Professional Documents
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FUEL CELL
SOFCs target military markets
A faster take on fuel reforming
Stationary power ready to roll
REVIEW
Hydrogen codes and standards
Portable electronics:
fuel cells eye the prize
An IOP Emerging Technology Review
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EDITORIAL
Editor Joe McEntee
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joe.mcentee@iop.org Volume 1 Issue 2 Aug/Sept 2004
Contributing editors Susan Curtis,
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Johnston
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SUBSCRIPTION RATES 2004 The view from Lucerne Researchers redefine the DMFC roadmap
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15 Patents leading electronics companies are gearing up to take
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● Sustainable fuels for MCFCs ● Steam
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the views or policies of the Institute of Physics, its reforming just gets better ● Hydrogen
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38 Talking Point
Hans Maru, CTO of FuelCell Energy, is a
true believer when it comes to the role that
high-temperature fuel cells may one day
Cover: Micro fuel cells are set to revolutionize power delivery in
play in stationary-power markets. portable electronic devices pp17–29 (Victoria Le Billon)
The organizers of the Lucerne Fuel Cell application within the next five years, according to a presenta-
MTU
Forum know how to give their delegates tion from MTU CFC Solutions of Germany. MTU boasts an
what they want – and we’re not just talk- impressive pedigree in the development of integrated MCFC
ing about beer at lunchtime and scenic systems. Its so-called HotModules have been put through their
evening cruises on Lake Lucerne. If it’s paces in a field-trial programme that’s been running since 2001.
hard technical information you’re after There are currently eight HotModule test sites across Germany,
on fuel-cell R&D, innovation and emerg- including hospitals, industrial plants and telecommunications
ing applications, then the historic Swiss exchanges (see photo, left).
city has established itself as the place to Meanwhile, the US Army’s Construction Engineering
head for when the summer conference circuit kicks in. Like Research Laboratory (CERL) elaborated on a simple yet effec-
others before it, this year’s event provided plenty of scope for tive strategy for fuel-cell testing. Over the past decade, it has
attendees to get to grips with the fine detail of fuel-cell materi- implemented a “kick it, and kick it hard” approach to evaluat-
als, components and systems development (165 presentations, ing the performance of 30 200 kW phosphoric-acid fuel-cell
60 poster contributions and 34 exhibitors from industry and power plants and, more recently, 75 residential-scale polymer-
academia testify to that, as does a set of conference proceedings electrolyte-membrane fuel-cell systems – all of them deployed
running to 2200 pages). at military and related facilities. CERL’s objective is to get away
Trouble is, sorting and evaluating the headline developments from what it calls “the traditional approach of fuel-cell devel-
in a sprawling programme like this is no easy task. Of course, opers” who “conduct carefully designed, tightly controlled field
it helps to remember that there’s a bigger market picture in play demonstrations”. The true test comes, it says, when the fuel
here and that, ultimately, fuel cells are a family of technologies cells are put into normal everyday operation and expected to
that will be driven not by the prejudices of the scientists or engi- deliver. The name of the game: to identify, in as short a time-
neers involved, but by the end-user. In this context, one of the frame as possible, any shortcomings associated with the fuel
encouraging aspects of the 2004 conference was the emphasis cells when they are exposed to a range of demanding conditions
it placed on reporting field demonstrations and R&D projects (i.e. high altitude, ground-water contamination and extremes
that are focused squarely on getting fuel-cell technology out of of temperature/humidity).
the controlled confines of the laboratory. Going forward, it’s clear that robust, no-nonsense approaches,
Unsurprisingly, for an event with two parallel sessions on like that of CERL, are going to be mandatory, and will ultimately
solid-oxide fuel cells (SOFCs), close-to-market high-tempera- enhance the commercial prospects of low- and high-tempera-
ture systems were very much to the fore. Swiss company Sulzer ture systems operating at all power levels. It will be intriguing to
Hexis, for example, detailed an ambitious three-year pro- see how much progress is made on this score by the time the fuel-
gramme of field trials involving deployment of 110 of its cell community meets up again in Lucerne next summer.
HX1000 Premiere units (based on a 1 kW SOFC system).
Working in partnership with the energy utilities, Sulzer has Subscriptions
been evaluating these “precommercial” prototypes for com-
bined heat and power applications in single-family homes, as Essential reading
well as in public buildings, laboratories and multitenant apart- Sign up now to secure your copy.
ments. Now, with more than 500 000 h of accumulated operat-
ing experience, the technical performance has made impressive
strides. Since the beginning of testing, says Sulzer, malfunctions Wry soundbite of the summer award goes to Michael J Binder
have been reduced by more than 80%, while downtime is less of the US Army’s CERL. “There are a lot of people making small
than 10% for 90% of systems tested since October 2002. On the fortunes in fuel cells today,” he told delegates in Lucerne.
back of this, a next-generation SOFC heating unit is already in “Trouble is, they all started out with big fortunes.” If you don’t
the works and should be ready for delivery in 2005. want to be one of the unfortunates in question, better make
Moving up several notches to the 250 kW regime, it appears sure you’re reading The Fuel Cell Review. But remember, if you
that molten-carbonate fuel cells (MCFCs) are emerging as a want to carry on receiving the magazine you must become a
credible, high-efficiency platform for decentralized cogenera- subscriber. I urge you to subscribe today – using the card at the
tion of electricity and heat using biofuels like sewage gas and front of the magazine or via our website.
landfill gas (see p32). What’s more, this sustainable slant on
MCFC technology could be ready for widespread commercial Joe McEntee, Editor (joe.mcentee@iop.org)
Transportation
Hydrogen safety
One of the fundamental challenges holding are fewer roadblocks to commercial implemen-
back commercialization of hydrogen tech- tation in Japan. ISO standards for compressed-
nologies is “the lack of safety information on and liquid-hydrogen-powered vehicles are
hydrogen components and systems used in a being developed, although at about the same
hydrogen fuel infrastructure, and the limited pace as in North America.
availability of appropriate codes and standards
to ensure uniformity and facilitate deploy- What role are the car makers playing?
ment”. With no less an authority than the US DaimlerChrysler, Ford, GM, Peugeot, Hyundai
Department of Energy (DOE) pushing that and the Japanese OEMs are focusing on 35 and
rather downbeat view, it’s probably time to lis- 70 MPa on-board storage systems, leveraging
ten up, especially as closer scrutiny reveals that the composite storage-tank technology devel-
rising to the aforementioned challenge is likely oped for compressed NGVs. BMW and the
to be far from straightforward – and not just Opel division of GM have been the only OEMs
where the US is concerned. that have shown an interest in on-board storage
For the time being, hydrogen and fuel-cell of liquid hydrogen. Both of these companies
companies are caught between a rock and a “Any organization wishing to sell hydrogen- have done a lot of development work, but there
hard place, most obviously when it comes to fuelled products on a commercial basis must be has been little interest in on-board liquid hydro-
deployment of hydrogen systems in automo- able to demonstrate that the safety risk has gen outside Germany.
tive and stationary-power applications. For been managed properly,” says BOC’s Bob Boyd.
starters, emerging technologies not yet recog- How important is government influence
nized within all-encompassing codes and stan- contribute to establishing a harmonized frame- in the development of relevant hydrogen
dards are certain to experience difficulties with work supporting the whole supply chain – safety codes and standards?
insurance, and could well be vulnerable to hos- from production to application. The DOE and National Renewable Energy
tile lawsuits. A lack of understanding of hydro- Excluding the changes being proposed to Laboratory (NREL) are doing a great job, with
gen fuel and hydrogen systems among local existing codes, we currently have codes and fewer resources than we would wish, to coor-
government officials, fire officers and the gen- standards for industrial hydrogen systems, dinate codes and standards development over a
eral public hardly helps. And competition natural-gas-vehicle (NGV) fuelling applica- wide range of organizations. Non-govern-
between standards and code-development tions, and traditional small and standby power mental agencies and industry-sponsored
organizations complicates things yet further. systems. But it is a big headache having to use organizations, such as the National Hydrogen
It may look messy, but when The Fuel Cell the industrial-hydrogen standards and existing Association (NHA) and Compressed Gas
Review spoke to Bob Boyd, project develop- building codes and standards to secure per- Association (CGA), also play a vital role, work-
ment manager, hydrogen energy, at The BOC mitting for demonstration fuel-cell projects. ing with the DOE and NREL to bring the tech-
Group in the US, it found there are still reasons nical issues and main players to the table.
to be optimistic that the hydrogen and fuel-cell How much progress has been made, and At the same time, commercial companies –
industry will be able to unify its efforts on remains to be made, in this context? like BOC – are contributing the man-hours
safety, codes and standards – and perhaps In terms of vehicle and hydrogen-fuelling needed to support the code-development
sooner rather than later. infrastructure, North America appears to be efforts. Some of that effort, to be sure, is there
on track to have codes and standards in place because these companies see commercial
FCR: What is the commercial importance for a major nationwide roll-out of fuel-cell opportunities [that require new codes], but the
of a coherent industry-wide approach to vehicles by 2015. Here, much of the develop- hydrogen economy will not develop unless
legal codes and technical standards ment on codes and standards going on today there is hope of commercial viability.
