CN115275242A - Device for continuously providing fuel for direct carbon solid oxide fuel cell - Google Patents
Device for continuously providing fuel for direct carbon solid oxide fuel cell Download PDFInfo
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- CN115275242A CN115275242A CN202210991342.9A CN202210991342A CN115275242A CN 115275242 A CN115275242 A CN 115275242A CN 202210991342 A CN202210991342 A CN 202210991342A CN 115275242 A CN115275242 A CN 115275242A
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- 239000003245 coal Substances 0.000 claims description 4
- 238000000926 separation method Methods 0.000 claims description 4
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- 229910052593 corundum Inorganic materials 0.000 claims description 3
- HBAGRTDVSXKKDO-UHFFFAOYSA-N dioxido(dioxo)manganese lanthanum(3+) Chemical compound [La+3].[La+3].[O-][Mn]([O-])(=O)=O.[O-][Mn]([O-])(=O)=O.[O-][Mn]([O-])(=O)=O HBAGRTDVSXKKDO-UHFFFAOYSA-N 0.000 claims description 3
- 229910000314 transition metal oxide Inorganic materials 0.000 claims description 3
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- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims description 2
- 229910052783 alkali metal Inorganic materials 0.000 claims description 2
- 150000001340 alkali metals Chemical class 0.000 claims description 2
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- 229910002076 stabilized zirconia Inorganic materials 0.000 claims description 2
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- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 2
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- 238000010248 power generation Methods 0.000 description 2
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- 229920000742 Cotton Polymers 0.000 description 1
- MYMOFIZGZYHOMD-UHFFFAOYSA-N Dioxygen Chemical compound O=O MYMOFIZGZYHOMD-UHFFFAOYSA-N 0.000 description 1
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- 230000001590 oxidative effect Effects 0.000 description 1
- NDLPOXTZKUMGOV-UHFFFAOYSA-N oxo(oxoferriooxy)iron hydrate Chemical compound O.O=[Fe]O[Fe]=O NDLPOXTZKUMGOV-UHFFFAOYSA-N 0.000 description 1
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- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
Images
Classifications
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- 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
- H01M8/02—Details
-
- 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
- H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
- H01M8/04082—Arrangements for control of reactant parameters, e.g. pressure or concentration
- H01M8/04089—Arrangements for control of reactant parameters, e.g. pressure or concentration of gaseous reactants
-
- 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
- H01M8/06—Combination of fuel cells with means for production of reactants or for treatment of residues
- H01M8/0606—Combination of fuel cells with means for production of reactants or for treatment of residues with means for production of gaseous reactants
-
- 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
- H01M8/10—Fuel cells with solid electrolytes
- H01M8/1016—Fuel cells with solid electrolytes characterised by the electrolyte material
-
- 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
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- Life Sciences & Earth Sciences (AREA)
- Engineering & Computer Science (AREA)
- Manufacturing & Machinery (AREA)
- Sustainable Development (AREA)
- Sustainable Energy (AREA)
- Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Fuel Cell (AREA)
Abstract
The invention relates to a device for continuously supplying fuel for a direct carbon solid oxide fuel cell. The device includes a channel, a fuel cell, a fuel tank, a solid fuel, and a barrier layer. The structure is as follows: a plurality of fuel tanks filled with solid fuel are arranged in the channel, and the fuel tanks are separated from each other by using isolating layers. The middle part of the channel is positioned in a working temperature area of the fuel cell, the inlet end and the outlet end of the channel are positioned in a normal temperature area, and a temperature-gradient heat preservation area is arranged between the working temperature area and the normal temperature area. When the battery is operated, the chemical energy of the carbon is converted into electric energy. When the fuel in the fuel tank is consumed to an extent that is insufficient to maintain the normal operation of the fuel cell, a new fuel tank filled with fuel is loaded at the inlet end of the channel, and the fuel tank is pushed toward the outlet end, so that the fuel tank filled with fuel, which is next to the fuel cell in the direction of the inlet end of the channel, is located right below the fuel cell, and the fuel tank with the consumed fuel is pushed toward the outlet end, and is gradually cooled.
Description
Technical Field
The invention relates to a solid oxide fuel cell technology, in particular to a direct carbon solid oxide fuel cell technology, and specifically relates to a method for continuously providing fuel for a direct carbon solid oxide fuel cell.
