Energy
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a r t i c l e i n f o a b s t r a c t
Article history: Distillation columns are one of the main methods used for separating air components. Their inconve-
Received 10 March 2011 nient is their high energy consumption. The distillation process is simulated in three types of columns
Received in revised form and the exergy losses in the different parts calculated. A sensitivity analysis is realized in order to
4 August 2011
optimize the geometric and the operational parameters of each type of column. A comparative exergy
Accepted 6 November 2011
analysis between the distillation columns considered for cryogenic air separation shows that the exergy
Available online 12 December 2011
efciency of a double diabatic column, with heat transfer all through the length of the column, is 23%
higher than that of the conventional adiabatic double columns.
Keywords:
Exergy analysis
2011 Elsevier Ltd. All rights reserved.
Distillation columns
Diabatic process
Cryogenic air separation
0360-5442/$ e see front matter 2011 Elsevier Ltd. All rights reserved.
doi:10.1016/j.energy.2011.11.012
418 J. Rizk et al. / Energy 37 (2012) 417e429
coefcients are those presented in [8] and the equation for the
interfacial surface is the one presented in [10].
The mass transfer coefcient in the vapor kG, is represented as
an average value between a laminar coefcient and a turbulent
coefcient (Eq. (12) [8]). The laminar and turbulent Sherwood
numbers are expressed by the VDI-Wrmeatlas correlations (Eq.
(13)). In Eqs. (12) and (13), ScG is the vapor Schmidt number, (dh/
lG,pe) is the ratio of the hydraulic diameter to the length of vapor
ow channel within a packing element, ReG,rv is the vapor Reynolds
number, calculated with the relative velocity (vG,e vL,e), and g is
the contact angle. The liquid/vapor friction factor xGL, is correlated
using the Colebrook equation for the friction factor in circular
channels, modied to have an explicit expression (Eq. (14) [11]) and
the hydraulic diameter dh (Eq. (15)) is calculated as a function of the
Fig. 3. Liquid and vapor ow rates in a nite volume i.
packing geometric parameters and the liquid lm thickness, given
by Nusselt formula for falling lms on inclined wall situation (Eq.
(16)).
Oxygen conservation in liquid:
Replacing m_ N2 by its values (Eq. (10)) in Eqs. (2), (3), (7), and (8) v2
gives the four equations (Eqs. (19)e(22)) used in the system to be DP 1:941h0:446
L f rg (23)
dh
solved to calculate the variables of the nite volume.
hL 0:0273Re0:331
L (24)
xi x*i
Li1 xi1 Li xi kL;i Si 0 (19) The friction coefcient in Eq. (23) is calculated as a function of
Vi
the vapor Reynolds number, as follows [12]:
Gi1 yi1 Gi yi kG;i Si Pi y*i yi 0 (20) 8:02ReG 105 0:364; if ReG < 1500
f (25)
1:43ReG 106 0:266; if ReG 1500
xi x*i hfg;N2 xi x*i It is remarkable that equations for the pressure drop, the mass
Li1 Li kL;i Si kL;i Si 0 (21) transfer coefcient, and the interfacial surface require the vapor
Vi hfg;O2 Vi
and the liquid thermodynamics properties. These properties being
function of variables to be calculated (molar fractions, pressures,
and temperatures), an iterative procedure is used. It could be
hfg;N2 *
Gi1 Gi kG;i Si Pi y*i yi kG;i Si Pi yi y i 0 (22) summarized by the following steps.
hfg;O2
1. Given the feed mass ow and molar composition, assume
When the conservation equations are to be written at the stage F
constant mass ow rates of liquid and vapor and linear varia-
where the feed is introduced to the column, Eqs. (19)e(22) are
tions of the liquid and vapor compositions through the N nite
replaced by Eqs. (19a)e(22a) in order to take into account the ow
volumes.
rates added.
2. Given the pressure at the boiler, assume constant pressure on
all nite volumes.
xF x*F
LF1 xF1 LF xF kL;F Si 0 (19a) 3. Using the pressure and the molar fractions from 1 and 2,
VF calculate the thermodynamic properties of ows at the liquid
saturation temperature, using REFPROP 8.0.
GF1 yF1 GF yF kG;F Si PF y*F yF m
_ F yF 0 (20a) 4. Using the vapor mass ow rates from 1 and the thermody-
namic properties from 3, evaluate the pressure drop using Eq.
