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Analysis and performance assessment of NH3 and

H2 fed SOFC with proton-conducting electrolyte

Yildiz Kalinci a,*, Ibrahim Dincer b,c

a
Dokuz Eylul University, Izmir Vocational School, Department of Technical Programs, Education Campus Buca,
Izmir, Turkey
b
University of Ontario Institute of Technology, Faculty of Engineering and Applied Science, Mechanical Engineering
Department, 2000 Simcoe Street North, Oshawa, Ont., L1H 7K4, Canada
c
Yildiz Technical University, Faculty of Mechanical Engineering, Besiktas, Istanbul, Turkey

article info abstract

Article history: The present paper investigates the performance of a solid oxide fuel cell based on proton-
Received 4 July 2017 conducting electrolyte (SOFC-Hþ) using one-dimensional steady-state model. The analysis
Received in revised form covers a detailed electro-chemical model for H2 and NH3 fuels. The direct internal
28 July 2017 reforming of NH3 is examined, and the effects of some operating parameters (e.g. tem-
Accepted 29 July 2017 perature, pressure, fuel utilization and oxidant utilization) on the reversible cell potential
Available online xxx are investigated. In addition, the overpotentials (including activation, ohmic and concen-
tration) are calculated to study the irreversible behavior of the SOFC-Hþ with some actual
Keywords: data operating conditions and material properties taken from the literature. In addition,
Solid oxide fuel cell effects of some operation and structural parameters on cell performance were examined.
Proton conducting electrolyte The present results indicate that the activation and the ohmic losses are considerable. The
Ammonia concentration overpotential at the anode side is negligible due to the fact that H2O is
Hydrogen produced at the cathode side. The maximum power density is calculated as 3212 and
Electrochemical performance 3113 W/m2 at 1073 K and 1 atm for the fuels of H2 and NH3. The results further show that H2
provides better performance than NH3 at the same partial pressure. Moreover, NH3 is an
excellent hydrogen carrier which is a potential candidate for SOFC-Hþ due to its high
hydrogen content and considerable cell performance.
© 2017 Published by Elsevier Ltd on behalf of Hydrogen Energy Publications LLC.

according to their temperatures, such as low temperature

Introduction
Fuel cells are commonly defined as devices which can convert
chemical energy of a fuel into electrical energy, directly.
SOFCs with relatively higher operation temperatures provide
some advantages, such as fuel flexibility, internal fuel
reforming and cooperation with other systems (e.g., gas tur-
bine) [1,2]. Also, SOFCs are classified into three categories
(500  Ce650  C), intermediate temperature (650  Ce800  C),
and high temperature (800  Ce1000  C). In addition, they are
categorized based on their types, such as integrated planar,
cone-shape, flat-tube, micro-tubular and honeycomb [3,4].
From the fuel flexibility point of view, hydrogen is considered
an excellent energy carrier with some technological issues
(e.g. storage, transportation and large-scale production).
Alternatively, NH3 is proposed as a more flexible fuel (and

* Corresponding author.
E-mail address: yildiz.kalinci@deu.edu.tr (Y. Kalinci).
http://dx.doi.org/10.1016/j.ijhydene.2017.07.234
0360-3199/© 2017 Published by Elsevier Ltd on behalf of Hydrogen Energy Publications LLC.

