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Design and Control of Acetaldehyde Production Process

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 Trends in Chemical Engineering
Volume 1, Issue 1

www.stmjournals.com

Design and Control of Acetaldehyde Production Process

K. Nagamalleswara Rao1, M. Venkata Ratnam1, P. Rajendra Prasad2, V. Sujatha2
1
Department of Chemical Engineering, Bapatla Engineering College (Autonomous),
Andhra Pradesh, India
2
Department of Chemical Engineering, AU College of Engineering, Andhra University, Vizag, India

Abstract
This paper discusses the steady state and dynamic simulations of acetaldehyde
production process by using Aspen Plus and Aspen Dynamics. The model developed in
the present study is the modification of the process developed by Eastman Chemical
Company of U.S. Patent 6,121,498. The proposed design consists of a FEHE (feed
effluent heat exchanger), reactor, absorption column, compressors and two distillation
columns. Acetic acid reacts with hydrogen and gives acetaldehyde as main product and
ethanol, ethyl acetate, acetone, and water as byproducts. The paper is divided into two
stages. In the first stage, the entire process plant is developed for steady-state simulations
and in the second stage, dynamic simulations are performed by providing decentralized
controllers for the entire plant. Tray temperature control loop and composition control
loop are designed to maintain final product purity. Results of dynamic simulation are
analyzed for different process conditions. The proposed plant with control structure
performs very well in rejecting various disturbances while maintaining the acetaldehyde
product purity at 95.17 mol%, with a settling time of less than 9 h.

Keywords: Apen Plus, Aspen Dynamics, temperature control loop,

U.S. Patent 6,121,498

*Author for Correspondence E-mail: kanidarapunag2001@gmail.com

INTRODUCTION Plant-wide control system design is useful for

Many efforts are being made to expand the
manufacture of chemical products in such a
way as to minimize pollution. The conceptual
design of such production plants involves
interplay between design and operational
requirements, which attempts to balance non-
commensurable objectives such as economics,
safety health, and environmental impact
[1–20].
Dynamic simulation and modeling have
become mandatory parameters for process and
control engineers; therefore, dynamic
simulation software is being used constantly
for the assessment of control and optimization
of technologies. Aspen Dynamics and Aspen
Custom Modeler enable commercial
simulation software users to perform quick and
reliable dynamic model bifurcation analysis,
without resorting to non-chemical engineering
specialized software [4].
economical operation over a wide range
(design throughput to maximum throughput)
encompassing multiple active constraint
regions [16].
Acetaldehyde is a versatile chemical
intermediate. It is commercially produced via
the Wacker process, the partial oxidation of
ethylene. The process is corrosive, requiring
expensive materials of construction. Eastman
Chemical Company has developed a selective
palladium catalyst that gives acetaldehyde
with selectivity of up to 86% at 46%
conversion. Byproducts formed include
ethanol, acetone and ethyl acetate, all of which
can be sold after purification [21].
This paper focuses on the development of a
decentralized plant-wide control structure for
the US patented process (patent
US006121498A) with modifications in the
process. A custom flow sheet is developed and
plant-wide control structure is developed for

