2nd Conference on Chemical Engineering and Advanced Materials (CEAM)

VIRTUAL FORUM
November 15th - 26th, 2010

Kinetics Study of Carbon Dioxide Absorption into Aqueous Potassium

Carbonate Promoted with Boric Acid
L. Pudjiastuti1, E.A.Saputra2, A.Altway3, Susianto4, Kuswandi5
Abstract Many commercial processes for removal of carbon dioxide from acid gases have used
aqueous potassium carbonate promoted with amines. This paper presents kinetic data and
absorption rate for aqueous potassium carbonate promoted with boric acid. Kinetics of the
absorption of CO2 into 30 wt% potassium carbonate promoted with boric acid were investigated
at 30, 40, 50oC by using a wetted-wall column apparatus. The addition of 0.162 0.485 mol.l-1
boric acid to 30 wt% potassium carbonate system results in a significant enhancement of CO2
absorption rates. Based on pseudo-first order for CO2 absorption, pseudo-first order reaction rate
constants were determined from the measured kinetics data. The reaction rate constants for boric
9.23.107 1.42.107 [ KBO2 ]
acid promoted absorption are k2 = 1.00.1020 exp
and

RT

2 . 397
1 . 2729
20
with average deviation 12,11% and 1,35%
k 2 KBO = 6 .2325 .10 exp
[ KBO 2 ]
2

RT

respectively. Copyright 2010 Praise Worthy Prize S.r.l. - All rights reserved.

Keywords: Absorption, CO2 Removal, Kinetics, Promoter, Boric Acid

Nomenclature
d
DCO2
g
h
k1
k1boric cid
k1
k2
k2,boric acid
k2,boric acid
kg
Q
q
r
R
Re
Sc
Sh
t

Diameter of Wetted Wall Column, m

Diffusivity of dissolved CO2, m2/s
Gravitational acceleration, m/s2
Height of Wetted Wall Coulumn, m
Rate constant of overall reaction, 1/s
Rate constant of overall reaction with
boric acid, 1/s
Second-order rate constant of reaction,
m3 / kmol.s
Second-order rate constant of reaction
with promotor, m3 / kmol.s
Second-order rate constant of reaction
with boric acid, m3 / kmol.s
k2,boric acid x [ KBO2] ,1/s.
Gas phase mass transfer coeficient,
kmol/ m2 .s
Quantity of gas absorbed by unit area in
time of contact t, kmol/m2

absorption rate (kmol/s)

Rate of reaction, kmol/(m3.s)

Gas constant, m3.Pa/kmol.K
Reynold Number.
Schmidt Number.
Sherwood Number.
contact time, s

T
u
us
v
V

Temperature, (K)
Distribution of velocity in film, m/s
Velocity in film surface , m/s.
Liquid flow rate, m3/s.
Volume of liquid, m3
Thickness of liquid film, m
Viscosity of liquid, kg /m.s
Density of liquid, kg/m3

I.

Introduction

Removal of acid gases, e.g. carbon dioxide (CO2), by

using reactive absorption with aqueous alkonalamine or
potassium carbonate solution is an important industrial
operation. The advantage of using alkanolamine solvent
is its high reaction rate with carbon dioxide. Several
investigators have explored the reaction rate of carbon
dioxide is un-promoted, promoted and blended aqueous
amines solution ([1] [7]). A problem with the use of
alkanolamines for carbon dioxide removal is that they
degrade as a result of long exposure or repeated use.
Several attempts have been made to use alternative more
stable solvent having high enough reaction rate with
carbon dioxide for example amino acid salts [8]. The
absorption of CO2 with potassium carbonate solvent has
gained widespread and has been accepted for removal of
CO2 from the natural and synthetic gas stream due to its
stability, low cost and low energy requirement for

