Accepted Manuscript

Towards better styrene distillation scheme: From grassroots design to retrofit

Chengtian Cui, Xingang Li, Dongrong Guo, Jinsheng Sun

PII: S0360-5442(17)31025-3

DOI: 10.1016/j.energy.2017.06.031

Reference: EGY 11039

To appear in: Energy

Received Date: 20 May 2016

Revised Date: 14 April 2017

Accepted Date: 06 June 2017

Please cite this article as: Chengtian Cui, Xingang Li, Dongrong Guo, Jinsheng Sun, Towards
better styrene distillation scheme: From grassroots design to retrofit, Energy (2017), doi: 10.1016/j.
energy.2017.06.031

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 ACCEPTED MANUSCRIPT

Towards better styrene distillation scheme: From grassroots design to retrofit

Chengtian Cuia, Xingang Lia, b, c, Dongrong Guod, Jinsheng Suna, *
aSchool of Chemical Engineering and Technology, Tianjin University, Tianjin, 300072, P. R. China
bNational Engineering Research Center of Distillation Technology, Tianjin, 300072, P. R. China
cCollaborative Innovation Center of Chemical Science and Engineering, Tianjin, 300072, P. R. China
dShandong Qilu Petrochemical Engineering Co. Ltd, Zibo, Shandong, 255400, P. R. China

Abstract
The current state-of-the-art commercial styrene distillation schemes, featured by conventional
distillation columns to purify styrene, are introduced with energy, exergy and economic analyses.
Amongst all the procedures the separation of ethylbenzene/styrene, the critical close-boiling system,
accounts for ~65% of the total energy requirement. To improve the energetic efficiency, double-effect
distillation (DED) and heat pump distillation (HPD) are suggested as competitive improvements on
conventional distillation schemes (CDSs), which give birth to advanced distillation schemes (ADSs). In
addition, sensitivity analysis is carried out to determine the optimal operational parameters of columns
in styrene distillation process. Taking the CDSs as benchmark processes, the ADSs with DED and
HPD can lower operating costs by up to 30% and 40%, respectively. The synergistic effect makes
retrofit proposals payback period very attractive, through considerably energy costs reduction and
uttermost equipment reuse. In the view of total annualized cost (TAC), the ADSs can cut a corner of
~35-40% from the CDSs. Specifically, the ADS using HPD slightly outperforms its DED counterpart
in TAC comparison. Despite energetic or monetary advantage, the ADSs also show their environmental
drawback of higher exergy losses than the CDSs.
Keywords: Styrene distillation scheme; Conventional distillation sequence; Grassroots process design;
Energy-saving distillation technology; Advanced distillation scheme; Retrofit proposals

1. Introduction
Styrene monomer (SM) is the simplest and by far the most important member of a series of
aromatic monomers that is used in the plastics industry [1]. It is widely used in synthesizing various
polymers and copolymers, such as polystyrene (PS), acrylonitrile-butadiene-styrene copolymers
(ABS), styrene-acrylonitrile copolymers (SAN), styrene-butadiene rubber (SBR), styrenic block
copolymers (SBC), styrene-butadiene latex (SBL) and adhesives [2]. The capacity of producing SM
has increased constantly with the commercial demand. It is estimated over 25 million tons of SM is
produced worldwide annually [1-3].
Currently, catalytic dehydrogenation of ethylbenzene (EB), shown in Fig. 1, overwhelms in
styrene industry [4]. When styrene production happens in dehydrogenation reactor, steam is added to
lower partial pressure of EB, boosting styrene conversion and suppressing undesirable byproducts,
such as lights (hydrogen, ethylene, carbon monoxide, carbon dioxide etc.), benzene, toluene and other
heavy components known as styrene tar [5]. After removal of lights and water from the
dehydrogenated products in a three-phase (vapor, aqueous and organic) decanter, the organic phase
(SM, benzene, toluene, unreacted EB and styrene tar) is to be separated or recycled in styrene

*Corresponding author

E-mail address: jssun2006@vip.163.com (J. Sun).

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distillation unit, the most popular option to manipulate reactor outputs commercially [6-7].
However, it is significantly energy intensive to treat the organic phase by conventional distillation
[6-7]. The low thermodynamic efficiency is the most responsible aspect of conventional distillation
column (CDiC), with high-grade energy at reboiler and a similar output of waste heat at condenser [8].
This gives opportunities to the suggestion of numerous energy efficient distillation pathways to lower
CDiC energy consumption [9-12]. The options, with the aid of intermediate heat exchangers to recover
heat in common, include double-effect distillation (DED) with an additional distillation column [13-
14], heat pump distillation (HPD) with a compressor [15-17], internally heat-integrated distillation
column (HIDiC) with a pressured rectifying section [18-21], and dividing wall column (DWC) with an
equivalent prefractionator [22-25]. Although HIDiC and DWC are very less commonly industrialized
[11], DED and HPD are welcomed by patent licensers and engineering companies for reliability with
rich design experience [26]. Recently, Jongmans et al. added a conceptual extractive distillation (ED)
to the warehouse of separating EB/SM system by using sulfolane [1,27,28] or ionic liquid [29] as the
extraction agent. ED was announced to be able to reduce energy requirement by ~40-45% compared to
conventional distillation [27]. However, this pathway is lack of reports of successful industrialization in
the field of styrene, possibly in fear of contamination of high purity SM product by external extraction
agents [27]. This uncertainty undermines the consideration of ED herein.
This work starts from energy, exergy and economic analyses (3E analyses) of current state-of-the-
art commercial styrene distillation schemes. Since these schemes are based on the CDiC, they are
referred to conventional distillation schemes (CDSs) later in this work, whose sequences are studied for
further amelioration. Then DED and HPD configurations are applied on the CDSs, to give birth to
advanced distillation schemes (ADSs). Finally, 3E analyses of ADSs are carried out, with the aid of
sensitivity analyses to investigate optimal operational parameters of columns. Moreover, an economic
evaluation of the payback period (PBP) for additional investment is necessary to determine the
feasibility of the ADSs.
To clearly compare total energy consumption of CDSs and ADSs, all of the utilities depletedas
secondary energy consumptionare converted into primary standard oil consumption, in close link
with economic expenditures. Together with operating costs, the capital investments, including
distillation columns, condensers, reboilers and compressors, are calculated and included into total
annualized cost (TAC) for economic evaluation.

