ARTICLE

pubs.acs.org/IECR

New Correlation for Mass Transfer Characteristics of Spray Column

Tsubsa Tanda,† Koichi Shirai,† Yukihiko Matsumura,*,‡ and Hiroyuki Kitahara§
†
Department of Mechanical Science and Engineering and ‡Division of Energy and Environment, Hiroshima University,
1-4-1 Kagamiyama, Higashi-Hiroshima, Hirohsima 739-8527, Japan
§
Total System Laboratory, 3-23-6 Kinunodai, Tsukuba-Mirai, Ibaraki 300-2436, Japan

ABSTRACT: This paper presents a study of the mass transfer characteristics of a spray column being used as a dehumidification
device for air. The experiment was conducted using high humidity air and polyethylene glycol (PEG) as a desiccant solution over a
range of process conditions including various liquid flow rates, gas flow rates, water concentrations of PEG, temperatures of PEG,
and nozzle diameters. The performance of the spray column was evaluated in terms of volumetric mass transfer coefficients. The
results were well expressed by the correlation using dimensionless groups including the physical properties of the liquid and nozzle
diameter.

1. INTRODUCTION
Dehydration of air using liquid desiccant can be achieved using
various gas
liquid contactors including a packed tower, fall-
ing film tower, bubble column, and spray column. The spray
column can achieve efficient absorption because it produces
a lot of small droplets, resulting in a large contact area. There
have been many studies on spray columns. Kuntz and
Aroonwilas,1 Javed et al.,2 Kies et al.,3 Javed et al.,4 and
Taniguchi et al.5 evaluated experimentally the mass transfer
performance of a spray column to determine the mass transfer
coefficient. Biswas et al.6 obtained a correlation for the
pressure drop in a column. Boundyopadhyay and Biswas,7,8
Rajmohan et al.,9 Chein et al.,10 and Yang and Shaw11 obtained
the removal efficiency of absorption. Bandyopadhyay and
Biswas12 developed the models of removal efficiency. Kumar Figure 1. Experimental apparatus.
et al.13 tested the performance of wire mesh packing for
reducing carryover from the outlet of the column. Meikap’s 2. EXPERIMENT
group has determined the removal efficiency of particles in the
spray column.14
17 However, reports on the mass transfer The schematic of the experimental apparatus is shown in
correlation in the spray column are few. Chung and Wu18 Figure 1. The spray column is made of acrylic pipe. It has an
obtained a mass transfer correlation for the spray column for a internal diameter of 150 mm and a height of 650 mm. The length
triethylene glycol
air system. This correlation is useful for of the contact between the spray and air is 434 mm. The nozzle
predicting the mass transfer coefficient, but unfortunately, the employed in this study is of solid cone type (H. Ikeuchi Co. Ltd.,
effects of the nozzle diameter and physical properties of the 1/8 M JJXP 010 S303 (1.0 mm), 1/8 M JJXP 015 S303
desiccant solution were not included. Since the condition of (1.5 mm)). The air is first delivered to the bubbling unit by
the spray varies largely due to the physical properties of the the blower and humidified. This air is mixed with air from
liquid and type of nozzle, it is essential to determine their another line to control the humidity by dilution. The humidity
effect on mass transfer in the spray column. Thus, lack of a of the air is controlled by adjustments to the flow rate of each line.
correlation including these effects hinders the proper design of The air temperature is controlled by a temperature control bath
the spray columns. This fact encouraged us to further inves- with a heater. Mixed air is sucked into the spray column by a fan
tigate the mass transfer characteristics of spray columns placed downstream. The temperature and humidity of the air are
related to dehumidification of air. measured with thermocouples and humidity sensors at the inlet
The purpose of this study is to obtain a mass transfer and outlet of the spray column. The air flow rate is controlled by
correlation that includes the physical properties of the liquid the fan and measured with the flow meter at the inlet side of the
and the nozzle diameter of the spray column. As a model
system, a dehumidification device using liquid desiccant is Received: May 7, 2011
studied, in which high humidity air is used as the gas and Accepted: October 4, 2011
polyethylene glycol (PEG) is used as the liquid to absorb Revised: September 25, 2011
moisture from the air. Published: October 04, 2011

