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 3 8 ( 2 0 1 3 ) 2 0 e2 8

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Improved durability of SOEC stacks for high temperature

electrolysis

Xiaoyu Zhang a, James E. O’Brien a,*, Robert C. O’Brien b, Joseph J. Hartvigsen c,

Greg Tao d, Gregory K. Housley a
a
Idaho National Laboratory, 101 Technology Dr., Idaho Falls, ID 83401, United States
b
Center for Space Nuclear Research, Idaho Falls, ID, United States
c
Ceramatec, Inc., Salt Lake City, UT, United States
d
Materials and Systems Research, Inc., Salt Lake City, UT, United States

article info abstract

Article history: An experimental study has been conducted at Idaho National Laboratory to demonstrate
Received 22 August 2012 recent improvements in long-term durability of solid oxide electrolysis cells (SOEC) and
Received in revised form stacks. Results of five stack tests are presented. Electrolyte-supported SOEC stacks were
25 September 2012 provided by Ceramatec Inc. and electrode-supported SOEC stacks were provided by
Accepted 25 September 2012 Materials and Systems Research Inc. (MSRI), for these tests. Long-term durability tests were
Available online 16 November 2012 generally operated for durations of 1000 h or more. Stack tests based on technologies
developed at Ceramatec and MSRI have shown significant improvement in durability in the
Keywords: electrolysis mode. Long-term degradation rates of 3.2%/khr and 4.6%/khr were observed for
Solid oxide electrolysis stack MSRI and Ceramatec stacks, respectively. One recent Ceramatec stack even showed
Durability negative degradation (performance improvement) over 1900 h of operation. Optimization
High temperature electrolysis of electrode and electrolyte materials, interconnect coatings, and electrolyteeelectrode
Hydrogen generation interface microstructures contribute to improve the durability of SOEC stacks.
Copyright ª 2012, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights
reserved.

1. Introduction increase to 64 million metric tons [3], compared to 9 million

Large-scale carbon-free hydrogen production based on high-
temperature electrolysis is under investigation at Idaho
National Laboratory (INL) as an alternative to steam methane
reforming, which accounts for about 95% of current hydrogen
production in the United States [1]. Most hydrogen
consumption in North America is for petroleum refining,
ammonia-based fertilizer production, and chemical indus-
tries [2]. Demand for hydrogen is increasing rapidly, primarily
due to refining requirements for increasing low quality
petroleum resources such as oil sands and heavy crudes.
Hydrogen demand in the United States in 2040 is projected to
metric tons in 2003 [2]. As the demand for hydrogen continues
to increase hydrogen production cannot rely solely on natural
gas. Hydrogen production based on nuclear or renewable
energy allows these carbon-free energy resources to
contribute to the transportation sector through petroleum
refining, synthetic fuels production, or ultimately through the
use of hydrogen as a direct vehicle fuel.
From a long-term perspective, sustainable methods must
be developed for large-scale hydrogen production [4]. A broad
overview of hydrogen production technologies is presented in
[5]. Among all the sustainable hydrogen production methods,
three advanced nuclear hydrogen production technologies,

