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PII: S0098-1354(17)30232-6
DOI: http://dx.doi.org/doi:10.1016/j.compchemeng.2017.05.023
Reference: CACE 5825
Please cite this article as: Ortiz-Espinoza, Andrea P., Noureldin, Mohamed
MB., El-Halwagi, Mahmoud M., & Jiménez-Gutiérrez, Arturo., Design,
simulation and techno-economic analysis of two processes for the
conversion of shale gas to ethylene.Computers and Chemical Engineering
http://dx.doi.org/10.1016/j.compchemeng.2017.05.023
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Design, simulation and techno-economic analysis of two processes
for the conversion of shale gas to ethylene
a
Departamento de Ingeniería Química, Instituto Tecnológico de Celaya, Celaya, Gto. 38010, México
b
Chemical Engineering Department, Texas A&M University, College Station, Texas 77843, U.S.
c
Chemical and Materials Engineering Department, King Abdulaziz University, Jeddah, Saudi Arabia
21589
Highlights
In addition to its use for energy, shale gas can be converted into value-added chemicals
Two processes for the conversion of shale gas to ethylene are presented
Abstract
Shale gas is being considered as feedstock for the production of major petrochemicals. One such
chemical is ethylene. Although the typical production for ethylene is carried out via thermal
cracking, alternative processes have been gaining importance recently. Among such alternatives
are the Oxidative Coupling of Methane (OCM) and the Methanol to Olefins (MTO) processes.
The first one is a direct conversion process while the second one involves several stages. The
aim of this work is to carry out an economic, energy and environmental assessment for these two
processes. The results show that the MTO process is more profitable under the economic and
technical scenario considered here. A sensitivity analysis was conducted to show the shale gas
and ethylene prices under which the OCM process would be economically attractive. An analysis
on catalyst improvement needed for the OCM process to be profitable is also reported.
Keywords: Shale gas; Ethylene; Oxidative coupling of methane; Methanol to olefins; Techno-
economic analysis; CO2 emissions.
Introduction
The new techniques developed for the extraction of unconventional gas have increased the
availability of natural gas during the last 10 years. Particularly, the combination of horizontal
drilling and hydraulic fracturing has made shale gas available in large quantities. Shale gas is
natural gas extracted from low permeability rocks called shale (Wang et al., 2014). By the year
2012, shale gas reached 40% of the natural gas supply in the U.S., and it is projected that by the
year 2040 it will cover 50% of the natural gas consumption in the U.S. (EIA, 2014a). Such
availability of shale gas has led to a reduction in the price of natural gas, and its use as a
feedstock for the production of valuable chemicals has been encouraged in addition to its use as
an energy source.
The main component of shale gas is methane, but in contrast to the conventional natural gas the
shale contains impurities such as nitrogen, carbon dioxide and light hydrocarbons, and
additionally the composition varies depending on the location of the play. These facts cause the
treatment for shale gas to be different from those existing for natural gas (Bullin and Krouskop,
2009). Therefore, the analysis of the possible processes that can be part of a supply chain of
shale gas is needed.
The production of chemicals such as methanol from shale gas has been recently analyzed
(Ehlinger et al., 2014; Julián-Durán et al., 2014), and there are other chemicals of major
importance that are worth of consideration. One such case is ethylene. The typical process for its
industrial production is the thermal cracking of naphtha or NGL from natural gas; however,
alternative processes in which methane is used as feedstock have been gaining recent
consideration (Sundaram et al., 2010). Among such alternatives, the Oxidative Coupling of
Methane (OCM) and a process using the Methanol to Olefins (MTO) technology stand out. The
OCM is a direct conversion process in which methane is converted into ethylene with a catalytic
reactor. In this process the purification stage consists of the removal of byproducts such as CO2
and water, and a series of cryogenic distillations to recover ethylene (Godini et al., 2013). On the
other hand, the production of ethylene via methanol involves three main stages. First, natural gas
has to be reformed to obtain synthesis gas, a mixture of CO and H2. Then, the synthesis gas is
sent to a reactor where crude methanol is synthesized (Ehlinger et al., 2014; Julián-Durán et al.,
2014). Finally, the crude methanol is converted into ethylene using a catalytic reactor, where
other low weight olefins are also produced (Barger et al., 2003).