r 2011 American Chemical Society 13554 dx.doi.org/10.1021/ie200989k | Ind. Eng. Chem. Res. 2011, 50, 13554–13560
Industrial & Engineering Chemistry Research ARTICLE

spray column. The desiccant solution (PEG) is sprayed so as to The absolute humidity can be obtained from eq 3
contact with moist air in the cocurrent flow. The inlet liquid
Mw P w Mw P w
temperature is controlled by a temperature control bath. To H ¼ ¼ ð3Þ
prevent carryover of the solution, demisters are set in the M a Pa Ma ðPatm
Pw Þ
entrance and exist of the spray column. The details of experi-
mental conditions are shown in Table 1. The experiments Subsequently, the difference in absolute humidity between the
are operated using different liquid flow rates, air flow rates, inlet inlet and outlet of the spray column can be calculated by eq 4.
water concentrations, inlet liquid temperatures, and nozzle
ΔH ¼ H2
H1 ð4Þ
diameters.
The molar amount of transferred water is evaluated as follows.
3. MASS TRANSFER COEFFICIENT Fa Va
The performance of the spray column is evaluated by the ΔX ¼
ΔH ð5Þ
Mw
volumetric mass transfer coefficient, which is calculated accord-
ing to the amount of transferred water and the water vapor The vapor pressure of the PEG solution can be obtained using
pressure difference between air and PEG solution. The amount the liquid temperature and water concentration by eq 6
of transferred water is obtained from the difference in the
absolute humidity between inlet and outlet of the spray column. Pi ¼ γi xi Pisat ð6Þ
The absolute humidity is calculated using the temperature and
relative humidity of the air. The saturated water vapor pressure where γ is an activity coefficient obtained from the UNIQUAC
can be obtained from eq 1. equation20 as shown in Table 2. Parameters of the UNIQUAC
equation are shown in Table 3.17 The water concentration of the
B outlet PEG solution is calculated using eq 7 because of difficulty
ln Pwsat ¼ A
ð1Þ
C þ T of measurement.
C1
where A, B, and C are constants of Antoine’s equation.19 A = ΔX þ qL
C2 ¼ 100  100 ð7Þ
23.1964, B = 3816.44, C =
46.13. The water vapor pressure of ΔX þ qL
air can be calculated using the relative humidity and saturated
water vapor pressure.
The vapor pressure difference between air and PEG solution is
expressed by the logarithmic mean vapor pressure difference.
Pw ¼ jPwsat ð2Þ
ðPw1
Pw1 Þ
ðPw2
Pw2 Þ
ΔPln ¼
 ð8Þ
Pw1
Pw1
Table 1. Experimental Conditions ln
Pw2
Pw2
base conditions variation range

nozzle diameter (mm) 1.0 1.0, 1.5

Table 3. Parameters of UNIQUAC Equation21
air temperature (°C) 22 Δu12
4.8
absolute humidity (g/kg-DA) 12.5 Δu21
1884.7
air flow rate (m3/min) 2.2 0.5
4.2 r1 44.6
PEG temperature (°C) 22 13
30 r2 7.8
water concentration (wt%) 3.0 0
13 q1 61.6
PEG flow rate (g/s) 24.2 12.3
34.1 q2 5.7

Table 2. UNIQUAC Equation20

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 Table 4. Experimental Data of This Study
run number 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27

nozzle diameter dn (mm) 1.0 1.0 1.0 1.0 1.0 1.0 1.0 1.5 1.5 1.5 1.0 1.0 1.0 1.0 1.0 1.0 1.0 1.0 1.0 1.0 1.0 1.0 1.0 1.0 1.0 1.0 1.0
length of cross section x (mm) 434 434 434 434 434 434 434 434 434 434 434 434 434 434 434 434 434 434 434 434 434 434 434 434 434 434 434
Industrial & Engineering Chemistry Research

