EP1502320A2 - Convertisseur chimio-electrique, systeme de convertisseur chimio-electrique, procede de production d'energie electrique et procede pour faire fonctionner un systeme de convertisseur chimio-electrique - Google Patents

Convertisseur chimio-electrique, systeme de convertisseur chimio-electrique, procede de production d'energie electrique et procede pour faire fonctionner un systeme de convertisseur chimio-electrique

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Publication number
EP1502320A2
EP1502320A2 EP03747083A EP03747083A EP1502320A2 EP 1502320 A2 EP1502320 A2 EP 1502320A2 EP 03747083 A EP03747083 A EP 03747083A EP 03747083 A EP03747083 A EP 03747083A EP 1502320 A2 EP1502320 A2 EP 1502320A2
Authority
EP
European Patent Office
Prior art keywords
chemoelectric
chemoelectric converter
electrodes
converter system
proton
Prior art date
Legal status (The legal status 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 status listed.)
Withdrawn
Application number
EP03747083A
Other languages
German (de)
English (en)
Inventor
Reinhart Radebold
Irmgard Radebold
Walter Radebold
Helmut Radebold
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Individual
Original Assignee
Individual
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
Priority claimed from DE10219585A external-priority patent/DE10219585C1/de
Application filed by Individual filed Critical Individual
Publication of EP1502320A2 publication Critical patent/EP1502320A2/fr
Withdrawn legal-status Critical Current

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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
    • H01M4/88—Processes of manufacture
    • H01M4/8878—Treatment steps after deposition of the catalytic active composition or after shaping of the electrode being free-standing body
    • H01M4/8882—Heat treatment, e.g. drying, baking
    • H01M4/8885—Sintering or firing
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B60—VEHICLES IN GENERAL
    • B60L—PROPULSION OF ELECTRICALLY-PROPELLED VEHICLES; SUPPLYING ELECTRIC POWER FOR AUXILIARY EQUIPMENT OF ELECTRICALLY-PROPELLED VEHICLES; ELECTRODYNAMIC BRAKE SYSTEMS FOR VEHICLES IN GENERAL; MAGNETIC SUSPENSION OR LEVITATION FOR VEHICLES; MONITORING OPERATING VARIABLES OF ELECTRICALLY-PROPELLED VEHICLES; ELECTRIC SAFETY DEVICES FOR ELECTRICALLY-PROPELLED VEHICLES
    • B60L50/00—Electric propulsion with power supplied within the vehicle
    • B60L50/50—Electric propulsion with power supplied within the vehicle using propulsion power supplied by batteries or fuel cells
    • B60L50/51—Electric propulsion with power supplied within the vehicle using propulsion power supplied by batteries or fuel cells characterised by AC-motors
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B60—VEHICLES IN GENERAL
    • B60L—PROPULSION OF ELECTRICALLY-PROPELLED VEHICLES; SUPPLYING ELECTRIC POWER FOR AUXILIARY EQUIPMENT OF ELECTRICALLY-PROPELLED VEHICLES; ELECTRODYNAMIC BRAKE SYSTEMS FOR VEHICLES IN GENERAL; MAGNETIC SUSPENSION OR LEVITATION FOR VEHICLES; MONITORING OPERATING VARIABLES OF ELECTRICALLY-PROPELLED VEHICLES; ELECTRIC SAFETY DEVICES FOR ELECTRICALLY-PROPELLED VEHICLES
    • B60L50/00—Electric propulsion with power supplied within the vehicle
    • B60L50/50—Electric propulsion with power supplied within the vehicle using propulsion power supplied by batteries or fuel cells
    • B60L50/60—Electric propulsion with power supplied within the vehicle using propulsion power supplied by batteries or fuel cells using power supplied by batteries
    • B60L50/64—Constructional details of batteries specially adapted for electric vehicles
    • 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
    • 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
    • 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
    • H01M8/20—Indirect fuel cells, e.g. fuel cells with redox couple being irreversible
    • 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
    • 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
    • Y02T—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO TRANSPORTATION
    • Y02T10/00—Road transport of goods or passengers
    • Y02T10/60—Other road transportation technologies with climate change mitigation effect
    • Y02T10/70—Energy storage systems for electromobility, e.g. batteries

