Energy 228 (2021) 120535

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Energy
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Optimal design, exergy and economic analyses of coal-to-ethylene

glycol process coupling different shale gas reforming technologies
Qingchun Yang a, Qing Yang a, Simin Xu a, Dawei Zhang a, Chengling Liu a,
Huairong Zhou b, *
a
School of Chemistry and Chemical Engineering, Hefei University of Technology, Hefei, 230009, PR China
b
College of Petrochemical Technology, Lanzhou University of Technology, Lanzhou, 730050, PR China

a r t i c l e i n f o a b s t r a c t

Article history: The large-scale sustainable development of the coal-to-ethylene glycol process is severely plagued by its
Received 25 January 2021 shortcomings such as high CO2 emissions, investment cost, and energy consumption. To address these
Received in revised form issues, three novel shale gas assisted coal to ethylene glycol (SCtEG) processes with different methane
28 March 2021
reforming technologies are proposed and compared: the SCtEG process integrated with dry reforming
Accepted 31 March 2021
Available online 5 April 2021
technology (D-SCtEG), the SCtEG process integrated with steam reforming technology (S-SCtEG), and the
SCtEG process integrated with dry and steam reforming technologies (D þ S-SCtEG) processes. The key
operational parameters of these novel processes are optimized firstly based on the system modeling and
Keywords:
Coal
simulation. Then a techno-economic analysis is conducted and compared with a conventional CtEG
Shale gas process. The results show that, the carbon utilization efficiency of the D-SCtEG, S-SCtEG, and D þ S-SCtEG
Ethylene glycol processes is increased from 21.09% to 59.47%, 58.51% and 59.33%, respectively. Their exergy efficiencies
Optimal design are increased by 17.70%, 20.66% and 13.66%, respectively. Among these processes, the D-SCtEG and D þ S-
System analysis SCtEG processes can achieve zero CO2 emission. Furthermore, the D-SCtEG, S-SCtEG, and D þ S-SCtEG
processes can greatly reduce the total capital investment and production cost, especially, their produc-
tion costs are saved by 10.48%, 13.23%, and 9.09%, respectively.
© 2021 Elsevier Ltd. All rights reserved.

1. Introduction For example, Yi et al. [2] found that the carbon emission of this
process is about 3.4 t/t-EG through conducting a carbon balance
Ethylene glycol (EG) is regarded as one of the most important analysis. Moreover, if the indirect carbon emissions of the CtEG
primary raw materials for the chemical industries and widely used process are considered, the total carbon emissions of this process
in polyester, antifreeze, plasticizer, and surfactant production in- are 4.9 t/t-EG higher than those of the traditional oil-based route
dustries. In recent years, the demand of ethylene glycol product is [3]. As a result, the competitive advantages of the CtEG process over
far outstripped its supply, especially in China. As a result, coal to other production routes will no longer exist if carbon tax or envi-
ethylene glycol (CtEG) process has gained extensive attentions ronmental penalty is considered [4]. Therefore, the high CO2
because of its low production cost. For example, 27 new CtEG plants emissions of the CtEG process could seriously hinder its large-scale
with a total capacity of more than 10.90 Mt/y has been built or sustainable development. It urgently needs to reduce the CO2
planned from 2018 to 2019 [1]. Up to march 2019, there are 22 CtEG emissions of the CtEG process. However, little literature has been
plants have been successfully put into operation. Unfortunately, reported to address this issue systematically.
similar with other coal-based energy and chemical processes, the On the other hand, lots of studies has been conducted to find the
CO2 emissions of the CtEG process is much higher than other pro- most effective way to reduce carbon emissions of other similar
duction routes, due to the difference of hydrogen to carbon ratio coal-based chemical processes, such as coal to methanol [5], coal to
between raw coal and ethylene glycol product [1]. olefins [6], and coal to liquid fuels [7]. Results show that cofed of
coal and hydrogen-rich resources (e.g., natural gas, shale gas, coke
oven gas, and coalbed gas) to chemicals process can significantly
reduce the CO2 emissions of the single coal-based process, and even
* Corresponding author. achieve zero emissions.
E-mail address: zhouhr@lut.edu.cn (H. Zhou).

https://doi.org/10.1016/j.energy.2021.120535
0360-5442/© 2021 Elsevier Ltd. All rights reserved.
Q. Yang, Q. Yang, S. Xu et al. Energy 228 (2021) 120535

Nomenclature HCS hydrogen and carbon monoxide separation

IRR internal rate of return
C production cost PSA pressure swing adsorption device
Ex exergy SCtEG shale gas assisted coal to ethylene glycol
F molar flow rate RF ratio factor
I equipment cost SG shale gas
MSG/MCoal feed ratio of shale gas to raw coal SMR steam methane reforming
Q production capacity S-SCtEG integrated with steam reforming technology
TCI total capital investment
Abbreviations TPC total production cost
AGR acid gas removal WGS water gas shift
CtEG coal to ethylene glycol
DMR dry methane reforming Greek Letters
D-SCtEG integrated with dry reforming technology aCO shift ratio of CO
D þ S-SCtEG integrated with dry and steam reforming b ratio of shale gas of the dry reforming unit to total
technologies input shale gas
EGR ethylene glycol refinery hC carbon utilization efficiency
EGS ethylene glycol synthesis f exergy efficiency
FCI fixed capital investment q domestic factor