relating to hydrogen safety – specifically has been an outgrowth of the work of the
in terms of vehicle applications? California Fuel Cell Partnership (CaFCP). Clearly, many interested parties are
BB: It’s vital. Failure to develop harmonized Through the CaFCP, almost all of the major involved in the development of hydrogen
codes, standards and legislation covering the OEMs have found a forum to learn and collab- safety codes and standards, with different
use of hydrogen in the public domain would orate on both vehicle-development issues and and sometimes competing agendas. Do
prevent widescale adoption of hydrogen as a hydrogen infrastructure standards. you think that’s a problem?
fuel. Any organization wishing to sell hydro- Elsewhere, Japanese OEMs seem to be further I think that the ad hoc approach is working
gen-fuelled products on a commercial basis along towards an earlier commercialization of about as well as we could hope. There is quite a
must be able to demonstrate that the safety risk hydrogen vehicles – certainly, they are ahead on diverse bunch of interested parties and the sup-
has been managed properly. At BOC, for exam- commercial hybrid-electric vehicles (see The Fuel port from DOE and NREL has been well
ple, we are participating in various working Cell Review June/July 2004 p7). In terms of codes focused on systems that support collaboration
▲
groups, committees and demonstrations that and standards, the general feeling is that there and harmonization.
titanium dopant acts like a molec- alanate as a titanium–aluminium role in the reaction. storage materials, see “Hydrogen
ular “key” to facilitate hydrogen compound called titanium alu- The group probed the samples storage: the grand challenge” in the
absorption. Until now, however, minide, rather than entering the with high-energy X-rays at the June/July issue (p17).
Nanofabrication
senses new goals
Plankton fuel cells take the plunge
Newport, Ore: Over the past two In three seafloor experiments to
Albany, NY: Albany NanoTech, years, scientists have successfully date, OSU researchers and col-
one of the world’s largest centres of tapped the chemical reactions from leagues at several US institutions
excellence in nanotechnology decomposing organic matter on have tested prototype fuel cells
research, is extending its hydrogen the ocean floor to create demon- consisting of graphite anodes shal-
and fuel-cell activities. With more stration fuel cells that provide low lowly embedded in marine sedi-
than $250000 of new funding in the levels of electrical power for many ments and connected to graphite
bank – around 80% of it from the months. Earlier this summer, cathodes in the overlying seawater.
US Department of Energy (DOE) – though, Oregon State University They found that power was gener-
the centre has initiated a pro- (OSU) researchers moved things ated both by the direct oxidation of
gramme to develop a range of opti- forward by harnessing the same Plankton power: OSU’s research dissolved sulphide – which is a
cal sensors for fuel-cell applications. power-producing decomposition on biological fuel cells is funded by-product of microbial decom-
The DOE cash will support the activity from plankton taken from by the US Department of Defense. position – and by the respiration
development of nanoscale chemi- the upper water column. processes of microorganisms that
cal sensors to monitor minute “We’ve only had the experiments like the hydrophones used by the attached themselves to the anode.
amounts of hydrogen and other running for about four weeks,” said US Navy or by OSU researchers for Over the past couple of months,
hazardous gases in solid-oxide Clare E Reimers, a professor in the listening for earthquakes. OSU has been testing the fuel
fuel-cell systems (operating at College of Oceanographic and “But by harnessing plankton capacity of plankton. Using the
500–1000 °C). The rest of the funds Atmospheric Sciences at OSU, “but power,” Reimers added, “we could same principle as the seafloor fuel
(just over $60 000 from the New it is clear that we can use plankton potentially fuel autonomous, cells, the researchers have so far
York State Energy Research and as a fuel source and that the water mobile instruments that would managed to direct about 10% of the
Development Authority, or column is rich in microorganisms glide through the water scooping energy associated with plankton
NYSERDA) will be channelled into adept at shuttling electrons to fuel- up plankton like a basking shark, decomposition into a usable
R&D on nanofabricated (20 nm cell electrodes.” and converting that to electricity. power source. Reimers added:
thick) palladium alloy films, the The seafloor fuel cells that OSU Such instruments carry sensors “Our focus is on developing power
optical properties of which will developed previously are station- and are used today to map the for oceanographic equipment.
form the basis of all-optical hydro- ary and designed to provide power changing chemical and physical Who knows what spin-offs will
gen-safety sensors. for equipment that doesn’t move – properties of the ocean.” develop beyond that?”
Superheating unit could well be hot stuff with a cathode enzyme. Redox polymers serve to “wire” the respective
FuelCell Energy, US, has developed a fuel-cell-stack end unit that enzymes to their electrode, while the cathode enzyme operates under
contains an integrated heat exchanger for superheating fuel gas before physiological conditions. The inventors say that their fuel cell does not
delivery into the stack (WO 2004/061998). It’s a set-up in which heat is require a membrane seal or case.
transferred from the hot cathode outlet stream to the cool fuel inlet
stream in a space adjacent to the stack’s end plate. The end unit – There’s more than one right answer
designed as a hollow box to form a shell around the heat exchanger – Two US companies have come up with
has openings that allow fuel-cell process gas to be taken directly from different takes on the storage and delivery of
the stack without the need for piping or duct-work to be attached to liquid fuels for portable electronic devices
thin manifolds. According to the filing, “separate chambers are powered by polymer-electrolyte-membrane
provided for both the cathode-outlet and anode-outlet gas, thereby fuel fuel cells. Silicon Valley-based PolyFuel, for
allowing all process connections to be made at one end of the stack”. bladder example, detailed a removable fuel cartridge
The end unit also features a current-collection post that is separated (shown left) comprising a flexible bladder, an
from the end cell of the stack by a number of members. These members expandable pressure member (to maintain a
provide structural support for the end unit and more uniform pressure member positive pressure on the bladder) and a
collection of electrical current than a single, large current post. scalable exit port for the fuel
(WO 2004/051781). The delivery system channels fuel from the exit
Deionization helps to keep things cool port to the fuel side of the polymer membrane. Meanwhile, Foamex of
A device for deionizing the cooling medium that circulates through Pennsylvania revealed an orientation-independent fuel reservoir
a fuel-cell stack is detailed in international patent application comprising a fuel container; a wicking structure from which the fuel
WO 2003/061044 (revised 8 July 2004). Developed by BASF may be metered (such as by pumping); a retainer to hold the wicking
Aktiengesellschaft, Germany, the deionizing unit sits within the fuel structure in a desired orientation; and a fuel outlet that links to the
cell’s cooling circuit in such a way that a liquid deionizing agent can wicking element (WO 2004/027243).
act upon the cooling medium on an intermittent basis. The
deionization device can comprise static mixers, with membrane Cathode protection can combat corrosion
separators connected downstream. A fuel-cell design incorporating a corrosion-resistant and protected
cathode catalyst layer is described in international patent application
Material magic yields new-look membranes WO 2004/061999, filed by UTC Fuel Cells, US. The cathode catalyst
Researchers at Creavis Gesellschaft für Technologie und Innovation, layer includes a platinum oxygen-reduction catalyst and an oxygen-
Germany, have published details of a new class of proton-conducting evolution catalyst. The latter, selected from the group that is more
ceramic membrane based on zirconium phosphates active than platinum, can either be uniformly applied within the
(WO 2003/069712; revised 1 July 2004). Processing begins with the catalyst layer or non-uniformly applied to high-corrosion areas. UTC
production of nanoscale zirconium phosphate in a microjet reactor. says the cathode catalyst may include heat-treated carbon support
This material is then applied as a suspension onto a flexible carrier, material and/or a heat-treated carbon black.
after which it undergoes solidification. The result is a flexible
cation/proton-conducting membrane that is impermeable to other In fabrication, simplicity equals success
materials. Creavis claims that the new materials can form the basis of a A simplified method for bonding and edge-sealing a fuel-cell
membrane-electrode assembly “without any problem”. membrane-electrode assembly (MEA) has been revealed by 3M of
the US (WO 2004/062015). The key steps look like this: providing
Inner space: biological fuel cells power up a suitable MEA lay-up; positioning an annular layer of thermoplastic;
Therasense, US, has unveiled details of a miniature biological fuel cell and applying pressure and heat sufficient to impregnate the
that it claims could one day find applications as a power source thermoplastic into the fluid transport layer(s) of the MEA lay-up,
implanted inside the human body (WO 2003/106966; revised 1 July simultaneously bonding those layers to the MEA’s polymer membrane
2004). The invention comprises an anode in electrical communication (which may be perforated in its outer sealing area). 3M is also seeking
with an anode enzyme and a cathode in electrical communication patent protection for MEAs made using the new approach.
Researchers redefine
the DMFC roadmap
P IOTR P IELA AND P IOTR Z ELENAY
A two-part special report on direct-methanol fuel cells kicks off with a review of the R&D advances that
have pushed the technology into the first phase of commercialization for portable power sources.
Mobile markets: but further innovation will be needed if electronics manufacturers are to fast-track the uptake of DMFC technology.