Definitions

  • Chemoelectric converter Chemoelectric converter, che oelectric converter system
  • the present invention relates to chemoelectric converters according to the preamble of claim 1, chemoelectric converter systems according to the preamble of claims 29 and 55, a method for generating electrical energy according to the preamble of claim 60 and methods for operating a chemoelectric converter system according to the preamble of the claims 63 and 64.
  • an electrical double layer has built up, consisting of the negative electrons and the protons remaining in the protonic conductor 3 (electrolytes) because they are much larger.
  • Such a double layer can be very high as a charged capacitor Capacity to be understood.
  • a chemoelectric converter consists of two electrodes, with oxygen (mostly) in the form of 0 2 being transported to the second electrode.
  • 0 2 is used here as an acceptor for two e " and two H + , provided that two electrons succeed in leaving the electronic (here mostly made of graphite) conductor 2 of this electrode and again using a quantum mechanical tunneling process to the 0 2
  • an electrical double layer with an electrical field and corresponding potential has formed, consisting of the two remaining positive electron holes 2h + and the chemically reduced oxygen as negative ion (0 2 ) 2 " .
  • protons and oxygen ions are located in the same protonic conductor 3, but separated from one another by a membrane 4.
  • the membrane 4 prevents the hydrogen that has been transported from accidentally reacting chemically with the oxygen that is being transported in a parasitic reaction with the uncontrolled release of considerable energy.
  • the task of the chemoelectric converter is to control the chemical reaction between hydrogen and oxygen in such a way that the energy released can largely be used in the form of electrical energy. That happens in 1 at the moment when the two electronic conductors are connected to one another via an electrical consumer, which is shown in FIG.
  • the two double layers have now dissolved as a result of the chemical reaction, and with them the two electrical fields have disappeared, not without having previously performed electrical work on the intermediate consumer.
  • the sum of the two individual potentials corresponds to the voltage at the consumer between the two electrodes.
  • the resulting short current pulses can be joined together to form a quasi-continuous (direct) current if the two starting materials hydrogen and oxygen are continuously transported accordingly.
  • Chemoelectric converters that work close to the ambient temperature have different technical structures and different properties, depending on the chemical form (and therefore also the physical state) in which the hydrogen is supplied.
  • Air-breathing alkaline and PEM (Proton Exchange Membrane) fuel cells which are operated with gaseous, molecular hydrogen H 2 as a hydrogen transfer agent and with gaseous, molecular oxygen 0 2 .
  • PEM Proton Exchange Membrane
  • the first problem is solved by hydrophobizing the gas-permeable electronic conductors.
  • the activation of H 2 as a second problem is optimally achieved by attachment to an electrode provided with Pt, which serves as a catalyst.
  • Pt which serves as a catalyst.
  • a porous membrane predominantly separates the two electrolyte spaces 3 serving as proton conductors, or a combination of proton conductors 3 and membrane 4 in the form of a polymeric membrane is omitted into the quasi-microscopic, acidic, water-containing channels, without alkaline electrolyte spaces are installed for proton conduction.
  • chemoelectric converters that work with a liquid hydrogen transfer agent, such as, for example, aqueous solutions of hydrazine N 2 H 4 , methanol CH 3 OH or glucose C 6 H 2 0 6 , and which take their oxygen requirement from the atmosphere.
  • these converters directly use hydrogen in the form of 2H, which is logistically packed with N 2 or C0 2 .
  • the electrodes have three layers and, according to FIG. 1, consist of an electronic conductor 2, a protonic conductor 3 and an interface 1 for building up the double layer; both electrodes are separated by a membrane 4.
  • the negative electrode is constructed much more simply and without the use of noble metal, since on the one hand a gaseous phase with the problems associated therewith does not occur, and on the other hand activation of the hydrogen via a catalyst is not necessary.
  • the costly and operationally complex PEM is no longer necessary and is replaced by a membrane that is compatible with the aqueous solutions.
  • the known method does not work with the 2H from the glucose and the 0 from the H 2 0 2 as donor and acceptor on the negative and the positive electrode, but rather the actual secondary donor D and the two additional reaction centers RZD2 and RZA2 actual secondary acceptor A formed in the electrolyte.
  • the secondary donors and secondary acceptors are two fluid redox systems that, after having released or taken up their electrons and protons upon contact with one of the electrodes, can be regenerated chemically via 2H or O at RZD2 and RZA2.
  • the electrodes on which the double layers are built up are graphite particles, which are suspended in the electrolyte and are components of a fluidized bed reactor, each with two fixed collecting electrodes. Theoretically, this method can achieve potential differences well above 1.2 V.
  • the method according to DE 195 19 123 C2 is based on biochemical principles of energy conversion in living cells.
  • the aim is to utilize the great potential of the radiation from the sun stored in the renewable raw materials through photosynthesis in a novel chemoelectric converter into electrical energy.
  • From DE 196 48 691 AI an improvement of the above-mentioned method is known, in particular through a qualitative and quantitative thermodynamic analysis of photosynthesis and breathing. (A block diagram with an exergy-anergy flow diagram of photosynthesis and respiration was published in VDI Report No. 1594 (2001), pages 345 to 354 as Fig. 1 by the applicant).
  • the reaction sequences of breathing in a living cell serve as a model for a process for converting the free reaction enthalpy stored in hydrogen-containing substances and oxygen into the energy of an electrodynamic field for / application in macroscopic and microscopic technical systems.
  • electrical energy from chemoelectric conversion is stored microscopically on molecules, macroscopically stored in synthetically produced structures with the function of a rechargeable battery. For example, alternating and three-phase currents of higher voltage can be obtained if the battery molecules discharge at a multiplicity of mutually insulated parallel electrodes, and the electrodes are then connected in series.
  • the state-of-the-art chemoelectric converters with liquid hydrogen transfer and gaseous or liquid oxygen transfer are constructed as macro systems. Macro systems, regardless of whether they are loaded with gaseous or fluid products, must be sealed against their surroundings. They are therefore always equipped with pressure-resistant seals to the environment between the membrane, metallic conductors and electrical rolyte with the dissolved redox partners contained therein, as well as with pipes and pumps for conveying the fluid products and products, with devices for the elimination of the C0 2 or N 2 as gaseous products as well as for the removal of the inevitable electrical and chemical Losses as heat with a relatively small temperature difference to the environment.
