CN109411778A - A kind of preparation process of solid oxide fuel cell stack - Google Patents
A kind of preparation process of solid oxide fuel cell stack Download PDFInfo
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- CN109411778A CN109411778A CN201811269936.9A CN201811269936A CN109411778A CN 109411778 A CN109411778 A CN 109411778A CN 201811269936 A CN201811269936 A CN 201811269936A CN 109411778 A CN109411778 A CN 109411778A
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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
- H01M8/002—Shape, form of a fuel cell
- H01M8/004—Cylindrical, tubular or wound
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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
- H01M8/10—Fuel cells with solid electrolytes
- H01M8/1007—Fuel cells with solid electrolytes with both reactants being gaseous or vaporised
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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
- H01M8/24—Grouping of fuel cells, e.g. stacking of fuel cells
- H01M8/2465—Details of groupings of fuel cells
- H01M8/2484—Details of groupings of fuel cells characterised by external manifolds
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- 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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- 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
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
- Y02P70/50—Manufacturing or production processes characterised by the final manufactured product
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Abstract
The invention discloses a kind of preparation processes of solid oxide fuel cell stack, include: that integrated molding idiosome is made in electrode in the cast of several tubular cells units and the inlet chamber by (1), is connected to the inner flow passage of electrode in the every cast with the inlet chamber;(2) one layer of electrolyte layer is coated on the outer wall of electrode in the every cast, then carries out first sintering processing;(3) one layer of outer electrode layer is coated on the electrolyte layer, is carried out second of sintering processes, is obtained the integral structure of several root canal type battery units and the inlet chamber.The preparation process of solid oxide fuel cell stack of the invention without again assembling every root canal type battery unit on inlet chamber after positioning one by one, not only make that the air-tightness between inlet chamber and the first stacks of cells is good and stability is high, the good isolation for realizing anodic gas and cathode gas, effectively improves the power generation performance and long-time stability of solid oxide fuel cell stack.
Description
Technical field
The present invention relates to field of fuel cell technology, in particular to a kind of system of solid oxide fuel cell stack
Standby technique.
Background technique
Solid oxide fuel cell (SOFC) is high with generating efficiency, discharge is low, is adapted to extensively pluralities of fuel gas
And UTILIZATION OF VESIDUAL HEAT IN is worth the advantages that high, is to provide the energy of clean and effective, alleviates the energy and environmental crisis, realizes that China can be held
One of the grand strategy technology of supervention exhibition.
SOFC is broadly divided into two class of template and cast at present.Wherein template SOFC battery pile be by template battery unit and
Sheet bipolar plate stack is formed, and in order to which anodic gas and cathode gas is isolated, is needed between template battery unit and sheet bipolar plates
Being fully sealed under the conditions of SOFC hot operation is realized, to the thermal expansion matching of sealing material, thermal stability, chemical stability
Equal requirements are very high.Compared with template SOFC, cast SOFC sealing structure is relatively easy, it also requires in tubular cells unit and
Junction between the entry/exit air cavity of internal gas is sealed so that anodic gas and cathode gas is isolated.
Technical solution currently used for sealing between tubular cells unit and entry/exit air cavity is more.Siemens-Westinghouse Electric
Cast SOFC battery pile between battery unit and air cavity use endless all-sealed structure.The cast SOFC electricity of Mitsubishi Heavy Industries Ltd
In the heap of pond, more complicated sealing structure is used between battery and air cavity: first at the position that tubular cells unit needs to seal
Using porcelain bushing in inorganic high-temp glue sticking, sealing-in is carried out between porcelain bushing and air cavity again.For middle-size and small-size mobile electricity
It stands or power supply is in order to meet mobile needs often has higher requirement to sealing, using the higher glass capsulation of sealing performance
Material carry out Leakless sealing, as Toto company cast SOFC pile in, tubular cells unit first uses glass base sealing material
Then sealing-in is attached with air cavity again on end metal pullover.
It requires to prepare tube-type fuel cell unit and inlet chamber respectively in the prior art, then again fires the cast of dispersion
Material battery unit is connected on inlet chamber according to certain arrangement mode.This sealing-in mode has the disadvantage that (1) battery pack
Assembly work amount is big, and the effect sealed is difficult to ensure;(2) air-tightness is carried out since connecting portion uses xenogenesis sealing material
Sealing-in --- inorganic high-temp glue and glass sealing material etc. as mentioned above, during quick repeated priming, different materials
Between the thermal stress that generates of thermal expansion coefficient difference will lead to connecting portion and be easy to appear cracking.Seal failure not only results in
It is on fire even to cause pile when serious for Performance data decline and pile failure.
Summary of the invention
The inventors discovered that the concentration of inlet chamber side reaction gas is higher, it is higher to seal request.In view of this, of the invention
A kind of solid oxide fuel cell stack and solid oxide fuel battery system provided, preferably overcomes above-mentioned existing skill
Art there are the problem of and defect, by the way that inlet chamber and every root canal type cell designs in the first stacks of cells are integrated
Connection structure not only makes inlet chamber and first without again assembling every root canal type battery unit on inlet chamber one by one after positioning
Air-tightness between stacks of cells is good and stability is high, realizes the good isolation of anodic gas and cathode gas, effectively mentions
The power generation performance and long-time stability of high solid oxide fuel cell group, while simplifying the assembler of solid fuel cell heap
Make.
