WO2001095414A1 - Molten carbonate fuel cell with immersed metal wire electrodes - Google Patents

Molten carbonate fuel cell with immersed metal wire electrodes Download PDF

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Publication number
WO2001095414A1
WO2001095414A1 PCT/RU2000/000455 RU0000455W WO0195414A1 WO 2001095414 A1 WO2001095414 A1 WO 2001095414A1 RU 0000455 W RU0000455 W RU 0000455W WO 0195414 A1 WO0195414 A1 WO 0195414A1
Authority
WO
WIPO (PCT)
Prior art keywords
gas
fuel cell
anode
cathode
differs
Prior art date
Application number
PCT/RU2000/000455
Other languages
French (fr)
Inventor
Mikhail Rudolfovich Predtechenskiy
Vladimir Yeliferyevich Nakoryakov
Igor Borisovich Kuznetsov
Lev Semyonovich Tchernoy
Andrey Nikolayevich Smal
Nikolay Vasilyevich Gelfond
Original Assignee
Aquarius Technologies Limited
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Aquarius Technologies Limited filed Critical Aquarius Technologies Limited
Priority to AU17446/01A priority Critical patent/AU1744601A/en
Publication of WO2001095414A1 publication Critical patent/WO2001095414A1/en

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Classifications

    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/8605—Porous electrodes
    • H01M4/8626—Porous electrodes characterised by the form
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/8605—Porous electrodes
    • H01M4/8621—Porous electrodes containing only metallic or ceramic material, e.g. made by sintering or sputtering
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/14—Fuel cells with fused electrolytes
    • H01M8/144—Fuel cells with fused electrolytes characterised by the electrolyte material
    • H01M8/145—Fuel cells with fused electrolytes characterised by the electrolyte material comprising carbonates
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/90—Selection of catalytic material
    • H01M4/9016—Oxides, hydroxides or oxygenated metallic salts
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/50—Fuel cells

