Journal of the Air & Waste Management Association

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Waste Gas Treatment in Biofilters

Hsiu-Mu Tang , Shyh-Jy© Hwang & Sz-Chwun Hwang

To cite this article: Hsiu-Mu Tang , Shyh-Jy© Hwang & Sz-Chwun Hwang (1996) Waste Gas
Treatment in Biofilters, Journal of the Air & Waste Management Association, 46:4, 349-354,
DOI: 10.1080/10473289.1996.10467470

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TECHNICAL PAPER
Waste Gas Treatment in Biofilters
Hsiu-Mu Tang and Shyh-Jy© Hwang
National Tsing Hua University, Hsin Chu, Taiwan, ROC
Sz-Chwun Hwang
Union Chemical Laboratories, ITRI, Hsin Chu, Taiwan, ROC
ABSTRACT
Biofiltration of polluted gas streams containing malodor-
ous triethylamine (TEA) was studied. The experiments
were conducted in a laboratory-scale reactor with a mixture
of sieved compost and chaff particles as the filter material
on which the microorganisms were immobilized. The
concentrations of TEA in the inlet gas varied from 0.32 to
3.45 g/m3 (78 ppmv to 841 ppmv), while the superficial ve-
locity of the inlet gas ranged from 60.1 to 322.2 m/hr. The
removal efficiency of triethylamine in the biofilter decreased
as the gas velocity or TEA concentration in the inlet gas
increased. Moreover, the elimination capacity of this biofilter
could reach up to 140 g/(m3 hr). When the loading of TEA
exceeded this critical value, substrate inhibition occurred
and the elimination capacity decreased. A mathematical
model predicting the removal efficiency of the pollutant
was also developed in this study. The inhibitory effect of
the substrate on the growth rate of the biomass was consid-
ered in this model. The proposed model could accurately
represent the experimental data obtained in this study.
INTRODUCTION
Amines are the major pollutants in the gaseous emissions
of chemical manufacturing factories. Triethylamine (TEA)
is a typical constituent of these organo-nitrogen pollutants.
Because amines have been demonstrated to be easily biode-
gradable, biofiltration is an excellent method to treat waste
gases containing these pollutants.1
IMPLICATIONS
Biofiltration has been validated as an advantageous air
pollution control technology for the purification of waste
gases with large volumes and low pollutant concentrations,
as compared to other conventional physical and chemical
methods such as incineration, scrubbing, and activated car-
bon adsorption. Moreover, biofiltration generally creates
no secondary pollution. This paper demonstrates that a
relatively high elimination capacity for triethylamine can be
obtained using a biofilter with an improved filter material.
In addition, the model developed in this paper can be used
to design the biofilter for the treatment of other waste gases,
especially when substrate inhibition occurs.
Volume 46 April 1996
ISSN 1047-3289 /. Air & Waste Manage. Assoc. 46: 349-354
Copyright 1996 Air & Waste Management Association
A biofilter contains filter materials (compost, peat, bark,
soil, or inert materials) on which microorganisms (mainly
bacteria) are immobilized to form a biolayer. When waste
gases pass through the reactor, target organic pollutants dif-
fuse into the biofilm as adsorption and instantaneous aero-
bic biodegradation occur. In general, natural filter materials
provide sufficient inorganic nutrients for microorganisms;
thus, the addition of nutrients is not required.2 Biofiltration
has been validated as an advantageous air pollution control
technology for the purification of waste gases with large vol-
umes and low pollutant concentrations, compared to other
conventional physical and chemical methods such as in-
cineration, scrubbing, and activated carbon adsorption.13
The reasons lie mainly in low investment and operating
costs, good operational stability, and high destruction effi-
ciency of pollutants.
Some experimental and theoretical investigations of
the biofilters have been performed. 410 Ottengraf et al.
studied the selection of the proper microorganisms for
the xenobiotic compounds, 4 kinetics of the biodegrada-
tion, 5 and reactor design.2-5 The inhomogeneous struc-
ture of natural filter materials such as compost and peat,
and the tendency for the packing materials to be com-
pacted or lumped, often induce nonuniform distribution
of the gas flow. This reduces the specific surface area,
and therefore the elimination capacity of the biofilter.
Several researchers2-6 have found new filter materials with
high porosity and adsorption capacity, hydrophilic prop-
erties, and minimum compaction. In addition, Peters et
al.7 modified the filter material with gypsum to prevent
the formation of clumps upon drying.
Leson et al.8 reported that the removal of ethanol in a
laboratory-scale biofilter was zero order with respect to etha-
nol. Ergas et al. 9 proposed that the removal of
dichloromethane, trichloroethene, and toluene followed first
