Solid State Ionics 135 (2000) 305–313

www.elsevier.com / locate / ssi

Advances in solid oxide fuel cell technology

S.C. Singhal*
Science and Technology Center, Siemens Westinghouse Power Corporation, 1310 Beulah Road, Pittsburgh, PA 15235, USA

Abstract

High temperature solid oxide fuel cells (SOFCs) offer a clean, pollution-free technology to electrochemically generate
electricity at high efficiencies. These fuel cells provide many advantages over traditional energy conversion systems
including high efficiency, reliability, modularity, fuel adaptability, and very low levels of NO x and SOx emissions.
Furthermore, because of their high temperature of operation ( | 10008C), natural gas fuel can be reformed within the cell
stack eliminating the need for an expensive, external reformer. Also, pressurized SOFCs can be successfully used as
replacements for combustors in gas turbines; such hybrid SOFC–gas turbine power systems are expected to reach
efficiencies over 70%. This paper reviews the materials and fabrication methods used for the different cell components, and
discusses the performance of cells fabricated using these materials; it also discusses the materials and processing studies that
are under investigation to reduce the cell cost. Finally, the paper summarizes the recently built power generation systems that
employed state-of-the-art SOFCs. A new design SOFC that combines the seal-less feature of tubular cells and a flattened air
electrode with integral ribs is also described; this new design has a shortened current path and hence lower cell resistance
and higher power output than tubular cells.  2000 Published by Elsevier Science B.V.

Keywords: Fuel cells; Oxide; Electricity (power) generation; Performance; Electrolyte; Electrodes; Gas turbine; Cost

Materials: ZrO 2 ; Y 2 O 3 ; Y 2 O 3 -stabilized ZrO 2 (YSZ); LaMnO 3 ; LaCrO 3 ; Ni

1. Introduction technology to electrochemically generate electricity

The high oxygen ion conductivity over wide
ranges of temperature and oxygen pressures in
stabilized zirconia has led to its use as a solid oxide
electrolyte in a variety of electrochemical applica-
tions. These include high temperature solid oxide
fuel cells (SOFCs) which offer a clean, pollution-free
*Present address: Pacific Northwest National Laboratory, 902
Battelle Boulevard, P.O. Box 999, Richland, WA 99352, USA.
Tel.: 11-509-375-6738; fax: 11-509-375-6605.
E-mail address: singhal@pnl.gov (S.C. Singhal).
at high efficiencies. These fuel cells provide many
advantages over traditional energy conversion sys-
tems including high efficiency, reliability, modulari-
ty, fuel adaptability, and very low levels of NO x and
SO x emissions. Quiet, vibration-free operation of
solid oxide fuel cells also eliminates noise usually
associated with conventional power generation sys-
tems. Furthermore, because of their high temperature
of operation ( | 10008C), natural gas fuel can be
reformed within the cell stack eliminating the need
for an expensive, external reformer system. Also,
pressurized SOFCs can be successfully used as

0167-2738 / 00 / $ – see front matter  2000 Published by Elsevier Science B.V.