For example, the novel coke oven gas-assisted coal-to-olefins suggested that the government should give strong supports to the
process proposed by Man et al. [8] greatly reduces the CO2 emis- development of shale gas industry after compared the technical,
sions of the traditional coal-to-olefin process from 5.79 to 0.30 t/t- economic and environmental performance of shale gas and coal-
olefins, and increases the energy efficiency from 36.5% to 46.5%. based synthetic natural gas processes. Therefore, shale gas should
Similar results can be also found in Xiang et al. [9], in which a novel be effectively used to produce high-value added, economical and
natural gas assisted coal to olefin process was proposed to the CO2 environmentally friendly chemicals. However, there is no published
emissions and production cost of the conventional coal to olefins literature has been reported to cofeed shale gas and coal for
process. Compared with the traditional coal-to-methanol process, ethylene glycol production to address the issues of high CO2
the carbon and energy efficiencies of the novel coke oven gas emission and low energy efficiency of the traditional CtEG process.
assisted coal to methanol process are increased by approximately Thus, the main contribution of the present research is to seek for
25% and 10%, while CO2 emissions are decreased by 44% [10]. Thus, the optimal way to produce ethylene glycol from coal and shale gas
they believed that coal-based chemical process cofed with with low CO2 emissions, high energy efficiency and economic
hydrogen-rich resources can significantly reduce CO2 emissions benefits. For that purpose, three shale gas assisted coal to ethylene
and improve the resource and energy efficiencies of the process due glycol (SCtEG) processes with different reforming technologies are
to a water gas shift unit is decreased. A novel coal and coke oven gas proposed and analyzed. To have a better technoeconomic perfor-
to synthesize natural gas is proposed to improve the system per- mance, the key operational conditions of these three processes are
formance of a traditional coal to natural gas process, which in- detailed investigated and optimized in terms of their whole
dicates that it can increase the energy efficiency by 4%, and reduce simulation models. Finally, their technoeconomic performance is
the CO2 emission and the production cost by 60% and 16.7% [11]. analyzed and compared to illustrate their competitiveness
However, most of the reported works are focused on selecting compared with traditional CtEG process.
coke oven gas or natural gas as hydrogen-rich resources to reduce
the CO2 emission of coal-based chemical process. Shale gas is 2. Process description
considered as a new type of green clean energy rich in methane gas.
The total global recoverable reserves of shale gas are currently To overcome the shortcomings of the traditional CtEG process,
expected to reach 214.5 trillion cubic meters, which is equivalent to three shale gas assisted coal to ethylene glycol (SCtEG) processes
61 years of global natural gas under current conditions [12]. are proposed by integrating with dry and/or steam methane
Therefore, the development and utilization of shale gas resources reforming technologies. They are the SCtEG process integrated with
has received widespread attention, especially in the United States dry reforming technology (D-SCtEG), steam reforming technology
and China. For example, the well-known American Shale Gas Rev- (S-SCtEG), as well as dry and steam reforming technologies (D þ S-
olution. China has become the third largest shale gas producer after SCtEG) processes as shown in Fig. 1 (a)-(d).
the United States and Canada, and plans to produce 3  1010 m3 of (a) Traditional CtEG process: It is set as a benchmark case. As
shale gas production by 2020 [13]. shown in Fig. 1 (a), the CtEG process includes eight units: coal
Compared with natural gas, shale gas is cheaper and more gasification (CG), air separation unit (ASU), water-gas shift (WGS),
abundant. It can be widely used to produce primary chemicals. For acid gas removal (AGR), hydrogen and carbon monoxide separation
example, Ehlinger et al. [14] used Aspen Plus software to model and (HCS), dimethyl oxalate synthesize (DMOS), ethylene glycol syn-
simulate a shale gas to methanol process. He et al. [15,16] analyzed thesis (EGS), and ethylene glycol refinery (EGR) units [19]. The H2 to
the feasibility of shale gas to ethylene process from the technical, CO ratio (H2/CO) of the crude syngas is much lower than the
economic and life cycle perspectives. It shows a good performance required value of the ethylene glycol synthesis reaction [20]. Hence,
in the production cost and life cycle of greenhouse gas emissions. In a WGS unit is needed in this process.
addition, compared with traditional oil-based ethylene and pro-
pylene process, the shale gas-based process has lower production (b) D-SCtEG process: As Fig. 1 (b) shown, different from the
cost and life cycle greenhouse gas emissions [17]. Zeng et al. [18] traditional CtEG process, the hydrogen-rich shale gas (SG) is
2
Q. Yang, Q. Yang, S. Xu et al. Energy 228 (2021) 120535

Fig. 1. Schematic diagram of the traditional CtEG (a), and the proposed D-SCtEG (b), S-SCtEG (c) and D þ S-SCtEG (d) processes.

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Q. Yang, Q. Yang, S. Xu et al. Energy 228 (2021) 120535