2. Theory
2.1. Distillation sequences
Currently most industrial multicomponent separations are carried out employing conventional
distillation sequences (CDiSs) [30]. A CDiC is defined as a separator with one feed with two products,
equipped with one condenser and one reboiler [31]. For a N-component mixture, if N product streams
are required, a CDiS is necessarily composed by N-1 CDiCs [32]. The number of possible CDiSs is
provided by Eq. (1) [33]:
[2( 1)]!
= (1)
!( 1)!
The introduction of state-of-the-art commercial styrene distillation schemes starts by the synthesis
of CDiSs, in hope of improving energy efficiency and economic benefit at the beginning. As shown in
Fig. 1, this separation process consists of five product streams and therefore four CDiCs are necessary
for the separation task. Herein, to reduce the enumeration of CDiSs, the SM and tar are lumped as the

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heavies, requiring an additional column. Under this circumstance, a pseudo four products to be purified
are benzene (a), toluene (b), EB (c), SM and tar (d). Fig. 2 enumerates all five possible CDiSs in
consideration. The molecular structures and normal boiling points (NBPs) of these products are listed
in Table 1. Notably, the NBP of EB is very close to that of SM, so EB/SM mixture is composed to a
close-boiling system.
Since SM will polymerize over a certain high temperature [5-6], the distillation operates under
vacuum with 2-sec-butyl-4,6-dinitrophenol (DNBP), as polymerization inhibitor, to be added in the
dehydrogenated products. Reasonably, it is favored by heating SM as fewer times as possible. In CDiSs
1 and 2, SM is boiled three times, but it is only heated twice in 3, 4 and 5, hence 1 and 2 are eliminated
for the sake of safety and higher SM yield. Practically, the mass flow rate of benzene and toluene is
much smaller than that of EB, so it consumes more steam to boil EB three times. Compared with only
two times in 3 and 5, sequence 4 is removed as well.
The CDiS analysis shows that only sequences 3 and 5 are acceptable in grassroots process design.
The choices are consistent with commercialized state-of-the-art styrene distillation schemes, which will
be referred to in detail in the following sections.

2.2. DED
DED (Fig. 3) implements two columns instead of one in CDiC [11,13-14]. It uses the overhead
vapor from high-pressure column (HPC) to drive the subsequent reboiler of the low-pressure column
(LPC), combining the condenser of the former with the reboiler of the latter, eliminating a heat
exchanger as well as the corresponding utilities. Instead of treating the entire crude feed in one column,
the feed is split into two approximately same streams and entered into HPC and LPC, respectively. The
pressure difference of adjacent columns provides temperature difference at HPC overhead and LPC
bottom, creating heat transfer drive from the pressured stream to the heat-receiving column. Compared
to CDiC, DED could upgrade half of low-grade heat and reuse it as hot utility, saving considerable
energy.

2.3. HPD
HPD facilitates the upgraded waste heat by compressing overhead vapor instead of enhancing
pressure of entire column to achieve heat upgrade and transfer, safely avoiding elaborate automatic
control scheme that DED required [9]. It is expected that HPD will bring about 20-50% of energy
savings [34].
HPD is classified into different patterns, such as vapor compression, thermal and mechanical
recompression [15], aiming at escalating and utilizing heat capacity of stream from the column top to
drive its bottom. Vapor compression (VC) and mechanical vapor recompression (MVR) are usually
available for commercial purposes [15]. The schemes of VC and MVR are shown in Fig. 4.
In VC, working fluid evaporated by top vapor of column discharges heat to the reboiler through a
compressor to provide required work input and an expansion valve to close the cycle. As a remarkable
feature, all units involved are external to the distillation process. Consequently, the column does not
require major modifications except for possible adjustments in heat exchangers for changing utilities.
On the other hand, MVR compresses overhead vapor of column to heat the reboiler, preventing the
intermediate medium from cooling below the boiling point of the top products, thus saving one more
heat exchanger and enjoying lower investments than VC.
The coefficient of performance (COP) [15] is usually used to evaluate the performance of heat

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pump. It is defined as discharging heat in condenser over electrical power required for upgrade the
energy. The higher the COP of a heat pump, the better the performance.