IS FUEL CELL technology on the verge of going mainstream? of fuel) point of view, hydrogen is the most suitable fuel for fuel
Could be – at least if the world’s leading consumer electronics cells. The hydrogen oxidation reaction is a simple electro-
manufacturers get their way. Heavyweight players such as chemical process, in which a diatomic molecule (H2) is con-
Sony, Toshiba and Nokia are investing serious money in the verted to two hydrated protons (2H+aq). The process takes place
development and commercialization of the direct-methanol efficiently on different electrode materials, of which platinum
fuel cell (DMFC), a system in which methanol fuel is electro- (Pt), palladium (Pd) and nickel (Ni) are the best performers.
oxidized directly, without any preprocessing, to generate elec- Unfortunately, hydrogen turns out to be difficult to store, espe-
trical power. They’re betting that the payback will be a cially in portable applications.
next-generation power source that revolutionizes the per- No efficient, practical method of storing hydrogen for fuel-
formance and ease-of-use of all sorts of portable electronic cell applications currently exists.1 So while liquefaction leads
gadgets – including mobile phones, laptop computers, video to a form of hydrogen that’s potentially attractive for use in
cameras and plenty more besides. And what makes all this larger fuel-cell systems, the energy density is low
even more intriguing is the fact that some of these companies (2.70 Wh/cm3) because of the ultralow gravimetric density of
are talking in terms of months rather than years when it comes the fuel. Furthermore, once the energy expended during the
to DMFC-based new product launches (see p25). liquefaction process is taken into account, the energy density
To put the emergence of the DMFC into context, however, it’s is lowered still further, by as much as 40%. On the fringes of the
worth revisiting a few of the fundamentals of the fuel cell itself technology spectrum, reversible storage of hydrogen in metal
– in particular, the relative merits of different fuels. After all, hydrides has been limited to date in terms of the achievable
from the electrochemical and specific-energy (energy per gram specific energy (Wh/g hydride).
▲
Equation 1. DMFC anode reaction Fuels for direct-feed polymer-electrolyte fuel cells
Fuel Fuel-cell reaction Specific Energy
Low pH: CH3OH + H2O → CO2 + 6 H+ + 6 e energy density
(Wh/g) (Wh/cm3)
High pH: CH3OH + 6 OH– → CO2 + 5 H2O + 6 e
CO2 + OH– → HCO3– Hydrogen H2 + 0.5 O2 → H2O 33.0 2.7*
Carbon C + O2 → CO2 9.1 19.2
Methane CH4 + 2 O2 → CO2 + 2 H2O 14.2 6.0*
Equation 2. DMFC cathode reaction Propane C3H8 + 5 O2 → 3 CO2 + 4 H2O 13.3 6.6*
Decane C10H22 + 15.5 O2 → 10 CO2 + 11 H2O 12.9 9.4
Low pH: 1.5O2 + 6 H+ +6 e → 3H2O
Methanol CH3OH + 1.5 O2 → CO2 + 2 H2O 6.1 4.8
High pH: 1.5O2 + 3 H2O + 6 e → 6 OH–
Ethanol C2H5OH + 3 O2 → 2 CO2 + 3 H2O 8.0 6.3
Ethylene glycol C2O2H6 + 2.5 O2 → 2 CO2 + 3 H2O 5.3 5.9
It’s all about the fuel
The problems associated with hydrogen generation and stor- Formaldehyde CH2O + O2 → CO2 + 2 H2O 4.8 3.9*
age have led the R&D community to focus on developing alter- Formic acid HCOOH + 0.5 O2 → CO2 + H2O 1.7 2.1
native, mostly organic, fuels for use in polymer-electrolyte fuel Oxalic acid C2O4H2 + 0.5 O2 → 2 CO2 + H2O 1.0 2.0
cells (see table, “Fuels for direct-feed polymer-electrolyte fuel
cells”). There are two main ways to utilize such fuels in a low- Ammonia NH3 + 0.75 O2 → 0.5 N2 + 1.5 H2O 5.5 3.9*
temperature polymer-electrolyte fuel-cell system: Hydrazine N2H4 + O2 → N2 + 2 H2O 5.2 5.3
● On-board processing, which involves extensive, multistep * Based on the density of liquefied gas
purification of the fuel, after which the resulting
hydrogen-rich gas mixture is supplied as a feed stream to
the fuel cell. (though being highly oxygenated, they are less energy-dense).
● Direct electro-oxidation of the fuel at the fuel-cell anode.
Health and environmental issues are likely to exclude the final
two options, ammonia and hydrazine, from widespread use in
The former typically involves several catalytic reactors in series, fuel-cell systems. Of all the partly oxygenated fuel molecules
a system often seen as too complex for reliable power delivery that undergo complete electro-oxidation at low temperatures,
over long timeframes and reasonably broad conditions of oper- methanol is the one that exhibits the best combination of energy
ation. The latter approach is far simpler as it requires only one cat- density and rate of electro-oxidation.
alytic converter – the fuel cell itself. Nevertheless, there are major
challenges, as high-rate, direct electro-oxidation of a carbona- DMFC processes
ceous fuel molecule at the fuel-cell anode is far more demanding In a DMFC, methanol (typically together with water) is supplied
catalytically than the electro-oxidation of dihydrogen. to the anode, where it undergoes electro-oxidation to CO2 with
When it comes to the choice of fuel, the energy content per the release of six electrons to the load (figure 1). To date, most
unit weight or volume is one of the key figures of merit. Of the of the systems described in the open literature involve a liquid
first five options listed in the table above, the four carbonaceous methanol–water feed, although in some platforms the
fuels can be oxidized only at temperatures much higher than methanol fuel can be supplied to the DMFC anode as a vapour.
100 °C, and even then not without problems. Of the two alco- Electrons are subsequently transferred via the external circuit
hols next on the list, methanol can be electro-oxidized all the (which includes the load) to the cathode, where they are utilized
way to CO2 at temperatures well below 100 ºC, but ethanol can- in the reduction of oxygen supplied to the cathode from air.
not. This has been explained by the catalytically more demand- The reactants and mobile species in the electrolyte are inti-
ing C–C bond activation in the case of ethanol. mately tied to the pH of the fuel-cell electrolyte. At low pH lev-
Even so, other molecules with C–C bonds have been shown to els, water is consumed in the anode process together with
electro-oxidize completely to CO2 at temperatures well below methanol, while protons are transported from the anode side
100 ºC – one example being ethylene glycol.2 The big difference across the electrolyte and consumed in the cathode process to
seems to be the higher degree of “oxygenation” of the fuel mole- form water. This is the case for the polymer-electrolyte fuel cell,
cule, reflected by an atomic oxygen:carbon ratio of ≥1. This as it is based on a proton-conducting poly(perfluoro-sulphonic
apparent condition is fulfilled for methanol and ethylene glycol, acid), known as poly(PFSA), membrane.
but not for ethanol; and while the former two fully electro-oxi- In high-pH systems, on the other hand, the effect is reversed:
dize to CO2 at low temperatures, the ethanol does not. Further water is now consumed on the cathode side of the cell in the
down the list are two substances – formaldehyde and formic oxygen-reduction process, forming hydroxyl ions. These ions
acid – that are essentially partly oxygenated methanol. Both are are transported across the cell to the anode, where they are con-
easy to oxidize to CO2 at low temperatures, as is oxalic acid sumed together with methanol fuel to form CO2. Equations 1
HH2O
O
CH OH
CH3OH + H2O CH 3OH
3 6H+ + 1.5O2 + 6e–
+
H+
H
CO2 + 6H+ + 6e– 3H2O
Electroosmotic
electro-osmotic
drag
drag
anode cathode
Operational principle of the proton-conducting, polymer-electrolyte DMFC. Methanol is supplied to the anode, usually with water,
where it undergoes electro-oxidation to CO2. Electrons pass to the cathode, where they are used in the reduction of oxygen.
and 2 describe, correspondingly, the anode and cathode reac- potential. The adsorbed CO moiety, remaining on the Pt cata-
tions at both low and high pH levels. The overall methanol fuel- lyst surface following the initial dehydrogenation step(s), can
cell reaction, as shown in the table, is identical to that for be electro-oxidized at a Pt electrode only at a significantly
combustion of methanol by direct reaction with oxygen. higher electrode potential.
High-pH electrolytes can promote higher rates of methanol Consequently, continuous electro-oxidation of methanol to
oxidation at a given temperature, because an alkaline environ- CO2 can be sustained at a Pt electrode only above 0.6–0.7 V. At
ment facilitates the formation of the active surface-oxygen these higher potentials, surface oxide (or hydroxide) starts
species required for completion of the methanol electro-oxi- forming on the Pt surface from adsorbed water. This surface-
dation process. However, a serious obstacle associated with oxygen species is crucial for the completion of the methanol
high-pH fuel cells is the absence of a hydroxyl-ion-conducting oxidation process, as it converts the adsorbed CO intermediate
membrane offering conductivity and reliability as good as that remaining after methanol dehydrogenation to CO2. The widely
of the poly(PFSA) membranes. Furthermore, the introduction accepted mechanism of methanol oxidation on Pt reflects this
of the liquid-alkaline electrolyte brings its own challenges: sequence of methanol dehydrogenation followed by electro-
chiefly, the formation of bicarbonate ions (see equation 1). oxidation of adsorbed CO, as shown in equation 3 overleaf.
