CN106207238A - A kind of molten salts compound intermediate temperature solid oxide fuel cell electrolyte - Google Patents
A kind of molten salts compound intermediate temperature solid oxide fuel cell electrolyte Download PDFInfo
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- CN106207238A CN106207238A CN201610868165.XA CN201610868165A CN106207238A CN 106207238 A CN106207238 A CN 106207238A CN 201610868165 A CN201610868165 A CN 201610868165A CN 106207238 A CN106207238 A CN 106207238A
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- fuel cell
- electrolyte
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- oxide fuel
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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
- H01M8/14—Fuel cells with fused electrolytes
- H01M8/144—Fuel cells with fused electrolytes characterised by the electrolyte material
-
- 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
- H01M8/14—Fuel cells with fused electrolytes
- H01M8/144—Fuel cells with fused electrolytes characterised by the electrolyte material
- H01M8/145—Fuel cells with fused electrolytes characterised by the electrolyte material comprising carbonates
-
- 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 molten salts compound intermediate temperature solid oxide fuel cell electrolyte, belong to fuel-cell electrolyte technical field.The present invention uses Ce (NO3)3·6H2O、Gd2O3、Li2CO3And Na2B4O7·10H2O is primary raw material, a kind of molten salts compound intermediate temperature solid oxide fuel cell electrolyte is prepared through sol-gel combustion method mechanical mixing, the relative density of this electrolyte reaches 99.9%, its in air atmosphere 700 DEG C time ionic conductivity reach 0.022S/cm, can be as the electrolyte of intermediate temperature solid oxide fuel cell.
Description
Technical field
The invention belongs to fuel-cell electrolyte technical field, be specifically related to a kind of compound middle temperature solid oxygen of molten salts
Compound fuel-cell electrolyte.
Background technology
The whole world demand expanding day to the energy, and gradually pay attention to the problem of ecological deterioration, traditional energy system is by nothing
Method adaptation is social, and to efficient, cleaning, the requirement of safe, economic energy system, the development of the energy will face huge challenge, because of
This fuel cell will become 21st century important energy source device.SOFC (SOFC) is anti-by electrochemistry
Answer process to make the chemical energy in fossil class A fuel A be converted into electric energy, owing to not burning and mechanical process, be greatly enhanced
Energy conversion efficiency, it is to avoid or decrease the generation of the pollutant such as toxic gas and dust；The operating temperature of SOFC is 500
DEG C ~ 1000 DEG C, its side-product is heat and the steam of high-quality, and in the case of cogeneration, capacity usage ratio is up to 80%
Left and right, is the energy resource system of a kind of clean and effective.
The operating temperature of the SOFC being commercially employed at present is general all at 1000 DEG C, works at such high temperatures
SOFC is made to there is many problems: electrode densification, metallic interconnection materials require high and battery hermetization bad, big with this
Add greatly the cost of SOFC, limit its business development.For SOFC commercialized development, it is necessary for dropping its operating temperature
Low, and electrolyte is as the part of core the most in SOFC, if electrolyte can obtain good at relatively low temperatures
Performance, then can obtain the preferable SOFC of middle temperature.Traditional electrolyte has not been suitable under middle temperature environment working, so
Novel electrolytic material must be developed.The electrolyte of the present invention can obtain high electrical conductivity under middle temperature working condition,
To meet the most required electrolyte that can be used in middle low temperature SOFC.
Summary of the invention
Present invention aims to prior art not enough, it is provided that a kind of compound middle temperature solid-oxide fuel of molten salts
Cell electrolyte.Using sol-gel combustion method-mechanical mixing to prepare novel mole percent is 80% Gd0.2Ce0.8O1.9-
10%Li2CO3-10%Na2B4O7(GLN) electrolyte, reaches through 1000 DEG C of its relative densities of composite electrolyte sheet being incubated 3h
99.9%；In air atmosphere 700 DEG C time ionic conductivity reach 0.022S/cm, higher than preparing with identical sol-gel combustion method
Common electrolyte Ce0.8Gd0.2O1.9Electrical conductivity 0.015S/cm.