2.4. Energy analysis based on standard oil

In order to compare the consumption of utilities with different energy qualities, all the utilities
depleted, including electrical power, recycling cooling water (CW) and steams with different bands, are
converted into standard oil consumption in reference to P. R. China national standard [35], provided in
Table 2. In this study, the price of standard oil was consulted to Shandong Qilu Petrochemical
Engineering Co. Ltd, and rated as 0.30US$/kg. It should be noted that this price is fluctuating with
international market.

2.5. Exergy analysis of distillation

As an important thermodynamic property, exergy () is defined as the maximum quantity of
mechanical work one could obtain from a given heat source [36-37]. Clearly, exergy can be used as the
measurement of energy quality, and energy quality degeneration leads to exergy loss. For a continuous
flow, the specific exergy is defined as:
= ( 0) 0( 0) (2)
where H and S are the enthalpy and entropy of a process stream under operational conditions. 0 is the
ambient standard temperature (e.g. atmosphere, river and ocean). According to Sun et al. [38], exergy
losses in a distillation column are mainly distributed in reboiler, condenser and trays.
In the reboiler, steams with different band are used as hot utility. If the transfer of an infinitesimal
quantity of heat is considered, and the temperature of the reboiler is , then the exergy of this heat
is:
0
= (1 ) (3)

The received infinitesimal exergy of the heated stream () is:
0
' = (1 ) (4)

The total exergy loss at reboiler is determined by integrating the difference between Eqs. (3) and
(4) from the inlet temperature to the outlet temperature :

(
0 0
)

, =
(5)

If constant temperature difference in reboiler is postulated, exergy loss is derived out as follow:

(
0 0
, =

) (6)

Inducing the derivative of , with respect to :

, 0
= >0 (7)
2

Eq. (7) tells that the larger the driving force, the larger exergy loss in reboiler, and the growth rate
of exergy loss is inversely proportional to the square of utility steam temperature. In other words, the
choice of proper steam band has great impact on the exergy loss during heat transfer.

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Likewise in the condenser, cooling utility () is required and the exergy loss is:

(
0 0
)

, =
(8)

If CW is chosen as the cold utility, its temperature will not maintain constant during heat transfer.
In this case, the should be replaced by the logarithmic mean of inlet and outlet temperature
difference ():

( )
0 0
, = (9)

where:
, ,
= (10)
(, ,)

Suppose that the heat loads of the condenser and reboiler are equal, the exergy loss in condenser
is usually larger than that in reboilers [38].
The exergy loss of the trays is due to the irreversible mass and heat transfer during distillation
process [38]. The vapor rising from i+1 tray encounters with the liquid falling from the i-1 tray, and the
higher temperature of the former will help less volatile components of the latter to condensate and
release heat on the ith tray. Simultaneously, absorbing the released heat, the more volatile components
of the latter will enrich in the vapor phase. Assuming this mass and heat transfer process is under
adiabatic condition, where = , then the exergy loss on trays will only determined by the
entropy of streams and can be obtained:
, = 0(, + 1 + , + 1 , ,) (11)
For a distillation column, the minimum work required for separation is the exergy difference
between the product streams and the feed streams [39]. This minimum work is accessible only if the
column has infinite theoretical stages and infinite heat exchangers [13]. Eq. (12) reveals this
relationship:
=
(12)

For a CDiC, it requires high-grade heat at reboiler and discharges low-grade heat at
condenser. The total work supplied from the utility system is given by:
0 0
= (1 ) (1 ) (13)

When a heat pump is involved into the distillation process, the utility supplies of electrical power,
' '
cold utility and steam are changed to , and . This way the total work supplied from utilities
should be rewritten as follow:
0 0
= + ' (1 ) ' (1 ) (14)

Based on Eqs. (12) ~ (14), the total exergy loss of the distillation column can be calculated as
follow:
, = (15)

2.6. Economic analysis

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To evaluate the performance of an industrial plant, economic analysis has to be involved. The cost
must be annualized to study the economics in terms of TAC (US$/year). TAC is composed by the
capital investment () in all units and operational expenditure () on utilities, expressed
as:
= + (16)
in which, f is annualization factor defined by Smith [32].
Given a fixed period n (year) at a fixed rate of interest I, f is presented as:

I (1 + I)
= (17)
(1 + ) 1
In this study, to simplify the mathematical model of TAC, only distillation columns, condensers,
reboilers and compressors are considered into the capital investment. The operating costs contain
thermal utilities (steam, CW) and electrical services. The annualization factor f=0.163 is considered,
which corresponds to a fixed rate of interest of 10% over a plant life span of 10 years. The annualized
operation period of plant is postulated to be 8000 hours.
The capital investment of distillation columns is estimated from column diameter and height. For
the diameter and height estimation the correlations of Rathore et al. [40] are used.
The diameter of the column (m) is estimated based on:

= [( 4
)()( + 1)(22.4)
1
( )( )( )]
1
273 3600
12
(18)

in which, V (m/s), D (kmol/h), RR, (K), P (atm) are average gas flow rate, overhead product molar
flow rate, reflux ratio, overhead temperature and pressure, respectively. The results of diameter are
rounded according to the national standard of P. R. China [41].
The estimation of average gas flow rate V (m/s) is:

= 0.761 ()
1

12
(19)

