Fuel Cells For A Sustainable Energy Future

Fuel Cells for a Sustainable Energy Future
Sossina M. Haile
Materials Science / Chemical Engineering California Institute of Technology
Graduate Students: Peter Babilo, William Chueh, Lisa Cowan, Mary Louie, Justin Ho, Wei Lai, Mikhail Kislitsyn, Kenji Sasaki, Ayako Ikeda Former Participants: Dane Boysen, Calum Chisholm, Tetsuya Uda, Zongping Shao, Mary Thundathil Funding: National Science Foundation, Department of Energy, Office of Naval Research, (past: Kirsch Foundation, Powell Foundation)
Contents
The Problem of Energy
Growing consumption Consequences Sustainable energy resources
Fuel Cell Technology Overview

Principle of operation Types of fuel cells and their characteristics
Recent (Caltech) Advances

Too many to cover
Towards a Sustainable Energy Future
The Problem of Energy

The Problem
Diminishing supply? Resources in unfriendly locations? Environmental damage?
The Solution
Adequate domestic supply Environmentally benign Conveniently transported Conveniently used
World Energy Consumption

(annual)
Source: US Energy Information Agency
264 211 158 106 52 0
8.4 6.7
5.0 3.3 1.7 0
1999 totals: 2020 projections:
400 Q-Btu, 422 EJ, 630 Q-Btu, 665 EJ,
13TW 21TW
90% fossil
Equivalent Power (TW, 1012)
Exa Joules (1018)
Fossil Fuel Supplies

00 0 . E+ 0 00 0 . E+ 0 (Exa)J 00 0 . E+ 0 00 0 . E+ 0 00 0 . E+ 0
Rsv = Reserves (90%) Rsc = Resources (50%)
Unconv Conv
Oil Rsv
Source
Oil Gas Coal
Oil Rsc
Gas Rsv
Gas Rsc
Coal Rsv
Coal Rsc
Total, yrs 23 - 55 18 - 65 300
Reserves, yrs 13 - 20 11 - 25 32
Resources, yrs 10 35 7 40 270
> 400 yrs
56-77
287-345
US Energy Imports/Exports: 1949-2004

35 30 Quad BTU 25 20 15 10
Imports
Quad BTU Total
6 5 4 3 2 1
Exports
Total
Coal
5 0 1950 1960 1970 35 30 25 20 15 10 5 0 1950
Petroleum 1980 1990 2000
Petroleum 1960 1970 1980 1990 2000
0 1950
Net
65% of known petroleum reserves in Middle East 3% of reserves in USA, but 25% of world consumption
Quad BTU
1957: Net Importer
1960
1970
1980
1990
2000
Environmental Outlook
Global CO2 levels
11 1 00 0 00 0 11 1 00 0 11 1 11 1 00 0
atmospheric CO0 [ppm]
2004: 378 ppm Projections: 500-700 ppm by 2020
Anthropogenic
Fossil fuel (75%) Land use (25%)
Industrial Revolution
00 00
11 11
11 11
11 11
11 11
00 00
Source: Oak Ridge National Laboratory

year
Environmental Outlook
CO2 CH4 (ppmv) (ppmv) 800 325 300 275 250 225 200 175 700 600 500 400 300 400 300 200 100 0
CO2 in 2004: 378 ppmv

-- CO2 -- CH4 -- T +4 0 -4 -8
Thousands of years before present (Ky BP)

Intergovernmental Panel on Climate Change, 2001; http://www.ipcc.ch N. Oreskes, Science 306, 1686, 2004; D. A. Stainforth et al, Nature 433, 403, 2005 Towards a Sustainable Energy Future
T relative to present (C)
Energy Outlook
Supply Fossil energy sufficient for world demand into the forseeable future High geopolitical risk Rising costs Environmental Impact Target
Stabilize CO2 at 550 ppm By 2050
Requires
20 TW carbon-free power One 1-GW power plant daily from now until then
Urgency Transport of CO2 or heat into deep oceans:

400-1000 years; CO2 build-up is cummulative
Must make dramatic changes within next few years
The Energy Solution

