processes

Article
Comparative Investigation of Different CO2 Capture
Technologies for Coal to Ethylene Glycol Process
Yanqing Ma 1 , Yitao Liao 1 , Yi Su 1 , Baojie Wang 1 , Yong Yang 2 , Dong Ji 2 , Hongwei Li 2 , Huairong Zhou 2 and
Dongliang Wang 2, *

1 Lanzhou Petrochemical Research Center, Petrochemical Research Institute, PetroChina,

Lanzhou 730060, China; [email protected] (Y.M.); [email protected] (Y.L.);
[email protected] (Y.S.); [email protected] (B.W.)
2 School of Petrochemical Engineering, Lanzhou University of Technology, Lanzhou 730050, China;
[email protected] (Y.Y.); [email protected] (D.J.); [email protected] (H.L.); [email protected] (H.Z.)
* Correspondence: [email protected]; Tel.: +86-0931-7823215

Abstract: The coal to ethylene glycol (CTEG) process has drawn much attention due to the serious
conflict between supply and demand of ethylene glycol in China. However, it is inevitably accompa-
nied by the problem of high CO2 emissions. Carbon capture is one of the most promising potential
effective ways to address this issue. However, the CTEG process, integrated with carbon capture
technology, will lead to energy and economic penalties. Thus, a comprehensive evaluation of CTEG
process with different CO2 capture technologies is urgently needed. This study analyzed the technoe-
conomic performance of four CO2 capture alternatives for the CTEG process: Rectisol, mono-ethanol
amine (MEA), chilled ammonia process (CAP) and dimethyl carbonate (DMC) technologies. Results
show the energy consumption of CO2 capture of the Rectisol process is the lowest, 1.88 GJ/tCO2 ,



followed by the DMC process, 2.10 GJ/tCO2 , the CAP process, 3.64 GJ/tCO2 , and the MEA process,

 5.20 GJ/tCO2 . The CO2 capture cost of the Rectisol process is lowest, CNY 169.5/tCO2 , followed by
Citation: Ma, Y.; Liao, Y.; Su, Y.; the DMC process, CNY 193.2/tCO2 , the CAP process CNY 232.6/tCO2 , and the MEA process CNY
Wang, B.; Yang, Y.; Ji, D.; Li, H.; Zhou, 250.5/tCO2 . As the Rectisol technology has the best comprehensive performance, it is the best option
H.; Wang, D. Comparative for CTEG industry in comparison with the MEA, CAP, and DMC technologies.
Investigation of Different CO2
Capture Technologies for Coal to Keywords: CO2 capture; performance analysis; coal to ethylene glycol; acid gas removal;
Ethylene Glycol Process. Processes process simulation
2021, 9, 207. https://doi.org/
10.3390/pr9020207

Received: 25 December 2020

1. Introduction
Accepted: 18 January 2021
Published: 22 January 2021
Ethylene glycol (EG) is one of the basic raw material of many chemical products.
However, its domestic production capacity cannot meet the market demand in China.
Publisher’s Note: MDPI stays neutral
Improving the production capacity of ethylene glycol is of great significance to China’s
with regard to jurisdictional claims in
economic development. The traditional ethylene glycol production route is based on the
published maps and institutional affil- petroleum-based route, which consists of three steps: first, ethylene is first produced from
iations. petroleum; then, the produced ethylene is oxidized to produce ethylene oxide; finally, the
ethylene oxide is hydrated to produce ethylene glycol [1]. Thus, the production scale of this
route cannot be greatly increased because it depends on the scale of the supporting ethylene
plant. Facing with the energy structure of rich coal and less oil, coal to ethylene glycol
Copyright: © 2021 by the authors.
(CTEG) technology is drawing more and more attention in China. In 2016, the National
Licensee MDPI, Basel, Switzerland.
Development and Reform Committee of China pointed out that the annual production
This article is an open access article
capacity of China’s coal-based ethylene glycol will be more than 15.25 million tons by
distributed under the terms and the year 2020 in the "13th Five-Year" Development Guide for Modern Coal Chemical
conditions of the Creative Commons Industry [2]. It also shows the aggressive ambitions of Chinese government to large-scale
Attribution (CC BY) license (https:// and efficient development of the CTEG industry.
creativecommons.org/licenses/by/ The first set of 0.2 million t/y CTEG projects was built in Tongliao in 2009. By 2018,
4.0/). 22 sets of CTEG plants had been successfully operated, and the total production capacity is

Processes 2021, 9, 207. https://doi.org/10.3390/pr9020207 https://www.mdpi.com/journal/processes

 The first set of 0.2 million t/y CTEG projects was built in Tongliao in 2009. By 201
Processes 2021, 9, 207
22 sets of CTEG plants had been successfully operated, and the total production 2 of 19
capac
is more than 4.42 million t/y [3]. However, the CTEG technology is inevitably accomp
nied by high CO2 emissions as shown in Figure 1. It is mainly caused by the difference
hydrogen–carbon (H/C) t/y
more than 4.42 million ratio
[3]. between
However, the raw coaltechnology
CTEG and ethylene glycol
is inevitably product. Name
accompanied
raw coal is rich
by high CO2 in carbonasand
emissions shown lessinhydrogen,
Figure 1. Itwhile
is mainlyethylene
caused glycol is rich inofhydrog
by the difference
hydrogen–carbon (H/C) ratio between raw coal and ethylene
and less carbon. In fact, the H/C ratio of raw coal is less than 1.0, resulting in glycol product. Namely, rawthat of t
coal is rich in carbon and less hydrogen, while ethylene glycol is rich in hydrogen and less
gasified gas is less than 1.0 [4]. However, it is required to be 2.0 for synthesizing ethyle
carbon. In fact, the H/C ratio of raw coal is less than 1.0, resulting in that of the gasified
glycol. Thus,
gas is lessthere is a[4].
than 1.0 big difference
However, of H/C ratio
it is required between
to be 2.0 the input
for synthesizing and output
ethylene glycol. of CTE
process. As
Thus, a result,
there the CTEG
is a big difference process
of H/C is inevitably
ratio between the input required
and output toofadd
CTEG a process.
water gas sh
As a result, the CTEG process is inevitably required to add
(WGS) unit for adjusting and increasing the H/C ratio of syngas. A large amounta water gas shift (WGS) unit for of C
adjusting
generated by and
the increasing
water gastheshiftH/Creaction,
ratio of syngas. A largecannot
however, amountbe of CO 2 generated
fixed by the
or reused. Thereby
water gas shift reaction, however, cannot be fixed or reused. Thereby, it causes the CTEG
causesprocess
the CTEG process
to suffer from highto suffer from high CO2 emission.
CO emission.
2

Figure 1. Figure 1. Schematic

Schematic diagramdiagram of high
of the the high
COCO 2 emission reasons
2 emission reasons for coal
for to ethylene
coal glycolglycol
to ethylene (CTEG)(CTEG)
process. process.

Carbon dioxide is one of the greenhouse gases causing global warming, which con-
Carbon dioxide
tributes more than is
60%one of the
of the greenhouse
enhanced gases
greenhouse causing
effect, global CO
thus reducing warming,
2 emissions
which co
tributes
hasmore
become than
one 60%
of theoftopthe enhanced
goals greenhouse
of the world effect,after
[5]. In addition, thusthe reducing
water gasCO 2 emissio
shift
unit, the shifted syngas contains a large amount of CO , which has a
has become one of the top goals of the world [5]. In addition, after the water gas shift un
2 significantly negative
impact on subsequent ethylene glycol synthesis and refining (EGSR) unit, for example,
the shifted syngas contains a large amount of CO2, which has a significantly negati
catalyst poisoning. Thus, high CO2 emissions of the CTEG process will inevitably hinder its
impact on subsequent ethylenedevelopment.
widespread use and sustainable glycol synthesis and refining
CO2 capture is regarded(EGSR) unit,
as the most for examp
promis-
catalyst
ing poisoning. Thus,CO
strategy to mitigate high CO2 emissions
2 emissions and spearheadof the CTEG
efforts process
to alleviate willchange
climate inevitably
[6]. hind
Currently, lots
its widespread useof CO
and2 capture technologies
sustainable have been developed,
development. CO2 capture suchis as regarded
Rectisol, MEAas the mo
(mono-ethanol amine), CAP (chilled ammonia process) and DMC
promising strategy to mitigate CO2 emissions and spearhead efforts to alleviate clima (dimethyl carbonate)
technologies [7]. However, CTEG process involving CO2 capture will simultaneously lead
change [6]. Currently, lots of CO2 capture technologies have been developed, such
to energetic and economic penalties. Thus, it is meaningful work to analyze the effects of
Rectisol, MEA
different CO(mono-ethanol amine), CAP (chilled ammonia process) and DMC (dim
2 capture technologies on the performance of the whole CTEG process.
thyl carbonate)
Previoustechnologies
works are focused [7].onHowever, CTEG
the new catalysts’ process involving
development, modeling and CO 2 capture w
simula-
tion, thermodynamic
simultaneously lead to analysis,
energetic economic analysis, conceptual
and economic penalties.design,
Thus,and optimization
it is meaningful of work
the CTEG process. For example, [8] systematically investigated the influence of low-cost
analyze the effects of different CO2 capture technologies on the performance of the who
dextrin coating on the performance of Cu–SiO2 catalysts for the vapor-phase hydrogenation
CTEGofprocess.
dimethyl oxalate to ethylene glycol. Wei et al. [9] focused on the improved design of the
Previous
reactors and works are focused
separation strategies,on the proposed
which new catalysts’ development,
a new four-stage fixed bedmodeling
tube-type and si
CO coupling reactor (CCR). Yang et al. [10,11] developed
ulation, thermodynamic analysis, economic analysis, conceptual design, and two coke oven gas-assisted coaloptimiz
tion of the CTEG process. For example, [8] systematically investigated the the
to ethylene glycol processes to improve the technoeconomic performance and reduce influence
CO2 emissions of the conventional CTEG process. However, little work has studied the
low-cost dextrin coating on the performance of Cu–SiO 2 catalysts for the vapor-pha
effects of different CO2 capture technologies on the performance of the CTEG process.
hydrogenation of dimethyl oxalate to ethylene glycol. Wei et al. [9] focused on the i
proved design of the reactors and separation strategies, which proposed a new four-sta
fixed bed tube-type CO coupling reactor (CCR). Yang et al. [10,11] developed two co
oven gas-assisted coal to ethylene glycol processes to improve the technoeconomic p
formance and reduce the CO2 emissions of the conventional CTEG process. Howev
little work has studied the effects of different CO2 capture technologies on the perfo
mance of the CTEG process.
Processes 2021, 9, 207 3 of 19