Specifically, the invention proposes embodiments in detail below:
A kind of preparation process of solid oxide fuel cell stack, comprising: the solid oxide fuel cell stack includes
Inlet chamber and the first stacks of cells connecting with one end face of inlet chamber, first stacks of cells include several root canals
Type battery unit, the every tubular cells unit include electrode in cast, the electricity for being coated on electrode outer surface in the cast
Solution matter layer and the outer electrode layer for being coated on the electrolyte layer outer surface;
The preparation method includes:
(1) integrated molding idiosome is made in electrode in the cast of several tubular cells units and the inlet chamber,
It is connected to the inner flow passage of electrode in the every cast with the inlet chamber;
(2) one layer of electrolyte layer is coated on the outer wall of electrode in the every cast, is then carried out at first sintering
Reason;
(3) after first sintering processing, one layer of outer electrode layer is coated on the electrolyte layer, is carried out second
Sintering processes obtain the integral structure of several root canal type battery units and the inlet chamber.
Further, the solid oxide fuel cell stack further includes at least one set of second stacks of cells, and described the
Pass through centre between one stacks of cells and second stacks of cells and between the second stacks of cells of two adjacent groups
Air cavity connection, each second stacks of cells includes several root canal type battery units, the every tubular cells unit packet
Electrode in cast is included, the electrolyte layer of electrode outer surface in the cast is coated on and is coated on the electrolyte layer outer surface
Outer electrode layer;
Include: in step (1) by the inlet chamber, first stacks of cells several root canal types in electrode, centre
Integrated molding idiosome is made in electrode in air cavity and several root canal types of at least one set of second stacks of cells.
Further, in step (1), the integrated molding idiosome is by using 3D printing molding, injection forming or gel
Injection moulding forming method is prepared.
It further, further include that preheating is carried out to the integrated molding idiosome of acquisition in step (1).
Further, the preheating temperature is 600~1000 DEG C, and the preheating time is 4~6h.
Further, in step (2), the first sintering treatment temperature is 1000~1500 DEG C, and the first time burns
The knot processing time is 2~18h;
In step (3), second of sintering processes temperature is 900~1300 DEG C, and the first sintering handles the time
For 8~20h.
Further, the material of electrode is perovskite composite oxide and spinel-type oxygen in several casts
At least one of compound or cermet;The material of the inlet chamber is identical as the material of electrode in the cast.
Further, the material of the electrolyte layer is rare earth ion doped cerium oxide or rare earth ion doped zirconium oxide;
The material of the outer electrode layer is at least one of perovskite composite oxide and spinel oxides or cermet.
It further, further include in inlet chamber outer surface before carrying out the first sintering processing in step (3)
Coat one layer of fine and close ceramic barrier layer.
Further, the solid oxide fuel cell stack further includes outlet chamber;
After step (3) further include: the solid oxide fuel cell stack further includes outlet chamber;Several casts
Electrode, the inlet chamber and the outlet chamber are integrally formed in the cast of battery unit.
Compared with prior art, the beneficial effect of the preparation process of a kind of solid oxide fuel cell stack of the invention
It is:
The preparation process of solid oxide fuel cell stack of the invention is by will be in inlet chamber and the first stacks of cells
Every root canal type battery unit be made for integral connecting structure, without positioning after every root canal type battery unit is assembled one by one again
On inlet chamber, not only make that the air-tightness between inlet chamber and the first stacks of cells is good and stability is high, realizes anodic gas
With the good isolation of cathode gas, the power generation performance and long-time stability of solid oxide fuel cell stack are effectively improved, simultaneously
Simplify the assembly work of solid fuel cell heap.
To enable the above objects, features and advantages of the present invention to be clearer and more comprehensible, preferred embodiment is cited below particularly, and cooperate
Appended attached drawing, is described in detail below.
Detailed description of the invention
In order to illustrate the technical solution of the embodiments of the present invention more clearly, below will be to needed in the embodiment attached
Figure is briefly described, it should be understood that the following drawings illustrates only certain embodiments of the present invention, therefore is not construed as pair
The restriction of range for those of ordinary skill in the art without creative efforts, can also be according to this
A little attached drawings obtain other relevant attached drawings.
Fig. 1 is the first structural schematic diagram of solid oxide fuel cell stack of the invention;
Fig. 2 is second of structural schematic diagram of solid oxide fuel cell stack of the invention;
Fig. 3 is the third structural schematic diagram of solid oxide fuel cell stack of the invention;
Fig. 4 is the cross-sectional structure schematic diagram of tubular cells unit of the invention;
Fig. 5 is a kind of structural schematic diagram of outlet chamber of the invention.
Main element symbol description:
100- inlet chamber;
The first stacks of cells of 200-;
300- outlet chamber;
310- connecting hole;
The second stacks of cells of 400-;
Air cavity among 500-;
600- tubular cells unit;
610- internal electrode layer;
620- electrolyte layer;
630- outer electrode layer.