1.2 x 10 TW at Earth surface 600 TW practical
5
Solar
The need: ~ 20 TW by 2050
2-4 TW extractable
Wind
Tide/Ocean Currents
2 TW gross
5-7 TW gross all cultivatable land not used for food
Biomass
Geothermal
12 TW gross over land small fraction recoverable
Hydroelectric
4.6 1.6 0.9 0.6 TW TW TW TW gross technically feasible economically feasible installed capacity
Waste disposal
Nuclear
1% / yr leakage -> lost in 100 yrs

Fossil with sequestration
The Energy Solution

Sufficient Domestic Supply
Coal, Nuclear, Solar
Environmentally Sustainable Supply

Solar (Nuclear?)
Suitable Carrier
Electricity? Hydrogen? Hydrocarbon?
Challenges
Convert solar (nuclear) to convenient chemical form Efficient consumption of chemical fuel
A Sustainable Energy Cycle

C-free Source Capture
eSolar or nuclear power plants ??? H2O, CO2
H2
Storage
Batteries
Hydrocarbon
Hydrides? Liquid H2?
Delivery
e-
Utilization
Fuel cell
H2O + CO2
A Few Words on Hydrogen Fuel Cells

Hydrogen energy density
High energy content per unit mass of hydrogen But best storage technologies are at ~ 5 wt% H2 5x the weight of gasoline (for same energy content)
Conventional hydrogen fuel cells require Pt

DOE target: 1 g/kW (0.75 g/hp) 100 hp engine 75g Pt $3,169 93% of US Pt is imported 80% of world reserves in one mine complex in SA
Another 15% in one mine complex in Russia
Converting US autos would double world consumption 4 yr auto lifetime, 20% recycling out in 40 yrs
Fuel Cells: Part of the Solution?

High efficiency
0 0 automotive engine: 11 kW - 11
low CO2 emissions
efficiency [%]
0 0 0 0 0 0 0 0
Size independent
Fuel Cells
Co
0
Various applications
stationary automotive portable electronics
ngines E ustion mb
0 0 0 0 0 0 0 0
Controlled reactions
Zero Emissions
power plant size [MW]
Operable on hydrogen
(if suitably produced)
*Can be as high as 80-90% with co-generation

Fuel Cell: Principle of Operation

best of batteries, combustion engines conversion device, not energy source
Anode
Cathode
eH2 H2 2H+ + 2eH+ O2 O2 + 2H+ + 2e- H2O
Electrolyte
Overall: H2 + O2 H2O
Fuel Cell Performance

H2 + O2 H2O
1.17 Volts (@ no current) 1.0
1.2
cross-over
0.8 theoretical voltage
fuel cross-over reaction kinetics electrolyte resistance slow mass diffusion
Voltage [V]
0.8 0.6 0.4 0.2 0.0 0.0 0.4
peak power 0.4 electrolyte resistance slow mass diffusion 0.8 1.2
0.2
power = I*V peak efficiency at low I peak power at mid I
0.0 1.6
Current [A / cm2 ]
Power [W / cm2]
voltage losses
slow reaction kinetics
0.6
Fuel Cell Components

Components
Electrolyte (Membrane)
Transport ions Block electrons, gases electrodes catalyst
Electrodes
Catalyze reactions Transport
Ions, electrons, gases
May be a composite
(electro)Catalyst + Conductors + Pore former
sealant electrolyte
Membrane-Electrode Assembly (MEA)
Fuel Cell Types

Types differentiated by electrolyte, temperature of operation
Low T H2 or MeOH; High T higher hydrocarbons (HC) Efficiency tends to as T , due to faster electrocatalysis Type C
[F]
PEM 90-110
[200-230]
AFC 100-250
[212-500]
PAFC 150-220
[300-430]
MCFC
500-700
[930-1300]
SOFC
700-1000
[1300-1800]
Fuel
Electrolyte
H2 + H2O
H2 KOH OH-
O2 + H2O
H2 H3PO4 H+ O2
HC + CO
HC + CO
Ion Oxidant
Nafion H3O+ O2
Na2CO3 CO32-
O2 + CO2
Y-ZrO2 O2- O2
By-products: H2O, CO2
Fuel Cell Choices