inlet air flow rate Va (m3/min) 2.2 2.2 2.2 2.2 2.2 2.2 2.2 2.2 2.2 2.2 0.5 1.2 1.7 2.4 4.2 2.2 2.2 2.2 2.2 2.2 2.2 2.2 2.2 2.2 2.2 2.2 2.2
inlet air temperature Ta1 (°C) 23.3 21.3 21.8 21.3 21.9 21.7 22.2 223 22.8 223 21.4 22.3 22.2 22.2 23.1 22.4 22.8 23.2 22.4 21.7 21.9 21.9 22.9 22.8 22.2 22.2 22.0
inlet absolute humidity H1 (g/k-DA) 13.0 12.8 12.5 12.7 12.2 12.6 11.9 12.5 12.8 12.4 13.0 12.7 12.9 12.9 12.8 12.7 12.5 12.9 12.2 12.5 13.0 12.3 12.6 12.9 12.3 13.1 12.6
inlet air vapor pressure Pw1 (Pa) 2070 2037 1992 2018 1945 2003 1901 1990 2029 1973 2069 2018 2052 2046 2041 2023 1983 2051 1941 1995 2065 1955 2009 2051 1951 2088 1916
outlet air temperature Ta2 (°C) 23.0 21.4 21.8 21.5 22.1 23.1 20.3 21.8 22.6 23.3 19.1 22.0 21.8 22.6 23.9 21.9 24.2 22.9 21.9 22.4 22.5 21.5 22.9 19.9 21.5 24.3 26.5
outlet absolute humidity H2 (g/kg-DA) 11.5 10.5 10.4 9.7 9.8 9.0 8.2 12.1 10.8 9.6 8.2 8.9 9.6 10.1 11.3 9.8 9.1 10.4 9.8 10.4 11.1 10.5 11.7 9.5 9.2 11.1 11.1
outlet air vapor pressure Pw2 (Pa) 1825 1682 1663 1555 1559 1436 1316 1926 1727 1536 1314 1417 1529 1608 1797 1573 1453 1668 1573 1657 1774 1674 1869 1520 1465 1773 1769

13556
inlet PEG flow rate qL (g/s) 14.3 18.4 18.4 24.2 24.2 32.6 32.6 12.3 24.6 34.1 24.2 24.2 24.2 24.2 24.2 24.2 24.2 24.2 24.2 24.2 24.2 24.2 24.2 24.2 24.2 24.2 24.2
inlet PEG temperature TL1 (°C) 22.3 20.8 21.4 21.1 21.9 22.1 21.0 221 22.4 23.0 21.3 20.0 20.1 21.7 23.2 18.9 22.9 22.0 21.5 23.3 22.8 22.1 22.7 13 18 28 29
water concentration of inlet PEG solution Cw1 (wt%) 3.0 3.1 3.1 3.1 3.1 2.9 2.9 3.2 3.0 3.1 3.0 3.0 3.0 3.0 3.0 0.0 0.0 5.1 6.0 6.0 8.9 9.0 12.8 3.0 3.0 3.0 3.0
vapor pressure of outlet PEG solution Pw1 * (Pa) 497 448 467 460 495 480 429 510 499 537 459 408 409 474 538 0 0 762 835 979 1252 1193 1577 217 355 812 911
outlet PEG temperature TL2 (°C) 24.4 23.3 24.0 24.0 24.6 25.4 23.5 22.7 24.2 25.1 23.5 22.4 22.4 24.3 24.7 20.6 24.8 24.1 23.0 25.7 24.5 23.3 24.0 15.9 21.8 29.1 29.7
water concentration of outlet PEG solution Cw2 (wt%) 3.5 3.6 3.6 3.6 3.6 3.42 3.4 3.3 3.3 3.4 3.24 3.39 3.48 3.6 3.6 0.5 0.6 5.5 6.40 6.41 9.22 9.28 12.9 3.6 3.6 3.4 3.3
vapor pressure of outlet PEG solution Pw2 * (Pa) 679 640 669 681 706 725 614 558 639 711 589 554 569 685 718 80 132 968 998 1246 1472 1347 1751 327 554 1006 1020
humidity variation ΔH (g/kg-DA)
1.6
2.3
2.1
3.0
2.7
3.6
3.7
0.4
1.9
2.8
4.8
3.8
3.3
2.8
1.8
2.9
3.2
2.4
2.3
2.2
1.9
1.8
0.9
3.4
3.1
2.2
1.5
volumetric mass transfer coeficient coefficient kGa (mmol/(m3 3 Pa 3 s)) 0.37 0.56 0.54 0.79 0.75 1.08 1.14 0.09 0.47 0.80 0.33 0.53 0.63 0.80 0.84 0.52 0.63 0.81 0.92 1.03 1.15 1.11 1.17 0.72 0.81 0.71 0.55
ARTICLE