Copyright 2010 Praise Worthy Prize S.r.l. - All rights reserved

L. Pudjiastuti, E.A.Saputra, A.Altway, Susianto, Kuswandi

solvent regeneration.
However, the reaction rate
between carbon dioxide with potassium carbonate is
lower than the reaction rate with amines solution ([9],
[10])
Several researchers have shown that the application of
piperazine/amines-promoted potassium carbonate could
accelerate the absorption process ([11] [15]). However,
many promoters are carcinogenic in nature and some
others are not stable at stripper conditions. In this case,
boric acid is environmental friendly.
There is some information available regarding the
absorption of carbon dioxide using aqueous solution of
potassium carbonate promoted with boric acid [16]. But
none of the literature discussed the detailed kinetics of
the reaction of carbon dioxide in the liquid phase for
boric acid promoted potassium carbonate solvent system.
The detailed kinetics of the reaction is essential for the
process design and simulation of CO2 absorption in boric
acid promoted potassium carbonate solvent.
This work focuses on expanding the investigation of
promoted potassium carbonate (K2CO3) by using boric
acid. The main purpose of this work is to investigate the
effect of boric acid on the reaction rate constant of CO2
absorption into aqueous potassium carbonate solution by
using a laboratory wetted wall column. Experimental
kinetic data were collected. A simplified model used to
interpret the results.

II.
II.1.

Theory
Reaction system

The absorption of CO2 into aqueous K2CO3 is

commonly represented by overall reaction
CO3 + H 2 O + CO2 ( aq ) 2 HCO3

The rate equation for the reaction of carbon dioxide

with unpromoted hot potassium carbonate is ([3], [12])

rOH = kOH OH [CO2 ] [CO2 ]e

(5)

The carbonate-bicarbonate system is buffer solution;

hence the concentration of OH- ion in the solution near
the surface of the liquid is not significantly affected by
the absorption of CO2. In this case, carbon dioxide
undergoes a pseudo-first-order reaction and Eq. (4a) can
be rewritten as ([3], [13])
rOH = k1 ( [CO2 ] [CO2 ] )e

(6)

When H3BO3 is added to the carbonate-bicarbonate

solution, the absorption process occurs via several
mechanisms. A convenient procedure for adding
potassium borate to the potassium carbonate scrubbing
solution is by adding boric acid, whereupon the boric
acid is converted to potassium borate in accordance with
the following reaction [10]:
2H3 BO3 + K2CO3 2KBO2 + CO2 + 3H2O

(7)

In this event, the potassium carbonate content of the

solution must be properly adjusted to compensate for that
consumed by reaction with the added boric acid.
The main role played by buffer solution, when KBO2
is present, is that of creating a medium in which the salt
can dissociate and then the catalytic activity may be
exploited. The rate equation for the catalyzed reaction,
which is always first-order with respect to carbon
dioxide, can be written in the following way [2]:

(1)

rpromoter = k promoter [CO2 ]

(8)

The reaction is usually described in term of two

parallel, reversible reactions.
CO2 ( aq ) + OH HCO3
(2)

rpromoter = k KBO2 BO2

(9)

HCO3 + OH CO32 + H 2O

Using the same approach for deriving Eq (5), gives

the following pseudo-first-order rate equation of carbon
dioxide with activated potassium in liquid phase:

(3)

Since the reaction with hydroxide is the rate-limiting

step, the forward reaction rate is represented as a second
order rate expression.
rCO2 = kOH OH [CO2 ]

(4)

This reaction, though important to the solution

equilibrium, is generally much slower than aqueous
amines, limiting its application in processes requiring a
high percentage of removal. It is often advantageous to
add a promoter to increase the absorption rate. The
energy required to reverse the reaction is typically less
than that required for amine solvents.

Copyright 2010 Praise Worthy Prize S.r.l. - All rights reserved

r = k KBO2 [ KBO2 ]

) ([CO2 ] [CO2 ]e )

(10)

Eqs.(5) and (10) lead to overall pseudo-first-order rate

equation of carbon dioxide with activated potassium
carbonate in liquid phase:
r=

(k

KBO2

OH + k KBO [ KBO2 ]
2

) ([CO ] [CO ] )
2

r = k1 ' [CO2 ] [CO2 ]e

(11)

2 e

(12)

2nd Conference on Chemical Engineering and Advanced Materials (CEAM)

L. Pudjiastuti, E.A.Saputra, A.Altway, Susianto, Kuswandi

where k is the overall apparent first-order rate constant

and is defined as [12],

k1 ' = kOH OH + k KBO2 BO2

(13)

II.3.

