Journal of The Electrochemical Society, 149 共7兲 S59-S67 共2002兲
0013-4651/2002/149共7兲/S59/9/$7.00 © The Electrochemical Society, Inc.
An ECS Centennial Series Article
A Historical Perspective of Fuel Cell Technology
in the 20th Century
M. L. Perry and T. F. Fuller*,z
UTC Fuel Cells, LLC,1 South Windsor, Connecticut 06074, USA
© 2002 The Electrochemical Society. 关DOI: 10.1149/1.1488651兴
Available electronically June 10, 2002.
In honor of the 100th anniversary of The Electrochemical Soci-
ety, a retrospective look at the development of fuel cell technology
over the past 100 years is presented. The development of fuel cells
can be traced back over 160 years to Sir William Grove’s invention
in 1839. The history of these very early years have been described
elsewhere.1-3 Additionally, comprehensive technical reviews of fuel
cell technology are also available 共see, for example, Ref. 4 and 5兲, as
well as recent review articles on the latest developments.6,7 There-
fore, this paper will emphasize the progress on fuel cells that has
been presented in the Journal of The Electrochemical Society 共JES兲
and other ECS publications throughout the Society’s first 100 years.
This historical review includes all the major types of fuel cells,
which are named according to the electrolyte employed in the cells:
the alkaline fuel cell 共AFC兲, the polymer-electrolyte fuel cell
共PEFC兲, the phosphoric-acid fuel cell 共PAFC兲, the molten-carbonate
fuel cell 共MCFC兲, and the solid-oxide fuel cell 共SOFC兲. We will
review the significant advances that have occurred and how these
developments have been influenced by external factors. Research
groups that have made substantial contributions to these develop-
ments and the fuel cell literature in ECS publications will be given
special emphasis.
Fuel Cell Development in the Last 100 Years
The development of fuel cells over the last century has been
heavily influenced by external factors. Initially, fuel cells were seen
as an attractive means for the generation of power because the effi-
ciencies of other technologies were very poor. However, as the ef-
ficiency of these other technologies rapidly improved, the interest in
fuel cells waned. Then, when the ‘‘space race’’ began in the late
1950s fuel cells were rapidly developed for deployment in space.
More recently, significant technical progress in fuel cell technology
has made fuel cells appear more viable than ever for a variety of
applications. Additionally, concerns about energy resources and the
environment have elevated interests in generating power with even
higher efficiencies and lower emissions, and this has also raised the
interest level in fuel cells.
Although some interesting work was done on fuel cells during
the first half of the 20th century, it appears that almost nothing was
published on this subject in ECS publications during this period.
This is not surprising, given that most of the early work on fuel cells
was conducted in Europe and the Society was primarily an Ameri-
can institution in the early days.8 In fact, the initial publication of
the Society was known as the Transactions of The American Elec-
trochemical Society until 1930 when the word ‘‘American’’ was
dropped from the name of the organization to reflect the increasing
global composition of the membership and the title was changed to
Transactions of The Electrochemical Society.9
* Electrochemical Society Active Member.
z
E-mail: Tom.Fuller@UTCFuelCells.com
1
UTC Fuel Cells, formerly known as International Fuel Cells 共IFC兲, is a subsidiary
of United Technologies Corporation 共UTC兲.
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S59
Development of Large-Scale Electricity Generation and
Distribution
The large-scale distribution of electric power began at the end of
the nineteenth century. Although Michael Faraday had discovered
electromagnetic induction in 1831 共i.e., the basic principle of a gen-
erator兲, it took a number of other developments to establish large-
scale generation of electric power. But, by the mid-1870s electric
arcs were illuminating the streets of many major cities in Europe
and America. Initially, power transmission was limited to relatively
short distances and power-generation stations were relatively small.
However, with the development of an ac system, principally due to
the contributions of George Westinghouse and Nikola Tesla, the era
of large-scale power generation and transmission was born. And, in
1896, power generated by a pair of high-speed turbines at Niagra
Falls was transmitted 26 miles to the city of Buffalo, NY.
However, early electric power generators were very inefficient.
For example, the coal-burning generation station built by Thomas
Edison in 1882 in lower Manhattan converted only about 2.5% of
the available energy into electricity. Even in the 1920s the overall
thermodynamic efficiencies of reciprocating steam engines was ap-
proximately 13-14%, and steam turbines obtained just under 20%.
These poor thermal efficiencies provided one of the major motiva-
tions for the pioneers of fuel cell development. In fact, in 1894,
Ostwald10 pointed out the wastefulness of the steam engine and
expressed the hope that the 20th century would become the ‘‘Age of
Electrochemical Combustion.’’ This still visionary paper also em-
phasized the reduction of emissions with the elimination of the burn-
ing of fuels: ‘‘kein Rauch, kein Russ’’ 共no smoke, no soot兲.
Early Fuel Cell Development Efforts
Given that a major fuel at the turn of the century was coal, it is
not surprising that much of the work on fuel cells at this time was
focused on using this energy source. Both direct and indirect coal
fuel cells were investigated.
Ludwig Mond, who founded the International Nickel company
and other chemical industries in England, had developed a process
in which coal and coke were used to derive a gas containing a large
proportion of hydrogen. With the assistance of Dr. Charles Langer,11
they pursued the dream of scaling-up Grove’s gas battery into some-
thing that would deliver useful power from converted fuels, whereas
Grove had only considered ‘‘effecting the decomposition of water
by means of its composition.’’12 Unfortunately, impurities in Mond’s
industrial gas poisoned the fuel cell’s platinum-black catalyst and
the high cost of the required loadings of this catalyst made this
alternative power-generation technology cost prohibitive. 共Both of
these problems continue to challenge fuel cell developers to this
day.兲 Mond and Langer did make some interesting advances that
significantly increased the power density of the fuel cell by greatly
enhancing what Grove referred to as the ‘‘notable surface of action.’’
