CN110224146A - A kind of online densifying method of fuel-cell electrolyte low temperature - Google Patents
A kind of online densifying method of fuel-cell electrolyte low temperature Download PDFInfo
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- CN110224146A CN110224146A CN201910435557.0A CN201910435557A CN110224146A CN 110224146 A CN110224146 A CN 110224146A CN 201910435557 A CN201910435557 A CN 201910435557A CN 110224146 A CN110224146 A CN 110224146A
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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
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/8647—Inert electrodes with catalytic activity, e.g. for fuel cells consisting of more than one material, e.g. consisting of composites
- H01M4/8652—Inert electrodes with catalytic activity, e.g. for fuel cells consisting of more than one material, e.g. consisting of composites as mixture
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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
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/8663—Selection of inactive substances as ingredients for catalytic active masses, e.g. binders, fillers
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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
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/88—Processes of manufacture
- H01M4/8875—Methods for shaping the electrode into free-standing bodies, like sheets, films or grids, e.g. moulding, hot-pressing, casting without support, extrusion without support
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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
- H01M8/1004—Fuel cells with solid electrolytes characterised by membrane-electrode assemblies [MEA]
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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
- H01M2300/00—Electrolytes
- H01M2300/0017—Non-aqueous electrolytes
- H01M2300/0065—Solid electrolytes
- H01M2300/0068—Solid electrolytes inorganic
- H01M2300/0071—Oxides
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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
- H01M2300/00—Electrolytes
- H01M2300/0088—Composites
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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 invention discloses a kind of online densifying methods of fuel-cell electrolyte low temperature, solid oxide fuel cell electrode (anode/cathode) material powder is mixed in a certain ratio with alkali metal hydroxide or alkali carbonate, is considered as mixed electrode (anode/cathode) material;Then, using the oxide anode material of anode material or above-mentioned mixing anode material or composite anode materials or alkali metal containing element as anode, using cathode material or mixing cathode material or composite cathode material as cathode, fuel cell is assembled into electrolyte.The solid oxide fuel cell is tested under middle low temperature in fuel cell atmosphere, can be obtained the online densification of electrolyte.This method have the advantages that it is easy to operate, low in cost, and can at low temperature (350-600 DEG C) realization.
Description
Technical field
The present invention relates to field of solid oxide fuel, and in particular to a kind of solid-oxide fuel battery electrolyte
The online densifying method of low temperature.
Background technique
Solid oxide fuel cell (SOFC) is a kind of energy conversion technology with high conversion efficiency, can directly by
The chemical energy of storage converts electric energy.Since its energy conversion efficiency is high, applied widely, the reasons such as environmental-friendly, in recent years
SOFC technology is widely paid close attention to by the whole world.
Solid oxide fuel cell mainly consists of three parts, cathode, anode and electrolyte.Electrolyte be located at cathode and
It is most important component in SOFC among anode, it can prevent electronics in inside battery transport, avoid short circuit, allow simultaneously
Transmission of the ion between anode and cathode.Moreover, another critical function of electrolyte be isolation Yin/Yang pole atmosphere, prevent to collaborate with
Gas leakage, so that SOFC performance be made to reach most preferably, it is fine and close enough that this requires electrolyte.Traditional electrolyte densifying method is will
Electrolyte is obtained by high-temperature calcination.Such as traditional samarium doping cerium oxide (SDC) and Yttrium oxide doping zirconium oxide (YSZ) electrolyte
It needs to be sintered at a high temperature of 1300 DEG C or more to reach fine and close.This sintering process not only consumes the energy, but also can break
The two-phase interface of bad electrolyte, to substantially reduce the ion transmission performance of electrolyte.Although by electrolyte powder
Middle addition sintering aid can reduce sintering temperature to a certain extent, but sintering temperature still rests on high temperature, Er Qie electricity
The densification of solution matter needs individual sintering process that could obtain always.