Definitions

  • the invention relates to fuel cells i.e. devices which transform chemical power to
  • electric power may be used as a source of electric power in any branch of industry, mainly in power engineering, mechanical engineering, and etc.
  • Fuel cells in general include a pair of porous electrodes, cathode and anode, and an ionic conductor, electrolyte, which is the solution of alkali, acid or melt of carbonates
  • fuel cells are classified as fuel cells with liquid electrolyte and solid electrolyte.
  • gaseous reagents come through porous electrodes: through the anode penetrates fuel and through the cathode penetrates the oxidant.
  • oxygen (0 2 ) including oxygen from air is used as an oxidant.
  • the fuel cells are specified with the high efficiency.
  • the closest analogue of the offered invention is a fuel cell as follows: it comprises
  • the cell has a surface adjacent to the melt of carbonates and containing a catalyst for a chemical reaction to occur, oxidation on
  • the electrolyte is made in the form of a plate of porous material.
  • the electrodes (cathode and anode) are tightly adjacent to the opposite surfaces of the plate with electrolyte and also made in the form of porous two-layers plates.
  • the layer of each of electrodes adjacent to the electrolyte has pores of such dimension that the capillary
  • the second layer of the electrode has larger pores and combines with delivery device of oxidative or fuel gas.
  • Working (fuel and oxidative) gases come on the surfaces of the respective electrodes, jointing to the electrolyte surface through the pores of electrodes and on the interface respective chemical reactions of oxidation and reduction occur and as a
  • the main imperfection of the said fuel cell is its high cost due to complicity of
  • the purpose of the invention is to reduce cost of a fuel cell on the account of
  • the solution of the problem is found by offering a fuel cell consisting of molten carbonates at temperature not lower the melting temperature, and cathode and anod each connected to the device supplying the working gas: fuel gas to the anode and oxidizing gas
  • the difference of the fuel cell is that it is provided with a housing chamber in which the molten carbonates are placed and each electrode is made in the form of a shell limiting its
  • the shell is immersed into the molten carbonates and is made of a metal wire or grid to keep the working gas inside the said electrode shells and the molten carbonates outside the shells on the account of the capillary forces. Furthermore, the offered fuel cell differs in the
  • the wire of the electrode shell is made in the shape of a spiral with a gap not exceeding
  • the metal grid of the electrode has a cell dimension of 1-200 micrometers
  • the cathode contains lithium-treated nickel oxide as a catalyst
  • the anode contains nickel or its alloys as a catalyst
  • - methane or natural gas is used as a fuel gas.
  • Fig. 1 outlines the fuel cell
  • fig. 2 outlines one variant of a fuel cell electrode.
  • the fuel cell comprises a housing chamber 1 , filled in with molten carbonates 2 of lithium, natrium or kalium (or mixture of them) and a pair of electrodes 3 and 4 as anode and cathode respectively.
  • Each electrode has a form of a shell 5 limiting the internal space
  • adjacent coils or nickel grid with a cell dimension of 1-200 micrometers.
  • Nickel is a catalyst for anode and during operation of the fuel cell rapid oxidation of the cathode's nickel grid occurs and a catalyst for cathode - lithium-treated nickel oxide is produced.
  • the internal space of the anode 3 is filled in with a fuel gas 6, e.g. hydrogen
  • the internal space of the cathode 4 is filed in with a working gas 8, oxygen or air, and is connected through a gas
  • the electrode shells made in the form of metal wire or grid cause to keep the
  • Pairs of the electrodes 3 and 4 may be placed in one common container filled in
  • the surfaces of the electrodes at least in the part adjoining to the electrolyte is covered with a layer of catalyst or the whole electrode is made of these materials. Since the electrodes operate in chemically corrosive medium the catalyst is required to be not only highly chemically active but highly chemically stable as well.
  • the lithium-treated nickel oxide may be used as a cathode catalyst. Nickel and its
  • alloys may be used as an anode catalyst.
  • each shell 5 of each electrode is made of metal grid with meshes of 1-200 micrometers, or of metal spiral with a gap between coils not exceeding 200 micrometers, each shell should be fully immersed into electrolyte and contain catalyst over all its surface.
  • the electrode shell may be made heterogenous, partially impermeable, partially permeable.
  • FIG. 2 shows the simplest variant of an electrode.
  • the shell 5 of the electrode is
  • the fuel cell can operate at the temperature not lower than the melting temperature for the carbonates.
  • the following reactions runs on the surface of the electrode shells:
  • the offered invention has a simpler structure compared to those earlier
  • electrolyte are no more required.

Landscapes

  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Manufacturing & Machinery (AREA)
  • Sustainable Development (AREA)
  • Sustainable Energy (AREA)
  • Ceramic Engineering (AREA)
  • Inert Electrodes (AREA)
  • Fuel Cell (AREA)

Abstract

The invention can be used in devices transforming chemical power to electric power. The main point of the invention is that a fuel cell comprises molten carbonates at temperatures not lower than the melting temperature placed in a housing chamber, a pair of electrodes - anode and cathode, each of them connected to a working gas supply: anode with a fuel gas and cathode with an oxidizing gas, and a surface adjoining the molten carbonates and containing a catalyst for a chemical reaction to run: oxidation on the anode and reduction on the cathode. Each electrode is made in the form of a shell limiting its internal space and filled in with a working gas, further, at least a part of the electrode shell is immersed into the molten carbonates and made of a metal wire or grid to keep the gas inside the electrode shell and the molten carbonates outside the mentioned shell by means of capillary forces. The metal wire of the electrode shell may be produced winded in the shape of spiral with a gap between adjacent coils not exceeding 200 micrometers, whereas the metal grid of the electrode shell may have a cell dimension of 1-200 micrometers. The lithium treated nickel oxide may be used as a cathode catalyst, nickel and its alloys melts may be used as an anode catalyst. Oxygen or air may be used as an oxidizing gas. Hydrogen or synthes gas or methane or natural gas may be used as a fuel gas. A mixture of lithium carbonate, kalium carbonate and natrium carbonate may be used as molten carbonates.

