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Design and development of a bench scale vegetable oil based wet packed
bed scrubbing system for removing producer gas tar compounds
Prakashbhai R. Bhoi a, Raymond L. Huhnke a,, Ajay Kumar a, Krushna N. Patil a, James R. Whiteley b
a
Department of Biosystems and Agricultural Engineering, Oklahoma State University, Stillwater, OK 74078, USA
b
School of Chemical Engineering, Oklahoma State University, Stillwater, OK 74078, USA
a r t i c l e i n f o a b s t r a c t
Article history: The overall goal of this study was to design, fabricate and evaluate a vegetable oil based wet packed bed scrubbing
Received 30 June 2014 system to study the removal of model producer gas tar compounds, i.e., benzene, toluene, and ethylbenzene. The
Received in revised form 23 January 2015 designed column was 0.5 m diameter by 1.1 m tall and contained 6-mm raschig rings. Soybean and canola oils
Accepted 30 January 2015
were used as solvents. These oils were not statistically (p N 0.05) different in removal efciencies of benzene,
Available online 14 February 2015
toluene and ethylbenzene. Packing specic constants of Billet and Schultes (1999) correlation (CV = 0.80 and
Keywords:
CL = 2.40) were found experimentally. These constants can be used to predict height equivalent to a theoretical
Biomass producer gas tars plate (HETP) of laboratory or pilot scale vegetable oil based wet packed bed scrubbing systems. The pressure drop
Wet packed bed scrubbing system across the column was in the range of 6.7 to 18.8 mm of water column.
Vegetable oil 2015 Elsevier B.V. All rights reserved.
1. Introduction high operating temperatures. Dry type cleaning devices include cyclone
separators, electrostatic precipitators (ESP), and various types of lters.
Given the growing concerns over climate change, national energy These equipments are mainly used for the particulate removal [1012].
security and increasing global demands, there is an urgent need for de- Wet gas cleaning processes are often used for tar removal. These include
veloping sustainable biofuels, bioproducts, biopower, and bioenergy [1]. spray towers, impingement scrubbers, venturi scrubbers, packed bed
Biomass has been identied as a potential source of sustainable energy scrubbers, wet electrostatic precipitators, wet cyclones, and oil based
due to its availability in large quantities [2,3]. Biomass conversion using gas washers.
thermochemical processes is one of the pathways in producing liquid Spray towers and impingement, venturi and packed bed scrubbers
biofuels and chemicals. are the most common types of wet scrubbers applied in producer gas
Gasication is one of the most common thermochemical conversion cleaning application [1317]. The performance of wet scrubbing
technologies. The major challenge of the gasication pathway is the re- systems is measured by wet scrubbing efciency which is dened as
moval of impurities including tars [46]. Tars mainly consist of aromatic the concentration difference between the inlet and outlet streams divid-
and poly aromatic hydrocarbons for the gasication temperature over ed by the inlet stream concentration [18]. Spray towers are simple and
800 C [7]. Primary methods of tar removal include optimization of op- inexpensive; however, they are the least efcient [19]. Impingement
erating and design parameters. Operating variables such as gasifying scrubbers are about 70% efcient. To achieve higher efciencies, im-
agent, equivalence ratio (ER), temperature, and residence time have pingement scrubbers are connected in series [20]. Tar removal efcien-
signicant effects on the tar formation and decomposition [8]. In the cies of venturi scrubbers range from 50 to 90% [10]. Packed bed wet
secondary methods, tar reduction measures are implemented on the scrubbers have the highest tar removal efciencies of 80 to 99% [21].
downstream side of the gasier. Secondary tar removal approaches Wet scrubbing of tars involves absorption of gaseous tar compounds
employ dry or wet-type equipment or high temperature (thermal or in the scrubbing solvents. Water is the most common scrubbing solvent
catalytic cracking) processes [9]. Thermal and catalytic tar cracking pro- in biomass producer gas based wet scrubbing studies [14,15,17,19]. The
cesses obtain high conversion efciencies; however, these processes are major drawbacks in using water as a scrubbing solvent is the low solu-
energy intensive and require an external energy supply to maintain the bility of tar compounds and costly wastewater treatment processes [22].