Please cite this article in press as: Kalinci Y, Dincer I, Analysis and performance assessment of NH3 and H2 fed SOFC with proton-
conducting electrolyte, International Journal of Hydrogen Energy (2017), http://dx.doi.org/10.1016/j.ijhydene.2017.07.234
2 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y x x x ( 2 0 1 7 ) 1 e1 3
hence hydrogen carrier or storing media) at industrial scale
without carbon content [5]. At present, the total annual NH3
production is about 146 million tons which is used mainly as
fertilizer for food production [6] as well as production of
plastics, fibers, nitric acid and intermediates for dyes and
pharmaceuticals [7].
In addition, NH3 offers a significant advantages with good
volumetric and gravimetric densities that NH3 can be easily
liquefied at ambient temperature and 10 atm or 33  C under
atmosphere pressure (Note that the volumetric and gravi-
metric densities for NH3 and H2 (250 atm) are 60 (mol L1 H2),
17.6 (wt% H2) and 10 (mol L1 H2), 100 (wt% H2), respectively [8].
Some other advantages are its easy storage and transportation
with well-established infrastructure [9], carbon-free fuel,
endothermic reaction during its cracking which provides
cooling effect [10,11] and less flammability compared to other
fuels [12]. Although its leakage is easily detected by nose, it
brings some concerns about its toxicity if excessive amounts
are leaked out [13,14].
During the past decade, there has been a focused research
on SOFCs with ion conducting electrolyte. The main aim was
to improve ionic conductance of the electrolyte and cell po-
tential with high operating temperature of SOFC. However,
higher operating temperatures may bring some issues related
to durability of material, stability problems and varying ther-
mal expansion behaviors of components [15]. In this regard,
researchers have been examining the performance of proton
conductive electrolytes and SOFCs-Hþ to solve the mentioned
problems. They do not have a problem as dilution of fuel at
anode side due to creating water vapor at cathode side. Also,
reducing operation temperature diversifies using areas of
SOFCs. Some studies by various researchers are presented to
investigate the SOFCs-Hþ with performance parameters in
open the literature. Taherparvar et al. [16] examined the ef-
fects of humidification at anode and cathode in SOFC-Hþ.
They carried out the experiments at 600  C800  C using Pt/
Yb-doped SrCeO3/Pt cell. They defined that total conductivity
increased with PO2 higher than 105 atm and decreased with
respect to PH2O, suggesting that electron hole formation was
suppressed in the presence of water. In addition,
SrCe0.95Yb0.05O3a electrolyte was prepared by Zisekas et al.
[17] and studied electrode kinetics using Pd electrodes and
CO2eH2eHe mixtures at temperatures between 400  C and
700  C. They reported that while low CO2 partial pressures
(0.05 kPa and 1 kPa) had a minor negative effect on exchange
and limited currents, higher partial pressure of CO2 (98 kPa)
affected cell performance significantly. Pekridis et al. [18]
investigated the electrode polarization measurements in the
FejSrCe0.95Yb0.05O2.975jAu. According to partial pressure of
hydrogen and cell operating temperature, they defined ex-
change and limited current densities, anodic and cathodic
charge transfer coefficients as well as the corresponding en-
ergies of activation.
Another study was also presented by Dailly and Marrony
[19] who manufactured a proton conducted SOFC (35  35 mm)
consisted of NiO-BaCe0.9Y0.1O3-d/BaCe0.9Y0.1O3-d/Nd2NiO4þd as
anode, electrolyte and cathode, respectively. A modest power
density was achieved as 60 mW/cm2 at 600  C and 1000 h of
long-term measurement without electrical degradation. Also,
Medvedev et al. [20] presented a comprehensive review about
Please cite this article in press as: Kalinci Y, Dincer I, Analysis and performance assessment of NH3 and H2 fed SOFC with proton-
conducting electrolyte, International Journal of Hydrogen Energy (2017), http://dx.doi.org/10.1016/j.ijhydene.2017.07.234
proton conductive electrolytes. They focused especially on
BaCeO3 investigating co-doping, doping by nonmetallic ele-
ments and composites development.
Some researchers have focused their works on the
modeling of SOFCs. For instance, Farhad and Hamdullahpur
[21] presented a computer simulation about NH3 fuelled a
100 W portable system. They investigated the effect of the cell
operating voltage and fuel utilization ratios on voltage, excess
air, duration of operation and heat transfer of the system.
Their results showed at the cell voltage 0.73 V with fuel utili-
zation ratio of 80%, first law efficiency is 41.1%. Ni [22] studied
the thermo-electrochemical modeling of NH3-fuelled SOFCs.
They modeled NH3 thermal decomposition in the anode.
Some other modeling examples can be found from literature
[23e25].
Furthermore, the literature indicates the lack of perfor-
mance analysis and assessment studies on how to improve
the system efficiency and effectiveness for NH3 fuelled SOFC-
Hþ at intermediate temperatures. In this regard, the present
study aims to contribute to filling this gap to help engineers
and researchers for system design, analysis and improve-
ment. The originality of the study, therefore, comes from the
fact that it dwells on investigating the critical effects of
varying operating and system parameters on the cell perfor-
mance for NH3 fuelled SOFC-Hþ. The presented one-
dimensional steady state model integrates two sub-models,
i) NH3 thermal decomposition, ii) electro-chemical model to
understand the activation, concentration and ohmic over-
potential with different operational and structural parame-
ters, such as T, P, Uf, Uo, thickness, porosity, pore size.
Analysis
In this section, the performance of the H2 and NH3 fed SOFC-
Hþ is investigated as shown in Fig. 1. The analysis consists of
four main sections: i) the ammonia decomposition process, ii)
reversible cell potential, iii) overpotentials, iv) effects of some
operation and structural parameters on the cell performance.
Some assumptions for the analyses are, in this regard, given
as follows:
 The fuel cell operates at steady state condition
isothermally.
 The pressure drops along the fuel cell channels are
negligible.
NH3 or H2 H2, N2, NH3
H2
Anode
Electrolyte H+ V
Cathode H2O
O2
Air (O2, N2) O2, N2, H2O
Fig. 1 e Schematic representation of the NH3 or H2 fed
SOFC-Hþ.
 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y x x x ( 2 0 1 7 ) 1 e1 3 3

 The fuel cell body is adiabatic.

vwmax ¼ zFDfdn (10)
 Only hydrogen reacts electrochemically.
 The air composition is 79% N2 and 21% O2. where F, z, Df and dn stand for Faraday's constant 96485 C/mol
 All gases are in the ideal gas form. e, electron number transferred per mol of the fuel, electric
potential difference and mole of ions, respectively. If the
Ammonia decomposition transport is reversible, the electric potential difference be-
0
tween the electrodes is named the electromotive force, E as
When NH3 is heated; it is cracked into hydrogen and nitrogen given below:
as given below:
vwmax ¼ zFE0 dn ¼ dG (11)
NH3 40:5N2 þ 1:5H2 (1) and
The reaction is an endothermic one based on its temper-
DG ¼ zFE0 (12)
ature and pressure. The thermodynamic equilibrium of the
reaction can be taken by minimizing the total Gibbs energy
E0 ¼ DG=zF (13)
(GEM) of the reaction:

 The equation is a well-known Nernst equation and
DGsystem T;P
¼0 (2) 0
commonly used for calculating the E value of a specific
and the chemical activity of a given species i can be written for chemical reaction [27].
The reactions:
real gas:

fi Anode: H2 42Hþ þ 2e (14)

gi ¼ gi ðT; PÞ þ RT ln (3)
f0
Cathode: 2Hþ þ 2e þ 0:5O2 4H2 O (15)
For ideal gas, the activity of gas species is equal to its partial
pressure in the system. It can be modified according to this
Overall: H2 þ 0:5O2 /H2 O (16)
and adding solid or condensed species:
X The relevant parameters are written as
Gsystem ¼ ni gi (4)
DG ¼ DGðT; P0 Þ þ RT ln K (17)
X

 X 
Gsystem ¼ ni gi þ RT ln yi P þ ni gi (5)
 
gas condensed PH2 O P0
DG ¼ DGðT; P0 Þ þ RT ln
 
 0:5 (18)
The GEM requires only the standard Gibbs function of all PH2 P0 PO2 P0
species. Then, using chemical equilibrium constant K, the and for P0 ¼ 1 atm
equilibrium composition of an ideal gas mixture can be
defined as below [26]: RT PH2 O
EOCV ¼ E0 ðT; P0 Þ  ln (19)
2F PH2 P0:5
O2
aA þ bB/cC þ dD (6)
Here, E0(T, P0) may be given as a function of operating
temperature for H2-O2 cell at 1 atm pressure as follows [28]:
K ¼ eDGðT;P0 Þ=RT (7)

and E0 ðT; P0 Þ ¼ 1:253  2:4516104 T (20)

OCV
 Dv¼cþdab where, E is well known as OCV in a cell and indicates the
ncC ndD P
K¼ (8) maximum voltage obtained from a cell.
naA nbB nT
The reactants are usually supplied more than their stoi-
Here, A and B state reactants and C and Dare products. n chiometry value to tolerate any sealing or unwanted re-
and v mean, mol value and stoichiometric coefficients. actions. At this point, utilizations of fuel and oxidant are
important parameters, because some of the fuel can be
Electromotive force (E) exhausted as unused. The utilization parameters can be given
as below:
There is a force pushing charged ions from an electrode to
other in cell which is known as electromotive force, cell ðFuelÞconsumed ðH2 Þconsumed
Uf ¼ ¼ (21)
ðFuelÞsupplied ðH2 Þsupplied
voltage or cell potential as volt (V).
The direction of a chemical reaction becomes the direction
of decrease in the Gibbs free energy. When a system un- ðAirÞconsumed ðO2 Þconsumed
Uo ¼ ¼ (22)
dergoes a reversible process as isothermal and isobaric, the ðAirÞsupplied ðO2 Þsupplied
maximum work done by the system becomes [27]: here, f and o mean fuel and oxidant.
dG ¼ vwmax (9) In addition, the Faraday's law is an important law in an
electro-chemical reaction and states the flux of reactants and
In a cell system, the work is electrical work which is products according to the electric current in the electro-
defined as chemical reactions. In the electrical current, I is a linear

Please cite this article in press as: Kalinci Y, Dincer I, Analysis and performance assessment of NH3 and H2 fed SOFC with proton-
conducting electrolyte, International Journal of Hydrogen Energy (2017), http://dx.doi.org/10.1016/j.ijhydene.2017.07.234
4 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y x x x ( 2 0 1 7 ) 1 e1 3

function of the molar flows. J(J ¼ I/A) is commonly used as

current density. Two moles electrons are produced while Jde
hohm ¼ Jde re ¼ (29)
1 mol of hydrogen is consuming so: se

J here, s gives ionic conductivity of the electrolyte.

NH2 ¼ (23)
2F
Concentration overpotentials
and

J The mass transfer of uncharged species is important due to

NO2 ¼ (24)
4F the reactants and products on the catalyst layer determine the
The Nernst potential cannot be obtained practically from a fuel cell performance. To minimize the concentration loss, it
cell due to irreversibility occurred. There are three types of can be optimized at the electrodes. The mass transport in a
voltage losses, mainly, activation, ohmic and concentration porous solid is ultimately known as a complex phenomenon.
which are defined as [29]: Under a constant system pressure, the mass flux may involve
ordinary molecular diffusion, Knudsen diffusion, and surface
E ¼ EOCV  hact;a  hact;c  hohm  hcon;a  hcon;c (25) migration. The surface migration only occurs where the
diffusion gasses are adsorbed in a mobile layer and this is
here, a and c are anode and cathode. Also, there may be other
negligible in most studies of SOFCs [27]. The Knudsen diffu-
problems, such as crossover the species through the electro-
sion considers the diffusion of gas molecules through very
lyte or electrical short circuits which are not considered in the
small capillary pores. If the pore diameter is smaller than the
present study, due to their negligibility.
mean free path length of the diffusing gas molecules and the
density of gas is low, the gas molecules will collide with the
Activation overpotential
pore walls more frequently than with each other. This process
is known as Knudsen diffusion [27]. If the pore diameter is
It is the amount of voltage required to overcome the activation
larger than the mean free path length, the molecular diffusion
energy of the electro-chemical reaction which can be
will be dominant.
expressed using Butler-Volmer equation:
The effective Knudsen diffusion can be written taking into