Specific embodiment
To facilitate the understanding of the present invention, it elaborates below with reference to the mode of embodiment to technical solution of the present invention,
In the following description, numerous specific details are set forth in order to facilitate a full understanding of the present invention.
But the invention can be embodied in many other ways as described herein, those skilled in the art can be with
Similar improvement is done without violating the connotation of the present invention, therefore the present invention is not limited to the specific embodiments disclosed below.
Unless otherwise defined, all technologies used herein and scientific term have and the common skill of fields of the present invention
The normally understood identical meaning of art personnel.When there is a conflict, the definition in this specification shall prevail.
Term as used herein:
Term "comprising" used herein, " comprising ", " having ", " containing " or its any other deformation, it is intended that covering
Non-exclusionism includes.For example, composition, step, method, product or device comprising listed elements are not necessarily limited to those and want
Element, but may include not expressly listed other elements or such composition, step, method, product or device it is intrinsic
Element.
Dosage, temperature or other values or parameter are excellent with range, preferred scope or a series of upper limit preferred values and lower limit
When the Range Representation that choosing value limits, this should be understood as specifically disclosing by any range limit or preferred value and any range
Any pairing of lower limit or preferred value is formed by all ranges, regardless of whether the range separately discloses.For example, when open
When range " 1~5 ", described range should be interpreted as including range " 1~4 ", " 1~3 ", " 1~2 ", " 1~2 and 4~
5 ", " 1~3 and 5 " etc..When numberical range is described herein, unless otherwise stated, otherwise the range is intended to include its end
Value and all integers and score in the range.
"and/or" is used to indicate that one of illustrated situation or both may to occur, for example, A and/or B includes (A
And B) and (A or B).
The present invention provides a kind of preparation processes of solid oxide fuel cell stack, wherein Fig. 1 to Fig. 5 is please referred to, it should
Solid oxide fuel cell stack includes inlet chamber 100 and the first stacks of cells 200 for connecting with 100 1 end face of inlet chamber,
Inlet chamber 100 has air inlet (not shown), and the first stacks of cells 200 includes several root canal type battery units 600.Often
Root canal type battery unit 600 includes electrode 610 in cast, is coated on the electrolyte layer 620 of 610 outer surface of electrode and packet in cast
It is overlying on the outer electrode layer 630 of 620 outer surface of electrolyte layer.The central hollow section of electrode 610 is inner flow passage in cast.
Solid oxide fuel cell stack preparation process includes:
Step (1): integrated molding is made in electrode 610 in the cast of several root canal type battery units 600 and inlet chamber 100
Idiosome, and it is connected to the inner flow passage of electrode 610 in every root canal type with inlet chamber 100.
Preferably, laser photocuring 3D printing molding, injection forming or vacuum gel-casting molding etc. can be used in the present invention
The existing integral formation method that can be used for is by electrode 610 and the air inlet in the cast of several tubular cells units 600
Integrated molding idiosome is made in chamber 100.
It is preferred that above-mentioned preparation method further includes that integrated molding idiosome to acquisition is cleaned, dried and preheating.Its
In, drying process for naturally dry or can be placed in 60~80 DEG C as dried in 60 DEG C, 65 DEG C, 70 DEG C, 75 DEG C or 80 DEG C of baking oven
It does to remove the remaining solvent of possibility being integrally formed in idiosome;During preheating: preheating temperature is preferably 600~
1000 DEG C such as 600 DEG C, 700 DEG C, 800 DEG C, 900 DEG C or 1000 DEG C, the preheating time be preferably 4~6h such as 4h, 4.5h,
5h, 5.5h or 6h etc..
Step (2): coating one layer of electrolyte layer 620 in every root canal type on the outer wall of electrode 610, then carries out for the first time
Sintering processes.
Preferably, it is existing that slurry impregnation, physical deposition methods, chemical deposition or electrophoretic deposition etc. can be used in the present invention
Process coats one layer of electrolyte layer 620 in every root canal type on the outer wall of electrode 610, naturally it is also possible to use other coatings
Mode coats one layer of electrolyte layer 620 in every root canal type on the outer wall of electrode 610, the thickness of electrolyte layer 620 is according to reality
It needs to be arranged.
Preferably, the first sintering treatment temperature be 1000~1500 DEG C as 1000 DEG C, 1100 DEG C, 1200 DEG C,
1300 DEG C, 1400 DEG C or 1500 DEG C etc.;The first sintering processing time is 2~18h such as 2h, 5h, 8h, 10h, 12h, 15h
Or 18h etc..
Step (3): after first sintering processing, coating one layer of outer electrode layer 630 on electrolyte layer 620, into
Second of sintering processes of row obtain the integral structure of several root canal type battery units 600 and inlet chamber 100, even if inlet chamber
100 and first every root canal type battery unit 600 in stacks of cells 200 be integrated connection structure.
Preferably, second of sintering processes temperature is 900~1300 DEG C such as 900 DEG C, 1000 DEG C, 1100 DEG C, 1200
DEG C or 1300 DEG C etc., second of sintering processes time is 8~20h such as 8h, 10h, 12h, 15h, 18h or 20h etc..