  • chemoelectric converter to be used in a decentralized manner using structures and with elements from macroscopic process engineering therefore has considerable weak points.
  • the weak points can hardly be mastered reliably even with the use of additional stabilizing structures such as pressure plates, which are clamped with bolts in order to apply large forces, since the forces easily cause deformations of seals and flanges, for example, of deformation of channels and electrodes with the risk of Cause blockages and leaks.
  • Macro systems are cumbersome to use; in the event of malfunctions, they have to be completely emptied and largely dismantled in order to reach defective areas.
  • Relatively high pressures are required internally in order to generate turbulent flows in the channels, necessary to obtain very thin boundary layers on the electrodes.
  • the fluid dynamic boundary layers in which the speed drops practically to zero and the liquid adheres, are, however, many orders of magnitude thicker: The exchange of starting materials and products with the electrodes essentially only comes about through diffusion, hardly through convection conditions .
  • a chemoelectric converter with electrodes from a liquid hydrogen transmitter, in particular aqueous solution of glucose, and oxygen as starting materials can couple electrical energy either via reaction centers and secondary donors or via reaction centers and secondary acceptors.
  • two porous, electron and proton-conducting solid bodies are provided as electrodes, the reaction centers and the secondary acceptors in the volume of the first solid body and the volume of the second solid body the reaction centers and the secondary donors are in the form of solid compounds and the first and second solids are in contact, separated by a proton-conducting membrane.
  • the control of the water content in the porous solids of the electrodes is essential.
  • microcapillarity macroscopic, capillary-active separate conduction paths with the function of wicks are therefore provided, both for the distribution of liquid starting materials and for the targeted removal of excess liquid.
  • the electrodes are also used to store electrical energy.
  • energy can be stored by the secondary acceptors and secondary donors, since, like a battery, they can initially take up or release electrons without the need for an external supply of starting materials.
  • metal-oxide compounds for example MnO 2 , in particular alkaline Fe (VI) oxide
  • MnO 2 in particular alkaline Fe (VI) oxide
  • organic compounds in particular C-hinone or flavine
  • inorganic cerium compounds as reaction centers for the secondary acceptor.
  • organic Compounds or metals especially bismuth, lead or iron, but also metal oxides such as Fe (II).
  • the electrodes of different signs designed as solid bodies do not have to work at the same pH values.
  • the positive electrode with its acceptors can work in the neutral or weakly acidic range
  • the negative electrode with its donors in the strongly basic range. This does not change the fact that protons ultimately have to flow from the boundary layer of the negative to the boundary layer of the positive electrode.
  • a protonic hole line can also be involved.
  • the secondary donors and / or the secondary acceptors can be regenerated chemically after their use via the reaction centers and / or by feeding in electrical energy. This makes it possible to electrically charge the chemoelectric converter, which can also serve as a memory.
  • reaction centers and / or the secondary donors and / or the secondary acceptors are advantageous to integrate in a gel-like matrix. Different materials and substances can be integrated flexibly. A binder which is elastic in the hardened state can also advantageously be used.
  • the solid bodies of the chemoelectric converter serving as electrodes and memory in a cuboid shape.
  • at least one of the solid bodies is electrically conductive Contact contacted.
  • the electrically conductive contact as a metallic grid that advantageously contacts the solid body on exactly one of its side surfaces.
  • nickel, carbon and / or another organic compound is applied to the metallic grid.
  • a chemically inert graphite foil which is used, for example, perforated or punched as a grid for contacting.
  • a spray device is provided with which educts and / or water can be sprayed onto the solid body. It is advantageous to use an aqueous solution of hydrazine N 2 H 4 / methanol CH 3 0H or glucose C 6 H 2 0 6 as the product, in particular as a hydrogen transfer agent. This ensures efficient transport of hydrogen carriers. Because macroscopic, capillary-active conduction paths are provided in the electrodes for the further transport and distribution of the liquid educts, the liquid educts can also be directly injected at a few excellent points on these conduction paths.
  • a chemoelectric converter system can couple electrical energy out of a liquid hydrogen transmitter, in particular an aqueous solution of glucose, and oxygen as starting materials via reaction centers and secondary donors and / or reaction centers and secondary acceptors.
  • a chemoelectric converter system can couple electrical energy out of a liquid hydrogen transmitter, in particular an aqueous solution of glucose, and oxygen as starting materials via reaction centers and secondary donors and / or reaction centers and secondary acceptors.
  • the electrodes of which are designed as porous, electrons and proton-conducting solids being in contact with one another via a proton-conducting layer and the proton-conducting membrane is arranged between the proton-conducting layer and the solids.
  • the proton-conducting layer is flat, the at least two electrodes, which can also serve as a memory, being in contact with the same side of the surface of the proton-conducting layer. It is advantageous to arrange the electrodes next to one another on the proton-conducting layer in such a way that they do not touch.
  • the proton-conducting membrane can advantageously also be arranged between the electrodes.
  • the electrodes are preferably arranged on the proton-conducting layer in such a way that two electrodes with different doping are always adjacent to one another. In this way, a scalable system can be produced from positive and negative electrodes, with the protons being transported via the proton-conducting layer.
  • the spray device is advantageously movable, in particular also rotatable. orderly.
  • the spraying device is designed as a solid matrix which can spray educts onto the electrodes at the desired locations.
  • a constant transport of starting materials and thus constant energy decoupling can be ensured via the spray device.
  • Water can serve as a phase transition agent for the removal of heat of reaction.
  • the control of the water content in the electrodes is essential, for which purpose separate capillary-active conduction paths are provided. This applies regardless of whether the liquid educts are supplied via a spray device or a direct injection.
  • the proton-conducting layer additionally has either reaction centers and secondary acceptors or reaction centers and secondary donors which serve for the intermediate storage of electrical energy. It is advantageous to contact the proton-conducting layer on its side facing away from the electrodes via electrically conductive contacts.