azFhact ð1  aÞzFhact account the porosity and tortuosity of the electrode [33,34] as
J ¼ J0 exp  exp  (26)
RT RT follows:

where a is known as transfer coefficient (or symmetry factor) sffiffiffiffiffiffiffiffiffi

eff 2ε 8RT
and its value changes in the range 0 < a < 1. Indeed, it is Di;k ¼ rp (30)
3t pMi
defined according to electrode materials (such as Pt, Ni, Ag)
and chemical reactions. Experimentally, it is often found to be where ε, t and rp mean porosity, tortuosity and average pore
about 0.5. Also, J0,i is the exchange current density and rep- radius of the porous media. M is molecular mass of species.
resents the readiness of an electrode to form an electro- The effective binary diffusion of chemical species, which is
chemical reaction [11]. The activation overpotentials for known as Chapman-Enskog equation [34,35] is given as
anode and cathode can be written as follows: sffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi

eff ε 1 1 1
2RT J Dij ¼ 0:0018583 T3 þ (31)
hact;i ¼ sinh
1
; i ¼ a; c (27) t Mi Mj Ps2ij UD;ij
zF 2J0;i
Here, sij is the mean characteristic length of the molecular
Ohmic overpotentials collision diameter of species i, j and given by

si þ sj
The charge transport means both electronic and ionic charges sij ¼ (32)
2
from production to consumption stages. In the SOFC-Hþ, Hþ is
considered to cross over through the electrolyte. The resis- Also, UD, ij is the collision integral as defined by
tance to the charge transport results in voltage losses (ohmic
1:06036 0:19300 1:03587
loss) [30]. For the ohmic overpotential of SOFC by considering UD; ij ¼ þ þ
G0:15610 expð0:47635GÞ expð1:52996GÞ
the contribution of each cell components (anode, cathode,
1:76474
electrolyte, and interconnector), the Ohm's law can be given þ (33)
expð3:89411GÞ
as [31,32],
and
hohm ¼ Jðda ra þ de re þ dc rc þ dint rint Þ (28)
kT
where, d and r stand for the thickness and resistivity for G¼ (34)
εij
anode, cathode, electrolyte and interconnector.
It is a fact that the ionic transport is more difficult and pffiffiffiffiffiffiffi
εij ¼ εi εj (35)
complex than the electric conduction. In the electrolyte, the
losses are dominant and caused by the ohmic overpotentials. For gas mixtures in the anode and cathode, the diffusion
It can be mathematically written as for the electrolyte: coefficients are written as below [36]:

Please cite this article in press as: Kalinci Y, Dincer I, Analysis and performance assessment of NH3 and H2 fed SOFC with proton-
conducting electrolyte, International Journal of Hydrogen Energy (2017), http://dx.doi.org/10.1016/j.ijhydene.2017.07.234
 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y x x x ( 2 0 1 7 ) 1 e1 3 5

1 1 1 main overpotential is ohmic losses, the concentration losses

eff
¼ eff
þ eff
(36) have a lesser effect at 1 atm and 1073 K. As can be seen from
Da DH2 N2 DH2 ; k
Fig. 2, the results of the present model and the experimental
! data show a good agreement.
1 1 1 1 1  
eff
¼ eff
þ eff
þ eff
 eff
1  yN2 (37)
DO2 DO2 ; k DO2 N2 DO2 H2 O DO2 N2 Ammonia decomposition results

!
1 1 1 1 1   The equilibrium parameters depend on the chemical compo-
eff
¼ eff
þ eff
þ eff
 eff
1  yN2 (38) sition at different temperatures and pressures. The balance
DH2 O DH2 O; k DH2 ON2 DO2 H2 O DH2 ON2
compositions can be defined by the GEM methods using Eqs.


(1)e(8). As can be seen in Fig. 3, the composition of ammonia is
PH2 O eff PO2 eff
c ¼
Deff DO2 þ DH2 O (39) favorable at high temperature and low pressure. Using the
P P
GEM method, the molar fractions for the decompositions of
The concentration differences of the gas species between ammonia can be determined at every temperatures and
the electrode-electrolyte interface and the bulk become the pressures. Here, for 1 atm pressure, the molar ratios for ni-
concentration overpotential which can be given for SOFC-Hþ trogen, hydrogen, and ammonia are considered and calcu-
as follows [37]: lated as 0.0162, 0.0486 and 0.9352 at 300 K and 0.249, 0.748 and
! 0.003 at 700 K, respectively. Accordingly, it can be said that full
RT PH conversion of ammonia can be achieved at 700 K and atmo-
hcon; a ¼ ln l 2 (40)
2F PH2 spheric pressure.
Having said that there may be issues related to the
0 !0:5 1
decomposition reaction speed of ammonia. The GEM method
RT @ PO2 PlH2 O
hcon;c ¼ ln A (41) gives the equilibrium compositions without any information
2F PlO2 PH2 O
about the reaction speed. Sometimes, a chemical reaction
The partial pressures at the electrode-electrolyte interface may have a high equilibrium constant, but achieving com-
of the gas species (Pli ) are defined by the Fickian diffusions [36]: plete reaction may take longer time. NH3 thermal decompo-
sition is generally slow at low temperatures without catalyst.
!

