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Keywords: Energy-saving separation processes for ethylene glycol (EG) were investigated. These processes were a basic
Exergy analysis separation process (BSP), a first-grade energy-saving process (FEP), and a secondary energy-saving process (SEP).
Environment and Economic analysis The optimal operating parameters for each process were determined through multiple indicator analysis-based
Ethylene Glycol
energy, exergy, environment, and economic performance. The energy analysis results indicated that the steam
Energy-saving process
Multiple indicator analysis
consumption of EG dehydration decreased from 12.21% to 0.64%, and the steam consumption of EG refined
(EGR) decreased from 20.89% to 3.20%. Furthermore, the total steam consumption for the SEP was 30.49%
lower than that of the BSP. The exergy analysis showed that the 50.69% exergy destruction and the 15.64%
exergy loss recorded for the SEP were lower than those for BSP, which were 43.42% and 9.50% lower than for
the FEP. Both the flow rate and cost of waste gas emissions for the SEP were reduced by 31.18%. The total annual
cost (TAC), operating cost (OC), and equipment cost for the SEP were 2.95 × 106 $/y, 3.47 × 106 $/y and 4.06 ×
106 $/y, respectively. The TAC and OC of the SEP process decreased by 11.20% and 13.16%, respectively,
compared to the benchmarked BSP process. The novel SEP process shows high energy efficiency, low economic
cost, and low exergy loss, and has great industrial application prospects compared to the benchmarked process.
* Corresponding author.
E-mail address: sxy@qust.edu.cn (X. Sun).
https://doi.org/10.1016/j.seppur.2021.119787
Received 7 August 2021; Received in revised form 20 September 2021; Accepted 20 September 2021
Available online 24 September 2021
1383-5866/© 2021 Elsevier B.V. All rights reserved.
S. Xiang et al. Separation and Purification Technology 279 (2021) 119787
widely used to explore various novel industrial processes in previous water, and its formula is as follows:
studies [18-21]. In these studies, an energy analysis was used to evaluate
C2 H4 O + H2 O→CH2 OH − CH2 OH(MEG) (1)
the energy-saving effect of a novel process based on the amount of en
ergy consumed [22,23]. However, there will always be situations where During the reaction, ethylene oxide and ethylene glycol react to
high-quality energy changes to low-quality energy. An exergy analysis produce diethylene glycol (DEG) as a by-product. The equation is as
considers not only the amount of energy being processed, but also the follows:
qualities of the energy [23-27]. Environmental and economic analyses
MEG + C2 H4 O→HOCH2 − CH2 − O − CH2 CH2 OH(DEG) (2)
are increasingly viewed as fundamental for the improvement of existing
processes. In this way, companies are better able to cope with increasing Diethylene glycol reacts with ethylene glycol to produce very small
requirements and expectations from regulations and stakeholders [28- amounts of triethylene glycol (TEG). The equation is as follows:
31]. These analysis benchmarks have also been shown to be an effective
DEG + C2 H4 O→HOCH2 CH2 − O − CH2 CH2 − OCH2 CH2 OH(TEG) (3)
way to judge the effect of a new process, and the development of new
research techniques has meant that a combination of multiple analytical The contents of each component in the crude EG solution obtained by
methods has attracted increasing attention from researchers [32-41]. the above reactions are as follow (see Table 1).
There have been many studies on the purification of crude EG In this work, SR-POLAR was selected as base property method is
products, but the research was mainly limited to the simple process shown in Fig. S1. Different unit have different property method for
simulation stage. If a key unit energy saving and consumption reduction obtaining an accurate separation result. The thermodynamic model was
analysis of an EG production process can be carried out in combination established by judging the polarity of the mixture and verifying the
with multiple indicators, such as energy, exergy, environment, and experimental data [42]. The sigma profile from Fig. S2 showed that EG
economy, then the analysis will substantially improve the energy and mixture is polar system. The comparison experimental data and simu
quality of the process. lation results as shown in Table S1. The result demonstrated that SR-
In this study, we propose a novel energy-saving process for the pu POLAR is in good agreement with the experimental data for this system.