The gas film mass transfer coefficient, kg, in the

wetted-wall column was determined as in [13] using SO2
absorption into 0.1 M NaOH. The results of the
experiments are correlated as in equation (22)

The rate constant has been measured by [3]

log kOH

2895
= 13, 635
0 , 08 I
T

II.2.

sh = 1, 075 Re Sc
h

(14)

Wetted Wall column is equipment commonly used to

study the kinetics of gas-liquid reaction. The liquid flow
in the wetted wall column is usually maintained in
laminar pattern. In this case the gas-liquid contact time is
determined as follows,
h
us

(15)

Re =

g 2
2

3 Qsol
gW

(17)

(18)

(19)

where:
C Ai =

kG PA + DA k1 C Ae
kG He + DA k1

C Ae =

K 2 [HCO3- ]2
K1[CO 22 ]

(23)

Sc =

DCO2

(24)

The gas film transfer coefficient can be found from

the following definition of the Sherwood number
(25)

III. Experimental Procedure

The absorption rate q is usually measured

experimentally. Then, equation (19) can be used to
determine the value of pseudo first-order reaction rate
constant of reversible reaction using the experimental
absorption rate data:
Q = ( CAi CAe ) t DA k1

(16)

If Q( t ) is amount of gas absorbed by unit area of

surface during a contact-time t, the total rate of
absorption q into the film is related to Q( t ) by
Q(t)
q
=
t
dh

ud

Sh = RTk g h / DCO2

and is the film thickness given by

=3

(22)

The Schmid number is:

where us is the liquid surface velocity given by

us =

0 ,85

The Reynolds number is defined as:

Wetted Wall Column

t =

Gas film mass transfer coefficient

(20)

(21)

Copyright 2010 Praise Worthy Prize S.r.l. - All rights reserved

The wetted-wall column, depicted in Fig.1 and 2, was

used as the gas-liquid contactor throughout the kinetic
data and absorption rate measurement. The contactor is
the same equipment as used in the work of [5],[8], and
[14]. The stainless steel, 9.3-cm in height and 1.3 cm in
outside diameter, is a tube extending from the liquid feed
line into the column. The liquid is pumped through the
inside of the tube, overflows, and is evenly distributed
across the outer surface of the tube. Gas enters near the
base of the column, counter-currently contacting the
fluid as it flows up to the gas outlet. The liquid flow rate
was varied in the range 5-10 cm3/s. The gas flow rate is
100 cm3/s . The CO2 absorption rate was measured from
the difference in inlet and outlet CO2 composition in the
gas as determined using by Orsat apparatus.

IV.

Results and Discussion

IV.1. Absorption Rates

The absorption experiments for CO2 into potassium

carbonate solution (30 mass % K2CO3) with the addition
of boric acid were carried out over the concentration
range 0.162 0.485 mol.l-1. The experiments were
carried out over the temperature range of 303 to 323 K.
All experiments were performed under atmospheric
pressure with partial pressure of CO2 near atmospheric
pressure.

2nd Conference on Chemical Engineering and Advanced Materials (CEAM)

L. Pudjiastuti, E.A.Saputra, A.Altway, Susianto, Kuswandi

C
P1
P2
R1
R2
T1
T2
T3
T4
T5
t
V1
V2
V3
WWC

: Heater
: Promoted K2CO3
pump.
: Water pump.
: Liquid rotameter.
: Gas rotameter.
: Waterbath
: Promoted K2CO3
tank.
: Overflow tank.
: CO2 tank
: Sample tank.
:Thermocouple
: Liquid Valve
: CO2Valve
:Valve ( by pass )
:Wetted wall
column.

v x 106
m3/s
5
6.667
8.333
10

TABLE I
EXPERIMENTAL RESULT OF ABSORPTION RATE
q x 108
t
T
kmol/s
s
K
Sol-1
Sol-2
Sol-3
0.817
2.001
3.982
5.211
0.675
4.965
5.944
7.548
303
0.581
5.944
10.765
12.188
0.515
9.810
14.537
16.536