This work aims to evaluate the profitability of the OCM and MTO processes for the production
of ethylene considering shale gas as a feedstock. The analysis is based on simulations using the
Aspen Plus process simulator. Considering a specific source for the shale gas, the objectives of
this work are: (a) to develop the flowsheets and conduct simulations for the two processes for the
production of ethylene, (b) to estimate the profitability and the environmental impact of each
process, (c) to perform an energy analysis to show the potential for heat integration and its effect
on process profitability, and (d) to carry out a sensitivity analysis in order to assess the effect of
different prices for ethylene and shale gas on the profitability of the processes.
OCM process
The OCM is a direct conversion process where methane from purified shale gas is converted into
ethylene using a catalytic reactor. This process has been investigated for several years, but its
industrial implementation has been compromised due to its medium conversion and selectivity
(Gradassi and Green, 1995; Zaman, 1999). Despite this factor, the process offers some potential
due to its exothermic characteristic and, since it is a direct process, it shows a simple flowsheet.
The purified shale gas and oxygen, obtained from an air separation unit, are fed to the OCM
reactor. The OCM reactor operates at 825 °C and atmospheric pressure (1.1 bar); the selectivity
and conversion used in this work were 0.40 and 0.45 respectively. There are several reactions
that take place, as shown in Table 3 (Godini et al., 2013). The reactor was modeled with a RStoic
module in ASPEN Plus. Since the reactor operates at high temperatures, a combustion reaction
takes place, generating high amounts of CO2 and water as by-products, thus affecting the process
downstream. The outlet stream of the reactor, containing ethylene and other by-products such as
water, CO2 and ethane, is sent to a multi-stage compressor where water is removed and pressure
is adjusted to 11 bar. Then, a cooler is used to lower the stream temperature to 40°C, after which
a CO2 removal process is used. There are different alternatives for the removal of CO2, but one
of the most widely used is the separation via absorption with amines such as MEA. Godini et al.
(2013) reported an experimental test for the OCM process, in which amine absorbers and a
combination of absorber and membrane units were tested at a mini scale plant. Removal of CO2
using this technique reached almost 100%, so this technology was considered in the simulation
of this process. After this stage, the stream is sent to a compressor, where the pressure is adjusted
to 35 bar, and finally it undergoes a series of cryogenic distillations where the unreacted methane
and other light gases are recovered for recycling, and ethane and ethylene are separated (Godini
et al., 2013). All distillation columns were modeled in Aspen Plus with RadFrac modules.
Ethylene was assumed to be required with a purity of 98% mass. The general flowsheet for the
process is shown in Figure 1. The compositions and operating conditions of the main streams of
the process, obtained from Aspen Plus simulations, are presented in Table 4.
MTO process
The production of ethylene using the MTO technology consists of three main stages. The first
stage is the reforming of the purified shale gas, which is converted to syngas. There are different
alternatives for the reforming stage, such as partial oxidation, steam reforming, dry reforming
and autothermal reforming (Noureldin et al., 2014; Martínez et al., 2014). Steam methane
reforming (SMR) has been reported as the predominant commercial technology for the
production of syngas (Noureldin et al., 2014), and it was chosen as the reforming alternative in
this work. The reactions occurring during the reforming stage are (Martínez et al., 2014),
The output of the reactor (modeled in Aspen Plus as an RPlug reactor model) is cooled, and the
unreacted syngas is separated in a flash unit and recycled to the methanol reactor at a 0.5 ratio.
Since methanol is to be used as a feedstock, the purification stage is not required.