order kinetics. Moreover, in the development of the kinetic
model, they considered the effect of the diffusion of the
substrates in the biofilm. Shareefdeen et al.10 derived and
validated a kinetic model of the biofiltration process for the
removal of methanol vapor. They took into account the ef-
fects of substrate inhibition and the diffusion of both the
substrate and oxygen.
Journal of the Air & Waste Management Association 349
 Tang, Hwang, and Hwang
For this research, the biofiltration of TEA was conducted
in a laboratory-scale biofilter. Effects of the gas flow rate and
inlet TEA concentration on the removal efficiency of TEA
were analyzed. The possibility of achieving higher elimina-
tion capacity in the biofilter with an improved filter mate-
rial, a mixture of narrow-sieved compost and chaff, was also
studied. Furthermore, a mathematical model was developed
to predict the elimination capacity, maximum elimination
capacity, and removal efficiency of TEA in the biofilter un-
der a wide range of operating conditions.
MATERIALS AND METHODS
Experimental Apparatus
The biofiltration experiments were conducted in a labora-
tory-scale reactor shown in Figure 1. The inner diameter
and the overall height of the reactor are 8 cm and 155 cm,
respectively. The biofilter was divided by perforated plates
into four 35 cm sections, and each section was packed with
25 cm of the filter material. A 5 cm distributor section filled
with 8 mm spherical glass beads was located at the bottom
of the column to ensure uniform distribution of the gas flow
across the biofilter.
Compressed air flowed through an air filter (Hankinson,
A20-04F-16P) before entering the humidification column.
The humidifier was an 8 cm ID acrylic column, 80 cm in
height, filled with 40 cm of 1/2-inch plastic pall-ring
packings (Norton). The relative humidity of the effluent air
stream from the humidifier was 95% to 99%, and its tem-
perature was controlled at 20 °C to 25 °C by using the water
in the humidifier.
Artificial waste gas was made by injecting pure liquid
TEA into the effluent air stream from the humidifier using a
syringe pump (Sage, Model 34IB) and a gas-tight syringe
Air
Humidifier
o o oo o
Drain
Figure 1 . Schematic diagram of the laboratory-scale biofilter unit: 1. air filter; 2. rotameter; 3. pall-
ring packings; 4. nozzle; 5.water reservoir; 6. pump; 7. gas-tight syringe; 8. syringe pump; 9. tem-
perature controller; 10. glass beads; 11. filter material; 12. sampling ports.
350 Journal of the Air & Waste Management Association
(Hamilton). TEA concentration of the gas flowing into the
biofilter was varied by adjusting the injection rate of the
solution and the flow rate of the air stream.
Operating Conditions
The concentration of TEA in the inlet gas varied from
0.32 g/m3 to 3.45 g/m3, while the superficial velocity of the
inlet gas ranged from 60.1 m/hr to 322.2 m/hr. The overall
loading of TEA increased from 18 to 261 g/(m3 hr). The
water content and pH of the filter material were kept at about
50% and 7%, respectively. It was found during the experi-
ments that ammonia formation was not significant. Most
of the nitrogen in TEA became N2 and soluble ammonium
salt. When the operating condition was changed, more than
three days were always required to reach the new steady
state, and the new steady-state TEA concentration profile
along the column was measured about four days after the
new steady state was reached.
Filter Material and Inoculum
The filter material was a mixture of an equal volume of
sieved compost (equivalent diameter: 1.2 mm to 2.5 mm)
and chaff (equivalent diameter 4 mm to 5 mm). The average
diameter of the compost particles was 2 mm. The compost
contained 45% digested sewage sludge and 55% yard trash.
The addition of chaff served to decrease the pressure drop
across the filter bed and prevent channeling. It also contained
certain nutrients that could be utilized by the microorgan-
isms. NaHPO4 and NaHCO3 were used as buffer salts to main-
tain the pH of the filter material in the range of 6 to 8.
The inoculum was activated sludge obtained from the
wastewater treatment plant of a fertilizer factory where
amines are the major pollutants treated. Microorganisms in
the activated sludge had been ac-
climated to the target pollutant;
thus, the required adaptation time
for microorganisms was reduced
considerably.
Sampling and Analytical
Methods
Five sampling ports separated by
equal distances were located along
the biofilter. Gas samples were col-
Purified gas lected simultaneously from the
sampling ports with Tedlar bags
over an approximate three-minute
period. After the bags were plunged
into an oven (50 °C) for one
minute to prevent the condensa-
tion of TEA, SOOu, gas samples were
then taken from the bags using a
gas-tight glass syringe. Concentra-
tions of TEA in the samples were
Volume 46 April 1996