For achieving the above object, the present invention adopts the following technical scheme that
A kind of molten salts compound intermediate temperature solid oxide fuel cell electrolyte, its composition is calculated as by mole percent: 80%
Gd0.2Ce0.8O1.9-10%Li2CO3-10%Na2B4O7(GLN).Its preparation method specifically includes following steps:
(1) Gd is prepared0.2Ce0.8O1.9；
(2) 8:1:1 weighs Gd respectively in molar ratio0.2Ce0.8O1.9、Li2CO3And Na2B4O7·10H2O, by three's machinery spheroidal graphite
3h so that it is mixing is abundant and uniform, then by mixed-powder after 600 ± 10 DEG C of pre-burnings 0.5 ± 0.1 hour, then at 800 ± 10
DEG C sintering 3 ± 0.1 hours, it is thus achieved that 80% Gd0.2Ce0.8O1.9-10%Li2CO3-10%Na2B4O7(GLN) powder；
(3) by step (two) gained 80% Gd0.2Ce0.8O1.9-10%Li2CO3-10%Na2B4O7Powder is put in mould,
Under the pressure of 300MPa, make a diameter of 13 ± 0.1mm, thickness is the disk of 0.5 ± 0.1mm, by disk with 3 DEG C per minute
Speed is heated to 1000 ± 10 DEG C, is incubated 3 ± 0.1 hours, obtains the compound intermediate temperature solid oxide fuel cell of molten salts
Electrolyte disk.
Gd described in step ()0.2Ce0.8O1.9Preparation method, specifically comprise the following steps that
1) Gd is pressed0.2Ce0.8O1.9Stoichiometric proportion weighs Ce (NO3)3·6H2O、Gd2O3, and press metal cation and citric acid
Mol ratio is that 1:1.5 weighs citric acid；
2) with the dust technology that mass concentration is 10%-15% by Gd2O3It is dissolved as nitrate；
3) by Ce (NO3)3·6H2O and citric acid add distilled water and dissolve；
4) by step 2) and step 3) gained solution pour into successively in Gadolinium trinitrate solution, and in solution, be added dropwise over mass concentration
For the ammonia of 15%-20%, to regulate solution ph for 7；
5) mixed solution that step 4) obtains is put into agitator is heated to 45 DEG C, be then maintained at continuous stirring at 45 DEG C,
And in whipping process, add ammonia, make the pH value of solution be maintained at 7, until forming gel；
6) gel is moved in evaporating dish, be placed on electric furnace heating, until occurring self-propagating combustion to form fluffy oxidate powder
End；
7) gained oxide powder is heated to 800 ± 10 DEG C, is incubated 3 ± 0.1 hours, then natural cooling, formed
Gd0.2Ce0.8O1.9Powder.
The beneficial effects of the present invention is: what the present invention prepared consolidate melts mixed type electrolyte, not only possesses solid electrolyte
Do not reveal the advantages such as pollution-free, be also equipped with the high performance feature of molten state electrolyte, and sufficiently lower electrolyte
Operating temperature, operating temperature has high electrical conductivity in the range of middle temperature (500 DEG C 700 DEG C), in air atmosphere 700 DEG C time
Ionic conductivity is up to 0.022S/cm, higher than common electrolyte Ce prepared with identical sol-gel combustion method0.8Gd0.2O1.9's
Electrical conductivity 0.015S/cm.
Detailed description of the invention
Below in conjunction with specific embodiment, the present invention will be further described, but the present invention is not limited only to these embodiments.