Developing low-temperature solid oxide fuel (400-600 DEG C) is emphasis studied both at home and abroad at present, wherein exploitation and system
Making low temperature and the simple electrolyte densifying method of operating method is one of solution to the problems described above.Because in this operation
In temperature range, cheap material and cost-effective method can use to develop suitable product.Develop solid oxidation at present
Object fuel operate at low temperature and so that it is obtained dense electrolyte method there are mainly two types of, one is reduce electrolyte layer thickness
Degree, makes traditional material, such as YSZ, can adapt to the operating environment of low temperature, this just proposes the preparation process of battery higher
It is required that.Another method is the electrolyte developed at low temperature with high ionic conductivity, for example creates two-phase abundant
Interface is to make full use of interface high ionic conductivity.It is reported that semiconductor strontium titanates (SrTiO3) and tradition SOFC electrolyte YSZ
The very big enhancement effect of ionic conductivity is observed in the heterojunction structure of composition.Zhu etc. is also reported at Sm doped cerium oxide (SDC)
It observed the very big of two-phase granular boundary conductivity with the compound system system of semiconductor material lanthanum-strontium cobalt iron oxide (LSCF)
Enhancing.However, high-temperature sintering process can seriously destroy the high ionic conductivity of the two-phase interface of material.Therefore, seek it is new both
Electrolyte granular interface ion transmission performance can be protected, the method that can reduce preparation temperature again it is particularly significant.
Summary of the invention
Based on the above the deficiencies in the prior art, technical problem solved by the invention is to provide a kind of soild oxide combustion
Expect cell electrolyte low temperature densification method, this method have the advantages that it is easy to operate, low in cost, and can be at low temperature
(350-600 DEG C) realization.
In order to solve the above technical problem, the present invention provides a kind of online densifying method of fuel-cell electrolyte low temperature,
Alkali metal hydroxide or alkali carbonate, the battery of assembling are added in the anode or cathode of solid oxide fuel cell
Obtain the densification of electrolyte online under fuel cell environment.Specific method is as follows:
(1) by solid oxide fuel cell electrode material powder and alkali metal hydroxide or/and alkali carbonate
It by mixing, and is fully ground, obtains mixed electrode material;
(2) with anode of solid oxide fuel cell material or mixing anode material or composite anode materials or alkali metal containing
The oxide anode material of element is as anode, using cathode material or mixing cathode material or composite cathode material as cathode,
Fuel cell is assembled into electrolyte;
(3) fuel cell obtained by step (2) is tested under low temperature in fuel cell atmosphere, can be obtained electrolysis
The online densification of matter.
As a preferred embodiment of the above technical solution, the online densifying method of fuel-cell electrolyte low temperature provided by the invention into
One step includes some or all of following technical characteristic:
As an improvement of the above technical solution, alkali metal hydroxide described in step (1) is in LiOH, NaOH, KOH
It is one or more.
As an improvement of the above technical solution, alkali carbonate described in step (1) is Li2CO3、Na2CO3、
K2CO3、NaHCO3、KHCO3One of or it is a variety of.
As an improvement of the above technical solution, in the step (1), solid oxide fuel cell electrode material powder with
The ratio of the amount of the substance of alkali metal hydroxide or/and alkali carbonate is 1:0.5~1:3.
As an improvement of the above technical solution, step (3) the fuel cell atmosphere are as follows: cathode be passed through gas be air or
Oxygen, it is hydrogen or steam-laden hydrogen that anode, which is passed through gas,.
As an improvement of the above technical solution, step (3) low temperature is 350-600 DEG C, and temperature should be higher than that in material
The fusing point of hydroxide corresponding to contained alkali metal element.
