Energy Saving of A Methyl Methacrylate Separation Process PDF
Energy Saving of A Methyl Methacrylate Separation Process PDF
pubs.acs.org/IECR
Figure 1. (a) Optimal design owsheet of original design. (b) Material balance lines of original design.
Also, the composition prole in the distillation column goes Table 1. UNIQUAC Model Parameters of the Studied
along the distillation boundary formed by two azeotropes (will Systemsa
be shown later). Thus, a larger reboiler duty was required at the
comp. i MeOH MeOH MMA
distillation column. Some contributions1620 mentioned a mix
with water in a decanter or extractor followed by distillation comp. j water MMA water
methods for this separation purpose, but they all lacked details aij 0 0 0
about the process and also the dynamic control of the process. aji 0 0 0
In this work, this concept will be implemented by simulations bij (K) 165.2623 44.6284 474.3300
and compared to the original design proposed by Wu et al.15 bji (K) 254.7308 411.6194 194.0000
a
Moreover, a feasible control structure will be developed and Aspen Plus UNIQUAC:
tested for the rejection of changes in feed composition or jij
i z
throughput. ln i = ln + qi ln i qiln ti qi + li + qi
xi 2 i j t j
2. ENERGY-SAVING DESIGN i
xjlj
2.1. Proposed Design Flowsheet. To correctly predict xi j
the thermodynamic behaviors of this ternary system, the
UNIQUAC model was selected as in previous work done by where
Wu et al.15 The UNIQUAC model and the binary parameters qixi qixi rx
i i
are shown in Table 1. The proposed conceptual design i = ; qT = qkxk ; i = ; qT = qkxk ; i = ; rT
qT qT rT
owsheet using the same process units by avoiding the saddle z
k k
point is shown in Figure 2a with the material balance lines = rkxk ; li = (ri qi) + 1 ri ; ti = kki ; ij
2
shown in Figure 2b. The fresh feed, containing 69.79 mol % k k
MeOH, 12.5 mol % water, and 17.71 mol % MMA, is rst bij
mixed with some water and condensed stripper overhead so = expaij + ; and z = 10
T
that the composition of this mixture is pulled within the liquid
liquid equilibrium (LLE) envelope. After liquidliquid
separation in the decanter at 50 C, the aqueous stream can mostly MeOH (MeOH/MMA azeotrope at the lowest
further be separated in a distillation column with top product of temperature in that distillation region) and the bottom product
3065 DOI: 10.1021/acs.iecr.6b00391
Ind. Eng. Chem. Res. 2016, 55, 30643074
Industrial & Engineering Chemistry Research Article
methanol, the prole will be in that region where MMA is the with 50% total liquid level is used because of a smaller density
lightest component. Otherwise, if there is so much MMA fed to dierence in two liquid phases. Then this steady-state
the column that some of MMA should go out from the bottom, simulation is exported to the dynamic simulations of Aspen
MMA must be less volatile than methanol, which can be Plus Dynamics. Pressure-driven simulations in Aspen Plus
achieved only with a high-energy-required composition prole Dynamics is selected with the top stage pressures of every
similar to that in the original design. The maximum MMA column set at atmospheric pressure. Pressure drops inside the
content allowed for the prole as in Figure 5b depends on the columns will be automatically calculated by Aspen Plus
product specications and material balance. This is why the Dynamics.
TAC with REC/H2O = 21 in Figure 3 exceeds that of the 3.1. Inventory Control Loops. The intuitive regulatory
original design. The composition prole changes to the high- control and inventory control loops are designed as follows.
energy-required one because the amount of recycled water is
Fresh feed ow rate is ow-controlled with a PI controller of
not enough to separate out most of the MMA in the decanter.
Kc = 0.5 and I = 0.3 min. Both column base levels are
controlled by manipulating their bottom ow rates separately.