* Corresponding author. Tel.: þ1 208 525 5409; fax: þ1 208 525 5754.
E-mail address: James.Obrien@inl.gov (J.E. O’Brien).
0360-3199/$ e see front matter Copyright ª 2012, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.
http://dx.doi.org/10.1016/j.ijhydene.2012.09.176
 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 3 8 ( 2 0 1 3 ) 2 0 e2 8
Nomenclature
MSRI Materials and Systems Research Inc.
HTE High temperature electrolysis HTE
SOEC Solid oxide electrolysis cell
SOFC Solid oxide fuel cell
INL Idaho National Laboratory
including sulfur-iodine (SI), high temperature electrolysis
(HTE), and hybrid sulfur process (HyS), were initially selected
by US DOE for further investigation. The goal was to down
select the most suitable technology for integration with the
next generation nuclear plant (NGNP) for large-scale hydrogen
production [6]. Based on the recommendation of an indepen-
dent review team [6], HTE was selected by the US DOE as the
most appropriate advanced nuclear hydrogen production
technology to be supported for further development and early
deployment.
The US Department of Energy, Office of Nuclear Energy has
supported development of HTE at the Idaho National Labo-
ratory (INL) since 2003. INL has demonstrated HTE at the
15 kW scale with a hydrogen production rate in excess of
5000 NL/hr [7]. However, long-term performance degradation
is the biggest barrier to scale up of HTE technology. Contin-
uous improvements on materials, seals, and microstructures
have been done and various SOEC stacks have been tested to
investigate ways to mitigate degradation at INL [8e11].
The major problems found in the previous stack tests were
air electrode delamination, Cr vapor poisoning, microstruc-
ture degradation, and seal leakage. Air electrode delamination
is often observed during high temperature electrolysis.
Oxygen partial pressure build-up in the electrodeeelectrolyte
interface is a proposed mechanism leading to air electrode
delamination [12e15]. Cr vapor poisoning mainly comes from
the stack interconnects which are usually made of a chro-
mium-rich alloy, typically a ferritic stainless steel or
specialty alloy such as Crofer. Investigations of the interaction
between metal interconnects and cell components and
methods to mitigate poisoning are well documented [16e21].
Microstructure degradation caused by interactions among the
material constituents results in a decrease in conductivity and
electrochemical activity [22,23]. Seal leakage is another
important factor that can cause identical cells to behave
differently in a stack. Seal failure often happens after thermal
cycles during the tests. Mismatch of coefficient of thermal
expansion (CTE) between the seal and other components can
cause cracks of the seal [24,25].
Much of the research on SOECs studying performance and
durability stays at single cell level. Besides our efforts, only
limited investigation addressed the performance and dura-
bility issues of SOEC stacks. Ebbesen et al. recently reported
SOEC stack tests for steam electrolysis and CO2/steam co-
electrolysis [26]. The stack and glass seals used in their tests
were designed by Topsøe Fuel Cells. Trace amounts of impu-
rity in the inlet stream was claimed to have significant impact
on the performance and durability of the stacks.
This paper provides a summary of results for the improved
durability of SOEC stacks tested at INL. Stack tests included
21
CTE Coefficient of thermal expansion
P&ID Piping and instrument diagram
CEM Controlled evaporation and mixing
vi Virtual instrument
ASR Area specific resistance
OCV Open circuit voltage
evaluation of initial performances and long-term durability in
the electrolysis mode. The objective of the test program is to
identify degradation mechanisms and to find ways to improve
SOEC stack durability.
2. Materials, experimental apparatus and
methods
The SOEC stacks used in this study were provided by Ceram-
atec Inc. and Materials and Systems Research Inc. (MSRI).
Ceramatec used electrolyte-supported cells for the stacks,
while MSRI used electrode-supported cells. Three 10-cell
Ceramatec stacks and two 5-cell MSRI stacks were tested at
INL. The configurations of the stacks and testing fixtures are
described below in detail.
2.1. Configuration of stacks
The Ceramatec stack consists of 10 planar electrolyte-
supported SOECs, interconnects, flow channels, seal gaskets,
and end plates. An exploded view of the stack is shown in
Fig. 1. The stack is externally manifolded with a cross-flow
configuration. The air outlet face is open, allowing for the
placement of supplemental instrumentation such as inter-
mediate voltage taps and internal stack thermocouples, as
needed. The standard materials used in Ceramatec SOECs are
scandia-stabilized zirconia (ScSZ) electrolyte, Ni-Ceria
steam/hydrogen electrode, and LaeCoeFe oxide based
perovskite air electrode. Each SOEC has an active area of
45 cm2. Corrugated metallic flow fields fabricated from nickel
and ferritic stainless steel (alloy 441) were used for gas
distribution as well as current collection on the steam/
hydrogen side and air side, respectively. The separator plate is
also ferritic stainless steel. The ferritic stainless components
are treated with a rare-earth coating/firing to support devel-
opment of a stable electronically conducting protective oxide
layer. Several different gasket materials were tested to mini-
mize leakage issue.
An exploded view of a 5-cell MSRI stack is provided in Fig. 2.
The stack is internally manifolded with process gases entering
and exiting at the bottom of the stack, flowing in an inverted-
U pattern in cross-flow. The oval flow passages around the
periphery of the cells, interconnects and gaskets provide gas
distribution to the micro-channel flow patterns in the inter-
connects. The MSRI stack uses electrode-supported cells. Each
MSRI stack has five identical Ni/YSZ-supported SOECs
(Ni/YSZ-YSZ-LSCF) with an active area of 100 cm2. MSRI SOECs
were fabricated using their state-of-the-art fabrication
processes and the materials and the microstructure of the
22 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 3 8 ( 2 0 1 3 ) 2 0 e2 8
Fig. 1 e Exploded view of a Cermatec 10-cell stack.
cells was optimized specifically for operation in the electrol-
ysis mode. Micro-channel flow patterns (12 cm  12 cm) were
directly machined into both surfaces of each interconnect,
