CN107799854A - A kind of high-temperature solid sodium ion air oxygen compound energy-storage battery - Google Patents
A kind of high-temperature solid sodium ion air oxygen compound energy-storage battery Download PDFInfo
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- CN107799854A CN107799854A CN201610807881.7A CN201610807881A CN107799854A CN 107799854 A CN107799854 A CN 107799854A CN 201610807881 A CN201610807881 A CN 201610807881A CN 107799854 A CN107799854 A CN 107799854A
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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
- H01M12/00—Hybrid cells; Manufacture thereof
- H01M12/08—Hybrid cells; Manufacture thereof composed of a half-cell of a fuel-cell type and a half-cell of the secondary-cell type
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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
- H01M8/12—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte
- H01M8/124—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the process of manufacturing or by the material of the electrolyte
- H01M8/1246—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the process of manufacturing or by the material of the electrolyte the electrolyte consisting of oxides
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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
Abstract
The present invention provides a kind of novel energy storage cell for integrating metal-air battery, conventional energy-storage battery and high-temperature solid fuel cell --- high-temperature solid sodium ion air oxygen compound energy-storage battery.The cell positive material includes Ni metal or C etc., and negative material selects the cathode material and Na of high-temperature solid fuel cell2O2Mixture, electrolyte selects solid-state β " Al2O3.The battery combination metal-air battery and common metal energy-storage battery principle, and high-temperature fuel cell electrode material feature, there is the advantages of cost is low.
Description
Technical field
The present invention relates to energy-storage battery technical field, more particularly to a kind of high-temperature solid sodium ion-air oxygen compound energy storage
Battery.
Background technology
Energy-storage battery is ubiquitous, is widely used in the every field such as extensive energy storage and power storage
Demand and prospect.In all energy-storage batteries, electrochemical storage is the one kind being most widely used, and wherein with metal member
Plain lithium and sodium it is most commonly used, typical represent is lithium ion battery and sodium-ion battery.However, either lithium-ion electric
, safety risks all the time be present in pond or sodium-ion battery.Therefore, solid ionic battery, such as all-solid lithium-ion battery and
Ceramic ZEBRA (Zero Emission Battery Research Activities) battery produces therewith.
However, either common metal ion battery, or solid metallic ion battery, its operating process, which be unable to do without, takes out
Vacuum mode, prepared such as under glove box.Moreover, common metal ion battery is due to metal excessively active in itself,
The danger such as high-temp combustion, blast also be present.
The content of the invention
The present invention combines metal-air battery and common metal energy-storage battery principle, and high-temperature fuel cell electrode material
Feature, propose a kind of novel energy-storing for integrating metal-air battery, conventional energy-storage battery and high-temperature solid fuel cell
Battery, the cell negative electrode material select the cathode material and Na of high-temperature solid fuel cell2O2Mixture, the high-temperature solid
The cathode material of fuel cell includes perovskite oxide, such as LSCF, LSM, BSCF, PSCF；Cell positive material is selected more
Hole is porous metals simple substance (such as Cu, Ni, Fe etc.) or C etc., is collected for storing Na and electronics；The electrolyte of battery
From β "-Al2O3.Under conditions of charging, the Na in negative pole2O2Resolve into metal sodium ion and oxygen, the electrolysis of Na ion permeables
Matter enters in positive pole, forms SODIUM METAL；In discharge process, the simple substance Na that is stored in positive pole loses electronics and becomes Na ions, Na from
Son forms Na through the oxygen that electrolyte enters in negative pole, with air2O2, and electronics is provided to external circuit, produce electric energy.This is specially
In profit, the novel energy storage cell is referred to as high-temperature solid sodium-air oxide energy-storage battery.
In order to improve the reserves of Na in positive pole, increase the ionic conductivity of positive pole, cell positive material also include β "-
Al2O3.Porous metals simple substance positive pole and C and β "-Al2O3Volume ratio can be adjusted according to sodium ion electrical conductivity, adjustable range
Preferably 1：10~7：10, more preferably 3：10~6：10, more preferably 35：100~45：100.
In order to improve the catalytic activity of oxygen in air, the preferred addition VPO catalysts material in negative pole, such as SOFC
The VPO catalysts of perovskite oxide, or the VPO catalysts such as Pt, Au, oxonium ion is reduced to catalytic oxygen, so as to sodium from
Son combines to form the oxide of sodium, while ensures there is higher electronic conductivity under high temperature air atmosphere.