The final stage is the Methanol-to-Olefins process, where the crude methanol is sent through a
catalytic reactor that uses the silicon aluminophosphates (SAPO-34) catalyst, which provides
high selectivity to small linear olefins. The main reactions for the conversion of methanol to light
olefins are (Vora et al., 1997),
The product distribution was calculated according to the data reported by Vora et al. (1997), as
shown in Table 5. The MTO reactor was modeled as a RYield reactor with an operation
temperature of 450 °C and pressure of 1.5 bar.
The outlet stream of the MTO reactor is quickly cooled in a quenching tower, followed by a
purification process, which consists of the removal of CO2 and water using an absorber and a
dryer, followed by the use of de-methanizer, de-ethanizer, de-propanizer and de-butanizer
columns, as well as C2-splitter and C3-splitter columns. The product streams consist mainly of
ethylene and propylene, containing other lights olefins (Ren et al., 2008). A general flowsheet of
the overall process is shown in Figure 2, with streams details given in Table 6. One can notice an
additional unit next to the MTO reactor in which air is used for catalyst regeneration by burning
the coke formed during the reaction. All the distillation columns where simulated in Aspen Plus
using RadFrac models.
Economic evaluation
For the economic analysis, an operating period of 7,920 hours per year was assumed, along with
a tax rate of 30%, a 10 year linear depreciation scheme, and a salvage value of 10%. Fixed (FCI)
and working capital investment (WCI) were taken as 85 and 15% of the total capital investment
(TCI) (El-Halwagi, 2012). Estimations of FCI of each process were made using the six-tenth rule
from reported data for plants with similar technologies (Godini et al., 2013; Julián-Durán et al.,
2014; Wu, 2010; Vora et al., 2013; Chen et al., 2004).
The profitability of each process was estimated from return on investment (ROI) values (El-
Halwagi, 2012):
(𝐴𝑛𝑛𝑢𝑎𝑙 𝑖𝑛𝑐𝑜𝑚𝑒𝑠 − 𝑂𝑝𝑒𝑟𝑎𝑡𝑖𝑛𝑔 𝑐𝑜𝑠𝑡𝑠 − 𝐴𝑛𝑛𝑢𝑎𝑙𝑖𝑧𝑒𝑑 𝑓𝑖𝑥𝑒𝑑 𝑐𝑜𝑠𝑡)(1 − 𝑡𝑎𝑥 𝑟𝑎𝑡𝑒) + 𝐴𝑛𝑛𝑢𝑎𝑙𝑖𝑧𝑒𝑑 𝑓𝑖𝑥𝑒𝑑 𝑐𝑜𝑠𝑡
𝑅𝑂𝐼 = ∗ 100
𝑇𝐶𝐼
Ethylene price was set at $0.65/lb for both processes, and for the MTO process the price for the
propylene byproduct was taken as $0.75/lb. The cost of shale gas and water for steam were
assumed at $3.50/kscf (equivalent to $3.50/MMBtu) and $0.74/m3 respectively (Ehlinger et al.,
2014; El-Halwagi, 2012). Lifetime of the catalysts was not considered as part of the operating
costs estimation.
Table 9 summarizes the main results for each process. Although the MTO plant requires a higher
TCI, a suitable ROI value of about 30% was obtained, while the OCM process reaches only a
ROI of about 6%, which is under commonly accepted values. Jasper and El-Halwagi (2015) have
recently reported an economic analysis of the MTO process to produce propylene, with ethylene
as byproduct; similar ROI values were reported as the ones obtained in this work for ethylene
production (with propylene as byproduct) based on that technology. The fairly complex nature of
the MTO flowsheet, on the other hand, might affect its potential implementation to replace the
well-established processes based on ethane cracking.
The results for the OCM-based process for ethylene production are consistent with reports
regarding its rather low perspectives for commercialization. Primarily, issues on the reactor
section due to combinations of high conversion and low selectivity, or high selectivity with low
conversions, as well as catalyst deactivation at high temperatures have been highlighted (Jašo et
al., 2010; Salehi et al., 2016).