As a consequence, most recent DMFC development activity Meanwhile, the search for a methanol electro-oxidation cat-
has focused on the proton-conducting polymer-electrolyte alyst exhibiting higher activity than that of Pt has been directed
configuration shown in figure 1. The membranes in question at materials which, as well as maintaining high methanol dehy-
have been primarily of the poly(PFSA) type, such as Nafion, drogenation activity, facilitate the rate-determining step of the
although alternatives do exist at various stages of development reaction (i.e. CO electro-oxidation). Researchers have focused
and supply. One example of the latter is the Z1 membrane from primarily on alloys of Pt with metals possessing a higher affin-
PolyFuel, based in Mountain View, California, US. ity with oxygen, with the most successful composition discov-
ered to date being a binary alloy of Pt with ruthenium (Ru).
Methanol at the anode At 70 °C, for example, Pt–Ru alloys in which the atomic frac-
Electro-oxidation of methanol is a six-electron process (see equa- tion of Ru varies between 0.3 and 0.6 will support complete,
tion 1) that, like other complex electrochemical reactions involv- sustained methanol electro-oxidation at an anode potential of
ing multi-electron transfer, proceeds via a reactant adsorption 0.25–0.30 V. That’s well below the anode potential required for
step at the electrode surface, followed by a one-by-one transfer the same process at a pure platinum catalyst. This methanol
of electrons from the molecule to the electrode. While providing anode-potential range corresponds to an anode loss (DMFC
sufficient bonding of a methanol molecule, Pt allows fast cell voltage loss due to the anode) of 0.20–0.25 V. And consid-
removal of the four hydrogen atoms from the adsorbed molecule ering the “direct” nature of the fuel cell (no losses in fuel pro-
onto adjacent Pt metal sites (dehydrogenation step), a process cessing steps upstream of the fuel cell), such an efficiency loss
facilitated by the high affinity of Pt metal sites to hydrogen atoms. due to the anode (≤20% of total fuel energy content) is suffi-
Thanks to this high level of dehydrogenation activity, the ciently low to make DMFC technology commercially viable.
onset of electro-oxidation of methanol on pure Pt takes place So how does adding Ru to Pt lower the potential for complete
at a potential as low as 0.2 V on the hydrogen reference scale. six-electron methanol oxidation, compared with that found
However, this initial process is limited to dehydrogenation using Pt alone? One explanation that has been put forward is
alone and is therefore not sustainable at such a low anode the so-called bifunctional effect. This considers the significant
Dehydrogenation
Pt(electrode) + CH3OH → Pt(electrode)–COH + 3H+ + 3e
Pt(electrode) – COH → Pt(electrode)–CO + H+ + e
methanol and, particularly, hydrogen affinity of Pt electrocat- the active surface area of the anode catalyst needs to be fairly
alysts in aqueous environments and, on the other hand, the high, which in turn requires significant loading of Pt–Ru (typi-
facile oxidative water decomposition on Ru to form a surface cally used in the form of a “black” or unsupported catalyst).
oxygen species in aqueous electrolytes.3 Accordingly, the When aiming for maximum power, the Pt–Ru loading is of
bifunctional mechanism involves the initiation of the surface the order of several mg/cm2 of cross-sectional (geometric) area
process at a Pt–Ru catalyst with the dehydrogenation steps tak- of the electrode. Since similar precious-metal loading has been
ing place at Pt surface sites, whereas Ru sites assume the role of required to date for the cathode as well, the overall precious-
providing the oxide/hydroxide species required to complete the metal loading can be as high as 10 mg/cm2. However, the emer-
oxidation of surface CO. The overall anode process at Pt–Ru is gence of alternative DMFC membrane-electrode assemblies
the same as in equation 3 down to the final two steps, which in (MEAs) – such as those developed at Los Alamos National
the case of the Pt–Ru alloy are described by equation 4. Laboratory – could allow system designers to cut down the cat-
Electronic effects provide another possible interpretation of alyst loadings significantly, with relatively small losses in out-
the observed benefit of adding Ru to Pt.4 According to this the- put power. This is possible because the power-output
ory, added Ru lowers the electron density in the 5d band of Pt, dependence on catalyst loading in polymer-electrolyte DMFCs
resulting in a shift of electronic charge from adsorbed CO to the is highly nonlinear, with ever-decreasing incremental gains in
metal catalyst and thereby facilitating oxidation of the power for incremental increases in catalyst loading at a total cell
adsorbed CO. Of the two interpretations offered, the formation loading exceeding 1 mg/cm2.
of a bifunctional surface – with discrete sites of high dehydro-
genation activity and of high surface-oxygen formation activity The dynamics of the cathode
– is generally believed to be the more important. Just like in a hydrogen fuel cell, the cathode reaction in a DMFC
As equation 4 suggests, the electrocatalytic process of anodic (equation 2) requires platinum to act as the oxygen-reduction
oxidation of methanol takes place on metal sites. What’s more, electrocatalyst. But while the major rate-limiting factor in the
there’s compelling experimental evidence – collected on the cathode process of hydrogen fuel cells is the sluggish interfa-
highly dispersed, unsupported Pt–Ru catalysts employed in cial kinetics of oxygen reduction, the DMFC cathode is addi-
DMFC anodes – that the significant amounts of various Ru tionally challenged by penetration of methanol and water
oxide species present in such dispersed alloy samples have no through the membrane from the anode side of the cell. High
active role in the methanol electro-oxidation process. In fact, methanol permeability in proton-conducting membranes is
excess oxide coverage on the Pt–Ru metal alloy sites inhibits the the source of so-called “methanol crossover”. Once on the cath-
rate of methanol electro-oxidation – as evidenced, for example, ode side of the cell, methanol typically reacts with oxygen at the
by the benefits produced by prereduction treatments.5 cathode catalyst to form CO2 and water. This amounts to a
Finally, it’s worth noting that the rate of methanol oxidation “chemical short” across the fuel cell, with the methanol
on Pt–Ru is strongly dependent on temperature, with high per- crossover corresponding to lost fuel.
formance obtained near and above 100 ºC.6 Such a temperature In addition to the loss of fuel, the cell current at some given
regime, however, is not compatible with simple stack/system cathode potential (i.e. some given DMFC voltage) is lowered by
hardware and long-term performance stability – and is partic- a value corresponding to the current of methanol crossover at
ularly impractical for smaller, portable power sources. If suffi- that cell voltage. The result is a loss of output power. However,
cient methanol oxidation rates at 40–80 ºC are to be achieved, the flip side of the methanol crossover phenomenon is that it
Performance matters: fuel-cell test set-up at Los Alamos National Laboratory. Inside the chamber is a high-power-density 23-cell
DMFC stack, designed and built at Los Alamos. On the right is a close-up of the DMFC stack inside the test chamber.
can be used for two beneficial purposes: water generation better than 50%. Further work, however, has revealed that the
within the cell when operating with 100% methanol feed (see rate of methanol crossover can be cut significantly when the cell
“DMFCs power up for portable devices”, p25), and heat genera- is under current, provided that the cell anode is designed to adjust
tion to hike the temperature of the cell and bring it, at a higher the concentration of methanol between the flow field and the
rate, to some design temperature above ambient. membrane surface without, at the same time, generating a too-
The permeation of water through the membrane and into the severe limitation on mass transport.7
cathode is another cause for concern in DMFCs fed by By lowering the crossover in this way, it is now possible to
water/methanol liquid. Around 20 molecules of water appear in achieve fuel utilizations as high as 90% with commercial
the DMFC cathode per single methanol molecule oxidized at the poly(PFSA) membranes such as Nafion, provided that the feed
anode, mainly as a result of electro-osmotic drag of water across concentration is dropped to ≤1 M. On this basis, a number of
the membrane by protons. But a high water flux can easily companies have reported rapid and encouraging progress in
“flood” the cathode, leading to performance loss. Consequently, terms of the development and manufacture of viable DMFC
effective removal of cathode water requires significant air flow at sources. Still, it’s clear that further significant advantages will
non-zero pressure – such that the air pump (compressor) can be accrue if the R&D community can come up with membranes
the largest source of parasitic energy loss in the DMFC system. that combine lower methanol permeability with Nafion-level
This also means that, to maintain the overall water balance, the protonic conductivity. Such membranes will enable more con-
significant mass of water leaving the cathode exhaust has to be centrated anode feeds; less exacting control of methanol con-
returned to the anode using condensers and pumps. centration in the anode feed loop; and an ability to maintain
high fuel utilization under dynamic load conditions.