Vegetable, engine, and waste cooking oils and biodiesel have been stud-
ied as solvents for the removal of tars and volatile organic compounds
Corresponding author at: 223 Agriculture Hall, Department of Biosystems and such as benzene, toluene, and, methanol in a bubble column [14,
Agricultural Engineering, Oklahoma State University, Stillwater, OK 74078-6021, USA. 2325]. Tar compounds including benzene, toluene, and ethylbenzene,
Tel.: +1 405 744 8417; fax: +1 405 744 6059.
E-mail addresses: prakash.bhoi@okstate.edu (P.R. Bhoi),
being lipophilic in nature, can mix comparatively well with vegetable
raymond.huhnke@okstate.edu (R.L. Huhnke), ajay.kumar@okstate.edu (A. Kumar), oils because these oils have saturated (palmitic and steric acids) and un-
patilkn@hotmail.com (K.N. Patil), rob.whiteley@okstate.edu (J.R. Whiteley). saturated (oleic, linolenic and linoleic acids) fatty acids which are also
http://dx.doi.org/10.1016/j.fuproc.2015.01.042
0378-3820/ 2015 Elsevier B.V. All rights reserved.
244 P.R. Bhoi et al. / Fuel Processing Technology 134 (2015) 243250
lipophilic in nature. Soybean oil is one of the largest sources of vegetable The design (operating) gas velocity of the column is often determined
oils in the U.S. [26]. Additionally, the state of Oklahoma is the second using the manufacturer's pressure drop correlation for the given pack-
largest producer of canola oil. These oils, i.e., soybean and canola, are ings. In the absence of manufacturer's data, the diameter of the
less expensive than organic solvents such as acetone and isopropanol column of 0.5 m was determined using a generalized pressure-drop
[27]. Because very little information is available on vegetable oil based correlation (GPDC) of Eckert [3133] as modied by Strigle [34].
wet packed bed scrubbing systems, the objective of this study is to
design, fabricate and evaluate such a system for the removal of tar
compounds. 2.1.2. Height of the column
The height of the packed bed column was determined using equilib-
2. Materials and methods rium stages and height equivalent to a theoretical plate (HETP).
compounds would vaporize completely. A check valve was installed be- n is the number of discharge hole of a liquid distributor
tween the heater and the injection port of the tar compounds to prevent g is the gravitational acceleration = 9.8 m/s2
back-ow of tar vapors. As a safety precaution, a brass rupture disc was h is the liquid head above the orice, m.
installed prior to the absorption column to release excessive pressure.
The model tar compounds were procured from Sigma Aldrich. The Using the above head-ow correlation, a liquid distributor was de-
purity values of benzene, toluene and ethylbenzene were 99.5%, 99.7%, signed considering the diameter of the holes of 0.15 mm, design solvent
and 99.8%, respectively [18]. A mixture of tar compounds was prepared ow rate of 63 ml/min, pressure head of 20 psig, and coefcient of dis-
by weight distribution, benzene: 50%, toluene: 30%, and ethylbenzene: charge of 0.4. The number of holes were determined as 9. Perry et al.
20% which is comparable to the content of tar collected from a uidized [28] recommended at least 40 irrigation points per m2 with 60
bed gasier [13]. The prepared mixture was lled in a 100-ml gas-tight 100 per m2 being ideal. He also stated that a drip point density over
syringe (part number 009760, SGE Analytical Science, Austin, TX) with a 40 showed little difference in packing efciency. In this study, a drip
luer lock needle (part number 039827, SGE Analytical Science, Austin, point density of 4125 drip points/m2 was determined considering that
TX). A syringe pump (Model KDS 280.200, KD Scientic, Holliston, the liquid distributor consists of 9 holes of 0.15 mm diameter and a
MA) was used to maintain a constant injection rate of the model tar packed column of 50 mm diameter which is well above the required
compounds mixture into the hot air stream. drip point density. As a comparison, Janzen et al. [42] distributed