used to increase the H2/CO ratio of the syngas. In addition, simultaneously utilize greenhouse gases (i.e., CH4 and CO2). Its
the dry methane reforming (DMR) unit is coupled to simul- modeling and simulation flowsheet is shown in Fig. 2. Before CH4
taneously consume greenhouse gases (CH4 and CO2) for enters the DMR reactor, it is firstly mixed with CO2 recycled from
additional syngas production (CH4 þ CO2 / 2H2 þ 2 CO). the AGR unit, then is preheated to 650  C in a heat exchanger. The
Because the H2/CO ratio of the syngas from the DMR unit is main chemical reactions of the DMR reaction are shown in Eqs.
about 1.0 [19], the WGS unit is still needed in the D-SCtEG (1)e(4) [22], which are reacted at 900  C [23] and 0.1 MPa [24]. Cui
process. et al. [25] compared the activity of a series of transition metals in
(c) S-SCtEG process: In this process, a SMR unit is integrated to the DMR reaction, and found the activity order of these catalysts is
make up hydrogen and simultaneously increase the H2/CO Ni > Ir > Pt > Pd, hence the Ni/Rh/Al2O3 catalyst is selected and
ratio of the syngas up to 2. Because the H2/CO ratio of the modeled by the RPlug model with the Langmuir-Hinshelwood re-
syngas produced from the SMR reaction (CH4þ H2O / action rate equation in terms of its kinetic parameters as list in
3H2 þ CO) is high to 3.0 [21], the S-SCtEG process can reduce Table S2. The physical property method of this unit selects the PR-
a water gas shift unit by optimizing the feed ratio of input BM method [26]. After cooled to 205  C, the output of the DMR
coal and shale gas as shown in Fig. 1 (c). Due to the SMR reactor is sent to the pressure swing adsorption device (PSA) to
reaction is a strong endothermic reaction, a combustion unit separate CO and H2 of the syngas for synthesis of ethylene glycol.
is added to meet the heat balance of the steam methane
reforming unit. Therefore, part of the cofed shale gas enters CH4þCO2/2H2þ2 CO (1)
the SMR unit, and the rest goes into the combustion unit. The
distribution ratio of shale gas of the S-SCtEG process should CO2þH2/CO þ H2O (2)
be analyzed and optimized, which will be detailed discussed
in the following section. Because the tail gas of the HCS unit 2 CO/CO2þC (3)
includes lots of CH4, CO and H2, it is also reused as the fuel gas
to provide heat for the combustion unit. CH4/2H2þC (4)
(d) D þ S-SCtEG process: The proposed D þ S-SCtEG process
avoids a WGS unit and combines the advantages of the dry
and steam methane reforming technologies as shown in
Fig. 1 (d). The cofed shale gas includes three parts: one part is 3.2. Modeling of the SMR unit
fed to the DMR unit, where CO2 is reacted with methane to
produce additional syngas; another part is fed to the SMR The modeling and simulation flowsheet of the steam methane
unit to effectively increase the amount of hydrogen and H2/ reforming process is shown in Fig. 3. The CH4-rich shale gas is
CO ratio of the process; the rest is sent into the combustion divided into two parts: part of CH4 mixed with O2 from the ASU into
unit to meet the heat balance of the SMR unit. The H2/CO the methane combustion chamber, and the other part of CH4 is
ratio of the syngas can be easily adjusted by optimizing the mixed with steam and enters the steam methane reforming reactor,
ratio of shale gas in SMR and DMR units. Therefore, the WGS in which some reactions are occurred as shown in Eqs. (5)e(8)
unit is also reduced in the D þ S-SCtEG process. under the conditions of 800  C, 3 MPa, water-carbon ratio (S/C)
3.5, and the NieCo/g-Al2O3 catalyst [27]. In this work, the RPlug
model with the Langmuir-Hinshelwood reaction rate equation is
3. Process modeling and simulation used to model the steam methane reforming reactor [28], and the
physical property method selects the PR-BM method. The detailed
The overall simulation flowsheet of three proposed processes, reaction rate expression is shown in Table S2. The reaction constant,
the D-SCtEG, S-SCtEG and D þ S-SCtEG processes, are built with the equilibrium constant and adsorption constant of steam methane
aid of the common simulator, Aspen Plus. Based on the pulverized reforming reaction is shown in Table S3. After cooling down to
coal pressurization technology, this paper uses Huolinhe lignite as 260  C, the syngas needs to be purified firstly. Hence, all of syngas
the raw material, the main parameters of the selected raw coal and stream are mixed together and fed into HCS unit to produce high-
shale gas are shown in Table 1 and Table 2. Compared with the purity CO and H2.
traditional CtEG process, different methane reforming technologies
(i.e., DMR and SMR) are added in the proposed processes. Since the CH4þH2O/COþ3H2 (5)
detailed models of the overall simulation flowsheet of the tradi-
tional CtEG system are established in our previous work [19]. Thus, CO þ H2O/CO2þH2 (6)
this study is aimed to describe the modeling and simulation pro-
cedures of the above additional units and ethylene glycol synthesis 2 CO/CO2þC (7)
(EGS) unit. The kinetic parameters of the main reactions, such as
DMR, SMR and EGS reactions, are shown in Tables S1 and S2. CH4/Cþ2H2 (8)

3.1. Modeling of the DMR unit Since the steam methane reforming reaction is a strong endo-
thermic reaction, large of additional heat is required to satisfy the
Dry methane reforming technology can effectively convert and heat balance of this reaction through the combustion of shale gas

Table 1
Proximate and elementary analysis of input lignite.

Proximate analysis (wt. %, ar) Elementary analysis (wt. %, ar) LHV (MJ/kg)

M FC V A C H O N S

28.4 57.86 35.14 21.97 75.82 5.54 13.36 1.17 0.60 16.82

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Q. Yang, Q. Yang, S. Xu et al. Energy 228 (2021) 120535

Table 2
Comparison of shale gas composition between China and the United States.

CH4(%) C2H6(%) C3H8(%) CO2(%) N2(%) H2Oa H2Sa

Weiyuan 90.1e99.3 0.3e0.8 0.01e0.03 0.02e1.38 0.01e7.15 e e

Changning 97.5e99.1 0.29e0.56 0.01e0.02 0.04e0.67 0.30e0.55 0.014e0.025 e
Fuling 98.16 0.69 0.32 0.34 0.49 e
Barnett 85.45 6.58 1.92 1.66 2.78 44.9 335.3
Bakken 57.81 19.98 11.35 0.57 5.22 32.2 115.7
Eagle Ford 74.25 13.76 5.40 1.52 0.16 17.1 307.2
This work 98.3 0.85 e 0.36 0.49 e e
a
: the unit is mg/scf.

Fig. 2. Modeling and simulation flowsheet of the DMR unit.

Fig. 3. Modeling and simulation flowsheet of the SMR unit.

and fuel gas from the HCS unit. Thus, a combustion unit is added. 4. Optimization of key operational parameters
The main combustion reactions are as follows [11]:
4.1. Effect of feed ratio on the H2/CO ratio and CO2 emissions of the
CH4þ2 O2/2H2O þ CO2 (9) D-SCtEG process