Preferably, as shown in Figure 2, Figure 3 and Figure 4, solid oxide fuel cell stack further includes at least one set of second battery
Unit group 400, between the first stacks of cells 200 and the second stacks of cells 400 and the second stacks of cells of two adjacent groups
It being connected to by intermediate air cavity 500 between 400, each second stacks of cells 400 includes several root canal type battery units 600,
Every root canal type battery unit 600 include electrode 610 in cast, be coated in cast the electrolyte layer 620 of 610 outer surface of electrode and
It is coated on the outer electrode layer 630 of 620 outer surface of electrolyte layer.
It should be noted that the quantity of above-mentioned second stacks of cells 400 can be designed as one group, two according to actual needs
Group, three groups, five groups or more second stacks of cells 400 of group etc..Tubular cells unit in every group of second stacks of cells 400
600 number can be identical also not identical, and the quantity with the tubular cells unit 600 in the first stacks of cells 200 also can phase
With also can not be identical.Preferably, the quantity of the tubular cells unit 600 in every group of second stacks of cells 400 is electric with first
The quantity of tubular cells unit 600 in cell stack 200 is identical, and is arranged in a one-to-one correspondence.
Correspondingly, in step (1): by inlet chamber 100, the first stacks of cells 200 several root canal types in electrode
610, integrated molding embryo is made in electrode 610 in several root canal types of the second stacks of cells 400 of intermediate air cavity 500 and at least one set
Body, and make inlet chamber 100, the first stacks of cells 200 several root canal types in electrode 610 inner flow passage, intermediate air cavity 500
It is connected to the inner flow passage of electrode 610 in several root canal types of at least one set of second stacks of cells 400.
For anode support type SOFC, the material of electrode 610 uses cermet in above-mentioned cast, it is preferred to use Ni, Co,
The cermet that the transition elements such as Fe, Mn and metal oxide are compounded to form, Ni, Co, Fe, Mn were waited in the cermet
The content crossed in race's element account for 20~80wt% such as 20wt%, 30wt%, 40wt%, 50wt%, 60wt%, 70wt% or
80wt% etc., metal oxide can be enumerated as rare earth ion doped cerium oxide, rare earth ion doped zirconium oxide or aluminium oxide etc..It is right
At least one of perovskite composite oxide and spinel oxides can be used in Ying Di, the material of outer electrode layer 630, i.e.,
Any one in perovskite composite oxide and spinel oxides can be used in the material of external electrode 630, can also be used
The compound of perovskite composite oxide and spinel oxides in any proportion.
For cathode support type SOFC, in above-mentioned cast the material of electrode 610 can be used perovskite composite oxide and
At least one of spinel oxides, i.e., perovskite composite oxide and point can be used in the material of electrode 610 in cast
Any one in spar type oxide, can also be used perovskite composite oxide and spinel oxides in any proportion
Compound;The material of electrode 610 can be also the mixed of perovskite composite oxide and rare earth ion doped cerium oxide in cast
Close object.Accordingly, cermet can be used in the material of outer electrode layer 630.
Preferably, the material of electrolyte layer 620 uses rare earth ion doped cerium oxide or rare earth ion doped zirconium oxide etc..
Wherein, rare earth ion doped cerium oxide is specific enumerable mixes for yttrium (Y) doped cerium oxide, gadolinium (Gd) doped cerium oxide, samarium (Sm)
Miscellaneous cerium oxide or lanthanum (La) doped cerium oxide etc.;Rare earth ion doped zirconium oxide it is specific enumerable for yttrium (Y) doped zirconia or
Scandium (Sc) doped zirconia.
It should be noted that the material of above-mentioned inlet chamber 100 and the material of intermediate air cavity 500 can be with electrodes in cast
610 material is identical, can not also be identical.When inlet chamber 100 and intermediate air cavity 500 are using different from electrode 610 in cast
When material, material can be enumerated as aluminium oxide, zirconium oxide, cerium oxide.Preferably, the material of inlet chamber 100 and intermediate air cavity 500
Matter is identical as the material of electrode 610 in cast.
Further, in order to guarantee the air-tightness of inlet chamber 100, one layer can also be coated in the outside wall surface of inlet chamber 100
Fine and close ceramic barrier layer.The ceramic barrier layer can be using ceramic materials such as aluminium oxide, zirconium oxide, cerium oxide.Preferably, the ceramics
Interlayer uses material identical with the electrolyte layer 620 in tubular cells unit 600.
Preferably, the size of all tubular cells units 600 of the first stacks of cells 200 is identical and the row of being parallel to each other
The size of cloth, all tubular cells units 600 in every group of second stacks of cells 400 is identical and arranged in parallel, and every
Root canal type battery unit 600 is vertically arranged with inlet chamber 100.First stacks of cells 200 and every group of second stacks of cells
400 cross section can be quadrangle, hexagon or circle etc..