However, there is a lot of literature on another coal-gasification-based process, in-

tegrated gasification combined cycle (IGCC) process. For example, Rezvani et al. [12]
analyzed the techno-economic characteristics of IGCC process with four different capture
technologies. Giuffrida et al. [13] focused on the thermodynamic performance of two IGCC
systems with post-combustion CO2 capture by chemical absorption to evaluate two dif-
ferent strategies of coal-derived gas clean-up. Shi et al. [14] developed a new integrated
gasification combined cycle (IGCC) plant with CO2 capture to achieve deep reductions
in emissions of CO2 . Comparing the IGCC process with CO2 capture, only part of the
syngas produced from coal gasification unit is fed into the water gas shift unit in the CTEG
process, which is usually less than 50% of the total syngas. Therefore, a considerable part
of the CO gas is kept in the input gas of the acid gas removal unit. Since CO is the raw
material for the synthesis of ethylene glycol, in addition to the high CO2 removal ratio, the
CTEG process with different CO2 capture technologies must also have a high CO recovery
ratio. However, it does not need this in the IGCC process. On the other hand, the mole
fraction of CO2 in the input gas of acid gas removal unit of CTEG process is lower than
that of IGCC by 10–20%, which means the carbon capture in CTEG process may be more
complicated than the IGCC process [15]. In summary, different from the IGCC process, the
carbon capture in the CTEG process is characterized by higher CO and lower CO2 .
As to a project investor or decision maker, the technoeconomic performance of dif-
ferent alternative technologies is one of the most concerned and important performances
when they attempt to select the best technology solution. For example, Pettinau et al. [16]
conducted a techno-economic comparison between different technologies for CO2 -free
power generation from coal. In our previous work [17], a thermodynamic and techno-
economic analysis of the CTEG process with different gasifiers was conducted to make
the appropriate and reasonable decision and choice of efficient, economical and cleaner
coal gasifier technologies. However, not many literature has been reported to the optimal
selection of CO2 capture technology for the CTEG process through technical and economic
analysis. Therefore, the technoeconomic performance of CTEG process with different CO2
capture methods is conducted and compared to find the optimal CO2 capture way for
this process.
To achieve mid to long-term CO2 reduction targets, cost effective CO2 capture from
CTEG plants needs to be evaluated, keeping in view of China’s growing demand of ethylene
glycol. This study is focused on systematically analyzing and comparing the CTEG process
with different CO2 capture absorption technologies, i.e., Rectisol, MEA, CAP and DMC
technologies. The main contributions of this work are: (1) the detailed model of the CTEG
process with different CO2 capture technologies (i.e., Rectisol, MEA, CAP and DMC) is
established; (2) the energy consumption of CO2 capture and the whole system is analyzed
on the basis of the energy balance; (3) the total capital investment, total production cost
and internal rate of return of the above CTEG processes are compared to demonstrate
their economic advantages and competitiveness; (4) the comprehensive performance of
these processes is assessed to seek the most promising CO2 capture technology for the
CTEG process.

2. Process Description and Modeling

A conventional CTEG process consists of six units: air separation unit (ASU), coal
gasification (CG), water gas shift, acid gas removal (AGR), CO and H2 separation (CHS),
and ethylene glycol synthesis and refinery units, as shown in Figure 2. The models of
these units are developed using the Aspen Plus simulator (Version 11.0), which is a large-
scale general process simulation software for the design, simulation and optimization of
chemical industry. The details of the modeling and simulation of these units are explained
as follows.
es 2021, 9, x FOR PEER REVIEW 4
Processes 2021, 9, 207 4 of 19

Figure 2. Schematic diagram of the CTEG process with different CO capture technologies.
Figure 2. Schematic diagram of the CTEG process with different2 CO2 capture technologies.
2.1. Air Separation Unit
2.1. Air Separation
Due to theUnit
high oxygen consumption of coal-based chemical industries, the mature
and widely used cryogenic air separation technology is selected in this work. The Peng–Rob
Due to the high oxygen consumption of coal-based chemical industries, the ma
method is selected as the physical property method of this unit. After cleaning, the air is
and widely usedinto
compressed cryogenic air separation
an air separation technology
column to separate O2 . The is selected
four-stage air in this work.
compressor and The P
Rob method is selected
the inter-stage as theare
cooler models physical property
used to simulate method of
the intercooling this unit.equipment.
compression After cleaning
As a result, the concentration of the output oxygen is about 95 mol%,
air is compressed into an air separation column to separate O2. The four-stage which is used as an air c
oxidant in the coal gasification unit.
pressor and the inter-stage cooler models are used to simulate the intercooling comp
sion equipment. As a Unit
2.2. Coal Gasification result, the concentration of the output oxygen is about 95 m
which is used as an
The coal oxidantisina the
gasification coalprocess
complex gasification
involvingunit.
a series of physical and chem-
ical interactions as shown in Table S1 in the Supplementary Material [18]. In this work,
Huolinhe lignite is selected as the feedstock of the coal gasification unit, and the dry pul-
2.2. Coal Gasification Unit
verized coal gasification technology, Choren coal gasifier (CCG), is adopted. The Peng–Rob
The coal isgasification
method selected as theisphysical
a complex process
property methodinvolving
of CG unita [19].
series of pretreatment,
After physical and chem
coal is fed into the gasifier to produce syngas. For modeling, a yield reactor, a continuous
interactions as shown in Table S1 in the Supplementary Material [18]. In this work,
stirred tank reactor, and a Gibbs reactor are used to model the coal drying, pyrolysis, as
olinhe well
lignite is selected
as gasification and as the feedstock
combustion of the coalThe
stages, respectively. gasification unit, and
detailed simulation the dry
model
verizedof coal gasification
the gasifier is shown technology, Choren
in Figure S1 in the coal gasifier
Supplementary (CCG),
Material. is adopted.
After recovering the The P
waste heat, the crude syngas is sent to the water gas shift unit to
Rob method is selected as the physical property method of CG unit [19]. After adjust the hydrogen to pret
carbon ratio. More detailed information of the modeling and simulation of coal gasification
ment, coal is fed into the gasifier to produce syngas. For modeling, a yield reactor, a
unit can be found in our previous work [20].
tinuous stirred tank reactor, and a Gibbs reactor are used to model the coal drying
rolysis, as well as gasification and combustion stages, respectively. The detailed sim
tion model of the gasifier is shown in Figure S1 in the Supplementary Material. A
recovering the waste heat, the crude syngas is sent to the water gas shift unit to adjus
hydrogen to carbon ratio. More detailed information of the modeling and simulatio
coal gasification unit can be found in our previous work [20].

2.3. Water Gas Shift Unit

Processes 2021, 9, 207 5 of 19

2.3. Water Gas Shift Unit

The H2 /CO ratio of the crude syngas produced by the coal gasification unit is far
from the requirements of ethylene glycol synthesis reaction. Therefore, the H2 /CO ratio
has to be adjusted to be about 2.0 by the water gas shift reaction, as shown in Equation (1).
Two equilibrium reactors are used to model this reaction for a high conversion of syngas [21].
In addition, a number of coolers and heat exchangers are used to generate saturated steam.
The shifted syngas is finally cooled to 40 ◦ C and is then fed into the acid gas removal
unit [21]. The whole simulation flowsheet and key operational parameters of the WGS unit
are shown in Figure S2 and Table S2 in the Supplementary Material.