  • the proton-conducting layer can thus be operated as an energy store, in principle a battery that can be regenerated from the outside by the chemoelectric converter and / or by feeding in energy.
  • the proton-conducting layer and the electrodes in contact with it are arranged on a flat or curved circuit board.
  • Means for controlling the electrochemical conversion and / or means for decoupling the electrical power and / or means for feeding in electrical energy are advantageously provided on the circuit board.
  • a push-pull flux converter for decoupling electrical power is included on the circuit board arranged. It is advantageous not to perform the parallel connection of the electrodes galvanically but inductively.
  • a transformer operating at high frequency contains one primary winding per pair of electrodes, with the associated switching transistors in the circuit thus formed.
  • the means for controlling the electrochemical conversion and / or means for decoupling the electrical power and / or means for feeding in electrical energy in particular also a push-pull flux converter, at least partially between the layers the board are arranged.
  • proton-conducting layers and electrodes are attached on both sides of the circuit board, so that the additional means for controlling the electrochemical conversion and / or means for decoupling the electrical power and / or means for feeding in electrical energy are located between them ,
  • modules can be produced which have both a converter area and the means necessary for controlling this converter area, in particular control electronics and means for decoupling electrical power.
  • a space-saving "sandwich" module is created by equipping the board with electrodes on both sides.
  • the additional means for controlling the electrochemical conversion and / or means for decoupling the electrical power and / or means for feeding electrical energy from the "sandwich” and moved to one end of the module the proton-conducting layers are combined or else on reduced a single proton-conducting membrane.
  • the individual electrodes of the same sign are combined on one side of the module. If the proton-conducting layers are omitted, their existing redox systems must be integrated into the positive electrode; the oxygen-breathing electrodes are covered with a layer of the known hydrophobic carbon mats.
  • the chemoelectric converter system can be scaled modularly by using several boards, whereby all the necessary means for controlling and coupling and decoupling energy are already on the boards.
  • the modules can be interconnected in different arrangements. It is advantageous to connect the chemoelectric converters, in particular the circuit boards, to one another via a plurality of electrical leads. In this way, a scaled system can be produced that is suitable for high performance.
  • an ultrasound source is provided with which at least parts of the chemoelectric converter system can be set into high-frequency mechanical vibrations. It is also advantageous to provide a container with which at least a part of the chemoelectric converter system, in particular the porous solids and / or circuit boards with chemoelectric converters, can be closed in a pressure-tight manner with respect to the environment. It is advantageous if an atmosphere of oxygen, nitrogen, water vapor and CO 2 can be maintained in the container in a steady state. The pressure in the container is advantageously periodic and / or too fixed. times can be changed, the container is advantageously coolable. Through these advantageous configurations, the throughput of starting materials, products and water through the porous solid body can be increased, as a result of which the coupling output can be increased.
  • a method for generating electrical energy with chemoelectric converters with which electrical energy can be coupled out from a liquid hydrogen carrier, in particular aqueous solution of glucose, and oxygen as starting materials via reaction centers and secondary donors and / or reaction centers and secondary acceptors.
  • the starting materials according to the invention are applied to at least one electrode which is designed as a porous, electron and proton-conducting solid and in the volume of which the reaction centers and the secondary acceptors or the reaction centers and the secondary donors are present as solid compounds.
  • the products are transported capillary into the porous solid.
  • the starting materials are thus transported without additional technical aids.
  • chemo-electrical converter system described above is advantageously operated in one of the following four operating states:
  • chemoelectric converter system It is also advantageous to operate a chemoelectric converter system described above in such a way that the low voltage generated by the chemoelectric converter system is transformed up with a push-pull flux converter to technically usual voltages, in particular 110V, 220V or 380V.
  • the voltage is preferably converted into two-phase or multi-phase alternating currents of adjustable frequency. In this way, technically usable voltages and currents can be achieved from the low voltage supplied by the chemoelectric converters.
  • the present invention is based on the idea that the previous coupling of microscopic processes with macroscopic Pick up technology as much as possible. It goes without saying that today's modern technologies (nanotechnology) only begin to penetrate into the nm range, their range of action should begin above 100 nm.
  • the present invention builds on this technology, for example on disordered microporous, capillary-active structures, on microdrops and their conveying systems, on condensation and evaporation on microroughness, on macroscopic wick-like conductor tracks for liquids.
  • the disordered, ordered microporous structures for example in that electronically and protonically conductive, permeable microscopic capsules, for example in the range of 10 ⁇ m, enclose the redox systems and reaction centers and in that the capsules are lined up to form quasi-crystalline structures.
  • the present invention thus integrates the components, redox systems and conductors for protons required for the chemoelectric conversion, storage and coupling-out of the electrical energy, and, as far as possible, dispenses with macroscopic hydrodynamic and hydraulic structures.
  • the present invention thus leaves methods and arrangements for chemoelectric conversion as described in the prior art, in which reaction centers and donors and acceptors are dissolved in the aqueous electrolyte, with excess water being present.
  • the invention is based on the use of reaction centers RZD1, RZD2, RZAl and RZA2 as well as of secondary donors D and acceptors A as shown in FIG. 2, but in contrast to the patent specification mentioned, it describes methods and arrangements,
  • the invention provides new degrees of freedom for chemo-electrical conversion. Only now that seals, hydrodynamic and also stabilizing structures and devices with their pressures and forces are no longer necessary, does a modular structure of the converter system, as in microelectronics, appear possible with its great advantages in production, operation and also accidents. In the case of a modular chemoelectric converter system, in principle any output power required by the customer can be achieved simply by adding modules that are plugged onto a common busbar and thus electrically connected in parallel.