Certainly, the present invention be not intended to limit the first stacks of cells 200 all tubular cells units 600 and every group described in
The size and arrangement mode of all tubular cells units 600 in two stacks of cells 400 can also use non-parallel arrangement,
Such as in radioactive ray arrangement or spiral shape arrangement, preferably can more effectively be arranged using the Fibonacci helix in space.
In addition, the tubular cells unit 600 that different tube diameters and different cross section shape also can be used carries out mixing arrangement, into one
Step improves the space density of tubular cells unit 600.
Further, solid oxide fuel cell stack further includes outlet chamber 300.
Preferably, outlet chamber 300 can be integrally formed with inlet chamber 100 and several tubular cells units 600 and be formed.
Certainly, several several root canal types electricity with the first stacks of cells 200 can also be designed in an end face of outlet chamber 300
The one-to-one connecting hole 310 of pool unit 600, as shown in figure 5, by every root canal type battery unit of the first stacks of cells 200
600 one end far from inlet chamber 100 are bonded in 310 periphery of corresponding connecting hole of outlet chamber 300 using high temperature adhesive, or
Barrel connector (not shown) is welded at the connecting hole 310 of outlet chamber 300, the outer diameter of connector is slightly larger than tubular cells
Then every 600 one end far from inlet chamber 100 of root canal type battery unit is inserted into the connector, then passed through by the outer diameter of unit 600
High-temp glue or glass capsulation connection gap.
Above-mentioned term " several " can be enumerated as 2,10,50 with, 100,200,500,800,1000
Deng.
It should be noted that above-mentioned inlet chamber 100, outlet chamber 300 and intermediate air cavity 500 can be respectively cylindrical, length
Cube shape or other shapes etc..
The preparation process of solid oxide fuel cell stack of the invention is by by inlet chamber 100 and the first stacks of cells
Every root canal type battery unit 600 in 200 is made for integral connecting structure, is not necessarily to after positioning again by every root canal type battery unit
600 are assemblied on inlet chamber one by one, not only make the air-tightness between inlet chamber 100 and the first stacks of cells 200 good and steady
Qualitative height realizes the good isolation of anodic gas and cathode gas, effectively improves the power generation of solid oxide fuel cell stack
Energy and long-time stability, while simplifying the assembly work of solid fuel cell heap.
In addition, requiring to prepare tubular cells unit and inlet chamber respectively in the prior art, then again by the cast of dispersion
Battery unit is connected on air cavity according to certain arrangement mode, due to pipe end joint position to be reserved, sealing station and adjacent
Assembly space between tubular cells unit, adjacent two root canals type battery unit spacing are larger.It is the tubular cells list of 8mm with diameter
For member, the centre distance of adjacent two root canals type battery unit is at least needed as 18mm.And the present invention is electric by inlet chamber 100 and first
Every root canal type battery unit 600 in cell stack 200 is made for integral connecting structure, is equally the cast electricity of 8mm with diameter
For pool unit, the centre distance of adjacent cast battery unit can be contracted to 10mm, effectively save between tubular cells unit 600
Assembly space, greatly improve cell density can.
It should be noted that can be applied to using the solid oxide fuel cell stack that preparation process of the invention obtains more
Kind solid oxide fuel battery system, including distributed power generation, portable power and fuel cell power system, inlet chamber
100 air inlet is by external pipeline and system air circuit connection, and outlet chamber 300 and system gas circuit are also by cavity socket or external
Piping connection.Preferably, gas distribution and heat exchange structure can also be set in inlet chamber 100 and outlet chamber 300.
Embodiment 1
(1) it is established in 100 root canal types after the Integrated Model of electrode 610 and inlet chamber 100 using 3 d modeling software,
610 size of electrode is identical in 100 root canal types and parallel arrangement, and whole cross section is square, inlet chamber 100 and outlet chamber
300 are located at the both ends of electrode 610 in 100 root canal types, and vertical with electrode 610 in 100 root canal types;Then pass through laser light
Solidify 3D printing forming technique and obtains the integrated molding idiosome comprising electrode 610 and inlet chamber 100 in several casts, every root canal type
The inner flow passage of interior electrode 610 is connected to inlet chamber 100;Wherein, inlet chamber 100 is printed using yttria-doped ceria slurry
It arrives, electrode 610 is all made of mixture (wherein, the LSM of strontium doping cobalt acid lanthanum (LSM) and yttria-doped ceria in 100 root canal types
Content is 60wt%) printing obtain.
(2) it after the integrated molding idiosome obtained to step (1) cleans, is then done naturally in the environment of shady and cool ventilation
It is dry, then preheating is carried out to the integrated molding idiosome after drying, preheating temperature is 600 DEG C, and the preheating time is 6h.
(3) it is prepared on the outer wall of electrode 610 in the outer surface of inlet chamber 100 and every root canal type using chemical deposition thick
The yttria-doped ceria film that degree is 5 μm, is then sintered 18h under 1000 DEG C of high temperature, makes in every root canal type on 610 outer wall of electrode
It forms one layer of electrolyte layer 620 and forms one layer of ceramic barrier layer in the outer surface of inlet chamber 100.