Present invention also offers a kind of structure of above-mentioned high-temperature solid sodium ion energy-storage battery, as shown in figure 1, being negative pole branch
The hollow layer structure of support.Cathode-supported layer, dielectric substrate and anode layer through-thickness are stacked on top of one another, and dielectric substrate includes
First dielectric substrate and the second dielectric substrate, the first dielectric substrate are located at the upper surface of cathode-supported layer, the second dielectric substrate position
In the lower surface of cathode-supported layer；Anode layer includes the first anode layer and the second anode layer, and the first anode layer is positioned at the first electrolysis
The upper surface of matter layer, the second anode layer are located at the lower surface of the second dielectric substrate；Cathode-supported layer sets hollow bore, the hole
There is openend in the side of cathode-supported layer.
Preferably, centered on cathode-supported layer, the first dielectric substrate is symmetric with the second dielectric substrate, i.e.,
The shape of one dielectric substrate and the second dielectric substrate, thickness etc. are completely the same, to reduce stress.
In order to improve battery strength, while it is easy to make, the present invention preferably improves the thickness of cathode-supported layer, the thickness
Preferably more than 1mm, more preferably more than 5mm, more preferably more than 10mm below 25mm are big with specific reference to cell area
Small decision.Because cathode-supported layer is thicker, so as to be manufactured using conventional method, therefore preparation technology simplifies, and prepares cost
Reduce.After cathode-supported thickness degree improves, in order to keep the laser propagation effect of fuel, cathode-supported layer material preferably uses hole
The higher cathode material used for high-temperature fuel cell of rate, such as perovskite oxide LSM, LSCF, BSCF, PSCF etc., porosity is excellent
Elect more than 50% as.
In the hollow layer structure of this cathode-supported, described anode layer thickness is preferably 1 μm~10 μm；Described
Dielectric substrate thinner thickness is advisable, preferably 1~100 μm, more preferably 5~10 μm.
The preparation method of the hollow layer structure of above-mentioned cathode-supported may include steps of：
(1) the cathode-supported layer with pore space structure is prepared
Using cathode-supported layer material as raw material, high temperature volatile substances of the landfill with certain size are as pore-creating wherein
Agent, by being molded, sintering, turning into formed body, wherein pore creating material volatilizees, and obtains the anode-supported layer with pore space structure, and
The hole has openend in the side of anode-supported layer；
Described pore former material is unlimited, including carbon-point, graphite, the carbon material etc. of CNT and other shapes.
Described forming method is unlimited, including the methods of hot pressing, curtain coating.
(2) dielectric substrate is prepared in cathode-supported layer upper and lower surface
The first dielectric substrate is prepared using the methods of coating, dipping, silk-screen printing in cathode-supported layer upper surface, in negative pole
Supporting layer lower surface prepares the second dielectric substrate using the methods of coating, dipping, silk-screen printing, obtains including first after sintered
The half-cell of dielectric substrate and the second dielectric substrate；
(3) anode layer is prepared in electrolyte layer surface
The first anode layer is prepared using the methods of coating, dipping, silk-screen printing in the upper surface of the first dielectric substrate；
The lower surface of two dielectric substrates prepares the second anode layer using the methods of coating, dipping, silk-screen printing；Negative pole is obtained after sintered
The hollow stratiform battery of support.
In described step (3), sintering temperature is preferably no greater than melting or the volatilization temperature of porous metals or C, avoids it
Melting is reunited or disappeared.
Present invention also offers the structure of another above-mentioned high-temperature solid sodium ion-air oxygen compound energy-storage battery, such as Fig. 2
It is shown, it is the layer structure of electrolyte-supported.That is, dielectric substrate is intermediate layer, and anode layer is located at electrolyte respectively with negative electrode layer
The upper and lower surface of layer.
Preferably, described dielectric substrate thickness is 0.1~5mm.
The preparation method of above-mentioned electrolyte supported structure can be：Electrolyte is pressed into by flat board branch using the method for tabletting
Support body or hollow structure, obtain dielectric substrate；Negative electrode layer is prepared in the dielectric substrate upper surface, in the dielectric substrate lower surface system
Standby anode layer；Then, it is sintered, obtains structure of whole solid state battery.
Described anode layer preparation method is unlimited, including the methods of use coating, dipping, silk-screen printing, it is preferred to use apply
It is prepared by the mode of covering.
Described negative electrode layer preparation method is unlimited, including the methods of use coating, dipping, silk-screen printing, it is preferred to use apply
It is prepared by the mode of covering.