For example, they employed a porous matrix to contain their liquid
electrolytes and they introduced the use of powdered electrocatalysts
like platinum black.
Other researchers pursued the direct coal fuel cell. W. W. Jacques
built relatively large carbon/air batteries capable of delivering up to
1.5 kW in 1896. Unfortunately, the lifetime of these cells was lim-
ited because they employed molten alkali electrolytes that are not
 S60 Journal of The Electrochemical Society, 149 共7兲 S59-S67 共2002兲

invariant in the presence of carbon. Although Jacques was an Ameri-

can, he did not describe his work in any scientific journal. Professor
Baur, working at the Swiss Federal Institute of Technology in Zur-
ich, also attempted to develop direct-coal fuel cells. He investigated
a series of electrolytes capable of operating at increasing elevated
temperatures, including molten carbonates. Baur and his students
brought good scientific discipline to the development of fuel cells,
and they made some impressive advances in cell design and perfor-
mance. However, they were plagued by numerous practical prob-
lems 共e.g., ash formation, incomplete oxidation, and the continuous
feeding of a solid fuel兲 that reduced their interest in the direct use of
carbon. In a comprehensive review of the technology in 1933, Baur
and Tobler conclude that the fuel cell showing the earliest promise
of commercial success is one that operates at ordinary temperatures
with alkaline electrolyte and hydrogen as a fuel.13 An interesting
review of all of this early work, which includes the progress made
on electrode structures, can be found elsewhere.1

The Bacon Cell

Sir Francis Bacon began his historical work on fuel cells in 1933,
and he obviously agreed with the assessment by Baur and Tobler,
given that he set out to develop a hydrogen-oxygen cell that oper-
ated at moderate temperatures using alkaline electrolytes and im-
proved catalysts. Bacon’s own account of the development of a high
power density AFC 共e.g., 1.11 A/cm2 at 0.6 V at 240°C and very
high pressures兲 is both interesting and entertaining.14 These cells
employed nickel electrodes with a dual-porosity structure that along
with differential gas pressures across the cell provided a thin elec-
trolyte film in the larger pores. However, the performance of these
cells degraded rapidly due to corrosion of the porous-nickel cath-
odes. This issue was eventually overcome after extensive experi-
mentation led to the development of a nickel-oxide electrode 共doped
with lithium for improved electronic conductivity兲 that was more
corrosion resistant. In 1959, this technology was licensed by Pratt
and Whitney 共now a subsidiary of United Technologies Corpora-
tion兲, and was developed into the fuel cell system employed by the
U.S. Apollo space program.
Fuel Cells in Space
The Sputnik launches in 1957 and the ensuing ‘‘space race’’ that
followed was undoubtedly one of the most significant historical
events to influence the development of fuel cells. The requirements
for space applications, namely a lightweight and very high effi-
ciency power plant 共to reduce the amount of fuel and oxidant re-
quired兲, are uniquely met by fuel cells, especially given that cost is
not an overriding factor. This new application spurred the develop-
ment of both AFC and PEFC power plants.
It is interesting to note that the very first fuel cell used in a
practical application was a PEFC, which is the same fuel cell type
that is currently the focus of many of the major development pro-
grams attempting to develop fuel cells for terrestrial applications.
The PEFC was invented at General Electric 共GE兲 in 1955 by Will-
iam Grubb,15,16 who was looking for new applications for ion-
exchange membranes 共See Fig. 1兲.17 These early PEFCs utilized
hydrocarbon-based polymers that have limited lifetimes in a fuel
cell environment. The polymer-electrolyte membranes were com-
posed of polystyrene-divinylbenzene sulfonic acid cross-linked with
an inert fluorocarbon film. The life-limiting factor of these cells was
the oxidative degradation of the CuH bonds in the membrane, par-
ticularly the ␣-H sites where the functional groups are attached.
Despite this limitation, GE developed this technology into the power
plant that was successfully deployed in the U.S. Gemini program
beginning in 1962. Another drawback of these early PEFC cells
were the high loadings of platinum catalysts required. The AFC,
operating at elevated temperature and pressure, required less expen-
sive catalysts.
Three 28 V power plants provided all the onboard electrical
power to the Apollo Command and Service Modules, Fig. 2. The
AFC developed by Pratt and Whitney for the Apollo program oper-
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Figure 1. Diesel oil is combined with air in a new General Electric fuel cell,
generating electricity directly to power the fan motor at right. Pouring the
fuel 共commercial 18-cents-a gallon diesel oil, simply purified兲 is Dr. Thomas
Grubb, pioneer with Dr. Leonard Niedrach 共left兲 in the development of the
first fuel cell to operate successfully with a broad range of inexpensive hy-
drocarbon fuels at moderate temperatures. The new cell has been operated
with a variety of other common liquid fuels as well as such gaseous hydro-
crabon fuels as propane and natural gas. 共Photo courtesy of Science Service.兲
ated at a higher temperature 共260°C兲, higher KOH concentration
(⬃85%), and lower pressure 共near atmospheric兲 than the Bacon
cell. The anodes and cathodes were still porous Ni and lithiated NiO,
respectively, but improvements in their structure provided compa-
rable performance at lower operating pressures.1 On the other hand,
the electrodes used in the Orbiter AFC, which are still in use on the
Space Shuttle missions, contain noble metals 共Pt/Pd anodes and
Pt/Au cathodes兲 that are bonded with PTFE to Ag-plated Ni screens.