5
6.667
8.333
10

0.817
0.675
0.581
0.515

5
6.667
8.333
10

0.817
0.675
0.581
0.515

313

323

2.994
5.944
8.850
11.715

4.965
6.918
11.715
14.537

5.944
7.886
12.660
16.536

3.982
7.886
10.765
12.660

4.965
9.810
12.660
15.469

6.918
9.810
13.601
17.320

Fig. 1. Experimental Apparatus

Fig. 3. CO2 absorption rate in various solutions at temperature 303K

Fig. 2. Wetted Wall Column

Table I are the rate of CO2 absorption as measured in

the wetted wall column, where solution 1(Sol-1) is the
addition of boric acid 1wt% into 30wt% K2CO3; solution
2(Sol-2) is the addition of boric acid 2 wt% into 30wt%
K2CO3 and solution 3(Sol-3) is the addition of boric acid
3 wt% into 30wt% K2CO3.
The CO2 absorption rate in various solutions is plotted
in Fig 3, 4, and 5.
Increasing the boric acid
concentration from 1wt% to 3 wt% affects the CO2
absorption rate enhancement by a factor of 1.63. CO2
absorption rate increase by factor of 3.99 with increasing
volumetric rate from 5 m3/s to 10 m3/s .
The effect of temperature on rate of CO2 absorption is
shown in figures 6, 7 and 8. It can be seen from that
figures, that the average CO2 absorption rate increase by
factor of 1.384 as temperature increases from 303K to
323K .

Fig. 4. CO2 absorption rate in various solution at temperature 313K

Fig. 5. CO2 absorption rate in various solutions at temperature 323K

Copyright 2010 Praise Worthy Prize S.r.l. - All rights reserved

2nd Conference on Chemical Engineering and Advanced Materials (CEAM)

L. Pudjiastuti, E.A.Saputra, A.Altway, Susianto, Kuswandi

CO3= + H 2 O HCO3 + OH

(29)

Both reactions (26) and (28) are slow and rate

determining [13]. Reaction rate constant (k1) for the
equation (26) is shown in Table II.
TABLE II
REACTION RATE CONSTANT OF EQUATION (26)
Temperature, K
k1(m3/kmol.s)
Reff
303
12170
313
24560
[9]
323
36950

Reaction rate constant for CO2 absorption into boric

acid promoted K2CO3 solution was determined
experimentally in this work, and is shown in Table III
and IV.

Fig. 6. CO2 absorption rate in Sol-1 in various temperature

TABLE III
EXPERIMENT RESULT OF REACTION RATE CONSTANT IN EQUATION
(28)
k2. 10-4 ( m3/kmol.s )

Solution
303 K

313 K

323 K

Sol-1

3.006

10.851

33.708

Sol-2

9.212

20.933

63.026

Sol-3

18.658

40.081

161.599

Table III shows the reaction rate constant for

equation (28) as measured in the wetted wall column.

Fig. 7. CO2 absorption rate in Sol-2 in various temperature

TABLE IV
EXPERIMENTAL RESULT OF REACTION RATE CONSTANT
k1' . 10-4 ( 1/s )

Solution

Fig. 8. CO2 absorption rate in sol-3 in various temperatures

IV.2. Kinetics of CO2 Reaction with Potassium

Carbonate and Boric Acid
CO2 react with aqueous solution of potassium
carbonate as follow:
HCO3

(26)

CO3= + H + HCO3

(27)

CO2 + H2O H + + HCO3

(28)

CO2 + OH

Copyright 2010 Praise Worthy Prize S.r.l. - All rights reserved

k2' . 10-4 ( 1/s )

303 K

313 K

323 K

303 K

313 K

323 K

Sol-1

0.488

1.761

5.464

0.486

1.755

5.452

Sol-2

2.981

6.775

20.397

2.980

6.771

20.387

Sol-3

9.054

19.451

78.416

9.053

19.447

78.408

Reaction rate constant (k2) is affected by temperature

and concentration of boric acid. Addition of boric acid
with concentration in the range 1wt% to 3 wt% into 30%
potassium carbonate solution and temperature range
from 303 K to 323 K, increases reaction rate constant
significantly.
The reaction rate constant (k2) for various solution are
plotted in Fig. 9 and are fitted by the following equation
(model-1)

( 9.23.107 1.42.107 [ KBO2 ]

k2 = 1.00.1020 exp
(30)

RT

Equation (30) indicates that addition of boric acid in

range 1-3 wt%, decreases the activation energy, and so
increases k2.

2nd Conference on Chemical Engineering and Advanced Materials (CEAM)

L. Pudjiastuti, E.A.Saputra, A.Altway, Susianto, Kuswandi

Average Relative Deviation (ARD) of k2 from

equation (30) and experimental data is shown in Table V.