Background
Solid Oxide Fuel Cells (SOFC) are composed of a dense layer of electrolyte and porous electrodes on either side of the electrolyte, and a continuous electrical output is obtained by supplying fuel to the anode and oxidant (typically air or oxygen) to the cathode in succession. Among various fuel cells, SOFC has outstanding advantages of high efficiency, all-solid structure, wide range of fuel usage, and the like. SOFCs can use not only gaseous fuels (hydrogen, water gas, natural gas, etc.) but also solid carbon fuels directly. SOFCs that use solid carbon fuel directly are also known as direct carbon solid oxide fuel cells (DC-SOFCs). The thermodynamic basis on which a DC-SOFC can operate is: the thermodynamic equilibrium product of excess carbon and oxygen at high temperatures is mainly CO, which can be used directly as fuel for SOFCs. When the DC-SOFC is started, gas purging is not generally needed for carbon fuel arranged on an anode, so that air remained in an anode chamber before starting is increased along with the temperature of the cell to start reaction with carbon, and when the temperature is increased to the working temperature (generally 800 ℃), CO generated in the anode chamber is generated, so that the cell has the operation condition. The specific working principle of the DC-SOFC is as follows: oxygen gas obtains electrons from an external circuit at the cathode and is reduced into oxygen ions
1/2O 2 +2e - ＝O 2- (1)
The oxygen ions reach the anode through the electrolyte (the electrolyte is an oxygen ion conductor), and are subjected to electrochemical oxidation reaction with CO in the anode chamber to generate CO 2 And supply electrons to external circuits
O 2- +CO＝CO 2 +2e - (2)
CO produced 2 Diffuse to carbon fuel and generate reverse Boudouard reaction to generate more CO
CO 2 +C＝2CO (3)
The generated CO diffuses to the anode, and the reaction (2) is maintained. In summary, DC-SOFCs consume carbon fuel and generate electricity externally by coupling reactions (2) and (3) to each other.
The DC-SOFC can directly convert the chemical energy of carbon into electric energy, the theoretical efficiency can reach 100 percent, and the tail gas is high-concentration CO 2 The method is beneficial to the capture and the sealing utilization of carbon, and is a potential technology for realizing efficient clean power generation by utilizing carbon-rich fuels such as coal, biomass and the like.
Conventional SOFCs that use gaseous fuels provide a continuous supply of fuel to the cell by the internal pressure of the fuel gas container (e.g., cylinder). However, the DC-SOFC using solid carbon fuel cannot provide carbon fuel continuously as gas is provided, and therefore, the current DC-SOFC disposes carbon fuel in the anode chamber at one time. The capacity of the anode chamber limits the amount of carbon fuel to be contained at one time, so that the operation time of the cell is limited, and the cell needs to stop working, cool to room temperature and reload the fuel after the contained fuel is consumed, which severely limits the application of the DC-SOFC and causes efficiency loss. In fact, the continuous fuel supply problem of DC-SOFC has been one of the important factors limiting the development of this new power generation technology to practical applications.
Disclosure of Invention
The invention aims to solve the problem of continuous fuel supply of the DC-SOFC, provides a method for continuously supplying fuel, and particularly relates to a device for continuously supplying carbon-rich solid fuel to the DC-SOFC.
The purpose of the invention is realized by the following technical scheme:
an apparatus for continuously supplying fuel to a direct carbon solid oxide fuel cell includes a channel, a fuel cell, a fuel tank, a solid fuel, and a barrier layer. The channel is a pipe gallery structure with openings at two ends, is made of high-temperature-resistant and oxidation-resistant materials (quartz, ceramics and the like), and is characterized in that at least one plane is provided, a cell window is arranged in the middle of the plane and used for packaging a fuel cell, and the size of the window is matched with the size of the fuel cell to be installed. The channel is a gallery structure capable of accommodating a plurality of fuel slots simultaneously along its length; the channel is provided with at least one plane, and a cell window is arranged in the middle of the plane and used for mounting the fuel cell. The fuel tank is provided with a groove structure for containing solid fuel, the cross section shape of the fuel tank is similar to that of the channel, the size of the fuel tank is slightly smaller, and the fuel tank can freely slide in the channel; the solid fuel is carbon-rich solid fuel; the isolation layer is positioned between adjacent fuel tanks; the isolation layer is made of high-temperature-resistant flexible materials and is characterized by heat preservation and adjustable air permeability; the device for continuously providing the solid fuel is characterized in that a plurality of fuel tanks filled with the solid fuel are arranged along the length direction of a channel, the openings of the fuel tanks are parallel to a plane of the channel filled with the fuel cells, and the opening of one fuel tank is opposite to the anode of the fuel cell; each fuel groove is separated by an isolating layer, and each fuel groove is directly contacted with the adjacent isolating layer; when the fuel cell is in operation, the fuel cell in the middle of the channel is in a cell working temperature zone, the inlet end and the outlet end of the channel are in a normal temperature zone, and a heat preservation zone with the temperature gradually reduced from the working temperature zone to the normal temperature zone is arranged between the working temperature zone and the normal temperature zone; the fuel cell operates in a working temperature zone, consumes the solid fuel in the fuel tank opposite to the fuel cell and generates electricity; after the fuel is consumed, adding a new fuel tank filled with fuel from the inlet end of the channel, and applying a thrust force to the outlet end from the inlet end to push all the fuel tanks in the channel to the outlet end until the fuel tank filled with fuel adjacent to the fuel cell is opposite to the anode of the fuel cell, so that the cell continues to operate; the continuous supply of the solid fuel is realized by the repeated operation, the direct carbon solid oxide fuel cell can continuously run, and the fuel tank to be consumed by the fuel is pushed to the outlet end, removed, emptied, filled with the fuel and recycled.