The PTFE 共which was not available when the Apollo electrodes
were developed兲 is used to form a more stable three-phase interface
共electrode/electrolyte/gas兲 than could be obtained in previous elec-
trodes.
Commercialization of Fuel Cells
Unlike some other so-called ‘‘spin-off’’ technologies 共i.e., tech-
nology developed for space applications that subsequently become
the basis of commercial products兲, fuel cells are not yet a major
commercial success. In fact, the only commercially available fuel
cell power plant, UTC Fuel Cells’ ‘‘PC-25,’’ is based on a different
technology 共PAFC兲 than the AFC-based power plants UTC makes
for NASA.
So, why are fuel cells still considered a relatively exotic technol-
ogy? Fundamentally, there are no insurmountable technical ob-
stacles that prevent fuel cells from enjoying commercial success.
And, the inherent advantages of fuel cells 共e.g., high efficiencies and
low emissions兲 relative to other electricity generation methods
makes them quite attractive. The main obstacle has undoubtedly
been the cost of this technology. Additionally, the requirement of
operating on readily available fuels and air 共vs. pure H2 and O2 兲
 Journal of The Electrochemical Society, 149 共7兲 S59-S67 共2002兲 S61

Figure 3. The number of papers appearing in the Journal which include the
phrase ‘‘fuel cell’’ in the title.

been active in this area, e.g., Energy Technology, Corrosion, High

Temperature Materials, and Physical Electrochemistry. Several of
the key fuel cell technologies 共e.g., SOFC, MCFC, and PEM兲 have
established recurring symposia and regularly published proceedings
volumes. In each case, these symposia bring together the leading
experts from the world and represent the cutting edge of fuel cell
technology.
According to Bacon, the expression ‘‘fuel cell’’ was not coined
until after 1937. The first paper with the specific phrase ‘‘fuel cell’’
appeared in the Journal in 1958 ‘‘The Fuel Cell Roundtable.’’19 This
was not a technical article; rather it was a report by R. Roberts of a
Figure 2. Apollo command and service modules.
discussion held on fuel cells at the 112th meeting in Buffalo, NY.
The battery division organized this roundtable, and about 150 people

makes terrestrial applications somewhat more challenging and com-

plex than the systems used in space. Fortunately, a lot of technical
progress has been made that help address these issues and should
enable fuel cells to enjoy widespread use in the near future.18 Addi-
tionally, market forces are making the attributes of fuel cells look
more attractive. For example, distributed power generation is ex-
pected to begin supplanting large centralized power stations due to a
variety of factors 共e.g., increased power demand, the need for high
quality power, deregulation of the power industry, less susceptibility
to terrorist attack, and environmental concerns兲. The automotive in-
dustry is also looking to obtain substantially higher efficiencies and
lower emissions than can be obtained by internal combustion en-
gines. Fuel cells have been identified as one of the most promising
technologies that can deliver these desirable attributes, and almost
all the major automakers have recently made substantial investments
into fuel cell development.

Fuel Cells and ECS

Much of the recent progress in fuel cell technology has been
documented in the Journal and other ECS publications. Therefore,
the remainder of this article will focus on some of the major ad-
vancements that have been presented in ECS publications, with an
emphasis on particular groups of researchers who have made sub-
stantial contributions to the fuel cell literature. 共For more exhaustive
reviews of fuel cell technology the reader is referred to the refer-
ences given in the introduction of this paper.兲
Figure 3 shows the number of paper published in the journal
which contain the phrase ‘‘fuel cell’’ in the title. There are undoubt-
edly many more papers of direct relevance to fuel cells, however, so
this data are not precise. They do, however, give us a qualitative
picture of the activity in fuel cells in the Society. There is a similar
increase in activity in the symposia and proceedings volumes with Figure 4. Ernest Yeager, President of the Society from 1965-1966 and Di-
‘‘fuel cells’’ in the title. The majority of these symposia have been rector of the Case Center for Electrochemical Sciences at case Western Re-
sponsored by the Battery Division, but many other divisions have serve University from 1976 to 1991.

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 S62 Journal of The Electrochemical Society, 149 共7兲 S59-S67 共2002兲
were in attendance. Roberts reports that the objective of the panel
was ‘‘to review the status of fuel cell development and potentialities
of fuel cells as power sources.’’ The Bacon cell was also reviewed in
some detail. One of the key speakers was Ernest Yeager 共Fig. 4,
President of the Society from 1965-1966兲 from Case Western Re-
serve University, where he also served as the director of the Case
Center for Electrochemical Sciences from 1976 to 1991. The num-
ber of ‘‘fuel cell’’ articles grew slowly with an increase in the late
1960s, presumably driven by the activity spurred by the aforemen-
tioned space race. It is interesting to note that few of these articles
dealt with the alkaline or PEM technologies that were vying for the
space program.
One of the more interesting early articles was an editorial from
1966 by V. Gardner entitled ‘‘Let’s Not Over-Sell the Fuel Cell.’’20
Even today similar questions are raised about the future of fuel cells.
Those of us who are trying to commercialize the fuel cell today were
heartened to see that the major concerns identified have been over-
come and it is likely that the obstacles facing fuel cells today will
not stand. Two issues of note were raised around developing a high
voltage output from the low voltage of a single cell, which is less
than 1 V. The first concern was the reliability of a large series con-
nected network of cells. To produce high voltage, hundreds of cells
must be placed in series, typically in a bipolar configuration. To
achieve a high reliability, a high mean time between failures for
individual cells or redundant cells are required. It was felt that the
only possible approach was the latter, but as we know today the
former can be achieved. For example the fleet of PAFC power plants
has about 5 million hours of operation in the field in over 200 units.