PII: S0167-2738( 00 )00452-5
306 S.C. Singhal / Solid State Ionics 135 (2000) 305 – 313
replacements for combustors in gas turbines; such
hybrid SOFC–gas turbine power systems are ex-
pected to reach efficiencies approaching 70%. This
paper reviews the current status of the solid oxide
fuel cell technology for power generation.
2. Materials and fabrication processes
A solid oxide fuel cell essentially consists of two
porous electrodes separated by a dense, oxygen ion
conducting electrolyte. Solid oxide fuel cells in
several different designs have been investigated;
these include planar and tubular geometries. The
materials for cell components in these different
designs are either the same or very similar in nature.
Fig. 1 illustrates the design of the tubular geometry
cell. In this design, the cell components are deposited
in the form of thin layers on a ceramic cathode (air
electrode) tube. The materials for different cell
components have been selected based on the follow-
ing criteria.
(a) Suitable electrical conducting properties re-
quired of different cell components to perform
their intended cell functions.
(b) Adequate chemical and structural stability at
high temperatures during cell operation as well as
during cell fabrication.
(c) Minimal reactivity and interdiffusion among
different cell components.
(d) Matching thermal expansion among different
cell components.
Fig. 1. Tubular solid oxide fuel cell design.
In addition to the above materials selection
criteria, the fabrication processes have been chosen
so that every sequential component fabrication pro-
cess does not affect those components already fabri-
cated onto the cathode tube and to minimize the cell
fabrication cost. The materials and fabrication pro-
cesses used for different cell components are dis-
cussed below.
2.1. Cathode (air electrode)
The air electrode operates in an oxidizing environ-
ment of air or oxygen at | 10008C and participates
in the oxygen reduction reaction,
1
]O 2 (g) 1 2e 2 5 O 22 (s) (1)
2
i.e. oxygen in the gas phase is reduced to oxide ions,
consuming two electrons in the process. The air
electrode in solid oxide fuel cells has to meet the
following requirements.
(a) High electronic conductivity.
(b) Chemical and dimensional stability in en-
vironments encountered during cell operation and
during fabrication of interconnection, electrolyte
and fuel electrode layers.
(c) Thermal expansion match with other cell
components.
(d) Compatibility and minimum reactivity with
the electrolyte and the interconnection with which
air electrode comes into contact.
(e) Sufficient porosity to facilitate transport of
molecular oxygen from the gas phase to the air
electrode / electrolyte interface.
To satisfy these requirements, lanthanum manga-
nite suitably doped with alkaline and rare earth
elements is used in the form of a porous tube onto
which other cell components are fabricated. Lan-
thanum manganite is a p-type perovskite oxide and
shows reversible oxidation–reduction behavior. The
material can have oxygen excess or deficiency
depending upon the ambient oxygen partial pressure
and temperature. Although, it is stable in air and
oxidizing atmospheres, it dissociates at 10008C at
oxygen pressures #10 214 atm. The electronic con-
ductivity of lanthanum manganite is due to hopping
 S.C. Singhal / Solid State Ionics 135 (2000) 305 – 313
of an electron hole between the 13 and 14 valence
states of Mn. This conductivity is enhanced by
doping with a divalent ion such as calcium or
strontium. The defect chemistry, electrical conduc-
tion, and cathodic polarization behavior of doped
lanthanum manganites have been studied in detail
[1,2], and alkaline earth doped lanthanum manganite
has been found to satisfy all the requirements to be
an effective air electrode. Furthermore, the reactivity
and interdiffusion studies [3,4] between doped lan-
thanum manganite and yttria stabilized zirconia
electrolyte have shown any interactions between
these two materials at 10008C to be minimal.
Over 90% of the weight of a tubular SOFC is that
of the doped lanthanum manganite air electrode tube.
Presently, the air electrode material is synthesized
using high purity component oxides such as La 2 O 3
and MnO 2 . Significant reduction in the cost of air
electrode material is possible if less expensive, lower
purity raw materials are used instead of pure lan-
thanum compounds to synthesize the air electrode
powder. Air electrode material cost can also be
reduced by utilizing compositions that have lower
rare earth content. Use of such lower cost air
electrode materials in fabricating SOFC cathode
