Interconnector for high temperature fuel cells

Information

  • Patent Grant
  • 6316136
  • Patent Number
    6,316,136
  • Date Filed
    Thursday, February 11, 1999
    25 years ago
  • Date Issued
    Tuesday, November 13, 2001
    22 years ago
  • Inventors
  • Original Assignees
  • Examiners
    • Brouillette; Gabrielle
    • Tsang; Susy
    Agents
    • Townsend and Townsend and Crew LLP
Abstract
The interconnector (1) for high temperature fuel cells is arranged between a first and a second planar electrochemically active element (2, 2′). In this it separates a chamber (41) containing a combustion gas from a chamber (51, 53) containing oxygen. A porous sinter body (10) of the interconnector has pores (101) which are at least partly sealed by a medium (11′). Through the sealing, a passage of gases between the named chambers (41, 51) is prevented.
Description




BACKGROUND OF THE INVENTION




1. Field of the Invention




The invention relates to an interconnector for high temperature fuel cells and to a fuel cell battery.




2. Description of the Prior Art




The fuel cells of a fuel cell battery in accordance with the invention comprise (see EP-A 0 714 147) in each case a so-called PEN and an interconnector which connects the cells adjacent to the PEN in an electrically conducting manner and at the same time separates a combustion gas (in particular a mixture of carbon monoxide and hydrogen) from a gaseous oxygen carrier (in particular air). The PEN has a planar three-layer construction consisting namely of a solid electrolyte (E), a positive electrode (P) and a negative electrode (N). Electrochemical reactions at the PEN with the fuel and the oxygen of the oxygen carrier take place at about 900° C.




Due to the high operating temperatures, a material must be used for the interconnectors of which the coefficient of thermal expansion is largely equal to that of the solid electrolyte. A powder-metallurgically manufactured alloy is known which is suitable for the manufacture of interconnectors. This material, which consists mainly of chromium (about 95% by weight) and which is manufactured through sintering at high pressure and high temperature, is expensive. The alloy is manufactured in plate form and must therefore be further processed in a form suited to the function of the interconnectors, with complicated and expensive work steps being required and material being lost.




SUMMARY OF THE INVENTION




The object of the present invention is to provide an interconnector which permits substantial cost savings.




The interconnector for high temperature fuel cells is arranged between a first and a second planar electrochemically active element, a so-called PEN. In this it separates a chamber containing a combustion gas from a chamber containing oxygen. A porous sinter body of the interconnector has pores which are at least partly sealed by a medium. Through the sealing, a passage of gases between the named chambers is prevented.




The interconnector in accordance with the present invention comprises a sinter body which prevents a mixing of the reactants and which is porous, with its pores being filled with an additional medium for the sealing off. The porosity permits more economical manufacturing methods. Other powder mixtures can also be used, for example those which consist to a large part of ceramic material with a low coefficient of thermal expansion and for which the manufacture of a tight, pore-free solid body would not be possible. In particular the powder mixture can also largely be brought into the form of the finished part though a form compression procedure.




Chromium is an important constituent in known interconnectors because this metal has a low coefficient of thermal expansion and its oxide is electrically conducting. At the operating temperature of the fuel cells, however, a material transport of sublimated chromium oxide takes place via the gas phase to the electrodes, through which their activity is impaired. For this reason it is necessary to coat the surfaces of the interconnector with a material which acts as a chromium oxide barrier (for this, cf. EP-A 0 714 147=P.6651).




For coating layers which act as chromium oxide barriers, ceramic materials (in particular Perovskite) or enamel come into consideration. An enamel, for example with the composition (in percentage by weight): MgO (5-15), Al


2


O


3


(15-30), B


2


O


3


(10-15), SiO


2


(35-55), MnO (15-30), has a softening point of about 1000° C., a coefficient of thermal expansion which coincides approximately with that of the solid electrolyte (about 8 10


−6


K


−1


at 800° C.) and the property of wetting an alloy well which is rich in chromium. This enamel is suitable not only as a chromium oxide barrier but also as a medium by means of which the pores of the sinter body can be sealed.











BRIEF DESCRIPTION OF THE DRAWINGS





FIG. 1

is a radial cross-section through an interconnector in accordance with the invention of a centrally symmetric part,





FIG. 2

is sectionally and in an enlarged view, a cross-section through a porous sinter body,





FIG. 3

is a schematic illustration relating to the gas and air flow in a fuel cell,





FIG. 4

is an interconnector in accordance with the invention illustrated in an oblique view,





FIG. 5

is a cross-section through the interconnector of

FIG. 4

with the two associated PEN's,





FIG. 6

is a detail of the interconnector of FIG.


4


and





FIG. 7

is a further embodiment of the interconnector in accordance with the invention.