K2CO3+ KBO3 + H2O systems. This kinetic model is

better than the first model.

Fig. 9. Reaction rate constant in various temperature

From Table V, average deviation (ARD) of the

second-order rate constant of reaction with promotor is
lower than 15%. This reaction rate model is found to be
satisfactory in representing the CO2 absorption into
K2CO3+ KBO3 + H2O systems
The reaction rate constant (k2KBO2) for various
solution are plotted in Fig.10 and are fitted by the
following Arrhenius equation (model-2):

Fig. 10. Reaction rate constant in various temperature

2.397
1.2729
k '2 KBO2 = 6.2325.1020 exp
(31)
[ KBO2 ]
RT

TABLE V
AVERAGE DEVIATION OF EQUATION (30)
k2 * 10-5
eksperiment
k2 (Eq 30 )
[KBO2]

(K)

(kmol/m3)

303

deviation

(m3/kmol.s)

(m3/kmol.s)

0.16173

0.3007

3.077.E+04

2%

313

0.16173

1.085

9.631.E+04

11%

323

0.16173

3.371

2.809.E+05

17%

303

0.32347

92.12

7.646.E+04

17%

313

0.32347

2.093

2.325.E+05

11%

323

0.32347

6.303

6.599.E+05

5%

303

0.48520

1.866

1.900.E+05

2%

313

0.48520

4.008

5.612.E+05

40%

1.550.E+06

4%

323

0.48520

161.6

ARD =

Fig. 11. Comparison of overall reaction rate constant (k1boric acid).

12.11%

Average Relative Deviation (ARD) of k2 from

equation (31) and experiment is shown in Table VI.
From Table VI, average deviation (ARD) of the
pseudo first-order rate constant of reaction with
promotor is 1.35%. This reaction rate model is found to
be satisfactory in representing the CO2 absorption into

Copyright 2010 Praise Worthy Prize S.r.l. - All rights reserved

The kinetic model in Eqs.(31) were compared with

the available literature data: for MDEA blended with
DEA [3]; K2CO3+ PZ [13]; MEA [3]; PZ and MDEA
[5]. Fig. 11 show the comparison of the overall reaction
rate constant ( k1KBO2) from this work with the available
literature values.
As shown in Fig. 11, the calculated value of k1KBO2
from this work appear to be comparable with most
available literature data.

2nd Conference on Chemical Engineering and Advanced Materials (CEAM)

L. Pudjiastuti, E.A.Saputra, A.Altway, Susianto, Kuswandi

[3]

TABLE VI
AVERAGE DEVIATION OF EQUATION (31)
T

[KBO2]

k2 experiment

k2 (eq. 31)

(K)

(kmol/m3)

(1/.s)

(1/s)

303

0.16173

30065.0643

30766.2532

0.26%

313

0.16173

108520.3163

96308.2032

1.25%

323

0.16173

337103.1421

280908.8011

1.85%

303

0.32347

92121.5208

76461.5334

1.89%

313

0.32347

209325.5231

232487.7614

1.23%

323

0.32347

630265.2363

659861.4003

0.52%

303

0.48520

186575.5100

190025.2866

0.21%

313

0.48520

400807.0510

561224.8736

4.45%

323

0.48520

1615986.9518

1550029.9950

0.45%

deviation

[4]
[5]

[6]
[7]

[8]

1.35%
[9]

V.

Conclusion

Kinetics of the absorption of CO2 into potassium

carbonate solution (30 wt % K2CO3) with the addition of
boric acid was investigated at 303,313, and 323 K using
a laboratory wetted wall column. Three system of which
30 wt % K2CO3 with 1,2 and 3 wt% boric acid were
studied. The addition of 1,2, and 3 wt% boric acid to 30
wt% potassium carbonate system results in a significant
enhancement of CO2 absorption rates. Two kinetic
models were proposed in this work. The first model,
based on second-order reaction rate constant
measurement, give the average deviation (ARD) of
12.11%. While the second model, based on pseudo firstorder reaction rate constant measurement, gives the
average deviation (ARD) of 1.35%. The latter kinetic
model is found to be more satisfactory in representing
the CO2 absorption into K2CO3+ KBO3 + H2O systems.