Each power plant has a single stack with over 200 cells in series.
The second concern was the conversion of the dc power to high
voltage ac. Whereas 40 years ago this was difficult to imagine in
anything other than small power applications, today hundreds of
kWs are routinely and reliably transformed with solid state inverters.
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Figure 5. LANL’s research team in
1986 共from left兲: W. K. Pai, E. A.
Ticianelli, C. R. Derovin, and S. Srini-
vasan.
At the height of the Energy Crisis in the early 1970s publications
with the word ‘‘fuel cells’’ almost disappeared. There were, how-
ever, frequent symposia focused on fuel cells during this period and
the Energy Technology Division was established. We know, for ex-
ample, that there was significant activity in phosphoric-acid fuel
cells, which will be discussed in some detail later. It wasn’t until the
1980s that we see a large and steady growth in ‘‘fuel cell’’ publica-
tions. Many of these papers were in molten-carbonate technology
with fewer in phosphoric-acid and solid-oxide technologies. 1988
brought the renaissance of PEM technology with a paper from S.
Srinivasan 共2001 Fellow of the Society and 1996 winner of the
Energy Technology Research Award兲 et al. entitled ‘‘Methods to
Advance Technology of Proton Exchange Membrane Fuel Cells.’’21
Figure 5 shows a few of the early members of Srinivasan’s team.
This was followed by a large body of work from the Los Alamos
group on PEM fuel cells. At roughly the same time the Ballard
company, which was formed in 1979, initiated their work on PEM
fuel cells.
Throughout the 1990s we have seen continued growth in the fuel
cell publications, to the point where one can find two or three ar-
ticles on fuel cells in every issue of the Journal. Part of the increase
can be attributed to the general increase in the number of articles
published in the Journal and larger international participation in the
Society, but it is unmistakable that research activity has increased
substantially.
Many of the papers that have been published on fuel cells deal
specifically with a particular type of fuel cell 共e.g., AFC, PEFC,
PAFC, MCFC, or SOFC兲. Before covering each of these fuel cell
types separately, it is worth reviewing some of the more general fuel
cell topics that have been widely covered by members of ECS over
the past 40 years.
 Journal of The Electrochemical Society, 149 共7兲 S59-S67 共2002兲
Figure 6. E. J. Cairns 共Society president 1989-1990 and ECS Fellow 1991兲
was one of the first to publish in the journal on fuel cells and has been active
since then. E. J. Cairns worked on the first PEM fuel cells at GE.
General Fuel Cell Topics
In addition to developing the first fuel cell system to be used in a
real application, the fuel cell research group at General Electric was
also the first to publish a series of technical articles on fuel cells in
the Journal. In addition to inventing and developing the PEFC, this
group of researchers examined the thermodynamics of fuel cells22,23
and did a considerable amount of work on direct-hydrocarbon fuel
cells,24-29 as well as direct-ammonia fuel cells.30,31 They also devel-
oped new electrode structures32,33 and examined new electrocata-
lysts for use with reformate fuels.34,35 This group worked with an
impressive array of low-temperature electrolytes; in addition to the
ion-exchange membrane cells they used a variety of liquid acid elec-
trolytes. An excellent review of this work, as well as a summary of
the state of fuel cell technology at the time, is presented by two of
the former GE workers, Liebhafsky and Cairns.1 It should be noted
that after leaving GE, Elton Cairns 共Fig. 6兲, has continued working
on fuel cells at Argonne National Laboratory, Lawrence Berkeley
National Laboratory, and at U.C. Berkeley. Elton Cairns is also an
ECS Fellow and a past President of the Society.
The renewed interest in fuel cells inspired a substantial amount
of research on the kinetics and mechanisms of the cathodic reduc-
tion of oxygen during the 1960s and 1970s. Because most of the
performance losses in a H2 /air fuel cell are due to the polarization
on the cathode it is not surprising that the kinetics of the oxygen-
reduction reaction 共ORR兲 received a lot of interest. In fact, the ORR
is quite complex and, even after all this work, the detailed reaction
mechanisms are still the subject of some controversy. Kinoshita has
provided an exhaustive review of this subject in Chapter 2 of his
ECS sponsored text on oxygen electrochemistry.4 Although the lit-
erature in this area is distributed among a variety of journals on
electrochemistry and catalysis, the Journal and Society meetings
have certainly been a key forum for discussion on this topic. Some
examples of this include: reviews by Yeager and Scherson at Case
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S63
Western Reserve University 共CWRU兲 on oxygen electrocatalysis in
aqueous electrolytes;36,37 ORR kinetic studies in H3 PO4 and other
acids by Appleby at Texas A&M,38,39 Volgol and other researchers at
UTC,40,41 and McBreen and O’Grady the Naval Research
Laboratory;42 as well the influence of particle-size effects43 and
physicochemical properties44 on the kinetics of the ORR.
Another topic of fundamental interest to all fuel cell researchers
is the preparation and properties of gas-diffusion electrodes 共GDEs兲.
In most fuel cells both of the electrodes are GDEs because both of
the reactants are typically gases. And, in order to achieve good per-
formance, especially with the slow ORR, a GDE with a very high
interfacial contact area is required. Thus, the key to good fuel cell
performance is constructing a stable and extensive interface between
the required three phases: solid 共electrode兲, liquid 共electrolyte兲, and
gas 共reactant兲. 共In the case of a true solid electrolyte, such as SOFC,
only two phases are required.兲 This is further complicated by the
continuous formation of the product water 共as liquid and/or vapor兲
that must be effectively removed to maintain stable performance. In
a GDE, three species must also be transported to or from the elec-
trocatalyst sites in order for the heterogeneous electrochemical reac-
tions to occur on a continuous basis. These species are (i) the elec-
trons in the solid matrix, (ii) the ions in the electrolyte, and (iii) the
gases dissolved in the electrolyte, as well as in the gas phase. Given
that each of these species must be transported either to or from the
catalyst sites, mass transport may control the rate of the reaction, in
addition to reaction kinetics; and therefore reaction rates throughout
a GDE tend to be nonuniform, especially at high current densities.