tubes appears promising.
2.2. Electrolyte
Solid oxide fuel cells are based on the concept of
an oxygen ion conducting electrolyte through which
the oxide ions (O 22) migrate from the air electrode
(cathode) side to the fuel electrode (anode) side
where they react with the fuel (H 2 , CO, etc.) to
generate an electrical voltage. Fluorite-structured
oxide materials such as yttria stabilized zirconia
(YSZ), rare earth doped ceria, and rare earth doped
bismuth oxide have been widely investigated as
electrolytes for a fuel cell [5,6]. Of these materials,
YSZ has been most successfully employed. The
yttrium oxide dopant serves dual roles: it stabilizes
the high temperature cubic phase in zirconia and also
generates oxygen vacancies through the following
defect reaction written in the Kroger–Vink notation:
ZrO 2
Y 2 O 3 → 2Y Zr
9 1 3O 3O 1 V ??O (2)
i.e. an oxygen vacancy is created for every mole of
307
the dopant Y 2 O 3 . The high oxide ion conductivity in
YSZ is attributed to these oxygen vacancies.
In tubular SOFCs, zirconia doped with about 10
mol.% yttria is used as the electrolyte. The con-
ductivity of YSZ at 10008C is maximum (about 0.1 S
cm 21 ) at about 10 mol.% yttria as shown by
Strickler and Carlson [7]; the activation energy is
also least near this composition. The thermal expan-
sion of 9–10 mol.% YSZ is about 10310 26 / 8C [8];
materials for all other cell components are chosen to
have thermal expansion near this value. For optimum
cell performance, the YSZ electrolyte must be free of
porosity so as not to allow gases to permeate from
one side of the electrolyte to the other, it should be
uniformly thin to minimize ohmic loss, and it should
have high oxygen ion conductivity with transport
number for oxygen ions close to unity and a trans-
port number for electrons as close to zero as
possible. Electrolytes with these desired properties
are deposited in the form of about a 40-mm-thick
layer by an electrochemical vapor deposition process
(EVD) [9,10]. Deposition of the YSZ electrolyte film
by a more cost-effective non-EVD technique, such as
plasma spraying or colloidal / electrophoretic deposi-
tion followed by sintering, is also being investigated
to reduce cell cost.
2.3. Anode ( fuel electrode)
The fuel electrode must be stable in the reducing
environment of the fuel, should be electronically
conducting, and must have sufficient porosity to
allow the transport of the fuel to and the transport of
the products of fuel oxidation away from the elec-
trolyte / fuel electrode interface where the fuel oxida-
tion reaction takes place, i.e.:
O 22 (s) 1 H 2 (g) 5 H 2 O(g) 1 2e 2 . (3)
The reducing conditions present on the fuel side of
an SOFC permit the use of a metal such as nickel
(alternately cobalt or ruthenium) as the fuel elec-
trode. However, the thermal expansion of nickel is
considerably larger than that of YSZ. Nickel can also
sinter at the cell operating temperature resulting in a
decrease in the fuel electrode porosity. These prob-
lems are circumvented by forming a skeleton of YSZ
around the nickel particles. The YSZ skeleton pre-
308 S.C. Singhal / Solid State Ionics 135 (2000) 305 – 313
vents sintering of the nickel particles, decreases the
fuel electrode thermal expansion coefficient bringing
it closer to that of the electrolyte, and provides better
adhesion of the fuel electrode with the electrolyte.
In tubular cells, a 100–150 mm thick layer of
nickel / YSZ is applied over the electrolyte by a
two-step process. In the first step, nickel powder
slurry is applied over the electrolyte. In the second
step, YSZ is grown around the nickel particles by the
same EVD process as used for depositing the
electrolyte. Deposition of a Ni–YSZ slurry over the
electrolyte followed by sintering has also yielded
anodes that are equivalent in performance to those
fabricated by the EVD process; use of this non-EVD
process will result in a substantial reduction in the
cost of manufacturing SOFCs.
Fig. 2 shows the microstructure of a cross section
of a Siemens Westinghouse SOFC consisting of the
air electrode, electrolyte and the fuel electrode.
2.4. Interconnection
Interconnection, in the form of a 9-mm-wide strip
along the cell length, serves as the electric contact to
Fig. 2. Microstructure of a cross-section of a Siemens Westinghouse solid oxide fuel cell.
the air electrode and also protects the air electrode
material from the reducing environment of the fuel
on the fuel electrode side. The requirements of the
interconnection are the most severe of all cell
components and include the following.
