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Techno-Economic Study of Hydrogen Production

via Steam Reforming of Methanol, Ethanol, and
Diesel

Seyyed Mohsen Mousavi Ehteshami & Siew Hwa Chan

To cite this article: Seyyed Mohsen Mousavi Ehteshami & Siew Hwa Chan (2014) Techno-
Economic Study of Hydrogen Production via Steam Reforming of Methanol, Ethanol, and Diesel,
Energy Technology & Policy, 1:1, 15-22, DOI: 10.1080/23317000.2014.933087

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Energy Technology & Policy (2014) 1, 1522
Published with license by Taylor & Francis Group, LLC
ISSN: 2331-7000 online
DOI: 10.1080/23317000.2014.933087

Techno-Economic Study of Hydrogen Production via Steam

Reforming of Methanol, Ethanol, and Diesel
SEYYED MOHSEN MOUSAVI EHTESHAMI* and SIEW HWA CHAN
Nanyang Technological University, Singapore, Singapore

Received April 2014, Accepted June 2014

Abstract: A large portion of industrial hydrogen is generated from the steam reforming (SR) of hydrocarbons.17 A rational choice of
fuel for hydrogen production from hydrocarbons is controversial due to the disadvantages of the fuels, including the cost, infrastructure
development, and energy efficiency of the corresponding reforming process.810 The optimum selection should be made considering all the
above factors. A techno-economic analysis of the steam reforming of strategic fuels, including methanol, ethanol, and diesel, is carried out.
The produced gas molecules, equilibrium composition of the products, appropriate operating conditions, and energy efficiency of the system
operating on corresponding fuels are studied applying the minimization of Gibbs free-energy technique. It is concluded that steam reforming
of methanol yields the most facile conversion. The appropriate steam reforming operating temperature for the studied fuels vary from low
to high temperatures, being 180220 C for methanol and up to 650700 C for other fuels. Furthermore, the economical evaluations of
the steam reforming process of the mentioned fuels provide a guideline for a rational selection of fuels for an integrated proton-exchange
membrane fuel cell and reformer system.
Keywords: Steam reforming, methanol, ethanol, diesel

1. Introduction In this study, a techno-economic analysis is carried out to eval-

A large portion of industrial hydrogen is generated from the
steam reforming (SR) of hydrocarbons.17 A rational choice
of fuel for hydrogen production from hydrocarbons is contro-
versial due to the disadvantages of the fuels, including the cost,
infrastructure development, and energy efficiency of the corre-
sponding reforming process.810 Production of hydrogen, as an
ideal energy carrier, through an economically and environmen-
tally sustainable path is an essential goal in the development
of alternative energy sources for future supply. This ideality
has produced an intensified interest in the exploration of hydro-
gen generation from various sources including hydrocarbons,
biomass, wind, solar, and nuclear energy.1118 The current sta-
tus of the hydrogen production, storage, and distribution is
not acceptable technically and economically.19,20 To develop a
hydrogen supply system fulfilling the industry requirements, con-
sidering the size and cost of the options, a wide range of fuels and
processing technologies, specifically steam reforming, have been
investigated extensively.2,5,6,2123
Seyyed Mohsen Mousavi Ehteshami and Siew Hwa Chan
This is an Open Access article. Non-commercial re-use, distribution,
and reproduction in any medium, provided the original work is prop-
erly attributed, cited, and is not altered, transformed, or built upon in
any way, is permitted. The moral rights of the named author(s) have
been asserted.
*Address correspondence to: Seyyed Mohsen Mousavi Ehteshami,
Nanyang Technological University, Singapore, Singapore. Email:
m080054@e.ntu.edu.sg
uate the energy efficiency and economical viability of methanol,
ethanol, and diesel steam reforming. The objective is to provide
a guideline for a rational selection of fuels for an integrated
proton-exchange membrane fuel cell and reformer system.
Natural gas, as the essential source of industrial hydro-
gen generation via steam reforming, includes mainly methane
(Figure 1).24 However, steam reforming of methane requires
a high operating temperature for complete conversion.3,23,25,26
Methanol as a liquid with high energy density has been well
studied because of its well-known facile reforming and availabil-
ity.27,28 Moreover, the infrastructure required for production and
distribution of methanol is not available.16,29 Therefore, other
high-energy-density liquid fuels that are abundant and obtained
more easily have been considered, such as ethanol, glycerol,
and dimethyl ether.2,4,5,3035 These fuels are environmentally
sustainable, ensuring the renewable energy nature of the pro-
cess. However, this group of fuels is not well developed and
economically and technically not viable yet. Oil-derived fuels
such as diesel, naphtha, and gasoline constitute another group
of hydrocarbons, generally called heavy hydrocarbons.16,36,37
These fuels are abundantly available and cheap. In addition,
having high energy densities, their required infrastructure is com-
mercially well developed. It should be noted that although there
might be issues regarding the low energy efficiency and non-
renewable nature of these fuels, they have the advantage of
the existing infrastructures, avoiding the economic burden of
extra capital cost required for hydrogen production. Based on
this discussion, methanol, ethanol, and diesel are considered for
this study. Some physicochemical properties of the fuels are
16 S. M. Mousavi Ehteshami and S. H. Chan