Alternative membranes The key is going to be overcoming the strong tie between pro-
One of the fundamental challenges confronting DMFC pio- tonic conductivity and high methanol permeability in polymer
neers is the realization of proton-conducting polymers with membranes (both properties scaling with water content). The
reduced methanol permeability – particularly relevant for schemes attempted so far have been mostly based on either
“mainstream” DMFCs based on water/methanol anode feeds. “seeding” the poly(PFSA) membrane with highly dispersed
In these conventional designs, the high methanol permeabil- hydrophilic oxide, or varying the polymer nanopore network
ity of poly(PFSA) membranes means that the local fuel con- structure by modifying the polymer’s chemical nature to
centration in the anode flow field has to be maintained at levels achieve essentially the same effect of enhancing the proton-to-
of less than 1 M methanol. This is necessary to achieve a suffi- methanol mobility ratio.
ciently high ratio of cell current to crossover current, and After several years of work along these lines, a number of
thereby secure acceptable fuel utilization. groups have reported promising results. In 2003, PolyFuel
Yet operation with such a dilute solution was previously con- announced that it was ready to manufacture its proprietary Z1
sidered impossible, based on a methanol permeation rate equiv- membrane.8 Compared with the most commonly used
alent to about 0.1 A/cm2, measured across a 175 µm-thick Nafion Nafion 117, the Z1 membrane is characterized by a threefold
membrane (Nafion 117) in 1 M solution at approximately 70 °C. reduction in both methanol and water permeation, without a
This rate of permeation is similar to the DMFC current densities, significant decrease in proton conductivity.
suggesting at first glance an unacceptable fuel utilization of no Elsewhere, a joint effort between Virginia Polytechnic
Performance stability
Work on advanced catalysts and membranes notwithstanding,
it is the long-term stability and durability of DMFCs that will
go a long way towards determining the success or otherwise of
commercial products out in the marketplace. As with other Scientists at Los Alamos National Laboratory recently
fuel-cell systems, however, the extensive study of DMFC per- performed a 3000 h lifetime test on a single-cell, liquid-fed
formance decay over, say, 103–104 h of operation is very much a DMFC. Cell temperature was 75 °C; cell voltage was 0.5 V. The
work in progress. current spikes are caused by short interruptions in the steady-
Figure 2 illustrates the measured drop in current with time of state operation of the cell, resulting in the reversal of
a single-cell DMFC operating at 75 ºC with a 0.3 M methanol “recoverable” performance loss.
feed. The total loss of about 40% of the initial current after 3000
h can be resolved into recoverable and unrecoverable losses,
where the recoverable portion is defined as the loss that can be layer and/or gas-diffusion layer (backing), often caused by a
reversed by interrupting the steady-state operation of the mismatch between the water-generation rate under high cur-
DMFC. The following phenomena have been identified as being rent operation and the air flow/pressure; a temperature drop
responsible for the degradation of DMFC performance over that causes local condensation; or, particularly, by gradual loss
extended operating periods: of the hydrophobic properties of the backing. Flooding can be
● Surface oxidation of the cathode catalyst (recoverable); partially reversed by stopping the cell and letting the cathode
● Cathode flooding;
dry for a while, possibly assisted by a stream of dry air. And
while some of the performance loss is unrecoverable, because
● Ru migration from anode to cathode and subsequent
of the generally irreversible nature of the change in the
deposition of Ru at the cathode; and hydrophobic properties of the cathode backing, it’s likely that
● Loss of active-catalyst surface area on either electrode. further improvements in overall design and wet-proofing of
the backing layers will help to mitigate the problem.
Let’s take a look at each of these contributory factors in more Migration of Ru through commonly used DMFC mem-
detail. When a DMFC is operated at a higher voltage targeting branes and its deposition at the cathode is another perform-
a high conversion efficiency (as in figure 2), the cathode poten- ance-loss mechanism that was recently studied in detail at Los
tial is sufficiently high (≥ 0.8 V) to encourage a slow, continuous Alamos National Laboratory.10 Ru negatively impacts on the
process of Pt surface oxidation. This Pt surface-oxide build-up cathode performance, as the Ru-covered Pt surface is an infe-
(and/or “ageing”) has been shown to significantly accelerate rior electrocatalyst for oxygen reduction and a better catalyst
with temperature at a given cathode potential inside the for oxidation of crossover methanol than pure Pt. Both effects
“Pt-oxide range”. Such surface-oxide formation inhibits the rate typically lead to a lowering of the cathode potential (cell volt-
of oxygen reduction at the cathode, reflected in a gradual drop- age) by as much as 40–50 mV, but in extreme contamination
off in DMFC performance over time. This decay-causing cases, possibly resulting from cell “maltreatment”, this loss
process can be reversed, however, by very short, periodic low- can reach 200 mV.
ering of the cathode potential (i.e. by brief lowering of the cell Ru migration appears to be caused by the nature of the active
voltage), resulting in electroreduction of the surface oxide and Pt–Ru blacks (unsupported catalysts) commonly used in the
regeneration of active Pt sites. This component of the decay is DMFC anode. In liquid-fed DMFCs with significant net water
consequently recognized as being (a) recoverable, and (b) less flux from anode to cathode, Ru species, most likely nanoparti-
likely to have similar magnitude at lower cell voltages. cles of RuO2 (abundant in Pt–Ru black catalysts), tend to leach
The phenomenon of cathode flooding, meanwhile, has been from the anode catalyst, and ultimately end up on the other side
amply documented for low-temperature fuel cells in general. It of the cell. The resulting cathode contamination by Ru is largely
results from slow accumulation of water at the cathode catalyst irreversible. Evaluation of the phenomenon suggests that fur-
ther optimization of the anode catalysts – for example, reduc- better dispersion of catalyst particles and advanced design
tion in “loose” Ru oxide species in the anode catalyst – should of electrode layers.
help to minimize any migration. ● Synthesizing polymer-electrolyte membranes with
Finally, it’s worth noting that the active surface area of both significantly reduced permeability to methanol and water,
electrodes can be halved in less than 2000 h of cell operation while maintaining high levels of protonic conductivity
under the operation conditions shown in figure 2. And while and performance durability.
surface-area loss of the anode is associated with a relatively
small performance loss, a similar decrease in the surface area When it comes to the catalyst, current DMFC MEA fabrication
of the cathode leads to a larger performance penalty. techniques do not allow for utilization greater than 50–60%.
What’s more, the possible advent of ultra-high-surface-area cat-
Taking stock alysts may actually lead to a further drop in utilization unless
Polymer-electrolyte DMFCs have advanced on many fronts in more sophisticated catalyst-layer-preparation techniques are
recent years. Alongside fundamental progress on the core elec- developed. Theoretical modelling of catalyst nano-array spatial
trocatalyst and MEA technologies, particularly Pt–Ru-based geometry will almost certainly shed light on this problem ini-
anodes, an innovative approach to cell and system design has tially, while further ahead the experimental use of nanotechnol-
helped developers get to grips with the problem of methanol ogy tools for fuel-cell fabrication will open up all sorts of
crossover – even when employing the “leaky”, but commer- intriguing opportunities for DMFC researchers.
cially available, Nafion membranes.
As a result, it is now possible to reach an areal power density Further reading
of 50 mW/cm2 at a relatively high cell voltage of 0.5 V (figure 2); 1. R Harris, D Book, P Anderson and P Edwards 2004 “Hydrogen
a maximum areal power density (of between 200 and storage: the grand challenge” The Fuel Cell Review June/July 17–23.
250 mW/cm2) is achievable at a voltage roughly 0.2 V lower at 2. E Peled, T Duvdevani, A Aharon and A Melman 2001 Electrochem. Solid-
the same cell temperature. This corresponds to a DMFC stack State Lett. 4 A38.
3. M Watanabe and S Motoo 1975 J. Electroanal. Chem. 60 275.
with a potential power density and efficiency combination of
4. Y Tong, H S Kim, P K Babu, P Waszczuk, A Wieckowski and E Oldfield
150 W/dm3 and 30%. Figures of merit like this suggest that 2002 J. Am. Chem. Soc. 124 468.
DMFCs can provide a portable-power technology that is supe- 5. H Dinh, X Ren, F Garzon, P Zelenay and S Gottesfeld 2000 J. Electroanal.
rior to incumbent rechargeable batteries (see p25). Chem. 491 222.
In summary, DMFCs are now about to enter the first phase of 6. X Ren, M S Wilson and S Gottesfeld 1996 J. Electrochem. Soc. 143 L12.
commercialization as small-scale power sources. Yet while that 7. X Ren and S Gottesfeld 2001 US Patent No. 6 296 964.
counts as a big leap forward, there is still plenty of scope for fur- 8. P Cox, S-Y Cha and A Attia 2003 Fuel Cell Seminar Book of Abstracts
ther progress – especially with respect to the kinetics of both 977–980. Presented at 2003 Fuel Cell Seminar, Miami Beach, FL, US.
electrode reactions. As far as fundamental research goes, the 9. Y S Kim, M J Sumner, W L Harrison, J S Riffle, J E McGrath and B S
following aspects need to be prioritized by the multidiscipli- Pivovar J. Electrochem. Soc. In press.
nary teams tasked with moving things forward. 10. P Piela, C Eickes, E Brosha, F Garzon and P Zelenay J. Electrochem. Soc.
In press.
