UCRL-JC-130198

PREPRINT

Unitized Regenerative Fuel Cell Systems

F. Mitlitsky
B. Myers
A. H. Weisberg
T. M. Molter

This paper was prepared for submittal to the

1998 Fuel Cell Seminar
Palm Springs, CA
November 16-19, 1998

September 10, 1998

n ce re
re mo l y
a w er na or
L iv tio rat
L a o
N ab
L
This is a preprint of a paper intended for publication in a journal or proceedings. Since
changes may be made before publication, this preprint is made available with the
understanding that it will not be cited or reproduced without the permission of the
author.
 DISCLAIMER

This document was prepared as an account of work sponsored by an agency of

the United States Government. Neither the United States Government nor the
University of California nor any of their employees, makes any warranty, express
or implied, or assumes any legal liability or responsibility for the accuracy,
completeness, or usefulness of any information, apparatus, product, or process
disclosed, or represents that its use would not infringe privately owned rights.
Reference herein to any specific commercial product, process, or service by trade
name, trademark, manufacturer, or otherwise, does not necessarily constitute or
imply its endorsement, recommendation, or favoring by the United States
Government or the University of California. The views and opinions of authors
expressed herein do not necessarily state or reflect those of the United States
Government or the University of California, and shall not be used for advertising
or product endorsement purposes.
 UNITIZED REGENERATIVE FUEL CELL SYSTEMS

F. Mitlitsky, B. Myers, and A.H. Weisberg Trent M. Molter

Lawrence Livermore National Laboratory Proton Energy Systems, Inc.
7000 East Avenue, L-174 50 Inwood Drive
Livermore, CA 94551-0808 Rocky Hill, CT 06067

Energy storage systems with extremely high specific energy (>400 Wh/kg) have been designed
that use lightweight pressure vessels to contain the gases generated by reversible (unitized)
regenerative fuel cells (URFCs).[1] URFC systems are being designed and developed for a variety
of applications, including high altitude long endurance (HALE) solar rechargeable aircraft (SRA),
zero emission vehicles (ZEVs), hybrid energy storage/propulsion systems for spacecraft, energy
storage for remote (off-grid) power sources, and peak shaving for on-grid applications.[1-10]
Energy storage for HALE SRA was the original application for this set of innovations, and a
prototype solar powered aircraft (Pathfinder-Plus) recently set another altitude record for all
propeller-driven aircraft on August 6, 1998, when it flew to 80,285 feet (24.47 km).[11]

Progress is reported on the development, integration, and operation of rechargeable energy storage
systems with such high specific energy. A primary fuel cell test rig with a single cell (46 cm 2
active area) has been modified and operated reversibly as a URFC for thousands of cycles at
LLNL.[1] This URFC uses bifunctional electrodes (oxidation and reduction electrodes reverse
roles when switching from charge to discharge, as with a rechargeable battery) for cathode feed
electrolysis (water is fed from the hydrogen side of the cell) or anode feed electrolysis (water is
fed from the oxygen side of the cell). The results of the cycle test are shown in Figure 1, and
demonstrate high cycle life with negligible degradation.[1] Improved URFC cells, with high
performance and reduced catalyst loading were demonstrated at LLNL, as shown in Figure 2.
Rapid cycle operation of URFC cells has been demonstrated at LLNL. These results were obtained
on the URFC test rig shown in Figure 3, using the cell in Figure 4. Proton Energy Systems, Inc.
has recently built a URFC test rig (Figure 5) for testing and developing URFC cells shown in
Figures 6 and 7. These cells are capable of producing up to 400 psi (2.8 MPa) gas by
electrochemical pressurization. Future designs may be capable of ~3000 psi (21 MPa).

LLNL recently started testing URFC cells using Nafion 105 membrane and reduced catalyst
loading. Cell #9804A uses Nafion 105, Hamilton Standard’s E-5 catalyst, and catalyst loading of 1
mg/cm2 per electrode. Figure 2 shows that fuel cell operation on URFCs is feasible at current
densities >2000 ASF (2.15 A/cm 2). Cathode feed electrolysis data was limited to 1200 ASF due to
cell dryout. Anode feed electrolysis data was taken at current densities >2000 ASF (2.15 A/cm2),
but has not yet been approved for publication. This figure shows that reduced catalyst loading
operation of PEM electrolyzers and URFCs is feasible, and shows that consumer markets that may
require reduced catalyst loading to achieve inexpensive unit costs at high volume may be filled by
PEM electrolyzers and URFCs. Experiments with alternate catalyst compositions and further
reduced catalyst loadings are in progress.