The fuel cell is a three-layer structure consisting of a dense electrolyte, a porous anode and a cathode on two sides of the dense electrolyte, and is sealed on the cell window of the channel, and the anode of the fuel cell faces the inside of the channel; the fuel cell is a planar SOFC, which is composed of a porous anode, a dense electrolyte and a porous cathode, the edge of the planar SOFC is connected to the edge of a channel window, the cell is sealed at the channel window by a high temperature sealing material (e.g., sealing glass), and the anode of the sealed cell faces the inner side of the channel. The fuel tank is a container for containing carbon-rich solid fuel and is characterized in that the cross section of the fuel tank is similar to the cross section of the channel, and the cross section size of the fuel tank is slightly smaller than the cross section of the channel so as to freely slide in the channel; the opening of the fuel tank is parallel to the plane with the battery window in the channel and is also made of high-temperature resistant and oxidation resistant materials; the fuel tank has a length that is much less than the length of the channel so that multiple fuel tanks can be placed in the channel at the same time. The isolating layer is made of high-temperature-resistant flexible materials, the high-temperature-resistant flexible materials can be ceramic wool, ceramic felt and the like, the shape and the size of the isolating layer are matched with the cross section of the channel, the isolating layer can be made by pressing and cutting the high-temperature-resistant flexible materials, and the thickness of the isolating layer is based on the fact that the cross section of the channel can be automatically blocked in the channel.
The continuous fuel supply device is assembled by simultaneously placing a plurality of fuel tanks filled with solid fuel in a channel in which the fuel cells are installed, wherein an opening of one fuel tank faces an anode of the fuel cell. The fuel tanks are separated by isolating layers and are closely arranged. When the device is operated, the channel is in three temperature zones, the fuel cell in the middle part is in a cell working temperature zone (generally 800 ℃), and the temperature of the temperature zone can be provided by an external heat source and also can be maintained by the heat generated by the cell when the cell works. The fuel cell runs in a working temperature area, consumes carbon fuel and generates electricity outwards, when the carbon fuel is consumed to the extent that the normal running of the cell cannot be maintained, a thrust force towards the direction of an outlet end is applied to a fuel tank arranged in a channel, so that the fuel tank moves towards the direction of an outlet until the fuel tank which is close to the cell and is filled with the fuel in the direction of the inlet is pushed to the position under the anode of the cell, the fuel cell converts the chemical energy of the carbon into electric energy through the coupling of CO electrochemical oxidation reaction on the anode and reverse Boudouard reaction on the fuel, the normal running of the cell is maintained, the fuel tank is preheated in a heat preservation area before reaching the working temperature area of the cell, the stable transition of the cell fuel is ensured, and meanwhile, the fuel tank which is just used is pushed to the heat preservation area close to the working temperature area of the cell on the outlet side, the temperature is slowly and gradually reduced, and the large thermal shock on the fuel tank is avoided.
Further, the channel cross-section is of various shapes; the shape is rectangular or semicircular.
Further, the channel is made of high-temperature-resistant and oxidation-resistant materials, and the high-temperature-resistant and oxidation-resistant materials are ceramic materials such as quartz or corundum.