dx.doi.org/10.1021/ie200989k |Ind. Eng. Chem. Res. 2011, 50, 13554–13560

Industrial & Engineering Chemistry Research
Figure 2. Volumetric mass transfer coefficient.
The volumetric mass transfer coefficient is expressed by the
logarithmic mean vapor pressure difference and amount of
transferred water as in eq 9.
ΔX
kG a ¼ ð9Þ
ΔPln V
The volumetric mass transfer coefficient is thus calculated by
using relative humidity, temperature of air, liquid temperature,
and water concentration, which are obtained at the inlet and
outlet of the spray column.
4. RESULTS AND DISCUSSIONS
The condition and resulting humidity change and volumetric
mass transfer coefficients are shown in Table 4.
As shown in Figure 2a, kGa increases with liquid flow rate.
According to Kuntz and Aroonwilas,1 increase in liquid flow rate
leads to reduction in droplet size, thus droplet specific surface
area increases. In addition, the number of droplets produced by
the nozzle also increases with the liquid flow rate. In this way, the
surface area available for mass transfer is increased. The same
trend is shown in the research of Javed et al.4
As shown in Figure 2b, kGa increases initially with an air flow rate
up to the value of 2.2 m3/min beyond which the kGa becomes
independent of the air flow rate. As for the low air flow rate, the
higher air flow rate should result in a thinner boundary layer on the
droplet, which should lead to higher values of kGa. As for the air flow
rate above 2.2 m3/min, the short contact time for the high air flow
rate may be the reason for this behavior, since the more the amount
of water transferred decreases the shorter the contact time.
As shown in Figure 2c, kGa increases with increasing water
concentration. It is known that the density and viscosity of the
13557
ARTICLE
Table 5. Comparison of the Parameters
parameter eq 11 eq 13 .
a 1.3  103 1.4  103 2.0  10
5
b 1.27 8.90 1.74
c 0.33 0.33 0.33
d 0.40
0.40
e 0.90 8.41 1.05
f
1.21 2.31
g
2.74
15.42
h
3.3
i
0.51
PEG solution decreases with increasing water concentration. The
range of variation in the PEG solution’s viscosity is 68
42 mPa 3 s
and that of the density is 1123
1117 m3/kg. This results in a
narrower spray angle. Subsequently, the surface area available for
mass transfer decreases.
As shown in Figure 2d, variation of the inlet liquid temperature
does not have a large effect on kGa. The range of variation in the
PEG solution’s viscosity is 87
39 mPa 3 s and that of the density is
1127
1115 m3/kg in this range of the inlet liquid temperature.
The effect of the inlet liquid temperature on the physical properties
of the liquid is large for the range studied here. Thus, the liquid
temperature should affect the value of kGa. However, we have to
note that the liquid desiccant is cooled or heated by air when the
liquid is sprayed. This change in temperature results in a change in
the driving force of mass transfer, and thus may cancel the expected
effect of viscosity and density, so that the variation in the inlet
liquid temperature does not have a large effect on kGa.
In this study two nozzles with different orifice diameters are
employed. As shown in Figure 2a, kGa decreases with an increase
in the orifice diameter of the nozzle. A small orifice diameter
increases the amount of small liquid droplets and thus leads to an
increase in the effective contact area available for absorption.
5. CORRELATION OF THE VOLUMETRIC MASS TRANS-
FER COEFFICIENT
The volumetric mass transfer coefficient obtained from eq 9 is
correlated using dimensional analysis. The volumetric mass
transfer coefficient is affected by the molecular weight of
transferred components, the diffusivity of water vapor in air, air
and liquid flow rates, and the physical properties of gas and liquid
phases. Two correlations are suggested in this study. As the first
correlation, the functional form of the volumetric mass transfer
coefficient of the gas film can be presented as eq 10.
ky a ¼ f ðM, dc , dn , DG , L, G, μG , μL , FG , FL Þ ð10Þ
Here, a gas-phase mass transfer coefficient ky, which is the mass
transfer coefficient with the driving force expressed in molar fraction,
is introduced to enable direct comparison with Chung and Wu.14
Please note that kG is the mass transfer coefficient with the driving
force expressed in vapor pressure. The above variables are arranged
into dimensionless groups by using the Buckingham Pi theory. The
resulting equation for the mass transfer coefficient including physical
properties of the liquid and the nozzle diameter is given in eq 11.
!g