 JRTda However, it can be improved at higher temperatures with Ni
PlH2 ¼ P  P  PH2 exp (42)
eff
2FDa catalyst. 100% NH3 conversion is possible with thin layers (a
few ten of microns) of the anode [39,40]. In addition, a com-
JRTdc plete conversion is achieved at nearly 600e650 K by employing
PlO2 ¼ PO2  eff
(43) special and expensive metal catalysts, e.g. ruthenium and
2FDc
platinum [41,42]. After checking the literature and results, one
can write that considering a full conversion of NH3 is
JRTdc
PlH2 O ¼ PH2 O þ eff
(44) conceptually reasonable enough from the view point of the
4FDc
model accuracy.
Finally, the power density for each cell is calculated as In a recent study by Appari et al. [14] on a micro-kinetic
follows: modeling of NH3 decomposition with Ni, their model was
validated by considering the temperatures ranging from 700 to
P ¼ JE (45)
1500 K and pressures ranging from 5.3 Pa to 100 kPa, respec-
tively with an experimental study of Ma et al. [8]. In the study
Results and discussion

In this section, the performance analysis and assessment re-

sults of direct H2 and NH3 fuelled SOFC-Hþ systems are dis-
cussed by considering the overpotentials. The software
Engineering Equation Solver (EES) is employed to analyze and
make the necessary calculations.

Model validation

The results of the electro-chemical model are compared with

the data taken from an experimental study by Ref. [38]. In their
experiment, a SOFC (Pt/SrCe0.95Yb0.05O3a/Pt) was used to
investigate the proton conductivity and cell performances at
different situations as fuel cell and steam electrolyzer at 1 atm
and different temperatures. Their cell performance was
calculated via the electro-chemical model. Here, the exchange
current density is taken 800 A/m2 for Pt electrodes. While the Fig. 2 e Comparison between theoretical modeling results
and experimental data from Ref. [38].

Please cite this article in press as: Kalinci Y, Dincer I, Analysis and performance assessment of NH3 and H2 fed SOFC with proton-
conducting electrolyte, International Journal of Hydrogen Energy (2017), http://dx.doi.org/10.1016/j.ijhydene.2017.07.234
6 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y x x x ( 2 0 1 7 ) 1 e1 3
Fig. 3 e Thermodynamic equilibrium of ammonia.
of Ma et al. [8], they compared NH3 and H2-fuelled SOFC at
600  C550  C. They reported that the cell efficiency was
smaller for NH3 due to the incomplete decomposition of NH3
at lower temperatures. Furthermore, Cinti et al. [10] investi-
gated the effect of decomposing ammonia (with an endo-
thermic reaction) which may help to manage the heat for a
better control of stack temperature and the cooling effect on
the NH3 decomposition.
Open cell potential (OCV) results
There are some parameters affecting the reversible potential,
such as temperature, pressure and molar ratios of gas species.
While the temperature changes from 700 to 1073 K, the
reversible cell potential decreases from 1.081 to 0.989 V at
1 atm pressure as illustrated in Fig. 4. Despite of this influence,
the high temperature provides better ion conductivity and
hence better cell performance practically. By considering the
Fig. 4 e The effects of temperature and pressure on the
OCV.
Please cite this article in press as: Kalinci Y, Dincer I, Analysis and performance assessment of NH3 and H2 fed SOFC with proton-
conducting electrolyte, International Journal of Hydrogen Energy (2017), http://dx.doi.org/10.1016/j.ijhydene.2017.07.234
effects of the varying pressure between 1 and 10 atm, as seen
in Fig. 4, increasing pressure gives a positive effect on the cell
potential, especially the rise of pressure between 1 and 3 atm.
At present, most of the fuel cells operate at atmospheric
pressure. It is a known fact that high pressures cause some
problems, related to material, durability, etc. On the other
hand, the higher pressures are required for integrated sys-
tems, such as the systems integrated with gas turbine
systems.
Also, fuel and oxidant utilization factors are considered as
important factors affecting the cell performance. While there
is H2 and N2 gas mixture taken from NH3 decomposition at the
anode side, air is used as an oxidant at the cathode side. The
partial pressures of the components at anode and cathode
sides change between input and output of the cell according to
the fuel and oxidant utilization factors. For instance, the
hydrogen molar ratio decreases from 0.74 to 0.13 with
increasing the fuel utilization (0.05e0.95) which is illustrated
in Fig. 5.
Although the high fuel utilization is desired to increase
system efficiency, it affects cell potential negatively as can be
seen in the same figure. In addition to this, a similar effect can
be seen for the oxidant utilization as well. Note that the high
oxidant utilization means that the molar concentration is less
for oxygen and more for H2O at the cathode exit. In other
words, increasing the molar concentration of H2O decreases
the OCV as shown in Fig. 6.
Overpotential results
The OCV is known as a theoretical potential which cannot be
obtained in the actual applications due to irreversibilities (so-
called: overpotentials). This section presents the overpotential
results for activation, ohmic and concentration. The input
parameters are taken from literature for the electro-chemical
analysis as listed in Table 1.
Activation overpotential results
The activation overpotential shows the energy required to
initiate the reaction. Sometimes it can be defined as an energy
barrier that the reactants have to overcome. The overpotential
depends on resistance of the electro-chemical reaction,
Fig. 5 e The effect of fuel utilization (NH3 fuel).
 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y x x x ( 2 0 1 7 ) 1 e1 3 7