DETAILED DESCRIPTION OF THE PREFERRED EXEMPLARY EMBODIMENTS





FIG. 1

shows an interconnector


1


which is assembled from two sinter bodies


10


. The inner sides of the sinter bodies


10


are treated with an enamel, which forms a gas tight boundary zone


11


through closure of the pores. The enamel additionally prevents a transport of chromium oxide.




The outer sides of the sinter bodies


10


have cover layers


12


and


12


′ respectively of a Perovskite which serves as a chromium oxide barrier and which is electrically conducting. The two sinter bodies


10


are connected, on the one hand, via electrically conducting solder films


13


to one another and, on the other hand, via the cover layers


12


,


12


′ to a first PEN


2


and to a second PEN


2


′ so that the interconnector


1


produces an electrical connection between the two PEN's.




Air


50


acting as an oxygen carrier enters via a supply point


5


into a cavity


51


of the interconnector


1


where it takes up heat. The preheated air enters via an outlet opening


52


into a chamber


53


bordering on the PEN


2


. After a giving off of oxygen to the PEN


2


, the air leaves the fuel cell again (arrow


502


).




The fuel cells are substantially centrally symmetric and are arranged in a stack with an axis


3


. Combustion gas


401


is fed in via an axial passage


4


into the cells. In a chamber


41


the outwardly flowing gas


40


is distributed over the surface of the PEN


2


′ and its components are brought to a reaction on the electrode, with water and carbon dioxide arising as an exhaust gas. The exhaust gas


402


leaves the cell at the periphery.




The body


10


shown in

FIG. 2

consists of powder grains


100


which are sintered together and between which pores


101


are filled with a medium


11


′. The powder grains


100


consist for example of metals, in particular of chromium, which together with a further metal, preferably iron, fuses to an alloy during the sintering. Further materials, for example ceramics, can be contained in the powder mixture which produce a favorable effect during the form compression. The powder grains


100


can also be metallically coated particles of ceramic materials.




The air


50


and combustion gas


40


respectively which flow between adjacent PEN's


2


,


2


′ in passages of the interconnector


1


are advantageously guided in passages in spiral or involute shape. The flow guidance in a group of passages


41


,


51


and


53


of this kind is schematically illustrated in FIG.


3


. Fresh, already preheated air


501


is fed in at the periphery of the interconnector


1


via an inlet tube


5


. After flowing through the passage


51


and a further heating up, the air


50


passes upwardly in the middle through the opening


52


and is conducted from there via the passage


53


back to the periphery, where it leaves the cell as exhaust air


502


. Fresh combustion gas


401


is fed in centrally from the axial passage


4


and conducted via the passage to the periphery, where it leaves the cell as exhaust gas


402


.




A particularly advantageous embodiment of the interconnector in accordance with the invention is shown in

FIG. 4

in an oblique view and in

FIG. 5

as a cross-section. The sinter body


10


produces a monolithic connection between electrically conducting contact surfaces


120


and


120


′ of the associated PEN's


2


,


2


′ (see FIG.


5


). A profiled film


15


, which has suitably arranged apertures for combs


16


of the sinter body


10


, forms a partition wall between parallel passages


51


and


53


(cf. FIG.


3


). The film


15


need not be electrically conducting; it can consist of a chromium-free alloy, for example of an alloy which contains aluminium and silicon and in which the developing oxide layers consist of aluminium or silicon oxide (electrically non conducting). A film


15


of an alloy of this kind need not be coated with a chromium oxide barrier.





FIG. 5

shows the three-layer construction of the PEN


2


: at the gas side an anode


2




a


, at the air side a cathode


2




c


and in between a solid electrolyte


2




b


which is permeable to oxygen ions at the operating temperature. The comb-like elevations


16


leave gaps free through which air


50


′ can flow in the radial direction from one passage


53


to the adjacent passage


53


′. Comb-like elevations


14


are likewise provided at the gas side which enable a radial flow


40


′ of the combustion gas


40


.




The pores of the sinter body


10


are at least partly sealed. The sealing is advantageously produced by an enamel which is applied from the air side (for example through the spraying on of a water suspension of enamel particles, then drying and melting of the enamel, with the melt penetrating into the pores as a result of capillary forces). As shown in

FIG. 6

a boundary region


101


on the air side can be sealed with enamel, whereas the pores of the remaining part


10


″ of the sinter body


10


remain open. The enamel on the air side also prevents a liberation of chromium oxide.




In comparison with the film


15


the sinter body


10


is designed with thick walls. The thermal expansion of the interconnector is thereby practically determined by the properties of the sinter body


10


alone. Therefore the film


15


can have a coefficient of thermal expansion which differs from that of the electrolyte


2




b


. In this respect there is a similarity to the interconnectors which are known from EP-A 0 749 171.