e
f
ky aMdc 2 d L dn FL
¼ aReG ScG ReL
b c
ð11Þ
D G FG G dc FG
dx.doi.org/10.1021/ie200989k |Ind. Eng. Chem. Res. 2011, 50, 13554–13560
Industrial & Engineering Chemistry Research ARTICLE

Table 6. Range of Dimensionless Numbers for Correlations

eq 11 eq 13 Chung and Wu (2000)

min max min max min max

ReG 4.92  10 3
3.90  10 4
4.92  10 3
3.90  10 4
1.17  10 4
2.30  104

1
1
1
1
1
ScG 6.00  10 6.07  10 6.00  10 6.07  10 5.78  10 6.08  10
1
ReL 1.90 5.49 1.90 5.49
L/G 2.77  10
1 2.2 2.77  10
1 2.28 7.77  10
1 1.71

3
2
3
2
dn/dc 6.67  10 1.00  10 6.67  10 1.00  10
FL/FG 9.32  102 9.45  102 9.32  102 9.45  102

5
L dn/FLσL
2
1.14  10 9.64  10
5
Pd/Ptotal 1.34  10
1 5.11  10
1

Figure 3. Comparison between experimental and predicted data.

Figure 4. Comparison between Chung and Wu’s experimental data and predicted data.

As the second correlation, an equation including the surface tension The gas-phase mass transfer coefficient ky is related to kG as shown
of the liquid is suggested. The functional form of the volumetric in eq 14.
mass transfer coefficient can be presented as in eq 12
kG aPtotal ¼ ky a ð14Þ
ky a ¼ f ðM, dc , dn , DG , L, G, μG , μL , FG , FL , σL Þ ð12Þ
The constants a, b, d, e, f, g, and h are determined by regression of the
The above variables are arranged into dimensionless groups, again experimental results. Note that due to the narrow range of the
using the Buckingham Pi theory. The resulting equation is given in Schmidt number in this study, we set the value of c to be 0.33, which
eq 13. is the value determined by Chung and Wu.14 The values of

e
f !g !g the parameters obtained from this study are shown in Table 5.
ky aMdc 2 d L dn FL L 2 dn The values of viscosity needed for the parameter determination
¼ aReG ScG ReL
b c
DG F G G dc FG σ L FL are measured using a rotary viscometer, whose error is less than 1%.
The values of surface tension were obtained by taking the average of
ð13Þ the values of water and PEG. In this table, the obtained parameters
13558 dx.doi.org/10.1021/ie200989k |Ind. Eng. Chem. Res. 2011, 50, 13554–13560
Industrial & Engineering Chemistry Research ARTICLE

are compared with Chung and Wu’s correlation14 expressed by ’ AUTHOR INFORMATION
eq 15.
Corresponding Author