Height of the column is calculated based on:

= 0.61 ()

+ 4.27 (20)

where is the number of theoretical stages, and is stage efficiency. This study postulates = 0.8 in
all stages [42].
Based on diameter and height of column, the capital investment of column (US$) is
estimated as [42]:

= (101.91.066 0.802 1.55

3.18 + 4.7 ) ( )
803
274
(21)

The capital investment of condensers and reboilers considers the heat transfer area (A) of heat
exchangers, which are calculated as:

= () (22)

= () (23)

where , , , , are condenser duty, condenser overall heat transfer coefficient, reboiler duty,
reboiler overall heat transfer coefficient and logarithmic mean temperature difference, respectively. In

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this study, the overall heat transfer coefficients of condenser and reboiler are postulated to be 600/(
2 ). With the knowledge of the heat transfer area, the capital investment (US$) of condensers and
reboilers is conducted based on the following equations [42]:
0.65
= 101.3 3.29 ( )
803
274
(24)

0.65
= 101.3 3.29 ( )
803
274
(25)

The capital investment (US$) of compressors is estimated by using the correlations of

Couper et al. [43]:
= 9476.170.62 (26)
where (kW) is the electrical power of compressor. In this study, all the compressions are considered
isentropic, with the isentropic efficiency postulated to be 0.8.
In this study, the straight PBP, not including tax and depreciation, is used to evaluate retrofit
proposals. The definition of the straight PBP is given by [44]:

= (27)

where TIC is the total investment cost. and represent operational expenditure of the CDS
and ADS, respectively. In this study, TIC only focuses on the costly investment of the distillation
column and compressor since they are much more expensive than other auxiliaries. In the calculation
of operational expenditures, the reboilers are heated by steams with suitable band, leaving minimum
temperature difference = 20. The cold utility uses CW, and its inlet and outlet temperature are
25Cand 40C, respectively. The utilities for heating, cooling, and electrical power are converted into
equivalent standard oil consumption, using data in Table 2, and then multiply with unit price of
standard oil, obtaining .

3. Design of CDSs
The purpose of this section is to introduce state-of-the-art commercial CDSs to refine styrene
from the dehydrogenated crude feed (Table 3), obtaining benzene and toluene as byproducts and
recycling EB as reactant back to the reactor. The crude feed data considered is from a real styrene plant
running in Northern China [45]. Based on Peng-Robinson model [5] predicting thermodynamic
properties, the purification demand in Table 4 must be satisfied [45]. CDiSs 3 and 5, as suitable
grassroots process design options, are referred to CDS-I and CDS-II, respectively, facilitating 3E
analyses and exploring better retrofit alternatives.
Fig. 5 presents the CDS-I as well as the operating parameters for each column. This scheme
designates to separate benzene and toluene (as distillates) from EB and heavy components (as bottoms)
initially in toluene/EB column C1. Its overhead product isfurther refined in benzene/toluene column
C4, while bottom products of C1 are fed into the EB column C2, where recycle EB is obtained
overhead. The styrene mixtures, leaving from bottom of C2, are refined in styrene column C3 with a
flash tank connected to further strip styrene from tar. The first three columns C1, C2 and C3 are run
under vacuum to suppress styrene polymerization. The operational parameters, including operating
pressure, number of theoretical stages, and feed location etc., are carried out with reference to in-situ
styrene plants [45]. Energy consumptions and exergy losses are illustrated in Table 5, while column
configurations and economic evaluations are shown in Table 6.
CDS-II (Fig. 6) removes benzene, toluene and EB initially in EB/SM column C5. The recycle EB

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is obtained at bottom of toluene/EB column C6, and C6 top products enter benzene/toluene column C8
to obtain benzene and toluene. Crude styrene product, leaving from bottom of C5, is refined in styrene
column C7. It is noteworthy that CDS-II requires only two columns C5 and C7 running sub-ambient,
instead of three in CDS-I. Likewise, the relevant results are shown in Tables 5 and 6.
The results show that TAC and exergy loss in CDS-II are slightly less than that in CDS-I, and the
purification of benzene, EB and SM as well as the purified SM yield of the former are more
competitive than the latter. In addition, economic evaluations indicate operating costs are more
responsible for TACs than capital investments. Consequently, diminishing TAC through cutting down
energy consumptions is critical.
Despite energy consumptions of condensers measured in energy quantity are approximately equal
to that of the reboilers (Table 5), the CW consumption is less responsible for operating cost when
relevant heat loads are measured in standard oil. In other words, cutting down heat duty in reboilers is
the priority for saving operating expenditures. In Fig. 7, on the basis of standard oil, heat duties of
reboilers in CDSs are distributed in two pie charts. Obviously, columns C2 and C5, occupying ~65% of
energy depletion in each scheme, are energy dominator in CDS-I and CDS-II, respectively. It is
revealed the fact that separating EB from SM is the most difficult and energy intensive step among the
whole distillation processes. This fact is also predictable from the close-boiling nature of the EB/SM
system [1,46]. On the other hand, caused by high reflux ratio as well as large number of stages, C2 and
C5 are the most expensive columns amongst C1 to C8. As a result, in order to lower operational
expenses, it will be favored by applying energy efficient distillation operations on C2 and C5.
Particularly in this case study, sequence 5 only slightly performs better than 3. It is still
unpredictable on final TAC results when energy efficient technologies are introduced into the CDSs,
since their TAC difference is only ~2.5%. In the following design of ADSs, DED and HPD
configurations are applied on CDSs to explore better styrene distillation scheme.