Sensitivity analysis
A sensitivity analysis was used to see how ROI values change for different product and
feedstock prices. Figures 3 and 4 show the effect of ethylene prices, ranging from $0.5 to $0.9
per pound, and shale gas prices, ranging from $2/kSCF to $6/kSCF. If ROI of 15% is taken as an
acceptable value (Ehlinger et al., 2014), one can see that the MTO process is attractive for almost
any price of ethylene and shale gas. For the OCM process to be profitable, the market price for
ethylene would need to be raised from 0.65 to $0.70/lb, or shale gas prices reduced from $3.5 to
about $3.0 /kscf.
Environmental Assessment
The environmental impact caused by each process was assessed through estimations of CO2
emissions. CO2 equivalents for the outlet streams of each process were obtained from Aspen Plus
simulations, while CO2 emissions from electricity consumption were assessed using a factor of
0.73 MT of CO2/MWh (EIA, 2014b). Finally, the emissions related to the use of heating utilities
were estimated using the EPA method for stationary combustion sources (EPA, 2008), which
involves the determination of carbon content of fuel combusted and applying that to the amount
of fuel burned. The estimation were carried out using the following equation,
𝑘𝑔 44 𝑘𝑔 𝑜𝑓 𝐶𝑂2
𝐶𝑂2 𝑒𝑚𝑖𝑠𝑠𝑖𝑜𝑛𝑠 ( ) = 𝐹 ∗ 𝐻𝐶𝑓𝑢𝑒𝑙 ∗ 𝐶𝑓𝑢𝑒𝑙 ∗ ( )
𝑑𝑎𝑦 12 𝑘𝑔 𝑜𝑓 𝐶
where F accounts for the fuel used for combustion in SCF/day, HCFuel represents the fuel heat
content, and CFuel is the coefficient for fuel carbon content. For the fuel, natural gas was assumed
with a heat content of 1,029 BTU/SCF and a carbon content coefficient of 14.47 kg of
carbon/MMBtu.
The estimation of CO2 emissions for each process is shown in Table 10. Since CO2 equivalents
for outlet streams of both processes were taken into account, the MTO process, in contrast to its
suitable ROI values, showed a higher carbon footprint. This is due to the purge streams located
after the methanol reactor that contain mainly syngas, which is translated into a high amount of
CO2 equivalents. This effect could be reduced by adjusting the recycling ratio to a value higher
than 0.5, or by using these streams as feedstock for another process. In order to find out the
relation between recycling ratios and CO2 emissions, different values were tried for the recycling
ratio of syngas. Table 11 shows the results obtained from this analysis. As can be seen, the
environmental impact of the MTO process could be reduced to a value that is comparable to the
impact of the OCM process at the same time that the profitability of the process increases,
making the MTO process a more attractive option.
Conclusions
Two processes for the production of ethylene from shale gas based on methanol-to-olefines and
oxidative coupling of methane have been analyzed. The analysis was aided by the use of the
Aspen Plus process simulator. The economic analysis of the two alternatives under consideration
showed that the MTO process had a higher ROI value than the OCM process. To examine the
role of the ethylene product and shale gas prices, set at market values of $65/lb and $3.5/kSCF, a
sensitivity analysis was conducted, which showed that the OCM process could only achieve an
attractive ROI at prices of ethylene above $0.70/lb or shale gas prices lower than $3/kSCF. This
drawback of the OCM process could be overcome if the catalyst performance could be enhanced
with respect to the information obtained as a basis for this study. A sensitivity analysis on the
catalyst performance was carried out in order to find the improvement needed to achieve an
acceptable ROI for the OCM process. The results showed that an increase in the selectivity of 5-
10% and an increase of 5-15% in conversion could make the OCM process profitable.
Information found about the starting of a demonstration facility to produce ethylene via OCM
(Greenwood, 2014) suggests that it is possible to achieve this target; however the yield or any
information about the performance of the catalyst was not available to the authors.
Both processes showed energy integration potential and the estimation of energy targets
indicated that they could reduce their heating requirements to zero, and that it is possible to
implement cogeneration processes to generate electricity for their own consumption. Even when
energy integration would contribute to the profitability of the processes, the analysis for the
OCM technology shows that this process would only be profitable if complete integration that
included heat content of process streams as well as heat duties of distillation columns was
implemented.