(23).
xF x*F hfg;N2 xF x*F 5. Using the new pressure prole from 4 and the molar fractions
LF1 LF kL;F Si kL;F Si 0 (21a)
VF hfg;O2 VF from 1, calculate the liquid saturation temperatures and new
thermodynamic properties for the mixtures.
hfg;N2 * 6. Using thermodynamic properties from 5, calculate mass
GF1 GF kG;F Si PF y*F yF kG;F Si PF yF yF transfer coefcients and interfacial surface.
hfg;O2
_F 0
m (22a) At this stage, six variables are to be found for each nite volume (Gi,
The evolution of the pressure in the column is function of the Li, xi, yi, xi*, yi*). The total number of variables is 6N. At the 1st and
pressure drop on each nite volume. Many studies have been the Nth nite volumes, four variables are added: the liquid ow
realized in order to correlate the pressure drop in structured sent to volume N (LN1, xN1) and the vapor ow sent to volume 1
packing [12e14]. They correlate the pressure drop using the linear (G0, y0). Equations needed to calculate these variables are the mass
pressure drop in a dry channel and applying corrections to the and species conservation at the boiler and the condenser:
vapor velocity and the friction factor.
G0 BL1
A correlation for the vapor velocity correction, as a function of
y 0 x1
the liquid and vapor properties and of the liquid velocity is (26)
LN1 CGN
proposed by Woerlee et al. [13]: two types of corrections are xN1 yN
applied to the velocity, a static correction, related to the decrease of
the channel section due to the liquid ow, and a dynamic correc- The iterative procedure continues after step 6 by the following:
tion, related to the interfacial velocity. Fernandez et al. [14] ach-
ieved CFD simulations of countercurrent liquid and vapor ows in 7. Write a (6N 4) (6N 4) matrix A, with Eqs. (1), (11),
a structured packing, by correcting the vapor ow velocity, stati- (19)e(22) written for each nite volume, and Eq. (26). Write
cally and dynamically. Values of the pressure drop calculated when a (6N 4) vector B, with constant values at the feed location.
applying both corrections on the vapor velocity did not differ much 8. Resolve the system AX it B.
from those obtained when applying the static correction only. 9. Using the mass ow rates and molar fractions from 8, repeat
Using this result, only a static correction is applied to the vapor steps 3e8. Calculate a new vector X(it1).
velocity in this study. 10. Calculate the relative differences between each line of vectors
Two correlations for the correction of the friction factor are X(it) and X(it1).
proposed in the literature in [12,14]. The friction factors 11. If the maximum of the relative differences is less than 104, go
calculated by each correlation are compared, and their values did to step 12. Else, go back to step 9, using the vector X(it1).
not differ signicantly. The correlation proposed by Darcy and 12. Exergy analysis, as shown in Section 2.2.
Weisbagh (Eq. (23)) calculates this factor as a function of the liquid
holdup [12]. The liquid holdup, dened as the fraction of liquid 2.2. Exergy analysis of a simple adiabatic column
occupying an element of vertical pipe, is given in Eq. (24), within
a 15% error, as a function of the liquid Reynolds number (correla- The exergy analysis of a simple adiabatic column accounts
tion of Collodziej). for exergy losses due to mass transfer in each nite volume and
J. Rizk et al. / Energy 37 (2012) 417e429 421
for exergy losses due to heat transfer in the boiler and the conditions on the liquid product (mass ow rate and purity). Exergy
condenser [6]. losses in the process are only evaluated for the columns providing
On a nite volume i, exergy losses are calculated by an exergy the desired product. These conditions allow the algorithm to
balance between the inlet ows and the outlet ows (Eq. (27) [7]). reduce the list of parameters, as follows:
And the exergy loss in the boiler is: The algorithm output data are exergy losses for each combina-
tion of the above parameters. Before proceeding to the overall
Tref
Exloss;boil G0 ExL1 ExG
0 Wboil 1 (30) optimization of the exergy losses in the simple adiabatic distillation
Tboil column, a sensitivity analysis shows the inuence of each param-
The thermodynamic efciency of the column equals the ratio of eter on the total exergy losses in the column and on the distribution
the minimum work required to the distillation process to the of losses in the different parts of the column.
effective work required (Eq. (31) [16]). The minimum work is
calculated by the column exergy balance (Eq. (32) [17]). 2.2.1. Sensitivity analysis
In order to study the effect of each parameter on the exergy
Wmin losses in the process of cryogenic separation of air components in
h P (31)
Wmin Exloss a simple adiabatic distillation column, each parameter is varied
alone for a set of xed values of the others.