then measured in a gas chromatograph (Varian 3400) equipped
with a 15ml x 0.53mm SPB-5 fused silica capillary column
with an immobilized polydimethylsiloxane liquid film 15(j,m
in thickness, and a flame ionization detector (FID). Nitrogen
was used as the carrier gas, and its flow rate was 12 ml/min.
A solution was made containing 2 g of the filter mate-
rial and 20 ml of distilled water. Its pH value, measured by a
pH meter (fenco, Model 6201), was defined as the pH value
of the filter material. In addition, water content of the filter
material was determined by drying the filter material at
105 °C for 12 hours.
THEORY
A schematic representation of the biofilm model is given in
Figure 2. The overall kinetics in the biofilter were represented
by the interactions among the microkinetics of the biodeg-
radation of the target pollutant in the biofilm, mass transfer
in the biofilm, and the flow pattern of the bulk gas phase.
Because the biofilm thickness is much smaller than the par-
ticle size, planar geometry can be used.
Microkinetics
The generalized form of the Monod equation11 is used in
this study to describe the microkinetics; thus the growth
rate for the microorganisms is given by:
s
[ iT (1)
V ! L SlmJ
where |x is the specific growth rate (1/hr), p,m is the maximum
specific growth rate (1/hr), ¥^ is the half saturation constant
(g/m3), S, is the substrate concentration in the liquid phase
(g/m3), and Slm is the maximum liquid-phase substrate
concentration above which growth is completely inhibited
(g/m3). The reaction rate for the substrate is given by:
(2)
where rs is the substrate utilization rate (g/(m3 hr)), Xv is
the biofilm dry density (g/m3), and Y, is the yield coefficient
(g biomass/g substrate).
Biofilm
sg Aerobic Anaerobic
Layer Layer
|
X
0i0M,
Figure 2 . Schematic representation of the model.
Volume 46 April 1996
Tang, Hwang, and Hwang
Material Balance
The material balance equations were established on the ba-
sis of the following assumptions:
(1) A steady state was reached in the biofilter for each
operating condition.
(2) The diffusion of the pollutant within the biofilm can
be represented by an effective diffusion coefficient,
De(m2/hr).
(3) The biofilm dry density was constant throughout the
filter bed.
(4) Mass transfer resistance in the gas phase was negli-
gible. Moreover, at the gas-biofilm interface, the pol-
lutant concentration in the gas phase was in
equilibrium with that in the biofilm, i.e., S{ = Sg/md,
where Sg is the substrate concentration in the gas
phase (g/m3), and md is the distribution coefficient.
(5) Triethylamine was degraded by aerobic microbial ac-
tivity. The thickness of the aerobic layer in the biofilm
or the effective biofilm thickness, 5e(|xm), is assumed
to be 15% of the actual biofilm thickness, 8.12
(6) Triethylamine was the only growth-limiting substrate
in the aerobic layer, while all other nutrients were in
excess.
(7) The flow pattern of the bulk gas was plug flow.
The material balance for the biofilm is:
d2S,
De- (3)
dx^
The boundary conditions are:
h (4)
x=0, Si =-2-
1 md
dS,
(5)
The mass balance for the bulk gas phase is:
dS^
(6)
The boundary condition is:
z = O,Sg = Sgi (7)
where Ug is the gas superficial velocity (m/hr), Sgi is the inlet
gas concentration (g/m3), z is the position along the biofilter
(m), As is the specific surface area (biolayer surface area per
unit volume of the biofilter, m2/m3), and N is the mass flux
of the substrate into the biolayer interface (g/(m2 hr)). Note
that N is given by:
dS!
dx x = 0
e (8)
""
Journal of the Air & Waste Management Association 351
Tang, Hwang, and Hwang

Numerical Method is assumed to be that of water, the biofilm thickness can

Sg and S, were obtained from equations 1 to 8 by orthogonal then be calculated from the following equations:
collocation, 13Newton-Raphson, and Runge-Kutta methods.
These methods were also used by Baltzis et al.14 (9)
N
and
Determinations of Model Parameters
The values of the parameters used in the model are shown (10)
in Table 1. The specific surface area, As, was obtained by the m
p