● Designing better and more stable anode catalysts that
DMFCs power up
for portable devices
S HIMSHON G OTTESFELD
Innovation in systems design and engineering will be critical if direct-methanol fuel cells are to
make the final transition from prototype demonstrations into mass-market power sources.
the power source that is the key figure of merit in terms of sys- maximizes the two efficiency-determining factors:
tem packaging. Under these circumstances, it is the energy den- a) Fuel utilization – that is, the conversion of fuel feed to
sity, rather than the specific energy, that is of greater interest. cell current;
The equivalent of equation 1 will then be equation 2. b) Fuel-cell voltage at the power demand by the load.
It is clear that designers must keep in mind the following pri-
orities if they are to capitalize on the intrinsic energy-density At present, the choice of fuel for portable power applications is
advantage of the fuel in a fuel-cell power source. effectively limited to hydrogen and methanol. But, as discussed
● Maximize E
wt
fuel (equation 1) with:
in the previous article (“Researchers redefine the DMFC
roadmap”, p17), there are significant problems associated with
a) Fuels of high energy density and significant
the storage of hydrogen for portable fuel-cell applications. The
electrocatalytic activity at well below 100 °C;
most promising solution appears to be the use of metal
b) Realistic fuel-storage options that maintain a large hydrides or chemical hydrides (see “Chemical warfare”, The Fuel
volume/weight fraction of the neat fuel and that are Cell Review June/July 2004 p10). In the former, controlled heat-
acceptable for handheld, consumer electronics ing is used to generate hydrogen, while the latter comprise a
applications. hydrogen-releasing solid (like sodium borohydride) that
typical hydride @ neering challenge in the DMFC, a system that aims to capital-
0.5 Wheff /cm3 fuel
80 ize on the simplicity of direct use of unprocessed liquid fuel of
high energy density.
60
Nevertheless, with optimized Pt-Ru alloy catalysts and well
40 prepared electrode structures, DMFCs can generate a maximum
DMFC @ areal power density in the range of 30–60 mW/cm2 at a temper-
20 1.5 Wheff /cm3 fuel
ature of around 45 °C. This is with no active air feed to the other
0 electrode, so that the cell is said to be operating in “air breathing”
0 2 4 6 8 10 12 14 16 18 20 22 24 26 28 30
energy (Wh) mode. A volume power density of around 100 mW/cm3 is pos-
sible under the same conditions. And while this figure of merit
Calculated total system volume as a function of the energy may be five times lower than that of a hydrogen–air cell, the
content of three portable power systems: a prismatic lithium-ion advantages of methanol (as a liquid fuel of superior energy den-
battery, a hydrogen–air fuel cell with metal-hydride fuel, and a sity) and the simplicity of the DMFC system provide a winning
DMFC. Projected energy-conversion efficiencies used to combination all the same (as shown in figure 1).
generate these plots are 30% for the DMFC and 50% for the The plots in figure 1 reveal the potential lowering of the over-
hydrogen–air fuel cell. The figure of merit quoted for the lithium- all system volume for 1 W fuel-cell systems compared with the
ion battery (0.2 Wh/cm3) is widely considered state-of-the-art, volume of a lithium-ion battery of energy density 0.2 Wh/cm3
though some advanced lithium-ion batteries have recently been – that’s as a function of overall energy content or use time (the
reported with values as high as 0.4 Wh/cm3. A ceiling near number of Wh equals the number of hours of use at the 1 W
0.5 Wh/cm3 is expected for rechargeable lithium batteries. power output considered). At a fuel-cell power density of 100
mW/cm3 (100 W/dm3), the energy density of a DMFC system
will exceed that of the lithium-ion battery for use times exceed-
undergoes a controlled reaction with water. A variant has also ing 4–6 h – assuming a BOP volume of 10 cm3 (equal to that of
been proposed based on direct electrochemical oxidation of a the fuel cell) and a system conversion efficiency of 20–30%.
hydride – employing potassium borohydride fuel dissolved in The lowest of the three parallel lines in the figure shows that,
an aqueous alkaline solution. at the projected volume of 20 cm3 for fuel cell plus BOP, sig-
The advantage of hydrogen fuel is its superior electrocat- nificant volume savings over the battery are obtained for use
alytic activity, particularly at low fuel-cell temperatures. It is times longer than 6 h. Furthermore, as the other two lines
far easier to achieve higher power density with a hydrogen- show, similar savings are still possible at slightly longer use
fuelled cell stack, which in turn also means a higher energy- times of 7–10 h, even if the volume of the non-fuel-contain-
conversion efficiency (because a hydrogen–air fuel cell would ing part of the system is 50%, or even 100%, greater.
be likely to provide the power demand at a higher voltage per Considering that the target use time per single refuelling is
cell). Unfortunately, however, a significant downside associ- typically between several days and one week, figure 1 clearly
ated with the potential use of hydrogen in portable-power shows that the effective energy content of the fuel, E vfuel, is the
applications is the limited energy packaging that is possible most significant parameter in establishing the energy-density
with realistic hydrogen-storage options. The overall weight advantage of the fuel-cell system.
percent of hydrogen in relevant metal hydrides (those releas-
ing hydrogen at temperatures under 100 °C) is as low as 1–2%; DMFC technology platforms
for the chemical hydrides, assuming the need to carry the Until very recently, DMFC system implementations were
water for the reaction, this figure can reach 6–8%. At 8% by overly complex, largely because of the difficulties associated
weight, Ewtfuel reaches a value of 2.4 Wh/g. That’s about 40% of with management of the fuel and, primarily, water. (The previ-
that of liquid methanol, which stores energy at 6.1 Wh/g. ous article provides a detailed discussion of the problems
Additionally, whereas safety concerns arise regarding the use caused by methanol crossover and water permeation through
of hydrogen in mass-market consumer products, neat the electrolyte membrane; see p17.) The challenge for the
methanol is a liquid that not only lends itself to simple pack- DMFC system designer is to reconcile the target of using neat
aging and distribution, but also raises little safety concern in (100%) methanol in the fuel tank/cartridge – to achieve the
handling and/or disposal at the quantities needed for power- greatest energy-density advantage – with the need for a suffi-
ing a portable electronic device. cient water supply to the anode. The mainstream approach to
pump driver
and logic
two 12-cell DMFC stacks
MeOH feed pump
water recovery
pump
recirculation
pump
water
anode out
Military R&D
Stationary power
GTI takes the longer view Sustainable success
GTI is a not-for-profit organization that MTU has been evaluating the direct
provides research, development and training to conversion of sustainable biofuels in
the natural-gas industry, as well as to emerging molten-carbonate fuel cells.
energy markets such as those based on
hydrogen and fuel-cell technology. The 38
researchers reporting to Gerry Runte in the Molten-carbonate fuel cells (MCFCs) are shap-
Hydrogen Energy Systems Center are involved ing up as a clean, high-efficiency platform for
in a range of activities embracing hydrogen decentralized cogeneration of electricity and
energy, alternative-fuelled vehicles, high- and heat using biofuels such as sewage gas and land-
low-temperature fuel-cell components and fill gas. And this sustainable slant on MCFC
systems, and fuel processors and catalysts. technology could be ready for widespread com-
In addition to its work on SOFCs, for mercial applications within the next five years,
example, the division is developing ways to according to a presentation from MTU CFC
improve the cost of components (such as Solutions at the Fuel Cell World conference in
membranes) in proton-exchange-membrane being proposed at a test facility in the south- Lucerne, Switzerland, earlier this summer.
fuel cells. It is also looking at direct-methanol west of the US: one combines photovoltaic and The German company knows a thing or two
fuel cells for low-power applications and membrane technologies to break down water, about MCFCs. For starters, it boasts an impres-
undertakes outsourced R&D into while the other uses the sun’s thermal energy to sive track record when it comes to the develop-
molten-carbonate fuel cells. crack water at high temperatures. ment of integrated MCFC systems in the
Meanwhile, other members of Runte’s team, GTI generates revenue from a number of 250 kW regime. Its so-called HotModules have
led by Bill Liss, are building a hydrogen fuelling sources: contract research, technology been put through their paces in a comprehen-
station for the US Department of Energy and development and education programmes; sive field-trial programme that’s been running
working on prototype hydrogen-production royalties and licence fees from GTI since 2001 at eight test sites across Germany,
systems. For the time being, these mostly run technologies that have been incorporated into including hospitals, industrial plants and tele-
on natural gas but, according to Runte, “the commercial products and services; direct coms exchanges. All of these systems are based
real deal is processing diesel and JP8”. The support from its investors for medium-term on a natural-gas fuel supply.
division is also researching methods of storing R&D; and the activities of GTI subsidiaries and At the same time, MTU and several European
hydrogen, such as solid-state storage in the technology investments. partners have been evaluating MCFC system
form of metal hydrides. GTI’s work on the 10 kW SOFC generator is performance with a range of biomass-based
In the near term, Runte hopes to receive led by Mike Onischak, head of hydrogen secondary gases – although only in laboratory
funding to research the use of solar power for production activities, and Robert Remick of the demonstrators so far. The studies have focused
hydrogen generation. Two solar projects are high-temperature electrochemistry group. on the development and design of adapted gas
clean-up systems for agricultural applications
and sewage-treatment plants. In each case, the
plant. Versa Power is a US-based joint venture If things go to schedule, the evaluation researchers report no problems when the
between GTI, FuelCell Energy, Materials and process should be completed sometime in MCFC stacks are operated using biogas and coal
Systems Research Inc, the University of Utah March 2005, after which the partners plan to gas. Post-test analysis indicates no adverse
and the Electric Power Research Institute. combine the best elements of their two systems interactions between biogas or coal gas and the
According to Runte, the collaboration with and scale up to a 10 kW SOFC platform. In the fuel-cell system components.