(4) one layer of nickel oxide (NiO) and yttria-doped ceria compound (nickel oxide are coated in 620 outer surface of electrolyte layer
(NiO) content accounts for 50wt%), be then sintered at 900 DEG C 20h formed outer electrode layer 630, obtain 100 by
Electrode 610 in cast is coated on the electrolyte layer 620 of 610 outer surface of electrode in cast and is coated on 620 outer surface of electrolyte layer
The tubular cells unit 600 that constitutes of outer electrode layer 630, the diameter of every root canal type battery unit 600 is 8mm, adjacent two root canal
The centre distance of type battery unit 600 is 12mm.
(5) outlet chamber 300 is prepared, 100 and 100 root canal type battery units 600 can be designed in an end face of outlet chamber 300
One-to-one connecting hole 310, welds barrel connector at the connecting hole 310 of outlet chamber 300, and the outer diameter of connector is slightly larger than
Then the connection is inserted into every 600 one end far from inlet chamber 100 of root canal type battery unit by the outer diameter of tubular cells unit 600
Part, then pass through high-temp glue or glass capsulation connection gap.
Embodiment 2
(1) using 3 d modeling software establish inlet chamber 100, in 500 root canal types electrode 610 and outlet chamber 300 one
Change model, 610 size of electrode is identical in 500 root canal types and parallel arrangement, and whole cross section is square, 100 He of inlet chamber
Outlet chamber 300 is located at the both ends of electrode 610 in 500 root canal types, and vertical with electrode 610 in 500 root canal types;Then pass through
Laser photocuring 3D printing forming technique obtains the integrated molding idiosome comprising electrode 610 and inlet chamber 100 in several casts,
The inner flow passage of electrode 610 is connected to inlet chamber 100 in every root canal type;Wherein, inlet chamber 100 uses yttria-doped ceria slurry
Printing obtains, and electrode 610 is all made of mixture (its of strontium doping cobalt acid lanthanum (LSM) and yttria-doped ceria in 500 root canal types
In, the content of LSM obtains for 60wt%) printing.
(2) it after the integrated molding idiosome obtained to step (1) cleans, is then done naturally in the environment of shady and cool ventilation
It is dry, then preheating is carried out to the integrated molding idiosome after drying, preheating temperature is 800 DEG C, and the preheating time is 5h.
(3) it is prepared on the outer wall of electrode 610 in the outer surface of inlet chamber 100 and every root canal type using chemical deposition thick
The yttria-doped ceria film that degree is 5 μm, is then sintered 10h under 1200 DEG C of high temperature, makes in every root canal type on 610 outer wall of electrode
It forms one layer of electrolyte layer 620 and forms one layer of ceramic barrier layer in the outer surface of inlet chamber 100.
(4) one layer of nickel oxide (NiO) and yttria-doped ceria compound (nickel oxide are coated in 620 outer surface of electrolyte layer
(NiO) content accounts for 50wt%), be then sintered at 1100 DEG C 13h formed outer electrode layer 630, obtain 500 by
Electrode 610 in cast is coated on the electrolyte layer 620 of 610 outer surface of electrode in cast and is coated on 620 outer surface of electrolyte layer
The tubular cells unit 600 that constitutes of outer electrode layer 630, the diameter of every root canal type battery unit 600 is 6mm, adjacent two root canal
The centre distance of type battery unit 600 is 8mm.
Embodiment 3
(1) one comprising electrode 610 and inlet chamber 100 in 100 root canal types is obtained using the vacuum gel-casting method of forming
Idiosome is formed, the inner flow passage of electrode 610 is connected to inlet chamber 100 in every root canal type;Wherein, 610 ruler of electrode in 100 root canal types
Very little identical and parallel arrangement, and whole cross section is square, inlet chamber 100 and outlet chamber 300 are located in 100 root canal types
The both ends of electrode 610, and it is vertical with electrode 610 in 100 root canal types;Wherein, electrode 610 is equal in the root canal type of inlet chamber 100 and 100
(content of Ni is 50wt%) to the cermet material for using Ni and yttria-doped ceria to be compounded to form.
(2) it after the integrated molding idiosome obtained to step (1) cleans, is then done naturally in the environment of shady and cool ventilation
It is dry, then preheating is carried out to the integrated molding idiosome after drying, preheating temperature is 1000 DEG C, and the preheating time is
4h。
(3) it is prepared on the outer wall of electrode 610 in the outer surface of inlet chamber 100 and every root canal type using slurry impregnation thick
The doped yttrium zirconia film that degree is 20 μm, is then sintered 4h under 1500 DEG C of high temperature, makes in every root canal type on 610 outer wall of electrode
It forms one layer of electrolyte layer 620 and forms one layer of ceramic barrier layer in the outer surface of inlet chamber 100.
(4) one layer of strontium doping cobalt acid lanthanum is coated in 620 outer surface of electrolyte layer, is then sintered at 1300 DEG C
10h forms outer electrode layer 630, obtain 100 by electrode 610 in cast, be coated on the electrolyte of 610 outer surface of electrode in cast
The tubular cells unit 600 that layer 620 and the outer electrode layer 630 for being coated on 620 outer surface of electrolyte layer are constituted, every tubular cells
The diameter of unit 600 is 8mm, and the centre distance of adjacent two root canals type battery unit 600 is 12mm.