resistance of electrolyte against ion transport. The ionic

transport is more complex and more influential than the
electronic charge transport, so the ionic resistance becomes
dominant in the reactions [28,30]. The ohmic overpotential
depends on three main parameters, such as the proton con-
ductivity, the electrolyte thickness and the current density, as
presented in Eq. (29). The protonic conductivity of
SrCe0.95Yb0.05O3a electrolyte at 1073 K is calculated as 0.637 S/
m, according to this, values of the ohmic overpotential change
between 0 and 0.628 V for 0e20000 A/m2 as shown in Fig. 8.

Concentration overpotential results

Fig. 6 e The effect of oxidant utilization (NH3 fuel).
Table 1 e Input parameters for the electrochemical
analysis.
Parameter
Operation conditions:
Anode/electrolyte/cathode
Operation temperature, T
Opertaion pressure, P
Fuel
Air
Uf
Uo
Material Properties:
Electrode porosity, ε
Electrode tortuosity, t
Electrode pore radius, rp
Anode supported SOFC-Hþ [34]
Anode thickness, da
Cathode thickness, dc
Electrolyte thickness, de
Electrolyte protonic conductivity, se 225.92 exp(6.3$103/T)
Electrode exchange current density, Jo 800 A/m2 [37]
There are some simultaneous activities in a fuel cell such as
transport of mass and heat as well as electric. While the re-
actants are sent to the electrochemical reaction regions, the
products have to be removed from the reaction sites to get a
steady electric production in SOFCs. So, the complex phe-
nomena consist of multi components and multi-dimensional
transport processes. The main reasons of the concentration
overpotential can be defined as i) the convective mass transfer
from the gas channel to the porous electrode ii) the diffusion
in the porous electrode iii) the slow diffusion of reactants/
products through electrolyte to/from the electrochemical re-
action regions [45].
Furthermore, the fed channels consist of H2 or H2, N2 for
Value the anode side and O2, N2, H2O for cathode side, but only H2
and O2, H2O flow in porous electrodes. The diffusion co-
Pt/SrCe0.95Yb0.05O3a/Pt [37] efficients relate to not only microstructure of the porous ma-
1073 [K]
terial (i.e., porosity, tortuosity, pore size) but also operation
1 [atm]
conditions (e.g. P, T) as given in Eqs. 30e39. The Lennard-Jones
NH3 or H2
0.21 O2þ0.79N2 intermolecular force parameters are given in Table 2, in
5% [43] addition to this, the Knudsen and binary diffusion coefficients
5% [43] are calculated and presented in Table 3.
Accordingly, H2 can pass to electrode-electrolyte interface
0.4 [37,39] quickly at anode side thanks to its high effective diffusion
5 [37,39]
coefficient. On the other hand, O2 and H2O which have high
0.5 mm [37,39]
molecular weights, diffuse in the cathode side with lower
500 mm diffusion coefficients. While the anode concentration over-
50 mm potential can be negligible, the concentration overpotential of
20 mm
(U1 m1 ¼ S/m) [37,44]

adsorption of reactants on the electrode surface and activa-

tion energy of the process. Also, it is assumed that the elec-
trochemical reactions occur at the electrode/electrolyte
interface. However, the effects of thickness of the electrodes
on the activation overpotential are considered negligible. In
the present study, the exchange current density defining
readiness of electrodes to the electrochemical reaction is
taken 800 A/m2 from Ref. [37]. According to these, the activa-
tion overpotentials for both anode and cathode side changes
from 0 to 0.335 V as shown in Fig. 7.

Ohmic overpotential results

Here, the electrical resistance represents the electrical resis-
tance of bipolar plates, cell interconnects, contacts and other
cell components, except that the ionic resistance gives the Fig. 7 e Activation overpotential.

Please cite this article in press as: Kalinci Y, Dincer I, Analysis and performance assessment of NH3 and H2 fed SOFC with proton-
conducting electrolyte, International Journal of Hydrogen Energy (2017), http://dx.doi.org/10.1016/j.ijhydene.2017.07.234
8 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y x x x ( 2 0 1 7 ) 1 e1 3

Fig. 8 e Ohmic overpotential.

Fig. 9 e Concentration overpotential.