Embodiment 1
(1) Gd is prepared0.2Ce0.8O1.9:
1) Gd is pressed0.2Ce0.8O1.9Stoichiometric proportion weighs 346.376 grams of Ce (NO3)3·6H2O, 36.25 grams of Gd2O3, and press metal
Cation is that 1:1.5 weighs citric acid 315.21 grams with the mol ratio of citric acid；
2) with the dust technology that mass concentration is 10% by Gd2O3It is dissolved as nitrate；
3) by Ce (NO3)3·6H2O and citric acid add distilled water and dissolve；
4) by step 2) and step 3) gained solution pour into successively in Gadolinium trinitrate solution, and in solution, be added dropwise over mass concentration
It is the ammonia of 15%, to regulate solution ph for 7；
5) mixed solution that step 4) obtains is put into agitator is heated to 45 DEG C, be then maintained at continuous stirring at 45 DEG C,
And in whipping process, add ammonia, make the pH value of solution be maintained at 7, until forming gel；
6) gel is moved in evaporating dish, be placed on electric furnace heating, until occurring self-propagating combustion to form fluffy oxidate powder
End；
7) gained oxide powder is heated to 790 DEG C, is incubated 3.1 hours, then natural cooling, form Gd0.2Ce0.8O1.9Powder
End；
(2) 8:1:1 weighs 139.152 grams of Gd respectively in molar ratio0.2Ce0.8O1.9, 7.389 grams of Li2CO3With 3.814 grams
Na2B4O7·10H2O, by three machinery spheroidal graphite 3h so that it is mixing is abundant and uniform, then by mixed-powder in 590 DEG C of pre-burnings
After 0.6 hour, sinter 3.1 hours then at 790, it is thus achieved that 80% Gd0.2Ce0.8O1.9-10%Li2CO3-10%Na2B4O7(GLN) powder；
(3) by step (two) gained 80% Gd0.2Ce0.8O1.9-10%Li2CO3-10%Na2B4O7Powder is put in mould,
Under the pressure of 300MPa, make a diameter of 13 ± 0.1mm, thickness is the disk of 0.5 ± 0.1mm, by disk with 3 DEG C per minute
Speed is heated to 1000 ± 10 DEG C, is incubated 3 ± 0.1 hours, obtains the compound intermediate temperature solid oxide fuel cell of molten salts
Electrolyte disk.
Embodiment 2
(1) Gd is prepared0.2Ce0.8O1.9:
1) Gd is pressed0.2Ce0.8O1.9Stoichiometric proportion weighs 346.376 grams of Ce (NO3)3·6H2O, 36.25 grams of Gd2O3, and press metal
Cation is that 1:1.5 weighs citric acid 315.21 grams with the mol ratio of citric acid；
2) with the dust technology that mass concentration is 15% by Gd2O3It is dissolved as nitrate；
3) by Ce (NO3)3·6H2O and citric acid add distilled water and dissolve；
4) by step 2) and step 3) gained solution pour into successively in Gadolinium trinitrate solution, and in solution, be added dropwise over mass concentration
It is the ammonia of 20%, to regulate solution ph for 7；
5) mixed solution that step 4) obtains is put into agitator is heated to 45 DEG C, be then maintained at continuous stirring at 45 DEG C,
And in whipping process, add ammonia, make the pH value of solution be maintained at 7, until forming gel；
6) gel is moved in evaporating dish, be placed on electric furnace heating, until occurring self-propagating combustion to form fluffy oxidate powder
End；
7) gained oxide powder is heated to 810 DEG C, is incubated 2.9 hours, then natural cooling, form Gd0.2Ce0.8O1.9Powder
End；
(2) 8:1:1 weighs 139.152 grams of Gd respectively in molar ratio0.2Ce0.8O1.9, 7.389 grams of Li2CO3With 3.814 grams
Na2B4O7·10H2O, by three machinery spheroidal graphite 3h so that it is mixing is abundant and uniform, then by mixed-powder in 610 DEG C of pre-burnings
After 0.4 hour, sinter 2.9 hours then at 810 DEG C, it is thus achieved that 80% Gd0.2Ce0.8O1.9-10%Li2CO3-10%Na2B4O7(GLN) powder
End；
(3) by step (two) gained 80% Gd0.2Ce0.8O1.9-10%Li2CO3-10%Na2B4O7Powder is put in mould,
Under the pressure of 300MPa, make a diameter of 13 ± 0.1mm, thickness is the disk of 0.5 ± 0.1mm, by disk with 3 DEG C per minute
Speed is heated to 1000 ± 10 DEG C, is incubated 3 ± 0.1 hours, obtains the compound intermediate temperature solid oxide fuel cell of molten salts
Electrolyte disk.