Description

MOLTEN CARBONATE FUEL CELL WITH IMMERSED METAL WIRE ELECTRODES
The invention relates to fuel cells i.e. devices which transform chemical power to
electric power. It may be used as a source of electric power in any branch of industry, mainly in power engineering, mechanical engineering, and etc.
Fuel cells in general include a pair of porous electrodes, cathode and anode, and an ionic conductor, electrolyte, which is the solution of alkali, acid or melt of carbonates
placed between the electrodes. Depending on the physical state of the electrolyte, the fuel
cells are classified as fuel cells with liquid electrolyte and solid electrolyte. During operation of the fuel cell gaseous reagents come through porous electrodes: through the anode penetrates fuel and through the cathode penetrates the oxidant. Hydrogen (H2) and more
rarely carbon oxide (CO) and methane (CH ) are usually used as a fuel for fuel cells, and
oxygen (02) including oxygen from air is used as an oxidant.
For example, in the oxygen-hydrogen fuel cell with an alkali electrolyte, the electric oxidation of the hydrogen on the anode occurs:
2H2 + 4OH~ → 4H2O +4e
and electric reduction of the oxygen occurs on cathode:
O2 + 2H2O + 4e → 4 0H
At the same time the hydroxide-ions move in the ionic conductor-electrolyte from anode to
cathode. The overall reaction is:
2H2 + O2→2H2O
As a result of the overall reaction the EMF (electromotive force) arises in the
external circuit between the anode and cathode, the direct electric current flows i.e. direct transformation of chemical reaction to the electric power takes place (NN. Koroviπ "Fuel
cells" - Soros's educational magazine, ΝolO, 1998, pgs.55-59). Since the described process of transformation of chemical energy to electric power
does not have any intermediate stage of heat generation, the fuel cells are specified with the high efficiency.
It is well-known, for example, a fuel cell consisting of porous matrix impregnated
with necessary quantity of liquid electrolyte and a pair of electrodes: fuel electrode
(supplying the hydrogen for the cell) and air electrode (supplying oxygen for the cell) which
are located on both sides of the porous matrix (Patent of USA No. 5677073 HOI
M27/00).
The imperfection of this generator is complicated and very expensive manufacture of the fuel cell due to special materials required for the matrix, to the need for special means of permanent control of the quantity of electrolyte decreasing during generator
operation and when being supplied to the matrix, and also the need for special means lor integration of elements in batteries.
The closest analogue of the offered invention is a fuel cell as follows: it comprises
molten carbonates at no less than melting temperature, a pair of electrodes, anode and
cathode, each of them connected with the means supplying them with a working gas, a fuel
gas to the anode and an oxidative gas to the cathode, The cell has a surface adjacent to the melt of carbonates and containing a catalyst for a chemical reaction to occur, oxidation on
the anode and reduction on the cathode (Patent of USA No. 4554225 H 01 M 27/00).
In the said patent the electrolyte is made in the form of a plate of porous material. The electrodes (cathode and anode) are tightly adjacent to the opposite surfaces of the plate with electrolyte and also made in the form of porous two-layers plates. The layer of each of electrodes adjacent to the electrolyte has pores of such dimension that the capillary
interaction with electrolyte takes place. It may be made of fibrous or powdery material. The second layer of the electrode has larger pores and combines with delivery device of oxidative or fuel gas. Working (fuel and oxidative) gases come on the surfaces of the respective electrodes, jointing to the electrolyte surface through the pores of electrodes and on the interface respective chemical reactions of oxidation and reduction occur and as a
result the EMF arises.
The main imperfection of the said fuel cell is its high cost due to complicity of
manufacture of porous elements - the plates for electrolyte and electrodes. Respectively, the unit of power obtained from such source is very expensive.
The purpose of the invention is to reduce cost of a fuel cell on the account of
simplification of its structure as a whole and its separate parts and, as such, reduce cost of
the power unit.
The solution of the problem is found by offering a fuel cell consisting of molten carbonates at temperature not lower the melting temperature, and cathode and anod each connected to the device supplying the working gas: fuel gas to the anode and oxidizing gas
to the cathode, and has a surface adjoining the molten carbonates and contains a catalyst
for a chemical reaction to occur: oxidation on the anode and reduction on the cathode.
The difference of the fuel cell is that it is provided with a housing chamber in which the molten carbonates are placed and each electrode is made in the form of a shell limiting its