3. OVERALL CONTROL STRATEGY DEVELOPMENT
Reux drum level is controlled by manipulating distillate ow
In this section, a proper control strategy for this optimal design rate. As for the decanter, the aqueous phase level is controlled
in Figure 4 will be devised based on open-loop and closed-loop by manipulating aqueous outlet ow, while the organic phase
sensitivity tests with Aspen Plus steady-state simulations. No level is controlled by manipulating organic outlet ow. P-only
online composition measurement will be used in the quality controllers are used in level control loops. To speed up closed-
control loops for wider industrial applications. This control
loop control behavior in the recycle loop, the settings Kc = 10
strategy is expected to hold the product purities at speci-
for the organic and aqueous phase level loops to manipulate
cations despite any feed composition change or throughput
change. organic or aqueous ow and Kc = 5 for the base level loop of
The tray sizing option in Aspen Plus is utilized to calculate distillation column to manipulate bottom ow rate are used.
the column diameters with the assumed tray spacing of 0.6096 m Otherwise, Kc = 2 is used in the other level control loops. The
and weir heights of 0.0508 m. The resulting column diameters pressure of the distillation column is controlled by manipulat-
are 0.890 m for the distillation column and 0.327 m for the ing the condenser duty, while the pressure of the stripper is
stripper. Other equipment sizing follows the recommendations controlled by manipulating the overhead vapor ow. In
by Luyben and Chien.22 Volumes of the column bases and the addition, there are two temperature controllers controlling
reux drum are sized to provide 10 min holdup with 50% liquid temperature of the condensed overhead ow and the stream
level. As for the decanter, it is sized bigger to allow the entering the decanter at 50 C by manipulating the cooler duty.
separation of two liquid phases. The holdup time of 40 min These pressure and temperature PI controller parameters are
3068 DOI: 10.1021/acs.iecr.6b00391
Ind. Eng. Chem. Res. 2016, 55, 30643074
Industrial & Engineering Chemistry Research Article
set at default Kc = 20 and I = 10 min for the purpose of tight specications despite any disturbance. To save time, closed-
control. loop sensitivity test is a test that can help us understand what
After the above regulatory control and inventory control kind of combinations of quality control loops will lead to better
loops are established, there are four remaining degrees of performance in closed-loop control because this test can be
freedom in this system, including reboiler duty and reux rate easily done with Aspen Plus steady-state simulation. This test
of the distillation column, reboiler duty of the stripper, and the assumes that the overall process will nally achieve perfect
recycled water ow rate, which are related to quality control. control after the anticipated disturbances are introduced to the
Thus, in sections 3.2 and 3.3, it will be illustrated how the system. Thus, what we should do is to change the input data,
additional four control loops are determined for manipulating such as feed ow rate or feed composition, as disturbance and
these four remaining degrees of freedom. then use the Design Spec option in Aspen Plus to vary the
3.2. Closed-Loop Sensitivity Test. A control strategy degrees of freedom to hold the product purities at specication.
is desirable if it is able to hold the product purities at Finally, this process will go to a new steady-state equal to
perfect control if the Design Specs options all work successfully.
The last step is to identify any process variables or ratios of
process variables that remain almost unchanged before and
after the introduced disturbance, which are suitable to be
selected as controlled variables.
For this process shown in Figure 4, as mentioned in the
section 3.1, there are four remaining degrees of freedom.
However, the number of product purities of interest are just
three, which means there is still one degree of freedom
untreated if we hold all of the product purities. Thus, a quality
control loop for one of the degrees of freedom should be
guessed again and again until all Design Spec options work
successfully. The process is tested under two types of distur-
bances: one is 20% throughput changes (feed 20%), and
the other is 10% methanol changes in the fresh feed
composition (MeOH 10%). In the feed composition change,
MMA and water composition increase or decrease simul-
taneously and proportionally to each other. The successful
guessed control loop is to x the reux ratio in the distillation
column; then the remaining three degrees of freedom are varied
to hold the purities. Parts of the results of the closed-loop
sensitivity test are listed in Table 4, including process variables
and some important ratios. Base case represents the results
before any disturbance, while the deviation means the results of
perfect control compared to the base case. The other results of
the closed-loop sensitivity test, tray temperatures in the
columns, will be used in section 3.3.