Water electrolysis Table 2. Chemical reactions of steam reforming of the fuels.

4%
Fuel Chemical reaction

Methanol CH3 OH+H2 O 3H2 +CO2

Coal gasification
18%
Steam reforming of
natural gas
48%
Steam reforming of
Naphtha
30%
Fig. 1. The main processes for producing industrial hydrogen.
presented in Table 1. In fact, a rational selection of the fuel is
debatable due to the disadvantages of the fuels, including the
cost, infrastructure development, and the energy efficiency of the
corresponding reforming process. The optimum selection should
be made considering all the effective factors.
The economic study carried out includes the evaluation of the
life cycle cost of each fuel considering several key parameters.
The goal of the economic study is to determine the feasibil-
ity of utilizing the studied fuels. The cost of raw materials and
the cost related to the greenhouse gases emission are taken into
account. The capital costs of hydrogen generation equipment and
hydrogen pumping stations are excluded from the comparison as
they will have a similar share for different fuel options. The end-
user instrument also plays a significant role in the economical
viability of the hydrogen economy. The cost of the fuel cell
driven power train in transportation applications is an essential
parameter for a convincing hydrogen energy justification. It is
necessary for governmental institutions to facilitate the appli-
cation of fuel cellpowered systems by subsidizing the price
of these systems. For example, the price of the fuel cell power
must be below US $30/kW by 2015 so that utilizing hydrogen
as the alternative fuel becomes justifiable.38 Taking into account
the effect of greenhouse gases, hydrogen and fuel celldriven
transportation would become more defendable.
2. Methodology
The thermodynamic simulations are carried out under chemi-
cal equilibrium conditions using the commercial package Aspen
Hysys, which facilitates the thermodynamic analysis of chemical
processes. Peng-Robinson equation of state is used to calculate
Ethanol C2 H5 OH+H2 O4H2 +2CO
Diesel Cn Hm +2nH2 O(m/2+2n)H2 +n CO2
the physicochemical properties of the fuels.39 The chemical
reactions of the fuels reforming are summarized in Table 2.
Diesel is considered to consist of an equi-volumetric amount of
hydrocarbons including 14 and 16 carbon atoms. The fuels under
investigation are considered to be fed into the system at room
temperature and atmospheric pressure with a constant flow rate.
The feedstock is premixed with water, and the aqueous solution
with different water-to-fuel molar ratios is pumped into the fuel
processor. The configuration of the system is depicted in Figure 2
and explained in the fuel processing section (section 2.1). Aspen
Hysys is used to calculate the composition of the products and
the energy requirements for each unit of the plant. The compu-
tational method and energy efficiency calculation is presented in
section 2.2.
2.1. Fuel Processing Unit
Figure 2 presents the configuration of the fuel steam reforming
unit integrated with a PEM fuel cell. The fuel processor includes
a reformer and a CO cleanup unit. The pre-heater section heats
up the feedstock to a higher temperature before entering to the
reformer. The reformer is considered an isothermal reactor that
is modeled by a RGIBBS module, although in the real reformer,
there are non-identical temperature profiles in the axial and
radial directions due to the endothermic nature of the reactions.
Minimization of Gibbs free energy is the basis of the calcula-
tion of products compositions. Heat integration is essential in
designing of a reforming system.40 The reactants usually have
to be heated to high temperatures and cooled down for the subse-
quent process unit. When taking into account the heat recovery/
integration, the disadvantage of high reforming temperatures will
be greatly reduced and might change the outcome of the inves-
tigation. However, since the objective of this report is to provide
a comparative evaluation of the fuels concentrating on the steam
reforming reaction, it is assumed that the heat requirements are
supplied from external heating units, for example, electric heaters
powered by the PEM fuel cell integrated with the fuel process-
ing unit. Obviously, the energy efficiency of the system would
be lower compared to others utilizing heat integration, such as
systems that couple catalytic combustors with the reformer.