The design, characterization, and analysis of these complex GDEs
have received considerable attention in the Journal. Although much
of this work is specific to a particular type of fuel cell, and will
therefore be covered in the subsequent section, some of the work
that is generally applicable to all fuel types will be reviewed here.
In low-temperature fuel cells, employing aqueous electrolytes,
the gas-transport phase is typically provided by using hydrophobic
PTFE, which prevents the electrolyte from completely flooding the
void spaces of the porous matrix. PTFE-based GDES were first
developed in the 1960s 共see, for example, Ref. 33, 45, and 46兲 and
were further characterized and optimized in the 1970s 共see, for ex-
ample, Ref. 47 and 48兲 In addition to providing hydrophobic gas
pore within the GDE, the PTFE also serves as the binder for the
small particles of supported electrocatalyst, or agglomerates, that
comprise the solid matrix of these GDEs. The electrocatalyst in
these cells is typically a noble metal 共such as Pt or a Pt alloy兲, and
the support 共if any兲 is typically a high-surface-area carbon. Carbon
supported catalysts have resulted in dramatic decreases in catalyst
loadings, however, because the carbon support will oxidize in a fuel
cell environment, special attention must be paid to the preparation of
these materials, as well as the operation of the fuel cell to mitigate
carbon corrosion. Kinoshita has provided an extensive overview of
carbonaceous support materials, their use in fuel cells, and treat-
ments used to improve their stability, as well as their application in
a variety of GDEs.49
Theoretical modeling of GDEs has provided considerable insight
into what limits the performance of fuel cells. A GDE is a very
complicated structure that is difficult to characterize, even on a mac-
roscopic level, and therefore a model of this structure can become
very complex. One way to simplify this problem is to specify the
size of the porous solid particles, and this is the basis of the
‘‘flooded-agglomerate model’’ first introduced by UTC researchers
in the late 1960s.50 They used this model of a modern PTFE-bonded
cathode to show that a Tafel slope twice the normal Tafel slope will
arise due to mass-transfer limitations of oxygen in the electrolyte at
high current densities. Other modelers have since employed the rela-
tively simple flooded-agglomerate model to treat various fuel cell
electrodes. For example, Iczkowski and Cutlip51 used this type of
model, which included the diffusion of oxygen in the hydrophobic
gas pores as well as in the electrolyte phase, to show that ohmic
losses in the electrolyte may be responsible for a major portion of
the potential losses at moderate current densities. However, these
 S64 Journal of The Electrochemical Society, 149 共7兲 S59-S67 共2002兲
Figure 7. Types of fuel cells and advantages and disadvantages of higher
temperatures.
early models employed Ohm’s law to treat ionic conduction in the
electrolyte, which is not applicable when concentration gradients
exist.52 More recent models have accounted for the effects of both
ionic migration and diffusion in the solution phase 共see, for ex-
ample, Ref. 53 and 54兲. These models predict that a double Tafel
slope may also arise when the current distribution is dominated by
ohmic losses in the GDE. In this case, the ORR exhibits half-order
dependence on the oxygen partial pressure, and this fact may be
used to differentiate between cathodes that are limited by gas trans-
port and those limited by ohmic losses.
Fuel Cell Development by Type
The temperature of operation and the type of electrolyte used
distinguishes the various types of fuel cells. As shown in Fig. 7, fuel
cells with a wide range of operating temperatures are being devel-
oped. The major advantages and disadvantages of each type are also
summarized in the figure.
Alkaline Fuel Cells „AFC…
Oxygen reduction kinetics is more facile in alkaline electrolytes
than in acid electrolytes, and therefore AFCs have been developed
that have impressive specific power and energy density even at low
operating temperatures. However, a critical disadvantage of alkaline
electrolytes 共e.g., KOH, NaOH兲 is that they do not reject CO2 ;
therefore applications are restricted to operation on fuel and oxi-
dants that do not contain CO2 共such as reformed fuels or air兲. For-
tunately, for very remote operations where pressurized hydrogen and
oxygen are considered viable reactants 共e.g., space, undersea, mili-
tary兲, cost is usually not a constraining factor and AFCs have there-
fore been competitive in these niche applications. However, unless
the carbonation issue in AFCs is somehow resolved, the recent de-
velopments in PEM fuel cells appear to make PEM the technology
of choice for a low-temperature cell that will operate on air and/or
reformed fuels.
Polymer Electrolyte Fuel Cells „PEFC…
Two major improvements have been made in PEFC technology
since the Gemini program. The first was the development of
perfluorosulfonic-acid membranes that are more stable than the
hydrocarbon-based membranes used in the early PEFCs. These
membranes, such as Nafion®, consist of a PTFE backbone with
perfluorinated-vinyl-polyether side chains terminated by a sulfonate
group. Nafion, and similar derivatives, are essentially fully fluori-
nated and therefore they do not suffer from rapid degradation in a
fuel cell since CuF bonds are more stable than CuH bonds.