4. Design of ADSs
4.1. Flowsheet description of ADSs
The purpose of designing ADSs is to reduce energy consumption in CDSs. As mentioned in Fig.
7, revamping on C2 and C5 is advantageous in reduction of operating cost as well as TAC. As a
consequence, DED and HPD configurations are applied on C2 and C5, respectively. For DED,
operating pressure of HPC should be chosen carefully to prevent styrene polymerization. While in
HPD, because overhead vapor of C2 and C5 is mainly EB, it is suitable to choose MVR instead of VC,
circumventing the procedure of introducing a new working fluid. In this study, only MVR type of HPD
is considered.
Advanced distillation configurations ADS-I-DED and ADS-I-HPD are based on the CDS-I. ADS-
I-DED (Fig. 8) is obtained by dividing C2 into a HPC C10 and a LPC C11, using C10 overhead vapor
to drive C11 bottom. Herein, the top pressure of C10 is identical to that of C2 to prevent styrene
polymerization. The C11 runs at 6.7kPa, creating sufficient temperature difference for heat integration.
In ADS-I-HPD (Fig. 9), the overhead vapor of EB column C15 is compressed to 80kPa to drive the
reboiler.
Likewise, ADS-II-DED (Fig. 10) revamps C5 into a HPC C18 running at 36kPa and a LPC C19
running at 6.7kPa, with operating pressure the same to that of C10 and C11. In ADS-II-HPD (Fig. 11),
the overhead vapor of EB/SM column C23 is compressed to 60kPa to drive the reboiler.

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4.2. Energy, exergy and economic analysis of ADSs

The calculation results of ADSs are shown in Tables 7 to 10. Energy consumptions of CDSs and
ADSs, based on energy quantity and quality, are illustrated in Fig. 12. It is concluded that, in terms of
energy quantity, scheme family II, including CDS-II, ADS-II-DED and ADS-II-HPD, requires much
less energy than scheme family I. However, when these energy consumptions are converted to primary
energy depletion, the former only slightly outperforms its counterpart. Taking CDS-I and CDS-II as
respective benchmark, ADS-I-DED, ADS-I-HPD, ADS-II-DED and ADS-II-HPD could lower
operating cost by 32.96%, 44.41%, 31.62% and 43.79%, respectively. Consequently, HPD
configuration outperforms DED in decrease of energy depletion. This is attributed to high heat pump
COP in ADS-I-HPD (11.41) and ADS-II-HPD (9.57).
Chemical/Petrochemical plants normally have an annual maintenance period of 10-14 days for
major repair and replacement [47]. The proposed retrofit from CDSs to ADSs is preferred to take place
within this period to avoid production loss. It is worth noting that the diameters of all columns in CDS-
I are same to the corresponding columns in ADSs. In practice, this means that the revamping of
existing plant is possible by reusing the existing columns. Specifically, for ADS-I-DED, a new column
C10 is required to facilitate the DED configuration, while for ADS-I-HPD, a new compressor is needed
to fulfill the retrofit. The corresponding PBPs for ADS-I-DED and ADS-I-HPD are 581 and 2459
hours, respectively. As for scheme family II, the retrofit of CDS-II to ADS-II-HPD no longer
requiresadditional column but a new compressor. The ADS-II-DED has 2 columns (C18 and C19) of
diameter 4.4 and 6.0m to form DED configuration (Table 10). The CDS-II has only one corresponding
column C5 with diameter of 6.8m. The existing column C5 can be used for retrofitting the C19, leaving
C18 as a new column needed to purchase. The PBPs for ADS-II-DED and ADS-II-HPD are 624 and
2912 hours, respectively. Notably, the attractive PBPs make such retrofit scenarios should be certainly
considered for revamping exiting styrene distillation plants.
The total exergy loss in CDSs and ADSs are shown in Fig. 13. The result indicates that the total
exergy losses in ADSs are always higher than those in CDSs. Compared with CDS-I and CDS-II,
ADS-I-DED, ADS-I-HPD, ADS-II-DED and ADS-II-HPD increase exergy loss by 27.36%, 58.35%,
25.07%, 63.53%, respectively. Exergy loss in scheme family II is slightly less than that in I, indicating
the former is more thermodynamic reversible than the latter.
As shown in Fig. 14, non-retrofit columns maintain approximately same exergy loss. In other
words, the higher exergy loss is due to the pressure varying in revamping columns. For example, C2 is
responsible for 313kW of exergy loss. C10, running under the same pressure as C2 but the feed
capacity halved, has 159kW of exergy loss, which is half of C2, indicating the extensive property of
exergy. While for C11, the lower pressure (6.7kPa) brings about three times of exergy loss (480kW)
compared to that in C10 (159kW). The higher exergy loss in C11 is attributed to: (1) low-pressure
operation reduces the separation difficulty, leading a lower minimum work required; (2) low-
pressure operation makes C11 a larger temperature difference between overhead and bottom (28.3C)
than that in C10 (14.9C), increasing total work supplied.
Likewise, for retrofit schemes using HPD, when heat pump is introduced, the exergy loss of C15
achieves to 851kW, which is much higher than that of the original C2 (313kW), because heat pump
consumes electrical power with high exergy compared to the low-quality steam utility.
Therefore, although energy efficient distillation could conclusively cut down considerable energy
consumption, it is also responsible for more exergy loss as punishment.
The TAC comparison of CDSs and ADSs is shown in Fig. 15. Because annualized capital costs