Temperature sets operational parameters & fuel choice
Ambient Temperature
Rapid start-up H2 or CH3OH as fuels Catalysts easily poisoned
High Temperature
Fuel flexible Very high efficiencies Long start-up
Applications
Portable power Many on/off cycles Small size
Applications
Stationary power Auxiliary power in portable systems
Technology Status
Many, many demonstrate sites and vehicles
Stationary PAFC (200 kW) at military sites since 1995 Stationary SOFC (100 kW) operated for 20,000 hrs Toyota and Honda PEM FC vehicles released 2002 DaimlerChrysler, Ford and GM, 2005; Hyundai planned
Legislation is a key driver

California zero emissions automotive standards China set for tough CAFE standards
Cost is a major barrier

Precious metal catalysts, fabrication, complexity
Uncertainty in future fuel infrastructure

Gasoline for how long? Hydrogen? Methanol?
Fuel Cell System Complexity

Membrane electrode assembly
sealant electrolyte electrodes catalyst
Electrolyte
System
Stack
Philosophy
Challenge Limitation of fuel cell materials places severe design constraints on fuel cell systems Approach Material modification for improved performance and system simplification New materials discovery for next generation fuel cell systems Novel system designs
Fuel Cell Innovations

New Electrolytes
Intermediate temperature operation
Lower the temperature below solid oxide fuel cells Raise the temperature above polymer fuel cells
New Catalysts
Enhance reaction kinetics (improve efficiency) Reduce susceptibility to poisons (reduce complexity)
Novel integrated designs

Dramatically improve thermal management Utilize micromachining technologies micro fuel cells
New Electrolytes: Solid Acids

NSF & DOE Sponsored Program (past ONR support)
PEM Fuel Cells

Proton Exchange Membrane or Polymer Electrolyte Membrane
H(H2O)n+ H2O
SO3- + (H2O)nH+
1 nm
Nafion (Dupont) saturate with H2O

inverse micelle structure
H(H2O)n+ ion transport High conductivity Flexible, high strength Requires humidification & water management Operation below 90C Permeable to methanol
(CF2)n
Kreuer, J Membr Sci 2 (2001) 185.
Target: 120-300C; examine inorganic H+ conductors

Solid Acids
Chemical intermediates between normal salts and normal acids: acid salts
(Cs2SO4) + (H2SO4) CsHSO4
d is o r d e r e d s tru c tu re
lo g ( c o n d u c t iv it y )
p o ly m e r
Physically similar to salts Structural disorder at warm temperatures Properties

Direct H+ transport Humidity insensitive Impermeable Water soluble!! Brittle
n o rm a l s tru c tu re s tru c tu ra l t r a n s it io n
T 0/ T
.
Proton Transport Mechanism
H S O Sulfate group reorientation 10-11 seconds
Proton transfer 10-9 seconds
Conductivity of Solid Acids

CsHSO4 [Baranov, 1982] CsHSeO4 [Baranov, 1982] (NH4)3H(SO4)2
[Ramasastry, 1981] 00 0 C 00 00 0 C 0 C 1 C 0 C 1 0
-0
log(conductivity) [S / cm]
-0 -0 -0 -0 -0 -0 -0
Superprotonic transition
Rb3H(SeO4)2
[Pawlowski, 1988]
Cs2(HSO4)(H2PO4)
[Chisholm & Haile, 2000]
-Cs3(HSO4)2(H2PO4)
[Haile et al., 1997]
K3H(SO4)2
[Chisholm & Haile, 2001]
00 11 00 11 00 00 . 0 . 1 . 0 . 1 . 0 . 0
0 0 /T K 00
-0
But sulfates and selenates are unstable under reducing conditions
Solid Acid Properties

The Good H+ transport only
No electro-osmotic drag No electron transport Alcohol impermeable
The Bad Known compounds are water soluble

Operate at T 100C Insoluble analogs?
Humidity insensitive conductivity Stable to ~ 250C Inexpensive Chemically non-aggressive
Few are chemically stable The Ugly Poor processability and mechanical properties
Composite membranes with inert polymers
CsH2PO4 as a Fuel Cell Electrolyte

Expected to have chemical stability
3CsH2PO4 + 11H2 Cs3PO4 + 3H3P + 8H2O dG(rxn) >> 0
But does it have high conductivity? Does it have sufficient thermal stability? Literature dispute
High conductivity on heating due to H2O loss High conductivity due to transition to a cubic phase
CsH2PO4 Dehydration
CsH2PO4 CsPO3 + H2O
pressure detector
11 .
CsH2PO4 + H2O
Tc = 230
Toper = 250C
0 0 0 0
00 . 00 . 11 . 00 . 00 0
P(H2O) operation
Cs H
2-2 x
PO
0 0 0 0
11 1
00 0
Cs
11 1
00 0
Temperature (C)
Use water partial pressure to suppress dehydration