rification of crude EG by ethylene oxide-catalyzed hydration, in which
the optimal process parameters were optimized using a sensitivity
analysis, and the influences of key component operational variables 2.2. Process description
were analyzed. The optimal operating process was determined and
designed based on multi-objective analysis-based energy, exergy, envi The separation processes for the EG mixture were established using
ronment, and economic performance. the Aspen Plus program. The basic separation process (BSP) can be
2.1. Materials Name Formula Weight Boiling Point(℃) Mass Fraction (wt%)
2
S. Xiang et al. Separation and Purification Technology 279 (2021) 119787
divided into multi-effect evaporation (MEE), EG dehydration (EGD), EG EG mixture were established. The optimum parameters were determined
refining (EGR), and DEG refining (DEGR), as shown in Fig. 1. An EG by considering the minimum total annual cost (TAC) as the object
mixture containing 88.47% water was successively concentrated to trace function. The energy, exergy, economic, and environmental perfor
by the MEE and EGD processes, and water was produced by the C04 unit. mances of the different processes were analyzed.
In this BSP, triple-effect evaporation was selected to save steam in the
evaporation section. The steam at the top of C01 was used as the heat 3.1. Optimization of process parameters
source for C02, and the steam at the top of C02 was used as the heat
source for C03. The excess steam generates 0.35 MPa saturated steam It is considered that optimizing the operating variables is crucial
from flash evaporation. The bottom solution from C04 entered the EGR when attempting to improve separation efficiency. The sensitivity
unit and a 99.9% EG product was obtained. The DEG and TEG products analysis in Aspen Plus is a very useful tool for determining suitable
were obtained from the DEGR. In the first-grade energy-saving process initial parameters. To determine the optimal process parameters more
(FEP), waste heat at the top of C03 can be recycled as the heat source for accurately, the minimum TAC in this study was taken as the objective
C04. The rest of the process is based on the BSP and is shown in Fig. 2. In function and the main operating variables in this study, such as oper
the secondary energy-saving process (SEP), the temperature difference ating pressure, total number of stages (NT), the reflux ratio (RR), and
between the top of C05 (153.15 ℃) and the bottom (160.68 ℃) is 7.53 feed stage (NF) were optimized. The sequence diagram of parameter
℃, and the heat duty of the condenser is 2.00 MW. Heat pump distil optimization is shown as Fig. S6. However, the corresponding energy,
lation during the SEP was adopted to achieve high-value energy recov economy, and environmental parameters will change as the process
ery, as shown in Fig. 3. improves, and qualitative and quantitative analyses are essential to
The influence of pressure variations upon distillation operation is compare the differences among the different processes.
essential as has been reported in some literature [12,43-46]. In this
system, a mixture of H2O, EG, DEG, and TEG was fed into the evapo
3.2. Energy analysis
ration unit, which was operated under variable pressure. The operating
pressures for C01, C02, and C03 were set at 1105 kPa, 900 kPa, and 460
The material balance is the basis of the energy balance and it is
kPa, respectively, which is consistent with the experimental data in the
essential to first calculate the material balance of the system [24,41].
factory (Please see Fig. S3~S5, Table S2). SR-POLAR was selected as the
The material and energy balance can be expressed as follows. An energy
total thermodynamic physical property method. It considers the mixture
analysis of any unit in the process can be carried out based on Eqs. (1),
to be a polar system and operates at high pressure. The main units for
(2), and (3), which are shown in Table 3.
this research used in the Aspen Plus model are listed in Table 2. The ∑ ∑
main assumptions for this model are summarized as follows [47,48]: Massbalance : m˙in = ṁout (1)
∑ ∑
(1). All the physical and chemical changes in the process have Materialbalance : xin m
˙ in = xout ṁout (2)
reached equilibrium states;
(2). All the raw materials and products are the ideal mixture ∑ ∑ ∑
Energybalance : Ẇ + m˙in hin = Q̇ + m˙out hout (3)
(3). In the process, the reference temperature t0 and the reference
pressure p0 are 25 ℃ and 101.325 kPa, respectively.
where ṁ is the mass flow rate, x is the mass fraction of the key
(4). The condition of the process is steady-state;
component, Q̇ is the heat duty, Ẇ is the power and h is the specific
(5). The kinetic energy and potential energy in the process are
enthalpy [49,50].
ignored.
In this study, three energy-saving processes for the separation of an An exergy analysis is used to determine the amount of energy that
can be converted into work in different states. For a steady system,
3
S. Xiang et al. Separation and Purification Technology 279 (2021) 119787
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S. Xiang et al. Separation and Purification Technology 279 (2021) 119787
Table 2 Table 3
Types and descriptions of the units of EG refining process. Mass/Material/Energy equations for each components of the SEP.