(a) Nearly 100% electronic conductivity.
(b) Stability in both oxidizing and reducing
atmospheres at the cell operating temperature
since it is exposed to air (or oxygen) on one side
and fuel on the other.
(c) Low permeability for oxygen and hydrogen to
minimize direct combination of oxidant and fuel
during cell operation.
(d) A thermal expansion close to that of the air
electrode and the electrolyte.
(e) Non-reactivity with the air electrode, elec-
trolyte and the electric contact material (e.g.
nickel).
To satisfy these requirements, doped lanthanum
chromite is used as the interconnection material.
Lanthanum chromite is a p-type conductor; its
conductivity is due to small polaron hopping from
 S.C. Singhal / Solid State Ionics 135 (2000) 305 – 313
room temperature to 14008C at oxygen pressures as
low as 10 218 atm. The conductivity is enhanced as
lower valence ions (e.g. Ca, Mg, Sr, etc.) are
substituted on either the La 31 or the Cr 31 sites. For
the Siemens Westinghouse tubular SOFC, the inter-
connection is deposited in the form of an |85-mm-
thick, 9-mm-wide strip along the air electrode tube
length by plasma spraying [11].
3. Cell operation and performance
The cell tube is closed at one end. For cell
operation, oxidant (air or oxygen) is introduced
through a ceramic injector tube positioned inside the
cell. The oxidant is discharged near the closed end of
the cell and flows through the annular space formed
by the cell and the coaxial injector tube. Fuel flows
on the outside of the cell from the closed end and is
electrochemically oxidized while flowing to the open
end of the cell generating electricity. At the open end
of the cell, the oxygen-depleted air exits the cell and
is combusted with the partially depleted fuel. Typi-
cally, 50 to 90% of the fuel is utilized in the
electrochemical cell reaction. Part of the depleted
fuel is recirculated in the fuel stream and the rest
combusted to preheat incoming air and / or fuel. The
exhaust gas from the fuel cell is at 600 to 9008C
depending on the operating conditions.
A large number of cells have been electrically
tested for up to about 25 000 h. These cells perform
satisfactorily for extended periods of time under a
variety of operating conditions with less than 0.1%
per 1000 h performance degradation. The voltage–
current characteristics of commercial prototypic 2.2-
cm diameter, 150-cm active length cells at 800, 900,
and 10008C with 89% H 2 111% H 2 O fuel (85% fuel
utilization) and air as oxidant (4 stoichs) are shown
in Fig. 3. These SOFCs have been found to tolerate
small levels of air- and fuel-side impurities without
any significant long-term performance problems. The
presence of moisture in air results in only a slight
decrease in voltage due to a small decrease in
oxygen partial pressure. With sulfur dioxide (SO 2 )
impurity in air, no voltage losses occur at con-
centrations up to 2 ppm, which is about 14 times the
US Environmental Protection Agency (EPA) air
quality limit. While operating with air containing
309
Fig. 3. Voltage–current density plots of a typical 2.2 cm diameter
cell.
seawater mist, some voltage losses occur but these
can be entirely attributed to water vapor; most of the
salt passes through the cell with only minimal
deposition on the inside of the air electrode tube.
On the fuel side, addition of up to 5000 ppm
ammonia (NH 3 ) had no adverse effect on SOFC
operation for up to 2500 h of testing; ammonia
actually acts as fuel increasing the cell voltage. The
addition of 1 ppm HCl also did not have any
detectable effect. However, the addition of 1 ppm
H 2 S to the fuel resulted in about a 10% drop in cell
voltage during the first 24 h and a declining slope in
voltage versus time curve thereafter. On removal of
H 2 S from the fuel, most of the lost voltage is
recovered indicating the deleterious effect of H 2 S in
the fuel to be reversible.
The tubular SOFCs have also shown the ability to
be thermally cycled to room temperature from
10008C over 100 times without any mechanical
damage or electrical performance loss. This ability to
sustain thermal cycles is essential for any SOFC
generator to be commercially viable.
The tubular SOFCs have also been tested at
pressures up to 15 atm on hydrogen and natural gas
fuels. Fig. 4 shows the effect of pressure on cell
power output for a 2.2-cm diameter, 150-cm active
length cell at 10008C. Operation at elevated
pressures yields a higher cell power at any current
density due to increased Nernst potential and reduced
cathode polarization, and thereby permits higher
310 S.C. Singhal / Solid State Ionics 135 (2000) 305 – 313