Water temperature ( C)
Equilibrium pH O(atm)
PO
4-x
Conductivity of CsH2PO4
Temperature [ C]
00 0 11 1 00 0 00 0 00 0 00 0 0 heating st 0 cooling st 0 heating nd 0 cooling nd
Humidified air p[H2O] = 0.4 atm
o
0.42 eV
log(conductivity) [ cm ]
-0 -0
-0
-0
-0
230 C
00 .
00 .
00 .
00 .
-0
11 .
11 .
0 0 /T [K ] 00
Proof of Principle
H2O, H2 | Cell | O2, H2O
T = 235C
00 .
50 mW/cm2
before after
0 0 0 0 0 0
Power density (mW cm )
-0
Cell voltage (V)
11 . 11 . 11 . 00 . 00 . 0 voltage power
Compared to polymers High open circuit voltage

Theoretical: 1.15V Measured: 1.00 V Polymers: 0.8-0.9 V
0 0 0 0 0 0 0
Power density
Polymers: > 1 W/cm2
0 0
00 00 00 00 00 0 0 0 0 0
-0
Current density (mA cm )

260m membrane; 18 mg Pt/cm2
Platinum content
Polymers: ~ 0.1 mg/cm2
D. A. Boysen, T. Uda, C. R.I. Chisholm and S. M. Haile, Science 303, 68-70 (2004)
Fuel Cell Longevity: Stable Performance

00 .
H2, H2O | cell | O2, H2O

260 m thick CsH2PO4 electrolyte T = 235C Current = 100 mA/cm2
Cell voltage (V)
11 . 11 . 11 . 11 . 00 .
on, 000 mA/cm
off
0 0
0 0
0 0
0 0
00 0
Time (h)
CsH2PO4 no degradation in 110 hr measurement CsHSO4 functions for only ~ 30 mins (recoverable degradation)
3rd Generation Fuel Cell

Fine CsH2PO4
H2, H2O | cell | O2, H2O
T = 248C 8 mg Pt/cm2
2 m
Slurry deposit
10-40 m pores, ~40% porosity Open circuit voltage: 0.9-1.0 V

T. Uda & S.M. Haile, Electrochem & Solid State Lett. 8 (2005) A245-A246
Peak power density: 285-415 mW/cm2
Impact
S. M. Haile, D. A. Boysen, C. R. I. Chisholm and R. B. Merle, Solid Acids as Fuel Cell Electrolytes, Nature 410, 910-913 (2001).
The promise of protonics Some Like It Medium Hot
Solid Acids Show Promise...
Nature: News & Views Science Now Magazine

Physics Today Online
Fuel Cell Stack
Direct Alcohol Fuel Cells

Methanol in proton exchange membrane fuel cells
CH3OH + H2O 6H+ + CO2 + 6eCH3OH + H2O 3H2 + CO2
SAFCS ideal thermal match

Reforming rxn: 200 300C Electrolyte: 240 280C Steam reforming: endothermic Fuel cell rxns: exothermic
Integrated design
Incorporate alcohol reforming catalyst in anode chamber
Direct Methanol Fuel Cells

With reformer
00 .
T = 260 C; 47 m membrane
Without reformer
Cell voltage (V)
11 . 11 . 00 . 00 .
hydrogen hydrogen reformate methanol

42 vol% 1%CO 24%CO2
11 . 11 . 11 .
methanol
00 . 00 .
11 .
00 .
00 . 00 1.5 .
00 .
0
00 .
00 .
00 .
Current density (A/cm )

Methanol power ~ 85% H2 power For polymer fuel cells ~ 10% Reformate power ~ 90% H2 power Methanol power ~ 45% H2 power
Power density (W /cm )
11 .
Direct Alcohol Fuel Cells

With reformer
80 proof
Vodka
36 vol%
ethanol
Ethanol power ~ 40% H2 power
New Cathodes for Solid Oxide Fuel Cells