X X Fig. 4(a) shows the effect of the reux ratio at the bottom of the
Wmin Exout Exin (32)
column, B, on the total exergy losses. Fixed values of the rest of the
Before comparing the simple adiabatic column to thermally parameters are listed below. Unless different values are given, these
coupled and heat-integrated distillation columns, an optimum xed values are the one used all through the sensitivity analysis for
conguration, dened by geometric and operating parameters, is the simple adiabatic distillation column.
searched for the simple conguration. Parameters to be optimized
are as follows: H 10 m;
d 18 m;
Column diameter, d. F 1 m;
Feed location from the bottom, F. P0 110 kPa;
Pressure at the boiler, P0. C 0.4.
Reux ratio at the bottom of the column, B.
Reux ratio at the top of the column, C. The feed mass ow rate varies with the reux ratio at the
bottom of the column and when B increases the feed mass ow rate
The molar composition of the feed stream is 78.1% of nitrogen increases. This leads to an increase in the energy needed to separate
and 21.9% of oxygen. The desired product is low pressure, oxygen the feed mixture components on one hand, and on another hand,
rich liquid (>95% of oxygen). The mass ow rate of products is that an increase in the pressure drop in the column. Consequently, total
of an actual distillation unit, 5000 tons per day. exergy losses in the column increase. The thermodynamic ef-
Parameters listed above are the input data of the simulation ciency of the column decreases from 29% to 15.2% when varying the
algorithm. Once step 11 is achieved, the algorithm veries reux ratio at the bottom from 0.56 to 0.83. It should be noted that,
Fig. 4. Total exergy losses in the column, (a) as a function of the reux ratio at the boiler stage, (b) as a function of the reux ratio at the condenser stage.
422 J. Rizk et al. / Energy 37 (2012) 417e429
Fig. 5. Inuence of the pressure on the total exergy losses. Fig. 7. Inuence of the feed location on total exergy losses.
J. Rizk et al. / Energy 37 (2012) 417e429 423
Fig. 9. Total exergy losses in different congurations of simple adiabatic columns. Fig. 11. Representative scheme of a Petlyuk distillation column [19].
424 J. Rizk et al. / Energy 37 (2012) 417e429
1. For a given combination of the reux ratios at the top and at the
bottom of columns, estimate initial values for Mfeed,HP and
Mfeed,LP, considering a liquid low-pressure product of
5000 tons/day and the energy balance at the intermediate heat
exchanger.
2. Simulate high-pressure column and then low-pressure column.
3. When convergence is obtained, correct Mfeed,HP and Mfeed,LP,
considering the 5000 tons/day liquid product ow rate and the
energy balance at the intermediate heat exchanger.
4. If the new values of the feed ow rates calculated differ from
previous values (relative difference > 104), go back to step 2.
Else, go to step 5.
5. If the oxygen molar fraction in the low-pressure liquid product
exceeds 95%, calculate the exergy losses in the column. Save the
results.
Fig. 12. Thermally coupled column for cryogenic air distillation.
Fig. 13. Inuence of the reux ratios in the high-pressure column on the total exergy losses, (a) effect of the reux ratio at the bottom, (b) effect of the reux ratio at the top.
Fig. 15 shows the effect of pressure levels in the columns on total column and the liquid feed in the low-pressure column at a 9-m
exergy losses. Since a constant temperature difference of 5 K is height from the bottom.
assumed at the intermediate heat exchanger between the high-
pressure vapor condensation and the low-pressure liquid evapo- 4. Diabatic distillation column
ration, the pressure level of the high-pressure column is calculated
for each value of the low-pressure to ensure this condition. An The thermal coupling between adiabatic columns includes an
increase in the low-pressure column is followed by an increase in intermediate heat exchanger where low-pressure liquid evaporates
the high-pressure column causing an increase in the compressor and high-pressure vapor condensates. Further thermodynamic
exergy losses. The compressor contribution in total exergy losses in improvements could be achieved in the distillation processes by
the double adiabatic column being the highest (50e60%), total distributing this thermal coupling over the height of the columns.