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DuPont originally developed perfluorosulfonic-acid membranes
in the early 1960s for use in the chlor-alkali industry, although it was
readily recognized that they are well suited for PEFCs, and the first
Nafion-based PEFC was tested in 1966. Yeo55 and Eisman56 pro-
vided excellent reviews of the properties of these membranes at ECS
meetings in the mid-1980s. Thinner membranes 共e.g., N112 and
composite membranes from W. L. Gore兲 have also greatly enhanced
the performance of PEFCs.
The second major improvement was the dramatic reduction of
catalyst loadings in PEFCs first demonstrated by Ian Raistrick at Los
Alamos National Laboratory 共LANL兲.57 By impregnating the elec-
trodes with perfluorinated ionomers in liquid form 共polymer dis-
solved in alcohol兲, a thin coating of the polymer electrolyte can be
deposited on the electrocatalysts. The resulting GDE has much
greater interfacial area than the previous conventional method of
simply hot-pressing the electrocatalysts to the membrane. In fact,
Raistrick demonstrated improved performance with an order-of-
magnitude less catalyst loading than the conventional PEFC elec-
trodes. Researchers at LANL subsequently refined these electrode
preparation techniques and developed the modern membrane elec-
trode assembly 共MEA兲 that is the heart of today’s PEFCs 共see, for
example, Ref. 58兲.
The fuel cell research conducted at LANL during the mid-1980s
and early 1990s laid the groundwork for the renaissance in PEFCs
that is still ongoing today. In addition to developing the state-of-the-
art MEA, LANL researchers conducted some very useful fundamen-
tal research on the kinetics of PEFCs,59-61 longer-term testing,62 and
developed PEFC models 共see, for example, Ref. 63兲. Supramaniam
Srinivasan, one of the original members of the LANL group, con-
tinued his PEFC kinetic studies at Texas A&M 共see, for example,
Ref. 64 and 65兲. LANL was also the first to propose using an air
bleed on the anode to improve the relatively poor tolerance of PEFC
to carbon-monoxide poisoning.66 Shimshon Gottesfeld 共ECS Fellow,
1999兲 and Tom Zawodzinski have provided an excellent review of
PEFC technology.5
A biennial series of ECS symposia on Proton Conducting Mem-
brane Fuel Cells has been organized. This symposium is presently
organized by S. Gottesfeld, T. Fuller, and others. The third in the
series will take place in Salt Lake City at the Fall 2002 meeting of
the Society. The development of PEFCs is currently an active area
of research with numerous companies striving to develop commer-
cial products for use in stationary power generation, automotive/
transportation applications, and as an alternative for batteries in por-
table electronics.
Phosphoric Acid Fuel Cells „PAFC…
In spite of all the recent activity in fuel cells over the last decade,
the phosphoric acid technology is still the only one used in commer-
cial product. Kinoshita4 provides a good review of the phosphoric-
acid technology; we will take time to review only the significant
contributions made through the Society. The technical challenges
with this technology are well known. The higher operating tempera-
tures 共150-200°C兲 reduce the complexity of power plants and make
the waste heat more valuable, but they also introduce materials chal-
lenges that are not nearly so difficult to meet as in PEM technology,
for example. In addition, the solubility of oxygen in phosphoric acid
is low and there is anion adsorption on the cathode catalysts, which
reduces the activity of the electrodes. Two areas are briefly reviewed
here: (i) improved materials, particularly, carbon supports and im-
proved cathode catalysts, and (ii) postmortem analysis of cells. Fab-
rication of electrodes in phosphoric acid fuel cells borrowed heavily
from the alkaline technology, with the early electrodes using metal
blacks. Platinum supported on carbon was used to reduce the load-
ings of the electrodes by about an order of magnitude. 共It is inter-
esting that we saw a similar path taken with PEM.兲 Early on, the
technology focused on high loaded platinum blacks and then the
transition was quickly made to supported catalysts. Putting the cata-
lysts on carbon supports allowed for a large improvement in perfor-
mance and reduction in catalysts loading, but issues with the stabil-
 Journal of The Electrochemical Society, 149 共7兲 S59-S67 共2002兲
Figure 8. PAFC Power Plant—To the First National Bank of Omaha just a
few milliseconds without electricity can mean hours of headaches and mil-
lions of dollars of lost revenues. Four UTC Fuel Cells 200 kW power plants
now serve as the bank’s primary source of power. Heat from the fuel cell
installation also provides energy for space heating, increasing the overall
efficiency of the fuel cell system to more than 80 percent.
ity of the high surface area carbon arose. Much of the contributions
centered on understanding and development of new carbon supports.
There are too many significant contributions to go into detail, but a
few are worth mentioning here. Some of the key contributors were J.
Bett, K. Kinoshita, H. R. Kunz 共1998 winner of the research award
of the Energy Technology Division兲, and G. A. Gruver. A second
area that was reported on relative to phosphoric acid fuel cells was
post mortem analysis of cells. As these fuel cell power plants ap-
proach commercialization, we saw a number of articles related to
corrosion resistance67 and platinum dissolution and migration,68 post
mortem analysis,69 and effects of impurities.70,71
UTC began commercial production of 200 kW PAFC power
plants that operate on natural gas in 1991 共shown in Fig. 8兲. Over
200 units have been sold and installed in 15 countries around the
world. Individual units have achieved over 40,000 hours of continu-
ous operation without a major overhaul, meeting the stated lifetime
goal of these power plants. The total accumulated hours of UTC’s
PAFC fleet is now over 5 million hours, with a fleet availability of
over 95 percent.