Acknowledgements
The authors wish to acknowledge the financial
support of:
- Guru Besar research grant administered by the
Department of Research and Social Services, Institute
Technology of Sepuluh Nopember, Surabaya , Indonesia.
- Research Grant Program for Doctoral Students by
Directorate of Higher Education, The Ministry of
National Education of Indonesia.

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Copyright 2010 Praise Worthy Prize S.r.l. - All rights reserved

[10]
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Authors Information
First Authors name: Lily Pudjiastuti
Place and date of birth:
Banjarmasin,
Indonesia, July 03th 1958.
Educational background: Bachelor s degree
in Chemical Engineering from Institut Teknologi
Sepuluh Nopember (ITS) Surabaya, Indonesia in
1983; Masters degree in Chemical Engineering
from Institut Teknologi Sepuluh Nopember
(ITS) Surabaya, Indonesia in 2002.
Second Authors name: Erwan Adi Saputra,
Place and date of birth: Surabaya, Indonesia,
August 03th 1980.
Educational background:
Bachelors degree in Chemical Engineering,
from
Institut
Teknologi
Sepuluh
Nopember,Surabaya, Indonesia in 2002.

2nd Conference on Chemical Engineering and Advanced Materials (CEAM)

L. Pudjiastuti, E.A.Saputra, A.Altway, Susianto, Kuswandi

Third Authors name: Ali Altway

Place and date of birth: Jakarta, Indonesia.
August 4, 1951
Educational background:
Masters degree in Chemical Engineering from
the University of Wisconsin , Madison, WI,
USA in 1979; Doctorate in Chemical
Engineering from Sepuluh Nopember Institute of
Technology, Surabaya, Indonesia in 2004. Dr. Altways major field of
study is transport phenomena.
Dr. Altway has authored several articles: 1. "Effect of Particle size on
simulation of three-dimensional solid dispersion in stirred tank",
TransIchemE., Vol. 79, No. A8, pp. 1011-1016 (2001); 2. Mass
Transfer and Chemical Reaction Aspects Concerning Acetaldehyde
Oxidation in Agitated Reactor, Studies in Surface Science and
Catalysis, Vol. 159 (2006); 3. Numerical Analysis of Macro-Instability
Characteristic in a Stirred Tank by Means of Large Eddy Simulations:
Off-Bottom Clearance Effect ,Chemical Product and Process Modeling,
Vol.3, Iss.1, Article 45 (2008); and 4. Effects of Feed Rate and
Residence Time on Environment of Rotary Dryer Processes in Applied
Science in Environment Sanitation, vol.4, No.1, January-April 2009.

Fifth Authors name: Kuswandi

Place and date of birth: Sumenep, Indonesia,
June 12, 1958.
Educational background:
Masters degree in Chemical Engineering from
the Universite de Technologie de Compiegne
(UTC), Compiegne, France in 1996. Doctorate
in Chemical Engineering from the Universite de
Technologie de Compiegne (UTC), Compiegne, France in 2000. Dr.
Kuswandis major field of study is thermodynamics.
Dr. Kuswandi has authored several articles: 1. "Dtermination
Exprimentale des Equilibres Liquide-Vapeur de Binaires Htroazotropiques", Entropie, No. 215, 1998; 2. "Separation of
Hydrocarbon by Liquid Surfactant Membranes, Rcent Progrs en
Gnie des Procds, No.68, Vol.13, 1999; and 3. "Effects of Feed Rate
and Residence Time on Environment of Rotary Dryer Processes"
Applied Science in Environment Sanitation, vol.4, No.1, January-April
2009.

Fourth Authors name: Susianto

Place and date of birth: Tegal, Indonesia.
August 20, 1962
Educational background:
Masters degree in Chemical Engineering from
the Institut National Polytechnique de Lorraine
(INPL), Nancy, France in 1996. Doctorate in
Chemical Enginnering from the Institut National
Polytechnique de Lorraine (INPL), Nancy,France in 2001. Dr.
Susiantos major field of study is reaction engineering.
Dr. Susianto has authored one article: Effects of Feed Rate and
Residence Time on Environment of Rotary Dryer Processes in Applied
Science in Environment Sanitation, vol.4, No.1, January-April 2009.

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2nd Conference on Chemical Engineering and Advanced Materials (CEAM)