data fitting method,10 while the values of K^, Yit p.m, and n in where rp is the average radius of the compost particles, m p is
Table 1 are typical values reported in the literature.11'15 The the average weight of a single compost particle, and Np is
value of md is obtained from vapor/liquid equilibrium data the number of compost particles in the sample. The biofilm
for the triethylamine/water system.16 Since water is the ma- dry density was obtained by the following equation:17
jor constituent of the biofilm, md for triethylamine/water
system can be used for triethylamine/biofilm system with x=
(11)
negligible error. The maximum allowable substrate concen-
tration in the gas phase, Sgm, was obtained experimentally Note that the value of Xv obtained in this study lies in the
in the biofilter. It was defined in this study as the concentra- range of the values reported by Fan et al.18
tion at which the removal efficiency approaches zero at very The diffusivity of TEA in water at 25 °C is estimated to
low gas superficial velocity (3.6 m/hr). Moreover, Slm is ob- be 6.8xl0-6 m 2 /hr by the Wilke-Chang equation.19 Fan et al.18
tained from Equation 4. proposed an empirical equation for predicting the diffusivity
The biofilm thickness and biofilm dry density (dry of a substrate in a biofilm relative to that in water:
weight of biomass of the biofilm/volume of the wet biofilm) 0.43 X'
=1-
were determined by the dry weight method. 917 Equal 11.19+0.27 X 0 J (12)
amounts (0.4 g) of compost particles were taken from each
where De and Dw are the diffusivity of TEA (m2/hr) in a
section of the filter bed and mixed together. The weight of
biofilm and in water, respectively. According to this correla-
this sample was defined as Wj. It was dried in an oven at
tion, the major factor influencing diffusivity in the biofilm
105 °C for 12 hours. The weight of this dried sample was
is the biofilm dry density. In this study, the experimental
defined as W2. It was then put in a furnace at 600 °C for
value of the biofilm dry density (125000 g/m3) was substi-
one hour to burn off the biomass surrounding the compost
tuted into the correlation and a relative diffusivity of 0.18
particles. The weight of the sample after burning was de-
was obtained. Thus, the effective diffusivity of TEA in the
fined as Wo. Because the ash weight of the biomass was small
biofilm was 1.2 x 10 6 m2/hr.
compared to the weight of the compost particle, Wo could
represent the weight of the dried compost particles. Another
RESULTS AND DISCUSSION
experiment with the same drying and burning processes was
In order to understand the start-up process of the biofilter
also conducted for the raw compost particles to determine
and the physical adsorption capacity of the filter mate-
the possible loss of weight because of these processes. The
rial, experiments were performed in active and in poi-
results showed that this weight loss was negligible. The to-
soned (sterilized by HgCl 2 solution) biofilters. The
tal biofilm weight was obtained by subtracting the weight
biofilters were operated at a gas superficial velocity of
of the dried compost particles, Wo, from the weight of the
60.1 m/hr, corresponding to a residence time of 1 minute.
wetted bioparticles, Wa. If the physical density of the biofilm
The concentration of TEA in the
inlet gas stream was 0.32 g/m3.
Table 1 . Notation of the symbols and the values of the parameters used in the model. It was found that for a biofilter
to be effective, degradation
Parameter Value Ref Denotation rather than adsorption of the
A s (m 2 /m 3 ) 180 — Biofilm surface area per unit volume of reactor target pollutant must take place
De (m2/sec) 3.5 *10- 1 0 — Diffusivity of triethylamine in the biofilm
Ks(g/m3)
in the biofilter. In addition, ac-
10.0 15 half saturation constant
md(-) 0.0038 distribution coefficient climation of the microbial
n(-) 1.0 11 constant population to TEA was relatively
slm(g/m3) 3290 — substrate concentration with complete inhibition rapid. It took only eight days for
Xv(kg/m3) 125 _ biofilm dry density the removal efficiency to reach
Yi(g/g) 0.53 15 yield coefficient
100%.20
(x m (1/hr) 0.216 15 maximum specific growth rate
6 e (m) 1.65*10-5 — effective biofilm thickness Figure 3 shows the effect of
the inlet TEA concentration on

3 5 2 Journal of the Air & Waste Management Association Volume 46 April 1996
 Tang, Hwang, and Hwang

the concentration profile along the biofilter and the re-
moval efficiency of TEA. As shown in this figure, the
concentration of triethylamine throughout the biofilter
increased with increasing TEA concentration in the
inlet. As a result, the removal efficiency, RE (defined as
1- Sg/Sgl), decreased as the inlet TEA concentration in-
creased. This is similar to observations by Shareefdeen
et al.10 and Deshusses et al.21 in their studies of purifica-
tion of the methanol and ketones (methyl ethyl ketone
and methyl isobutyl ketone), respectively. Also shown in
this figure is the comparison of the experimental and
predicted values for TEA concentration in the biofilter.
This figure indicates that the predicted values agreed
with those obtained experimentally. The effect of the gas
velocity on the concentration profile along the biofilter
and the removal efficiency of TEA is shown in Figure 4.
The total amount of TEA entering the biofilter increased
with an increase in the gas velocity. Therefore, the removal
efficiency decreased as the gas velocity increased. The
predicted values shown in this figure agree well with the
experimental data, except for higher gas velocity. The
model underestimates the substrate concentration at
high gas velocity. This may be due to gas backmixing
and channeling.
Figure 5 compares the experimental data with those
predicted by the proposed model and Ottengraf's model.5
It is seen in this figure that the proposed model predicts
more accurately than Ottengraf's model, particularly for