NSF & DOE Sponsored Program (past DARPA support)
State-of-the-Art SOFCs
Component Materials
cathode (air electrode) electrolyte anode (fuel electrode) (La,Sr)MnO3 Zr0.92Y0.08O2.96 = yttria stabilized zirconia (YSZ) Ni + YSZ composite
Operation: ~1000 C Fuel flexible, efficient But

All high temp materials Costly (manufacture) Poor thermal cyclability
Goal: 500 800 C Challenges

Slower kinetics Electrolyte resistance Poor anode activity Poor cathode activity
Solid Oxide Fuel Cell Cathodes

Traditional cathodes
A3+B3+O3 perovskites Poor O2- transport Limited reaction sites
(Ba0.5Sr0.5)(Co0.8Fe0.2)O2.3
Our approach
High O2- flux materials Extended reaction sites A2+B4+O3 perovskites triple-point path
O2 Oad O2Oad 2eO2
almost 1 in 4 vacant
electrode bulk path

Oad 2ecathode O2-
cathode electrolyte
O2-
electrolyte
Cathode Electrocatalysis
O2 2e
-
+
Electrolyte cathode layers
Symmetric cell resistance measurements
O2, Ar, (CO2) Ag current collectors
O=
2e O2
Equivalent circuit
Distinguish resistance contributions using frequency dependent measurements
Rcathode Relectrolyte Rcathode
Cathode Electrocatalysis
Temperature (C)
o
.cm 0)
0 0
00 0 0 00 00 00 0 0 00 0 0 0 0
00 0
00 0
0 0
O2 slow fast
Oad
2eO2O2-
cathode electrolyte
P(O2) = 0.21 atm

0 0
Cathode area specific resistance (
Ea same as oxygen surface exchange (113 kJ.mol-1)
00 .
0.5 0.6 cm2
00 .
Ea=000 kJ.mol
00 . 0
-0
Bulk diffusion is fast (46 kJ.mol-1) Other advanced cathodes (PrSm)CoO3: 5.5 cm2 (LaSr)(CoFe)O3: 48 cm2
Symmetric cell0 -electrode) ( Half cell 0-electrode) (

00 . 00 . 11 . 11 .
-0
00 . 0
11 .
11 .
0 0/T (K ) 00
Cell Fabrication
Anode supported NiO + SDC (Ce0.85Sm0.15O2) Dual dry press SDC NiO + SDC Calcine, 950oC 5h, inert gas Spray cathode Sinter, 1350oC 5h
600oC 5h, 15%H2
cathode electrolyte anode Anode: 700 m
Porous anode
Electrolyte surface
0.71 cm2
~ 20m Electrolyte Cathode: 20 m

2 m
1.3 cm
Fuel Cell Power Output

H2, 3% H2O | fuel cell | Air
00 . 11 . 11 . 00 . 00 . 00 . 0
> 1 W/cm2 at 600C!!!
00 0 00 0 0
00 00
00 00
00 00
-0
00 00
Current density (mA.cm )

Comparison: literature cathode material 350 mW/cm2 at 600C
Power density (mW.cm )
Voltage (Volts)
000 C 00 00 o 000 C o 000 C o 0 000 0 0 C o 000 C 00 0
-0
Impact
Cooler Material Boosts Fuel Cells
Z. Shao and S. M. Haile, A High Performance Cathode for the Next Generation Solid-Oxide Fuel Cells, Nature 431, 170-173 (2004).
SOFC cathode is hot stuff Next generation of fuel cells
Tech Research News R & D Focus

Fuel Cell Works
Summary & Conclusions

Sustainable energy is the grand challenge of the 21st century
Solutions must meet the need, not the hype Fuel cells can play an important role
Solid acid fuel cells

Radical alternatives to state-of-the-art Viability demonstrated; spin-off company established
Solid oxide fuel cells

Promising alternative cathode discovered
Still plenty of need for fundamental research

The stone age didnt end because we ran out of stones.
-Anonymous
Acknowledgments
The people
Tetsuya Mary Justin Zongping
Wei
Calum
Dane Kenji
The agencies
National Science Foundation, Office of Naval Research, DARPA, California Energy Commission, Department of Energy, Kirsch Foundation, Powell Foundation
Selected Relevant Publications