As an improvement of the above technical solution, at least one of in the anode and cathode for assembling obtained fuel cell
Contain one of alkali metal elements such as Li, Na, K in the material of pole;And when anode is without alkali metal elements such as Li, Na, K, yin
Pole is necessary for the mixing cathode material of alkali metal containing hydroxide
Compared with prior art, technical solution of the present invention has the following beneficial effects:
The present invention is different from previous method, and this method in electrode material by adding alkali metal hydroxide or alkali gold
Belong to carbonate, densify its electrolyte layer.Electrolyte needs not move through special sintering process to reach densification, but
It is obtained by the online reaction of battery, so that the manufacturing process of battery greatly simplifies, while battery needs not move through high temperature sintering,
Not only facilitate the two-phase interface of protection composite electrolyte, but also the production temperature of battery is greatly reduced.The advantages of invention is
It is easy to operate, low temperature operability is strong, low in cost.
The above description is only an overview of the technical scheme of the present invention, in order to better understand the technical means of the present invention,
And it can be implemented in accordance with the contents of the specification, and in order to allow above and other objects, features and advantages of the invention can
It is clearer and more comprehensible, below in conjunction with preferred embodiment, detailed description are as follows.
Detailed description of the invention
In order to illustrate the technical solution of the embodiments of the present invention more clearly, the attached drawing to embodiment is simply situated between below
It continues.
Fig. 1 is that the battery that the embodiment of the present invention 1 is prepared by powder pressing method is electric through the cross-sectional scans after line densifies
Mirror figure (is followed successively by anode, electrolyte, cathode layer) from top to bottom;
Fig. 2 be the online low temperature densification of the embodiment of the present invention 1 before electrolyte layer scanning electron microscope (SEM) photograph;
Fig. 3 is the scanning electron microscope (SEM) photograph of the electrolyte layer after the online low temperature densification of the embodiment of the present invention 1;
Fig. 4 be the online low temperature densification of the embodiment of the present invention 2 before electrolyte layer scanning electron microscope (SEM) photograph;
Fig. 5 is the scanning electron microscope (SEM) photograph of the electrolyte layer after the online low temperature densification of the embodiment of the present invention 2;
Fig. 6 is the scanning electron microscope (SEM) photograph of the electrolyte layer after the online low temperature densification of the embodiment of the present invention 6.
Specific embodiment
The following detailed description of a specific embodiment of the invention, as part of this specification, by embodiment come
Illustrate that the principle of the present invention, other aspects of the present invention, feature and its advantage will become apparent by the detailed description.
Embodiment 1:
With nickel cobalt aluminium oxidate for lithium (NCAL) for anode and cathode, Ce0.8Sm0.2O1.9With La0.6Sr0.4Co0.2Fe0.8O3
(SDC+LSCF) composite material passes through powder by the way that above-mentioned powder to be sequentially placed into powder compressing machine grinding tool as electrolyte
Last pressed disc method is assembled into fuel cell.Then battery is placed at 550 DEG C, and each leads into oxygen and hydrogen in battery cathode and anode
Gas can be obtained the online densification of electrolyte after a period of time.
Fig. 1 be the battery that is prepared by powder pressing method of embodiment 1 through after line densifies cross-sectional scans electron microscope (from
Anode, electrolyte, cathode layer are followed successively by under), fuel cell structure is complete as we can see from the figure, anode, electrolyte, yin
Pole interface is clear.Fig. 2 be the online low temperature densification of embodiment 1 before electrolyte layer scanning electron microscope (SEM) photograph, this figure illustrates densification
There are apparent gap and hole, electrolyte in cellular before change between electrolyte layer particle.Fig. 3 is the online low temperature of embodiment 1
The scanning electron microscope (SEM) photograph of electrolyte layer after densification, it can be found that without obvious hole in the electrolyte layer after line densification
Hole is in densifie state.The comparative illustration of Fig. 2 and Fig. 3 this method can achieve the purpose that electrolyte densifies online.
