5073% of total COD, in the thermophilic MBR efuent. The observed yield in the
thermophilic MBR was 40% of that observed in the conventional MBR.
r 2005 Elsevier Ltd. All rights reserved.
Keywords: Thermophilic; MBR; Removal efciency; High strength wastewater; Oily wastes
0043-1354/$ - see front matter r 2005 Elsevier Ltd. All rights reserved.
doi:10.1016/j.watres.2005.08.030
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4300 R. Kurian et al. / Water Research 39 (2005) 42994308
settleability as documented by C - etin and Surucu (1990), generated from a rendering facility in St. Marys,
Barr et al. (1996), Tripathi and Grant Allen (1999) and Ontario, producing intermediates for pet food from
Lapara and Alleman (1999) with increasing tempera- byproducts of meat processing industry. The wastewater
ture. At the low biomass yields observed under is characterized by particularly high concentrations of O
thermophilic conditions, the washout of biomass due & G, which would be detrimental to any biological
to poor settlability is a critical issue, affecting process treatment system. The wastewater generated at this
stability. MBR technology becomes particularly attrac- facility undergoes physical separation of solids and O &
tive when the retention of solids for extended periods of G using a DAF. The high variability in the wastewater
time is a critical issue (Chen et al., 2003). MBR generated is depicted in Table 1. In the experiments
technology has been widely used to treat industrial conducted in this study the DAF efuent was employed.
wastewaters (Bouhabila et al., 2001; Scott and Smith,
1997) at mesophilic or room temperatures. But few 2.1. Experimental setup
researchers have explored the potential of a thermophilic
MBR (Lopetegui and Sancho, 2003; Joore et al., 2002; 2.1.1. Thermophilic MBR
Lapara et al., 2001). The system setup, as illustrated in Fig. 1(a), consisted
Limited information exists on MBR systems treating of a 0.5 L intermediate storage tank followed by a 3.5 L
the same high strength wastewater at thermophilic glass reactor. Thermophilic seed sludge was obtained
conditions and at typical MBR conditions or with no from an existing thermophilic treatment facility operat-
temperature control. The novelty of this research project ing at 40 1C. The reactor temperature was maintained at
lies primarily in the comparative side-by-side perfor- 4573 1C using a Corning hotplate stirrer. The reactor
mance assessment of the two MBR and its application in was aerated continuously with compressed air through
treating animal fat-contaminated wastewaters. The air diffusers. A peristaltic pump (Minipuls3, Gilson Inc.,
project also deals with a highly complex wastewater Canada) was used to pump inuent continuously into
and the results presented here contradict existing the reactor and mixed liquor through an external cross
literature available on thermophilic treatment systems ow membrane, with the retentate recycled back to the
with respect to the yield and impact of food to reactor and the permeate collected. The membrane
microorganism ratio (F/M). The failure of the conven- employed was a UMP-153, Pall Biopharmaceuticals,
tional anaerobic digester to treat this wastewater makes with a pore size of 0.2 mm and surface area of 0.08 m2.
this research an interesting and potential solution to the The particular membrane was selected owing to its
problem. In this paper, the authors compare the ability to withstand high temperatures (maximum of
performance of two MBR systems operated at thermo- 80 1C) as compared to that used in the conventional
philic range (45 1C) and room temperature (1820 1C) to MBR (maximum of 40 1C).