  • reaction centers RZD2 and RZA2 are introduced as solid substances in microporous structures or in gel-like matrices, and which after use can be regenerated both chemically via the reaction centers RZD2 and RZA2, but also directly electrically.
  • a metal such as bismuth or lead can advantageously be used as the donor, since, for example, its oxides can be reduced by glucose via reaction centers RZD1 and RZD2, but also metal oxides, for example based on Fe (II), which change in value, for example Fe (III) function can also be reduced by glucose via the reaction centers RZD1 and RZD2.
  • metal oxides for example based on Fe (II), which change in value, for example Fe (III) function can also be reduced by glucose via the reaction centers RZD1 and RZD2.
  • secondary acceptor A compounds may, for example, such as Mn0 2 are used on the basis of metal oxides, then alkaline Fe can (III) oxide on H 2 0 2 to Fe0 2 ", an Fe (VI) oxide, as oxidize very effective acceptor.
  • Organic compounds such as quinones have already been mentioned as the RZAl reaction center; here, for example, in addition to flavins and other organic compounds, inorganic cerium compounds which bind molecular oxygen as a complex and reduce it to H 2 0 2 are also suitable.
  • FIG. 1 shows a schematic representation of a chemoelectric converter according to the prior art
  • FIG. 2 shows a schematic representation of a method for generating electrical energy from renewable biomass according to the prior art
  • FIG. 3 shows a schematic exploded view of a chemoelectric converter system according to the invention
  • Figure 4 a schematic, not to scale sectional view by a microporous, disordered solid of a chemoelectric converter according to the invention
  • FIG. 4b shows a schematic, not to scale, sectional view through a microporous, ordered solid of a chemoelectric converter according to the invention
  • FIG. 5 shows a schematic exploded view of a chemoelectric converter system according to the invention in a second embodiment
  • FIG. 6 shows a schematic exploded view of a chemoelectric converter system according to the invention in a third embodiment
  • FIG. 7 shows a schematic circuit diagram of a push-pull flux converter
  • FIG. 8 shows a schematic sectional illustration of a further, cost-effective “economy version” of a module of the chemoelectric converter system according to the invention.
  • FIG. 9 shows a schematic illustration of an inductive coupling of a plurality of electrode pairs via a high-frequency transformer.
  • FIG. 3 shows a schematic exploded drawing of the invention which is not to scale, based on the chemoelectric part of a chemoelectric converter system.
  • the individual electrodes of the chemoelectric converter system are designed as strip-like, porous and capillary-acting solid bodies 7, 8.
  • the electrodes also act as storage for electrical energy.
  • the solids 7, 8 are on the one hand, by integrating reaction centers and secondary donors present as solid connections into the porous structure as a negative electrode storage structure 7 and, on the other hand, by integrating reaction centers and secondary acceptors in the porous structure as a positive electrode storage structure 8.
  • Grid 9 alternately connected to negative and positive electron-conducting power lines 10 of a two-strand power bus 11, that is to say connected in parallel overall.
  • each pair of the electrode storage structures 7 and 8 is inductively coupled to one another via a secondary winding via switching transistors and a separate, separate primary winding of the high-frequency transformer.
  • Such a coupling is shown for example in FIG. 9.
  • the proton-conducting membrane 6 can also be arranged in the joint between the two electrode storage structures 7, 8 or contain the material of the proton-conducting membrane 6.
  • the parting line can also be filled with an isolator.
  • the proton-conducting layer 5 and the membrane 6 are assigned to all of the electrode storage structures 7, 8 together.
  • electrode storage structures 7, 8 as strips, as shown here, is expedient but not mandatory. In principle, any geometrical shapes and arrangements can gene, such as circles or in the form of a chessboard.
  • the electrode storage structures 7, 8 are formed by porous, capillary-active, electronically and protonically conductive solid bodies, in which the protective, supporting and current collecting grid 9, advantageously with a prepared surface, is integrated or placed.
  • the respective solid 7, 8 contains either reaction centers RZD1 and RZD2 or RZAl and RZA2 according to FIG. 2 and the description of the prior art therein, including the redox system of the secondary donors D or secondary acceptors A, but not now in dissolved, fluid the form, but as fixed connections.
  • the inner interfaces to build up the potential-determining double layers are very large. Since the porous solid-state structure, for example by adding graphite or carbon black, is also electron-conductive because an electron-conducting matrix is formed, the secondary donors D integrated into the porous solid-state structure can accept electrons via the protection, support and current collecting grid 9 give off the power bus 11 and the secondary acceptors A receive electrons via the power bus 11. In the embodiment shown in FIG. 9, the galvanic coupling is replaced by an inductive coupling.
  • a heat transfer takes place between the electrodes 7, 8 with one another and with the proton-conducting layer 5, in which the resulting thermal energies can be exchanged with one another.
  • the structure internally transfers heat at the temperature of the structure (anergy).
  • anergy is released, roughly the same level as the removal of 24H from glucose. This ensures a constant flow of heat between see the electrodes instead.
  • FIG. 4a is a schematic sectional view, not to scale, of one of the microporous, disordered, capillary-active solid bodies which form the electrode storage structures. It shows the electron-conducting matrix formed from the particles 22 and the particles 23 of the corresponding proton-conducting matrix arranged offset therefrom. Furthermore, the complexes 24, to which the reaction centers RZD1, RZD2 and donors D are combined in the case of a negative electrode storage structure and the reaction centers RZAl, RZA2 and acceptors A in the case of a positive electrode storage structure. The complexes 24 are present as solid connections in the porous solid. The complexes 24 can also be present in a gel-like matrix.
  • the interfaces 21 required to build up the double layers arise between the particles 22 of the electron-conducting matrix and the complexes 24.
  • the spaces between the different particles 22, 23 and the complexes 24 form the microscopic capillary system.
  • the capillary-active macroscopic conductor tracks are omitted.
  • FIG. 4b is a schematic sectional illustration, not to scale, of a microporous, ordered, capillary-active solid in a further embodiment, which are used as electrode storage structures. It shows electronically and protonically conductive, permeable microscopic capsules in which the reaction centers RZD1, RZD2 and donors D in the case of a negative storage structure 7 or reaction centers RZAl, RZA2 and acceptors A in the case of a positive electrode storage structure 8 are enclosed.
  • the complexes 24 are present as fixed connections.