Table 1. Physicochemical properties of the fuels.

Heat of Lower heating Energy Heat Flammability
Density Boiling vaporization value density capacity limits
Fuel Formula (kg.m3 ) point ( C) (kJ.mol1 ) (kJ.mol1 ) (MJ.L1 ) (J.mol1 .K1 ) (Vol. %)

Hydrogen H2 0.090 252.70 0.92 240 0.89 28.6 4.1, 74

Methanol CH3 OH 794.000 64.60 35.20 643 17.00 49.0 7.3, 36
Ethanol C2 H5 OH 790.000 78.30 38.90 1240 22.00 77.3 4.3, 19
Diesel C16 H34 0.856 120430 47.00 8080 34.20 340.0 1.0, 6
Hydrogen Production via Steam Reforming 17

Oxygen/ air

Syn gas PEM

Electrolytic fuel cell
CO removal stack
Pre-heater Pure
unit
power (Qheater) H2

Fuel-water Water
Pump
mixture

Condenser
Preheater

Pump power
(Wp) Reformer Water
condensate
Reformer
power (Qreformer)

Fig. 2. The system configuration of fuel processor-PEM fuel cell system.

 i=1 
The hydrogen-rich gas produced in the reformer can be  +
ni [Gfoi + RT lnP + RT lnyi + RT ln (i aik )] = 0
purified by several approaches, such as water gas shift reac- N k
(4)
tion, methanation and preferential CO oxidation, pressure swing
adsorption, and Pd membranes.4145 These processes are greatly
According to the experimental and theoretical studies in the lit-
dependent on the catalytic performance and operate at high tem-
erature, hydrogen, carbon monoxide, carbon dioxide, methane,
peratures. In the current study, it is assumed that an electrolytic
and acetaldehyde are considered to be present in the prod-
CO oxidation system investigated in our group is used, which
ucts.27,36,47 In the case of methanol, only hydrogen, carbon
operates at the outlet temperature of the reformer and atmo-
monoxide, and carbon dioxide are considered. The presence of
spheric pressure.46 Such a system generates pure hydrogen by
carbon is excluded as the core comparisons are made at suffi-
removing CO and other impurities available in reformate pro-
ciently high water-to-fuel ratios at which the carbon formation is
duced in the reformer. In addition, it offsets the required energy
avoided. In addition, the focus of this study is to provide a broad
by production of extra hydrogen. The power requirements of such
picture of the reforming process and to present guidelines for
a unit are negligible. Therefore, the energy analysis of the reform-
choosing the optimum fuel for hydrogen production considering
ing system is not affected. The PEM fuel cell is considered an
both the technical and economical aspects. However, for a more
adiabatic reactor (modeled by RSTOIC in Aspen Hysys), which
detailed study, the kinetics of the reactions and catalyst deacti-
operates at 80 C and 1 atm. The efficiency of the fuel cell is
vation due to the presence of solid carbon should be taken into
assumed to be 65%.
account.