CO + H2 O ↔ CO2 + H2 (1)

2.4. Acid Gas Removal/CO2 Capture Unit

To prevent poisoning of dimethyl oxalate and ethylene glycol synthesis catalysts,
the acid gases (such as CO2 , H2 S and COS) should be firstly removed or captured. In
this work, three mature CO2 technologies, i.e., Rectisol (methanol as absorbent), MEA
(monoethanol amine as absorbent) and CAP (chilled ammonia as absorbent) technologies,
and a novel DMC technology (dimethyl carbonate as absorbent) are compared to seek
out the most economically CO2 capture method for CTEG process. Membrane separation
technology, one of new chemical separation technologies, is based on the difference of
the permeation rate of each component in the membrane. However, as for large-scale
CO2 capture systems, the membrane separation method still has a large gap in production
cost and reliability. Thus, it is not discussed in this paper. In addition, there is a gas
pretreatment subprocess and a H2 S removal subprocess before CO2 capture subprocess,
and these three subprocesses are the main components of the acid gas removal unit. As H2 S
removal and CO2 capture are simultaneously considered and inseparable in the AGR unit
in the coal chemical industry, H2 S removal and CO2 capture processes are considered as a
whole to analyze their effects on the performance of CTEG process rather than considering
the endogenous relationship between them. To facilitate the modeling and simulation of
the CTEG process with different CO2 capture technologies, their Aspen Plus model and
key parameters are summarized and presented in Table 1.

Table 1. Key parameters for the simulation of four CO2 capture technologies.

Operational Operational
Technology Equipment Model Equipment Model
Parameters Parameters
Rectisol a Lean cooler Heater Tout = −58 ◦ C, ∆P = 0 CO2 Flash1 Flash P = 1.38 MPa, Q = 0
Acid gas Absorber Radfrac N = 20, P = 5.5 MPa H2 S con. column Radfrac N = 20, P = 0.2 MPa
SO2 Flash Flash P = 0.69 MPa, Q = 0 H2 S Radfrac N = 10, P = 0.3 MPa
MEA b Cooler Heater Tout = 40 ◦ C, ∆P = 0 Desorber Radfrac N = 11, P = 0.19 MPa
Absorber Radfrac N = 11, P = 0.12 MPa Lean cooler Heater Tout = 40 ◦ C, ∆P = 0
Rich-pump Pump P = 0.21 MPa, η = 0.8 Lean pump Pump P = 0.21 MPa, η = 0.8
CAP c Heat exchanger HeatX Tcold = 95 ◦ C, ∆P = 0 Separator Flash2 Tout = 40 ◦ C, ∆P = 0
Contact cooler Radfrac N = 5, P = 0.12 MPa Rich-pump-2 Pump P = 0.14 MPa, η = 0.8
Absorber Radfrac N = 20, P = 0.12 MPa Heat exchanger-2 HeatX ∆Tcold = 5 ◦ C, ∆P = 0
Rich-pump-1 Pump P = 1.0 MPa, η = 0.8 Lean pump Pump P = 0.14 MPa, η = 0.8
Heat exchanger-1 HeatX ∆Tcold = 5 ◦ C, ∆P = 0 NH3 -desorber Radfrac N = 5, P = 0.12 MPa
Desorber Radfrac P = 2.0 MPa Cooler-2 Heater Tout = 40 ◦ C, ∆P = 0
Lean cooler-1 Heater Tout = 25 ◦ C, ∆P = 0 Lean cooler-2 Heater Tout = 10 ◦ C, ∆P = 0
Flash Flash2 Tout = 40 ◦ C, ∆P = 0 Mixer Mixer Adiabatic mixing
N = 10, P = 2.84 MPa,
DMC c Absorber Radfrac Heat exchanger HeatX Tlean = 30 ◦ C, ∆P = 0
∆P = 0.02 MPa
Flash Flash2 Tout = 30 ◦ C, ∆P = 0 Lean MEA - 35 mol%
a b c
[17]; [22]; [15].
 Processes 2021, 9, 207 6 of 19

2.4.1. Rectisol Technology

The Rectisol acid gas removal technology uses physical absorbent, chilled methanol
(chilled to −50 ◦ C), to remove CO2 and H2 S from syngas [23]. It mainly consists of
acid gas absorption column, CO2 desorption column, H2 S concentration column, solvent
regenerator and flashes as shown in Figure 3. After being cooled by the low-temperature
product gas, the syngas is pre-cooled to −20 ◦ C and goes to flash to remove water. The
output gas of the flash is fed to the bottom of the acid gas absorption column, where it is in
◦
Processes 2021, 9, x FOR PEER REVIEW countercurrent contact with low temperature methanol at −50 C. As a result, the CO2 and 6 of 1
H2 S of syngas are sufficiently absorbed by the low-temperature methanol, and the purified
syngas is obtained from the top of the absorption column [23].

Purified syngas

Chilled methanol H2S

Refrigerator
Refrigerator Tail gas

Acid gas CO2 Cooling water

absorber Methanol
+CO 2
H2S
Cold product concentration
gas column

Solvent
Crude syngas Methanol regenerator
+CO 2, H2S CO2
Desorption
column
Warm product Steam
gas

Water
Methnaol N2
splitter

Steam

H2O

Figure 3. Simplified
Figure 3. Simplifiedsimulation flowsheetofof
simulation flowsheet thethe Rectisol
Rectisol technology.
technology.

2.4.2.
2.4.2. MEA MEA Technology
Technology
TheThe MEAtechnology,
MEA technology, oneoneof of
mature gas stream
mature scrubbing
gas stream methods,methods,
scrubbing has been indus-
has been in
trialized for almost 70 years [15]. Its simplified flowsheet is shown in Figure 4 [24]. The
dustrialized for almost 70 years [15]. Its simplified flowsheet is shown in Figure 4 [24]
crude syngas is previously cooled and purified by reacting with the lean amine solution
Theincrude syngasasisshown
the absorber previously cooled
in Equations and [22].
(2)–(8) purified by amine
The rich reacting without
solution thefrom
leanthe
amine so
lution in the
absorber absorber
goes as shown
to the stripper in Equations
after heated (2)–(8)
with the lean amine[22]. The The
solution. richelectrolyte
amine solution
non- ou
from the absorber goes
random-two-liquid to the
(NRTL) modelstripper after heated
with electrolyte inserts with
for thethe
MEA lean amine
physical solution. Th
property
method isnon-random-two-liquid
electrolyte selected as the physical method
(NRTL)due to it contains
model withnew parametersinserts
electrolyte and Henry’s
for the MEA
constant for CO2 in MEA [25]. The key parameters for the modeling and simulation of this
physical property method is selected as the physical method due to it contains new pa
technology are present in Table 1.
rameters and Henry’s constant for CO2 in MEA [25]. The key parameters for the model
ing and simulation of this technology 2H2 O ↔ +
areHpresent
3 O + OH in−Table 1. (2)

2H2 O↔↔H3HO+O+ +
2H2 O + CO OH3−
HCO (3) (2
H2 O2H O +3−CO
+ HCO ↔ H↔
3 OH +
+
O CO −
+23HCO (4) (3
+H
MEAH O+
O 3+ ↔ MEAH
HCO
+
↔ H O+ H
+2 O
CO (5) (4
MEAH + HCO3− ↔ MEACOO + H2 O −
(6)
MEA + H O ↔ MEAH + H O (5

MEAH + HCO ↔ MEACOO + H O (6

MEA + CO + H O ↔ MEACOO + H O (7
 Processes 2021, 9, 207 7 of 19

Processes 2021, 9, x FOR PEER REVIEW 7 of 19

cesses 2021, 9, x FOR PEER REVIEW MEA + CO2 + H2 O ↔ MEACOO− + H3 O+ (7) 7 of
−
CO2 + OH ↔ HCO3− (8)

Clean syngas CO2

Gas cooler
Clean syngas CO2
Gas cooler Separator
MEA
(Make up) Separator
MEA
Stripper
(Make up)
Crude Lean cooler
Stripper
syngas Heat
Absorber Lean cooler
Crude Cooler exchanger
syngas Heat
Absorber
Cooler exchanger