Furthermore, the fuel cell is of a flat plate type structure and is prepared by adopting general materials and processes; the electrolyte in the fuel cell employs yttria stabilized zirconia YSZ. The anode can be made of a material with good ionic conductivity and electronic conductivity and a certain catalytic effect on carbon fuel, and can be made of a nickel-YSZ composite metal ceramic material, a silver-GDC (gadolinium doped cerium oxide) composite metal ceramic material, a copper-based composite metal ceramic material, a perovskite-based anode material and the like. The cathode can adopt a material with higher ion electronic conductivity and higher electro-catalytic activity on oxygen molecules, and can adopt a metal ceramic material compounded by silver and GDC and a composite material doped with lanthanum manganate or lanthanum cobaltate and YSZ; the preparation process adopts a tape casting method to prepare the anode and the electrolyte and adopts a screen printing method to prepare the cathode.
Further, the fuel tank has a groove structure, the cross-sectional shape of which is similar to that of the channel, the size of which is slightly smaller, and the opening of which is parallel to the plane of the channel on which the fuel cell is mounted.
Further, the solid fuel is a carbon-rich solid, and the solid fuel is refined pure carbon, activated carbon, biomass carbon or coal, or is loaded with a catalyst for promoting a reverse boudouard reaction, and the catalyst is a transition metal oxide, an oxide or a carbonate of an alkali metal or an alkaline earth metal.
Further, the barrier layer is of a shape similar to the cross-section of the channel and is of a thickness sufficient to form a barrier layer in the channel; the isolation layer is made of a high-temperature-resistant flexible material, and the high-temperature-resistant flexible material is ceramic cotton, ceramic felt or asbestos; the air permeability can be adjusted by selecting a suitable thickness and pressing it with a suitable pressure.
Further, the overall size of the device is mainly determined by the size of the channel, and can be centimeter-sized in a laboratory or meter-sized in practical application according to needs. Typically, the length of the channels should be greater than 6 times the length of the fuel slots; the height and width of the fuel tank should be 0.9 to 0.99 times the height and width of the channel interior; and the height and width of the prepared flexible barrier layer should be 1-1.05 times of the height and width of the inner part of the channel.
In the invention, when a new fuel tank is pushed to the cell working area, the position of the fuel tank is left at the inlet end part of the channel normal temperature area, and at the moment, the new fuel tank filled with fuel and the isolating layer can be arranged in the channel. After a period of operation, the fuel tank which has started to be used is pushed out of the outlet end of the channel constant temperature area. The pushed fuel tank can be removed, the residue (mainly containing catalyst, ash and carbon which is not consumed) left in the fuel tank can be poured out for centralized treatment, and the emptied fuel tank can be recycled.
Compared with the prior art, the invention has the advantages that:
(1) The fuel cell is arranged in the middle of the channel, and the fuel tank for containing fuel is arranged in the channel, so that the continuous supply of the carbon-containing solid fuel is realized, and the continuous operation of the DC-SOFC is realized. The device has simple structure and is easy to realize.
(2) Three temperature regions which are necessarily involved in the high-temperature fuel cell, namely a cell working temperature region, a heat preservation region and a normal temperature region, are skillfully utilized. The fuel in the fuel groove of the battery working temperature area is used by the battery by arranging a series of fuel grooves in the channel at the same time, and meanwhile, the fuel groove to be used at the inlet side end of the channel can be gradually preheated and heated along with the reduction of the distance close to the battery working temperature area, so that the temperature fluctuation in the replacement process of the fuel groove is small, and the battery can stably run; and the spent fuel tank may be gradually cooled to room temperature with distance from the outlet end. The inlet and outlet ends of the channel are positioned in the normal temperature area, which is beneficial to the adding and removing operation of the fuel tank.
(3) The use of isolation layer can play suitable heat preservation effect to the channel is inside, forms the air lock to the gas in the channel simultaneously, is favorable to fuel cell to the abundant oxidation of fuel, plays the effect that improves battery performance and electricity conversion efficiency.
(4) The method for continuously supplying the solid fuel does not need any gas as a carrier gas. Loading and unloading fuel cells into and from the channels can be accomplished in a variety of ways at ambient temperatures.
Drawings
Fig. 1 is a cross-sectional view of an apparatus for continuously supplying solid fuel to a direct carbon solid oxide fuel cell according to the present invention.
FIG. 2-1 is a cross-sectional view of the channel;
FIG. 2-2 is a top view of the channel;
fig. 2-3 are left side views (cross-sectional shapes) of two possible channels.
FIG. 3-1 is a cross-sectional view of a solid oxide fuel cell;
fig. 3-2 is a top view of a solid oxide fuel cell.