TCE (2014) 1-11© STM Journals 2014. All Rights Reserved Page 1
Acetaldehyde Production Process
process controllability analysis performed
using Aspen Dynamics.
PROCESS STUDIED
The process flow diagram is shown in Figure
1. The process contains mixer, feed effluent
heat exchanger (FEHE or HX1), absorption
column, heat exchangers, compressors and
distillation columns.
The fresh feed contains 100 kmol/h of
hydrogen, 100 kmol/h of acetic acid,
50 kmol/h of ethanol. The absorber is operated
at low pressure (1.41 atm), which results in a
loss of acetic acid of quantity 133 kmol/h. The
hydrogen is vent off in the distillation column
(C1). Acetaldehyde is obtained from second
Fig. 1: Process Flow Sheet for Production of Acetaldehyde.
Absorber
The column in the process has 10 stages and
feed is fed on stage 5. The operating pressure
is 1.41 atm. Diameter of the column is 2 m.
Distillation Column (C1)
The column has 10 stages and feed stage is
stage 5, which is the optimum feed stage to
minimize reboiler heat input. The operating
pressure is 1.97 atm, which gives a reflux
drum temperature of 278.15 K. The reflux
ratio is low (RR = 2), energy consumption
TCE (2014) 1-11© STM Journals 2014. All Rights Reserved
Rao et al.
distillation column (C2) in pure form. The
Aspen NRTL physical property model is used
in all units of the process.
Mixing and Reactor Preheating
Acetic acid, hydrogen and ethanol at 298 K,
9.8 atm pressure are mixed and preheated to
reactor temperature 335 K in HX1. Heat duty
of the HX1 is 47444.2 cal/s.
Reactor (R1)
A vapor stream is fed into the reactor. The
reactor heat duty is 700341 cal/s and reactor
exit temperature is 673.15 K. Since the
reaction is exothermic, the lower the
temperature the higher the chemical
equilibrium constant.
3.96 MW, and the column diameter is 2 m.
Reboiler temperature is 485 K and heat input
is 2.82 MW.
Distillation Column (C2)
Distillate from column C1 is rich of
acetaldehyde product, so it is separated from
the unwanted products in column C2. The
number of trays in the column is 10.
Condenser is total condenser; reboiler is kettle-
type, reflux ratio 2. Feed stream enters above
stage 5 of the column. Heat duty of the
Page 2
Trends in Chemical Engineering
Volume 1, Issue 1

condenser is 3.2 MW and temperature is Figures 2–6 give T-xy diagrams for several
102.18 K. Reboiler temperature is 418.7 K binary pairs. They are water/ethanol,
heat duty is 2.96 MW. water/ethyl acetate, ethanol/ethyl acetate,
acetic acid/ethyl acetate, and acetic
REACTION KINETICS acid/ethanol. Three azeotropic compositions
The production of acetaldehyde involves the are found from the ternary plots. The
following main and side reactions. azeotropes are formed between water/ethanol,
CH3COOH + H2 → CH3CHO + H2O (main) (1) water/ethyl acetate, and ethanol/ethyl acetate.
CH3COOH + 2H2 → C2H5OH + H2O (2) From the plots, it is evident that separation of
CH3COOH + C2H5OH → C2H5COOCH3 (3)
2CH3COOH + 4H2 → CH3COCH3 + CH4 + 3H2O (4)
ethyl acetate and acetic acid is easy due to
Reaction (1) is the main reaction and the difference in boiling points. The normal
selectivity of the acetaldehyde is up to 86% at boiling points of water 100.02 °C, acetic acid
46% conversion. Byproducts formed include 118 °C, ethanol 78.31 °C, ethyl acetate
ethanol, acetone and ethyl acetate. 77.2 °C. Figures 7 and 8 show the ternary
diagrams for ethyl acetate/water/acetic acid
and ethyl acetate/water/ethanol, respectively,
PHASE EQUILIBRIUM
at 1 bar. Azeotrope is formed for ethyl acetate
NRTL physical properties are used in Aspen
and water system at 71.39 °C for ethyl acetate
simulations. There are three basic separations,
and ethanol system at 71.78 °C and for ethanol
namely, acetic acid/acetaldehyde,
and water system at 70.33 °C.
acetaldehyde/ethanol and acetaldehyde/water.

T-xy diagram for ACETICAC/ACEHYD

120
115
110
T-x 1.0133 bar
105 T-y 1.0133 bar
100
95
90
85
Temperature, C

80
75
70
65
60
55
50
45
40
35
30
25
20
0.00 0.05 0.10 0.15 0.20 0.25 0.30 0.35 0.40 0.45 0.50 0.55 0.60 0.65 0.70 0.75 0.80 0.85 0.90 0.95 1.00
Liquid/vapor mole fraction, ACETICAC

Fig. 2: T-xy Plot for Acetic acid/Acetaldehyde.

