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CHAPTER 1
1. Introduction
1.1. What Is a Fuel Cell?
A fuel cell is an electrochemical energy converter that converts chemical
energy of fuel directly into DC electricity. Typically, a process of electricity generation from fuels involves several energy conversion steps, namely:
1. combustion of fuel converts chemical energy of fuel into heat,
2. this heat is then used to boil water and generate steam,
3. steam is used to run a turbine in a process that converts thermal
energy into mechanical energy, and finally
4. mechanical energy is used to run a generator that generates
electricity.
A fuel cell circumvents all these processes and generates electricity in a
single step without involving any moving parts (Figure 1-1). It is this
simplicity that attracts attention. Such a device must be simpler, thus less
expensive and far more efficient than the four-step process previously
depicted. Is it really? Today—not really! Or better, not yet. But fuel cells
are still being developed. This book intends to provide a basis for engineering of fuel cell devices. It includes state-of-the-art designs and materials (as they exist at the time of this writing), which are likely to change in
the future as this technology continues to develop (perhaps even sooner
than the students using this book as a textbook get jobs in the fuel cell
industry). However, the engineering basis will not change, at least not dramatically and not so quickly. The knowledge of engineering principles will
allow future fuel cell engineers to adopt these new designs and new materials and, we hope, come up with even newer designs and materials. This
is what the purpose of an engineering education should be. This book will
not teach the principles of thermodynamics, catalysis, electrochemistry,
heat transfer, fluid mechanics, or electricity conduction, but it will apply
those engineering disciplines in the engineering of a fuel cell as an energy
conversion device.
1
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2 PEM Fuel Cells: Theory and Practice
hydrogen
electrode
FUEL CELL
electrolyte
oxygen
electrode
waste heat
water
FIGURE 1-1. Fuel cell generates DC electricity from fuel in one step.
The efficiency of an energy conversion process is one of the most important aspects of that conversion. Some typical questions are usually tackled
by engineering textbooks: How much energy of one kind is required to
generate one unit of energy of another kind? What is the theoretical
limit? How close we can come to that limit in practical applications? This
last question is where most engineering textbooks fail—in providing practical results and real—not theoretical—efficiencies. As an example, let us
examine the Carnot process or the Carnot engine. Every engineering
student should know that the Carnot process is the most efficient process
to operate between given temperatures. The fact that such an engine cannot
be made, and even if it could be made it would have to operate infinitesimally slow to allow the heat transfer processes to happen with no losses,
is maybe mentioned in some textbooks. But the fact that such an engine
would be very efficient at generating no power is never emphasized enough.
Yes, the famous Carnot engine would have to operate at the efficiencies
lower than the famous Carnot efficiency in order to generate useful power.
This book emphasizes the efficiency. But not only the theoretical efficiency, but the efficiency of practical, power-generating devices. That is
why there is a subsection on efficiency in almost every chapter. The chapter
on Fuel Cell Thermodynamics deals with theoretical fuel cell efficiencies.
As important as it is to learn about the Carnot efficiency, it is equally
important to learn about theoretical limits in fuel cells. The chapter on
Fuel Cell Electrochemistry introduces various losses that are unavoidable
because of the physical properties of the materials involved. These losses
obviously have an effect on the efficiency of energy conversion. The chapter
on Fuel Cell Systems discusses various supporting devices that are needed
to get the fuel cell going. Most of those devices need power, which means
that some of the power produced by a fuel cell would be used to run those
supporting devices, and therefore less net power would actually be delivered by the fuel cell system. This means that the practical efficiency will
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Introduction 3
be somewhat lower than the theoretical one. How much lower? That would
depend on the system configuration, design, and selection of auxiliary components. And finally, the efficiency of an energy conversion device in a practical application will probably depend on how that device is being used.
Does it run all the time at constant power output or does the power output
vary? If it varies, how much and how often? These are the reasons why the
efficiency is discussed in almost every chapter of this book.
Another important aspect of an energy conversion process is the cost.
It is the cost of produced energy that matters in practical applications.
Obviously, this cost depends greatly on the efficiency of the energy conversion process and the cost of the consumed (or thermodynamically, the
more correct term would be “converted”) energy. The cost of the energy
conversion device itself must also be taken into account. The cost of any
device depends on the cost of the materials and the efforts (labor) involved
to process those materials and make the components, and finally to assemble those components into a working device. Unfortunately, there is not
enough information available on fuel cell costs, either materials or labor.