Rich-pump

Lean-pump
Rich-pump
Figure 4. Simplified simulation flowsheet of the MEA technology.
Lean-pump
2.4.3. CAP Technology
FigureFigure
4. Simplified
4. Simplifiedsimulation
simulationflowsheet
flowsheet ofofthethe
MEAMEA technology.
technology.
The chilled ammonia process (CAP) is divided into carbon dioxide capture system
2.4.3.and
CAP ammonia
2.4.3. CAP capture system as shown in Figure 5. The crude syngas is cooled to 10 °C
Technology
Technology
and fed tochilled
the absorber. The lean ammonia solution is sent to the top of the absorber to
The The
remove chilled
CO 2 in
ammonia process
ammonia
the syngas. process
The
(CAP)
(CAP)
rich
is divided
ammonia
into carbon
is divided
solution into
is
dioxide
carbon
sent to
capture
the
system
dioxide
solvent ◦
and
capture
regeneration syste
ammonia capture system as shown in Figure 5. The crude syngas is cooled to 10 C and
and column
ammonia
fed to the capture
after system
heat exchange
absorber. The as shown
with
lean ammonia in solution.
thesolution
lean Figure
is sent to 5.The
The
the crude
lean
top syngassolution
of ammonia
the absorber is remove
to cooled from tothe
10
and bottom
fed
CO2to in the
of the
the absorber. The The
desorber
syngas. lean ammonia
is ammonia
rich recycled solution
to the absorber.
solution is sent to the is solvent
sent toregeneration
Although the CAP
the top of the absorber
process
column greatly
remove after
reducesCO2the
heat in the
exchange
escapesyngas.
with
ratio ofThe
the rich ammonia
lean solution.
ammonia The solutionofisthe
lean
in the absorber ammonia sent to thedioxide
solution
carbon fromsolvent
the regenerati
bottom
capture sys-
of
tem, the
thedesorber
exhaust is recycled
gas from to
thethe absorber.
top of this Although
column the
still
column after heat exchange with the lean solution. The lean ammonia solution from t CAP
contains process
a greatly
large reduces
amount of the
ammonia
escape
gas [26]. ratio
Thus, of ammonia
an additionalin the absorber
ammonia of capture
the carbon dioxide
system iscapture
required system,
to CAPthe exhaust
further reduce greaam-
bottom of the desorber is recycled to the absorber. Although
gas from the top of this column still contains a large amount of ammonia gas [26]. Thus, an
the process
monia
reduces in the
the escape exhaust
ratio gas. The
of ammonia syngas from the
in the absorber top of the absorber
of theammonia enters
carbonindioxide the ammonia
capture sy
additional ammonia capture system is required to further reduce the exhaust
capture
tem, the
gas.exhaustsystem
The syngas and
gasfrom
from is contacted
thethetoptop with
ofabsorber
of the the
this column low-concentration
entersstill containscapture
the ammonia ammonia
a largesystem solution
amount andof in the
is ammon
NH 3-absorber. As a result, the concentration of ammonia in the syngas can be less than 10
contacted
gas [26]. Thus,with an the low-concentration
additional ammonia ammonia
capture solution
system in the is NH 3 -absorber.
required As a result,
to further reduce a
ppm. The key parameters
the concentration of ammonia forinthe modeling
the syngas and
can be lesssimulation
than 10 ppm. of this technology
The key parameters are indi-
monia in the exhaust gas. The syngas from the top of the absorber enters the ammon
cated
for theinmodeling
Table 1. and simulation of this technology are indicated in Table 1.
capture system and is contacted with the low-concentration ammonia solution in t
NH3-absorber. As a result, the concentration of ammonia in the syngas can be less than
ppm. The key parameters for theCOmodeling and simulation of this technology are in
Clean gas
2

Make up
cated in Table 1. Flash
Water
(Make up)

Lean Lean
cooler-2 cooler-1 Cooler-2 NH3-
Absorber desorber
CO2
Desorber
CleanNH
gas3-
Make up absober
Water Heat
Rich-pump Flash (Makeexchanger-2
up)
water
Crude Lean Lean
Heat
syngas cooler-2 cooler-1
Contact Cooler-2
Rich-pump-2 NH3-
Absorber exchanger-1
Cooler-1 cooler Desorber desorber
Lean-pump
NH3-
absober Heat
Simplified simulation exchanger-2
Figure
Figure 5.5.Simplified
Rich-pump simulationflowsheet of the
flowsheet CAP
of the technology.
CAP technology.
water
Crude 2.4.4. DMC Technology
Heat
syngas Contact exchanger-1 Rich-pump-2
Cooler-1 cooler
Due to high solubility of CO2 in DMC and a low toxicity, it shows a better perfor-
Lean-pump

mance over traditional physical solvents in an appropriate temperature range and is re-
Figure 5. Simplified
garded simulation
as a promising flowsheet
and of absorbent
effective the CAP technology.
for CO2 capture [15]. The simplified
 Processes 2021, 9, 207 8 of 19

2.4.4. DMC Technology

Due to high solubility of CO2 in DMC and a low toxicity, it shows a better performance
over traditional physical solvents in an appropriate temperature range and is regarded as a
Processes 2021, 9, x FOR PEER REVIEW promising and effective absorbent for CO2 capture [15]. The simplified flowsheet of the 8 of 19
DMC technology is present in Figure 6. The syngas counter-currently contacts with the
lean DMC solution under the conditions of 3.0 MPa and 15 ◦ C. The rich solution enters
the high- and low-pressure flashes to regenerate lean solution. After mixing with makeup
mixing
DMC, with makeup
the lean DMC,
solution the lean
is recycled solution
to the is recycled
absorber. to the absorber.
The key parameters for theThe key param-
modeling
eters for the modeling and simulation of this technology
and simulation of this technology are shown in Table 1. are shown in Table 1.

DMC
Clean
(make up)
syngas
CO2 Tail gas

HP
flash

LP
flash Desorber
Absorber
N2

Crude syngas

Heat
exchanger
Pump

Figure
Figure6.6.Simplified
Simplified simulation flowsheet
simulation flowsheet ofof
thethe DMC
DMC technology.
technology.

2.5. CO
2.5. COand
andHH2 2Separation
Separation Unit
Unit
Thepurified
The purified syngas
syngasisiscooled
cooledin the mainmain
in the heat exchanger and then
heat exchanger sentthen
and to a flash.
sent toThea flash.
gasgas
The stream of theof
stream flash
theis flash
heatedisand fed into
heated the fed
and PSA into
equipment
the PSAto obtain high-purity
equipment to obtain
hydrogen. The liquid stream of the flash is successively sent to the CO/CH 4
high-purity hydrogen. The liquid stream of the flash is successively sent to the CO/CH and CO/N 2 4
separation columns to produce high-purity CO. The tail gas of this unit can be used as
and CO/N2 separation columns to produce high-purity CO. The tail gas of this unit can be
additional fuel to provide heat of coal gasification or other units. The RK-SOVE method is
used as additional fuel to provide heat of coal gasification or other units. The RK-SOVE
selected as the physical property method of this unit.
method is selected as the physical property method of this unit.
2.6. Ethylene Glycol Synthesis and Refinery Unit
2.6. Ethylene Glycol Synthesis
The high-purity CO from andthe
Refinery Unitis reacted with methyl nitrite (MN) and
CHS unit
converted to dimethylCO
The high-purity oxide
from(DMO) as shown
the CHS unitinisEquation
reacted (9) [27].
with The NO
methyl is reacted
nitrite (MN) and
with oxygen and methanol to produce methyl nitrite as shown in Equation
converted to dimethyl oxide (DMO) as shown in Equation (9) [27]. The NO (10), whichis isreacted
recycled and used as the raw material of the DMO synthesis reaction.
with oxygen and methanol to produce methyl nitrite as shown in Equation (10), which is
recycled and used as the raw material
2CO + MN of→theDMO
DMO synthesis reaction.
+ 2NO (9)
2CO
2NO + 0.5O + MN → DMO + 2NO
2 + 2CH3 OH → 2MN + H2 O (10) (9)
2NO + 0.5O
After separation and purification + 2CHtheOH
processes, DMO→ 2MN +enters
stream H O the ethylene glycol (10)
synthesis reactor, in which it is reacted with the hydrogen from the CHS unit to produce
After separation and purification processes, the DMO stream enters the ethylene
ethylene glycol as shown in Equations (11)–(13) [9]. The kinetic data of these reactions are
glycol
shownsynthesis reactor,
in Table S3 in which it is Material.
in the Supplementary reacted with the hydrogen
Considering the mainfrom the CHS
components areunit to
produce
polar substances, this unit uses the NRTL-RK method as the thermodynamic method. of these
ethylene glycol as shown in Equations (11)–(13) [9]. The kinetic data
reactions are shown in Table S3 in the Supplementary Material. Considering the main
DMO +this
components are polar substances, → 2MG
2H2unit uses+the
CHNRTL-RK
3 OH (11)
method as the thermody-
namic method.
DMO + 2H → 2MG + CH OH (11)
MG + 2H → 2EG + CH OH (12)
 Processes 2021, 9, 207 9 of 19

MG + 2H2 → 2EG + CH3 OH (12)