water in an 80-mm diameter column using a multipoint source distrib-
2.2.3. Liquid (solvent) distribution utor, having a drip point density of 3976 drip points/m2.
The liquid distribution is the most important aspect of the wet scrub- A liquid (solvent) distribution system consists of a multi-point liquid
bing system because it inuences the mass transfer efciency of the distributor to provide a uniform distribution of solvent (Fig. 3), a sump,
packing. Perry et al. [28] stated that a single spray nozzle can serve the and peristaltic pump (model PC2 70-7002, Harvard Apparatus,
purpose of liquid distribution in a small column. Accordingly, prelimi- Holliston, MA) which is compatible with the selected solvents. The
nary tests were conducted using six different types of commercial sump (0.8 l in volume) was placed in the water bath heater to maintain
spray nozzles to determine the spray distribution of soybean and canola the solvent at the desired temperature.
oils. Results showed that the selected nozzles were not able to
adequately spray the oils due to the high viscosities of oils. Other
spray nozzle options claiming to handle high viscous liquids were 2.2.4. Instrumentation and measurements
explored; however, these were deemed too expensive. As the result, it A mass ow controller (Model GFC37S-VADL2-A0, Aalborg Instru-
was decided to design and fabricate a liquid distributor to spray vegeta- ments and Controls, Inc., Orangeburg, NY) was used to measure and
ble oils uniformly on the top of the packings. control the air ow rate. Type-K thermocouples were used to measure
Perry et al. [28] stated that the orice liquid distributor is a common the temperature of inlet and outlet air streams, air at tar injection
type of liquid distributor for an absorption process. The liquid distribu- point, and solvent. A U-tube manometer (020 of H2O) was installed
tor was designed based on the head-ow correlation given below. on the packed bed column to monitor the pressure drop across the col-
umn. A differential pressure transducer (Model number GC52, Ashcroft
p
Q C D Ah n 2gh 2 Inc., Stratford, CT) was used to log the pressure drop across the column.
Temperatures, air ow rate, and pressure drop across the column were
where, recorded using a DaqView program (part number OMB-DAQ-55, Omega
Engineering, Inc., Stamford, CT, USA). The compositions of inlet and out-
Q is the volume ow rate, m3/s let gas streams were analyzed using a gas chromatography/mass spec-
CD is the coefcient of discharge = 0.4 troscopy (GC/MS). Two replications of each experimental condition
Ah is the cross sectional area of a hole, m2 were used. A statistical analysis was performed using a split plot
P.R. Bhoi et al. / Fuel Processing Technology 134 (2015) 243250 247
100
60
40 SO - 30C
SO - 40C
SO - 50C
20 CO - 30C
CO - 40C
CO - 50C
0
0 10 20 30 40 50 60
Time, min
Fig. 5. Effect of solvent type and temperature on the removal efciency of toluene at a bed
height of 0.5 m and solvent ow rate of 53 ml/min [SO: soybean oil, CO: canola oil at
solvent temperatures of 30, 40 and 50 C].
Fig. 3. Photographic view of solvent distributor.
100 100
Ethylbenzene Removal Efficiency, %
Benzene Removal Efficiency, %
80 80
60 60
40 SO - 30C 40 SO - 30C
SO - 40C SO - 40C
SO - 50C SO - 50C
20 CO - 30C 20 CO - 30C
CO - 40C CO - 40C
CO - 50C CO - 50C
0 0
0 10 20 30 40 50 60 0 10 20 30 40 50 60
Time, min Time, min
Fig. 4. Effect of solvent type and temperature on the removal efciency of benzene at a bed Fig. 6. Effect of solvent type and temperature on the removal efciency of ethylbenzene at
height of 0.5 m and solvent ow rate of 53 ml/min [SO: soybean oil, CO: canola oil at a bed height of 0.5 m and solvent ow rate of 53 ml/min [SO: soybean oil, CO: canola oil at
solvent temperatures of 30, 40 and 50 C]. solvent temperatures of 30, 40 and 50 C].