Described sintering temperature is preferably no greater than melting or the volatilization temperature of porous metals or C, avoid its melting reunite or
Disappear.
In summary, the present invention utilizes metal-air battery and common metal energy-storage battery principle, with reference to high-temperature fuel electricity
Pond electrode material feature, a kind of energy-storage battery of new structure is obtained, is had the advantages that：
(1) battery uses all solid state form, and energy storage negative material selects the cathode material of high-temperature solid fuel cell, Gu
Body electrolyte is non-volatile, general non-combustible, therefore cost is low, has excellent security；
(2) electrolyte selects solid-state β "-Al in battery2O3, relative to porous gel electrolyte and immersion liquid electricity
The porous septum of liquid is solved, solid electrolyte is fine and close, and has higher intensity and hardness, can effectively prevent metallic dendrite
Pierce through, therefore improve the security of battery, while also make it possible use of the metal as positive pole.
(3) the manufacture whole process of battery is not necessarily required to the protection of inert atmosphere, reduces battery to a certain extent
Manufacturing cost.
Brief description of the drawings
Fig. 1 is the hollow flat board of the cathode-supported of high-temperature solid sodium ion of the present invention-air oxygen compound energy-storage battery
Structure；
Fig. 2 is the flat board knot of the electrolyte-supported of high-temperature solid sodium ion of the present invention-air oxygen compound energy-storage battery
Structure.
Embodiment
The invention will be further described for embodiment below in conjunction with the accompanying drawings, but present disclosure is not limited solely to down
The embodiment in face.
Reference in Fig. 1 is：Cathode-supported layer 1, the first dielectric substrate 21, the second dielectric substrate 22, the first positive pole
The 31, second anode layer 32 of layer, hole 4.
Reference in Fig. 2 is：Support dielectric substrate 5, anode layer 6, negative electrode layer 7.
Embodiment 1：
In the present embodiment, the structural representation of high-temperature solid sodium ion-air oxygen compound energy-storage battery is as shown in figure 1, be
The hollow layer structure of cathode-supported, it is stacked on top of one another by cathode-supported layer 1, dielectric substrate and anode layer through-thickness.Electricity
Solution matter layer includes the first dielectric substrate 21 and the second dielectric substrate 22, and the first dielectric substrate 21 is located at the following table of cathode-supported layer
Face, the second dielectric substrate 22 are located at the upper surface of cathode-supported layer.Anode layer includes the upper anode layer of first anode layer 31 and second
32, the first anode layer 31 is located at the lower surface of the first dielectric substrate 1, and the second anode layer 32 is located at the upper table of the second dielectric substrate 1
Face.C anode-supporteds layer 1 sets several holes 4, and the hole has openend in the side of anode-supported layer 1.
Centered on cathode-supported layer 1, the first dielectric substrate 21 is symmetric with the second dielectric substrate 22.That is, first
Dielectric substrate is identical with the material of the second dielectric substrate, and shape is identical, and thickness is identical, in 1 μm~10 μ ms.
Centered on cathode-supported layer 1, the first anode layer 31 is symmetric with the second anode layer 32.That is, the first positive pole
Layer 31 is identical with the material of the second anode layer 32, and shape is identical, and thickness is identical, in 10 μm~100 μ ms.
Cathode material perovskite oxide LSCF, LSM of the material selection high-temperature solid fuel cell of cathode-supported layer 1,
One or more kinds of combinations in BSCF, PSCF etc., the catalyst material of the various oxygen such as sodium metal oxide and Pt, Au
Material.The thickness of cathode-supported layer 1 is 2~10mm.
First dielectric substrate 21 is identical with the material of the second dielectric substrate 22, from β "-Al2O3。
First anode layer 31 is identical with the material of the second anode layer 32, from porous metals Cu, Fe, Ni or C etc. and β "-
Al2O3And other trace elements.
The preparation side of the high-temperature solid sodium ion of the hollow layer structure of above-mentioned anode-supported-air oxygen compound energy-storage battery
Method comprises the following steps：
(1) it is, raw material is hot-forming or directly dry-pressing formed using negative material as raw material by carbon-point landfill in the feed.
Then sinter, sintering temperature is 800~1300 DEG C, obtains the cathode-supported layer 1 with described hole structure；
(2) by the coating of the slurry of electrolyte layer, impregnate or be screen printed onto the upper and lower surface of cathode-supported layer 1,
Then sinter, obtain the half-cell for including the first dielectric substrate 21 and the second dielectric substrate 22；
(3) by the coating of the slurry of positive pole layer material, the upper surface for impregnating or being screen printed onto the first dielectric substrate 21 with
The lower surface of second dielectric substrate 22, is then sintered, and obtains the first anode layer 31 and the second anode layer 32.