treat high strength rendering wastewater. The system was operated for 158 days: at a 7-day
HRT and SRT of 35 days for 75 days (days 075) and at
5-day HRT and SRT of 30 days for 83days (days
2. Experimental conditions 76158). The SRT was calculated based on wastage of
sludge incurred due to the washing of the membrane
Laboratory-scale MBRs were operated under varying rather than deliberate wastage, as this was deemed
hydraulic retention time (HRT) and temperature condi- unnecessary. The membrane was disconnected and
tions. The wastewater treated in the experiment was cleaned by backwashing using tap water, reversing the
Table 1
Raw and DAF efuent characteristics
inuent and efuent ports and nally washing with 1% revealed that less than 1.5% of the suspended solids
nitric acid solution as recommended by vendor. The were ner than 1.2 mm, accordingly TSS and VSS were
cleaning procedure took 1520 min per washing, there- measured using the Standard method 1.2 mm lter paper
fore, did not signicantly interrupt the continuous (APHA, 1998). Samples were dried at 105 1C till
operation of the MBR. constant weight was attained, weighed, and then heated
to 550 1C for 15 min and weighed again. Total and
2.1.2. Conventional MBR soluble COD were determined using the HACH Odyssey
The experimental setup, as illustrated in Fig. 1(b), Analyzer and the heating reactor with standard HACH
consisting of a 150 L storage tank followed by a 27 L testing kits. Ammonia, nitrate and nitrite were deter-
activated sludge reactor, was started with sludge from a mined using a high-performance liquid chromatograph
local municipal treatment plant. The reactor, operating (HPLC, Dionex Canada Ltd., Oakville, Ont). Soluble
at room temperature of 1872 1C, was aerated with samples were extracted by ltering through a 0.45 mm
compressed air through air diffusers. The ZW-1 lter paper (Wheaton). Dissolved oxygen (DO) was
membrane module from Zenon Environmental, Oak- measured with a portable YSI Dissolved Oxygen Meter
ville, Ont, with a pore size of 0.04 mm and surface area of Model 50. The VFA concentration was analyzed by a
0.047 m2 was employed to retain reactor solids. A gas chromatograph (Varian CP 3800) with ame
peristaltic pump (Minipuls3, Gilson Inc., Canada) was ionization detector (FID) equipped with a fused silica
used to draw permeate through the immersed membrane column (30 m 0.32 mm 5 mm). Nitrogen was used as
unit and pump inuent into the reactor. The storage carrier gas at 5 mL/min. detector and injector tempera-
tank was replenished with DAF efuent every 57 days. ture were set at 200 1C while the oven was programmed
The system operation continued over 105 days: at 6.3- to 110165 1C at a ramp of 20 1C/min for 9.25 min.
day HRT for 85 days (day 085) and at 5-day HRT for
20 days (days 86105). The SRT was calculated as 290
days based on sludge wastage due to sampling and 3. Results and discussion
membrane cleaning.
3.1. Contaminant removal
2.2. Analytical methods
The two systems operated as completely stirred
The two systems were closely monitored throughout bioreactors with membrane modules serving to com-
the operating period. Inuent, reactor-mixed liquor and pletely retain biomass and are compared on the basis of
membranes permeate (nal efuent) were collected 23 HRT, though the reactors were of different volumes.
times per week for analytical purposes. Parameters The inuent and efuent quality at steady state for each
analyzed included total suspended solids (TSS), volatile HRT for thermophilic conditions and conventional
suspended solids (VSS), COD, BOD5, ammonia-N, MBR conditions is summarized in Table 2. It is
nitrate-N, nitrite-N and O & G. Inuent, reactor-mixed noteworthy that despite the short 20-day operation of
liquor and nal efuent samples were analyzed for the conventional MBR at 5-day HRT steady state was
BOD5 using Standard methods (APHA, 1998). Particle attained as reected by the low-standard deviations
size distribution in the thermophilic MBR, determined (Table 2), particularly considering the inuent varia-
using Masterizer 2000 (Malvern Instruments Ltd., UK), bility.