One of the reasons the fuel cells are expensive is that they are not being
mass produced. And one of the reasons they are not being mass produced
is that their markets are limited because they are expensive. This “chicken
and egg” problem is typical for any new technology.
This book will interweave the theory and practice of the fuel cell and
fuel cell system design, engineering, and applications. This book will not
provide a recipe on how to build the best possible fuel cell, but it will give
an engineering student an understanding of the basic processes and materials inside a fuel cell. It will also supply enough tools and instructions on
how to use them, to design a fuel cell or a fuel cell system, or how to select
a fuel cell for a particular application. This book does not provide a direct
answer to all fuel cell-related questions, but it provides the engineering
tools needed to find those answers.
A fuel cell is in some aspects similar to a battery. It has an electrolyte,
and negative and positive electrodes (Figure 1-2), and it generates DC electricity through electrochemical reactions. However, unlike a battery, a fuel
cell requires a constant supply of fuel and oxidant. Also, unlike in a battery,
the electrodes in a fuel cell do not undergo chemical changes. Batteries
generate electricity by the electrochemical reactions that involve the
materials that are already in batteries. Because of this, a battery may be
discharged, which happens when the materials that participate in the electrochemical reactions are depleted. Some batteries are rechargeable, which
means that the electrochemical reactions may proceed in reverse when
external electricity is applied—a process of recharging the battery. A fuel
cell cannot be discharged as long as the reactants—fuel and oxidant—are
supplied. Typical reactants for fuel cells are hydrogen and oxygen; however,
neither has to be in its pure form. Hydrogen may be present either in a
mixture with other gases (such as CO2, N2, CO), or in hydrocarbons such
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4 PEM Fuel Cells: Theory and Practice
hydrogen
electrode
electrolyte
oxygen
electrode
waste heat
water
FIGURE 1-2. A fuel cell is similar to a battery in that it has electrodes and an
electrolyte, but it needs a fuel and oxidant supply and it generates waste heat and
water.
as natural gas, CH4, or even in liquid hydrocarbons such as methanol,
CH3OH. Ambient air contains enough oxygen to be used in fuel cells. Yet
another difference between a fuel cell and a battery is that a fuel cell generates by-products: waste heat and water, and the system is required to
manage those (a battery also generates some heat but at a much lower rate
that usually does not require any special or additional equipment).
1.2. A Very Brief History of Fuel Cells
The timeline of fuel cell development history is shown in Figure 1-3. The
discovery of the fuel cell operating principle—the gaseous fuels that generate electricity, is attributed to Sir William Grove in 1839 [1], although it
appears that a Swiss scientist Christian F. Shoenbein independently discovered the very same effect at about the same time (or even a year before)
[2]. However, in spite of sporadic attempts to make a practical device,
the fuel cell, or the “gaseous voltaic battery” as it was called by Grove [3],
remained nothing more than a scientific curiosity for almost a century.
E. Chen, in Fuel Cells Technology Handbook [4], provides a very detailed
description of these early fuel cell developments. It was another Englishman, Francis T. Bacon, who started working on practical fuel cells in 1937,
and he developed a 6 kW fuel cell by the end of the 1950s. However, the
first practical fuel cell applications were in the U.S. Space Program. General
Electric developed the first polymer membrane fuel cells that were used in
the Gemini Program in the early 1960s. This was followed by the Apollo
Space Program, which used the fuel cells to generate electricity for life
support, guidance, and communications. These fuel cells were built by
Pratt and Whitney based on license taken on Bacon’s patents (Figure 1-4).
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Introduction 5
Invention of fuel cell
Scientific curiosity
Reinvention
Industrial curiosity
Space program
Entrepreneural phase
Birth of new industry
1839
1939
1960’s
1990’s
FIGURE 1-3. Fuel cell history timeline.
FIGURE 1-4. Apollo fuel cells. (Courtesy of UTC Fuel Cells.)