1.0 0

0.9 10
U =75.6 m/hr
0,8 20

0.7 30

" 0.6 40
'Si
^ 0.5 50
an
60
0,4

Pred. Expt. S gi 70
0.3
— • 1.25 g/m3 80
0.2 A 1.84 g/m3
3
• 2.69 g/m 90
0.1

0.0 100
0.0 0.1 0.2 0.3 0.4 0.S 0.6 0.7 0.8 0.9 0.0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9

Figure 3. Effect of the inlet substrate concentration on the concen- Figure 4. Effect of the gas superficial velocity on the concentration
tration profile along the biofilter. profile along the biofilter.

1,0 (g/m3)
3
Ug=60.1 m/hr, Sgj-3.45 g/m 0.6 0.9 1.2 1.5 1.8 21 2.4 2.7 3.0 3.3 3.6 3.9
0.9 proposed model 180
Ottengrafs model
0.8 9 experimental data 160
U =75.6 m/hr
0.7
140 •
T 0-6
120
K* 0.5
dty

•
100
0.4
!
el
o
0.3 80 proposed model
Ug=322.2 m/hr, Sgi»0.32 g/m5 -- Ottengrafs model
Elii

0.2 proposed model experimental data

60
Ottengrafs model - / *
0.1 A experimental data
40

0.0 0.1 0.2 0,3 0.4 0.S 0,6 0.7 0.8 0.9 1,0 30 60 90 120 150 180 210 240 270 30C

Loading [g/(m3hr)]

Figure 5. Comparison of the experimental and predicted values Figure 6. Effect of the loading on the elimination capacity of the
for the substrate concentration in the biofilter. biofilter.

Volume 46 April 1i§6 Journal of the Air & Waste Management Association 3S3
Tang, Hwang, and Hwang
high inlet TEA concentration. The effect of the loading
on the elimination capacity of the biofilter is shown in
Figure 6. The elimination capacity EC g/(m3 hr) is de-
fined as:
EC= ^ - S -S (13)
V * »
where Q is the gas flow rate (m3/hr), Vf is the bulk vol-
ume of the filter material (m3), and Sge is the exit TEA
concentration (g/m3). Unlike the previous reports,514 the
elimination capacity did not reach a constant value but
decreased gradually from a peak value. This decrease was
the result of substrate inhibition. The maximum elimi-
nation capacity of the biofilter for TEA was approximately
140 g/(m3 hr) at the gas velocity of 75.6 m/hr. This value
was relatively high compared to the previous investiga-
tions for the biofiltration process.514-21-22 For the load-
ing of TEA lower than 140 g/(m3 hr), the removal
efficiency was always 100%. However, the removal
efficiency decreased when the loading is higher than
140 g/(m3 hr). It should be noted in this figure that the
elimination capacity predicted by the proposed model
agreed with that obtained experimentally. Moreover, the
model proposed in this study is better than that pro-
posed by Ottengraf5 when substrate inhibition occurs in
the biofilter.
CONCLUSIONS
This study shows that a laboratory-scale biofilter with
sieved compost and chaff particles as the filter material
effectively removes TEA from the gas stream. Increasing
either the gas velocity or inlet TEA concentration in-
creases the amount of TEA introduced into the biofilter,
and the removal efficiency of the biofilter decreases as
the amount of TEA introduced into the biofilter increases.
In addition, the elimination capacity of this biofilter can
reach up to 140 g/(m3 hr). As a result, when the loading
of TEA is lower than 140 g/(m3 hr), this pollutant can be
removed completely by the biofilter. A model derived in
this study to describe the biodegradation of TEA in the
biofilter is experimentally validated under various oper-
ating conditions. Moreover, the proposed model is bet-
ter than Ottengraf's model, especially at high inlet TEA
concentration or loading.
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About the Authors
S.-J. Hwang and H.-M. Tang are professor and Ph.D.
candidate, respectively, at the Department of Chemical
Engineering, National Tsing Hua University, Taiwan,
ROC. Dr. S.-C. Hwang is a research chemical engi-
neer at Union Chemical Laboratories, Industrial Tech-
nology Research Institute, Taiwan, ROC.
Volume 46 April 1996