LLNL is working with industrial partners to design lightweight pressure vessels for hydrogen
powered vehicles, where the vessels are either conformable to existing rectangular packaging
envelopes, or are cylindrical and incorporated into new “designed from the ground up”
vehicle configurations. URFC systems coupled with lightweight pressure vessels have been
designed for automobiles and are expected to be cost competitive with primary fuel cell
powered vehicles that operate on hydrogen/air.[4] URFC powered vehicles can be safely and
rapidly (< 5 minutes) refueled from high pressure hydrogen sources, when available, to
achieve driving ranges in excess of 360 miles (600 km). URFC powered systems could save
the consumer the capital cost of a home hydrogen generation unit, since the consumer would
be able to electrically recharge at any available electrical source, instead of being tethered to a
single home electrolysis unit. Such URFC systems would be dual-fueled vehicles that can use
the existing electrical infrastructure, or a hydrogen infrastructure when available, for rapid
 MITLITSKY ET AL
-2-

refueling. They would enable regenerative braking by electrolysis and power peaking by
oxygen supercharging.

2.1 2.1
2.0 Electrolyzer (EC) at: 2.0
1.9 320ASF(344mA/cm2) 1.9
1.8 240ASF(258mA/cm2) 1.8
1.7 160ASF(172mA/cm2) 1.7
1.6 86ASF (80 mA/cm2) 1.6
1.5 Cell ID LLNL01 1.5
Voltage [V]

1.4 Active Area 0.05 ft2 (46 cm2) 40 psig (0.37 MPa) H2 / H2O 1.4
1.3 Nafion 117, E-5™ (4 mg/cm2/electrode) 50 psig (0.45 MPa) O2 / H2O
Inlet Temp 120 °F (49 °C) 300 sec FC at 100 ASF (108 mA/cm2) 1.3
1.2 Cycle number 2010 measured Feb 1997 300 sec EC at 240 ASF (258 mA/cm2) 1.2
1.1 1.1
1.0 Fuel Cell (FC) at: 1.0
0.9 40ASF (43 mA/cm2) 0.9
0.8 100ASF(108mA/cm2) 0.8
0.7 160ASF(172mA/cm2) 0.7
0.6 220ASF(237mA/cm2) 0.6
0.5 0.5
0.4 0.4
0 500 1000 1500 2000 2500 3000
Cycle Number (600 seconds / cycle)

Figure 1. URFC cycle test at LLNL demonstrated negligible degradation after 2010 cycles.[1]
 MITLITSKY ET AL
-3-

2.3 2.3
2.2 Cathode Feed 2.2
2.1 Electrolysis 2.1
2.0 2.0
1.9 1.9
1.8 1.8
1.7 CELL# 9734A CELL# 9804A 1.7
Active Area 0.05 ft2 (46 cm2) Active Area 0.05 ft2 (46 cm2)
1.6 1.6
Voltage [V]

Nafion 117, E-5™ Catalyst Nafion 105, E-5™ Catalyst

1.5 1.5
4 mg/cm2/electrode 1 mg/cm2/electrode
1.4 78 PSIG H2/H2O (0.64 MPa) 78 PSIG H2/H2O (0.64 MPa) 1.4
1.3 145 PSIG O2/H2O (1.1 MPa) 145 PSIG O2/H2O (1.1 MPa) 1.3
1.2 Inlet Temp 195 °F (91 °C) Inlet Temp 195 °F (91 °C) 1.2
1.1 Internal resist 6.3 mΩ at 24 °C Internal resist 4.0 mΩ at 24 °C 1.1
1.0 Measured May 1997 Measured April 1998 1.0
0.9 0.9
0.8 0.8
0.7 0.7
0.6 0.6
0.5 0.5
0.4 0.4
0 200 400 600 800 1000 1200 1400 1600 1800 2000
2152
Current Density [ASF] mA/cm2

Figure 2. High performance URFCs were demonstrated at LLNL with reduced catalyst loading.
 MITLITSKY ET AL
-4-

Figure 4. LLNL URFC 0.05 ft2 (46 cm 2) cell.

Figure 3. LLNL URFC test rig.

Figure 6. Proton URFC 0.05 ft2 (46 cm 2) cell.