Under conditions of charging, the Na in cathode-supported layer 12O2Metal sodium ion and oxygen are resolved into, metal sodium ion is saturating
Cross the first dielectric substrate 21 or the second dielectric substrate 22 enters the first anode layer 31 and stored in the second anode layer 32, form sodium list
Matter.Under discharge scenario, the metal simple-substance Na in the first anode layer 31 and the second anode layer 32 forms Na ions, and through first
The dielectric substrate 22 of dielectric substrate 21 or second enters in cathode-supported layer 1, and sodium metal oxide is formed with the oxygen in air, and
Electronics is provided to external circuit, produces electric energy.Because dielectric substrate and anode layer are located at the both sides up and down of cathode-supported layer, therefore produce
Raw stress is effectively offset, and stress significantly reduces.
Embodiment 2：
In the present embodiment, the structural representation of high-temperature solid sodium ion-air oxygen compound energy-storage battery is as shown in Fig. 2 be
The layer structure of electrolyte-supported.That is, dielectric substrate 5 is intermediate layer, and anode layer 6 is with negative electrode layer 7 respectively positioned at dielectric substrate 5
Upper and lower surface.
The thickness of dielectric substrate 5 is 0.1~5mm.
Solid electrolyte β "-Al in the material selection common metal energy-storage battery of dielectric substrate 52O3。
Material selection porous metals such as Fe, Cu, Ni or C of anode layer 6 etc. and β "-Al2O3And other trace elements.
Cathode material perovskite oxide LSCF, LSM of the material selection high-temperature solid fuel cell of negative electrode layer 7, BSCF,
One or more kinds of combinations in PSCF etc., the catalyst material of the various oxygen such as sodium metal oxide and Pt, Au with
Na2O2Mixing.
The preparation side of the high-temperature solid sodium ion of the layer structure of above-mentioned electrolyte-supported-air oxygen compound storage energy-storage battery
Method is：Electrolyte is pressed into by flat support body or hollow structure using the method for tabletting, obtains dielectric substrate；In the electrolyte
Layer upper surface prepares negative electrode layer using coating, dipping or the method for silk-screen printing, the dielectric substrate lower surface using coating,
Dipping or the method for silk-screen printing prepare anode layer；Then, it is sintered, obtains structure of whole solid state battery.
Under conditions of charging, the sodium metal oxide in negative electrode layer resolves into metal sodium ion and oxygen, metallic sodium from
Son enters anode layer through dielectric substrate, forms SODIUM METAL.Under discharge scenario, metal simple-substance Na in anode layer formed Na from
Son, Na ion permeables dielectric substrate enter in negative electrode layer, form sodium metal oxide with the oxygen in air, and external circuit is carried
Supplied for electronic, produce electric energy.
Technical scheme is described in detail embodiment described above, it should be understood that it is described above only
For the specific embodiment of the present invention, it is not intended to limit the invention, all any modifications made in the spirit of the present invention,
Supplement or similar fashion replacement etc., should be included in the scope of the protection.
Claims (10)
1. a kind of high-temperature solid sodium ion-air oxygen compound energy-storage battery, it is characterized in that：Positive electrode includes Cu or C, negative pole material
Cathode material and Na of the material from high-temperature solid fuel cell2O2Mixture, electrolyte selects solid-state β "-Al2O3；
Under conditions of charging, the Na in negative pole2O2Metal sodium ion and oxygen are resolved into, metallic sodium ion permeable electrolyte enters
Enter positive pole, form sodium simple substance；Under discharge scenario, the metal simple-substance Na stored in positive pole forms Na ions, Na ion permeables electricity
Solve matter to enter in negative pole, sodium metal oxide is formed with the oxygen in air, and electronics is provided to external circuit, produce electric energy.
2. high-temperature solid sodium ion as claimed in claim 1-air oxygen compound energy-storage battery, it is characterized in that：The negative pole material
Expect for perovskite oxide and Na2O2；
Described perovskite oxide preferably includes one or more kinds of combinations in LSCF, LSM, BSCF, PSCF etc..
3. high-temperature solid sodium ion as claimed in claim 1-air oxygen compound energy-storage battery, it is characterized in that：Described is porous
Metal simple-substance is Cu, Fe or Ni.