In the mid-1960s General Motors experimented with a fuel cell-powered
van (these fuel cells were developed by Union Carbide). Although fuel cells
have continued to be successfully used in the U.S. Space Program until
today, they were again “forgotten” for terrestrial applications until the early
1990s. In 1989, Perry Energy Systems, a division of Perry Technologies,
working with Ballard, a then emerging Canadian company, successfully
demonstrated a polymer electrolyte membrane (PEM) fuel cell-powered
submarine (Figure 1-5). In 1993, Ballard Power Systems demonstrated fuel
cell-powered buses. Energy Partners, a successor of Perry Energy Systems,
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6 PEM Fuel Cells: Theory and Practice
FIGURE 1-5. PC1401 by Perry Group powered by PEM fuel cells (1989). (Courtesy
of Teledyne Energy Systems.)
demonstrated the first passenger car running on PEM fuel cells in 1993
(Figure 1-6) [5]. The car companies, supported by the U.S. Department of
Energy, picked up on this activity and by the end of the century almost
every car manufacturer had built and demonstrated a fuel cell-powered
vehicle. A new industry was born. The stocks of fuel cell companies, such
as Ballard and PlugPower, soared in early 2000 (Figure 1-7), based on a
promise of a new energy revolution (eventually in 2001 they came down
with the rest of the market). The number of fuel cell-related patents worldwide, but primarily in the United States and Japan, is increasing dramatically (Figure 1-8) [6,7], showing continuous interest and involvement of the
scientific and engineering community.
1.3. Types of Fuel Cells
Fuel cells can be grouped by the type of electrolyte they use, namely:
• Alkaline fuel cells (AFC) use concentrated (85 wt%) KOH as the
electrolyte for high temperature operation (250°C) and less concentrated (35–50 wt%) for lower temperature operation (<120°C). The
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Introduction 7
FIGURE 1-6. Energy Partners’ GreenCar, the first PEM fuel cell-powered passenger
automobile, 1993. (Courtesy of Teledyne Energy Systems.)
120
100
80
60
40
20
Aug 1997
Jan 1999 Jan 2000 Jan 2001
Aug 2002
FIGURE 1-7. The stocks of fuel cell companies soared in early 2000 (example of
Ballard).
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8 PEM Fuel Cells: Theory and Practice
number of patent publications
3000
2500
2000
1500
1000
500
0
1990
1992
1994
1996
1998
2000
2002
FIGURE 1-8. Fuel cell patent publications per year worldwide. (Adapted from [6]
and [7].)
electrolyte is retained in a matrix (usually asbestos), and a wide
range of electrocatalysts can be used (such as Ni, Ag, metal oxides,
and noble metals). This fuel cell is intolerant to CO2 present in
either fuel or oxidant. Alkaline fuel cells have been used in the space
program (Apollo and Space Shuttle) since the 1960s.
• Polymer electrolyte membrane or proton exchange membrane fuel
cells (PEMFC) use a thin (50 mm) proton conductive polymer membrane (such as perfluorosulfonated acid polymer) as the electrolyte.
The catalyst is typically platinum supported on carbon with loadings of about 0.3 mg/cm2, or, if the hydrogen feed contains minute
amounts of CO, Pt-Ru alloys are used. Operating temperature is
typically between 60 and 80°C. PEM fuel cells are a serious
candidate for automotive applications, but also for small-scale
distributed stationary power generation, and for portable power
applications as well.
• Phosphoric acid fuel cells (PAFC) use concentrated phosphoric acid
(~100%) as the electrolyte. The matrix used to retain the acid is
usually SiC, and the electrocatalyst in both the anode and the
cathode is platinum. Operating temperature is typically between
150 and 220°C. Phosphoric acid fuel cells are already semicommercially available in container packages (200 kW) for stationary electricity generation (UTC Fuel Cells). Hundreds of units have been
installed all over the world.
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Introduction 9
• Molten carbonate fuel cells (MCFC) have the electrolyte composed
of a combination of alkali (Li, Na, K) carbonates, which is retained
in a ceramic matrix of LiAlO2. Operating temperatures are between
600 and 700°C where the carbonates form a highly conductive
molten salt, with carbonate ions providing ionic conduction.
At such high operating temperatures, noble metal catalysts are
typically not required. These fuel cells are in the precommercial/
demonstration stage for stationary power generation.