Unit Type Description Unit Equations
C01 Distillation column Multi-level evaporation column 1 M01 ṁ30 +ṁ23 =ṁ24 ṁ30 x30 +ṁ23 x23 =ṁ24 x24
C02 Distillation column Multi-level evaporation column 2 P01 ẆP01 = ṁ19 h19 − ṁ18 h18
C03 Distillation column Multi-level evaporation column 3
P02 ẆP02 = ṁ30 h30 − ṁ29 h29
C04 Distillation column Dehydration column
C05 Distillation column Refinery column P03 Ẇp03 = ṁ23 h23 − ṁ20− 1 h20− 1
C06 Distillation column Cyclical column P04 ẆP04 = ṁ25 h25 − ṁ21 h21
C07 Distillation column Refinery column
P05 ẆP05 = ṁ31 h31 − ṁ27 h27
F01 Flash flash steam generator1
F02 Flash flash steam generator2 V1 ṁ8 h8 =ṁ11 h11
V1 Valve Throttle valve 1 V2 W1hW1 = ṁS4 hS4
V2 Valve Throttle valve 1
F01 ṁ6 + ṁ7 = ṁ8 + ṁ9
M01 Mixer Flow mixer
COMPR Compressor Gas compressor ṁ6 x6 +ṁ7 x7 =ṁ8 x8 + ṁ9 x9
E01 Multi-stream heat exchanger Dehydration column condenser Q̇F01 =ṁ6 h6 + ṁ7 h7 − ṁ8 h8 − ṁ9 h9
E02 Multi-stream heat exchanger Dehydration column condenser F02 ṁ10 + ṁ11 + ṁ15 = ṁ12 + ṁ13
E03 Multi-stream heat exchanger Dehydration column condenser
ṁ10 x10 + ṁ11 x11 + ṁ15 x15 = ṁ12 x12 + ṁ13 x13
E04 Multi-stream heat exchanger Stream heater
E05 Multi-stream heat exchanger Product condenser QF02 =ṁ10 h10 + ṁ11 h11 + ṁ15 h15 -ṁ12 h12 -ṁ13 h13
E06 Multi-stream heat exchanger Stream heater C01 ṁ1 + ṁH2 O− 1 = ṁ2 + ṁ3
E07 Multi-stream heat exchanger Stream heater ṁ1 x1 + ṁH2 O− 1 xH2 O− 1 =ṁ2 x2 + ṁ3 x3
E08 Multi-stream heat exchanger Product condenser
Q̇C01 =ṁ2 h2 + ṁ3 h3 − ṁ1 h1 − ṁH2 O− 1 hH2 O− 1
P01 Pump Feeding pump
P02 Pump Circulating pump C02 ṁ3 + ṁH2 O− 2 = ṁ4 + ṁ5
P03 Pump Circulating pump ṁ3 x3 + ṁH2 O− 2 xH2 O− 2 =ṁ4 x4 + ṁ5 x5
P04 Pump Discharge pump
Q̇C02 =ṁ4 h4 + ṁ5 h5 − ṁ3 h3 − ṁH2 O− 2 hH2 O− 2
P05 Pump Feeding pump
C03 ṁ5 + ṁH2 O− 3 = ṁ14 + ṁ16
S01 Splitter Splitter of stream W2
S02 Splitter Splitter of stream 22 ṁ5 x5 + ṁH2 O− 3 xH2 O− 3 =ṁ14 x14 + ṁ16 x16
Q̇C03 =ṁ14 h14 + ṁ16 h16 − ṁ5 h5 − ṁH2 O− 3 hH2 O− 3
S02 ṁ22 = ṁS1 +ṁ22− 1 ṁ22 x22 = ṁS1 xS1 +ṁ22− 1 x22−
0.568 kW/K··m2, respectively [56]. The equipment materials were 1
assumed to be carbon steel, the payback period was set to 5 years, and
the annual operating time was 8000 h. A value of 1468.6 for M&S has
environmental performance of different heating methods. The calcula
been reported in some papers [57-59]. The plate efficiency was set at
tion formula is as follows [62]:
0.75 and the plate spacing was 0.61 m. Where Wpump is the power con
sumption of the pump, then Cpump is 0.25 when Wpump is in the range 0.02 MGAS = aGAS ∙MCoal (14)
~ 0.3 kW, 0.45 when Wpump is in the range 0.3 ~ 20 kW, and 0.84 when
Wpump is in the range 20 ~ 200 kW. The cost calculation formulas for MCoal =
(QR + QPR )N
each piece of equipment are listed in Table 4. Qstandard ηcoal,trans
where aGAS is the emission conversion factor for standard coal, MCoal is
3.5. Environmental analysis the mass of the standard coal, ηcoal,trans is the coal transfer efficiency and
is assumed to be the isentropic efficiency, and Qstandard is the calorific
Environmental performance analyses of systems are also important
value of standard coal, which is equal to 29307.6 kJ/kg [62].
because increasing attention is being paid to environmental protection.