providing gas separation, current collection, and flow distri-
bution. A contact aid was used to enhance electric conduction.
Sealing was provided by a means of compliant seal developed
by MSRI.
2.2. Experimental apparatus and methods
A piping and instrument diagram (P&ID) for stack testing is
shown in Fig. 3. Steam is generated either by bubbling a carrier
gas through the humidifier, or by a controlled evaporation and
mixing (CEM) system (Bronkhorst USA Inc.). Bubbling gas
through the humidifier is simple, but it is limited to
Fig. 2 e Exploded view of an MSRI 5-cell stack.
a maximum steam content of about 55%. One advantage of
using the CEM system to deliver steam is that it can achieve
higher steam content, as high as 90%. The other advantage of
using the CEM system is that the steam content can be
adjusted promptly compared to the humidifier, which usually
takes more than 1 h before stabilizing at a specified bath
temperature. The carrier gases used in the CEM are either pure
hydrogen or a hydrogen-nitrogen mixture. Two CEM systems
with different flow ranges, 100 g/hr and 1000 g/hr, were used
in the tests to evaporate liquid demineralized/deionized (DI)
water. The carrier gas contains at least 10% hydrogen in order
to prevent oxidation of the steam/hydrogen electrode.
Humidity transducers are placed at the inlet and outlet of the
stack in the steam/hydrogen line to provide a direct
measurement of steam consumption rate, which is equal to
the hydrogen production rate on a molar basis. The humidity
measurements therefore provide an independent verification
of the hydrogen production rate for comparison to the rate
determined by application of Faraday’s law, based on electric
current.
The test fixture for Ceramatec stacks is shown in Fig. 4. It
shows a Ceramatec stack, mounted on its inconel test fixture,
which rests on the furnace base. The power leads are inconel
rods insulated with alumina tubing. The hydrogen/steam and
air inlet tubes are coiled to provide additional length for heat
transfer upstream of the stack. The cross bar on top of the
stack is used to apply a mechanical compression load. The
load can be adjusted by tightening the springs underneath the
test stand through the linkage rods. More detailed description
of this experimental set-up can be found in [9].
A totally different test fixture was developed for testing
MSRI stacks. Fig. 5 shows a 3D overview drawing of the test
fixture. Two inconel bars were pre-welded vertically onto two
inconel plates, working as the current collectors. The bottom
 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 3 8 ( 2 0 1 3 ) 2 0 e2 8
Fig. 3 e Piping and instrument diagram for the INL high temperature steam electrolysis.
alumina tube sitting on a stand (not shown) supports the
whole test fixture. The top alumina tube is used to transfer the
mechanical compression load from the springs and to insulate
the top inconel plate from the other parts. The spring loading
assembly stays outside the furnace, so that the compression
load can be adjusted during the curing process. The stack was
sandwiched between two inconel plates, serving as the
current collectors and the end plates for compression. Coiled
tubes were welded onto the bottom inconel plate for pre-
heating of the inlet gases. Internal gas flow channels were
also machined into the bottom inconel plate for flow
distribution.
Prior to each test, the furnace temperature was slowly ram-
ped up to 800  C or 850  C with dry gases flowing through the
stack. After reaching the operating temperature, each stack was
conditioned in a reducing atmosphere for curing of the seals and
reduction of the steam/hydrogen electrode. During the electrode
reduction process, the downstream humidity sensor indicates
an elevated dew point temperature associated with reduction of
nickel oxide to nickel metal in a hydrogen atmosphere, which
produces steam. By the end of the curing and reduction
processes, both the inlet and the outlet humidity sensors will
indicate 0  C dew point. After the conditioning procedure, the
furnace temperature was set at 800  C. Then the initial perfor-
mance of each stack was evaluated by DC polarization scans in
the electrolysis mode and the fuel cell mode. Both electrolysis
and fuel cell sweeps were conducted at ambient pressure with
different steam concentrations. The long-term durability test in
the electrolysis mode was performed immediately after the
initial performance characterization. The long-term operating
23
conditions for each stack test are listed in Table 1. In the
Ceramatec stack tests, steam was generated by bubbling gas
through a humidifier. Typically 56% inlet steam content was
obtained by setting the humidifier bath temperature to 80  C. In
the MSRI and St. Gobain stack tests, steam was produced by
a CEM system. 70% steam content was recommended for oper-
ating MSRI stacks as well as maintaining the reducing condition
at the electrode.
For all the tests, Agilent units (34972 A LXI data acquisi-
tion/data logger switch unit with two 34901 A 20 channel
multiplexer modules) were used for data acquisition. A DC
power supply (Lambda GEN20-38) was used to provide elec-
trical power to the stacks during electrolysis. An electronic
load (AMREL FCL400-20-100E) was used for operating the
stacks in the fuel cell mode. All the instruments were
remotely controlled by computer using a Labview based
virtual instrument (VI). All of the ultra high purity (UHP)
hydrogen cylinders, the liquid nitrogen dewars, and a pre-
mixed safety gas cylinder were purchased from Norco Inc.
Air was supplied by the air compressor in the building.
3. Results and discussion
3.1. Ceramatec stacks
A series of DC polarization sweeps were performed with
different steam contents before the long-term tests. The
initial VI sweeps were conducted in both the fuel cell and the
electrolysis modes, in order to evaluate the initial
24 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 3 8 ( 2 0 1 3 ) 2 0 e2 8
Fig. 4 e 3D view of the test fixture for Cermatec stack
testing.
performance of the stacks. The bubbler temperature was set
at 20  C, 50  C, 70  C, and 80  C to humidify the fuel side inlet
gas. The corresponding steam contents are 2.7%, 14.5%, 37%,
and 56%. Fig. 6 shows the results of the initial DC character-
ization of Ceramatec stack #2. The nonlinearity in the curves