Table 4 shows that every degree of freedom should change
for the sake of perfect control, but some of the ratios can
be xed. These ratios which change least are the reux ratio in
the distillation column (RR), ratio of reboiler duty in C-1 to the
aqueous phase ow rate (QR1/AQ), and ratio of reboiler duty
in the stripper to the organic phase ow rate (QR2/OR). Thus,
xing these three ratios is feasible for perfect control. The
Figure 6. (a) Closed-loop sensitivity test on temperature prole in C-2 remaining degree of freedom is the recycled water ow rate,
stripper. (b) Open-loop sensitivity test with reboiler duty (QR2) on which must be manipulated with the aid of a tray temperature
temperature prole in C-2 stripper. controller.
Table 5. Results in Tray Temperatures from Closed-Loop Sensitivity Tests
deviation
base case (kmol/h) (kW) MeOH + 10% MeOH 10% feed + 20% feed 20%
Ratio and Temperatures
QR2/OR 6.092 0.36% 0.37% 0.13% 0.03%
T2 81.061 0.00% 0.06% 0.13% 0.08%
T36T33 11.126 0.15% 0.05% 0.18% 0.13%
T33T28 9.573 1.18% 1.12% 2.38% 2.12%
[T2], temperature on 2nd stage in C-2; [T36T33], temperature dierence between 36th and 33rd stages in C-1; [T33T28], temperature
dierence between 33rd and 28th stages in C-1.
3.3. Selection of Temperature Control Stage(s). Open- sensitivity (large temperature deviation in open-loop sensitivity
loop and closed-loop sensitivity tests are used to determine the test) to the manipulated variables. On the other hand, as men-
tray temperature control point for both columns. The open- tioned before, an appropriate temperature control point should
loop sensitivity test is performed in which 0.1% changes in also be almost unchanged (small deviation in closed-loop
one of the degrees of freedom is given when others are xed. sensitivity test) for the sake of perfect control. Thus, the control
An appropriate temperature control point should have large point is determined based on both open-loop and closed-loop
sensitivity tests.
For the C-2 stripper, the results of tray temperature deviation
in the closed-loop sensitivity test are shown in Figure 6a, and
the results in the open-loop sensitivity test are shown in Figure 6b.
Although temperature on the rst stage deviates the least under
perfect control, it has less sensitivity to the reboiler duty. The
best temperature control point is the second stage considering
both requirements discussed above. However, in section 3.2, we
know that the reboiler duty can also be manipulated with xed
ratio to the organic phase ow rate. In Table 5, deviations of
this ratio and the temperature on second stage (T2) in closed-
loop sensitivity test are compared. This temperature is better
as a controlled variable because of less deviation, while this ratio
can still be applied as an inner-loop ratio control for better
dynamic performance.