2.2. Computational Method

2.3. Energy Efficiency Calculation
As mentioned, Gibbs free energy minimization method is used
The global energy efficiency of the system is calculated using
to perform the thermodynamic analysis. The system total Gibbs
equation (5):
free energy should reach a minimum at the operating temperature
when the system reaches thermodynamic equilibrium. The total Ps Paux
Gibbs free energy of the system is calculated using equation (1): = (5)
nf .LHVf
N
nG = ni G (1)
i=1 Where Ps , Paux , nf , and LHVf are the power generated by fuel cell
stack (kW), power required by all of the auxiliary units (including
Where the molar Gibbs free energy of each component G is the pump, heater, CO removal electrolyzer) (kW), the fuel molar
calculated from equation (2): flow rate (mol.s1 ) and low heating value of the fuels (kJ.mol1 ),
respectively. The fuel cell stack power is calculated consider-
f
G = Gio + RTln (2) ing the hydrogen flow rate produced from the fuel processor
fio and the fuel cell electrochemical efficiency, which is assumed
Where fi is the fugacity of the components. Therefore, the total to be 0.6.
Gibbs free energy of the system is rewritten to
  3. Economic Analysis
  f
nG = (ni Gi ) + RT
o
ni ln o (3)
fi The goal of the economic study is to determine the feasibility of
utilizing the studied fuels for hydrogen generation through the
Lagrange multiplier is then used to calculate the composition of SR process. The cost of raw materials and the cost related to the
the components at which the Gibbs free energy of the system is greenhouse gases emission and fuel efficiency of the reforming
minimized: systems are taken into account. It is desired to propose the
18 S. M. Mousavi Ehteshami and S. H. Chan

fuel that presents the optimum efficiency of the SR process to
generate hydrogen. As the fuel processing price including the
capital, operation, and maintenance costs have a similar share
for different fuel options, they will have negligible effect on the
comparative study. To calculate the greenhouse gases emission
(CO and CO2 ), the specific values of CO and CO2 production
from steam reforming of the fuels under the study are used.
5. Effect of Water to Fuel Ratio (R)
In this section, the effect of the water-to-fuel ratio on the equi-
librium composition of the products and net energy efficiency
of the system is analyzed. Figure 4 presents the equilibrium
composition of the steam reforming of the fuels under study.
The compositions of the components are presented in molar

4. Results and Discussion a)

0.8
H2
CO
A parametric study based on the developed integrated process

Equilibrium composition (mol %)

CO2
model is used to determine the optimal operating conditions of H2O
0.6
the system. The effect of reforming temperature and water-to- CH3OH
fuel ratio are considered for the parametric study. The following
procedure is used to perform the thermodynamics analysis:
0.4
required heat input is applied to the pre-heater to maintain the
reforming temperature. Having set the water-to-fuel ratio, the
feed flow rate, and the reforming temperature, the thermodynam-
ics model calculates the reformate temperature, composition, and 0.2
flow rate of the products.
Figure 3 presents the equilibrium conversion efficiency of
atmospheric steam reforming of different fuels at a water-to- 0.0
fuel ratio of 1.5. Conversion efficiency of a fuel determines 0 1 2 3 4
the percentage of the fuel that converts into products within Water/ fuel ratio / (mol/mol)

the reformer. It can be seen that methanol is converted almost b)

fully at temperatures around 200210 C, while other fuels 0.8
require higher reforming temperatures to yield high conver-
Equilibrium composition (mol %)

sion efficiencies. Ethanol also has high conversion efficien-

cies even at low temperatures (350450 C), but it should be 0.6
noted that ethanol conversion products include acetaldehyde H2
and methane besides hydrogen and CO/CO2 . In other words, CO
the high conversion efficiency necessarily does not imply the 0.4 CO2
H2O
high hydrogen production rate. To make a meaningful compar- CH4
ison among the fuels from the hydrogen generation perspective,
the composition of hydrogen along with other products should 0.2
be considered. In the case of diesel, high reforming temper-
atures (up to 650 C) are required to yield high conversion
0.0
efficiencies. 2 4 6 8
Water/ fuel ratio / (mol/mol)
c)
1.0 0.8
Equilibrium composition (mol %)

0.9
Diesel 0.6
Methanol
Conversion/ %

H2
0.8 Ethanol CO
0.4 CO2
H2O
0.7 CH4

0.2
0.6

0.5 0.0
200 400 600 800 1000 0.0 0.5 1.0 1.5 2.0 2.5 3.0
Temperature/ C Water/ fuel ratio / (mol/mol)