Figure 5. Proton Energy Systems URFC test rig. Figure 7. Proton URFC 0.1 ft2 (93 cm 2) cell.
 MITLITSKY ET AL
-5-

ACKNOWLEDGMENTS

A. Baris and P.J. Regna (Aero Tec Laboratories), C.J. Anderson and O.A. Velev
(AeroVironment), S.P. Worden (Air Force), S.L. Rodgers and D.G. Talley (Air Force Research
Laboratory), B.D. James and I.F. Kuhn, Jr. (Directed Technologies), S. Gronich and N.
Rossmeissl (DOE), J. O’Sullivan (EPRI), R.I. Sims (Ford Motor Corporation), J.F. McElroy
(Hamilton Standard), P.H. Carter II, M.L. Dickerson, M.J. Eckart, and W.A. Jensen (LLNL), J.
Baer-Riedhart (NASA Dryden), L. Moulthrop and W. Smith (Proton Energy Systems, Inc.), E.H.
Stokes (Southern Research Institute), R.P. Golde and R.K. Kunz (Thiokol Corp.). This work was
performed under the auspices of the U.S. DOE by LLNL under contract number W-7405-Eng-48.

REFERENCES

1. F. Mitlitsky, A.H. Weisberg, and B. Myers, “Regenerative fuel cell systems,” Energy &
Fuels, 12 (1), 56-71, January 12 (1998); UCRL-JC-128267 Rev 1;
http://pubs.acs.org/isubscribe/journals/enfuem/jtext.cgi?enfuem/12/i01/html/ef970151w.html .

2. P.H. Carter II, F. Mitlitsky, A.H. Weisberg, J.C. Whitehead, and R.W. Humble, “Design
trade space for a Mars ascent vehicle for a Mars sample return mission,” IAA Conference on
Low-Cost Planetary Missions, Pasadena, CA, April 27-May 1 (1998); UCRL-JC-130277.

3. W.A. de Groot, L.A. Arrington, J.F. McElroy, F. Mitlitsky, A.H. Weisberg, P.H. Carter II, B.
Myers, B.D. Reed, “Electrolysis propulsion for spacecraft applications,” AIAA 97-2948, 33rd
AIAA/ASME/SAE/ASEE Joint Propulsion Conf., July 7-9 (1997).

4. F. Mitlitsky, B. Myers, and A.H. Weisberg, “Lightweight pressure vessels and unitized
regenerative fuel cells,” 1996 Fuel Cell Seminar, November 17-20 (1996); UCRL-JC-
125220 (paper) and UCRL-MI-125220 (viewgraphs).

5. F. Mitlitsky, W.A. deGroot, L. Butler, and J.F. McElroy, “Integrated modular propulsion and
regenerative electro-energy storage system (IMPRESS) for small satellites,” AIAA Small
Satellite Conference, September 16-20 (1996); UCRL-JC-125242.

6. F. Mitlitsky, B. Myers, and F. Magnotta, “Lightweight bladder lined pressure vessels,”

Disclosure and Record of Invention, DOE Case No. IL-9722, 1995; U.S. patent no. 5,798,156,
August 25, 1998.

7. F. Mitlitsky, N.J. Colella, and B. Myers, “Unitized Regenerative Fuel Cells for Solar
Rechargeable Aircraft and Zero Emission Vehicles,” 1994 Fuel Cell Seminar, pp. 624-627,
Nov. 28-Dec. 1, 1994 (UCRL-JC-117130 and UCRL-MI-117130).

8. F. Mitlitsky, N.J. Colella, B. Myers, and C.J. Anderson, “Regenerative Fuel Cells for High
Altitude Long Endurance Solar Powered Aircraft,” Proc. 28th IECEC, Vol. 1,. pp. 1255-1262,
Aug. 8-13, 1993 (UCRL-JC-113485).

9 P.J. Chludzinski, I.F. Danzig, A.P. Fickett, and D.W. Craft, "Regenerative fuel cell
development for satellite secondary power," General Electric Company, Technical Report
AFAPL-TR-73-34, Jun. 1973.

10. F. Mitlitsky and B. Myers, “Development of an advanced, composite, lightweight, high

pressure storage tank for on-board storage of compressed hydrogen,” Fuel Cells for
Transportation TOPTEC: Addressing the Fuel Infrastructure Issue, Alexandria, VA, April 1-
2, 1996 (UCRL-MI-123802).

11. NASA Dryden Press Release 98-64, August 7, 1998;

 MITLITSKY ET AL
-6-

http://www.dfrc.nasa.gov/PAO/PressReleases/1998/98-64.html .