Embodiment 2:
By SOFC electrode material NiO powder and alkali metal hydroxide LiOHH2O, it is uniform according to the mass ratio of the material 1:3
Mixing, and be fully ground, obtain mixed electrode material Ni O+LiOHH2O.Using NiO as anode, Ce0.8Sm0.2O1.9(SDC) it is
Electrolyte, mixing cathode material NiO+LiOHH2O passes through powder pressing method assembling fuel cell as cathode.It then will be electric
Pond is placed at 550 DEG C, is each led into air and hydrogen in battery cathode and anode, be can be obtained the online of electrolyte after a period of time
Densification.
Fig. 4 be the online low temperature densification of embodiment 2 before electrolyte layer scanning electron microscope (SEM) photograph;Fig. 5 is that embodiment 2 is online
The scanning electron microscope (SEM) photograph of electrolyte layer after low temperature densification.As we can see from the figure densify before SDC electrolyte granular it
Between have an apparent hole, and after densifying between particle without obvious hole, be in densifie state.The comparative illustration of Fig. 4 and Fig. 5
This method can achieve the purpose that electrolyte densifies online.
Embodiment 3:
By SOFC electrode material NiO powder and alkali metal hydroxide LiOHH2O and alkali carbonate Li2CO3, press
It according to the mass ratio of the material 1:1.4:0.6, uniformly mixes, and is fully ground, obtain mixed electrode material Ni O+LiOH+Li2CO3.With this
Mixed electrode material Ni O+LiOH+Li2CO3For anode, LiNiO2For cathode, with Ce0.8Sm0.2O1.9With
La0.6Sr0.4Co0.2Fe0.8O3(SDC+LSCF) composite material is assembled into fuel electricity as electrolyte, by powder pressing method
Pond.Then battery is placed at 430 DEG C, and each leads into air and hydrogen containing 3% vapor in battery cathode and anode, one section
It can be obtained the online densification of electrolyte after time.
Embodiment 4:
Nickel cobalt aluminium oxidate for lithium (NCAL) powder is tabletted by pressed powder, as anode;Then curtain coating is utilized
Method prepares yttria-stabilized zirconia (YSZ) film as electrolyte in NCAL on piece, and dries and remove glue.By above-mentioned sample and yin
Pole material La0.6Sr0.4Co0.2Fe0.8O3(LSCF) it is assembled into fuel cell.Then battery is placed at 500 DEG C, and in battery
Cathode and anode each leads into oxygen and hydrogen, can be obtained the online densification of electrolyte after a period of time.
Embodiment 5:
By SOFC anode material NiO powder and Li2CO3It according to the mass ratio of the material 1:0.5, uniformly mixes, and is fully ground,
Obtain mixed electrode material Ni O+Li2CO3.Sofc cathode material lanthanum-strontium-manganese oxide (LSM) and NaOH are pressed into the mass ratio of the material 1:
0.5 mixing, obtains mixed electrode material LSM+NaOH.With mixed electrode material Ni O+Li2CO3For anode,
BaZr0.1Ce0.7Y0.2O3(BZCY) be electrolyte, mixed electrode material LSM+NaOH is as cathode, is assembled by powder pressing method
Fuel cell.Then battery is placed at 600 DEG C, air and hydrogen is each led into battery cathode and anode, after a period of time
Obtain the online densification of electrolyte.
Embodiment 6:
SOFC anode material NiO powder is uniformly mixed with KOH according to the mass ratio of the material 1:1 respectively, and is fully ground, is obtained
To mixed electrode material Ni O+KOH.Be electrolyte using the mixed electrode material Ni O+KOH as anode, SDC, nickel cobalt aluminium it is lithium
Object (NCAL) is cathode, passes through powder pressing method assembling fuel cell.Then battery is placed at 500 DEG C, in battery cathode and anode
Air and the hydrogen containing 3% vapor are each led into, can be obtained the online densification of electrolyte after a period of time.
Fig. 6 is the scanning electron microscope (SEM) photograph of the electrolyte layer after the online low temperature densification of the embodiment of the present invention 6.The densification it
Preceding electrolyte layer scanning electron microscope (SEM) photograph is similar to Fig. 4, is in cellular.Do not have in electrolyte layer after densifying as can see from Figure 6
There is obvious hole, is in densifie state, shows that this method can achieve the purpose that electrolyte densifies online.