Fig. 3. Equilibrium conversion of atmospheric steam reforming of Fig. 4. Equilibrium composition of atmospheric steam reforming of
different fuels at water to fuel ratio of 1.5. (a) methanol at 250 C, (b) ethanol at 650 C, and (c) diesel at 650 C.
Hydrogen Production via Steam Reforming 19

percentage. Maximum values for hydrogen generation molar per-
centage are observed as R increases to 1, 4, and 2 in the case of
methanol, ethanol, and diesel, respectively.
The hydrogen equilibrium composition is observed to increase
at low R values and decrease at higher R values in the case of
methanol and ethanol. The increase is because of adding more
steam to the water-gas shift equilibrium, which leads to genera-
tion of more hydrogen. The decrease at higher R values might be
related to the lack of fuel to be steam reformed. Another obser-
vation is the decrease of CO equilibrium concentration for all the
fuels as the R value increases. It is also related to water-gas shift
concentration at higher temperatures. The formation of remark-
able amounts of methane reduces the hydrogen generation at
reforming temperatures lower than 600 C in the case of ethanol.
Similarly, the same trend is observed in the case of diesel steam
reforming. This indicates the decomposition of the fuel at lower
temperatures. With the increase in reforming temperature, the
a)
0.8

Equilibrium composition (mol %)

reaction, which extends more at higher R values, leading to the
decrease in the CO equilibrium concentration. However, it should 0.6 H2
be noted that high R value means the higher energy requirement H2O
to vaporize the water. CO
Figure 5 presents the energy efficiency of the system oper- 0.4 CO2
ating on methanol, ethanol, and diesel at 650 C. The energy CH3OH
efficiency of the system operating on different fuels increases in
the order: diesel < ethanol< methanol. The maximum energy 0.2
efficiency of the system happens at R = 1, 4, and 3 in the case
of methanol, ethanol, and diesel, respectively. Methanol with
an energy efficiency of 35% appears to be the fuel providing 0.0
the most energy-efficient system. It should be noted that the 200 400 600 800 1000
efficiency values presented in Figure 5 are calculated for the spe- Temperature/ C
cific system configuration depicted in Figure 2. Higher efficiency b)
0.8
values would be achieved if heat integration is implemented.
Equilibrium composition (mol %)

6. Effect of the Reforming Temperature 0.6

H2
In this section, the effect of reforming temperature on the equi-
CO
librium concentration of the products and net system efficiency 0.4 CO2
are investigated. Figure 6 presents the equilibrium composition of H2O
the steam reforming of the fuels under study. The compositions CH4
of the components are presented in molar percentage. A similar 0.2
incremental trend is observed for the CO equilibrium concen-
tration with the increase in reforming temperature, in the case
of all the fuels under the study. This is related to exothermic
0.0
nature of the water-gas shift reaction, which increases the CO 200 400 600 800
Temperature/ C
c)
40 0.8
EtOH
Equilibrium composition (mol %)

MeOH
Diesel
30 0.6
Enegry efficiency/ %

H2
20 0.4 CO
CO2
H2O
CH4
10 0.2

0 0.0
0 2 4 6 8 200 400 600 800
Water/ fuel ratio / (mol/mol) Temperature/ C

Fig. 5. Energy efficiency of the fuel processor: fuel cell system Fig. 6. Equilibrium composition of atmospheric steam reforming of
operating on different fuels at 650 C. (a) methanol at R = 1, (b) ethanol at R = 4, and (c) diesel at R = 2.
20 S. M. Mousavi Ehteshami and S. H. Chan

reduction of methane and increase of hydrogen production is 1.8

observed. Therefore, the temperature range required for ethanol
1.6 CO2

Specific emissions production

and diesel steam reforming would be higher than 600 C. CO

(kg of emission/kg of fuel)