(5) outlet chamber 300 is prepared, 100 and 100 root canal type battery units 600 can be designed in an end face of outlet chamber 300
One-to-one connecting hole 310, welds barrel connector at the connecting hole 310 of outlet chamber 300, and the outer diameter of connector is slightly larger than
Then the connection is inserted into every 600 one end far from inlet chamber 100 of root canal type battery unit by the outer diameter of tubular cells unit 600
Part, then pass through high-temp glue or glass capsulation connection gap.
Embodiment 4
(1) it is obtained using filling forming method comprising inlet chamber 100, electrode 610 and outlet chamber 300 in 100 root canal types
It is integrally formed idiosome, the inner flow passage of electrode 610 is connected to inlet chamber 100 and outlet chamber 300 in every root canal type;Wherein, 100
610 size of electrode is identical in cast and parallel arrangement, and whole cross section is square;Inlet chamber 100 and outlet chamber 300 are distinguished
The both ends of electrode 610 in 100 root canal types, and it is vertical with electrode 610 in 100 root canal types;Wherein, inlet chamber 100 and 100
Electrode 610 and outlet chamber 300 are all made of the cermet material that Ni and yttria-doped ceria are compounded to form (Ni's contain in root canal type
Amount is 50wt%).
(2) it after the integrated molding idiosome obtained to step (1) cleans, is then done naturally in the environment of shady and cool ventilation
It is dry, then preheating is carried out to the integrated molding idiosome after drying, preheating temperature is 800 DEG C, and the preheating time is 5h.
(3) it is prepared on the outer wall of electrode 610 in the outer surface of inlet chamber 100 and every root canal type using slurry impregnation thick
The yttria-doped ceria film that degree is 5 μm, is then sintered 10h under 1200 DEG C of high temperature, makes in every root canal type on 610 outer wall of electrode
It forms one layer of electrolyte layer 620 and forms one layer of ceramic barrier layer in the outer surface of inlet chamber 100.
(4) one layer of strontium doping cobalt acid lanthanum is coated in 620 outer surface of electrolyte layer, is then sintered at 1300 DEG C
10h forms outer electrode layer 630, obtain 100 by electrode 610 in cast, be coated on the electrolyte of 610 outer surface of electrode in cast
The tubular cells unit 600 that layer 620 and the outer electrode layer 630 for being coated on 620 outer surface of electrolyte layer are constituted, every tubular cells
The diameter of unit 600 is 8mm, and the centre distance of adjacent two root canals type battery unit 600 is 12mm.
Embodiment 5
(1) electrode group in 100, two groups of casts of inlet chamber, intermediate air cavity 500 and outlet chamber are established using 3 d modeling software
After 300 Integrated Model, electrode group includes that 50 sizes are identical and electrode 610 in the cast of parallel arrangement in every group of cast,
And every group of entirety cross section is square, intermediate air cavity 500 is located in two groups of casts between electrode group, inlet chamber 100 and outlet
Chamber 300 is located at both ends, and intermediate air cavity 500, inlet chamber 100 and outlet chamber 300 hang down with 610 groups of electrode in two groups of casts
Directly;Then laser photocuring 3D printing technique obtains comprising electrode group, intermediate air cavity 500 in 100, two groups of casts of inlet chamber and goes out
The integrated molding idiosome of air cavity 300 inner flow passage of electrode 610 and inlet chamber 100, intermediate air cavity 500 and goes out in every root canal type
Air cavity 300 is connected to;Wherein, inlet chamber 100, intermediate air cavity 500, in every root canal type electrode 610 and outlet chamber 300 be all made of Ni and
Cermet slurry (content of Ni is 50wt%) printing that the cerium oxide of doped yttrium is compounded to form obtains.
(2) it after the integrated molding idiosome obtained to step (1) cleans, is then done naturally in the environment of shady and cool ventilation
It is dry.
(3) it is prepared on the outer wall of electrode 610 in the outer surface of inlet chamber 100 and every root canal type using electrophoretic deposition thick
The doped yttrium zirconia film that degree is 5 μm, is then sintered 12h under 1200 DEG C of high temperature, makes in every root canal type on 610 outer wall of electrode
It forms one layer of electrolyte layer 620 and forms one layer of ceramic barrier layer in the outer surface of inlet chamber 100.
(4) one layer of strontium doping cobalt acid lanthanum is coated in 620 outer surface of electrolyte layer, is then sintered at 1000 DEG C
15h forms outer electrode layer 630 so that every group of stacks of cells include 50 by electrode 610 in cast, be coated in cast it is electric
The tubular cells that the electrolyte layer 620 of 610 outer surface of pole and the outer electrode layer 630 for being coated on 620 outer surface of electrolyte layer are constituted
The diameter of unit 600, every root canal type battery unit 600 is 8mm, and the centre distance of adjacent two root canals type battery unit 600 is
12mm。
It should be noted that the obtained solid oxide fuel cell stack of embodiment 1 and embodiment 2 is being applied to solid
It before being generated electricity in oxide fuel battery system, need to be heated in reducing atmosphere at 500~800 DEG C, anode will be used as
Outer electrode layer in nickel oxide be reduced to W metal.