Versa Power enables the partners to work from final phase of the project (which is currently MTU reckons that its HotModule design is
a systems standpoint from day one. “Fuel-cell not funded), the aim is to optimize the hard- “perfectly adapted to the direct utilization of
and fuel-processing technologies are not plug- ware into a beta prototype unit. The whole pro- hydrocarbons and synthesis gases” – such as
and-play, so you need to work closely with the gramme is expected to take around three years. biogas, mining gas, synthesis gases from pyrol-
system,” he explained. Looking ahead, it’s clear that SOFC genera- ysis and other thermal-gasification products of
By the beginning of next year, the goal is to tors of this type could find plenty of applica- biomass and/or waste materials. In their paper
have both 3 kW SOFC prototypes ready for tions beyond the military arena. “The most at the Lucerne conference, MTU’s Alexander
evaluation by another of the partners in the logical non-military application is as auxiliary Gienapp and Gerhard Huppmann point out
contract, the US Department of Defense Fuel power supplies for large trucks,” noted Runte. that the MCFC converts gases with a high
Cell Test and Evaluation Center (FCTec), which Use of SOFC generators would mean that methane content to electricity with an effi-
is based in Johnstown, Pennsylvania. A range truckers would no longer have to idle their ciency of around 50% (which drops to around
of technical specifications will be assessed, engines to power climate-control systems and 42% for synthesis gases such as hydrogen and
including fuel efficiency, stack performance, electrical accessories (such as CD players and CO). They conclude: “The utilization of bio-
effectiveness of sulphur removal and durabil- TVs) in the cab and sleeper compartments of mass-based secondary gases is the most impor-
ity of the SOFC stack. FCTec will also consider their vehicles. It’s also worth noting that NASA tant and attractive application of the carbonate
whether the protocols that currently guide the and leading aircraft manufacturers like Boeing fuel cell. This would reduce [atmospheric] CO2
design and manufacture of today’s military are looking into how they could use SOFCs in production enormously.”
generators are appropriate for next-genera- auxiliary power systems. Volume manufacture of MTU’s HotModules
tion, fuel-cell-powered systems. Siân Harris is slated to begin in 2006. ●
Consumer electronics
Transportation
steam
water
combustion
out the answer to their very own multibillion- recuperator
primary start-up exhaust
fuel
dollar conundrum: how to transition fuel-cell air inlet
cars from trade-show curiosity into mass-
market phenomenon. More specifically, they
combustion
start-up
vaporizer
reformer
want to know how they can ensure that the
mixer
air exhaust
zone
transition from A to B dovetails seamlessly air recuperator
with the roll-out of an international network
of hydrogen-fuelling stations. spark-
Yet with capital investment in that fuelling plug port
infrastructure likely to be staggered over prewarmed air
decades rather than years, car manufacturers
will need to make some incremental moves in
the interim – one of which could involve the Above: system overview of PNNL’s rapid-start
reforming of gasoline to hydrogen on board a reforming gas flow steam reformer. The red elements are active
fuel-cell vehicle. The favoured technique uses a only during the start-up phase, while the blue
fuel processor based on steam reforming, in elements come into play only during steady-
which hydrocarbon fuel reacts with steam at state operation. The new panel configuration
high temperatures over a catalyst to produce (left) for the steam-reforming reactor
hydrogen and carbon monoxide. Steam reform- combustion provides very short flow distances for the
gas flow
ing is the most cost-effective method of generat- heating gas. Hot gases flow through the large
ing hydrogen, and is also the most efficient. surface-area of the panel.
Unfortunately, there’s a snag. To date, the
best steam-reformer prototypes have taken steam-reforming reactor, causing it to heat up.
around 15–20 min to reach a temperature high The reactor is also a microchannel device that
enough to start generating hydrogen – a delay contains supported catalysts inside its flow
that isn’t going to pass muster with the average channels. Additional heating is provided by the
driver intent on beating the morning gridlock. combustion gases, which travel in a cross-flow
Now, however, engineers at Pacific Northwest arrangement.
National Laboratory (PNNL) in the US have high rates of heat and mass transfer and rapid ● After steam has flowed for a few seconds, fuel
made what looks like a fundamental break- steam-reforming kinetics. is injected into the steam plume and the
through: a compact steam reformer that can “The key feature of the new design is that the fuel–steam mixture flows past the catalyst in
produce large amounts of hydrogen-rich gas reforming reactor and water vaporizer are con- the reactor to produce syngas – a mixture of
from liquid gasoline in only 12 s. figured as thin panels, with the hot gases flow- hydrogen, carbon monoxide, carbon dioxide,
ing through the large surface area of the panel,” methane and steam. Reformation occurs at
Hot stuff said Greg Whyatt, lead engineer on the project. temperatures of 650 °C and above. At this
The reformer is the highest-temperature com- “The panel configuration also allows higher point, carbon monoxide (CO) concentrations
ponent within a fuel-processing system, and combustion temperatures and flows without are relatively high – about 15 mole per cent at
therefore represents the biggest hurdle to risking damage to the metal structure.” steady state, with a steam:carbon ratio of 3.
rapid start-up. Hence the PNNL demonstrator So what are the building blocks of the PNNL Since proton-exchange-membrane (PEM) fuel
looks like a notable advance towards a com- system, and how do they work? In outline, the cells can only support about 10 ppm of CO at
plete on-board fuel processor that is able to steam reformer consists of a number of vapor- steady state, its concentration needs to be
start up from cold in 30 s – a milestone that the izers, reactors, heat exchangers and a combus- reduced to acceptable levels by the subsystems
US Department of Energy (DOE) would like to tor linked together in the following way: that follow. On the other hand, the reformate
reach before 2010. Central to PNNL’s success ● At start-up, the fuel is burned in a combustor, could be used as it stands for solid-oxide fuel
is the use of microfabrication techniques to which provides heat to produce the steam. The cells, which can run on a CO feedstock.
fashion a series of tiny catalyst-loaded chan- steam generator is a microchannel device ● From the steam-reforming subsystems, the
nels inside the reforming reactor. These designed to provide very low combustion-side gases flow into a high-temperature recupera-
microchannels ensure low resistance to com- pressure losses. tor, which extracts enough of the heat for the
bustion gas flows, which in turn equates to ● Steam from the generator flows through the flow to become compatible with the next part
of the system, the water-gas-shift subsystem. Review. “This can be accomplished; it’s largely (APU) on a military vehicle. Ultimately, the
Recuperated heat is recycled to produce steam, a budget issue rather than a technical barrier.” goal is to operate the APU on diesel fuel. In a
and to drive the endothermic steam-reforming He added: “We also need to continue to lower related development, Battelle launched a spin-
reactions. PNNL is also developing a new two- system mass, even though we are compatible out company, Velocys, in 2001 to commercial-
stage water-gas-shift subsystem that lowers the with DOE targets now. As a national lab, we are ize microchannel technology for merchant-
CO content by “shifting” it to carbon dioxide focused on showing the feasibility of our hydrogen, ethylene production and other
by reaction with the steam (and using catalysts approach and not necessarily developing a pro- chemical-industry applications.
from various commercial suppliers). totype ready for large-scale manufacture. As “It is difficult to estimate when real large-
● The next stage is a preferential oxidation sub- such, our reactor designs tend to be overly scale commercial deployment will occur, but
system. This reactor lowers the CO content to robust, so they could be trimmed down.” APU development on the 1–5 kW scale could
10 ppm or less, by preferentially adsorbing the Lack of long-term stability in the presence of happen in the next five years or so,” claimed
gas onto a catalyst surface, where it is oxidized sulphur (a common constituent of transporta- Pederson. He cites the collaboration between
to carbon dioxide. A heat exchanger subse- tion fuels) is another significant obstacle. Delphi Corporation and BMW, for example,
quently adjusts the temperature of the refor- Sulphur tends to adsorb onto catalyst surfaces which has already demonstrated an APU based
mate steam to ensure compatibility with a and poison them. It also deposits onto the reac- on solid-oxide fuel cells. That system operates
PEM fuel cell. tor walls and must be removed to very low lev- on gasoline and uses a partial-oxidation
● A condenser/vapour-liquid separator (devel- els in order to prevent rapid performance reformer. The bottom line, says Pederson, is
oped at PNNL) can then be used to adjust the degradation in PEM fuel cells. “We have a small that APUs are a key application for fuel cells –
vapour pressure in the reformate to the desired effort in this area now and hope to expand it,” one in which “many of the technical require-
level. This device is also intended to recover noted Pederson. ments of the reformer would be relaxed, such
moisture from gas flows leaving a PEM fuel cell. Meanwhile, as a prelude to commercializa- as start-up time and start-up energy”.
tion, the scientists will need to couple their Belle Dumé, Paris
A matter of prioritization reformer into working fuel-cell systems to
Despite the encouraging progress, PNNL optimize efficiency and long-term durability. Further reading
acknowledges that there’s plenty of work still With this in mind, Battelle Memorial Institute G A Whyatt et al. 2004 Development of a
to do. Top of the list is the systems engineering. in Columbus, Ohio, which operates PNNL for rapid-start on-board automotive steam
“We need to integrate all of our subsystems so the DOE, is currently developing a microchan- reformer. Presented at the American Institute
that they operate together seamlessly,” Larry nel fuel processor/PEM fuel-cell system for Chemical Engineering 2004 Spring
Pederson, the project leader, told The Fuel Cell intended for use as an auxiliary power unit National Meeting (New Orleans, Louisiana).