FIG. 4-1 is a cross-sectional view of a fuel tank;
fig. 4-2 is a left side view of a possible two configurations of fuel cell.
FIG. 5-1 is a cross-sectional view of a barrier layer;
fig. 5-2 is a left side view of two possible spacer layers.
The figures show that: 1. a channel; 2. a fuel cell; 3. a fuel tank; 4. a solid fuel; 5. an isolation layer; 6. a battery window; 7. a high temperature sealing agent; 8. an inlet end; 9. an outlet end; 10. and (4) residue.
Detailed Description
The present invention will be described in further detail with reference to examples and drawings, but the scope of the present invention is not limited to the scope of the embodiments.
Example 1
As shown in fig. 1, the device for continuously supplying carbon-rich solid fuel to DC-SOFC includes a channel 1, a fuel cell 2, a fuel tank 3, a solid fuel 4 and a separation layer 5. The channel 1 is a pipe gallery structure with openings at both ends, and a plane is arranged above the channel, and a cell window 6 is reserved in the middle of the plane and used for installing the fuel cell 2. The fuel cell 2 is sized slightly larger than the cell window 6 and the fuel cell 2 is encapsulated in the cell window 6 of the channel 1 using a high temperature seal 7 while the window 6 is sealed. The anode of the fuel cell 2 faces the inside of the channel 1. The fuel tank 3 is a container of a groove structure whose opening is parallel to the plane of the channel 1 in which the fuel cell is accommodated, and whose cross section is similar in shape to the cross section of the channel 1 and is slightly smaller in size so as to be freely movable in the channel 1. When the device is operated, a plurality of fuel tanks 3-f1, 3-f2 and … … which contain carbon-rich solid fuel 4 and are identical to the fuel tank 3 are arranged in the channel 1, the fuel tanks are separated by adopting the isolating layer 5, and the isolating layer 5 is contacted with the inner wall of the channel 1 but can freely move along with the fuel tanks in the channel 1. The middle part of the channel 1 is positioned in the working temperature zone (generally 800 ℃) of the fuel cell, when the cell runs, a fuel tank 3 containing solid fuel 4 is positioned under the fuel cell 2, and the fuel cell 2 realizes the conversion of the chemical energy of carbon into electric energy through the coupling of CO electrochemical oxidation reaction on the anode and reverse Boudouard reaction on the fuel. When the fuel 4 in the fuel tank 3 is nearly exhausted, a new fuel tank full of fuel is loaded at the inlet end 8 of the channel 1 and pushed towards the outlet end 9 by the distance of one fuel tank, so that the fuel tank full of fuel close to the fuel cell 2 in the direction of the inlet end is positioned right below the fuel cell 2, and the fuel cell is operated normally. The spent fuel tanks 3-e1, 3-e2, … … have the residue 10 left therein, and the fuel tank containing the residue 10 is pushed toward the outlet end 9 and gradually cooled.
In the implementation process, the channel 1 is made of high-temperature-resistant and oxidation-resistant materials. In this embodiment, quartz is used, and the channel 1 is smooth inside, so as to facilitate the sliding of the fuel tank 3 and the isolating layer 5. Fig. 2-1 shows a cross-sectional view of a channel 1 having a length L and a height H, above which a cell window 6 has a length L cw (lower corner indicates cell window). Fig. 2-2 show a top view of the channel 1, clearly showing the plane above the channel 1 and its cell window 6, the width of the inner wall of the channel 1 being W, and the width of the cell window 6 being W cw . The cross section of the channel 1 can be of various shapes on the premise of ensuring that the upper part of the channel 1 is a planeFig. 2-3 show two possible cross-sectional shapes for the channel 1, one rectangular (fig. 2-3 a) and one semicircular (fig. 2-3 b), which is used in this embodiment.