T-xy diagram for ETHANOL/ACEHYD

80

75
T-x 1.0133 bar

70 T-y 1.0133 bar

65

60
Temperature, C

55

50

45

40

35

30

25

20
0.00 0.05 0.10 0.15 0.20 0.25 0.30 0.35 0.40 0.45 0.50 0.55 0.60 0.65 0.70 0.75 0.80 0.85 0.90 0.95 1.00
Liquid/vapor mole fraction, ETHANOL

Fig. 3: T-xy Plot for Ethanol/Acetaldehyde.

TCE (2014) 1-11© STM Journals 2014. All Rights Reserved Page 3
Acetaldehyde Production Process Rao et al.

T-xy diagram for ETHANOL/EACETATE

78.5
78.0
77.5 T-x 1.0133 bar
T-y 1.0133 bar
77.0
76.5
76.0
Temperature, C

75.5
75.0
74.5
74.0
73.5
73.0
72.5
72.0
71.5
0.00 0.05 0.10 0.15 0.20 0.25 0.30 0.35 0.40 0.45 0.50 0.55 0.60 0.65 0.70 0.75 0.80 0.85 0.90 0.95 1.00
Liquid/vapor mole fraction, ETHANOL

Fig. 4: T-xy Plot for Ethanol/Ethyl Acetate.

T-xy diagram for WATER/ETHANOL

102

100
T-x 1.0133 bar
98 T-y 1.0133 bar

96

94
Temperature, C

92

90

88

86

84

82

80

78
0.00 0.05 0.10 0.15 0.20 0.25 0.30 0.35 0.40 0.45 0.50 0.55 0.60 0.65 0.70 0.75 0.80 0.85 0.90 0.95 1.00
Liquid/vapor mole fraction, WATER

Fig. 5: T-xy Plot for Water/Ethanol.

T-xy diagram for ACETACID/ETHANOL

120
T-x 1.0133 bar
115
T-y 1.0133 bar
110

105
Temperature, C

100

95

90

85

80

75
0.00 0.05 0.10 0.15 0.20 0.25 0.30 0.35 0.40 0.45 0.50 0.55 0.60 0.65 0.70 0.75 0.80 0.85 0.90 0.95 1.00
Liquid/vapor mole fraction, ACETACID

Fig. 6: T-xy Plot for Acetic Acid/Ethanol.

TCE (2014) 1-11© STM Journals 2014. All Rights Reserved Page 4
Trends in Chemical Engineering
Volume 1, Issue 1
Fig. 7: Ternary Map for Ethanol/Water/Ethyl
Acetate.
Fig. 8: Ternary Map for Hydrogen/Acetic
Acid/Acetaldehyde.
TCE (2014) 1-11© STM Journals 2014. All Rights Reserved
Fig. 9: Residue Curve Mapping for Acetic
Acid/Hydrogen/Acetaldehyde.
Fig. 10: Residue Curve Mapping for
Water/Ethanol/Ethyl Acetate.
Figures 9 and 10 show the residue curves; they
lead from the minimum-boiling azeotrope to
the highest-boiling component.
Page 5
Acetaldehyde Production Process
PROCESS DYNAMICS AND
CONTROL
This section deals with a systematic approach
to design a control structure for the
acetaldehyde production process. The design
steps followed are: (1) determination of
temperature control tray, (2) placing the
decentralized PI controllers, (3) application of
relay feedback to find ultimate gain (Ku) and
ultimate period (Pu), and (4) application of
Fig. 11: Plant-Wide Control Structure for Acetaldehyde Production Process.
Controller Design
Once the decentralized control structure was
designed, dynamic simulations were
performed using Aspen Dynamics.
Proportional-integral controllers were used for
flow, pressure, composition, temperature, and
level controls. Relay feedback tests were
performed on temperature loops to find the
ultimate gain (Ku) and ultimate period (Pu).
Initial controller parameters were calculated
according to Kc (Ku/3) and tI (2Pu). In order
to obtain an acceptable damping, further
detuning from the initial settings was done.
TCE (2014) 1-11© STM Journals 2014. All Rights Reserved
Rao et al.
Tyreus-Luyben (TL) and Ziegler-Nichols
tuning to find controller settings.
Control Structure
Figure 11 shows the plant-wide control
structure developed for the acetatldehyde
plant. Before performing dynamic simulations
on the developed control structure,
conventional PID controllers are arranged in
all loops.
Pressure Controller
Pressure controller is arranged for distillation
columns and condensers and the tuning
constants are with a gain of 20 and integral
time of 12 min. Controller output is the heat
removal rate in the condenser to do this task
the controller action assigned as reverse.
Level Controllers
There are a total of five level controllers
arranged for the absorber and for the two
distillation columns. All level loops are
proportional with KC = 10 and integral time of
60 min. For column C1 at base level, one level
controller is arranged and its action is direct.
Page 6
Trends in Chemical Engineering
Volume 1, Issue 1