  • the capsules are more or less made of electron-conducting, much smaller ones too spherical particles 22, for example formed from carbon, which surround the more or less spherical complex 24 in a thin, crystalline layer.
  • the proton conductor 23 is located in the cavities between these particles. These capsules can be arranged in ordered layers and are in electronic contact. The gussets between the capsules form the microscopic capillary system. As in FIG. 4a, the macroscopic, capillary-active conductor tracks are not shown.
  • the proton-conducting layer 5 is understood as a common "protonic mass", the corresponding protons migrate through this layer from the negative electrode storage structure 7 to the two adjacent positive electrode storage structures 8. The narrower the electrode storage structures, the shorter their path 7, 8 are designed. In contrast to conventional fuel cells, the common proton-conducting layer 5 makes it possible to supply the positive and negative chemoelectric converters 7, 8 together with starting materials from one side (and not, as previously, from two sides).
  • the liquid hydrogen carrier is sprayed onto the negative electrode storage structures 7 via a spray device in the form of a printer system with a printer head 13, nozzles and delivery systems, as is known in terms of the dimensions and function of inkjet printers.
  • the oxygen from the surrounding atmosphere has access to the positive electrical the memory structure 8.
  • a printhead bar not shown here, to be moved or a permanently installed printhead matrix can be used as the spraying device.
  • each printer head 13 has at least one second nozzle and conveying system, with which it can spray water as a reaction partner and means for heat transport onto the electrode storage structures 7, 8.
  • This second nozzle and delivery system is programmed in such a way that aqueous solutions of glucose or hydrazine and the additional water, if necessary, spray onto the corresponding electrode storage structure 7, 8 or parts thereof, leaving out the joints between the solids 7, 8.
  • the microdroplets 12 are picked up by the capillary-active electrode storage structures 7, 8 and distributed within them by the acting capillary forces.
  • the reservoirs, from which the printer head 13 is supplied via flexible supply lines, as well as its mechanics and its control bus, are not shown in the drawing.
  • this water which is initially in liquid form within the porous, capillary-active electrode storage structures 7, 8, is evaporated by the sum of the losses of the chemoelectric conversion in the form of heat at the temperature of the electrode storage structure 7, 8. preferably on quasi-crystalline areas or microroughness, which act as a seed for evaporation. If there is an excess of liquid that cannot escape through evaporation, the macroscopic, capillary-active conductor tracks come into operation for removal. An almost isothermal removal of the heat loss from the microporous electrode storage structure 7, 8 into the atmosphere surrounding it is possible, the heat loss from the surrounding atmosphere being subsequently removed again by condensation of the water vapor on appropriately cooled surfaces.
  • the electrode storage structures 7, 8 are converted into high-frequency by an ultrasound transmitter (not shown here) mechanical vibrations offset.
  • the concept of the printer head 13 is fully used when a liquid oxygen carrier such as H 2 O 2 , diluted with water, is sprayed on via a third nozzle and conveyor system in the printer head 13. Oxygen diffusion is eliminated, current density and voltage increase dramatically. If the entire system is still to be air-breathing, it is necessary to outsource the reduction of 0 2 via the RZAl to a type of lung, i.e. to decouple the functions of RZAl and RZA2 spatially and temporally. High power density is achieved with increased effort.
  • the electrode storage structure 8 changes only insignificantly, if at all.
  • the electrical regeneration of the used donors D and acceptors A can be achieved as an alternative to the chemical regeneration described so far in the variants of the invention described here directly via externally supplied electrical energy. consequences.
  • the electrical energy is coupled into the electronically conductive matrix of the electrode storage structures 7, 8 via the power bus 11 with its power lines 10, via the protective, support and current collecting grids 9.
  • the electrical regeneration of the redox systems means charging the internal storage.
  • a protonic current of equal size must flow internally.
  • the chemoelectric conversion system has the property of being able to charge its memory not only externally via electrical energy but also internally by supplying chemical energy.
  • the converter system therefore knows four operating states:
  • FIG. 5 shows a further variant of the invention, based on the chemoelectric part of the converter system, with direct air breathing, expanded oxygen diffusion and with a greatly enlarged memory.
  • the air-breathing, positive electrode storage structure 8 in FIG. 3 is traced back to an exclusively air-breathing electrode structure 14, which has now been increased in volume and thus correspondingly in surface area.
  • the formerly associated storage structure with its secondary acceptors A is shifted into the common proton-conducting layer 5 according to FIG 3, so that a new proton line electrode storage structure 15 has arisen.
  • this third structure is connected via power lines to the now three-strand power bus 16. tet.
  • the entire chemoelectric converter system is modular.
  • operating state 1 steady state
  • the electrical energy is released by electrode structures 7 and 14, while in operating states 2 and 3 the electrode structures 7 and 15 are activated via the power bus 16.
  • the regenerating electrode memory structures operate via the electrode structures 7 and 14, while other electrode memory structures to be regenerated are connected to the power bus 16 via their electrode memory structures 7 and 15, so that electrical energy is transferred internally.
  • modules can be operated simultaneously, which can be coupled in parallel or in series via an electrical busbar, depending on the requirements.
  • a module in operating state 4 emits electrical energy in order to regenerate the redox systems of a second module, this requires the transfer of electrical energy via a busbar common to all modules, at the level of the power bus 16 each Module adjusting chemoelectric potential difference.
  • each chemoelectric module can deliver electrical energy to a common busbar as a two-, three- or multi-phase current with adjustable frequency and with technically usual voltage
  • a cross-module internal regeneration of the redox systems requires the use of two common rails, a direct current rail with low voltage and high currents and an alternating or rotary Busbar with voltages of, for example, 380 V require, which means a considerable technical effort.
  • the preference is given to a non-cross-module operating state 4 for which a low-voltage direct current rail is unnecessary.
  • FIG. 6 shows an example of a complete, internally regenerable module of a chemoelectric conversion system, consisting of the chemoelectric part, here in the form of the variant according to FIG. 5, together with its periphery, constructed as a multilayer board and from its printer system.
  • the exploded view shows the different layers and layers of the module.