CH4þ3 O2/4H2O þ CO (10) In general, the H2/CO ratio of the ethylene glycol synthesis re-
action is required to 1.85e2.05 from the actual operation experi-
2H2þO2/2H2O (11) ence in industry. In the D-SCtEG process, its H2/CO ratio can be
adjusted by changing the feed ratio of shale gas to raw coal (MSG/
MCoal) and the shift ratio of CO (aCO) [29]. The effect of the MSG/
MCoal on the aCO and mole flowrate of H2 and CO is shown in Fig. 4.
When the feed ratio of shale gas to coal is zero, the H2/CO ratio of
3.3. Modeling of DMOS, EGS and EGR units the syngas from the CG unit is only 0.46, which is far less than the
value required for synthesizing ethylene glycol. Therefore, about
The syngas, produced from the coal gasification, DMR, and SMR 51.25% of syngas (i.e., aCO ¼ 51.25%) is shifted to produce H2 for
units, should be firstly sent to the H2 and CO separation unit (HCS) increasing H2/CO ratio by water gas shift reaction. When MSG/MCoal
to produce high-purity H2 and CO. In this paper, the RCSTR model is is increased from 0 to 1.1 t/t, the mole flowrate of H2 and CO is
selected to simulate the kinetic control reaction and equilibrium gradually increased. As a result, the shift ratio of CO is gradually
control reaction of catalytic oxidation coupling reaction in the decreased from 51.25% to 40.54%. Thus, increasing of the MSG/MCoal
DMOS unit at 130  C and 0.5 MPa. The RPlug model is applied to can greatly increase the H2/CO ratio of the syngas.
model the dimethyl oxalate hydrogenation reactor at the condi- To find the optimal feed ratio of shale gas to coal, its effect on the
tions of 235  C and 3.0 MPa. The outlet of the reactor is then sent produced and consumed CO2 of the D-SCtEG process is shown in
into the ethylene glycol refinery unit to obtain high quality ethylene Fig. 5. It can be seen that the produced CO2 is gradually decreased
glycol product. The main reactions and kinetic expressions are along with the increase of the MSG/MCoal. It is mainly because that
shown in Table S2. To shorten the length of the paper, more detailed the shift ratio of CO is greatly decreased when the MSG/MCoal is
information of the modeling and simulation of the DMOS, EGS and increased. Furthermore, more and more CO2 are consumed in the
EGR units can learn from our previous works [3,19,20].
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Q. Yang, Q. Yang, S. Xu et al. Energy 228 (2021) 120535

Fig. 6. Effect of MSG/MCoal on the H/C ratio, produced H2, CO and CO2 of the S-SCtEG
Fig. 4. Effect of MSG/MCoal and aCO on the molar flowrate of H2 and CO. process.

D-SCtEG process because more and more CO2 are recycled to the from 0.53 t/t to 1.07 t/t. However, increasing the MSG/MCoal means
DMR unit and reacted with methane to increase the production of more and more shale gas are fed into the SMR unit, which is an
syngas. When the MSG/MCoal is equal to 0.72 t/t, the amount of endothermic reaction. As a result, it requires more and more fuel
produced CO2 is equal to that required for the dry methane gas burnt for meeting the heat balance of the steam methane
reforming unit. Thus, it can be determined that the optimal MSG/ reforming reaction. Simultaneously, it could lead to the increase-
MCoal is 0.72 t/t, which the shift ratio of CO is suggested to 40.54% to ment of CO2 emissions. To facilitate the comparison with CtEG and
obtain a reasonable H2/CO ratio of the syngas. D-SCtEG processes, the H2/CO ratio of the S-SCtEG process is same
to 1.9. Therefore, the MSG/MCoal of the S-SCtEG process is deter-
4.2. Effect of feed ratio on the H2/CO ratio and CO2 emissions of the mined to be 0.75 t/t.
S-SCtEG process
4.3. Effect of feed ratio on the H2/CO ratio and CO2 emissions of the
Different from the D-SCtEG process, the S-SCtEG process in- D þ S-SCtEG process
tegrates the SMR technology to adjust the H2/CO ratio of its syngas.
The effect of the MSG/MCoal on the performance of the S-SCtEG The H2/CO ratio of the D þ S-SCtEG process can be adjusted by
process is shown in Fig. 6. It can be found that the mole flowrate of changing the MSG/MCoal and the ratio of shale gas of the dry
CO and H2 is greatly increased when the MSG/MCoal is increased. reforming unit to total input shale gas (b) as shown in Fig. 7 (a) and
Because the shale gas is a hydrogen-rich resource and the H2/CO (b). When the b is increased from 0 to 1, the H2/CO ratio of the
ratio of the syngas of steam methane reforming unit is about 3.0, syngas is greatly decreased as shown in Fig. 7 (a). Due to the H2/CO
the H2/CO ratio of the total syngas of the S-SCtEG process is obvi- ratio of the syngas produced from the DMR unit is much less than
ously increased from 1.72 to 2.07 when the MSG/MCoal is increased that of the SMR unit. Increasing b means more and more shale gas
are fed into the DMR unit. When b is equal to 1, which all of shale
gas are fed into the DMR unit, the H2/CO ratio of the syngas does not
change and keeps to be 0.59 because the mole flowrate of CH4 is
greatly excessive. Therefore, even if the feed ratio is increased, the
H2/CO ratio does not change. When the b is zero, which all of shale
gas are fed into the steam methane reforming unit, the H2/CO ratio
of syngas is increased from 2.05 to 2.36 along with the increase of
MSG/MCoal due to the high H2/CO ratio of the syngas produced from
steam methane reforming unit. Hence, the excessive shale gas fed
in to the steam methane reforming unit will make the H2/CO ratio
of the syngas is higher than that of ethylene glycol synthesis
reaction.
As shown in Fig. 7 (b), too high feed ratio of shale gas to coal
leads to a large excess of methane because of the produced CO2 is
totally converted, and the H2/CO ratio of the syngas is higher than
2.0. It means that lots of precious carbon element are wasted.
Therefore, after comprehensively considering the H/C ratio of the
syngas and CO2 emissions, a reasonable feed ratio of shale gas to
coal is to 1.25 t/t with b ¼ 0.15.

5. Technical and economic analysis

Fig. 5. Molar ratio of produced and consumed CO2 with different MSG/MCoal. To find the optimal integration approach of shale gas and coal
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Q. Yang, Q. Yang, S. Xu et al. Energy 228 (2021) 120535

Fig. 7. Effect of MSG/MCoal and b on H/C ratio (a) and CO2 molar flowrate (b).

for ethylene glycol production, the technical, economic and envi-

ronmental performance of three proposed processes is analyzed
and compared in detail. The effect of the key operational conditions
on the economic performance of the above processes is discussed
via a sensitivity analysis.