248 P.R. Bhoi et al. / Fuel Processing Technology 134 (2015) 243250
of tar compounds in the solvent increases due to solvent recycling. It is aph is the specic interface area between the phases, m2/m3
also important to note that the concentration of solute in solvent has a dh is the hydraulic diameter of the dumped packing, m
signicant impact on tar absorption efciency [39]. L is the kinematic viscosity of liquid, m2/s
V is the kinematic viscosity of gas or vapor, m2/s
3.2. Determination of Billet and Schultes [38] packing specic constants for DV is the diffusion coefcient of solute in gas or vapor, m2/s
the prediction of height equivalent to a theoretical plate (HETP) DL is the diffusion coefcient of solute in liquid, m2/s.
Perry et al. [28] stated that the height equivalent to a theoretical Theoretical liquid holdup correlation of Billet and Schultes [38] is
plate (HETP) which applies to design dilute absorption columns is given below:
given below.
1 =
1 2 3
ln hL 12 L uL a : 12
HETP HTU OV 4 g L
1
myx Billet and Schultes [38] theoretical holdup is based on the channel
L. 5 model which assumes the void volume of random packing by vertical
V ow channels. However, in real applications, the ow of phases deviates
due to the shape of random packing and the surface area of the packing
where, often partially covered by liquid. Therefore, theoretical liquid holdup
prediction deviates from the real column holdup. Billet and Schultes
HETP is the height equivalent to a theoretical plate, m [38] stated that the deviation of real holdup from theoretical holdup
is the stripping factor can be conveyed by considering hydraulic surface area of the packing.
myx is the slope of the equilibrium curve, kmol/kmol Accordingly, the real holdup of the column can be predicted by the fol-
L is the molar ow of the liquid, kmol/h lowing equation provided by Billet and Schultes [38].
V is the molar ow of the gas or vapor, kmol/h
1 = 2
1 h =3
HTUOV is the overall height of a gas-phase mass transfer unit, m. 2 3 a
hLS 12 L uL a 13
g L a
The overall height of a gas-phase mass transfer unit (HTUOV) de-
pends on the height of a gas-phase mass transfer unit (HTUV) and height The hydraulic surface area (ah) equation described by Billet and
of a liquid-phase mass transfer unit (HTUL). The overall height of a gas- Schultes [38] is given as follows.
phase mass transfer unit (HTUOV) correlation provided by Billet and !0:1
Schultes [38] is given below. uL L ah uL L 0:15 uL 2 a
ReL b5 : Ch 14
uV myx uL a L a a L g
HTU OV HTU V HTU L 6
V aph L=V L aph !0:1
uL L a u 0:25 uL 2 a
ReL 5 : h C h 0:85 L L 15
1=2 a L a a L g
1=6 01=2 DL aph
L aph C L 12 u L a 7
dh a where,
Table 3
dh 4 11
a Experimental liquid holdup for air-vegetable oil wet packed bed scrubbing system for the
given bed height, solvent temperature and solvent ow rate.
where,
Bed height Temperature Liquid holdup, ml
m C
Flow rate
uV is the velocity of gas or vapor with reference to free column
cross section, m/s 53 ml/min 63 ml/min 73 ml/min
uL is the velocity of liquid with reference to free column cross Mean S.E. a
Mean S.E. a
Mean S.E.a
section, m/s 0.5 30 145 21 168 18 190 14
Vaph is the gas phase volumetric mass transfer coefcient, 1/s 0.5 40 135 7 140 0 165 7
Laph is the liquid phase volumetric mass transfer coefcient, 1/s 0.5 50 110 14 120 14 135 7
CL is the packing specic constant for liquid phase 0.8 30 270 14 290 0 315 7
0.8 40 240 0 260 0 280 0
CV is the packing specic constant for gas or vapor phase 0.8 50 215 7 225 7 243 4
uL is the mean effective velocity of liquid, m/s 1.1 30 385 7 425 7 455 7
hL is the column liquid holdup, m3/m3 1.1 40 360 14 375 21 390 28
is the void fraction, m3/m3 1.1 50 330 0 345 7 360 14
a is the specied surface area of the dumped packing, m2/m3 a
Standard error.