EG + H2 → ET + CH3 OH (13)
Processes 2021, 9, x FOR PEER REVIEW 9 of 19
The output of the ethylene glycol synthesis reactor enters the high- and low-pressure
flashes for preliminary separation. The liquid stream is sent to the ethylene glycol refin-
ery system, which involves five columns: the methanol recovery column, dehydration
andcolumn,
dealcoholization columns
dealcoholization areEG
column, used to remove
product columnwater
and EGand low-boiling
recovery column alcohols.
[20]. In Fi-
nally, the column,
the first high-purity ethylene
the recovery glycol isproduct
methanol recycled is
to obtained
synthesize from thedehydration
MN. The ethylene glycol
and dealcoholization
product and recovery columns
columns.are used to remove water and low-boiling alcohols. Finally,
the high-purity ethylene glycol product is obtained from the ethylene glycol product and
2.7.recovery columns.
Flowsheet Simulation and Validation
AFlowsheet
2.7. simplified simulation
Simulation flowsheet of the CTEG process with different CO2 capture
and Validation
technologies is shown
A simplified in Figure
simulation 7. To simulate
flowsheet of the CTEGthe whole
processflowsheet of CTEG
with different process, the
CO2 capture
keytechnologies
parametersisfor shown in Figure 7. To simulate the whole flowsheet of CTEG process,with
modeling and simulation of four different CTEG processes the Rec-
keyMEA,
tisol, parameters
CAP forandmodeling and simulation
DMC technologies of shown
are four different CTEG
in Table processes
2. After with Rectisol,
simulation, the mass
MEA, CAP and DMC technologies are shown in Table 2. After simulation,
and energy balance of these processes are then obtained with the aid of simulator, Aspen the mass and
energy
Plus balance
software. of these
Table processes
3 shows the are then obtained
comparison withof
results thethe
aidsimulation
of simulator,and
Aspen Plus re-
literature
software. Table 3 shows the comparison results of the simulation and literature reported
ported data of the key streams. It can be seen that the simulation results are in good
data of the key streams. It can be seen that the simulation results are in good agreement
agreement with the literature reported data, i.e., the established models of four CTEG
with the literature reported data, i.e., the established models of four CTEG processes can
processes
be used can be following
for the used for the following
system analysis.system
The basicanalysis. The basic
performance performance
of the whole CTEGof the
whole CTEG process in terms of the simulation results is present in Table
process in terms of the simulation results is present in Table 4. The CTEG process consumes 4. The CTEG
process
118.98consumes
t/h raw coal118.98 t/h raw
to produce coal
37.50 t/hto produce
ethylene 37.50
glycol t/h ethylene
products glycol
and about 2.19 products
t/h CO2 and
about 2.19 t/h CO
are captured 2 are
in the AGRcaptured in thethe
unit. Thus, AGR unit. and
technical Thus, the technical
economic and economic
performance of these per-
processes are analyzed and compared based on the simulation results.
formance of these processes are analyzed and compared based on the simulation results.

Figure 7. Simplified
Figure simulation
7. Simplified flowsheet
simulation flowsheetof
of CTEG processwith
CTEG process withdifferent
different
COCO 2 capture
2 capture technologies.
technologies.

Table 2. Key parameters for modeling and simulation of four CTEG processes.

Unit Key Parameters Value Key Parameters Value

ASU unit O2 supplied mole purity 99.8% N2 supplied mole purity 99.9%
CG unit Gasification pressure 4.0 MPa Gasification temperature 1500 °C
Oxygen to coal 0.42 Steam to coal 0.25
Processes 2021, 9, 207 10 of 19

Table 2. Key parameters for modeling and simulation of four CTEG processes.

Unit Key Parameters Value Key Parameters Value

ASU unit O2 supplied mole purity 99.8% N2 supplied mole purity 99.9%
CG unit Gasification pressure 4.0 MPa Gasification temperature 1500 ◦ C
Oxygen to coal 0.42 Steam to coal 0.25
WGS unit Pressure 3.65 MPa Shift ratio 49.25%
1st shift reactor temperature 350 ◦ C 2nd shift reactor temperature 220 ◦ C
AGR unit Shown in Table 1
CHS unit H2 recovery ratio 95.17% CO recovery ratio 91.75%
EGSR unit DMO reactor temperature 130 ◦ C DMO reactor pressure 0.5 MPa
Regeneration temperature 40 ◦ C H2 /DMO (mole ratio) 42
EG reactor temperature 235 ◦ C EG reactor pressure 3.0 MPa
Recovery column temperature 90 ◦ C Pressure 0.1 MPa
Methanol recovery ratio 99.5% DMC removal ratio 95.2%

Table 3. Comparison of the simulation and reported results of key streams.

CO H2 CO2 H2 O N2 +Ar H2 S Others

Crude syngas a Simulation results 59.58 27.37 12.09 - 0.68 0.25 0.03
Industrial data b 61.30 27.10 10.47 - 0.87 0.24 0.02
Shifted syngas Simulation results 23.17 43.83 32.04 0.22 0.53 0.18 0.03
Industrial data c 22.18 40.85 35.59 0.24 0.94 0.18 0.02
Clean syngas Simulation results 34.59 63.39 - - 2.02 - -
Industrial data d 34.60 63.96 - - 1.43 - 0.01
H2 product Simulation results 0.01 99.91 - - 0.04 - -
Industrial data d - 99.95 - - 0.05 - -
CO product Simulation results 99.06 - - - 0.94 - -
Industrial data d 98.00 - - - 2.00 - -
a dry basis; b [28]; c [29]; d [20].

Table 4. Basic performance of the CTEG performance.

Item Value
Input coal 118.98 t/h
Air consumption 20,2600 Nm3 /h
CO consumption 1529 kmol/h
H2 consumption 2846 kmol/h
Methanol consumption 3.38 t/h
HNO3 consumption 2.23 t/h
NaOH consumption 0.54 t/h
CO2 captured (AGR unit) 2.19 t/h
Captured CO2 purity ≥95.0%
EG product 37.50 t/h

3. Comparison of the Four Different CO2 Capture Technologies

In this study, the energy consumption, capital investment, CO2 capture cost, pro-
duction cost, and internal rate of return are conducted to compare the technoeconomic
performance of the CTEG process with Rectisol, MEA, CAP and DMC technologies.

3.1. Comparison of Energy Consumption and Energy Efficiency

In this section, the energy consumption of CO2 capture, the total energy consumption
and energy efficiency of whole CTEG processes are performed to compare the technical
performance of the CTEG process with different CO2 capture technologies. The calculation
of the energy consumption of CO2 capture with Rectisol, MEA, CAP and DMC technologies
is shown in Equation (14). Referring to the total input and output energy, the energy
Processes 2021, 9, 207 11 of 19

efficiency of the CTEG process with different CO2 capture technologies can be analyzed as
shown in Equation (15).

Qreb + Wcol + Wcom + Wpum

W= (14)
mCO2

Eoutput
η= × 100% (15)
Einput
where W means the total energy consumption of CO2 capture; Qreb is the heat duty of
the regeneration process; W col , W com and W pum are the work consumption of cooling
equipment, compressors and pumps, respectively; η is the energy efficiency; Eoutput is the
energy of output ethylene glycol; Einput is the total input energy including coal, electricity,
steam, etc.
As Figure 8 shows, the energy consumption of CO2 capture of the CTEG process
with MEA technology is the highest, 5.20 GJ/tCO2 , and the CTEG process with Rectisol
technology is the lowest, 1.88 GJ/tCO2 , followed by the DMC process, 2.10 GJ/tCO2 , and
MEA process, 3.64 GJ/tCO2 . The main reasons are that:
1. In general, there is an ASU unit in a CTEG plant, which can simultaneously provide
oxygen and cold nitrogen. The cold nitrogen is at very low temperature and has
a relative high cooling ability. Therefore, the cold utility of the Rectisol and DMC
processes can be greatly reduced by integrating with the cold nitrogen stream of the
ASU unit, which will also reduce the amount of other coolants to cool the methanol.
As a result, the energy consumption of CO2 capture of these two processes is lower
than that of the MEA and CAP processes.
2. The electricity consumption of the Rectisol process is significantly lower than that of
the DMC process. Thus, although both the Rectisol and DMC are part of the physical
absorption method and have a relative similar flowsheet, the CO2 capture and total
energy consumptions of the Rectisol process are lower than those of the DMC process.
3. As the MEA process is a chemical absorption method, it needs an amount of steam
to heat the rich solution in the reboiler. In fact, the regeneration duty of the MEA
process is about 4.08 GJ/tCO2 , accounting for 78.46% of the total CO2 capture energy
consumption. However, most of the CO2 of the Rectisol and DMC processes is
discharged in the multistage flashes, resulting in low regeneration duty.
4. In addition to the heat duty of CO2 regeneration column (1.26 GJ/tCO2 ), the CAP
process requires additional steam to heat the ammonia regeneration column, which is
about 1.42 GJ/tCO2 . Thus, the energy consumption of the regeneration process of the
CAP process is far less than that of the MEA process, resulting in a low CO2 capture
energy consumption. Compared with the MEA and CAP processes, the Rectisol and
DMC process requires less regeneration duty due to the high solubility of acid gas.
5. As for the compression work, the MEA process consumes the highest electricity,
1.12 GJ/t CO2 , because of the highest pressure of the CO2 stream from this process
in comparison with other processes. It also leads to the high energy consumption of
this process.
6. As Figure 8 shows, the total energy consumption of the CTEG process with Rectisol,
MEA, CAP and DMC technologies is 41.38 GJ/t, 48.44 GJ/t, 45.12 GJ/t, 41.85 GJ/t,
respectively. Assuming that the ethylene glycol production of these four processes
is the same up to 37.5 t/h, their total output energy is the same up to 19.10 GJ/T.
Thus, the energy efficiency of the CTEG process with Rectisol, MEA, CAP and DMC
technologies is 46.16%, 39.43%, 42.33% and 45.64%, respectively. Therefore, the CTEG
process with Rectisol technology has the best thermodynamic performance.
Processes 2021,
Processes 9, x9,FOR
2021, 207 PEER REVIEW 12 of 19 12 of 19