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are much less than annualized operating costs, additional capital investment in ADSs becomes less
responsible for TAC. Compared with corresponding CDS, ADS-I-DED, ADS-I-HPD, ADS-II-DED
and ADS-II-HPD can save TAC by 35.62%, 41.47%, 34.09% and 40.79%, respectively. In this case,
the TAC requirement for unit styrene production in CDS-I, CDS-II, ADS-I-DED, ADS-II-DED, ADS-
I-HPD and ADS-II-HPD are 0.0290US$/kg, 0.0282US$/kg, 0.0187US$/kg, 0.0186US$/kg,
0.0169US$/kg and 0.0167US$/kg, respectively (Fig. 15). It is concluded that the ADS-II-HPD is the
most competitive scheme amongst all these proposed styrene distillation schemes. Because the TAC
will vary under various economic models and international market, more detailed economic evaluation
should be considered during engineering design period.

4.3. Sensitivity analysis and optimization

In this study, sensitivity analysis is used to determine the optimal operational parameters of
columns in styrene distillation process [38]. Herein, the effect on revamping columns is considered of
the operating pressure and the number of theoretical stages, which are responsible for the significant
increase of exergy loss and potentially to be diminished.
Fig. 16 shows the effect of pressure on exergy loss distribution on trays of C2. In this case, other
operational parameters are maintained while the C2 top pressure is changed from 36kPa, the C2s
original pressure, to 6.7kPa, the C11s operating pressure. As a result, with the decrease in C2s
pressure, the exergy loss on each tray is increased. Exergy loss on each tray in rectifying section is
higher than that in stripping section, touching local maxima at feed stage. In other words, stripping
trays are more efficient than rectifying cousins and feed mixing with inner column streams causes more
thermodynamic irreversibility. Fig. 17 shows the monotonous relationship of exergy loss on trays in C2
and column top-bottom temperature difference versus operational pressure. The exergy loss on trays
increases from 349kW to 973kW when C2 top pressure is descended from 36kPa to 6.7kPa. This is
attributed to the ascending pressure decreases the top-bottom temperature difference. For example,
when top pressure is 36kPa, the temperature difference is 14.9C, while when the former decreases to
6.7kPa, the latter increases to 28.3C. Consequently, it is concluded that the exergy loss increase is
largely dependent on top-bottom temperature difference. In other words, increasing pressure benefits
decreasing tray exergy losses, explaining the higher exergy loss in LPCs C11 and C19.
Because the operating pressure of HPCs C2, C10 and C18 is restricted by the styrene stability, in
the aim of minimum exergy losses, 36kPa is an optimum. This is naturally induced that, in order to
minimize exergy losses, maintain styrene stability and construct DED setup, 6.7kPa of overhead
pressure in C11 and C19 is also an optimum.
Likewise, the effect of number of theoretical stages has influence on exergy loss. In order to lower
exergy loss on each tray, more stages are required in a column [38]. Taking C11 (a representative of
LPC in DED) as an example, because rectifying trays loss more exergy than stripping ones, an
increment of 10 theoretical stages is specified on rectifying section of C11 stepwise. As shown in Fig.
18, exergy loss on each tray in rectifying section decreases gradually. However, the total exergy loss on
trays increases from 480kW to 483kW when the number of theoretical trays varies from 92 to 142 (Fig.
19). On the other hand, the increase in number of theoretical trays brings in only a slight decrease in
reboiler energy consumption (Fig. 19), at the cost of higher capital investment as well as TAC.
Therefore, the best strategy is to maintain the current number of theoretical stages. This conclusion can
be extended to other LPCs.
For C15 and C23, as columns using MVR setup, their operational parameters are identical to C2

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and C5. Based on Eqs. (14) and (15), higher exergy in electrical power is the main reason for their
higher exergy loss (Fig. 14). In other words, varying column configuration has less impact on
decreasing exergy losses. However, it is noteworthy that higher exergy loss is not necessary correspond
to high TACs. In order to lower retrofit difficulty, the best strategy is to maintain the current pressure
and number of theoretical stages.

5. Conclusions
Significant energy savings as well as TAC reductions are obtained in the styrene distillation
schemes by the aid of DED and HPD. Compared to the corresponding CDS, ADSs with DED and HPD
can achieve energy savings up to 30% and 40%, respectively. Due to a synergistic effect of
considerably reducing energy costs and highly reusing most of the equipment, the PBPs of retrofit
designs are very attractive. Specifically, the proposed ADS-I-DED, ADS-I-HPD, ADS-II-DED and
ADS-II-HPD can save TAC by 35.62%, 41.47%, 34.09% and 40.79% compared to the CDSs, and
decrease unit styrene yield cost to 0.0187US$/kg, 0.0186US$/kg, 0.0169US$/kg and 0.0167US$/kg,
respectively. The results show both DED and HPD are attractive options in industrial implementation,
although the latter is slightly better than the former. This study also shows that although the ADSs can
reduce the energy requirements greatly, they can also cause higher exergy losses than the CDSs.
This study puts forward several retrofit strategies for styrene manufacture. The proposed schemes
are suitable for either grassroots process design of a new plant or retrofit of an existing one. Moreover,
the revamping procedure in this paper is general to be extended to other distillation systems.