Table 2 e Lennard-Jones intermolecular force parameters thicknesses affect the gas transport to/from TPB layers
[46]. directly. Here, the transport of hydrogen in the porous anode
Molecular Weight (kg/kmol) s (Aº) ε/k (K) is fast, so the concentration overpotential of the anode may be
H2 2.016 2.915 38 negligible. Increasing the cathode thickness hinders transport
O2 32.0 3.433 113 of O2 and H2O at cathode side, so the concentration over-
N2 28.02 3.681 91.5 potential increases as shown in Fig. 11a.
H2O 18 2.641 809.1 In the literature, considering durability of the cell, the
cathode thickness is commonly taken as 50 mm for anode
the cathode can be important at high current densities as supported SOFC-Hþ, see Refs. [10,36,37,39]. Other important
shown in Fig. 9. One may obtain from this figure that the component is the electrolyte, of which thickness affects the
current density changes from 0 to 20000 A/m2 while the con- ohmic loss directly. The proton transfer through the electro-
centration overpotential of the cathode increases between lyte is a difficult problem related to material conductivity. It
0 and 0.12 V. can be seen clearly in Fig. 11b, the higher current density and
Consequently, the most part of the overpotentials belongs thicker electrolytes may damage to the cell potential. The
to the activation losses, followed by the ohmic losses. In losses may be decreased with thin electrolytes as possible or
addition to this, the maximum power density is calculated as using high proton conductivity materials. The electrolyte
3212 and 3113 W/m2 at 7000 A/m2 for H2 and NH3. It can be thicknesses change between 8 and 50 mm for anode
seen from Fig. 10 that the cell voltage and power density reach supported-SOFC [10,36,37].
zero at about 15000 A/m2, due to the high voltage losses at
high current densities. Effect of operating temperature

Effect of thickness of main components As mentioned earlier, the effect of increasing temperature on
the OCV is negative as shown in Fig. 4. However, the
By neglecting the activation overpotential, the other over-
potential values relate to the component thicknesses.
Considering the concentration overpotentials, the electrode

Table 3 e The Knudsen and binary diffusion values.

eff
DK,i(m2/s) DK; i
(m2/s)
H2 11.19$104 0.895$104
O2 2.81$104 0.225$104
H2O 3.75$104 0.3$104
N2 3.002$104 0.24$104
eff
Dij (m2/s) Dij (m2/s)
H2-N2 6.495$104 0.519$104
O2-N2 1.816$104 0.145$104
H2O-N2 2.224$104 0.178$104
H2O-O2 2.292$104 0.183$104
Fig. 10 e Polarization curve of SOFC-Hþ.

Please cite this article in press as: Kalinci Y, Dincer I, Analysis and performance assessment of NH3 and H2 fed SOFC with proton-
conducting electrolyte, International Journal of Hydrogen Energy (2017), http://dx.doi.org/10.1016/j.ijhydene.2017.07.234
 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y x x x ( 2 0 1 7 ) 1 e1 3 9

Fig. 11 e Effects of thicknesses of main components on a) concentration overpotential b) ohmic overpotential.

Fig. 12 e Effect of operating temperature on a) ohmic overpotential b) activation overpotential c) concentration overpotential
d) power density.

Please cite this article in press as: Kalinci Y, Dincer I, Analysis and performance assessment of NH3 and H2 fed SOFC with proton-
conducting electrolyte, International Journal of Hydrogen Energy (2017), http://dx.doi.org/10.1016/j.ijhydene.2017.07.234
10 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y x x x ( 2 0 1 7 ) 1 e1 3
cumulative influence on the cell potential may be different, so
its examination with the overpotentials is important.
The ohmic overpotential is sensitive to the operating
temperature. Increasing temperature enhances proton con-
ductivity of the electrolyte, so reduces the ohmic over-
potential, considerably. As illustrated in Fig. 12a, the
conductivity of the electrolyte increases from 0.348 to 1.051 S/
m, while the temperature increases from 973 to 1173 K. Thus,
the ohmic overpotential reduces from 0.402 to 0.133 V at the
same temperature range. On the contrary, both activation and
concentration overpotentials increase with increasing tem-
peratures as shown in Fig. 12b and c, due to the fact that a
slight increase in the concentration overpotential is caused by
the gas density. It is noted that increase of the concentration
overpotential is not as significant as change of the activation
overpotential. Finally, the net effect of increasing temperature
on the power density is positive which helps in decreasing of
the ohmic overpotential importantly, as shown in Fig. 12d,
respectively.
Effect of pore size and porosity
The effect of electrode microstructure on the overpotentials
can be defined by examining the activation and the concen-
tration overpotentials. The electrode microstructure de-
termines the TPB length which influences the electrochemical
reactions near the region so the activation overpotential. Also,
the exchange current density can be determined with two
approaches in the literature. In some cases, it is assumed to be
constant. In some other cases, the effects of operation con-
ditions and structural parameters on the exchange current
density can be examined with different correlations. While
some correlations can be founded in the literature for SOFC-
O-, it is not commonly used for SOFC-Hþ [47]. Therefore, the
exchange current density is taken as constant for the activa-
tion overpotential in the study. In other words, effects of the
pore size and the porosity on the cell potential are
Fig. 13 e Effect of pore size on a) concentration overpotential b) power density.
Please cite this article in press as: Kalinci Y, Dincer I, Analysis and performance assessment of NH3 and H2 fed SOFC with proton-
conducting electrolyte, International Journal of Hydrogen Energy (2017), http://dx.doi.org/10.1016/j.ijhydene.2017.07.234
investigated by focusing on the concentration overpotential
and power density, in the study. Therefore, the present study
examines the effects of the parameters not their optimum
values.
The gas components diffuse in the porous electrodes ac-
cording to combination of Knudsen and ordinary diffusions.
The pore size obviously affects the diffusion coefficients of
the gas species. In accordance to this, increasing pore size
facilities the Knudsen diffusion and reduces the concentra-
tion overpotentials in the electrodes. While the pore size
changes from 0.5 to 3 mm, the concentration overpotential
reduces from 0.0508 to 0.0382 V. So the power density in-
creases from 3113 to 3203 W/m2 at 1073 K, as shown in
Fig. 13a and b.
In addition, the porosity has a similar effect as given in
Fig. 14a and b. Increasing porosity reduces the concentration
overpotential due to facilitating the gas diffusion in the
electrodes. As a result, increasing of the porosity from 0.3 to
0.5 enhances the power density from 3028 to 3169 W/m2 at
1073 K. But, there is an optimum porosity value which should
give the largest length of TPB to decrease the activation
overpotential.
Some related studies are available in the literature. For
instance, Patcharavorachot et al. [36] examined a planar
SOFC-Hþ which used commonly materials as Pt and
SrCe0.95Yb0.05O3a for electrode and electrolyte. They reported
that their maximum power density was 2600 W/m2 at 4800 A/
m2 for H2 fuel and 50 mm electrolyte. Another study was also
investigated by Arpornwichanop et al. [37] for CH4 fuel with
same materials. They defined 3600 W/m2 maximum power
density for Uf ¼ 0.9 and 0.6 V cell voltage. Also, Ni et al. [39]
conducted a SOFC-Hþ study using Ni based electrode and
Sm-doped Ba(CeO3) electrolyte for NH3 and H2 fuels. The
maximum power densities at anode supported system were
defined as 4800 and 4400 W/m2 at 10000 and 9000 A/m2 current
densities for H2 and NH3 (the values were roughly taken from
the respective figure).
 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y x x x ( 2 0 1 7 ) 1 e1 3 11