FIG. 7

shows an embodiment of the interconnector


1


in accordance with the invention which is assembled in two layers from a sinter body


10


and a profiled film


15


′. An example of the film


151


is disclosed in the European application No. 96810723.5 (=P.6766). Examples of film material include metallic felt or metallic felt parts, which consist of, for example nickel-based alloys that contain chromium and that form volatile chromium oxides in an oxidizing environment. Additionally, an electrically conductive ceramic foam structure may be used, for example. This film


15


′ must be electrically conducting in contrast to the film


15


of the above described exemplary embodiment. Therefore alloys containing chromium are to be used, which makes covering layers necessary due to the chromium oxide.




The sinter body has a porosity in the range between about 5 and 35%. The porosity preferably amounts to about 20 to 30%.



Claims
  • 1. An interconnector for high temperature fuel cells that is arranged between a first and second planar electrochemically active element, a first chamber containing a combustion gas, and a second chamber containing oxygen that is separate from the first chamber, and a porous sinter body including pores, wherein the pores are at least partly sealed by a medium in such a manner that a passage of gases between the first and second chamber is prevented, wherein the interconnector comprises the porous sinter body, and wherein the porous sinter body is between the first and second chamber.
  • 2. The interconnector in accordance with claim 1, wherein the sinter body is manufactured from a powder mixture, and wherein the powder mixture is brought substantially into the form of a finished part through compression during the manufacturing process.
  • 3. The interconnector in accordance with claim 1, wherein the sinter body is a part of a heat exchanger for a gaseous oxygen carrier, wherein, together with a second element, at least one passage for the oxygen carrier is formed between a supply point and an outlet opening, and wherein the oxygen carrier is supplied to the first electrochemically active element at the outlet opening, wherein the second element is a film.
  • 4. The interconnector in accordance with claim 1 wherein the sinter body produces a monolithic connection between electrically conducting contact surfaces of the associated first and second electrochemically active element.
  • 5. The interconnector in accordance with claim 1 wherein the sinter body includes chromium, wherein sinter body surfaces that come into contact with oxygen have a coating that acts as a barrier against giving off chromium oxide into the chamber containing oxygen, and wherein the coating is at least partly formed by the pore sealing medium.
  • 6. The interconnector in accordance with claim 5, wherein parts of a surface of the sinter body which are in contact with the first and second planar electrochemically active element are coated with a material that is electrically conducting and that forms a chromium oxide barrier.
  • 7. The interconnector in accordance with claim 1, wherein the sinter body has a porosity in a range between approximately 5 and 35%.
  • 8. The interconnector in accordance with claim 7, wherein the porosity is about 20-30%.
  • 9. A fuel cell battery comprising a stack of fuel cells with interconnectors, wherein each interconnector is arranged between a first and a second planar electrochemically active element, each interconnector including a first chamber containing a combustion gas and a second chamber containing oxygen that is separate from the first chamber, and a porous sinter body including pores, wherein the pores are at least partly sealed by a medium in such a manner that a passage of gases between the first and second chamber is prevented, wherein the fuel cells are substantially centrally symmetric, wherein the combustion gas is fed by a distributor along a stack axis, and wherein at a periphery of the stack there are arranged inlet points for an oxygen carrier and outlet points for the combustion gas and the oxygen carrier after passage through the fuel cells.
  • 10. The fuel cell battery in accordance with claim 9, wherein a structure forming components of the interconnectors are each assembled from a sinter body and a profiled sheet metal film.
Priority Claims (1)
Number Date Country Kind
98810125 Feb 1998 EP
US Referenced Citations (3)
Number Name Date Kind
5064734 Nazmy Nov 1991
5270131 Diethelm Dec 1993
5691075 Batawi Nov 1997
Foreign Referenced Citations (9)
Number Date Country
410159 A Jun 1990 EP
410166 A Jul 1990 EP
0410159A1 Jan 1991 EP
0410166A1 Jan 1991 EP
0424732A1 May 1991 EP
0714147A1 May 1996 EP
8287929 Nov 1996 JP
WO 9628855 Sep 1996 WO
WO 9735349 Sep 1997 WO
Non-Patent Literature Citations (4)
Entry
Chemical Abstracts, vol. 126, No. 6, Feb. 10, 1997, Columbus, Ohio, US; abstract No. 77495, Fujimoto, Tetsuo Et Al: “Planar ceramic interconnectors for solid electolyte fuel cells and their manufacture”, XP002071911, Abstract, & JP 08 287 929 A (Mitsubishi Heavy Ind) Nov. 1, 1996.
Patent Astracts of Japan, vol. 97, No. 3, Mar. 31, 1997 & JP 08 287929 A (Mitsubishi Heavy Ind), Nov. 1, 1996, Abstract.
Patent Abstracts of Japan, vol. 096, No. 011, Nov. 29, 1996 & JP 08 185870 A (Tonen Corp; Sekiyu Sangyo Kasseika Center) Jul. 16, 1996, Abstract.
Patent Abstracts of Japan, vol. 096, No. 011, Nov. 29, 1996 & JP 08 171924 A (Tonen Corp; Sekiyu Sangyo Kasseika Center), Jul. 2, 1996, Abstract.