The cost of exhaust gas emissionZGAS is calculated by the following
Emissions of CO2, SO2, and NOx are considered indicators of the
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S. Xiang et al. Separation and Purification Technology 279 (2021) 119787
Table 4
the cost calculation formula of each equipment.
Unit Equations Reference
formula [62].
Fig. 4. T-x-y of DEG/TEG mixture.
ZGAS = MGAS ∙cGAS (16)
where cGAS refers to the unit damage emission cost. The aGAS and cGAS
constants for CO2, SO2, and NOx are listed in Table 5.
Table 5 Fig. 6. Variations in water content at the bottom of C03 and TAC.
aGAS and cGAS of CO2, SO2 and NOx.
Name aGAS (kg/kg) cGAS taking into account utilities and operations, it can be seen from Fig. S7
and Fig. S8. When the water content at the bottom of C03 is fixed, the
CO2 2.493 5.209 steam consumption of the C01 reboiler can be lowered by reducing the
SO2 0.075 0.373
NOX 0.0375 0.745
operating pressure of the evaporators. As can be seen from Fig. 7, the
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S. Xiang et al. Separation and Purification Technology 279 (2021) 119787
Fig. 7. PC01 relationship with the temperature of C01, C02, and C03, and mass flow rate of the total steam at different PC01 values.
C01 pressure decreased from 1580 kPa to 1105 kPa and the pressure at with the sensitivity analysis. The specific process parameters were
the top of C02 decreased from 1100 kPa to 900 kPa, which meant that optimized and determined as shown in Table 6.
1.14 t/h of total steam consumption was saved. In this study, PC01 and
PC02 were 1105 kPa and 900 kPa, respectively. 4.2. Energy analysis results
In the above analysis, the optimum parameters were determined by
taking the minimum TAC as the object function. It was then combined The energy analysis in this study can be used as an important guide
for determining the efficiency of the energy-saving process. Energy
consumption by the different processes was analyzed and the results
Table 6 from Fig. 8 showed that the total steam consumption of the SEP was
Main operating parameters of different processes.
12.81 t/h, which was 30.49% lower than that of the BSP. According to
Unit BSP FEP SEP the steam consumption values for each piece of equipment in the BSP,
F(kg/h) 39,05038384 39,05038384 39,05038384 the steam consumption by MEE, EGD, and EGR, the key components of
NT1 5 5 5 the energy saving process, reached 95.60%. Therefore, there is great
NT2 5 5 5 potentiality of energy conservation in EGD and EGR. After imple
NT3 18 18 18
NT4 21 21 21
mentation of the energy-saving process, energy consumption by EGD
NT5 21 21 21 and EGR in the SEP was reduced to 0.64% and 3.20%, respectively. It
NT6 5 5 5 can be seen from the changing process for the energy-saving effect that
NT7 34 34 34 the SEP can save substantial amounts of energy, heat pump for SEP can
RR1 0.1497 0.1497 0.1497
get better energy saving effect.
RR2 0.1546 0.1546 0.1545
RR3 0.1395 0.1395 0.1395
RR4 0.0653 0.1283 0.1285 4.3. Exergy analysis results
RR5 8.2959 8.2959 0.9218
RR6 1.1525 1.1688 1.1549
Exergy analysis is an effective way to evaluate the potential for en
RR7 0.3298 0.3302 0.3285
QR1(kW) 6022.95 6022.95 6022.95 ergy savings. Many researchers have used this method to optimize the
QR4(kW) 1218.08 63.40 44.45 energy utilization efficiency of a process, which can provide a reference
QR5(kW) 2080.07 2079.90 219.78 for energy-saving processes [63-67]. The exergy destruction and loss
QR6(kW) 321.82 325.14 353.12 values for the different processes were compared in this study. The
QR7(kW) 79.77 79.77 80.05
exergy analysis shown in Fig. 9 indicates that the exergy destruction
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S. Xiang et al. Separation and Purification Technology 279 (2021) 119787
values for the BSP, FEP, and SEP were 2460.56 kW, 2144.50 kW, and
1213.38 kW, and the exergy losses were 4652.2 kW, 4336.18 kW, and
3924.46 kW, respectively. The exergy destruction and losses for the SEP
and BSP were 50.69% and 15.64%, respectively. The above results
suggest that the SEP is superior to the BSP and FEP, and that the
available energy from EGD and EGR for the SEP were recycled effi
ciently. This conclusion is reflected in the exergy flow diagram shown in
Fig. 10.