at low steam content is associated with the high sensitivity of
the Nernst potential to small changes in the average steam
content. Also, in the electrolysis mode, higher current densi-
ties can lead to steam starvation if the average steam content
is low. A high inlet dew point temperature, typically 60  C or
higher is suggested for long-term operation in the electrolysis
mode [12]. Therefore, a voltage limit of the power supply was
set for long-term electrolysis operation, in order to prevent
high voltage shock on the stack in the incident that the steam
content becomes low.
Fig. 7 presents results of a 1000 h electrolysis long-term
durability test of Ceramatec stack #1. Constant current
Fig. 5 e 3D view of the test fixture for MSRI stack testing.
densities of 0.25 A/cm2 and 0.317 A/cm2, were applied
alternately during the long-term test to evaluate the effect of
current density on degradation. The average degradation rate
at the lower current density is 5.66%/khr, while at the higher
current density is 4.62%/khr. The degradation rate was
calculated based on linear curve fitting of the stack voltage
data. The average ASR is also lower at higher current density,
which is consistent with the results obtained during initial
polarization scans. The ASR increased from 1.25 U cm2 to
1.52 U cm2 when operating at 0.25 A/cm2. These average
results indicate a lower degradation rate at the higher current
density. However, if degradation rates are recalculated from
300 to 1000 h, the degradation rates at 0.25 A/cm2 and
0.317 A/cm2 are very close. In other words, increasing the
current density has no obvious impact on the degradation
rate, at least over this range of current densities. Fig. 7 also
shows the intermediate stack voltages, which represent the
voltages across two intermediate cells. It is seen that all the
two-cell units behaved similarly during the tests.
Compared to our previous stack tests [9,27], Ceramatec
stack #1 demonstrated significant improvement on the dura-
bility of the SOEC stack. Several changes and improvements
were included with this stack. First, the active area of each cell
in stack #1 was reduced from 61 cm2 to 45 cm2, which helps to
manage the thermal stress distribution and improve sealing
quality. Second, the material and microstructure on the air-
side electrode were modified to mitigate the electrode
delamination. Finally, the stainless steel based interconnects
were pre-treated with spinel coatings to prevent oxidation
and Cr vapor formation.
 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 3 8 ( 2 0 1 3 ) 2 0 e2 8
Table 1 e Operating conditions for long-term stack testing.
Stack Temperature  C Flow rate (slpm)
H2 N2
Ceramatec #1 800 1 1
#2 800 1 1
#3 800 1 1
MSRI #1 800 2.5 2.5
#2 800 0.75 0 4.1a
a N2 was used instead of air as the air-electrode sweep gas during MSRI stack tests.
Fig. 8 represents results of a 1000 h electrolysis test of
Ceramatec stack #2. The stack was operated galvanostatically
at 0.25 A/cm2 during the long-term test. The average per-cell
ASR increased from 1.69 U cm2 to 1.77 U cm2. Stack perfor-
mance increased during the first 70 h, which may be due to
initial conditioning of the stack. Thereafter the stack perfor-
mance started degrading. Based on the time period from 70 h
to the end of the test, the degradation rate is 6.87%/khr based
on voltage. The degradation rate is slightly higher than that of
the stack #1, mainly due to nonuniform behaviors of the cells
in the stack. The intermediate voltages shown in Fig. 8 indi-
cate that some cells degraded faster than others. As
a comparison, intermediate voltage #5 degraded 11.3% over
1000 h, while intermediate #1 voltage degraded only 1.5% over
1000 h. It is difficult to identify the exact reason why those
cells behaved differently. It might be attributed to the defect
formed during cell fabrication and stack assembling, the flow
distribution in the stack, the leakage, etc.
Compared to the stack #1, a modified composite functional
layer that incorporates YSZ was added in each cell of the stack
#2 to improve bonding between the electrolyte and the air
electrode. In addition, a novel coating was applied on each
interconnect to further mitigate oxidation and Cr vapor
formation. Either one of the improvement did not further
mitigate the degradation, at least for some cells.
Fig. 6 e Initial VI sweeps with different steam contents of
Ceramatec stack #2. The calculated ASR values are shown
as the straight lines. The stack is operated at 800  C at
ambient pressure.
25
Steam content Current density (A/cm2) Steam generation
Air
5 56% 0.25, 0.317 Humidifier
5 56% 0.25 Humidifier
5 56% 0.25 Humidifier
4.1a 70% 0.2 Large CEM
70% 0.2 Small CEM
Fig. 9 illustrates the performance of Ceramatec stack #3
during long-term electrolysis. This stack was operated galva-
nostatically at 0.25 A/cm2 for about 1900 h and it was by far the
best performing Ceramatec stack that has ever been tested at
INL. Unfortunately the stack test was shut down due to an off-
normal event that happened at 1900 h and the performance
did not recover after that. The stack degraded over the first
200 h, but thereafter the performance started increasing. After
1600 h of operation, the stack voltage became stabilized. Based
on the time period from 200 h to the end of the test, the
performance increased 7.4% over 1700 h. Inlet and outlet dew
point temperatures were constant over the period, indicating
a constant hydrogen production rate consistent with the
constant current conditions of the test. The overall area
specific resistance (ASR) was used to quantify cell perfor-
mance. ASR is calculated based on the following equation:
ASR ¼ ðV  Vo Þ=J (1)
where J is the current density; V and Vo are the operating
voltage and the open circuit voltage, respectively. This defi-
nition of ASR is actually an apparent ASR since it is based on
the observed open-cell voltage at zero current density. The
initial and final average ASR values for this test were
1.59 U cm2 and 1.76 U cm2, respectively. The ASR reached
a peak of 1.92 U cm2 after a brief power outrage that occurred
around 500 h. Intermediate voltages in stack #3 behaved
differently over the first 500 h. After that time, the
Fig. 7 e Ceramatec stack #1 1000 h test with different
current density applied alternately in electrolysis mode.
26 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 3 8 ( 2 0 1 3 ) 2 0 e2 8