Figure 3-1 shows a cross-sectional view of a fuel cell 2 mounted on a cell window 6 having a length l along the length of the channel 1 c (the lower corner symbol represents a battery, cell). The fuel cell 2 consists of a porous anode 2-1, a dense electrolyte 2-2 and a porous cathode 2-3, and the materials and the preparation of the cell can adopt the existing general method, namely: the anode material adopts ceramic metal compounded by nickel and Yttrium Stabilized Zirconia (YSZ); YSZ is adopted as the electrolyte; the cathode is made of a composite material of an oxide with electronic conductivity (such as doped lanthanum manganate) and YSZ. FIG. 3-2 shows a top view of a fuel cell 2 with a width w c . The length and width of the fuel cell 2 is slightly greater than the length and width of the cell window 6 in the channel 1, i.e. application l c ＞l cw ，w c ＞w cw 。
The fuel cell 2 is sealed over the cell window 6 using a high temperature seal 7. The high-temperature sealing agent can adopt ceramic glue or silver conductive glue which are purchased in the market. The specific sealing method comprises the following steps: the high-temperature sealing agent 7 is coated on the edge of the cell window 6, then the anode of the fuel cell 2 facing the inside of the channel 1 is placed on the cell window 6, the high-temperature sealing agent 7 coated on the edge of the window 6 bonds the edges of the fuel cell 2 and the cell window 6 together, and after standing and drying, the fuel cell 2 is tightly sealed on the channel 1 through high-temperature roasting treatment.
The fuel tank 3 may be made of the same material as the channel 1 and requires a smooth outer surface in order to slide in the channel 1. Figure 4-1 shows a cross-sectional view of a fuel tank 3, which, when placed in a channel 1, has a length l along the length of the channel 1 t (lower corner symbol denotes fuel tank, tank) and a height h t . The cross section of the fuel tank 3 is similar to that of the channel 1, corresponding to two shapes of the cross section of the channel 1 (fig. 2-3), the two cross-sectional shapes of the fuel tank 3 are shown in the left view (fig. 4-2), and the width of the fuel tank 3 is w t The fuel tank uses a rectangular groove. The length L of the channel 1 is much greater than the length L of the fuel tank 3 t In the channel 1Can simultaneously accommodate a plurality of fuel tanks 3, 3-f1, 3-f2, … …, 3-e1, 3-e2 and … …, and generally requires L to be more than 6L t . Height h of fuel tank 3 t And width w t The height H and the width W of the inner wall of the channel 1 are smaller than those of the inner wall of the channel 1, so that the fuel tank 3 can be placed into the channel 1 and can freely move in the channel 1; however, the dimensions of the fuel tank 3 must not be too small, which would reduce the space utilization of the device. In general, a reasonable size range is 0.90H ≦ H t Not more than 0.99H and not more than 0.90W t ≤0.99W。
The solid fuel 4 is a carbon-rich solid, which may be refined pure carbon. The solid fuel 4 is generally in the form of powder or granules. To increase the reactivity of the fuel, a catalyst that promotes the reverse Boudouard reaction may also be loaded into the fuel, for example: transition metal oxide Fe 2 O 3 . In the implementation of the fuel supply for a DC-SOFC, solid fuel 4 is directly contained in the fuel tank 3 and enters the channels 1 with the fuel tank 3.
The isolation layer 5 is made of high-temperature-resistant flexible heat-insulating materials and can be made of ceramic wool. These high temperature resistant flexible materials have the characteristics of heat preservation and ventilation, and the ventilation can ensure the discharge of the product gas of the battery, but the efficient operation of the DC-SOFC also needs the anode to ensure a certain positive pressure state, so the isolation layer 5 needs to have enough air resistance. The thermal insulation properties and the air permeability (air resistance) can be adjusted by applying pressure or by using different thicknesses. FIG. 5-1 shows a cross-sectional view of a spacer layer 5 having a height hs (lower corner symbol denotes spacer) and a thickness t s . FIG. 5-2 shows a left side view of the isolation layer 5, which has the same shape as the cross-sectional shape of the channel 1, and in order to make the isolation layer 5 closely contact the inner wall of the channel 1, the size of the isolation layer 5 can be slightly larger, generally, the more reasonable size range is H ≦ H s H is less than or equal to 1.05 and W is less than or equal to W s ≤1.05W。