Molten Carbonate Fuel Cells „MCFC…
As mentioned earlier, Baur and co-workers started using molten
carbonate electrolytes in their attempts to develop a direct coal fuel
cell at the beginning of the last century. However, after almost three
decades of work, Baur became disillusioned with molten salts and
took the position that solid electrolytes would be the best candidate
for high temperature fuel cells.72 However, the desire to develop a
fuel cell with a greater flexibility to use readily available hydrocar-
bon fuels continued to motivate others to pursue the development of
MCFCs to the present day. In fact, soon after Baur decided to aban-
don melts, H. Greger made a significant contribution to MCFC tech-
nology by showing that when carbon dioxide from the anode is
recycled to the cathode that the electrolyte could be kept invariant.73
Then, in the 1950s and 1960s, a lot of development work was done
on MCFCs that is well summarized in a 1965 book edited by B. S.
Baker;74 important contributors during this period included re-
searchers from Holland 共G. H. J. Broers兲, France 共A. Salvadori兲,
England 共H. H. Chambers and A. D. S. Tantram兲, and the United
States 共E. Gorin, H. Recht, D. L. Douglas, I. Trachtenberg, and B. S.
Baker兲.
The relatively high operating temperature (⬃650°C) of MCFCs
provides several key advantages: (i) the opportunity to achieve very
high efficiencies with co-generation cycles, (ii) noble metal cata-
lysts are not required, and (iii) better tolerance to different fuels.
However, the higher temperature also limits the materials that can be
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S65
used. For example, whereas PTFE is used in PEFCs and PAFCs to
help establish a stable gas/liquid interface, in MCFCs controlling the
pore size is the only method available to maintain this key interface
共akin to the Bacon AFC兲. Electrolyte management in MCFCs is
definitely key to long-term performance, and the various processes
that contribute to the redistribution of molten carbonate in MCFC
stacks has been discussed in the ECS publications by both H.
Maru75 and R. Kunz.76 Additional issues that are still being ad-
dressed in MCFCs are hardware corrosion, cathode dissolution, and
low power density. However, companies in Europe, Japan, and the
United States have programs dedicated to developing stationary
power plants 共typically 100-250 kW兲 using MCFCs with improved
performance and endurance.
J. R. Selman, I. Uchida, and others have organized a recurring
symposia on Molten Carbonate Technology. Selman and Uchida
were awarded the 2001 Research Award of the Energy Technology
Division. Five proceedings volume dedicated to this technology
have resulted.
Solid Oxide Fuel Cells „SOFC…
The ‘‘Nernst Glower’’ was the first use of a solid ionic conductor,
demonstrated in the end of the nineteenth century.77 In the 1940s
Carl Wagner 共winner of the Society’s Olin Palladium Medal, 1951兲
explained the conduction process, and the first article on a SOFC
appeared in the Journal in 1962.78 This early work by Weissbart and
Ruka was done at Westinghouse, which has continued to be a leader
in SOFC technology to the present day.
SOFCs are the only fuel cells that utilize a true solid electrolyte,
and therefore electrolyte-management problems that are common to
other fuel cell types are not a concern for SOFCs. 共Note that the
membranes used in PEFCs must be hydrated to function well and
therefore require careful management of the water within the cell.兲
Additionally, the high operating temperature, typically about
1000°C, makes the SOFC much more tolerant of reformed fuels and,
because water is generated on the anode, in-cell reformation of hy-
drocarbon fuels is feasible. SOFCs are also potentially capable of
very high electrical efficiencies in a co-generation system 共e.g., in-
tegrated with gas microturbines兲. However, much like the MCFC,
the high operating temperature also creates a host of durability is-
sues, such as very limited selection of robust sealant materials 共e.g.,
glasses兲. To address the negative effects of glass-based seals, a va-
riety of stack designs other than the traditional bipolar-plate stack
design 共e.g., tubular or monolithic兲 have been pursued. The most
severe challenge in planar SOFC stacks is the poor lifetime of co-
efficient of thermal expansion matching ferritic stainless steels that
are being used as interconnects and the requirement for sealants,
mostly based on glass ceramics, in cross-flow stack configuration.
The seal-less tubular design of Siemens-Westinghouse has been
demonstrated with 150 kW power plants for up to 16,000 h with
acceptably low degradation rates, which proves the robustness of the
set of SOFC materials in this tubular stack configuration. Although
significant demonstrations of solid oxide cells have been made,79
several challenges must be overcome for commercialization of pla-
nar configurations. N. Minh has provided an excellent technical re-
view of SOFC technology.80
Today, the SOFC is an area of active research in academia, in-
dustry, and governmental laboratories. Over the last decade, nearly
half of the papers published in the Journal with ‘‘fuel cell’’ in the
title were devoted to SOFC technology. Although the advantages of
lower operating temperatures were recognized very early on,81 re-
ducing the temperature from 1000° to 700°C, or even 500°C, is
presently one of the key areas of research. This reduction in tem-
perature is accomplished by using alternate ionic conductors to
yttria-stabilized zirconia 共YSZ兲, e.g., ceria and doped lanthanum
gallates. A lower temperature allows the use of stainless steel in cell
stack construction, which would greatly reduce the cost. At the same
time, these temperatures are not so low as to eliminate the advan-
tages of SOFC technology. The primary challenges with lowering
the temperature are reducing the ohmic losses, electrolyte stability,
 S66 Journal of The Electrochemical Society, 149 共7兲 S59-S67 共2002兲
Figure 9. Honda’s newest fuel cell powered vehicle, the FCX-V4.
and cathode polarization. The conductivity of the solid electrolyte is
strongly dependent on the temperature. Acceptable conductance of
the separator can be achieved by using thinner films or doping to
increase the conductivity.