Fig. 14 e Effect of porosity on a) concentration overpotential b) power density.

In summary, the above listed results clearly show that NH3

Conclusions can be considered as an alternative fuel.

The present study examines electrochemical and thermody-

namic analyses of a direct ammonia and H2 fed SOFC-Hþ. The
one-dimensional steady state model consists of four main Acknowledgements
sections as the ammonia decomposition process, reversible
cell potential, overpotentials and effects of some operation The authors gratefully acknowledge the support provided by
and structural parameters on the cell performance. Some of Dokuz Eylul University, Yildiz Technical University and
the key findings of this study are listed as follows: University of Ontario Institute of Technology as well as the
Natural Sciences and Engineering Research Council of
 The cracking reaction of NH3 produces N2, H2 with un- Canada.
converted NH3. The mole fractions of the components after
NH3 decomposition are selected accordingly as 0.249, 0.748
Nomenclature
and 0.003 at 700 K for N2, H2 and NH3, respectively.
 The largest overpotential belongs to the total activation d thickness of electrode (m)
overpotential of anode and cathode. The overpotential is D diffusion coefficient (m2 s1)
calculated as 0e0.335 V for 0e30000 A/m2 current density. E cell potential (V)
 The ohmic overpotential essentially relates to conductivity f fugacity of chemical species in the system ()
and thickness of the electrolyte. The proton conductivity is F Faraday's constant (96485 C mol e1)
g specific molar Gibbs energy (J mol1)
defined as 0.6368 S/m for SrCe0.95Yb0.05O3a electrolyte at
G Gibbs energy (J)
1073 K, and the ohmic overpotential is obtained as 0.219 V
I current (A)
for 7000 A/m2. Thinner and higher proton conductive
J current density (A m2)
electrolyte materials can improve the ohmic overpotential.
J0 exchange current density (A m2)
 The gas diffusion in porous material is a very complex
K balance constant of a chemical reaction ()
issue, comprising of operating and structural parameters.
M molecular mass (g mol1)
Although the concentration overpotential is not important
at the results, it may become more dominant and influ- n number of mol (mol)
ential at higher current densities. N molar flux (mol s1 m2)
 The activation and the concentration overpotentials in- P pressure and power density (atm, Pa and W m2)
crease at higher temperature, while the ohmic over- R universal gas constant (J mol1 K1)
rp average pore radius (m)
potential decreases. Increasing temperature has a negative
T temperature (K)
influence on the OCV, while increasing temperature im-
U utilization ratio ()
proves the power density due to the reduced ohmic
v stoichiometric coefficient ()
overpotential.
W work (J)
 Larger pore sizes and porosity values improves the gas
y molar fraction of chemical species ()
diffusion and hence enhances the power density. But, It
z number of electrons transferred per mole of fuel
should be used their optimum values.

Please cite this article in press as: Kalinci Y, Dincer I, Analysis and performance assessment of NH3 and H2 fed SOFC with proton-
conducting electrolyte, International Journal of Hydrogen Energy (2017), http://dx.doi.org/10.1016/j.ijhydene.2017.07.234
12 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y x x x ( 2 0 1 7 ) 1 e1 3

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conducting electrolyte, International Journal of Hydrogen Energy (2017), http://dx.doi.org/10.1016/j.ijhydene.2017.07.234
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