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4302 R. Kurian et al. / Water Research 39 (2005) 42994308
94.2712.5 (7)
62.3710.5 (6)
97.7715.3 (5)
The nal efuent contained only soluble contaminants
99.773.5 (7)
% removal
(Table 2) in both systems. Membranes facilitated
biomass retention and sludge age control as reected
100
by biomass concentrations as high as 15 g VSS/L in the
conventional MBR system and as high as 2.8 g VSS/L in
the thermophilic MBR. The steady-state biomass con-
11437360 (7)
451730 (6)
58780 (5)
centrations in the two MBRs (Table 3) reveal that in the
2575(7) conventional MBR, reactor biomass actually increased
5 days
Based on average inuent O & G value of 608372480 (6) mg/l during 5-day HRT run (numbers within parenthesis reect number of samples.).
extremely long SRT for both the runs), but decreased in
0
59.4710.2(8)
99.773.2 (8)
94.4712 (8)
4877150 (8)
71.6712 (6)
% removal
685778 (6)
596769 (6)
95.571.7 (11)
97.770.8 (11)
69.371.0 (10)
Thermophilic MBR nal efuent
78.7710 (10)
93.871.0 (8)
296717 (10)
6675 (8)
289373000 (10)
11997351 (39)
18177548 (28)
NH4N
TBOD5
O&G
(mg/L)
TCOD
Table 2 further corroborates the kinetic limitation and substantiates that increased solubility in and by itself
short contact time alluded to above. would not result in better O & G removal, as evidenced
Thermophilic treatment is reported to enhance O & G by the O & G removal in the conventional and
or lipid removal efciencies (Becker et al., 1997; Li thermophilic MBR at 20 1C and 45 1C, respectively.
et al., 2002). However, the data of this study clearly
3.1.3. Contaminant removal across membrane
It is clear from Fig. 2, depicting the relation between
Table 3 permeate and reactor sCOD, that 28% and 32% of
TSS and VSS maintained in the MBRs sCOD removal occurred by ltration, in thermophilic
TSS (mg/L) VSS (mg/L)
and conventional MBRs, respectively. Given the varia-
bility of the data, the contribution of physical ltration
Thermophilic MBR 31457106 (12) 27977100 (12) to sCOD removal in both reactors is deemed to be the
HRT 7day same. Since the overall COD removals were over 90%
Conventional MBR 85277814 (10) 79757589 (10) (except in thermophilic at 5-day HRT) the contribution
HRT 6.3day of membrane ltration to overall removal of sCOD is of
Thermophilic MBR 17667443 (7) 15687423 (7) the order 2%. The reduced physical COD removal
HRT 5day
observed in the thermophilic MBR can be attributed to
Conventional MBR 20,74274282 (6) 14,72573742 (6)
the coarser membrane (pore size 0.2 mm) employed in
HRT 5day
comparison to the membrane (pore size 0.04 mm) used in
(Numbers within parenthesis reect number of samples.). the conventional MBR. Furthermore, the higher solu-
bility of contaminants at 45 1C contributed to the escape
of contaminants through the membrane pores in the
14000 Conventional MBR thermophilic MBR.
y = 0.72x Thermophilic MBR
Membrane permeate COD (mg/L)
Table 4
Data on VFA in efuent and inuent of thermophilic MBR
Steady-state data
Ammonia-N (mg/L)
Nitrate-N (mg/L)
during the treatment of municipal sludges. Fothergill
and Mavinic (2000) have demonstrated the accumula- 1.5
tion of VFA in ATADs reaching as high as 757 mg/L at 220
digestion time of 3 days, clearly reecting incomplete
1
biodegradation.
In the conventional MBR 499% BOD removal
efciency was attained with VFAs contributing 21% of 210
0.5
the efuent COD during both runs. Acetic acid
contributed o5% of the efuent VFA in the conven-
tional MBR. The breakdown of VFAs in the conven- 200 0
tional MBR efuent is as follows: acetic acid: 572 mg/ 0 1 2 3 4
L, propionic acid: 2577 mg/L, isobutyric acid: Time (hr)
3279 mg/L, butyric acid: 2678 mg/L, valeric acid:
Fig. 3. Variation of NH4-N and NO3-N measured in batch
13 mg/L and isovaleric acid: 1773 mg/L. It is interesting experiments.