As for the C-1 distillation column, results of both tests are
shown in Figure 7a,b. The selection is not obvious because
stages with larger open-loop sensitivity all have much
temperature deviation under perfect control. Large deviation
in product purities is further conrmed after the introduction of
any disturbance by using either single-end or dual-end
temperature control. However, temperatures on stages 2836
have similar temperature deviations under perfect control. This
means that a smaller deviation in temperature dierence
between any two of these stages can be achieved. If the
temperature dierence between any two stages is selected as a
controlled variable, it should also have enough open-loop
sensitivity to the manipulated variables, which is the subtraction
of two sensitivities for these two stages. Thus, one of the stage
temperatures should have larger sensitivity, while the other one
should have smaller sensitivity. Figure 7b shows that temper-
ature dierence between stages 28 and 33 (T33 T28) has the
largest open-loop sensitivity. However, the nal selected tem-
perature dierence is that between stages 36 and 33 (T36
Figure 7. (a) Closed-loop sensitivity test on temperature prole in C-1 T33) for better closed-loop performance as listed in Table 5, at
column. (b) Open-loop sensitivity test with recycled water ow rate the cost of just a little decrease in the open-loop sensitivity,
(REC) on temperature prole in C-1 column. shown in Figure 7b. Here, controlling a temperature dierence
can also be viewed as a single-tray temperature control with a xed ratio of reboiler duty in C-1 column to aqueous
oating set point from another tray. phase ow rate (QR1/AQ), controlling temperature on second
3.4. Closed-Loop Dynamic Control Behaviors. In stage (T2) in C-2 stripper by manipulating the ratio of its
summary of sections 3.2 and 3.3, the four quality control reboiler duty to organic phase ow rate (QR2/OR), and
loops are determined: xed reux ratio in C-1 column (RR), controlling the temperature dierence between the 36th
3071 DOI: 10.1021/acs.iecr.6b00391
Ind. Eng. Chem. Res. 2016, 55, 30643074
Industrial & Engineering Chemistry Research Article
and 33rd stages (T36-T33) in C-1 column by manipulating For the single-tray temperature controller, the resulting
the recycled water ow rate. PI controllers are used in parameters are Kc = 0.931 and I = 10.56 min with reverse
these two temperature control loops with 1 min deadtime. action. For the controller controlling temperature dierence,
They are iteratively tuned by relay feedback test provided the resulting parameters are Kc = 0.295 and I = 65.34 min with
in Aspen Plus Dynamics with TyreusLuyben tuning rules.23 direct action.
3072 DOI: 10.1021/acs.iecr.6b00391
Ind. Eng. Chem. Res. 2016, 55, 30643074
Industrial & Engineering Chemistry Research Article
The overall proposed control structure is shown in Figure 8. between the 36th and 33rd stages in the C-1 column, and the
Note that two inner-loop ratio controls are added for faster temperature at the second stage in the C-2 stripper. Two inner-
dynamic response: ratio of recycled water ow rate to fresh feed loop ratio controls are added to enhance the dynamic
ow rate and ratio of reboiler duty in the stripper to organic performance. Results show that with the aid of this control
phase ow rate. Thus, both temperature controllers adjust these strategy, the process quickly reaches another steady state within
two ratios separately, rather than directly manipulating recycled 6 h and all the product purities are still maintained near their
water ow rate or the reboiler duty. specications despite any disturbance, such as feed composition
Two types of disturbances will be used to test the proposed changes or throughput changes.
control strategy. The tough disturbance of unmeasurable fresh
feed composition changes is considered rst. Large variations AUTHOR INFORMATION
of 10% methanol changes (MeOH 10%) in the fresh
feed composition are tested, and MMA and water in feed Corresponding Author
composition increase or decrease simultaneously and propor- *Tel: +886-3-3366-3063. Fax: +886-2-2362-3040. E-mail:
tionally to each other. For example, in the +10% MeOH case, [email protected].
the feed composition changes from 69.79 mol % MeOH, Notes
12.50 mol % H2O, and 17.71 mol % MMA to 76.77 mol % The authors declare no competing nancial interest.
MeOH, 9.61 mol % H2O, and 13.62 mol % MMA. Figure 9
shows the closed-loop dynamic responses to feed composition ACKNOWLEDGMENTS
changes. It is observed that the temperature in the C-2 stripper
and the temperature dierence in the C-1 column are The research funding from the Ministry of Science and
quickly controlled back to their set point values within 6 h. Technology of R.O.C. under Grant MOST 104-2218-E-002-
Three product ow rates increase or decrease according to the 006 is greatly appreciated.
unmeasurable feed composition changes. Most importantly, all
three product purities are maintained near their specications
despite these unmeasurable disturbances.
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