exergy losses will increase due to the increase in the compressor Instead of increasing the high-pressure in the column in order to
exergy losses. ensure a 5-K pinch at the intermediate heat exchanger, a lower
For the double adiabatic column, the geometric parameters value of the pressure could be tested if the heat exchange between
(diameters and heights of columns and feed locations) present the the columns is still achieved through wall contacts of the two
same effect as for the simple adiabatic column. Total exergy losses columns.
decrease when the column diameters increase because the pres- The rst approach for creating diabatic ows in distillation
sure drop decreases. The feed location, in both columns, has very columns was by adding sequential heat exchangers all through the
little effect on total exergy losses. column height [5,7,22,25,26]. Fig. 17 shows heat exchangers, adding
heat to the stripping section of the column, and removing heat from
3.2.2. Overall optimization of the column the rectifying section. In this conguration, the exergy destruction,
Several possible combinations of geometric and operating located principally in the boiler and the condenser, is distributed on
parameters are considered and total exergy losses are calculated for trays [5]. As a result, the diabatic column destructs half the exergy
each combination. A decreasing curve is obtained (Fig. 16) and a conventional column would destroy for the same separation.
optimal congurations are deduced. Minimum exergy losses of Rivero et al. [22,25] searched for the optimal allocation of the
31.4 kW/kg of vapor feed are calculated for a conguration where sequential heat exchangers leading to the best thermodynamic
the low-pressure column operates at 110 kPa and the high-pressure performances, and calculated 39% exergy loss decrease in the dia-
column at 750 kPa. The columns are 22-m diameter and 10-m batic column, compared to the conventional column.
length each. The reux ratios are as follows: 0.1 at the high- Recently, a new type of diabatic distillation column was pre-
pressure boiler, 0.6 at the high-pressure condenser and 0.8 at the sented. Known as internally heat-integrated distillation column, it
low-pressure condenser. The vapor feed in the high-pressure has the same approach of adding and removing heat through the
column is introduced at a 1-m height from the bottom of the column height, but the stripping section and the rectifying section
Fig. 14. Effect of the bottom reux ratio in the low-pressure column on exergy losses. Fig. 15. Effect of pressures in the columns on total exergy losses.
426 J. Rizk et al. / Energy 37 (2012) 417e429
Fig. 16. Total exergy losses in different congurations of double adiabatic columns.
are put into contact and form a heat exchanger, where heat is
transferred from the hot source (the HP rectifying section) to the
cold sink (the LP stripping section) [2,3,27]. The ideal conguration
of the internally heat-integrated columns contains neither boiler Fig. 18. Ideal internally heat integrated distillation column.
nor condenser. Therefore, it reduces the total exergy losses in the
column and increases its efciency.
In this paper, an ideal internally heat-integrated distillation the high-pressure vapor and the evaporation of the low-pressure
column is considered and represented in Fig. 18. liquid. On the nite volume i of Fig. 3, an additional variable, the
The simulation of the diabatic column operation differs from the heat transferred, is to be added.
previous studied adiabatic columns, where an industrial packed To calculate the amount of heat transferred, an overall heat
column was considered. The conservation equations should be transfer coefcient is rst correlated. It takes into account
adapted to take into account the additional heat transfers through a convective heat transfer coefcient during the condensation of
the column. vapor mixtures at high pressure, a convective heat transfer coef-
cient during the evaporation of liquid mixtures at low-pressure and
a conductive heat transfer coefcient through the heat exchanger
4.1. Simulation of the diabatic distillation column
wall. Correlations for convective heat transfer coefcients are
detailed in [28]. Thome correlation for evaporation in the low-
In order to simulate the diabatic column, we assume that the
pressure column and Ackers correlation for the condensation in
distillation process is realized in a heat exchanger which surface
the high-pressure column are used in this study. When the overall
contact area is sufcient to exchange heat between the low-
heat transfer coefcient is evaluated, the heat exchanged is calcu-
pressure mixtures and the high-pressure mixtures.
lated as a function of the temperature difference between the two
In this distillation conguration, mass ow rates of the liquid
columns.
and vapor mixtures vary more markedly, due to condensation of
The conservation equations with heat transfer are replacing Eqs.