6 50

45

Energy consumption of CO2 capture (GJ/t-CO2)

5

Total energy consumption (GJ/t-EG)

40

35
4
30

3 25

20
2
15

10
1
5

0 0
Rectisol MEA CAP DMC

8. Energy
Figure 8.
Figure Energyconsumption
consumptionof of
CTEG process
CTEG withwith
process different CO2 capture
different technologies.
CO2 capture technologies.
Thus, integration of the cold nitrogen stream from the ASU unit to the AGR unit could
3.2. Comparison
greatly ofCO
reduce the Totalcapture
Capitalenergy
Investment
consumption, resulting in low energy consumption
2
The
of the conventional
Rectisol and DMC Chemical Engineering
processes. It could alsoPlant
affectCost
theirIndex (CEPCI)
economic method as
performance is used to
discussed in the following section.
estimate the total capital investment (TCI) of the CTEG process with different CO2 cap-
ture technologies. The total capital investment of a process mainly includes fixed capital
3.2. Comparison of Total Capital Investment
investment and working capital [30]. The former is employed to purchase equipment,
The conventional Chemical Engineering Plant Cost Index (CEPCI) method is used
piping, electrical, buildings, land, etc. In general, the equipment investment (EI) greatly
to estimate the total capital investment (TCI) of the CTEG process with different CO2
determines the fixedThe
capture technologies. and total
total capital
capital investments
investment [31].
of a process The includes
mainly cost of equipment
fixed capital is esti-
mated via Equation
investment and working(16).capital
The main[30].parameters
The formercontaining
is employed this equation equipment,
to purchase are listed in Table
5.piping,
The other costs of the total capital investment can be estimated on
electrical, buildings, land, etc. In general, the equipment investment (EI) the basis of their ra-
greatly
tios to the investment
determines the fixed andoftotal
equipment. Their corresponding
capital investments [31]. The costratio factor is is
of equipment shown in Table S3
estimated
viathe
in Equation (16). The main
Supplementary parameters
Material. Then, containing
the totalthis equation
capital are listed in
investment Table
can be 5.estimated
The as
other costs of the total
shown in Equation (17) [32].capital investment can be estimated on the basis of their ratios to
the investment of equipment. Their corresponding ratio factor is shown in Table S3 in the
Supplementary Material. Then, the total 𝑆capital investment
𝐶𝐸𝑃𝐶𝐼 can be estimated as shown in
Equation (17) [32]. 𝐸𝐼 = 𝐸𝐼 × × ×𝑓 (16)
𝑆 𝐶𝐸𝑃𝐶𝐼
!s f !
S CEPCI2018
EI = EIre f𝑇𝐶𝐼
× = 𝐸𝐼 × × 1 + CEPCI
𝑅𝐹 ×f (16) (17)
Sre f re f

!
where S means the processing capacity; RFi is the ratio factor of the ith capital investment;
TCI = EI × 1 + ∑ RFi (17)
the subscript ref. means the benchmark case fori
equipment cost.
where S means the processing capacity; RFi is the ratio factor of the ith capital investment;
Table 5. Reference equipment investment of each unit.
the subscript ref. means the benchmark case for equipment cost.
Unit Benchmark sf Sref EIref (106 CNY) CEPCIref f
ASU a Oxygen supply 0.50 91.75 t/h 105 584.6/2012 0.5
CG a Coal input 0.67 114.21 t/h 135.21 394.3/2001 1.0
WGS b Syngas input 0.67 30,697 kmol/h 11.56 525.4/2007 0.6
Rectisol a Syngas input 0.67 200 kNm3/h 52.3 584.6/2012 0.65
MEA c CO2 output 0.67 66,509 t/d 206.55 525.4/2007 0.65
CAP d CO2 output 0.67 419.16 t/h 117.15 584.6/2012 0.65
DMC d CO2 output 0.67 66,509 t/d 244.45 525.4/2007 0.8
DMOS e H2 input 0.65 2845.50 kmol/h 55.20 576.1/2014 0.6
 Processes 2021, 9, 207 13 of 19

Table 5. Reference equipment investment of each unit.

OR PEER REVIEW 13 of 19
Unit Benchmark sf Sref EIref (106 CNY) CEPCIref f
ASU Oxygen supply a 0.50 91.75 t/h 105 584.6/2012 0.5
CG a Coal input 0.67 114.21 t/h 135.21 394.3/2001 1.0
EG output
WGS b 0.65
Syngas input 37.50 t/h0.67 84.32
30,697 kmol/h 11.56576.1/2014 525.4/2007 0.6 0.6
Rectisol a Syngas input 0.67 200 kNm3 /h 52.3 584.6/2012 0.65
H2 output 0.67 21.3 kg/s 45.92 575.4/2008 1.0
MEA c CO2 output 0.67 66,509 t/d 206.55 525.4/2007 0.65
H2 inputCAP d 0.70CO2 output 944 Nm3/h 0.67 0.83
419.16 t/h 576.1/2014
117.15 584.6/2012 1.0 0.65
DMC d [21]; b [33]; c [15];
CO2a output 0.67d [34]; e [10]; f [19].
66,509 t/d 244.45 525.4/2007 0.8
DMOS e H2 input 0.65 2845.50 kmol/h 55.20 576.1/2014 0.6
EGS e DMO input 0.65 74.21 t/h 77.76 576.1/2014 0.6
EGR e The total capital investment
EG output 0.65 of the37.50 CTEG t/h process with
84.32 different576.1/2014
CO2 capture tech-
0.6
nologies
HCS a
is Hindicated
2 output in Figure
0.67 9a,b. To 21.3purify
kg/s the same amount of 575.4/2008
45.92 syngas, the CTEG1.0
PSA f 944 Nm3 /h
process with Rectisol technology takes the highest capital investment, followed by the
H2 input 0.70 0.83 576.1/2014 1.0
a [21]; b [33]; c [15]; d [34]; e [10]; f [19].
CAP, DMC and MEA technologies as shown in Figure 9a. The investment cost of the
Rectisol, CAP and DMC processes is about 1.27, 1.21 and 1.18 times that of the MEA
The total capital investment of the CTEG process with different CO2 capture technolo-
process, respectively.
giesThe high capital
is indicated in Figure investment
9a,b. To purify of thethe Rectisol process
same amount is mainly
of syngas, dueprocess
the CTEG to
the more complexwith heatRectisol
exchange
technologynetwork takes theandhighest
materialscapitalintegration system.byThe
investment, followed highDMC
the CAP,
investment cost of the CAP process is mainly because it requires an additional ammoniaCAP
and MEA technologies as shown in Figure 9a. The investment cost of the Rectisol,
and DMC processes is about 1.27, 1.21 and 1.18 times that of the MEA process, respectively.
capture system to decrease the escape ratio of ammonia. As a result, the total capital in-
The high capital investment of the Rectisol process is mainly due to the more complex heat
vestment of the CTEG withnetwork
exchange Rectisol andtechnology
materials integration is the highest,
system. The4.49 × investment
high 109 CNY, cost followed
of the CAP
by the CAP technology,
process is4.45
mainly× 10 9 CNY,
because DMC an
it requires technology,
additional ammonia4.42 × capture
10 CNY,
9
systemand MEA the
to decrease
technology, 4.28 × escape
10 CNY.
9 The
ratio of distributions
ammonia. As a result, of thethetotal
total capital
capital investment
investment are present
of the CTEG with Rectisol
9 CNY, followed by the CAP technology, 4.45 × 109 CNY,
in Figure 9b. It shows that the proportion
technology is the highest, 4.49 of the ethylene glycol synthesis and refinery
× 10
DMC technology, 4.42 × 109 CNY, and MEA technology, 4.28 × 109 CNY. The distributions
unit is the largest, of
52.90%, which includes the dimethyl oxide synthesis, ethylene glycol
the total capital investment are present in Figure 9b. It shows that the proportion of
synthesis, and ethylene glycol
the ethylene glycolrefinery
synthesis processes.
and refinery In addition, the coal
unit is the largest, gasification
52.90%, and the
which includes
acid gas removal units
dimethylalso
oxidecontribute remarkable
synthesis, ethylene proportions,
glycol synthesis, accounting
and ethylene for 19.31%
glycol refinery processes.
and 12.64%, respectively. Thus, more attention should be paid to reduce the capital in-
In addition, the coal gasification and acid gas removal units also contribute remarkable
proportions, accounting for 19.31% and 12.64%, respectively. Thus, more attention should
vestment of these three units.
be paid to reduce the capital investment of these three units.