From an environmental point of view, the MTO process, in contrast to its superior economic
performance, showed a higher environmental impact than the OCM process. However, changes
on the process design, such as the recycling ratio of syngas after the methanol synthesis step,
could be considered to reduce its environmental impact and make it comparable to the OCM
process.
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CAPTIONS FOR FIGURES
Table 5. Products distribution for the MTO reaction (Vora et al., 1997).
Feed, MTA Products, MTA Yield on C basis (%)
Methanol 2,330 - -
Ethylene - 500 49.0
Propylene - 327 32.0
Butylene - 100 10.0
C5 + - 22 2.0
H2,C1,C2,C3, saturates - 35 3.5
CO2 - 5 0.5
Coke - 31 3.0
Water - 1,310 -
Total 2,330 2,330 100.0
Table 6. Key streams for the MTO process
Component Units Pure Shale Gas Steam H2 Syngas Purge Gas Crude Methanol Tail gas Ethane Propane Mixed C4 C5+ Propylene Ethylene
Methane kg/h 253,079.0 0.0 987.9 37,842.6 652.7 349.3 1,104.5 0.0 0.0 0.0 0.0 0.0 0.2
Ethane kg/h 478.5 0.0 0.1 1.9 0.1 0.2 0.0 1,083.7 47.4 0.0 0.0 0.0 21.0
Propane kg/h 0.1 0.0 0.0 0.0 0.0 0.0 0.0 0.1 19,613.8 1.0 0.0 204.5 0.0
Carbon Dioxide kg/h 3,515.3 0.0 196.8 12,592.0 237.9 2,926.5 0.0 0.0 0.0 0.0 0.0 0.0 0.0
Nitrogen kg/h 995.9 0.0 24.7 959.8 9.3 2.1 0.0 0.0 0.0 0.0 0.0 0.0 0.0
Water kg/h 0.0 775,108.0 93.0 1.5 0.0 372.8 0.0 0.0 0.0 0.0 0.0 0.0 0.0
Hydrogen kg/h 0.0 0.0 27,457.8 16,563.8 48.1 1.3 1,104.7 0.0 0.0 0.0 0.0 0.0 0.0
Carbon Monoxide kg/h 0.0 0.0 9,184.7 98,060.4 523.9 41.3 316.3 0.0 0.0 0.0 0.0 0.0 0.0
Methanol kg/h 0.0 0.0 0.0 3,942.9 9.7 290,508.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0
Ethylene kg/h 0.0 0.0 0.0 0.0 0.0 0.0 0.3 25.7 0.0 0.0 0.0 0.0 63,109.4
Propylene kg/h 0.0 0.0 0.0 0.0 0.0 0.0 0.0 41.0 0.0 2.4 0.0 37,030.6 0.0
Butanes kg/h 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 12,615.2 4.4 0.0 0.0
Pentanes kg/h 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 0.0 2.0 2,775.2 0.0 0.0
Total Flow kg/h 258,069.0 775,108.0 37,944.9 169,965.0 1,481.6 294,202.0 2,525.8 1,150.5 19,661.2 12,620.6 2,779.7 37,235.2 63,130.6
Temperature °C 26.0 223.0 39.5 45.0 0.0 0.0 -163.0 -6.6 71.2 66.0 108.2 52.3 -28.5
Pressure Bar 26.0 25.0 20.0 75.0 10.0 10.0 8.8 20.4 27.0 7.6 7.6 21.9 20.4
Table 7. Raw material consumption for each process (kg/kg ethylene).
OCM MTO
Shale gas 3.26 4.09
Water 12.28
Oxygen (From air) 6.80
OCM MTO
Heating (MMBtu) 0.0092 0.0478
Cooling (MMBtu) 0.0554 0.0811
Refrigerants (MMBtu) 0.0101 0.0027
Electricity (kW-h) 6.4381 1.3071