Acknowledgement
The authors are grateful for the industrial consultant of Shandong Qilu Petrochemical Engineering
Co. Ltd, Zibo, Shandong, China.

Nomenclature

Acronyms

ABS acrylonitrile-butadiene-styrene
ADS advanced distillation scheme
CDiC conventionaldistillation column
CDiS conventional distillation sequence
CDS conventional distillation scheme
COP coefficient of performance
CW coolingwater
DED double-effect distillation
DNBP 2-sec-butyl-4,6-dinitrophenol
DWC dividingwall column
EB ethylbenzene
ED extractive distillation
HIDiC heat-integrated distillation column
HPC high-pressure column
HPD heat pump distillation

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LPC low-pressure column

MVR mechanical vapor recompression
NBP normal boiling point
PBP payback period
PS polystyrene
SAN styrene-acrylonitrile
SBC styrenic block copolymers
SBL styrene-butadiene latex
SBR styrene-butadiene rubber
SM styrene monomer
TAC total annualized cost
VC vapor compression
3E analyses energy, exergy and economic analyses

Roman letters

A heat transfer area

C cost
D overhead product molar flow rate
Dc diameter of the column
E exergy
f annualization factor
H enthalpy
Hc height of the column
m mass flow rate
Nt number of theoretical stages
OE operationalexpenditure
P pressure
Q heat
RR reflux ratio
S entropy
T temperature
TIC total investment cost
U overall heat transfer coefficient
V average gas flow rate
W work or power

Greek letters

stage efficiency

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Fig. 1. Styrene production process using EB dehydrogenation technology

Fig. 2. CDiSs for four-product separation

Fig. 3. CDiC and DED

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Fig. 4. VC and MVR

Fig. 5. Conventional design of CDS-I

Fig. 6. Conventional design of CDS-II

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Fig. 7. Energy consumption (based on standard oil) distribution of CDS-I and CDS-II

Fig. 8. Advanced design of ADS-I-DED

Fig. 9. Advanced design of ADS-I-HPD

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Fig. 10. Advanced design of ADS-II-DED

Fig. 11. Advanced design of ADS-II-HPD

Fig. 12. Energy consumption in quantity and standard oil

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Fig. 13. Total exergy loss of CDSs and ADSs

Fig. 14. Exergy loss distribution of CDSs and ADSs

Fig. 15. Total annualized cost and TAC requirement for unit styrene of CDSs and ADSs

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Fig. 16. The effect of pressure on exergy loss distribution on trays of column C2

Fig. 17. The effect of pressure on total exergy loss on trays and top-bottom temperature difference of column C2

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Fig. 18. The effect of number of theoretical stages on exergy loss distribution on trays of column C11

Fig. 19. The effect of number of theoretical stages on reboiler energy consumption and exergy loss of column C11

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Highlights
1. Energy efficient distillation technologies are applied on EB/SM column
2. Innovative retrofit scenarios with attractive payback periods are proposed
3. Significant reduction in energy consumption as well as total annualized cost
4. Optimization of advanced distillation schemes through sensitivity analysis
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Table 1. Molecular structures and NBPs of each component

Component Molecular structure NBP (C)

Benzene 80.1

Toluene 110.6

EB 136.2

SM 145.7

Styrene tar - >145.7

Table 2. The conversion of utilities into standard oil

Utility type Remark Utility unit Equivalent standard oil (kg)

Electrical power ----- kWh 0.26

Recycling CW ----- ton 0.10
Band 10.0MpaG steam 7.0MpaG P ton 92
Band 5.0MpaG steam 4.5MpaG P < 7.0 ton 90
Band 3.5MpaG steam 3.0MpaG P < 4.5 ton 88
Band 2.5MpaG steam 2.0MpaG P < 3.0 ton 85
Band 1.5MpaG steam 1.2MpaG P < 2.0 ton 80
Band 1.0MpaG steam 0.8MpaG P < 1.2 ton 76
Band 0.7MpaG steam 0.6MpaG P < 0.8 ton 72
Band 0.3MpaG steam 0.3MpaG P < 0.6 ton 66
Band <0.3MpaG steam ----- ton 55

Table 3. Dehydrogenated crude feed data

Component Mass flow rate (kg/h) Component Mass flow rate (kg/h)

Benzene 156.929 Alpha-methylstyrene 265.821

Toluene 597.781 Isopropylbenzene 0.641
EB 15327.930 N-propylbenzene 4.664
SM 26123.890 C10H14 42.024
DNBP 162.576 C13H12 71.360
P-xylene 1.861 C14H14 207.551
M-xylene 4.206 C18H14 393.408
O-xylene 0.303

Temperature 83.4C
Pressure 24kPa
Flow rate 43419.7kg/h

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Table 4. Purification demand on products

Product Purification demand (wt%)