Its steady state value for the base level is Selecting Temperature/Composition Control
0.625 m. Gain is 10 and integral time 60 min. Tray Location
The second level controller is arranged for the Figure 12 shows a large change in the
reflux drum. PV signal comes from the level temperature profile in the lower part of the
on stage 1. OP goes to valve V15. For this column. Stage 3 is selected for temperature
controller, a direct-acting proportional-only control in column C1. Figure 13 shows the
controller is specified. For this, set point is column composition profile. Figures 14 and 15
0.625 m and bias 50%, gain 10, and integral show the vapor-to-liquid flow rate and relative
time 60 min. Similarly, for second column C2 volatility profiles, respectively.
and for absorption column-level controllers,
pressure controllers are arranged.

Block C1: Temperature Profile

220

200

180

160
Temperature C
140
Te mperature C

120

100

80

60

40

20

0
1 2 3 4 5 6 7 8 9 10
Stage

Fig. 12: Temperature Profile for Distillation Column C1.

Block C1: Liquid Composition Profiles

1.00

0.90

0.80 ACETICAC
H2
0.70 ACEHYD
WATER
0.60
X (mole frac)

EACETATE
ACETONE
0.50
METHANE

0.40 ETHANOL

0.30

0.20

0.10

0.00
1 2 3 4 5 6 7 8 9 10
Stage

Fig. 13: Composition Profile for Column 1.

TCE (2014) 1-11© STM Journals 2014. All Rights Reserved Page 7
Acetaldehyde Production Process Rao et al.

Block C1: Molar Flow Ratios

3.50
3.25 Vapor to liquid flow ratio
3.00
2.75
2.50
2.25
Flow Ratio (Mole)

2.00
1.75
1.50
1.25
1.00
0.75
0.50
0.25
0.00
1 2 3 4 5 6 7 8 9 10
Stage

Fig. 14: Vapor-to-Liquid Flow Rate in C 1.

Block C1: Relative Volatility

55

50 ACETICAC
ACEHYD
45
WATER
40 EACETATE
RelVol-ACETICAC

35

30

25

20

15

10

0
1 2 3 4 5 6 7 8 9 10
Stage

Fig. 15: Relative Volatility Profile in C1.

Tray Temperature Control Composition Control

A temperature controller is arranged to hold
the temperature on stage 3 by adjusting the
reboiler heat input. PID controller is selected
for its built-in relay feedback test capability.
The PV is selected is the temperature on stage
3. The OP is selected to be the reboiler heat
input. Values are initialized. The normal
controller output is 1.96 MMkcal/h. The
controller action is set at reverse because for
the increase of tray temperature reboiler heat
input decreases. Then closed loop ATV test is
performed. The default value of the relay
output amplitude is 5%, which is usually good.
Relay feedback test is performed.
Controllers are arranged to the hydrogen and
acetic acid feed streams and the controller
action is specified as “Reverse.” The PV is the
mole fraction of hydrogen in the feed. In the
next step, initialization and dynamic runs are
performed for convergence of steady state
conditions
Performance Evaluation
For disturbances, the performance is evaluated
from transient response plots. From the closed
loop ATV tests for temperature controller
arranged for column C1, results are reported
as: Ultimate gain 69, ultimate period 1.2 min.
Tyreus-Luyben parameters are gain 21.5
Integral time 2.64 min.