  • the upper layers are used for chemoelectric conversion, here sprayed by a single printer head 13, as shown in a simplified manner by way of example.
  • the lower layers contain the periphery, consisting of power electronics 18 and a microelectronic control system 19 together with data and energy bus 20.
  • the multilayer circuit board 17 forms the support structure of the module in terms of construction.
  • the circuit board is composed of non-conductive foreign layers 17.1 to 17.4, the individual strands of the power bus 16 being located in the three intermediate layers. These are, insulated from one another and lying close to one another, in the form of electron-conducting plates 16.1 to 16.3 with very low internal resistance, each connected to the chemoelectrically active structures via the leads 10.
  • the bus 20 also reaches the sensors via intermediate layers.
  • the microelectronic control system with 19 with its bus 20 for data transfer and for supplying actuators and sensors with energy has the task of detecting the state of the individual components of the module with regard to the reactions and processes taking place, and the printer system in its various embodiments as an actuator to control depending on the chemoelectric conversion and its operating states.
  • each module is connected via plug connectors and via a bus, not shown here, to a higher-level computer, not shown here, which is responsible for the control of the entire chemoelectric converter system.
  • the power electronics 18 consist of a known push-pull flux converter, the diagram of which is shown in FIG. 7, i.e. of semiconductor switches such as transistors, of a transformer with two windings on each side and of a capacitance and of diodes on the output side.
  • This arrangement is operated at frequencies from approximately 50 kHz, which reduces the dimensions of the transformer to such an extent that it can be inserted into the module.
  • the transformer is connected directly to the plates 16.1 to 16.3 of the power bus 16, for example via vias and partially integrated, not only to save space, especially to reduce the leakage inductances.
  • only the double-layer capacitance of the chemoelectric structures is used as the capacitance of the push-pull flux converter on the low-voltage side.
  • the current coming from the collecting plates, broken down into high-frequency pulses via the semiconductor switches and brought to technically customary voltages via the transformer is then, according to the invention, adjustable in two-phase or multi-phase alternating currents from approximately 400 Hz to below implemented a few Hz, for example to operate three-phase motors for vehicle drives via the chemoelectric converter system or to supply a fixed network with 50 Hz, 60 Hz or 400 Hz.
  • Each module of the converter system has corresponding plug connections for connection to busbars, not shown here.
  • the push-pull flux converter extended by appropriate circuits and components and thereby modified, is used in operating state 3 in the opposite direction, namely for feeding braking energy in the form of frequency-variable three-phase currents when using the modular chemoelectric Converter system, for example in vehicles.
  • the storage of the chemoelectric converter system is charged by internal regeneration of the redox systems, advantageously in each module of the variant according to FIG. 6 independently of the other modules, the push-pull flux converter blocking the module.
  • the regeneration within the module is controlled via the control of the printer head, in that it supplies only part of the chemoelectric structures and the structures that are not supplied are charged accumulatively.
  • FIG. 8 shows a schematic illustration of a further, cost-effective “economy version” of a module of the chemoelectric converter system according to the invention in a schematic sectional view.
  • This module basically consists of two parts, a first part of the chemoelectric conversion shown in the drawing in the upper area and a second part, which is arranged in the lower area in the drawing and which comprises the entire microelectronic components and the power electronics 18, 19.
  • the chemoelectric part of the module is enclosed by two printed circuit boards 29 which are rigidly connected to one another via spacers 28.
  • the structure is as shown in FIG
  • the electrode storage structures 7 and 8 face each other and are only electronically isolated from one another by the proton-conducting membrane 6.
  • the positive electrode 8 is covered with one of the known hydrophobized carbon mats 25.
  • the contacting 9 takes place through a graphite foil or another derivative into which channels 27 for conducting air or air with an enriched 0 2 component are stamped or molded.
  • the negative electrode storage structure 7 is also provided with a graphite foil 9 or another derivative.
  • the drainage channels 26 are introduced, which continue through the board 29, necessary to spray or inject the liquid hydrogen carrier.
  • the electrode storage structures can be pressed against the leads 9 and the membrane 6 and against one another, so that the contacts are secured. Incidentally, it is achieved that oxygen does not come into contact with the donors.
  • the pressure build-up required for enriching the air with 0 2 in an external, known pressure change machine for N 2 removal via special coal preparations is used to advantage in the modules described.
  • the entirety of the modules is represented by a enclosed container, so that the aforementioned, controlled atmosphere can build up inside.
  • Nitrogen, water vapor and C0 2 are in a steady state, whereby oxygen can be added depending on the arrangement.
  • a periodic or temporary change in the pressure of the inner atmosphere is advisable.
  • the mean value of the pressure of the internal atmosphere differs only slightly from the pressure of the surrounding atmosphere.
  • the container contains the bushings required for the operation of the modular chemoelectric converter system for the transfer of liquids and gases, electrical energy and data as well as surfaces cooled from outside for heat transfer to the outside through internal condensation.
  • Figure 9 shows schematically the principle of inductive power coupling.
  • a pair of electrodes 7, 8 are short-circuited via an inductor 30 and the circuit thus created is switched at high frequency by a transistor 31, in particular a MOSFET.
  • the high frequency can be in the range of 50-70 kHz, for example.
  • the intermediate inductor 30 simultaneously forms a primary winding of a high-frequency transformer, the inductors 30 of a plurality of electrode pairs 7, 8 thus forming the entire primary winding of the high-frequency transformer.
  • the coupling of the individual electrode pairs 7, 8 takes place via the magnetic flux of the transformer core, which is transformed into high-voltage pulses in the secondary winding 32 of the high-frequency transformer.
  • chemoelectric converter which can couple electrical energy from a liquid hydrogen carrier, in particular an aqueous solution of glucose, and oxygen as starting materials either via reaction centers and secondary donors or via reaction centers and secondary acceptors, at least one porous, electron and proton conductive solid is provided, in the volume of which either the reaction centers and the secondary acceptors or the reaction centers and the secondary donors are present as solid compounds.