SM 99.80
Recycle EB 98.00
Toluene 99.00

Table 5. Energy consumptions and exergy losses of CDS-I and CDS-II

Conventional distillation scheme CDS-I CDS-II

Total condenser duty (kW) 25,164 23,193

Standard oil (10 kg/s)
-3 37.10 34.18
Total reboiler duty (kW) 25,216 23,796
Standard oil (10 kg/s)
-3 641.91 628.21
Total standard oil (10 kg/s) -3 679.01 662.39
Total exergy loss (kW) 1,022 980

Table 6. Column configurations and economic evaluations of CDS-I and CDS-II

Conventional distillation scheme CDS-I CDS-II

Column C1 C2 C3 C4 C5 C6 C7 C8
Diameter (m) 3.0 6.0 4.6 0.3 6.8 1.4 4.4 0.3
Height (m) 43.92 74.42 31.72 30.96 74.42 43.92 31.72 30.96
Condenser area (m2) 234.55 380.90 217.88 1.66 506.87 28.84 197.84 1.41
Reboiler area (m ) 2 311.24 1,328.59 454.60 6.87 1,374.93 180.41 421.24 6.43
Column cost (US$) 66,941 219,793 81,944 4,194 252,341 29,252 78,058 4,194
Condenser cost (US$) 33,917 46,483 32,330 1,358 55,970 8,685 30,365 1,221
Reboiler cost (US$) 40,765 104,707 52,147 3,418 107,066 28,598 49,627 3,274
Total capital cost (US$) 687,998 648,651
Total operational cost (US$/year) 5,866,646 5,723,050
Total annualized cost (US$/year) 5,978,790 5,828,780

Table 7. Energy consumptions and exergy losses of advanced distillation scheme I

Advanced distillation scheme ADS-I-DED ADS-I-HPD

Total condenser duty (kW) 17,001 11,591

Standard oil (10-3kg/s) 25.06 17.10
Total reboiler duty (kW) 16,933 10,589
Standard oil (10-3kg/s) 430.12 267.79
Total electrical power (kW) 0 1,282
Standard oil (10 kg/s)
-3 0 92.59
Total standard oil (10 kg/s)
-3 455.18 377.48
Total exergy loss (kW) 1,291 1,619

Table 8. Column configurations and economic evaluations ofadvanced distillation scheme I

Advanced distillation scheme ADS-I-DED ADS-I-HPD

Column C9 C10 C11 C12 C13 C14 C15 C16 C17

Diameter (m) 3.0 4.4 6.0 4.6 0.3 3.0 6.0 4.6 0.3

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Height (m) 43.92 74.42 74.42 31.72 30.96 43.92 74.42 31.72 30.96
Condenser area (m ) 2 234.55 2.38 567.3 196.66 1.66 234.55 51.26 217.87 1.66
Reboiler area (m )
2 311.24 669.29 0 423.7 6.87 311.24 109.7 454.6 6.87
Column cost (US$) 66,941 156,265 219,793 78,058 4,194 66,941 219,793 81,944 4,194
Condenser cost (US$) 33,917 1,716 60,221 30,247 1,358 33,919 12,622 32,329 1,358
Reboiler cost (US$) 40,765 67,053 0 49,815 3,418 40,765 20,697 52,147 3,418
Compressor cost (US$) 0 0 0 0 0 0 800,810 0 0
Total capital cost (US$) 813,761 1,370,938
Total operational cost (US$/year) 3,716,237 3,261,427
Total annualized cost (US$/year) 3,848,880 3,484,890

Table 9. Energy consumptions and exergy losses of advanced distillation scheme II

Advanced distillation scheme ADS-II-DED ADS-II-HPD

Total condenser duty (kW) 15,196 9,555

Standard oil (10-3kg/s) 22.40 14.08
Total reboiler duty (kW) 15,800 8,577
Standard oil (10 kg/s)
-3 430.56 243.96
Total electrical power (kW) 0 1,582
Standard oil (10 kg/s)
-3 0 114.26
Total standard oil (10 kg/s)
-3 452.96 372.30
Total exergy loss (kW) 1,226 1,603

Table 10. Column configurations and economic evaluations ofadvanced distillation scheme II

Advanced distillation scheme ADS-II-DED ADS-II-HPD

Column C18 C19 C20 C21 C22 C23 C24 C25 C26
Diameter (m) 4.4 6.0 1.4 4.4 0.3 6.8 1.4 4.4 0.3
Height (m) 74.42 74.42 43.92 31.72 30.96 74.42 43.92 31.72 30.96
Condenser area (m2) 0.20 662.4 28.09 197.84 1.41 74.28 32.47 197.84 1.35
Reboiler area (m2) 702.71 0.00 181.97 425.52 6.43 113.83 173.26 421.24 6.43
Column cost (US$) 156,265 219,793 29,252 78,058 4,194 252,341 33,805 78,058 4,194
Condenser cost (US$) 343 66,604 8,537 30,365 1,221 16,063 9,381 30,365 1,187
Reboiler cost (US$) 69,211 0 28,759 49,954 3,274 21,200 27,856 49,627 3,274
Compressor cost (US$) 0 0 0 0 0 912,307 0 0 0
Total capital cost (US$) 745,830 1,439,658
Total operational cost (US$/year) 3,720,038 3,216,672
Total annualized cost (US$/year) 3,841,608 3,451,336