P.R. Bhoi et al. / Fuel Processing Technology 134 (2015) 243250 249
for the raschig rings of 6-mm size. Therefore, the hydraulic constant (Ch) the friction between uid streams and packing surfaces and thus the
was determined using experimental data of the column holdup of this pressure drop across the column increases.
study in which the bed height ranged from 0.5 to 1.1 m, solvent temper-
ature ranged from 30 to 50 C and solvent ow rate ranged from 53 to
4. Conclusions
73 ml/min (Table 3). The average value of Ch = 2.52, found experimen-
tally using liquid holdup data provided in Table 3, was used to predict
A vegetable oil based bench scale wet packed bed scrubbing system
the liquid holdup in the subsequent calculation.
was successfully designed, fabricated and evaluated to study the remov-
The prediction of the overall height of a gas-phase mass transfer unit
al of model tar compounds. The system consists of a gas mixing system
(HTUOV) requires empirical packing specic constants (CV and CL). Billet
designed to achieve a desired concentration of tar in an air stream and a
and Schultes [38] provided these constants for various packings which
liquid distributor that was designed and fabricated to uniformly distrib-
were validated for an air-water system. However, these constants are
ute the high viscous vegetable oils.
not available for the raschig rings of 6 mm size used in this research.
It was found that soybean and canola oils were not statistically
For the estimation of CV and CL, an experimental HETP is required. The
(p N 0.05) different in removal efciencies of benzene, toluene and eth-
experimental HETP of 0.11 m was determined using the optimum bed
ylbenzene. The packing specic constants CV = 0.80 and CL = 2.40 of
height of 1.1 m reported in Bhoi et al. [18] and 10 theoretical stages as
Billet and Schultes [38] correlation were found using experimental
determined in Section 2.1.2. Using the experimental HETP of 0.11 m of
data. These constants can be used to predict the height equivalent to a
this study, constants CV = 0.80 and CL = 2.40 were determined using
theoretical plate (HETP) for laboratory or pilot scale vegetable oil
Billet and Schultes [38] mass transfer correlations.
based wet packed bed scrubbing systems.
The pressure drop across the column varied in the range of 6.7 to
3.3. Pressure drop across the column
18.8 mm of water column which is well within the acceptable range
of pressure drop for a bench or laboratory scale wet packed bed
Even though the packing material provides large interfacial area for
scrubbing system.
the mass transfer of model tar compounds, it increases pressure drop
across the column due to friction between uid streams and the packing
surface. A high mass transfer and a low pressure drop resulting in low Acknowledgments
energy consumption are very important for the performance of wet
packed bed absorption column. For the given packings, solvent, and This study was funded, in part, through a grant from the National Sci-
air ow rate, the pressure drop across the column is a function of the ence Foundation EPSCoR Program No. EPS-0814361 and the Oklahoma
packed bed height, solvent temperature, and solvent ow rate. The Agricultural Experiment Station. Authors also acknowledge vital contri-
pressure drop across the column as a function of bed height and solvent butions of the Biosystems and Agricultural Engineering Department
ow rate for two solvent temperatures (30 and 50 C) is shown in Fig. 7. staff members: Mr. Mark Gilstrap, Mr. Wayne R. Kiner, Mr. Jason Walker
As shown, at the solvent temperature of 30 C, as the bed height in- and Mr. Mike Veldman and Dr. Mark E. Payton from the Department of
creased from 0.5 to 1.1 m, the pressure drop across the column in- Statistics.
creased by over 100% from 7.3 to 16.1, 8.0 to 17.9 and 8.7 to 18.8 mm
of water column at the solvent ow rates of 53, 63, and 73 ml/min, re-
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