Embodiment 7:
With lithium-containing oxides anode material LiCoO2It is electrolyte, La for anode, SDC0.6Sr0.4Co0.2Fe0.8O3(LSCF)
As cathode, pass through powder pressing method assembling fuel cell.Then battery is placed at 480 DEG C, is led to respectively in battery cathode and anode
Enter air and hydrogen, can be obtained the online densification of electrolyte after a period of time.
Embodiment 8:
By SOFC anode material NiO powder and NaHCO3It uniformly mixes, and is fully ground according to the mass ratio of the material 1:1, obtain
To mixed electrode material Ni O+NaHCO3.With mixed electrode material Ni O+NaHCO3It is electrolyte, LiNiCuZn for anode, SDC
Oxide (LNCZ) is used as cathode, passes through powder pressing method assembling fuel cell.Then battery is placed at 350 DEG C, in battery
Cathode and anode each leads into air and the hydrogen containing 3% vapor, can be obtained the online densification of electrolyte after a period of time.
The bound of each raw material cited by the present invention and each raw material of the present invention, section value and technological parameter
Bound, the section value of (such as temperature, time) can realize the present invention, embodiment numerous to list herein.
The above is a preferred embodiment of the present invention, cannot limit the right model of the present invention with this certainly
It encloses, it is noted that for those skilled in the art, without departing from the principle of the present invention, may be used also
To make several improvement and variation, these, which improve and change, is also considered as protection scope of the present invention.
Claims (7)
1. a kind of online densifying method of fuel-cell electrolyte low temperature, which is characterized in that comprise the following steps:
(1) by solid oxide fuel cell electrode material powder and alkali metal hydroxide or/and alkali carbonate by mixed
It closes, and is fully ground, obtain mixed electrode material;
(2) with anode of solid oxide fuel cell material or mixing anode material or composite anode materials or alkali metal containing element
Oxide anode material as anode, using cathode material or mixing cathode material or composite cathode material as cathode, with electricity
Solution material is assembled into fuel cell;
(3) fuel cell obtained by step (2) is tested under low temperature in fuel cell atmosphere, can be obtained electrolyte
Online densification.
2. the online densifying method of fuel-cell electrolyte low temperature as described in claim 1, it is characterised in that: in step (1)
The alkali metal hydroxide is one of LiOH, NaOH, KOH or a variety of.
3. the online densifying method of fuel-cell electrolyte low temperature as described in claim 1, it is characterised in that: in step (1)
The alkali carbonate is Li2CO3、Na2CO3、K2CO3、NaHCO3、KHCO3One of or it is a variety of.
4. the online densifying method of fuel-cell electrolyte low temperature as described in claim 1, it is characterised in that: the step
(1) in, solid oxide fuel cell electrode material powder and the substance of alkali metal hydroxide or/and alkali carbonate
The ratio of amount is 1:0.5~1:3.
5. the online densifying method of fuel-cell electrolyte low temperature as described in claim 1, it is characterised in that: step (3) institute
State fuel cell atmosphere are as follows: it is air or oxygen that cathode, which is passed through gas, and it is hydrogen or steam-laden hydrogen that anode, which is passed through gas,
Gas.
6. the online densifying method of fuel-cell electrolyte low temperature as described in claim 1, it is characterised in that: step (3) institute
Stating low temperature is 350-600 DEG C, and temperature should be higher than that the fusing point of hydroxide corresponding to contained alkali metal element in material.
7. the online densifying method of fuel-cell electrolyte low temperature as described in claim 1-6, it is characterised in that: the assembling
Contain one in the alkali metal elements such as Li, Na, K at least one of pole material in the anode and cathode of obtained fuel cell
Kind;And when anode is without alkali metal elements such as Li, Na, K, cathode is necessary for the mixing cathode material of alkali metal containing hydroxide
Material.
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