internal space filled in with the working gas, furthermore, at least a part of the electrode
shell is immersed into the molten carbonates and is made of a metal wire or grid to keep the working gas inside the said electrode shells and the molten carbonates outside the shells on the account of the capillary forces. Furthermore, the offered fuel cell differs in the
following: - the wire of the electrode shell is made in the shape of a spiral with a gap not exceeding
200 micrometers between adjacent coils,
- the metal grid of the electrode has a cell dimension of 1-200 micrometers,
- the cathode contains lithium-treated nickel oxide as a catalyst,
- the anode contains nickel or its alloys as a catalyst,
- oxygen or air is used as an oxidizing gas,
- hydrogen is used as a fuel gas,
- synthes gas is used as a fuel gas,
- methane or natural gas is used as a fuel gas.
- mixture of lithium, kalium and natrium carbonates is used as a molten carbonate.
Fig. 1 outlines the fuel cell; fig. 2 outlines one variant of a fuel cell electrode.
The fuel cell comprises a housing chamber 1 , filled in with molten carbonates 2 of lithium, natrium or kalium (or mixture of them) and a pair of electrodes 3 and 4 as anode and cathode respectively. Each electrode has a form of a shell 5 limiting the internal space
and is made of either a nickel spiral with a gap not exceeding 200 micrometers between
adjacent coils, or nickel grid with a cell dimension of 1-200 micrometers.
Nickel is a catalyst for anode and during operation of the fuel cell rapid oxidation of the cathode's nickel grid occurs and a catalyst for cathode - lithium-treated nickel oxide is produced. The internal space of the anode 3 is filled in with a fuel gas 6, e.g. hydrogen
and is connected through a gas flue 7 with a device supplying it with hydrogen as a fuel gas
(hydrogen may be replaced by a synthes gas, methane or natural gas). The internal space of the cathode 4 is filed in with a working gas 8, oxygen or air, and is connected through a gas
flue 9 with a device supplying it with oxygen or air. The electrode shells made in the form of metal wire or grid cause to keep the
working gas inside the shell 5 by means of capillary forces and the molten carbonates 2 outside the shells 5.
Pairs of the electrodes 3 and 4 may be placed in one common container filled in
with molten carbonates in rows both along width and length of the container.
In order to intensify the chemical processes running in the fuel cell (oxidation on the
anode and reduction on the cathode), the surfaces of the electrodes at least in the part adjoining to the electrolyte is covered with a layer of catalyst or the whole electrode is made of these materials. Since the electrodes operate in chemically corrosive medium the catalyst is required to be not only highly chemically active but highly chemically stable as well. The lithium-treated nickel oxide may be used as a cathode catalyst. Nickel and its
alloys may be used as an anode catalyst.
If the shell 5 of each electrode is made of metal grid with meshes of 1-200 micrometers, or of metal spiral with a gap between coils not exceeding 200 micrometers, each shell should be fully immersed into electrolyte and contain catalyst over all its surface. The electrode shell may be made heterogenous, partially impermeable, partially permeable.
In this case only the permeable part of the shell provided with the openings shall be
immersed in the electrolyte and contain the respective catalyst.
Figure 2 shows the simplest variant of an electrode. The shell 5 of the electrode is
made of a metal grid on the frame 1 functioning as a case for the grid-like walls 2. The
internal space of electrode is connected through the pipes 3 to the device supplying the
shell with a working gas. The fuel cell can operate at the temperature not lower than the melting temperature for the carbonates. When the cell operates, the following reactions runs on the surface of the electrode shells:
2H2 + 2CO3 2"- 2H2O + 2CO2 + 4e
02 + 2CO2 + 4e → 2 CO3 2"
The chemical reactions mentioned above result in rise of the EMF in the external
circuit (10) between anode and cathode, direct electric current flows, i.e. chemical reaction directly transforms into electric power.
When the fuel cell operates, in the internal space of the electrodes overpressure of the gas is maintained on the level for the working gas to stay inside the shell and for the
electrolyte to stay outside and not to penetrate into the internal space of the electrode.
Furthermore, along the edge of the openings made in the shell of the electrode so called triple boundary is created where the respective catalyst, working gas and liquid electrolyte are together and where the desirable chemical reactions run.
Thus, the offered invention has a simpler structure compared to those earlier
known, much lower cost, since expensive microporous electrodes are substituted with
electrodes made of metal wire or grid and expensive and complicated matrices for
electrolyte are no more required.