8.0 4.6
4.5
Total investment capital (10 9 CNY)
Invsetment of AGR unit (108 CNY)

7.0
4.4
6.0
4.3
5.0 4.2
4.0 4.1

3.0 4.0
3.9
2.0
3.8
1.0 ASU CG WGS
3.7 AGR CHS EGSR
0.0 3.6
Rectisol MEA CAP DMC
(a) (b)

Figure 9. Total
Figurecapital investment
9. Total capital of CTEG
investment process
of CTEG processwith
with different CO
different CO 2 capture
2 capture technologies.
technologies.

3.3. Comparison of Capture and Production Costs

In this study, the CO2 capture cost and total production cost (TPC) are considered to
further compare the economic performance of the CTEG process with different CO2
capture technologies. They are defined as follows [26]:
𝑇𝑇𝑇𝑇𝑅𝑅𝑎𝑎，𝐴𝐴𝐴𝐴𝐴𝐴 + 𝐶𝐶𝐶𝐶𝑀𝑀𝑎𝑎,𝐴𝐴𝐴𝐴𝐴𝐴 − 𝐶𝐶𝑠𝑠𝑠𝑠,𝐴𝐴𝐴𝐴𝐴𝐴
Processes 2021, 9, 207 14 of 19

3.3. Comparison of Capture and Production Costs

In this study, the CO2 capture cost and total production cost (TPC) are considered
to further compare the economic performance of the CTEG process with different CO2
capture technologies. They are defined as follows [26]:

TCR a,AGR + COMa,AGR − Csa,AGR

Cost of CO2 capture = (18)
mCO2 ,a

∑i TCR a,i + ∑i COMa,i − ∑i Csa,i

TPC = (19)
m EG,a
TCR a,i = TCIi × CRF (20)
r
CRF = (21)
1 − (1 + r ) − n
where TCR a,i is the total capital investment required for ith unit; Csa,i means the salvage
value of ith unit; CRF is the capital recovery factor; r and n are the discount rate (12%)
and plant lifetime (20 years) [34]; COMa,i shows the annual cost of the operational and
maintenance of ith unit, which can be calculated as follows [35]:

OMa,i = FOMa,i + VOMa,i (22)

where FOM and VOM represent the costs of fixed and variable operation and mainte-
nance, respectively.
The CO2 capture cost and total production cost of the CTEG process with different
CO2 capture technologies are calculated in terms of the simulation results and the market
price of raw material and utilities as is shown in Table 6. As Figure 10a shows, the CO2
capture cost of the Rectisol process is lowest, CNY 169.5/tCO2 , followed by the DMC
process, CNY 193.2/tCO2 , the CAP process, CNY 232.6 /tCO2 , and the MEA process,
CNY 250.5/tCO2 . It is mainly because the utilities of the MEA and CAP processes are
much higher than those of the Rectisol and DMC processes. Compared with the DMC
process, the Rectisol process is more maturity, resulting in a low operation and maintenance
cost. Thus, the total production cost of the CTEG process with Rectisol technology is the
lowest CNY 4631/tEG, followed by the DMC technology, CNY 4644/tEG. The MEA and
CAP technologies have a relatively high total production cost, CNY 4750/tEG, and CNY
4716/tEG, respectively. From the perspective of the compositions of total production cost,
there is no obvious difference in the costs of wage (CW) and period expenses (CP) of the
four process as Figure 10b shown. The MEA process has the lowest cost of maintenance
(CM) due to its lowest capital investment. However, it can be seen that the cost of utilities
(CU) and raw material (CR) of the Rectisol process is relatively lower than the other process
due to its low energy consumption and high CO2 removal ratio. Therefore, the CTEG
process with Rectisol technology has the best production cost advantage compared with
the MEA, CAP and DMC technologies.

Table 6. Average market price of main raw material, utilities, product and byproduct.

Items Price Items Price

Raw material and Raw coal CNY 450/t Fuel coal CNY 200/t
utilities Electricity 0.65 kWh/t Water CNY 4.5/t
Steam CNY 70/t Ammonia CNY 2200/t
Methanol CNY 2000/t MEA CNY 10, 600/t
DMC CNY 5500/t NaOH CNY 2000/t
HNO3 CNY 2500/t Catalysts CNY 300/t
Product and Ethylene glycol CNY 7500/t Light diol CNY 1966/t
byproduct Dimethyl carbonate CNY 5500/t Sulfur CNY 1026/t
Mixed alcohol ester CNY 7700/t Heavy component CNY 6154/t
Sulfuric acid CNY 250/t Cinder CNY 43/t
Processes 2021,
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Processes 2021, 9, x FOR PEER REVIEW 15 of 19

300 5000
DMC
4500 CP
CAP

Total production cost (CNY/t-EG)

250
300 5000
2)

4000
(CNY/t-CO

DMC
MEA
4500
3500 CP
CW CAP
Rectisol

Total production cost (CNY/t-EG)

200
250
2)

4000
(CNY/t-CO

3000
TPC

MEA
TPC

TPC

TPC
3500 CW
CO2 capture

150
200 2500 CR Rectisol
3000
TPC

COM TPC

COM TPC

COM TPC
2000
COM
capture

150
100 2500 CR
1500 CU
2000
CO2 of

1000
COM

100
Cost ofCost

COM

COM
50
COM

1500 CU
500 CM
TCR

TCR

TCR
TCR

1000
500 0
Rectisol MEA CAP DMC 500 CM 0 200 400 600 800 1000 1200 1400 1600 1800
TCR

TCR

TCR
TCR

0 0
Rectisol MEA (a) CAP DMC 0
(b)
200 400 600 800 1000 1200 1400 1600 1800
Figure
Figure 10.10. (a)
(a) Total
Total production
(a) cost,
production (b)(b)
cost, production cost cost
production compositions of theof
compositions CTEG
the process with different
CTEG(b)process CO2 capture
with different CO2
technologies.
capture technologies.
Figure 10. (a) Total production cost, (b) production cost compositions of the CTEG process with different CO2 capture
technologies.
3.4. Comparison of Internal Rate of Return
3.4. Comparison of Internal Rate of Return
Internal rate
3.4. Comparison of return
of Internal Rate(IRR) is an important indicator to compare the competitive-
of Return
Internal rate of return (IRR) is an important indicator to compare the competitiveness
ness of alternative technologies. It can be expressed as follows [20]:
Internal rate
of alternative of return (IRR)
technologies. It canisbe
anexpressed
importantas
indicator
followsto compare the competitive-
[20]:
ness of alternative technologies. It can be expressed as follows [20]:
n𝑁𝐶𝐹 × 1 + 𝐼𝑅𝑅 =−0j (23)
∑ NCFj × (1 + IRR
𝑁𝐶𝐹 × 1 + 𝐼𝑅𝑅 =0
) =0 (23)
j =0 (23)
where NCFj means the net cash flow of jth year.
whereThe
where NCF
NCF totalmeans the of
revenue netthe
cash
CTEG of jth year.
flowprocess
j jmeans the net cash flow of jth year.
is calculated by the simulation results and the
marketThe price
total of product
revenue of and
the byproduct
CTEG as
process
The total revenue of the CTEG process is calculated shown in Table
is calculated by5.the
by the According
simulation
simulation to the results
results
results and andofthe
the
Sections
market 3.2
price and
of 3.3,
product the internal
and rate
byproduct of return
as shown of the
in CTEG
Table
market price of product and byproduct as shown in Table 5. According to the results of 5.process
Accordingwith different
to the CO2 of
results
capture
Sections technologies is calculated and presented in Figure 11.
Sections 3.2 and 3.3, the internal rate of return of the CTEG process with different CO2 CO2
3.2 and 3.3, the internal rate of return of the CTEG The internal
process with rate of return
different
of the CTEG
capture
capture process
technologies
technologies isiswith the MEA
calculated
calculated andand and CAP in
presented
presented technologies
in Figure
Figure areThe
11. 11.
The the internal
lowest,
internal rate 16.91%
rate and
of return
of return
17.12%,
of respectively. This is mainly because their production
of the CTEG process with the MEA and CAP technologies are the lowest, 16.91% and and
the CTEG process with the MEA and CAP technologies costs
are are
the much
lowest, higher
16.91% than
the Rectisol
17.12%,
17.12%, and DMC
respectively.
respectively. This processes.
This isismainly
mainlyThe internal
because
because rate
their
their of return costs
production
production of the DMC
costs
are are process
much much
higher (17.38%)
higher
than than
is
the
the similar
Rectisol with
and the
DMCRectisol process
processes. The (17.25%)
internal because
rate of of its
return similar
of the
and DMC processes. The internal rate of return of the DMC process (17.38%) total
DMC capital
processinvestment
(17.38%) is
and
similar production
is similarwith
with thethe cost.
Rectisol However,
Rectisolprocess compared
process(17.25%) with
(17.25%)because
becauseof the DMC
ofits technology,
itssimilar
similar total the Rectisol
total capital investment tech-
investment and
nology
production
and has cost.
production beencost.
successfully
However,
However, operated
compared
compared forwith
with decades
thetheDMC andtechnology,
DMC has a largerthe
technology, market share.
Rectisol
the Rectisoltechnology
tech-
nology
has beenhas been successfully
successfully operated operated for decades
for decades and has andahas a larger
larger marketmarket share.
share.
18.0
18.0
17.0
17.0
16.0
16.0
(%)(%)