• Solid oxide fuel cells (SOFC) use a solid, nonporous metal oxide,
usually Y2O3-stabilized ZrO2 (YSZ) as the electrolyte. These cells
operate at 800 to 1000°C where ionic conduction by oxygen ions
takes place. Similar to MCFC, these fuel cells are in the precommercial/demonstration stage for stationary power generation,
although smaller units are being developed for portable power and
auxiliary power in automobiles.
Figure 1-9 summarizes the basic principles and electrochemical reactions
in various fuel cell types.
load
edepleted oxidant and
product gases out
depleted fuel and
product gases out
H2
H2O
OH-
O2
H2O
AFC
H2
H+
O2
H2O
PEMFC
PAFC
CO3=
O2
CO2
MCFC
650 ∞C
SOFC
600-1000 ∞C
H2
CO2
H2O
(CO) H2
(CH4) H O
2
(CO)
O=
fuel in
O2
65-220 ∞C
60-80 ∞C
205 ∞C
oxidant in
anode
electrolyte
cathode
FIGURE 1-9. Types of fuel cells, their reactions and operating temperatures.
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10 PEM Fuel Cells: Theory and Practice
Sometimes, a direct methanol fuel cell (DMFC) is categorized as yet
another type of fuel cell; however, according to the previous categorization
(based on electrolyte), it is essentially a polymer membrane fuel cell that
uses methanol instead of hydrogen as a fuel.
1.4. How Does a PEM Fuel Cell Work?
Although some general engineering principles may be applicable to all
fuel cell types, this book is about PEM fuel cells, their operation, design,
and applications. PEM stands for polymer electrolyte membrane or proton
exchange membrane. Sometimes, they are also called polymer membrane
fuel cells, or just membrane fuel cells. In the early days (1960s) they were
known as solid polymer electrolyte (SPE) fuel cells. This technology has
drawn the most attention because of its simplicity, viability, quick startup, and the fact that it has been demonstrated in almost any conceivable
application, as shown in the following sections.
At the heart of a PEM fuel cell is a polymer membrane that has some
unique capabilities. It is impermeable to gases but it conducts protons
(hence the name, proton exchange membrane). The membrane that acts as
the electrolyte is squeezed between the two porous, electrically conductive
electrodes. These electrodes are typically made out of carbon cloth or
carbon fiber paper. At the interface between the porous electrode and the
polymer membrane there is a layer with catalyst particles, typically platinum supported on carbon. A schematic diagram of cell configuration and
basic operating principles is shown in Figure 1-10. Chapter 4 deals in greater
detail with those major fuel cell components, their materials, and their
properties.
Electrochemical reactions happen at the surface of the catalyst at the
interface between the electrolyte and the membrane. Hydrogen, which is
fed on one side of the membrane, splits into its primary constituents—
protons and electrons. Each hydrogen atom consists of one electron and one
proton. Protons travel through the membrane, whereas the electrons travel
through electrically conductive electrodes, through current collectors, and
through the outside circuit where they perform useful work and come back
to the other side of the membrane. At the catalyst sites between the membrane and the other electrode they meet with the protons that went through
the membrane and oxygen that is fed on that side of the membrane. Water
is created in the electrochemical reaction, and then pushed out of the
cell with excess flow of oxygen. The net result of these simultaneous reactions is current of electrons through an external circuit—direct electrical
current.
The hydrogen side is negative and it is called the anode, whereas
the oxygen side of the fuel cell is positive and it is called the cathode.
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Introduction 11
external load
collector
plate
electrode membrane electrode
oxygen feed
collector
plate
O2
2e2H+
H2 Æ 2H+ + 2e-
1/2O2 + 2H+ + 2e- Æ H2O
Carbon
support
H2
H2O
Porous
electrode
structure
hydrogen feed
Membrane
Platinum
FIGURE 1-10. The basic principle of operation of a PEM fuel cell.
Chapters 4 and 5 explain in greater detail all the processes involved in
making the fuel cell work. Because each cell generates about 1 V, as will be
shown subsequently, more cells are needed in series to generate some practical voltages. Depending on application, the output voltage may be
between 6 V and 200 V or even more. How the cells are stacked up, and
what the issues are in stack design, is discussed in Chapter 6.
A fuel cell stack needs a supporting system (as explained in Chapter
9) to:
• Handle the supply of reactant gases and their exhaust, including the
products;
• Take care of waste heat and maintain the stack temperature;
• Regulate and condition power output;
• Monitor the stack vital parameters; and
• Control the start-up, operation, and shutdown of the stack and
system components.