Claims

1. Fuel cell comprising molten carbonates at temperature not less than melting temperature, a pair of electrodes - anode and cathode, each of them connected with a device supplying it with the working gas: anode with a fuel gas and cathode with an oxidizing gas, and has the surface adjoining the molten carbonates and
containing a catalyst for chemical reaction to run: oxidation on anode and reduction
on anode, differing from the analogues in that the molten carbonates are placed in a housing chamber, each electrode is made in the form of a shell limiting its internal space filled in with working gas, furthermore, at least a part of the electrode shell is
immersed into the molten carbonates and made of a metal wire or grid to keep the working gas inside the said electrode shells and molten carbonates outside the said
shells by means of capillary forces.
2. A fuel cell according to claim differs in that the electrodes are made of a metal
spiral with a gap not exceeding 200 micrometers between adjacent coils.
3. A fuel cell according to claim differs in that the electrodes are made of a metal grid
with a cell dimension of 1-200 micrometers.
4. A fuel cell according to claim differs in that the cathode contains lithium-treated nickel oxide as a catalyst.
5. A fuel cell according to claim differs in that the anode contains nickel or its alloys as
a catalyst.
6. A fuel cell according to claim differs in that oxygen or air is used as an oxidizing
gas.
7. A fuel cell according to claim differs in that hydrogen is used as a fuel gas.
8. A fuel cell according to claim differs in that synthes gas is used as a fuel gas.
9. A fuel cell according to claim differs in that methane or natural gas is used as a fuel
gas.
10. A fuel cell according to claim differs in that a mixture of lithium, kalium and
natrium carbonates is used as a molten carbonate.
PCT/RU2000/000455 2000-06-08 2000-11-10 Molten carbonate fuel cell with immersed metal wire electrodes WO2001095414A1 (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
AU17446/01A AU1744601A (en) 2000-06-08 2000-11-10 Molten carbonate fuel cell with immersed metal wire electrodes

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
RU2000114497 2000-06-08
RU2000114497 2000-06-08

Publications (1)

Publication Number Publication Date
WO2001095414A1 true WO2001095414A1 (en) 2001-12-13

Family

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WO (1) WO2001095414A1 (en)

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US6586129B2 (en) * 2000-08-06 2003-07-01 Aquarius Technologies Limited Liquid electrolyte fuel cell

Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
FR1459418A (en) * 1964-11-06 1966-04-29 Eindhoven Tech Hogeschool High temperature fuel cell
US4554225A (en) * 1983-03-31 1985-11-19 Tokyo Shibaura Denki Kabushiki Kaisha Molten carbonate fuel cell
DE4302347C1 (en) * 1993-01-28 1994-06-23 Deutsche Aerospace Laminated carbonate melt fuel cell with lithiated nickel oxide cathode
WO1999012220A1 (en) * 1997-09-01 1999-03-11 Rmg Services Pty. Ltd. Improved fuel cell and a process of using a fuel cell

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
FR1459418A (en) * 1964-11-06 1966-04-29 Eindhoven Tech Hogeschool High temperature fuel cell
US4554225A (en) * 1983-03-31 1985-11-19 Tokyo Shibaura Denki Kabushiki Kaisha Molten carbonate fuel cell
DE4302347C1 (en) * 1993-01-28 1994-06-23 Deutsche Aerospace Laminated carbonate melt fuel cell with lithiated nickel oxide cathode
WO1999012220A1 (en) * 1997-09-01 1999-03-11 Rmg Services Pty. Ltd. Improved fuel cell and a process of using a fuel cell

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US6586129B2 (en) * 2000-08-06 2003-07-01 Aquarius Technologies Limited Liquid electrolyte fuel cell

Also Published As

Publication number Publication date
AU1744601A (en) 2001-12-17

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