5.1. Technical performance analysis

5.1.1. Carbon utilization efficiency

Carbon utilization efficiency (hc ), one of the indicators for
evaluating resource utilization efficiency, is defined as the ratio of
the total output and input carbon of the D-SCtEG, S-SCtEG, and
D þ S-SCtEG processes, which is formulated as follows [11]:

out
Fcarbon out
2FEG
hC ¼ in
 100% ¼ in þ F in
 100% (12)
Fig. 8. Total input carbon and carbon utilization efficiency of the four processes.
Fcarbon Fcoal SG

out refers to the molar flow rate of the product EG, F in and
where FEG coal 5.1.2. Exergy efficiency
in refer to the molar flow rate of carbon element contained in the
FSG Compared with energy analysis, exergy analysis based on the
input coal and gas, respectively. second law of thermodynamics can determine the location,
The total input carbon element and carbon utilization efficiency magnitude, type and source of inefficiencies of an energy conver-
of the CtEG, D-SCtEG, S-SCtEG, and D þ S-SCtEG processes are sion system [30]. Exergy efficiency (f) is used as a potential analysis
shown in Fig. 8. The total carbon input carbon of the CtEG, D-SCtEG, and evaluation tool in exergy analysis method [31]. It is defined as
S-SCtEG, and D þ S-SCtEG processes is 3.443  105 kmol/h, the ratio of the output exergy of product to the total input exergy as
1.221  105 kmol/h, 1.409  105 kmol/h, 1.224  105 kmol/h, shown in Eq. (13) [32]:
respectively. When all the processes produce 225 t/h ethylene
glycol which contain 7258.06 kmol/h carbon, the carbon utilization Exproduct ExEG
f¼  100% ¼  100% (13)
efficiency of the D-SCtEG, S-SCtEG, and D þ S-SCtEG processes are Exinput Excoal þ ExSG þ Exutilities
increased from 21.09%, 59.47%, 58.51%, and 59.33%, respectively.
The main reasons are that most of the CO2 generated by the water where ExEG refers to exergy of ethylene glycol product; Excoal, ExSG
gas shift and coal gasification units is reused in the DMR unit of and Exutilities refer to the input exergy of coal, shale gas, and utilities,
both the D-SCtEG and D þ S-SCtEG processes. Moreover, the syngas respectively.
of the S-SCtEG process does not feed into the water gas shift unit, The exergy balance of the traditional CtEG process and three
resulting in CO does not be converted into CO2. In addition, because proposed processes is established according to the modeling and
the H2/CO ratio of the syngas produced by the SMR unit of the S- simulation results as indicated in Fig. 9. The total input exergy of the
SCtEG and D þ S-SCtEG processes is much higher than that of the S-CtEG process is the lowest, 2170.56 MW, followed by the D þ S-
syngas produced by the coal gasification unit, all of the CO in these SCtEG process, 2744.76 MW, and the D-CtEG process, 2515,80 MW.
two processes is used to synthesis target product; while about 50% Due to the amount of the ethylene glycol product of the above four
of that in the CtEG process is wasted as CO2. Hence, their carbon processes are assumed to be the same, the total output exergy of
utilization efficiencies are much higher than that of the traditional these four processes is same to 1217.08 MW. As a result, the exergy
CtEG process. efficiency of CtEG, D-SCtEG, S-SCtEG and D þ S-SCtEG is 30.68%e
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Q. Yang, Q. Yang, S. Xu et al. Energy 228 (2021) 120535

Table 3
Basic parameters for calculation of total capital investment [10,20,24].

Unit Benchmark q Qref Iref(108 CNY)

ASU Oxygen supply 0.5 21.3 kg/s 2.83

CG Daily coal input 0.8 39.2 kg/s 4.84
AGR CO2 absorption 0.65 7431.8 kmol/h 2.03
WGS Material caloric value 0.67 1450 MW 2.47
HCS H2 input 0.5 21.3 kg/s 2.87
PSA H2 input 0.5 21.3 kg/s 2.83
DMOS H2 input 0.65 2845.5 kmol/h 3.45
EGS DMO input 0.65 74.21 t/h 4.86
EGR EG output 0.65 37.50 t/h 5.27
DMR Mixed gas to reforming 0.8 33451 kmol/h 3.15
SMR Mixed gas to reforming 0.8 33451 kmol/h 3.15

and Iref refer to the production capacity and investment of the

established project [20].
After the equipment investment of the above-mentioned pro-
Fig. 9. Total exergy input and exergy efficiency of the four processes. cesses is estimated, their total capital investments are obtained by
Eq. (14) as shown in Fig. 10. Compared with the CtEG process, the
total capital investment of the S-SCtEG and D þ S-SCtEG processes
48.31%, 51.34%, and 44.34%, respectively. Thus, the combination of are reduced from 12,416 CNY/t/y to 10,078 CNY/t/y and 10,338 CNY/
DMR and SMR units can greatly improve the resource utilization t/y, respectively. The main reasons are: firstly, after reducing the
and exergy efficiencies of the CtEG process. Moreover, the inte- water-gas shift unit, the additional DMR and the SMR units are
gration of hydrogen-rich shale gas into the D-SCtEG, S-SCtEG and relatively simple; secondly, the equipment investment of the coal
D þ S-SCtEG processes can greatly increase the resource and energy gasification and acid gas removal units of the proposed processes
utilization efficiencies of the traditional CtEG process. In summary, are greatly reduced along with the reduction of CO2 emissions;
compared with the traditional CtEG process, the three proposed thirdly, the equipment investment of the air separation unit is
processes have better thermodynamic performance, especially the greatly decreased since the required amount of oxygen is signifi-
S-SCtEG process. cantly decreased. However, the total capital investment of D-SCtEG
process is added from 12,416 CNY/t/y to 12,684 CNY/t/y, which is
5.2. Economic performance analysis mainly due to the additional dry methane reforming unit and the
remaining water gas shift unit in this process.
5.2.1. Total capital investment
Total capital investment (TCI) estimation is an important part of
economic analysis and plays a decisive role in project feasibility.
The TCI of construction projects mainly includes fixed capital in-
vestment (FCI) and working capital (WC) [33]. The former refers to 5.2.2. Total production cost
the costs required for equipment and facilities related to the pro- The calculation model of the total production cost (TPC) is as
duction process of the plant, mainly including equipment, instru- shown in Eq. (16) [19]. The total production cost mainly includes
mentation, installation of pipelines, electrical appliances, plant, operating costs and general expenses. The cost of raw materials,
land, engineering design and construction costs, and unforeseen water and electricity is calculated based on the corresponding
fees; while working capital refers to the costs required for the consumption and market average prices in China in 2019 as shown
maintenance of the normal operation of the plant [34]. In the early in Table 4. Assuming the service life is 20 years and the salvage
stage of the project, it can be roughly calculated based on the data value is 5%, the depreciation expense is calculated by the straight-
of similar established factories. In this paper, to evaluate the eco- line method [34]. Operating labor costs are calculated on the basis
nomic indicators of the 1.8 Mt/y ethylene glycol project, the cost of previous work [36], and the remaining product costs are calcu-
coefficient method is used to estimate the equipment investment of lated with the proportional coefficient summarized and indicated
the proposed project as shown in Eq. (14) [20]. The main parame- in Table S5 [37].
ters of the benchmark to estimate the equipment investment are
shown in Table 3. The other costs of fixed investment are estimated
using the coefficient ratio method, and calculation as shown in Eq.
(15) [35]. The specific investment range of each part is summarized
in Table S4.
!sf
Q
I ¼ Iref  q  (14)
Qref