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1.5. Why Do We Need Fuel Cells?
Fuel cells are a very promising energy technology with a myriad of possible applications as discussed next and in greater detail in Chapter 10. Fuel
cells have many properties that make them attractive when compared with
the existing, conventional energy conversion technologies, namely:
• Promise of high efficiency—Because the fuel cell efficiency is much
higher than the efficiency of internal combustion engines, fuel cells
are attractive for automobile applications. Also, fuel cell efficiency
is higher than the efficiency of conventional power plants, and
therefore the fuel cells may be used for decentralized power generation. However, new energy conversion technologies, such as
hybrid electric vehicles and combined cycle power plants, also have
high conversion efficiencies.
• Promise of low or zero emissions—Fuel cells operating on hydrogen
generate zero emissions—the only exhaust is unused air and water.
This may be attractive not only for transportation but also for many
indoor applications, as well as submarines. However, hydrogen is
not a readily available fuel, and if a fuel cell is equipped with a fuel
processor to generate hydrogen, or if methanol is used instead of
hydrogen, some emissions are generated, including carbon dioxide.
In general, these emissions are lower than those of comparable conventional energy conversion technologies.
• Issue of national security—Fuel cells use hydrogen as fuel. Although
hydrogen is not a readily available fuel it may be produced from
indigenous sources, either by electrolysis of water or by reforming
hydrocarbon fuels. Use of indigenous sources (renewable energy,
nuclear, biomass, coal or natural gas) to generate hydrogen may
significantly reduce dependence on foreign oil, which would
have an impact on national security. However, widespread use of
hydrogen would require establishing a hydrogen infrastructure
or the so-called hydrogen economy, which will be discussed in
Chapter 11.
• Simplicity and promise of low cost—Fuel cells are extremely
simple. They are made in layers of repetitive components, and they
have no moving parts. Because of this, they have the potential to be
mass produced at a cost comparable to that of existing energy conversion technologies or even lower. To date, the fuel cells are still
expensive for either automotive or stationary power generation,
primarily because of use of expensive materials, such as sulfonated
fluoropolymers used as proton exchanged membrane, and noble
metals, such as platinum or ruthenium, used as catalysts. Mass production techniques must still be developed for fabrication of fuel
cell components and for the stack and system assembly.
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Introduction 13
• No moving parts and promise of long life—Because a fuel cell does
not have any moving parts, it may be expected to exhibit a long life.
Current fuel cell technology may reach the lifetime acceptable for
automotive applications (3000–5000 hours), but their durability
must be improved by an order of magnitude for use in stationary
power generation (where the requirement is >40,000–80,000 hours).
• Modular—Fuel cells are by their nature modular—more power may
be generated simply by adding more cells. Mass produced fuel cells
may be significantly less expensive than traditional power plants.
Instead of building big power plants, which must be planned well
in advance, and whose permitting process may be extremely cumbersome, it may be cost-effective to gradually increase generation
capacity by adding smaller fuel cells to the grid. Such a concept of
distributed generation may not only be cost-effective but also may
significantly improve reliability of the power supply.
• Quiet—Fuel cells are inherently quiet, which may make them attractive for a variety of applications, such as portable power, backup
power, and military applications.
• Size and weight—Fuel cells may be made in a variety of sizes—from
microwatts to megawatts—which makes them useful in a variety
of applications, from powering electronic devices to powering entire
buildings. The size and weight of automotive fuel cells approaches
those of internal combustion engines, and the size and weight of
small fuel cells may offer advantage over the competing technologies, such as batteries for electronic devices.
1.6. Fuel Cell Applications
Because of their attractive properties, fuel cells have already been developed and demonstrated in the following applications (some of which are
shown in Figure 1-11):
• Automobiles—Almost every car manufacturer has already developed and demonstrated at least one prototype vehicle, and many
have already gone through several generations of fuel cell vehicles.
Some car manufacturers are working on their own fuel cell technology (General Motors, Toyota, Honda), and some buy fuel cell
stacks and systems from fuel cell developers such as Ballard, UTC
Fuel Cells, and DeNora (DaimlerChrysler, Ford, Nissan, Mazda,
Hyundai, Fiat, Volkswagen).