Safety
Handle with care. That’s a mantra that scien- 18% by volume at normal temperature and
tists, technologists and engineers would do well pressure – compares well to methane (6.3%)
to remember when working with hydrogen and propane (1.1%). Also, hydrogen’s lower
and fuel-cell systems. Whichever way you look concentration limit for ignition (4% by volume)
at it, hydrogen is a tricky gas to deal with. It’s is roughly the same as that of methane (4.4%),
highly volatile and flammable; it can explode and a lot better than that of propane (1.7%).
when mixed with air in certain concentrations; Clearly, argues Wasserle, a well-thought-out
and it leaks through small orifices more rapidly strategy on hydrogen detection and safety will
than any other gas – 2.8 times faster than go a long way towards eliminating the risks of
methane and 3.3 times faster than air. ignition or explosion in automotive fuel-cell
A slippery customer like this demands spe- applications – even if putting such a strategy
cial treatment. Specifically, that means a bul- into practice is far from straightforward.
letproof approach to fuel-cell system design –
one that minimizes any fuel leaks as well as Drive on: hydrogen sensors can eliminate the Think safe, stay safe
monitoring for leaks on an ongoing basis dur- risks of ignition or explosion in automotive On-board vehicle monitoring imposes a string
ing the system’s lifetime. Nowhere is this more and industrial fuel-cell applications. of exacting requirements concerning the per-
important than in early-stage fuel-cell vehicles, formance and technical specifications of a
in which the considerable technical obstacles Wasserle, product line manager for hydrogen hydrogen sensor. Long lifetime, cast-iron dura-
to commercialization are matched, to a degree, sensor modules at MST Technology (formerly bility and a compact footprint are a given as far
by the negative public perception of hydrogen ATMI), Germany. Yet that fear is somewhat as the car industry is concerned – as are low
created by more than 60 years of bad press. misplaced. In fact, hydrogen is no more or less power consumption and a wide operational
“Many people are scared of using hydrogen dangerous than many flammable liquid or temperature range. Another must-have is
because they have the story of the Hindenburg gaseous fuels in common use today. The mini- compatibility of the sensor’s signal output with
in the back of their mind,” says Elizabeth mum concentration needed for detonation – in-vehicle control systems (such as the
CANbus serial data communication protocol the balance of plant. Second, there’s the loca-
employed by leading car makers, including tion of leaks during repair and maintenance.
BMW, Volvo, Saab and Renault). And finally, there’s the 24/7 monitoring that’s
Taking all of this into account, MST claims needed when a vehicle is out on the road.
that its intelligent H2 Sensormodule is the For now, Sensistor is concentrating its ener-
“ideal solution” for the detection of hydrogen gies on the first two areas, although the firm
in not only vehicular, but also stationary appli- also has detectors installed in several prototype
cations. It’s an electrochemical three-electrode hydrogen and fuel-cell vehicles. When it comes
device that uses a special membrane to selec- to on-board systems, Nylander believes that
tively distinguish hydrogen, while excluding simply identifying a higher-than-usual level of
other gases such as carbon monoxide, nitrogen hydrogen is not enough. Intelligent monitor-
oxide or gasoline. The sensor is capable of ing is what counts. “You don’t just want to
detecting hydrogen concentrations as low as know that there is hydrogen in a car, because
100 ppm. Response time is less than 5 s and there are a number of other sources of hydro-
power consumption is just 800 µA. gen, such as cigarette smoke or flatulence. You
Wasserle says that one important advantage want to know if it [the hydrogen] is from the
is the sensor’s size – the standard product meas- fuel and whether it’s dangerous.”
ures just 58 × 22 × 22 mm. This makes it suitable At the heart of Sensistor’s flagship product,
for large-scale transport applications in cars, the H2000, is a field-effect-transistor sensor
trucks and boats, although she claims that it that is able to detect and locate leaks as small
could also pave the way for integration into as 5 × 10–7 mbar-l/s (or 0.5 ppm). The unit
portable electronic devices. And because the includes a suite of powerful algorithms to
sensor is based on a modular design, Wasserle evaluate the source of any hydrogen. A leak,
says it can be adapted to fit custom require- for example, will yield a fairly constant supply
ments as necessary. of hydrogen, while other sources (such as
Another critical factor is temperature per- cigarette smoke) are characterized by concen-
formance. In-car systems must be able to han- trated bursts of hydrogen that disperse rapidly
dle seasonal variations, as well as geographical with proper ventilation.
extremes ranging from the blistering heat of Smart sensing: the market for intelligent Countermeasures aside, sensible vehicle
an Athens summer to the dead of winter in hydrogen-sensing modules will grow in line design and strict quality assurance will go a
downtown Montreal. For this reason, MST’s with the commercial development and roll-out long way towards minimizing the risks associ-
hydrogen sensor operates from –25 to 85 °C. of fuel-cell vehicles. MST’s H2 Sensormodule ated with hydrogen leakage. For the engineer-
“There are many hydrogen sensors available, (top) and Sensistor’s H2000 (bottom) are just ing teams at Ford, Toyota, Honda and the like,
but most have an upper limit of around 40 or two of the products that are currently being it’s not just a case of making sure that a fuel-cell
50 °C,” claims Wasserle. “For many applica- lined up to meet the car makers’ needs. system is leak-proof at the outset, but also of
tions this is fine, but fuel cells often operate at taking into account the likely effects of wear
higher temperatures.” some serious pedigree, evidenced by a cus- and tear thousands of miles down the road.
Beyond the standard product that MST tomer base that includes Whirlpool, Electrolux, The fuel-cell system “may be leak-tight at the
launched last year, Wasserle reckons that there’s Bosch and GM. Early on, the company chose to start, but you have to consider what might hap-
plenty more innovation to come. “For our next use hydrogen as a “tracer” gas and developed a pen in two years’ time and ensure adequate
generation [sensor] we will use a new measure- family of dedicated sensors to support its ventilation of critical areas”, adds Nylander.
ment principle that is independent of oxygen,” approach. The tracer is normally a ready-made One thing is clear: while the development of
she says. The product, slated for commercial industrial gas mixture containing 5% hydrogen hydrogen and fuel-cell vehicles may still be in its
launch at the end of 2005, is based on a novel in a carrier gas such as nitrogen. infancy, companies like MST, Sensistor and their
solid-state gas sensor. “In addition to the new “We introduced hydrogen as a tracer peers are already betting that on-board hydro-
measurement principle, the sensor modules because the molecules are very small and dis- gen monitoring will prove to be a long-term
will have an extended temperature range (–40 sipate very quickly – ideal for pinpointing leaks money-spinner. It won’t be an easy market to
to 125 °C) and a longer lifetime (up to 10 years).” in pipes and testing the tightness of industrial crack, however. The car manufacturers are
components and systems,” adds Nylander. demanding customers, and they will be pushing
Technology transfer “Having been a supplier of hydrogen leak-test- for sensor/detector companies to deliver a
However, having a good sensor is only part of ing equipment for many years we have a lot of “triple-whammy” of ongoing miniaturization,
the story, says Claes Nylander, managing direc- expertise and know-how, so we think we have a enhanced levels of intelligence and price reduc-
tor of Sensistor Technologies, Sweden. “People unique position in the emerging [hydrogen tion in their next-generation products.
can go the wrong way with specifying sensitiv- and fuel-cell] market.” Even so, Nylander shares Wasserle’s view that,
ity and response time for sensors,” he explains. Nylander identifies three areas in which apart from anything else, hydrogen sensors are
“With hydrogen-[fuelled] cars, for example, Sensistor’s technology can help with the going to be essential tools for alleviating public
you need to know that you’ll get an early, rele- design and engineering of automotive hydro- fears. “Hydrogen is odourless,” he concludes.
vant and reliable warning.” gen and fuel-cell systems. First, there’s the iden- “It’s psychological – people won’t accept hydro-
Sensistor was set up in 1981 and specializes tification of leaks during development and gen-powered cars without [appropriate] sen-
in the supply of digital leak-detection systems production – whether the leak emanates from sors because they cannot smell it.”
for a range of industrial applications. It’s got the fuel-cell stack itself or somewhere else in Siân Harris