Fig. 4. Effect of pressure on cell power at 10008C.

stack efficiency and greater power output. With

pressurized operation, SOFCs can be successfully
used as replacements for combustors in gas turbines;
such hybrid SOFC–gas turbine power systems are
expected to reach efficiencies approaching 70%, and
thus result in reduced fuel consumption and reduced
capital cost per unit power output.
To reduce the physical size and cost of SOFC
generators, an alternate geometry cell has been
investigated. Such alternate geometry cells combine
all of the advantages of the tubular SOFCs, such as
not requiring high temperature seals, while providing
higher power per unit length and higher volumetric
power density. This new design, referred to as high
power density solid oxide fuel cell (HPD-SOFC),
has closed ends similar to the tubular design that
provide integral air return paths for air to flow the
entire length of the cell from the closed to the open
end. The HPD-SOFC departs from the tubular design
in that it is flattened and incorporates ribs in the air
electrode that act as bridges for current flow. Fig. 5
compares the current paths in tubular and HPD-
SOFCs. The ribs reduce the current path length,
which in turn reduces the internal resistance of the
Fig. 5. A comparison of the current path in a tubular SOFC and in
cell. The presence of the ribs, due to the decreased an HPD-SOFC.
internal resistance of the cell, also allows use of
thinner air electrodes which reduces the air electrode higher polarization). The ribs also form air channels
polarization (a thicker air electrode results in a that eliminate the need for full length air injector
higher diffusion path for oxygen from the gas phase tubes.
to the air electrode / electrolyte interface resulting in A comparison of the theoretically predicted and
 S.C. Singhal / Solid State Ionics 135 (2000) 305 – 313
Fig. 6. Comparison of theoretical and actual performance for the tubular SOFC and the HPD-SOFC on a stack volume basis.
actual performance of a tubular SOFC and an HPD-
SOFC on a stack volume basis is shown in Fig. 6.
The higher performance of the HPD-SOFC on a
stack volume basis results from the decreased resist-
ance and tighter packing of the cells compared to the
tubular SOFC. However, while the predicted peak
power density for an HPD-SOFC is 0.43 W/ cm 3 , the
actual peak power density obtained so far in pre-
liminary experiments has been 0.28 W/ cm 3 . The
difference between the predicted and the actual peak
power density is thought to be due to larger polariza-
tion losses at the air electrode / electrolyte interface.
Work on the optimization of the air electrode / elec-
trolyte interface in HPD-SOFCs to obtain decreased
polarization losses is underway.
4. SOFC power generation systems
Since 1984, successively larger size SOFC power
generation systems have been designed, built, and
tested. The design and operation of these systems
have been described previously [12]. Recently, two
25 kW systems, each consisting of 576 50-cm active
311
length cells (with EVD electrolyte, EVD fuel elec-
trode, and plasma sprayed interconnection), were
built and operated. One system was operated at the
Southern California Edison Company’s Highgrove
Generating Station in Grand Terrace (near San
Bernardino), California, under a program with the
US Department of Defense’s Advanced Research
Projects Agency (ARPA). In addition to the SOFC
generator, this system also consisted of a logistic fuel
processor, located external to the SOFC stack,
enabling the system to operate on either natural gas
or on reformate from a logistic fuel (DF-2 diesel or
JP-8 jet turbine fuel). This system was successfully
operated for 5582 h before the project completion in
early 1996; 766 h on jet turbine fuel, 1555 h on
diesel fuel, and 3261 h on natural gas. During this
time, the system endured five thermal cycles to room