The sizes of all the components in the device can be centimeter-level in a laboratory or meter-level in practical application. For example, the following dimensions may be taken in the laboratory: l =30cm, W =3.0cm, H =1.5cm, L cw ＝2.0cm、w cw ＝2.3cm、l c ＝2.5cm、w c ＝2.8cm、l t ＝2.5cm、h t ＝1.4cm、w t ＝2.8cm、t s =0.2cm, the effective area of the cell is the area of the window, i.e.: l cw ×w cw ＝＝2.0cm×2.3cm＝4.6cm 2 . The channel 1 and the fuel tank 3 are made of quartz, and have a rectangular cross-section structure, and if the wall thickness of the fuel tank 3 is 0.1cm, the volume of the fuel tank 3 is (l) t -0.2)×(w t -0.2)×(h t -0.1)＝7.8cm 3 . Active carbon powder is used as fuel, and the tap density of the fuel is about 0.4gcm -3 . One fuel tank 3 can hold about 3g of activated carbon fuel. At present, the fuel utilization of DC-SOFC in the laboratory has exceeded 40%, with conservative estimates, fuel cell 2 at 1A (0.22 Acm) -2 ) Discharge operation by current of about 9Ah g, since the capacity of carbon -1 Therefore, the time for which one fuel tank 3 can discharge the battery is 3g × 40% × 9Ah g -1 /1A＝10.8h。
As shown in fig. 1, a fuel tank 3 is filled with a solid fuel 4 rich in carbon. When the system operates, the system can be divided into three temperature zones according to the ambient temperature of the channel 1: working temperature zone, heat preservation zone and normal temperature zone. The working temperature zone of the battery where the battery is operated is generally maintained at 800 ℃, the temperature environment can be provided by external heating equipment (such as an electric furnace), and the temperature environment can also be maintained by using waste heat generated in the operation process of the battery; the inlet end 8 and the outlet end 9 of the channel 1 are positioned in a normal temperature zone, so that the fuel tank can be conveniently added and removed; between the battery working temperature area and the normal temperature area is a heat preservation area with the temperature gradually decreasing from the high-temperature battery working temperature area to the normal temperature area. When the fuel tank 3 under the fuel cell 2 in the cell working temperature zone finishes the discharging consumption, a new fuel tank full of carbon fuel and a new isolating layer are added at the inlet end 8 of the normal temperature zone, and a thrust force towards the outlet end 9 direction of the channel is applied to the fuel tank and the isolating layer thereof, so that all the fuel tanks and isolating layers in the channel 1 move towards the outlet direction, and the fuel tank full of fuel 3-f1 close to the fuel cell 2 in the inlet direction is pushed to the position under the fuel cell 2, and the fuel tank 3-f1 is gradually heated to the working temperature close to the fuel cell 2 in the temperature preserving zone, so the cell can continuously and stably run; and the fuel tank 3-e1 which is just used up is pushed to the outlet end 9 direction, and the temperature is slowly reduced. In this way, the fuel cell 2 can be operated continuously by periodically adding a new fuel tank full of fuel from the inlet port 8. When the spent fuel tank reaches the outlet end 9 at the isothermal zone, the respective barrier layer and fuel tank are removed. The removed fuel tank can be emptied and reloaded with fuel for reuse. By this method, 1kg of carbon fuel allowed the experimental apparatus to be continuously operated for 3600 hours.
Example 2
This embodiment is the same as embodiment 1 except that the channel 1 is made of a corundum ceramic material and the channel 1 has a semicircular cross-sectional shape as shown in fig. 2-3 b. The fuel cell uses symmetrical electrodes, and the electrode material adopts Ag and GDC composite ceramic material with ion electronic conductivity. In this embodiment, the fuel tank 3 is a semicircular quartz boat, as shown in the left view of the fuel tank 4-2 b. The solid fuel 4 is activated carbon fuel loaded with ferric oxide. The isolation layer 5 is made of ceramic fiber paper.
Example 3
This embodiment is the same as embodiment 1, the channel 1 is made of quartz material, and the cross-sectional shape of the channel 1 is semicircular as shown in fig. 2-3 b. The fuel cell uses a composite cermet material with Ag and GDC as symmetrical electrodes. In this embodiment, the fuel tank 3 is a semicircular quartz boat, as shown in the left view of the fuel tank 4-2 b. The solid fuel 4 is coal fuel.