The solid oxide fuel cell stack that the embodiment of the present invention 1~5 is prepared is applied to using hydrogen as fuel
It is every in the solid oxide fuel cell stack that the embodiment of the present invention 1~5 is prepared when in solid oxide fuel battery system
The starting open-circuit voltage values of root canal type battery unit are 1.05~1.15V, and the open-circuit voltage values after running 1000h are without being remarkably decreased
(decreasing ratio is less than 5%);And under the same test conditions, (inlet chamber and every root canal type battery unit are using high for the prior art
Warm glue sealing assembly) in the starting open-circuit voltage values of every root canal type battery unit be 0.95~1.0V, the open circuit after running 1000h
Voltage value decreased significantly (decreasing ratio is 20%~26%).
Therefore, the power generation performance for the solid oxide fuel cell stack that the present invention is prepared compares existing skill with stability
The hair for the solid oxide fuel cell stack that art (inlet chamber and every root canal type battery unit are assembled using high-temp glue sealing) obtains
Electrical property and stability significantly improve.
The above description is merely a specific embodiment, but scope of protection of the present invention is not limited thereto, any
Those familiar with the art in the technical scope disclosed by the present invention, can easily think of the change or the replacement, and should all contain
Lid is within protection scope of the present invention.
Claims (10)
1. a kind of preparation process of solid oxide fuel cell stack, it is characterised in that: the solid oxide fuel cell stack
Including inlet chamber and the first stacks of cells connecting with one end face of inlet chamber, first stacks of cells includes several
Root canal type battery unit, the every tubular cells unit include electrode in cast, are coated on electrode outer surface in the cast
Electrolyte layer and be coated on the outer electrode layer of the electrolyte layer outer surface;
The preparation method includes:
(1) integrated molding idiosome is made in electrode in the cast of several tubular cells units and the inlet chamber, made every
The inner flow passage of electrode is connected to the inlet chamber in cast described in root;
(2) one layer of electrolyte layer is coated on the outer wall of electrode in the every cast, then carries out first sintering processing;
(3) after first sintering processing, one layer of outer electrode layer is coated on the electrolyte layer, is carried out second and is sintered
Processing, obtains the integral structure of several root canal type battery units and the inlet chamber.
2. the preparation process of solid oxide fuel cell stack according to claim 1, it is characterised in that: the solid oxygen
Compound fuel cell unit further includes at least one set of second stacks of cells, first stacks of cells and the second battery list
It is connected to by intermediate air cavity between tuple and between the second stacks of cells of two adjacent groups, each second battery unit
Group includes several root canal type battery units, and the every tubular cells unit includes electrode in cast, is coated in the cast
The electrolyte layer of electrode outer surface and the outer electrode layer for being coated on the electrolyte layer outer surface;
Include: in step (1) by the inlet chamber, first stacks of cells several root canal types in electrode, intermediate air cavity
Integrated molding idiosome is made with electrode in several root canal types of at least one set of second stacks of cells.
3. the preparation process of solid oxide fuel cell stack according to claim 1, it is characterised in that: in step (1),
The integrated molding idiosome is prepared by using 3D printing molding, injection forming or vacuum gel-casting forming method.
4. the preparation process of solid oxide fuel cell stack according to claim 1, it is characterised in that: in step (1),
It further include that preheating is carried out to the integrated molding idiosome of acquisition.
5. the preparation process of solid oxide fuel cell stack according to claim 4, it is characterised in that: at the pre-burning
Managing temperature is 600~1000 DEG C, and the preheating time is 4~6h.
6. the preparation process of solid oxide fuel cell stack according to claim 1, it is characterised in that: in step (2),
The first sintering treatment temperature is 1000~1500 DEG C, and the first sintering processing time is 2~18h;
In step (3), second of sintering processes temperature is 900~1300 DEG C, the first sintering processing time is 8~
20h。
7. the preparation process of solid oxide fuel cell stack according to claim 1, it is characterised in that: described in several
The material of electrode is at least one of perovskite composite oxide and spinel oxides or cermet in cast;
The material of the inlet chamber is identical as the material of electrode in the cast.
8. the preparation process of solid oxide fuel cell stack according to claim 1, it is characterised in that: the electrolyte
The material of layer is rare earth ion doped cerium oxide or rare earth ion doped zirconium oxide;The material of the outer electrode layer is Ca-Ti ore type
At least one of composite oxides and spinel oxides or cermet.
9. the preparation process of solid oxide fuel cell stack according to claim 1, it is characterised in that: in step (3),
It further include coating one layer of fine and close ceramic barrier layer in inlet chamber outer surface before carrying out the first sintering processing.
10. the preparation process of solid oxide fuel cell stack according to claim 1, it is characterised in that: the solid
Oxide fuel cell group further includes outlet chamber;Electrode in the cast of several tubular cells units, the inlet chamber and
The outlet chamber is integrally formed.
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