TCE (2014) 1-11© STM Journals 2014. All Rights Reserved Page 8
Trends in Chemical Engineering
Volume 1, Issue 1

Ziegler-Nichols setting test results are gain Response of column C1 for top and bottom
31.3, integral time 1 min. The values show flow rates is shown in Figure 16.
good controlling action of the controllers.
100.0

25. 0

300.0
50. 0 100.0 150.0 200.0 250.0
75. 0
S TRE AMS (" S 28" ).F kmol/hr

S TRE AMS (" S 24" ).F kmol/hr

S TRE AMS (" S 26" ).F kmol/hr

20. 0
50. 0

15. 0
25. 0

10. 0
0.0

0.0 0.5 1.0 1.5 2.0 2.5 3.0

Tim e Hours

Fig. 16: Response Plot for Tops and Bottoms for C1.
0.80 000 7

24 5.524 24 5.526 24 5.528 24 5.53

2.0
Controller Output kmol/hr
P roce ss V ariable bar

S et P oint ba r
1.5
0.80 000 2

1.0
0.79 999 7

0.0 1.0 2.0 3.0 4.0 5.0 6.0

Time Hours
Fig. 17: Pressure Controller Response Plot Absorber.
10000.015000.020000.0
0.6 0.65 0.7 0.75 0.8 0.85
Controller Output kg/hr
Process Variable m
Set Point m

0.0 0.5 1.0 1.5 2.0 2.5 3.0 3.5 4.0 4.5 5.0
Time Hours
Fig. 18: Level Controller Response Plot for C1.

TCE (2014) 1-11© STM Journals 2014. All Rights Reserved Page 9
Acetaldehyde Production Process Rao et al.

150.0 200.0 250.0 300.0

25.0
S TREAMS ("S 24").F kmol/hr

S TREAMS ("S 26").F kmol/hr

10.0 15.0 20.0

0.0 5.0 10 .0 15 .0
Time Hours
Fig. 19: Tops and Bottoms Response Plot for 20% Increase in Hydrogen Flow Rate.

Figures 17 and 18 show the response of maintained despite the large disturbances
pressure and level controllers of the absorber. present in the process and the plant settling
Figure 19 shows the tops and bottoms of time is identified as of less than 9 h. The
column C1 response corresponding to the developed control structure parameters are:
+ 20% disturbance in hydrogen feed rate. ultimate gain 69 and ultimate period 1.2 min
Process reached the steady state at 8.54 h. which is the desired result for a stable
operation of a plant.
CONCLUSIONS
This paper presents a realistic steady-state The byproducts, namely, acetic acid, ethanol,
model and a plant-wide control structure for ethyl acetate, and acetone can be collected at
production of acetaldehyde. No other design the outlet streams of the distillation columns
and control study of this system has been and can be stored. The above results show that
reported in open literature. Three distillation the developed plant-wide control structure is
regions are identified from the residue curves; stable for large disturbances and the designed
they are between water, ethanol, and ethyl plant is environmentally friendly and safe to
acetate. Due to the presence of azeotropic operate.
regions, two distillation columns are used to
separate the products acetaldehyde, ethanol, ACKNOWLEDGMENT
ethyl acetate, water, acetone, hydrogen, and The authors are grateful to Bapatla
methane. The design and operating variables Educational Society, Bapatla, Guntur District,
identified in this process are temperature of Andhra Pradesh, India.
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