e
 *Fax: +81-82-422-7193. E-mail: mat@hiroshima-u.ac.jp.
ky aMdc 2 c L Pd i
¼ aReG ScG
b
ð15Þ
DG F G G Ptotal
’ NOMENCLATURE
The ranges of the dimensionless numbers for the correlations are A = Antoine’s constant in eq 1
shown in Table 6. The curves in Figure 2 are the predictions B = Antoine’s constant in eq 1 (K)
calculated using eq 11, eq 13, and Chung and Wu’s correlation. A C = Antoine’s constant in eq 1 (K)
comparison between experimental and predicted data is shown in C = water concentration of PEG in eq 7 (mol/kg)
Figure 3. The predicted values from eq 11 agree well with experi- dc = column diameter (m)
mental data with an average error of 18.9%, and those in eq 13 agree dn = nozzle diameter (m)
better with an average error of 10.4%. Equation 13 agrees better with DG = diffusion coefficient (m2/s)
experimental data because of the inclusion of surface tension. The G = superficial air mass velocity (kg/(m2 3 s))
predicted values using Chung and Wu’s correlation are also shown in H = absolute humidity of air (kg/kg-DA)
Figure 3. Chung and Wu’s correlation is unable to predict the kGa = volumetric mass transfer coefficient (mol/(m3 3 Pa 3 s))
experimental data of this study. A prediction of the Chung and Wu’s kya = volumetric mass transfer coefficient (mol/(m3 3 s))
experimental data was also made, as shown in Figure 4. The li = pure component bulk factor (
)
predicted values from eq 11 agree well with Chung and Wu’s L = superficial liquid mass velocity (kg/(m2 3 s))
experimental data and the average error is 18.1%, but agreement M = molecular weight of water (kg/mol)
between those and the prediction from eq 13 is not so good with an P = vapor pressure (Pa)
error of 27.8%. The average error obtained from Chung and Wu’s Patm = atmospheric pressure (Pa)
correlation is about 8%. Although the correlation obtained in this Psat
i = saturation pressure of pure component i (
)
study does not predict Chung and Wu’s data as well as their Psat
w = saturated vapor pressure of water (Pa)
correlation, eq 11 can express both our data and Chung and Wu’s Ptotal = total pressure (Pa)
experimental data within an error of 20%. In addition, eq 11 can Pw* = vapor pressure of PEG solution (Pa)
predict a wider range for the gas-phase volumetric mass transfer ΔPln = logarithmic mean vapor pressure (Pa)
coefficient in the range of 0.01
0.12 kmol/(m3 3 s). Thus, inclusion qL = liquid flow rate (kg/s)
of the nozzle diameter and liquid property improves the correlation. qi = molecular surface area parameter for component i (
)
Especially, eq 11 developed in this study can be applied to the ri = molecular volume parameter for component i (
)
prediction of the mass transfer coefficient for the spray column for a ReG = Reynolds number (
)
wider range of parameters. However, since the mass transfer coeffi- ScG = Schmidt number (
)
cient in spray columns strongly depends on the spray properties such T = temperature (K)
as the liquid distribution, the droplets size distribution and the mean Δuij = effective UNIQUAC binary interaction parameter (
)
size of droplets, it is to be noted that strictly speaking, the correlations V = reactor volume (m3)
developed in this study are applicable to the type of nozzle used here. Va = air flow rate through the column (m3/s)
x = mol fraction (
)
6. CONCLUSION xi = liquid-phase mole fraction of component i (
)
ΔX = amount of transferred water (mol/s)
The mass transfer characteristics of the spray column were γi = activity coefficient of component i
investigated experimentally. In this investigation, high humidity θi = area fraction of component i (
)
air was used as a gas and PEG was employed as a liquid desiccant. μ = viscosity (Pa 3 s)
The mass transfer correlation was developed by dimensional F = density (kg/m3)
analysis. The correlation obtained from this study was compared τij = effective UNIQUAC binary parameter related to Δuij (
)
with Chung and Wu’s correlation. The predicted values of the j = relative humidity (
)
volumetric mass transfer coefficient from eq 11 ji = fugacity coefficient of component i (
)

0:90

1:21 !
2:74
ky aMdc 2 L dn FL Subscripts
¼ 1:3  103 ReG 1:27 ScG 0:33 ReL 0:40
DG FG G dc FG a = air
d = desiccant solution
were in good agreement with the experimental results, and the G = gas
average error was 18.1%. By including the surface tension as in eq 13, L = liquid
w = water
ky aMdc 2 1 = inlet
¼ 1:4
DG FG 2 = outlet

8:41
2:31 !
15:42 !
3:3

0:40 L dn FL L2 dn
10 ReG
3 8:90
ScG 0:33
ReL
G dc FG σ L FL ’ REFERENCES
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