T. Uda, D. A. Boysen, C. R. I. Chisholm and S. M. Haile, Alcohol Fuel Cells at Optimal Temperatures, Electrochem. Solid State Lett. 9, A261-A264 (2006). T. Uda and S. M. Haile, Thin-Membrane Solid-Acid Fuel Cell, Electrochem. Solid State Lett. 8, A245-A246 (2005). D. A. Boysen, T. Uda, C. R.I. Chisholm and S. M. Haile, High performance Solid Acid Fuel Cells through humidity stabilization, Science Online Express, Nov 20, 2003; Science 303, 68-70 (2004). D. A. Boysen, S. M. Haile, H. Lui and R. A. Secco High-temperature Behavior of CsH2PO4 under both Ambient and High Pressure Conditions, Chem. Mat. 15, 727-736 (2003). R. B. Merle, C. R. I. Chisholm, D. A. Boysen and S. M. Haile, Instability of Sulfate and Selenate Solid Acids in Fuel Cell Environments, Energy and Fuels 17, 210215 (2003). S. M. Haile, D. A. Boysen, C. R. I. Chisholm and R. B. Merle, Solid Acids as Fuel Cell Electrolytes, Nature 410, 910-913 (2001). Z. P. Shao, S. M. Haile, J. M. Ahn, P.D. Ronney, Z. L. Zhan and S. A. Barnett, A thermally self-sustained micro Solid-Oxide Fuel Cell stack with high power density, Nature 435, 795-798 (2005). Z. Shao and S. M. Haile, A High Performance Cathode for the Next Generation Solid-Oxide Fuel Cells, Nature 431, 170-173 (2004). S. M. Haile, Fuel Cell Materials and Components, (invited) Acta. Met. 51, 59816000 (2003). S. M. Haile, Materials for Fuel Cells, (invited) Materials Today 18, 24-29 (2003).

Fuel Cells For A Sustainable Energy Future

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Fuel Cells for a Sustainable Energy Future

Fuel Cell Technology Overview

Recent (Caltech) Advances

Towards a Sustainable Energy Future

The Problem of Energy

Towards a Sustainable Energy Future

World Energy Consumption

264 211 158 106 52 0

5.0 3.3 1.7 0

1999 totals: 2020 projections:

400 Q-Btu, 422 EJ, 630 Q-Btu, 665 EJ,

Towards a Sustainable Energy Future

Equivalent Power (TW, 1012)

Exa Joules (1018)

Fossil Fuel Supplies

Rsv = Reserves (90%) Rsc = Resources (50%)

Resources, yrs 10 35 7 40 270

> 400 yrs

US Energy Imports/Exports: 1949-2004

5 0 1950 1960 1970 35 30 25 20 15 10 5 0 1950

Petroleum 1980 1990 2000

Petroleum 1960 1970 1980 1990 2000

1957: Net Importer

Towards a Sustainable Energy Future

atmospheric CO0 [ppm]

2004: 378 ppm Projections: 500-700 ppm by 2020

Source: Oak Ridge National Laboratory

CO2 in 2004: 378 ppmv

Thousands of years before present (Ky BP)

T relative to present (C)

Urgency Transport of CO2 or heat into deep oceans:

Must make dramatic changes within next few years

Towards a Sustainable Energy Future

The Energy Solution

The need: ~ 20 TW by 2050

5-7 TW gross all cultivatable land not used for food

1% / yr leakage -> lost in 100 yrs

Fossil with sequestration

The Energy Solution

Environmentally Sustainable Supply

Towards a Sustainable Energy Future

A Sustainable Energy Cycle

Hydrides? Liquid H2?

A Few Words on Hydrogen Fuel Cells

Conventional hydrogen fuel cells require Pt

Fuel Cells: Part of the Solution?

low CO2 emissions

power plant size [MW]

*Can be as high as 80-90% with co-generation

Fuel Cell: Principle of Operation

eH2 H2 2H+ + 2eH+ O2 O2 + 2H+ + 2e- H2O

Fuel Cell Performance

0.8 theoretical voltage

fuel cross-over reaction kinetics electrolyte resistance slow mass diffusion

0.8 0.6 0.4 0.2 0.0 0.0 0.4

power = I*V peak efficiency at low I peak power at mid I

Towards a Sustainable Energy Future

slow reaction kinetics

Fuel Cell Components

Membrane-Electrode Assembly (MEA)

Towards a Sustainable Energy Future

Fuel Cell Types

By-products: H2O, CO2