 X 
TCI ¼ IEI 1 þ RFi (15)

where IEI is the main equipment investment; RFi is the proportional

coefficient between direct and indirect investment and equipment
investment; q is the domestic factor; sf is the production scale
factor; Q and I are the production capacity and equipment cost; Qref Fig. 10. Total capital investment of the four processes.

8
Q. Yang, Q. Yang, S. Xu et al. Energy 228 (2021) 120535

Table 4 processes is calculated and present in Fig. 12. The internal rate of
Market price of raw material, by-product and utilities. return of the D-SCtEG, S-SCtEG and D þ S-SCtEG processes are
Raw material Price(CYN/t) Byproduct Price (CYN/t) 13.64%, 18.65%, 16.43% respectively, while the traditional CtEG is
Raw coal 350 EG (superior product) 8500
only 11.19%. Since the internal rate of return of the D-SCtEG, S-
Shale gas 1.5 CYN/m3 EG (qualified product) 7480 SCtEG and D þ S-SCtEG processes are higher than the benchmark
CH3OH 2100 DMC 3846 value 12%. Therefore, the three proposed processes are considered
HNO3 1485 Mixed alcohol 2136 to be economically feasible and much better than the CtEG process.
NaOH 3400 Sulfur 1450
A high internal rate of return can guarantee higher profitability and
ability to cope with market risks. Thus, the S-SCtEG process could
be more competitive from the perspective of economic
performance.
TPC ¼ CR þ CU þ COM þ CFC þ CPOC þ CGE (16)

where CR refers to the price of raw materials; CU refers to the cost of 5.3. Sensitivity analysis
utilities; COM refers to the cost of operation and maintenance; CFC
refers to the fixed cost; CPOC refers to the plant overhead cost; and 5.3.1. Effect of the processing scale on total capital investment
CGE refers to the general expenses, mainly including sales expenses, Properly increasing the processing scale can effectively reduce
administrative expenses, research development costs, and financial the total investment of the process. The total capital investment of
costs. the CtEG, D-SCtEG, S-SCtEG and D þ S-SCtEG processes is greatly
According to the Eq. (16) and Table S5, the total production cost decreased along with the increasement of the processing scale as
of the above-mentioned four processes is indicated in Fig. 11. shown in Fig. 13. When the processing scale is increased from
Compared with the traditional CtEG process, the total production 0.3 Mt/y to 2.1 Mt/y, the total capital investment of the traditional
cost of the D-SCtEG, S-SCtEG and D þ S-SCtEG process is reduced CtEG process is decreased from by 2335 CNY/t/y, that of the pro-
from 5100 CNY/t/y to 4565 CNY/t/y, 4425 CNY/t/y, 4636 CNY/t/y, posed D-SCtEG, S-SCtEG and D þ S-SCtEG processes is decreased by
respectively. It is mainly because the cofed low-price shale gas 2566 CNY/t/y, 2566 CNY/t/y, 2789 CNY/t/y respectively. In addition,
greatly reduces the amount of the high-price coal. As a result, it the total capital investment of both the traditional and proposed
greatly reduces the cost of raw material. processes is obviously decreased when the processing scale is
increased from 0.3 Mt/y to 1.2 Mt/y; however, it is not obviously
changed when the processing scale is higher than 1.2 Mt/y. Thus,
5.2.3. Competitiveness analysis the processing scale of the new built SCtEG plant is suggested to be
The internal rate of return (IRR) is considered as one of the most higher than 1.2 Mt/y, which is also in line with the development
common used economic indicators for evaluating economic bene- trend of the CtEG industry.
fits and the feasibility of a project. It mainly evaluates the project’s
time value, service life and cash flow to measure the project 5.3.2. Effect of the raw coal price on total production cost
feasibility [38]. The IRR is specifically the discount rate when the Because the cost of raw material has a large proportion in the
present value of the capital inflow is equal to the total value of the total production cost, the effect of raw coal price on the TPC of the
capital flow and the net present value is equal to zero as formulated CtEG, D-SCtEG, S-SCtEG and D þ S-SCtEG processes is investigated
as shown in Eq. (17) [39]. The internal rate of return represents the as indicated in Fig. 14. The TPC of the four processes is lower than
profitability of the project, that is, the larger the index, the greater 4880 CNY/t if the price of coal is lower than 250 CNY/t. However, as
the profitability. Generally, when the IRR is higher than or equal to the coal price continuously increases, the TPC of the traditional
the benchmark rate of return which is assumed to 12% in this work, CtEG process is increased sharply; while that of three proposed
the project can be considered as a feasible project [40]. processes is slowly increased and not higher than 5000 CNY/t. The
main reason is that the proportion of the cost of raw coal of the
n 
X 
1
NCFi  ¼0 (17)
i¼0 ð1 þ IRRÞi

where NCFi refers to the annual net cash flow of the project in the
ith year.
The IRR of the CtEG, D-SCtEG, S-SCtEG, and D þ S-SCtEG

Fig. 11. Total production cost of the four processes. Fig. 12. Internal rate of return of the four processes.