The Society has been one of the primary forums for communi-
cating results in SOFC development. S. Singhal 共ECS Fellow, 1996兲
has co-organized a biennial series of symposia in conjunction with
the SOFC Society of Japan since 1989. These have been some of the
best attended international meetings and most successful proceed-
ings volumes on fuel cells. Seven proceedings volumes have been
published by the International Symposia on Solid Oxide Fuel Cells.
This volume contains papers dealing with the materials for cell com-
ponents, fabrication methods for components, and complete cells.
Also contained in this volume are cell electrochemical performance
and modeling, stacks and systems, and field testing of SOFC dem-
onstration units. Companies in Europe, Japan, and the U.S. are pres-
ently working on various SOFC systems in various stages of devel-
opment. For example, both Siemens-Westinghouse and Sulzer/Hexis
are presently developing prototypes of small (⭐5 kW) SOFC
power plants.
Future Directions
More work is being done on fuel cell development than ever
before. Multiple companies around the world are focused on the
commercialization of fuel cells for stationary power, and almost all
of the major automotive companies have either internal fuel cell
development programs and/or they are working closely with other
companies to develop power plants for transportation applications.
The widespread commercialization of stationary fuel cell power
plants appears inevitable, with the only major technological barriers
remaining being cost and proven lifetimes. However, because PAFC
power plants with suitable lifetimes (⬃40,000 h) for stationary ap-
plications have already been developed, it appears reasonable to
expect that the lifetime requirements will be met by fuel cells that
operate at even lower temperatures 共e.g., PEFC兲. In regard to cost, a
major advantage of PEFC is that all the repeat parts 共e.g., MEAs and
bipolar plates兲 can be manufactured by high-volume processes that
are already being demonstrated by multiple companies. Undoubt-
edly, improving the lifetime and cost of fuel cells will be a major
focus for many years to come given that continuous improvement in
these two critical areas will increase the number of applications
where fuel cells are competitive with other power-generation tech-
nologies.
The cost targets for automotive applications are roughly an
order-of-magnitude more demanding than those for stationary appli-
cations. This, and other technical challenges, will inevitably delay
the widespread introduction of fuel cell powered automobiles. How-
ever, demonstration vehicles have already been introduced and
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many more are in development 共Fig. 9兲. The resources being dedi-
cated to these efforts are impressive and will undoubtedly accelerate
the commercialization of fuel cells in both stationary and transpor-
tation sectors. Another issue that must be resolved before fuel cells
find widespread acceptance in transportation applications is the
availability of a suitable fuel infrastructure. Hydrogen would be the
fuel of choice, but the volume and weight of the various hydrogen-
storage technologies still do not compare favorably with liquid fuels.
Therefore, efforts to develop fuel cell vehicles that operate on gaso-
line, methanol, or other fuels are ongoing. Because of the fuel in-
frastructure issue, fleet vehicles that operate on hydrogen and refuel
at a central station will be introduced first. In particular, buses are an
attractive application for fuel cells because the cost, volume, and
range requirements are not typically as challenging as those for the
automotive targets.
The development of new materials will continue to have a major
influence on the development of fuel cells. Just as the introduction
of PTFE enabled new GDEs for aqueous-electrolyte fuel cells and
the availability of ion-exchange membranes resulted in the creation
of PEFCs, the introduction of new materials will enable both im-
proved designs and new types of fuel cells. Currently, an active area
of research is the search for new polymer-electrolyte membranes.
Ideally, these membranes will possess high ionic conductivity with-
out the presence of liquid water, which will enable them to operate
at higher temperatures, resulting in simpler PEFC systems due to
improved heat rejection and CO tolerance. At the other end of the
temperature spectrum, the development of solid oxide conductors
that have suitable conductivity at lower temperatures would be de-
sirable because this might allow alternative sealing materials to be
employed in SOFCs and should help mitigate material degradation
issues. Other examples of new materials that would aid in the com-
mercialization of fuel cells are advanced electrocatalysts 共e.g., with
higher activity, and/or lower cost, and/or improved stability兲, low-
cost composites with excellent stability and electrical conductivity
that could be used to construct bipolar plates, and robust sealing
materials 共especially for high-temperature fuel cells兲. Finally, the
development of advanced hydrogen-storage materials would greatly
aid in the introduction of hydrogen-powered vehicles.
Another need that is clearly evident to those of us who are work-
ing towards the commercialization of fuel cells is a workforce of
engineers that have a good understanding of electrochemistry and
the design of electrochemical systems. Currently, there are very few
engineering programs that offer courses in these subjects, especially
at an undergraduate level. However, the development, design, and
manufacture of a complete fuel cell power plant involves a lot of
engineering work that requires at least a working knowledge of elec-
trochemical principles. Universities that recognize this need and
provide quality programs in electrochemical engineering, at both the
undergraduate and graduate level, will produce graduates who are in
high demand as electrochemistry-based industries, including fuel
cells, continue to grow. For example, many chemical engineering
departments now offer the opportunity for undergraduates to empha-
size a particular area by taking several optional courses in that field
共e.g., biochemical engineering兲; a similar program in electrochemi-
cal engineering would also appear to be well justified and potentially
very beneficial for both industry and the new graduates.
Although one cannot project the future of fuel cells over the next
hundred years, it can be stated with some certainty that The Elec-
trochemical Society will continue to play a prominent role in the
development of fuel cells. Society members will undoubtedly con-
tinue to lead research in fuel cell technologies as well as train others
in the field. And the meetings and publications sponsored by the
Society will continue to be an important forum for the discussion of
these developments. Hopefully, when the 200th anniversary of the
Society arrives fuel cells will be as ubiquitous as the internal com-
bustion engine is today.
 Journal of The Electrochemical Society, 149 共7兲 S59-S67 共2002兲
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