15.0
IRRIRR

15.0
14.0
14.0
13.0
13.0
12.0
12.0 Rectisol MEA CAP DMC
Rectisol MEA CAP DMC
Figure 11. Internal rate of return of CTEG process with different CO2 capture technologies.
Figure Internalrate
11. Internal
Figure 11. rateofofreturn
returnofof CTEG
CTEG process
process with
with different
different CO2CO 2 capture
capture technologies.
technologies.
Processes 2021, 9, x FOR PEER REVIEW 16 of 19
Processes 2021, 9, 207 16 of 19

3.5. Comparison of the Overall Performance

To comprehensively
3.5. Comparison compare the performance
of the Overall of the CTEG process with different
Performance
CO2 capture technologies, the best value of an evaluation indicator among the compara-
To comprehensively compare the performance of the CTEG process with different
tive processes is assumed to be 1.0, and the relative value of this indicator of one process
CO2 capture technologies, the best value of an evaluation indicator among the comparative
is its value divided by the best value for determining their relative disadvantage. Results
processes is assumed to be 1.0, and the relative value of this indicator of one process is its
show that the CTEG process with Rectisol technology has the best comprehensive per-
value divided
formance compared byMEA,
with the the best
CAP,value
and for
DMCdetermining their relative
processes, especially disadvantage.
in capture en- Results show
that the CTEG process with Rectisol technology has the best
ergy consumption and cost as shown in Figure 12. The comprehensive performance of comprehensive performance
compared with the MEA, CAP, and DMC processes, especially
the MEA is the worst because of the high capture energy and cost. However, its total in capture energy consump-
tion and
capital investment is cost as lower
greatly shownthanin Figure 12. The
three other comprehensive
technologies. performance
In summary, the Rec- of the MEA is the
worstis because
tisol technology of thefor
a good choice high
the capture energy
CTEG process to and
CO2 cost. However, its total capital investment is
capture.
greatly lower than three other technologies. In summary, the Rectisol technology is a good
choice for the CTEG process to CO2 capture.

capture energy
1 Good Rectisol

0.8 MEA

0.6 capture CAP

IRR
0.4 investment DMC

0.2
0 Poor

TPC TCI

capture cost

Figure 12. Comprehensive performance of CTEG process with different CO2 capture technologies.

4. Conclusions
Figure 12. Comprehensive performance of CTEG process with different CO2 capture technologies.
This study analyzed the technoeconomic performance of four CO2 capture alternatives
4. Conclusions
for the coal to ethylene glycol (CTEG) process: Rectisol, MEA, CAP and DMC. The main
This study analyzed
results gainedthe technoeconomic
from performance
this work can of four CO
be drawn briefly 2 capture alterna-
as follows:
tives for the coal to ethylene glycol (CTEG) process: Rectisol, MEA, CAP and DMC. The
1. The energy consumption of CO2 capture of the CTEG process with Rectisol technology
main results gained from this work can be drawn briefly as follows:
is the lowest, 1.88 GJ/tCO2 , and the CTEG process with MEA technology is the
1. The energy consumption of CO2 capture of the CTEG process with Rectisol tech-
highest, 5.20 GJ/tCO2 . That of the CTEG process with CAP and DMC technologies
nology is the lowest, 1.88 GJ/tCO2, and the CTEG process with MEA technology is
are 3.64 GJ/tCO and 2.10 GJ/tCO2 .
the highest, 5.20 GJ/tCO2. That2 of the CTEG process with CAP and DMC technolo-
2. The investment cost of the Rectisol, CAP and DMC technologies is about 1.27, 1.21
gies are 3.64 GJ/tCO2 and 2.10 GJ/tCO2.
and 1.18 times that of the MEA process, respectively. As a result, the total capital
2. The investment cost of the Rectisol, CAP and DMC technologies is about 1.27, 1.21
investment of the CTEG with Rectisol technology is the highest, 4.49 × 109 CNY,
and 1.18 times that of the MEA process, respectively. As a9 result, the total capital
followed
investment of the CTEG by with
the CAP technology,
Rectisol technology is ×
4.45 the10highest,
CNY, 4.49
DMC× technology,
109 CNY, 4.42 × 109 CNY,
followed by and MEA
the CAP technology,
technology, × 10×
4.454.28 109 CNY.
9 CNY, DMC technology, 4.42 × 109 CNY,
3. technology,
and MEA The CO2 4.28
capture
× 109cost
CNY.of the Rectisol process is the lowest, CNY 169.5/tCO2 , followed
3. The CO2 captureby the
costDMC
of theprocess, CNY 193.2/tCO
Rectisol process 2 , the
is the lowest, CNYCAP process
169.5/tCO CNY 232.6/tCO2 , and the
2, followed

by the DMC process, CNY 193.2/tCO2, the CAP process CNY 232.6/tCO2, and the cost of the CTEG
MEA process CNY 250.5/tCO 2 . Therefore, the total production
MEA process process with the 2Rectisol
CNY 250.5/tCO process
. Therefore, is the
the total lowest, CNY
production cost 4631/tEG,
of the CTEG and that of the MEA
process withprocess is the
the Rectisol highest,
process CNY
is the 4750/tEG.
lowest, CNY 4631/tEG, and that of the MEA
process4.is theThe internal
highest, CNYrate of return of the CTEG process with Rectisol technology is similar to
4750/tEG.
the DMC technology, which is higher than that of the CTEG process with the MEA
and CAP technologies.
Thus, compared with the MEA, CAP, and DMC technologies, the CTEG process with
Rectisol technology has the best comprehensive performance, especially in capture energy
consumption and cost. It can be selected as the most suitable CO2 capture technology for
CTEG industry. The models and results obtained in this study can be used to guide the
coal chemical industry for selecting the best carbon capture technology, such as coal to
ethylene glycol/methanol/olefins/SNG industries.
Processes 2021, 9, 207 17 of 19

Supplementary Materials: The following are available online at https://www.mdpi.com/2227-9

717/9/2/207/s1, Table S1: Main reactions take place in gasifier, Table S2: Key parameters for the
simulation of four CO2 capture technologies, Table S3: Ratio factor of the components in the TCI.
Author Contributions: Conceptualization, H.Z.; methodology, H.Z.; software, Y.Y.; validation, Y.M.;
formal analysis, Y.M.; investigation, Y.S.; resources, Y.S.; data curation, Y.L.; writing original draft
preparation, Y.M.; writing review and editing, Y.M.; visualization, B.W.; supervision, D.J.; project
administration, H.L.; funding acquisition, D.W. All authors have read and agreed to the published
version of the manuscript.
Funding: This research received no external funding.
Data Availability Statement: Data is contained within the article.
Conflicts of Interest: The authors declare no conflict of interest.

Abbreviations

η energy efficiency
Csa,i salvage value of ith unit
COMa,i annual cost of the operational and maintenance of ith unit
CRF capital recovery factor
FOM fixed cost
n plant lifetime
N number of stages
NCFj net cash flow of jth year
P pressure
∆P pressure drop
r discount rate
RFi ratio factor of ith capital investment
S processing capacity
T temperature
∆T temperature difference
TCR a,i total capital investment required for ith unit
VOM variable operation and maintenance cost
W col work consumption of cooling equipment
W com work consumption of compressor
W pum work consumption pump
ASU air separation unit
AGR acid gas removal
CG coal gasification
CHS CO and H2 separation
CTEG coal to ethylene glycol
CCG choren coal gasifier
CCR CO coupling reactor
CAP chilled ammonia process
CEPCI Chemical Engineering Plant Cost Index
DM dimethyl carbonate
EG ethylene glycol
EGSR ethylene glycol synthesis and refining
EI equipment investment
H/C hydrogen–carbon
IGCC integrated gasification combined cycle
IRR internal rate of return
MEA mono-ethanol amine
NRTL non-random-two-liquid
TCI total capital investment
TPC total production cost
WGS water gas shift
Processes 2021, 9, 207 18 of 19

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