Chemistry: electrical current producing apparatus – product – and – With pressure equalizing means for liquid immersion operation
Reexamination Certificate
2001-05-15
2003-09-23
Gulakowski, Randy (Department: 1716)
Chemistry: electrical current producing apparatus, product, and
With pressure equalizing means for liquid immersion operation
C429S006000, C429S006000
Reexamination Certificate
active
06623881
ABSTRACT:
BACKGROUND OF THE INVENTION
The present invention relates to an apparatus, such as a solid electrolyte fuel cell, incorporating compliant electrode/electrolyte structures that include opposing electrodes disposed on and electrically interconnected through a compliant electrolyte sheet, and a method of making such structures and apparatus.
The use of solid electrolyte materials for fuel cells and oxygen pumps has been the subject of a considerable amount of research for many years. The typical essential components of a solid oxide fuel cell (“SOFC”) include a dense, oxygen-ion-conducting electrolyte sandwiched between porous, conducting metal, cermet, or ceramic electrodes. Electrical current is generated in such cells by the oxidation, at the anode, of a fuel material, such as hydrogen, which reacts with oxygen ions conducted through the electrolyte from the cathode.
Practical power generation units will typically include multiple fuel cells of such configuration interconnected in series or parallel with electronically conductive ceramic, cermet, or metal interconnect materials. At the present time, the materials of choice for such devices include yttria-(Y
2
O
3
) stabilized zirconia (ZrO
2
) for the electrolyte, nickel-ZrO
2
cermet for the anode material, strontium-doped lanthanum manganite (LaMnO
3
) for the cathode, and metals, especially Cr/Fe alloys and Ni alloys, intermetallics, and Sr or Ba doped LaCrO
3
, for interconnect structures. Alternative oxygen ion conductors are known. At sufficient temperatures (e.g., 600° C. or above), zirconia electrolytes can exhibit good ionic conductivity but low electronic conductivity.
Several different designs for solid oxide fuel cells have been developed, including, for example, a supported tubular design, a segmented cell-in-series design, a monolithic design, and a flat plate design. All of these designs are documented in the literature, with one recent description in Minh, “High-Temperature Fuel Cells Part 2: The Solid Oxide Cell,”
Chemtech
., 21:120-126 (1991).
The tubular design comprises a closed-end porous zirconia tube exteriorly coated with electrode and electrolyte layers. The performance of this design is somewhat limited by the need to diffuse the oxidant through the porous tube. Westinghouse has numerous U.S. patents describing fuel cell elements that have a porous zirconia or lanthanum strontium manganite cathode support tube with a zirconia electrolyte membrane and a lanthanum chromate interconnect traversing the thickness of the zirconia electrolyte. The anode is coated onto the electrolyte to form a working fuel cell tri-layer, containing an electrolyte membrane, on top of an integral porous cathode support or porous cathode, on a porous zirconia support. Segmented designs proposed since the early 1960s (Minh et al.,
Science and Technology of Ceramic Fuel Cells
, Elsevier, p. 255 (1995)), consist of cells arranged in a thin banded structure on a support, or as self-supporting structures as in the bell-and-spigot design.
A number of planar designs have been described which make use of free-standing electrolyte membranes. A cell is formed by applying single electrodes to each side of an electrolyte sheet to provide an electrode-electrolyte-electrode laminate. Typically these single cells are then stacked and connected in series to build voltage. Monolithic designs, which characteristically have a multi-celled or “honeycomb” type of structure, offer the advantages of high cell density and high oxygen conductivity. The cells are defined by combinations of corrugated sheets and flat sheets incorporating the various electrode, conductive interconnect, and electrolyte layers, with typical cell spacings of 1-2 mm for gas delivery channels.
U.S. Pat. No. 5,273,837 to Aitken et al. covers sintered electrolyte compositions in thin sheet form for thermal shock resistant fuel cells. It describes an improved method for making a compliant electrolyte structure wherein a precursor sheet, containing powdered ceramic and binder, is pre-sintered to provide a thin flexible sintered polycrystalline electrolyte sheet. Additional components of the fuel cell circuit are bonded onto that pre-sintered sheet including metal, ceramic, or cermet current conductors bonded directly to the sheet as also described in U.S. Pat. No. 5,089,455 to Ketcham et al. U.S. Pat. No. 5,273,837 to Aitken et al. shows a design where the cathodes and anodes of adjacent sheets of electrolyte face each other and where the cells are not connected with a thick interconnect/separator in the hot zone of the fuel cell manifold. These thin flexible sintered electrolyte-containing devices are superior due to the low ohmic loss through the thin electrolyte as well as to their flexibility and robustness in the sintered state.
Another approach to the construction of an electrochemical cell is disclosed in U.S. Pat. No. 5,190,834 Kendall. The electrode-electrolyte assembly in that patent comprises electrodes disposed on a composite electrolyte membrane formed of parallel striations or stripes of interconnect materials bonded to parallel bands of electrolyte material. Interconnects of lanthanum cobaltate or lanthanum chromite bonded to a yttria stabilized electrolyte are suggested. Unfortunately, the electrolyte/interconnect junctions in this design are sufficiently weak that a usefully compliant electrode/electrolyte structure cannot be obtained.
The internal circuit of the fuel cell circuit consists of the electrolyte, electrodes, and current conductors. The performance of a fuel cell, i.e., the current carrying capacity and hence the overall efficiency of the cell, is limited by its internal resistance, the maximum power for any power supply being given by P
max
=V
2
/4R
internal
. Internal resistance is the sum of several components including the electrode ohmic resistance, the electrolyte resistance, the electrode/electrolyte interfacial resistance to charge transfer reaction, and the current conductor resistance. The interfacial resistance to charge transfer depends mainly on the electrochemical behavior and physical and chemical nature of the electrode.
Precious or “noble” metals such as gold, silver, platinum, palladium, rhodium etc. have been suggested as candidates for electrode materials in high temperature fuel cells, silver and its alloys, including silver-palladium, being amongst the best electrical conductors known. One disadvantage of silver as an electrode material, however, is its high volatility at temperatures over about 800° C. Fuel cell operation at temperatures in the neighborhood of 700° C. would significantly reduce metal volatilization, and should also allow the use of relatively inexpensive stainless steel components for the fabrication of manifold and other mechanical elements of the cells. Also, the volatility of precious metal electrode materials such as silver can be further reduced by introducing them in admixture with refractory ceramic fillers as cermet electrodes. Silver/yttria-doped zirconia cermet cathodes, for example, are advantageous due to high electronic conductivity and good catalytic properties, and can be made economically in thin film form by continuous magnetron sputtering.
The present invention is directed to providing an improved fuel cell construction, applicable to any of a variety of planar fuel cell designs, which avoids many of the difficulties of fuel cell manufacture while providing a cell of improved physical, thermal, and electrical properties.
SUMMARY OF THE INVENTION
In an important aspect, the present invention is based on a thin, compliant electrode/electrolyte structure for a solid oxide fuel cell that offers improved cell design flexibility while retaining high strength, mechanical integrity, and resistance to thermal degradation from temperature cycling and thermal shock. The electrode/electrolyte structure of the invention comprises a thin flexible solid oxide electrolyte sheet incorporating a plurality of positive air and negative fuel electrodes bonded to opposing sides of the sheet. Thus the elect
Badding Michael E.
Brown Jacqueline L.
Ketcham Thomas D.
St. Julien Dell J.
Wusirika Raja R.
Corning Incorporated
Gulakowski Randy
Scaltrito Donald V.
Sterre Kees van der
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