Claims (10)
1. An apparatus for continuously supplying fuel for a direct carbon solid oxide fuel cell, characterized by comprising a channel (1), a fuel cell (2), a fuel tank (3), a solid fuel (4) and a separation layer (5); the channel (1) is a gallery structure capable of accommodating a plurality of fuel slots (3) simultaneously along its length; the channel (1) is provided with at least one plane, and the middle part of the plane is provided with a cell window which is used for installing the fuel cell (2); the fuel cell (2) is a three-layer structure consisting of a dense electrolyte, a porous anode and a cathode on two sides of the dense electrolyte, the fuel cell (2) is sealed on the cell window of the channel, and the anode faces the inside of the channel; the fuel tank (3) is provided with a groove structure and is used for containing solid fuel (4), the cross section shape of the fuel tank is similar to that of the channel, the size of the fuel tank is slightly smaller, and the fuel tank can freely slide in the channel; the solid fuel (4) is a carbon-rich solid fuel; the isolation layer (5) is positioned between adjacent fuel tanks (3); the isolation layer (5) is made of high-temperature-resistant flexible material; the device for continuously providing the solid fuel is characterized in that a plurality of fuel tanks (3) filled with the solid fuel are arranged along the length direction of a channel (1), the openings of the fuel tanks (3) are parallel to a plane of the channel provided with the fuel cells (2), and the opening of one fuel tank (3) is opposite to the anode of the fuel cell (2); each fuel groove is separated by a separation layer (5), and each fuel groove (3) is directly contacted with the adjacent separation layer (5); when the fuel cell (2) runs, the fuel cell (2) in the middle of the channel (1) is in a cell working temperature area, the inlet end (8) and the outlet end (9) of the channel (1) are in a normal temperature area, and a heat preservation area with the temperature gradually reduced from the working temperature area to the normal temperature area is arranged between the working temperature area and the normal temperature area; the fuel cell operates in a working temperature zone, consumes the solid fuel in the fuel tank opposite to the fuel cell and generates electricity; after the fuel is consumed, adding a new fuel tank filled with fuel from the inlet end of the channel, and applying a thrust force to the outlet end from the inlet end to push all the fuel tanks in the channel to the outlet end until the fuel tank filled with fuel adjacent to the fuel cell is opposite to the anode of the fuel cell, so that the cell continues to operate; the continuous supply of the solid fuel is realized by the repeated operation, the direct carbon solid oxide fuel cell can continuously run, and the fuel tank to be consumed by the fuel is pushed to the outlet end (9), removed, emptied, filled with the fuel and recycled.
2. The apparatus for continuously supplying fuel to a direct carbon solid oxide fuel cell as claimed in claim 1, wherein the channels (1) have at least one flat surface with a plurality of shapes in cross section; the shape is rectangular or semicircular.
3. An arrangement for continuously supplying fuel to a direct carbon solid oxide fuel cell according to claim 1, characterized in that the channels (1) are made of a high temperature resistant, oxidation resistant material, which is quartz or corundum.
4. The apparatus for continuously supplying fuel to a direct carbon solid oxide fuel cell according to claim 1, wherein the fuel cell (2) has a flat plate structure and is prepared by using general materials and processes; the electrolyte in the fuel cell (2) adopts yttrium stabilized zirconia YSZ; the anode is made of a nickel and YSZ composite metal ceramic material, a silver and GDC composite metal ceramic material, a copper-based composite metal ceramic material or a perovskite-based anode material; the cathode is made of silver-based composite metal ceramic material, or composite material doped with lanthanum manganate or lanthanum cobaltate or YSZ.
5. The apparatus of claim 4, wherein the anode and the electrolyte are prepared by a casting process, and the cathode is prepared by a screen printing process.
6. An arrangement for continuously supplying fuel to a direct carbon solid oxide fuel cell according to claim 1, characterized in that the fuel tank (3) has a groove structure with a cross-sectional shape similar to the shape of the channel and a slightly smaller size, the opening of which is parallel to the plane of the channel in which the fuel cell is installed.
7. The apparatus for continuously supplying fuel for a direct carbon solid oxide fuel cell according to claim 1, wherein the solid fuel (4) is a carbon-rich solid, and the solid fuel is refined pure carbon, activated carbon, biomass charcoal or coal.
8. The apparatus of claim 1, wherein a catalyst that promotes the reverse boudouard reaction is loaded in the solid fuel, and the catalyst is a transition metal oxide, an oxide of an alkali metal, an alkaline earth metal, or a carbonate.
9. An arrangement for continuously supplying fuel to a direct carbon solid oxide fuel cell as claimed in claim 1, characterized in that the barrier layer (5) is of a shape similar to the cross-section of the channels and of a thickness sufficient to form a barrier layer in the channels; the isolation layer is made of high-temperature-resistant flexible materials, and the high-temperature-resistant flexible materials are ceramic wool, ceramic felt, ceramic fiber paper or asbestos.
10. An arrangement for continuously supplying fuel to a direct carbon solid oxide fuel cell according to claim 1, characterized in that the length of the channels (1) is more than 6 times the length of the fuel tank (3); the height and width of the fuel tank should be 0.9 to 0.99 times the height and width of the channel interior; and the height and width of the prepared flexible isolation layer should be 1-1.05 times of the height and width of the inner part of the channel.
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