9
Q. Yang, Q. Yang, S. Xu et al. Energy 228 (2021) 120535

impact of price fluctuations of raw coal and ethylene glycol on the

internal rate of return of the above four processes, as shown in
Fig. 15 (a) and (b). When the coal price is increased from 150 CNY/t
to 600 CNY/t, the IRR of the CtEG, D-SCtEG, S-SCtEG and D þ S-
SCtEG processes is reduced along with the increasement of the coal
price as shown in Fig. 15 (a). Moreover, the IRR of the D-SCtEG, S-
SCtEG and D þ S-SCtEG processes is significantly larger than the
benchmark rate of return, 12%, which means this process is prof-
itable. However, since coal price is higher than 300 CNY/t, the IRR of
the traditional CtEG process is lower than 12%, which means it does
not have economic competitiveness. The main reason is that the
consumption of raw coal of the D-SCtEG, S-SCtEG and D þ S-SCtEG
processes is lower than that of the traditional CtEG process, which
reduces the raw material cost, leading to reducing the TPC and
increasing the IRR.
As Fig. 15 (b) shown, the IRR of the CtEG, D-SCtEG, S-SCtEG and
D þ S-SCtEG processes is increased when the price of ethylene
glycol product is increased from 7000 to 9250 CNY/t. The IRR of the
S-SCtEG process is the highest, followed by the D-SCtEG process
and D þ S-SCtEG process. In order to obtain a higher IRR than 12%,
the ethylene glycol price of the CtEG, D-SCtEG, S-SCtEG and D þ S-
Fig. 13. Effect of the processing scale on the total capital investment. SCtEG processes is expected to be higher than 8750 CNY/t, 8200
CNY/t, 7250 CNY/t, and 7750 CNY/t, respectively. Therefore, the
economic competitiveness of the S-SCtEG process is the most sig-
nificant, followed by the D-SCtEG and D þ S-SCtEG processes.

5.4. Environmental performance

Since the proposed D-SCtEG, S-SCtEG and D þ S-SCtEG pro-

cesses are aimed to reduce the CO2 emission of the traditional CtEG
process, the CO2 emission of these processes is analyzed to compare
their environmental performance based on their carbon balance
models, which are shown in Fig. 16.
The total carbon input of the coal gasification unit of the tradi-
tional CtEG process is 34,222 kmol C/h as shown in Fig. 16 (a). After
the coal gasification unit, 10,932 kmol C/h carbon is required to be
shifted in the water gas shift unit where CO is converted into CO2 to
increase the amount of H2. These produced CO2 containing
12,942 kmol C/h carbon are discharged after the acid gas removal
unit. Finally, 9090 kmol C/h carbon is used to produce ethylene
glycol product.
As Fig. 16 (b) shown, the input carbon of the coal gasification
unit of the D-SCtEG process is reduced from 34,422 kmol C/h to
6457 kmol C/h due to the D-SCtEG process introduces the
hydrogen-rich shale gas, which obviously reduces the amount of
Fig. 14. Effect of the raw coal price on the total production cost of four processes.
input coal. In addition, 5750 kmol C/h shale gas are added in the
DMR unit. From Fig. 16 (b), about 6045 kmol C/h carbon is not
converted by the water gas shift unit. 5502 kmol C/h CO2 are
proposed processes is greatly lower than that of the CtEG process. recycled into the DMR unit, and reacted with CH4 to generate the
Besides, when the price of coal is less than 250 CNY/t, the TPC of the synthesis gas for the production of ethylene glycol. Compared with
D þ S-SCtEG process is higher than that of the traditional CtEG the traditional CtEG process, the CO2 emitted from the acid gas
process; however, when it is higher than 250 CNY/t, that of the removal unit is reduced from 12,942 kmol C/h to 307 kmol C/h.
D þ S-SCtEG process is lower than the CtEG process, especially, the Besides, the carbon loss ratio of the H2/CO separation unit is
price of raw coal is relatively high. Since the price of raw coal is reduced from 168 kmol C/h to 123 kmol C/h.
general higher than 400 CNY/t, the TPC of three proposed processes As for the S-SCtEG process (shown in Fig. 16 (c)), shale gas
is much lower than that of the traditional CtEG process. In practical, containing 5750 kmol C/h carbon enters the steam methane
the S-SCtEG process has the greatest cost advantage, followed by reforming unit, and 1680 kmol C/h carbon are directly used as the
the D-SCtEG process and D þ S-SCtEG process. fuel gas of the combustion chamber in which they are converted
into CO2. Unlike the CtEG process, the S-SCtEG process avoids the
WGS unit. The synthesis gas from the CG unit is directly fed into the
5.3.3. Effect of the price of coal and ethylene glycol on internal rate AGR unit for CO2 removal reaction, which reduces the carbon loss
of return from 12,942 kmol C/h to 387 kmol C/h.
The economic benefits and competitive advantages of the pro- As for the D þ S-SCtEG process (shown in Fig. 16 (d)), the shale
posed processes will be influenced by the price fluctuations of raw gas containing 7750 kmol C/h C are divided to three parts: input
materials and target products. Therefore, this paper studies the carbon of the DMR units is 2304 kmol C/h, that of the SMR unit is
10
Q. Yang, Q. Yang, S. Xu et al. Energy 228 (2021) 120535

Fig. 15. Effect of the price of coal and ethylene glycol on the competitiveness of the four processes.

Fig. 16. Equivalent carbon balance of the four processes.