Figure 7 presents the energy efficiency of the system oper- 1.4
ating on methanol, ethanol, and diesel at R = 2.5. The energy 1.2
efficiency of the system operating on different fuels increases
in the order: diesel < ethanol < methanol. According to the 1.0
model, the maximum energy efficiency of the system happens 0.8
at reforming temperatures of 200 C, 700 C, and 600 C in the 0.6
case of methanol, ethanol, and diesel, respectively. Methanol
with energy efficiency of 36.5% provides the fuel for the most 0.4
energy-efficient system. 0.2
It is essential to consider the environmental effect of the fuel
0.0
to select the best option for hydrogen production through the SR 10 Methanol Ethanol Diesel 40
process. Therefore, the corresponding specific CO and CO2 pro- Low heating value of the fuel (MJ.l1)
duction of the fuels under the study are calculated at the best
operating conditions of the steam reforming process. These con- Fig. 8. Specific emission production due to steam reforming of dif-
ditions are R = 1 and T = 250 C for methanol, R = 4 and ferent fuels (R = 1, T = 250 C for methanol, R = 4 and T = 650 C
T = 650 C for ethanol, and R = 3 and T = 650 C for diesel. for ethanol, and R = 3 and T = 650 C for diesel).
The results are presented in Figure 8, where the fuels are com-
pared from both the energy content and greenhouse emission Table 3. The economic analysis of the steam reforming process of
point of views. A negligible amount of CO is produced from the fuels.
steam reforming of methanol compared to ethanol and diesel.
The CO content of the synthetic gas is a very important factor Cost parameters
for selection of a fuel since PEM fuel cells, as the end-users, are
CO2 social cost CO social cost
much susceptible to CO concentration available in the hydrogen
Raw material US$/ kg H2 US$/ kg H2
stream.48 The CO concentration in the synthetic gas increases in
US$/ Gasoline produced from produced from
the order: methanol< ethanol< diesel. On the other hand, CO2 Fuel equiv. (l) SR SR
concentration follows a different trend, increasing in the order:
ethanol< methanol< diesel. Methanol 0.95 0.55 1.5
Table 3 presents the cost parameters of steam reforming pro- Ethanol 1.08 0.14 4.7
cess of the fuels under the study. The price components of raw Diesel 0.95 0.37 4.3
material cost and CO2 and CO emission cost are considered
in the analysis. The former components are obtained from the
International Energy Agency (IEA) databases, while the latter among the raw materials costs. Significantly different values of
ones are calculated based on the equilibrium optimum operating the social costs of greenhouse gases emission are found in dif-
conditions as points at which the hydrogen and CO/ CO2 produc- ferent studies as different approaches have been taken by other
tions are calculated per kg of fuel. There is not a big difference researchers to calculate this cost parameter.4951 Therefore, this
study considers the average social cost as observed in different
studies. Based on the current analysis, methanol appears to be a
40 more promising candidate for hydrogen generation through SR.
The focus of this study is to compare the key cost parameters
of hydrogen generation through SR. Therefore, the raw material
30 and the social costs induced by the hydrogen generation through
Enegry efficiency/ %

SR of the corresponding fuels are taken into account. Also, it

EtOH should be noted that because all the studied fuels are in liq-
MeOH
uid form, other cost parameters such as the transportation cost,
20 Diesel
infrastructure cost, and operation/maintenance costs would not
be so different. Having said the above, to have a broader view
of the cost parameters, the whole life-cycle cost of the hydrogen
10 generation should be considered.

0
7. Conclusion
200 400 600 800 1000
Temperature/ C A techno-economic analysis of the steam reforming of strate-
gic fuels, including methanol, ethanol, and diesel, is carried out.
Fig. 7. Energy efficiency of the fuel processor-fuel cell system The produced gas molecules, composition of the products, appro-
operating on different fuels at R = 2.5. priate operating conditions, and energy efficiency of the system
Hydrogen Production via Steam Reforming
operating on corresponding fuels are studied applying the min-
imization of Gibbs free-energy technique. It is concluded that
steam reforming of methanol yields the most facile conversion
exhibiting the highest energy efficiency among the studied fuels.
Water/fuel ratio and operating temperature affect the hydro-
gen and carbon oxides yield significantly. The appropriate steam
reforming operating temperature for the studied fuels vary from
low to high temperatures, being 180220 C for methanol and
up to 650700 C for other fuels. Furthermore, an economical
evaluation of the steam reforming process of the mentioned
fuels is performed. Raw material and social cost of greenhouse
gases emission are considered in the study. Based on the analy-
sis, methanol appears to be the optimum choice for production
of hydrogen via the SR process. The results obtained from the
techno-economic study would provide guidelines for a rational
selection of the optimum fuel for an integrated proton-exchange
membrane fuel cell and reformer system.
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