temperature, produced up to 27 kW on each of the
three fuels, and showed no evidence of performance
degradation. In January 1998, without any modi-
fications to the SOFC generator, the system was
restarted on natural gas at the National Fuel Cell
Research Center at the University of California,
Irvine.
312 S.C. Singhal / Solid State Ionics 135 (2000) 305 – 313
The other system, built for a consortium of Osaka
Gas and Tokyo Gas, completed 13 194 h of success-
ful operation on desulfurized natural gas with |0.1%
per 1000 h of performance degradation. During this
period, the unit achieved 25 kW of power output and
endured 10 thermal cycles to ambient temperature.
A 100 kW SOFC power generation system began
operation in December 1997 in The Netherlands
under a program with a consortium of Dutch and
Danish utilities (EDB / ELSAM). This system is
installed and operated in Westervoort near Arnhem,
at a district heating system owned by NUON, one of
the group of five Dutch gas and electricity dis-
tribution utilities which belong to the EDB consor-
tium. The system employs 1152 state-of-the-art cells
(2.2 cm diameter, 150 cm active length); these cells
are prototypic of the cells that are planned to be used
in commercial SOFC generators. The system is
currently delivering over 100 kW AC to the grid at
an efficiency of 43% (AC / LHV). In addition, it is
producing |85 kW of hot water for the local district
heating system, yielding a total fuel effectiveness (at
100 kW AC) of 73%. The maximum power output of
the system is 160 kW net AC. Such atmospheric
SOFC systems with electrical generation efficiencies
(AC / LHV) in the 45–50% range are ideally suited
for distributed power generation and cogeneration.
The systems described above have been operated
at 1 atm pressure. Elevated pressure SOFCs in
conjunction with a gas turbine (GT) have the po-
tential to provide still higher power generation
efficiencies. Such hybrid systems can be configured
in a number of ways depending upon the turbine
selected and the capacity required. In the simplest
recuperated SOFC / GT configuration, efficiencies of
60–65% can be achieved. If a reheat cycle is used
with a split shaft turbine, efficiencies of greater than
70% are possible. Megawatt-class commercial
SOFC-GT power systems are expected to be price
competitive with other power generation systems of
comparable size because of their high efficiency,
high availability and low maintenance costs. A 250
kW hybrid pressurized SOFC-GT power generation
system is presently being fabricated in a program
with Edison Technology Solutions (ETS) for proof-
of-concept testing. The system will integrate a 200
kW SOFC stack (1152 cells of 2.2 cm diameter and
150 cm active length) operating at about 3.5 atm
pressure with a 50 kW microturbine generator. It is
expected to achieve an electrical efficiency of 57%
(net AC / LHV).
5. Summary
High temperature solid oxide fuel cells (SOFCs)
provide a highly efficient, pollution-free power gene-
ration technology. Their performance has been con-
firmed by successful operation in several atmos-
pheric pressure power generation systems of up to
100 kW size. Electrical generation efficiencies of
over 70% are possible in pressurized SOFC–gas
turbine combined cycle power systems. Atmospheric
and pressurized solid oxide fuel cell based power
systems are ideal distributed power generation sys-
tems – reliable, clean, quiet, environmentally friend-
ly, and fuel conserving.
Acknowledgements
The development of the SOFC technology is
supported by the US Department of Energy (DOE),
the Gas Research Institute (GRI), and various utility
and commercial sources. The pressurized SOFC
testing effort is supported by Ontario Hydro and its
Canadian funding partners, and New Energy De-
velopment Organization (NEDO) of Japan and its
participating electric power companies.
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