11
Q. Yang, Q. Yang, S. Xu et al. Energy 228 (2021) 120535

4886 kmol C/h, and that of the COM unit is 672 kmol C/h. The input the paper. Furthermore, for the industrial implementation of the
carbon of raw coal of this process is 4486 kmol C/h. Since it avoids SCtEG processes, their heat exchanger network and water network
the water gas shift unit, the carbon discharged from the AGR unit is should be paid more attention for the degree of integration of those
decreased to 493 kmol C/h CO2, which is mixed with 672 kmol C/h processes is increased.
CO2 emitted from the combustion chamber and fed into the DMR
unit to react with CH4 for the production of CO. There are the
6. Conclusions
9592 kmol C/h syngas in total is then sent into the H2/CO separation
unit.
Three novel shale gas assisted coal to ethylene glycol processes
are proposed to improve the technoeconomic performance and
5.5. Comprehensive comparison reduce the CO2 emissions of the traditional CtEG process. The key
operational conditions of the proposed processes are investigated
To compare the comprehensive performance of the D-SCtEG, S- and optimized after modeling and simulation. Then the technical,
SCtEG and D þ S-SCtEG processes with the traditional CtEG process, economic and environmental performance of the D-SCtEG, S-SCtEG
their processing capacity is same to 1.8 Mt/y. Hence, the main and D þ S-SCtEG processes are analyzed and compared with those
evaluation metrics of these processes are indicated in Table 5. Due of the traditional CtEG process. The results show that compared
to the D-SCtEG, S-SCtEG and D þ S-SCtEG processes introduce with the traditional CtEG process, three proposed processes have a
hydrogen-rich shale gas to optimal the H2/CO ratio of syngas, their better performance in carbon utilization efficiency, exergy effi-
input coals are reduced by 2.6 t/t, 2.6 t/t, and 2.73 t/t, respectively. ciency, economic benefit, and CO2 emission. Specifically, the main
Since the S-SCtEG process has no water gas shift unit, its CO2 conclusions are obtained as follows:
emissions are reduced from 3.46 t/t-EG to 0.35 t/t-EG. Moreover,
the D-SCtEG and the D þ S-SCtEG processes can achieve zero (1) The optimal feed ratio of shale gas to coal of the D-SCtEG, S-
emission because the additional methane dry reforming unit can SCtEG and D þ S-SCtEG processes is 0.72 t/t, 0.75 t/t, 1.25 t/t,
completely utilize the CO2 emissions for the production of syngas. respectively. The optimal shift ratio of CO of the D-SCtEG is
As a result, the carbon efficiency of the D-SCtEG, S-SCtEG and D þ S- 40.54%, and the feed ratio of shale gas of the dry reforming
SCtEG processes is significantly larger than that of the CtEG process. unit of the D þ S-SCtEG process is suggested to 0.15.
After system integration, the exergy efficiency of the D-SCtEG, S- (2) The technical performance of three proposed processes is
SCtEG and D þ S-SCtEG processes is increased from 30.68% to better than that of the traditional CtEG process. Compared
48.31%, 51.34%, and 44.34%, respectively. Namely three proposed with the traditional CtEG process, the carbon utilization ef-
processes have better technical performance than that of the CtEG ficiency of the D-SCtEG, S-SCtEG and D þ S-SCtEG processes
process. Since the processing capacity of the coal gasification and has increased by 38.39%, 37.42% and 38.24%, respectively. The
acid gas removal units is greatly decreased and the methane exergy efficiency of the D-SCtEG, S-SCtEG, and D þ S-SCtEG
reforming technologies are relatively simple, the total capital in- processes are increased by 17.70%, 20.66% and 13.66%,
vestment of the S-SCtEG and D þ S-SCtEG processes is reduced by respectively.
18.83% and 16.74%. In addition, the total production cost of the D- (3) Three proposed processes have better economic perfor-
SCtEG, S-SCtEG and D þ S-SCtEG processes is saved by 10.48%, mance compared with the traditional CtEG process. In
13.23%, and 9.09%, respectively. As a result, the internal rate of re- particular, the total production cost of the D-SCtEG, S-SCtEG
turn of the D-SCtEG, S-SCtEG, and D þ S-SCtEG processes is and D þ S-SCtEG processes are saved by 10.48%, 13.23%, and
improved from 11.90% to 13.64%, 18.65%, and 16.43%, respectively. 9.09%, respectively. The internal rate of return of the D-
Therefore, all of three proposed processes can greatly increase the SCtEG, S-SCtEG and D þ S-SCtEG processes is increased by
technical, economic and environmental performance of the tradi- 2.45%, 7.46%, 5.24%, respectively.
tional CtEG process, especially the S-SCtEG, and D þ S-SCtEG (4) Compared with the traditional CtEG process, the CO2 emis-
processes. sions of the S-SCtEG process is reduced from 3.46 t/t-EG to
Although this study only discusses lignite as the raw material, 0.35 t/t-EG. Furthermore, the D-SCtEG and D þ S-SCtEG
three proposed shale gas assisted coal to ethylene glycol (SCtEG) processes can achieve zero CO2 emission. Thus, the envi-
processes are also suitable for anthracite, hard coal, brown coal and ronmental performance of three proposed processes is better
lignite by adjusting the feed ratio between coal and shale gas. Their than that of the traditional CtEG process.
technical, economic and environmental performances can be
analyzed in terms of the above established system analysis models, Therefore, all of three proposed processes can greatly increase
which will be discussed in our next work to shorten the length of the technical, economic and environmental performance of the

Table 5
Material comparison between the CtEG, D-SCtEG, S-SCtEG and D þ S-SCtEG processes.

Item CtEG D -SCtEG S-SCtEG D þ S-SCtEG

Input Raw coal(t/t-EG) 3.17 0.57 0.57 0.44

Shale gas(kmol$h1/t-EG) 0 1.58 1.64 2.14
Oxygen(t/t-EG) 1.51 0.87 1.06 0.94
Water(t/t-EG) 25.6 20.57 19.37 19.05
Electricity (kw h/t-EG) 1575 2766 1031 2357
Output Ethylene glycol (Mt/y) 1.80 1.80 1.80 1.80
Carbon utilization efficiency (%) 21.09 59.47 58.51 59.33
Exergy efficiency (%) 30.68 48.31 51.34 44.34
Total capital investment (CNY/t/y) 12,416 12,684 10,078 10,338
Total production cost (CNY/t) 5100 4565 4425 4636
Internal rate of return (%) 11.90 13.64 18.65 16.43
Process CO2 emission (t/t-EG) 3.46 0 0.35 0

12
Q. Yang, Q. Yang, S. Xu et al. Energy 228 (2021) 120535

traditional CtEG process. integration of shale gas to methanol. ACS Sustainable Chem Eng 2013;2(1):
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Qingchun Yang, Conceptualization, Writing e review & editing, [16] He C, You F. Toward more cost-effective and greener chemicals production
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curation, Writing e original draft, Simin Xu, Conceptualization, [17] Yang M, You F. Comparative techno-economic and environmental analysis of
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