• Scooters and bicycles—Several companies (Palcan, Asian Pacific,
Manhattan Scientific) have demonstrated fuel cell-powered scooters and bicycles using either hydrogen stored in metal hydrides or
methanol in direct methanol fuel cells.
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14 PEM Fuel Cells: Theory and Practice
FIGURE 1-11. Collage of fuel cell applications and demonstrations to date
(mid-2004). (Courtesy of Toyota, Asian Pacific Fuel Cell Technologies, Schatz
Energy Center—Humboldt State University, Honda, Aprilia, Teledyne Energy
Systems, Daimler-Chrysler, Ballard Power Systems, Fuel Cell Propulsion Institute,
Plug Power, MTU, Teledyne Energy Systems, Proton Energy Systems, MTI Micro
Fuel Cells and Smart Fuel Cells.)
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Introduction 15
• Golf carts—Energy Partners demonstrated a fuel cell-powered
golf cart in 1994 (it was used in Olympic Village at the 1996
Olympic Games in Atlanta). Schatz Energy Center developed fuel
cell-powered golf carts to be used in the city of Palm Desert in
California.
• Utility vehicles—Energy Partners converted three John Deere Gator
utility vehicles to fuel cell power [8] and demonstrated them in
service at Palm Springs airport (1996). John Deere is working with
Hydrogenics, Canada, on development of fuel cell-powered electric
utility vehicles, including those for lawn maintenance.
• Distributed power generation—Several companies are working on
development of small (1–10 kW) fuel cell power systems intended
to be used in homes. Some of them are combined with boilers to
provide both electricity and heat (PlugPower with Vaillant, and
Ballard with Ebara).
• Backup power—Ballard announced plans to commercialize 1 kW
backup power generators in cooperation with Coleman (2000), but
then bought back the technology and continued to sell the units
(2002). Proton Energy Systems demonstrated regenerative fuel cells
combining its own PEM electrolyzer technology with Ballard’s Nexa
units [9]. A regenerative fuel cell generates its own hydrogen during
periods when electricity is available.
• Portable power—Many companies (MTI, Motorola, NEC, Fuji, Matsushita, Medis, Manhattan Scientific, Polyfuel) are developing
miniature fuel cells as battery replacements for various consumer
and military electronic devices. Because of fuel storage issues, most
of them use methanol in either direct methanol fuel cells or through
microreformer in regular PEM fuel cells.
• Space—Fuel cells continue to be used in the U.S. Space Program,
providing power on the space orbiters. Although this proven technology is of the alkaline type, NASA announced plans to use PEM
fuel cells in the future.
• Airplanes—In November 2001 Boeing announced that it was modifying a small single-engine airplane by replacing its engine with
fuel cells and an electric motor that would turn a conventional propeller. Test flights are scheduled to begin in early 2004, and are
being conducted with the intention of using fuel cells as auxiliary
power units on jet airliners in the future.
• Locomotives—Propulsion Research Institute started a consortium
that demonstrated a fuel cell-powered locomotive for mining operations (the fuel cell was built by DeNora).
• Boats—MTU Friedrichschaffen demonstrated a sailboat on lake
Constanze (2004) powered by a 20 kW fuel cell, developed jointly
with Ballard.
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• Underwater vehicles—In 1989 Perry Technologies successfully
tested the first commercial fuel cell-powered submarine, the twoperson observation submersible PC-1401, using Ballard’s fuel cell
[10]. Siemens has been successfully providing fuel cell engines for
large submarines used by the German, Canadian, Italian, and Greek
Navies.
References
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2.
3.
4.
5.
6.
7.
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Bossel, U., The Birth of the Fuel Cell 1835–1845 (European Fuel Cell Forum,
Oberrohrdorf, Switzerland, 2000).
Grove, W. R., On a Gaseous Voltaic Battery, London and Edinburgh Philosophical Magazine and Journal of Science, Series 3, 21, 417–420, 1842.
Chen, E., History, in G. Hoogers (editor), Fuel Cell Technology Handbook
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Switzerland, June 1999.
Barbir, F., S. Nomikos, and M. Lillis, Practical Experiences with Regenerative
Fuel Cell Systems, in Proc. 2003 Fuel Cell Seminar (Miami Beach, FL, 2003).
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