to contrast the persistence of higher VFA (propionic
through valeric acid) relative to acetic acid in the
conventional and thermophilic systems. Higher VFAs the reactors were operating at the same pH of 8.3, the
are known to be more slowly biodegradable aerobically different operational temperatures would affect different
than acetic acid, and thus their persistence in the ammonia stripping rates. Based on the reactor tempera-
conventional MBR is expected. Paradoxically, under tures and pH, the unionized ammonia would be 30%
thermophilic aerobic conditions, the higher VFAs are and 7% of the total ammonium nitrogen (TAN) in the
degraded while acetic acid and propionic acid are not. thermophilic and conventional MBR, respectively,
calculated based on Eq. (1) (Wyffels et al., 2003).
3.1.5. Ammonia removal
In the thermophilic MBR ammonia removal efcien- NH3 -N=TAN 10pH =e6344=273 C
10pH . (1)
cies of 83% and 62% were observed during the HRT Taking into consideration the low yield observed in
runs of 7 and 5 days, respectively, corresponding to the thermophilic MBR, it is understandable that a
average efuent concentrations of 197 and 363 mg/L considerable amount of the ammonia removal is due to
with minimal variation (Table 2). At the same time, the stripping of free ammonia. A nitrogen balance across
removal efciencies in the conventional MBR for the 6.3 the thermophilic MBR was calculated. The ammonia
and 5-day HRT runs were 59% and 62%, respectively stripped was calculated using Eqs. (2) and (3) (Tchoba-
(Table 2). noglous et al., 2003).
Batch nitrifying activity tests conducted on the
thermophilic MBR sludge, both at 45 1C and 20 1C ye H C 0o =PT , (2)
revealed no increase in nitrates or nitrites (Fig. 3). The
log10 H A=T B, (3)
nitrites were measured to be zero throughout both
experiments. It must be asserted that during both tests at where ye is the moles of ammonia gas per mole of air; H
20 1C and 45 1C, despite a drop of 10 mg/L of NH4-N is the Henrys constant at 45 1C (atm); C 0o is the
over the 4 h experimental period, the lack of increase in concentration of unionized ammonia in the reactor
nitrates indicates the minimal observed differences (mol NH4/mol liquid); PT is 1 atm; A, B are constants
between initial and nal concentrations are either due for temperature correction and T is temperature (1K).
to analytical error or due to abiotic losses. The lack of At the 7-day HRT steady-state period, ammonia-N
nitrates and nitrites in both lab-scale continuous MBRs stripped constituted 66%, N removed as efuent 21%
conrms the absence of nitrication. Therefore, ammo- and N removed in sludges was 13% of the inuent TKN
nia removal mechanisms in the systems are cell synthesis concentration of 1389 mg/L. These percentages corre-
and stripping of free ammonia. Considering that both spond to losses totaling to 459 mg N/d, 148 mg TKN/d
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R. Kurian et al. / Water Research 39 (2005) 42994308 4305
and 78 mg TKN/d, respectively. Similarly, at the 5-day A sustained increase in the F/M, beyond 1.1 g COD/g
HRT the percentages were: ammonia-N stripped, 75%; VSS day, in the thermophilic MBR was followed by a
efuent N, 25%; wasted sludge, 1.4% of inuent TKN dip in the COD removal efciency after a lag period of
of 2200 mg/L. These percentages for the 5-day HRT one HRT. This was observed twice. From day 88 to day
correspond to mass rates of 843 mg N/d, 298 mg TKN/d 95 the F/M was sustained over 1.1 g COD/g VSS, the
and 31 mg TKN/d, respectively. It is obvious from these COD removal efciency dropped immediately after the
results that the major mechanism for nitrogen removal 88th day and fell below 80% by day 95. The trend was
in the thermophilic was stripping. The difference in repeated when F/M was sustained over 1.1 g COD/g
ammonia stripped at the two HRTs is due to the VSS from day 127158, during which COD removal
difference in the efuent ammonia concentrations (Table dropped from over 90% to less than 80%. Similar trends
2), given the airow rate was same, 3 Lpm, throughout were observed in the conventional MBR when the F/M
the study. Since the unionized ammonia in the conven- increased above 0.5 g COD/g VSS day as apparent from
tional MBR was only 7% of TAN (Table 2) compared Fig. 4(b) with COD removal efciencies dropping to less
to the 30% in the thermophilic MBR, at the than 85%.