8
S. Xiang et al. Separation and Purification Technology 279 (2021) 119787
Fig. 13. Gas emission cost analysis when the SEP is operated for different
lengths of time.
Fig. 11. Gas emission and emission cost of different processes.
characteristics of the BSP, FEP, and SEP, along with other processes,
processes. It can be seen that the SEP decreases these factors by 31.18%
were comprehensively analyzed based on energy, exergy, environment,
compared to the BSP when the annual operating time is the same. The
and economy. The results are as follows:
analyzed results demonstrate the superior performance of the SEP with
regards to emissions and emission costs. The emissions and emission
(1) The multi-objective analysis indicated that the variations in
costs of the SEP at different operating times were also studied in order to evaporated water, water content, and top temperature of the
observe the change relationship between operating time and environ
column are key components of the variable analysis. In this study,
mental factors more intuitively during the most successful process. the optimal parameters were determined by the minimum TAC.
Fig. 12 and Fig. 13 show that reducing the operating cycle gradually
(2) The energy analysis showed that the total steam consumption of
decreases the emissions and emission costs. In summary, the SEP has a the BSP, FEP, and SEP were 18.43 t/h, 16.25 t/h, and 12.81 t/h,
better environmental performance than the other processes because
and total steam consumption by the SEP was 30.49% lower than
CO2, NOx, and SO2 emissions are linked to energy consumption. that of the BSP. The energy consumption proportion due to EGD
and EGR in the SEP decreased to 0.64% and 3.20%, respectively.
4.5. Economic analysis results (3) The exergy analysis showed that the exergy destruction values for
the BSP, FEP, and SEP were 2460.56 kW, 2144.50 kW, and
An economic analysis is an important method that is often used to 1213.38 kW, and the exergy losses were 4652.2 kW, 4336.18 kW,
evaluate the economic performance of processes [70,71]. In this study, and 3924.46 kW, respectively. The exergy destruction and exergy
the TAC for different processes was calculated using the Douglas model losses of 50.69% and 15.64% for the SEP were lower than those
and the results are shown in Fig. 14 and Fig. 15. The TACs of the BSP, for the BSP, respectively, which were 43.42% and 9.50% lower
FEP, and SEP were 4.57 × 106 $/y, 4.36 × 106 $/y, and 4.06 × 106 $/y, than those for the FEP.
respectively. The analysis of equipment investment showed that the SEP (4) The environment analysis showed that compared to the bench
had the highest cost at 2.95 × 106 $/y because of the newly added marked BSP, the emissions and emission costs of the novel SEP
compression system. However, the operating cost was significantly were significantly reduced by approximately 31.18%.
lower. The TAC of the SEP was 4.06 × 106 $/y, which was equivalent to (5) The results of the economic analysis showed that the TAC of the
88.80% of the BSP and was 6.57% lower than that of the FEP. The results novel SEP process was 11.20% and 6.57% lower than that of the
above demonstrate that the economic performance of the SEP was su benchmarked BSP and FEP, respectively. As an important energy-
perior to the other processes. saving technology, the commercial promotion and application of
this novel SEP process has strong development prospects.
5. Conclusion
6. Notes
In this study, the separation process for an EG mixture was studied,
and the efficient purification of EG, TEG, and DEG was realized. The The authors declare no competing financial interest.
We declare that we have no financial and personal relationships with
other people or organizations that can inappropriately influence our
work, there is no professional or other personal interest of any nature or
kind in any product, service and/or company that could be construed as
influencing the position presented in, or the review of, the manuscript
entitled.
Fig. 12. Gas emission rate analysis when the SEP is operated for different
lengths of time.
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S. Xiang et al. Separation and Purification Technology 279 (2021) 119787
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