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Abstract

L'invention concerne un convertisseur chimio-électrique pourvu d'électrodes qui peut, à partir d'une substance hydrogénante liquide, en particulier une solution aqueuse de glucose, et d'hydrogène en tant qu'éduits, soit par l'intermédiaire de centres de réaction et de donneurs secondaires, soit par l'intermédiaire de centres de réaction et d'accepteurs secondaires, émettre de l'énergie électrique. Comme électrodes, on utilise deux corps solides (7, 8) poreux qui conduisent les électrons et les protons. Dans le volume du second corps solide (8), les centres de réaction (RZD1, RZD2) et les donneurs secondaires (D) se présentent sous la forme de composés solides (24), et les premier et second corps solides (7, 8) sont en contact tout en étant séparés par une membrane (6) conduisant les protons.
EP03747083A 2002-04-26 2003-04-25 Convertisseur chimio-electrique, systeme de convertisseur chimio-electrique, procede de production d'energie electrique et procede pour faire fonctionner un systeme de convertisseur chimio-electrique Withdrawn EP1502320A2 (fr)

Applications Claiming Priority (3)

Application Number Priority Date Filing Date Title
DE10219585 2002-04-26
DE10219585A DE10219585C1 (de) 2003-04-25 2002-04-26 Chemoelektrischer Wandler, chemoelektrisches Wandlersystem, Verfahren zur Erzeugung elektrischer Energie und Verfahren zum Betrieb eines chemoelektrischen Wandlersystems
PCT/DE2003/001387 WO2003092086A2 (fr) 2002-04-26 2003-04-25 Convertisseur chimio-electrique, systeme de convertisseur chimio-electrique, procede de production d'energie electrique et procede pour faire fonctionner un systeme de convertisseur chimio-electrique

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EP1502320A2 true EP1502320A2 (fr) 2005-02-02

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EP03747083A Withdrawn EP1502320A2 (fr) 2002-04-26 2003-04-25 Convertisseur chimio-electrique, systeme de convertisseur chimio-electrique, procede de production d'energie electrique et procede pour faire fonctionner un systeme de convertisseur chimio-electrique

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DE2055675A1 (en) * 1970-11-12 1972-05-18 Battelle Institut E V Electrodes for fuel cells - using hydrogen peroxide as oxidant contain quinoid cpd and non-catalytic conductor
US4578323A (en) * 1983-10-21 1986-03-25 Corning Glass Works Fuel cell using quinones to oxidize hydroxylic compounds
SE9304203L (sv) * 1993-12-20 1994-11-21 Ragnar Larsson Förfarande för produktion av elektrisk energi i en biobränsledriven bränslecell
DE19519123C2 (de) * 1994-05-17 1997-02-06 Reinhart Dr Radebold Verfahren zur Erzeugung elektrischer Energie aus nachwachsender Biomasse
WO1997017828A2 (fr) * 1995-11-17 1997-05-22 Radebold, Walter Procede de transformation de l'enthalpie de reaction libre accumulee dans des matieres contenant de l'hydrogene et dans de l'oxygene en l'energie d'un champ electrodynamique
DE19821980A1 (de) * 1997-05-17 1999-02-11 Radebold Reinhart Verfahren und Vorrichtung zur Auskopplung von Energie aus chemoelektrischen Systemen

Non-Patent Citations (1)

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Title
See references of WO03092086A2 *

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