Fig. 10 e Initial VI sweeps with different steam contents of

Fig. 8 e Ceramatec stack #2 1000 h test at 0.25 A/cm2 in MSRI stack #2. The calculated ASR values are shown as the
electrolysis mode. straight lines. The stack is operated at 800  C at ambient
pressure.

intermediate voltages followed similar trends except for the

top one, which seemed to be affected significantly by the a Ceramatec button cell recently tested at INL also showed
power outage. similar behavior [28]. Its performance also increased contin-
To our knowledge, this is the first time that a SOEC stack uously over a 4000 h operation in the electrolysis mode.
exhibited significant negative degradation (i.e. performance Additional research is needed to fully understand this
improvement) in a long-term durability test. However, the exceptional behavior.
reason that caused this exceptional, yet promising, behavior
remains unclear and needs further investigation. A few
3.2. MSRI stacks
factors different from the previous tests were found. In the
preparation, the only difference between the stack #3 and the
Initial characterization was also conducted with the MSRI
previous one was the composition of the ceria-based func-
stacks. DC potential sweeps were performed over a range of
tional layer used in each cell. During initial characterization in
inlet steam content prior to the long-term tests. During the
the fuel cell mode, this stack indicated oxygen starvation,
initial performance evaluation, the lower steam content
despite adequate air flow. A problem with the sealing of the air
values were obtained by bubbling gas through the humidifier,
inlet manifold was later discovered post-test. This problem
while 70% steam content was achieved using the CEM system.
did not impact operation in the electrolysis mode. However,
Fig. 10 shows the results of the initial DC characterization of
none of these factors can easily explain the observed perfor-
MSRI stack #2. Compared to Ceramatec electrolyte-supported
mance increase over the long time period. As a comparison,
SOECs, MSRI electrode-supported cells have much lower ASR