400450 mg/L of TAN, ammonia stripping would
account for less than 2% of the inuent TKN loss and 3.2.2. Yield comparison
can therefore be neglected. There is a wide variability in thermophilic yields
documented. Research studies conducted on slaughter-
house efuent at 45 1C recorded yield of 0.35 g SS/g
3.2. Operational performance parameters CODremoved (Gariepy et al., 1989; Couillard and Zhu,
1993). Others have reported yields of 0.022 g SS/g
3.2.1. Foodto-microorganism ratio (F/M) CODremoved (Johnson and Hall, 1996) at 45 1C for
F/M was calculated based on inuent total COD, synthetic whitewater and 0.16 g SS/g CODremoved
HRT and VSS in the reactor. The variability in F/M (Berube and Hall, 2000) at 55 1C for synthetic kraft
during the study was due to variations in inuent pulp mill condensate. In this experiment, the yield was
contaminant and not due to changes in biomass calculated from a plot of cumulative VSS produced
concentrations in the reactors. Interestingly, at similar versus the cumulative COD consumed as shown in Figs.
contaminant loading, the thermophilic system showed 5(a) and (b) for the thermophilic and conventional
2.2 times higher biomass-specic COD removal ef- system, respectively. The yield calculations for the
ciency than the conventional MBR as illustrated in Figs. thermophilic biomass were based on the sludge wastage
4(a) and (b), possibly due to enhanced solubility of long incurred by membrane cleaning and were found to be
chain organics at higher temperature. This indicates a 0.08 g VSS/g COD. The TSS to VSS ratio in the
biokinetic advantage for thermophilic treatment sys- thermophilic MBR was 1.1470.1 throughout
tems, in this case, contrary to the ndings of Lapara et the experimental period. The yield of 0.08 g VSS/g
al. (2000). COD is in agreement with the 0.0570.03 g VSS/g COD
HRT = 7 d HRT = 5d
120 4
110 3.50
HRT 6.3 HRT 5 3.5
100
COD removal efficiency (%)
100 d d 3.00
COD removal efficiency (%)
3
F/M (gCOD/gVSS-d)
F/M (gCOD/gVSS-day)
2.50 80
90 2.5
2.00
60 2
80
1.50 1.5
70 40
1.00 1
60 20
0.50 0.5
50 0.00 0 0
0 50 100 0 50 100 150
(a) Time (days) (b) Time (days)
Fig. 4. Effect of F: M ratio on COD removal efciency (a) conventional MBR; (b) thermophilic MBR.
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4306 R. Kurian et al. / Water Research 39 (2005) 42994308
y = 0.076x R2 = 0.9963
2
R = 0.9762 y = 0.186x+11.14
3 180
160
2.5
140
Cumulative VSS
Cumulative VSS
produced (g)
produced (g)
2 120
1.5 100
80
1 60
0.5 40
20
0 0
0 5 10 15 20 25 30 35 0 200 400 600 800 1000
(a) Cumulative
( COD consumed (g) b) Cumulative COD consumed (g)
Fig. 5. Yield calculation for biomass in (a) thermophilic MBR; (b) conventional MBR (Acharya et al., 2003).
a signicant impact on COD removal efciencies in both Gariepy, S., Tyagi, R., Couillard, D., Tran, F., 1989.
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