(19)e(22), and give Eqs. (36)e(39).
xi x*i Qi
Li1 xi1 Li xi kL;i Si xeq (36)
Vi hfg;eq
Qi
Gi1 yi1 Gi yi kG;i Si Pi y*i yi xeq (37)
hfg;eq
hfg;N2 *
Gi1 Gi kG;i Si Pi y*i yi kG;i Si Pi yi yi
hfg;O2
Q
i (39)
hfg;eq
The method of simulation of the diabatic distillation process in determine the number of passes needed to ensure the 5000 tons
a heat exchanger is as follows: per day of the liquid product.
Before proceeding to the general optimization of the process,
1. The feed mass ow rate and molar composition being known, a sensitivity analysis is achieved, to study the effect of each
assume a linear variation of the liquid and the vapor mass ow parameter on total exergy losses in the column, producing 5000
rates and compositions. tons per day of oxygen rich liquid at low-pressure.
2. Assume a linear variation of the pressures.
3. Calculate liquid saturation temperatures using REFPROP 8.0 4.2.1. Sensitivity analysis
with compositions and pressures from 1 and 2. The effect of each parameter on total exergy losses in the dia-
4. Calculate thermodynamic properties of liquid and vapor batic column is now studied, by choosing xed values for other
mixtures on both pressure levels. parameters.
5. Calculate pressure drops using properties from 4. First, the effect of pressure levels on each side of the column is
6. Calculate corrected thermodynamic properties using pressures studied. Fig. 19 shows the effect of the pressure ratio between the
from 5. two sides of the heat exchanger on the total exergy losses.
7. Calculate heat transfer coefcients and heat exchanged. Fig. 19(a) represents the total exergy losses per kg of high-
8. Calculate mass transfer coefcients. pressure vapor feed and Fig. 19(b) represents them per kg of
9. Write 6N equations for the high-pressure column and resolve low-pressure liquid product. The xed values of other parameters
the system AX B. are xed to:
10. Using L1 and x 1 at high pressure, write 6N equations for the
low-pressure columns and resolve the system AX B. H 10 m
11. Calculate the relative differences for both columns. dLP 44 mm
12. If maximum relative difference higher than 104, repeat from dHP 44 mm
step 4. Else, proceed to exergy analysis. Mfeed 0.1 kg/s/pass.
Fig. 19. Exergy losses as a function of the pressure ratio, (a) per kg of vapor feed, (b) per kg of liquid product.
428 J. Rizk et al. / Energy 37 (2012) 417e429
Fig. 20. Exergy losses as a function of geometric parameters, (a) as a function of the column height, (b) as a function of low-pressure pass diameter.
Performances of double adiabatic columns and diabatic columns aP Packing surface area (m2/m3)
are compared regarding total exergy losses calculated in optimal bP Corrugation base length (m)
congurations. A total of 23% decrease in total exergy losses are B Reux at the boiler
calculated when replacing the local intermediate heat exchanger of C Reux at the condenser
the double adiabatic column by an overall heat transfer between d Column diameter (m)
the columns. This decrease is due mainly to the decrease in the dh Hydraulic diameter (m)
pressure in the high-pressure column (from 750 kPa to 450 kPa), D Diffusion coefcient (m2/s)
decreasing exergy losses in the compressor. It is also due to the Ex Exergy (W)
decrease in irreversibilities in the column due to heat transfers. f Friction factor
The comparison with the simple adiabatic column cannot be F Feed location (m)
made on a similar basis since the products of the simple adiabatic h Enthalpy (J/kg)
column distillation are different from those of the double column hfg Heat of vaporization (J/kg)
(presence of a high-pressure nitrogen rich vapor product in the hL Liquid holdup
double columns). Besides, the simple adiabatic column has no hP Corrugation height (m)
compressors and the production of the cold source for the hpe Height of the packing element (m)
condensation at the top is not considered. H Column height (m)
k Mass transfer coefcient
K Henry constant
lG,pe Length of the vapor ow channel within a packing
element (m)
L Liquid mass ow rate (kg/s)
m_ Mass ow rate (kg/s)
P Pressure (bar)
Q Heat (W)
s Entropy (K/kg.K)
sP Corrugation side length (m)
Si Interfacial surface (m2)
T Temperature (K)
v Velocity (m/s)
V Vapor mass ow rate (kg/s)
Vm Molar volume (m3/mol)
x Nitrogen molar fraction in the liquid
Fig. 21. Exergy losses in the diabatic column for different congurations. x0 Oxygen molar fraction in the liquid
J. Rizk et al. / Energy 37 (2012) 417e429 429
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