Fig. 9 e Ceramatec stack #3 1900 h test at 0.25 A/cm2 in Fig. 11 e MSRI stack #1 1000 h test at 0.2 A/cm2 in
electrolysis mode. electrolysis mode.
 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 3 8 ( 2 0 1 3 ) 2 0 e2 8
Fig. 12 e MSRI stack #1 1000 h test at 0.2 A/cm2 in electrolysis mode.
values, corresponding to higher energy efficient during
electrolysis.
Fig. 11 represents the results of a long-term electrolysis test
on MSRI stack #1. The stack was operated galvanostatically at
0.2 A/cm2 for 1000 h. The overall degradation rate was 8.9%/khr
based on voltage, which is calculated based on linear curve
fitting. The average ASR increased from 0.41 U cm2 to 0.90 U cm2.
This degradation rate was higher than expected, mainly due to
the rapid degradation of the top cell, as shown in Fig. 11. The
degradation rate of the top cell was 26.8%/khr, while other cells
were close to 3.7%/khr. The rapid degradation on the top tell
might be caused by Cr poisoning since it has direct contact with
inconel current collector on the air side. A special surface
treatment was suggested to mitigate the top cell degradation.
Compared to the test of MSRI stack #1, the operating
conditions were adjusted in the test of the stack #2. The fuel-
side carrier gas flow rate was decreased from 5 slpm to
0.7 slpm by switching from the large CEM system to the small
CEM system. Also, pure hydrogen was used instead of
hydrogen/nitrogen mixture. The adjustment resulted in
a higher steam utilization value of 40%. Fig. 12 shows the
results of a long-term electrolysis test on MSRI stack #2. The
stack was operated galvanostatically at 0.2 A/cm2 for 1100 h
with an overall degradation rate 3.2%/khr. The improvement
of the overall stack durability was mainly attributed to the
modification of the top cell. Examination of Fig. 12 reveals that
all the cells behaved similarly during the long-term test,
which indicates that the treatment on the top cell significantly
mitigated its degradation. An alternative way to mitigate the
top cell degradation is by adding a dummy cell to separate the
top cell and the inconel plate. The dummy cell works as
a barrier as well as a current collector.
Generally, both the electrode-supported and the electrolyte-
supported SOEC stacks tested showed improved durability in
the long-term HTE operations. No general conclusion can be
made on which cell configuration is better than the other, since
each configuration has its own advantages. The electrode-
supported SOEC stacks have much lower ASR values due to
the thin electrolyte layers, which results in a lower power input
requirement for a specified current density or hydrogen
production rate. However, the electrolyte-supported SOEC
27
stacks may be more robust during long-term operations. Our
experience shows that the electrolyte-supported stacks have
better chance to survive through thermal cycles due to power
outages. The electrode-supported stacks may also be more
sensitive to unintentional redox events which can cause irre-
versible damage to the thick steam-hydrogen electrodes.
4. Conclusion
Significant improvements on the durability of the SOEC stacks
have been achieved. The state-of-art stack design, using
advanced materials, and the novel treatment of interconnects
all help to mitigate the degradation of the SOEC stacks in elec-
trolysis operations. Three electrolyte-supported SOEC stacks
provided by Ceramatec were tested. The degradation rates of
the first two stacks were between 4.62%/khr and 6.87%/khr. The
third stack demonstrated exceptional performance, which
showed negative degradation over 1900 h test. To the best of the
authors’ knowledge, this is the first SOEC stack ever docu-
mented in the literature for which the performance increased
steadily during a long-term electrolysis tests. However, the
factors that caused this exceptional result remain for further
investigations. Two electrode-supported SOEC stacks provided
by MSRI showed promising long-term durability. The most
recent stack demonstrated an overall degradation rate of only
3.2%/khr, which was the best result obtained to date at INL. A
degradation rate of w1%/khr or lower is needed for commer-
cialization of SOEC stacks for high temperature electrolysis.
More stacks are under testing at INL to verify various strategies
for further mitigating the degradation.
Acknowledgments
This work was supported by the U.S. Department of Energy,
Office of Nuclear Energy, Next Generation Nuclear Plant
Program under DOE Operations Office Contract DE-AC07-
05ID14517.
28 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 3 8 ( 2 0 1 3 ) 2 0 e2 8

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