4. high-temperature solid sodium ion as claimed in claim 1-air oxygen compound energy-storage battery, it is characterized in that：Described negative pole
In also include the catalyst of oxygen；
Preferably, the catalyst of described oxygen is one or two kinds of in Pt, Au.
5. high-temperature solid sodium ion-air oxygen compound energy-storage battery as described in any claim in Claims 1-4, its
It is characterized in：For the layer structure of electrolyte-supported, dielectric substrate is intermediate layer, and anode layer is located at dielectric substrate respectively with negative electrode layer
Upper and lower surface.
6. high-temperature solid sodium ion as claimed in claim 5-air oxygen compound energy-storage battery, it is characterized in that：Using tabletting
Electrolyte is pressed into flat support body or hollow structure by method, obtains dielectric substrate；Prepared in the dielectric substrate upper surface negative
Pole layer, anode layer is prepared in the dielectric substrate lower surface；Obtain structure of whole solid state battery；
Preferably, described dielectric substrate thickness is 0.1~5mm.
7. high-temperature solid sodium ion-air oxygen compound energy-storage battery as described in any claim in Claims 1-4, its
It is characterized in：For the hollow layer structure of cathode-supported；Cathode-supported layer, dielectric substrate and anode layer through-thickness levels
Folded, dielectric substrate includes the first dielectric substrate and the second dielectric substrate, and the first dielectric substrate is located at the upper surface of cathode-supported layer,
Second dielectric substrate is located at the lower surface of cathode-supported layer；Anode layer includes the first anode layer and the second anode layer, the first positive pole
Layer is located at the upper surface of the first dielectric substrate, and the second anode layer is located at the lower surface of the second dielectric substrate；Cathode-supported layer is set
Hollow bore, the hole have openend in the side of cathode-supported layer；
Preferably, centered on cathode-supported layer, the first dielectric substrate is symmetric with the second dielectric substrate.
8. high-temperature solid sodium ion as claimed in claim 7-air oxygen compound energy-storage battery, it is characterized in that：Cathode-supported layer
Thickness be more than 1mm, preferably more than 5mm, more preferably more than 10mm below 25mm.
9. high-temperature solid sodium ion as claimed in claim 7-air oxygen compound energy-storage battery, it is characterized in that：Described positive pole
Thickness degree is 1 μm~10 μm；
Described dielectric substrate thickness is preferably 1~100 μm, more preferably 5~10 μm.
10. high-temperature solid sodium ion as claimed in claim 7-air oxygen compound energy-storage battery, it is characterized in that：Preparation method bag
Include following steps：
(1) the cathode-supported layer with pore space structure is prepared
Using cathode-supported layer material as raw material, high temperature volatile substances of the landfill with certain size are as pore creating material wherein,
By being molded, sintering, turn into formed body, wherein pore creating material volatilizees, and obtains the cathode-supported layer with pore space structure, and the hole
Hole has openend in the side of cathode-supported layer；
Described pore former material is preferably carbon-point, graphite, or CNT；
Described forming method is preferably hot pressing or curtain coating；
(2) dielectric substrate is prepared in cathode-supported layer upper and lower surface
The first dielectric substrate is prepared using the methods of coating, dipping, silk-screen printing in cathode-supported layer upper surface, in cathode-supported
Layer lower surface prepares the second dielectric substrate using the methods of coating, dipping, silk-screen printing, obtains including the first electrolysis after sintered
The half-cell of matter layer and the second dielectric substrate；
(3) anode layer is prepared in electrolyte layer surface
The anode layer of metallic sodium first is used in the upper surface of the first dielectric substrate；The hollow stratiform of cathode-supported is obtained after sintered
Battery.
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| CN201610807881.7A CN107799854A (en) | 2016-09-05 | 2016-09-05 | A kind of high-temperature solid sodium ion air oxygen compound energy-storage battery |
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| CN201610807881.7A CN107799854A (en) | 2016-09-05 | 2016-09-05 | A kind of high-temperature solid sodium ion air oxygen compound energy-storage battery |
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN110289387A (en) * | 2019-05-17 | 2019-09-27 | 宁波大学 | A kind of all solid state neutral zinc-air battery |
| CN113725445A (en) * | 2021-08-17 | 2021-11-30 | 中国科学院上海微***与信息技术研究所 | High-efficiency all-solid-state sodium-oxygen-water battery |
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| CN1479404A (en) * | 2003-06-18 | 2004-03-03 | 北京双威富能科技有限公司 | Fast actuating metal air cell |
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