Embodiment 3
(1) Gd is prepared0.2Ce0.8O1.9:
1) Gd is pressed0.2Ce0.8O1.9Stoichiometric proportion weighs 346.376 grams of Ce (NO3)3·6H2O, 36.25 grams of Gd2O3, and press metal
Cation is that 1:1.5 weighs citric acid 315.21 grams with the mol ratio of citric acid；
2) with the dust technology that mass concentration is 12% by Gd2O3It is dissolved as nitrate；
3) by Ce (NO3)3·6H2O and citric acid add distilled water and dissolve；
4) by step 2) and step 3) gained solution pour into successively in Gadolinium trinitrate solution, and in solution, be added dropwise over mass concentration
It is the ammonia of 18%, to regulate solution ph for 7；
5) mixed solution that step 4) obtains is put into agitator is heated to 45 DEG C, be then maintained at continuous stirring at 45 DEG C,
And in whipping process, add ammonia, make the pH value of solution be maintained at 7, until forming gel；
6) gel is moved in evaporating dish, be placed on electric furnace heating, until occurring self-propagating combustion to form fluffy oxidate powder
End；
7) gained oxide powder is heated to 800 DEG C, is incubated 3 hours, then natural cooling, form Gd0.2Ce0.8O1.9Powder；
(2) 8:1:1 weighs 139.152 grams of Gd respectively in molar ratio0.2Ce0.8O1.9, 7.389 grams of Li2CO3With 3.814 grams
Na2B4O7·10H2O, by three machinery spheroidal graphite 3h so that it is mixing is abundant and uniform, then by mixed-powder in 600 DEG C of pre-burnings
After 0.5 hour, sinter 3 hours then at 800 DEG C, it is thus achieved that 80% Gd0.2Ce0.8O1.9-10%Li2CO3-10%Na2B4O7(GLN) powder；
(3) by step (two) gained 80% Gd0.2Ce0.8O1.9-10%Li2CO3-10%Na2B4O7Powder is put in mould,
Under the pressure of 300MPa, make a diameter of 13 ± 0.1mm, thickness is the disk of 0.5 ± 0.1mm, by disk with 3 DEG C per minute
Speed is heated to 1000 ± 10 DEG C, is incubated 3 ± 0.1 hours, obtains the compound intermediate temperature solid oxide fuel cell of molten salts
Electrolyte disk.
The method of testing of electrical conductivity:
The conductance for alternating current of electrolyte uses two-terminal method to measure.Gained after sintering 3 ± 0.1 hours at 1000 ± 10 DEG C
80% Gd0.2Ce0.8O1.9-10%Li2CO3-10%Na2B4O7(GLN) silver slurry is coated on electrolyte disk two sides, then in 450 DEG C of roastings
Silver electrode is prepared after 2h.With filamentary silver, the silver electrode at two ends is connected with alternating current impedance instrument.The alternating current impedance instrument used is Shanghai occasion
Instrument Ltd. of China model is CHI660E electrochemical workstation, applies current potential 10mV, measures frequency range 1kHz-20MHz,
The temperature measuring conductance for alternating current is 500-800 DEG C, measures in air atmosphere.Electrical conductivity uses equation below to calculate:
In formula, σ is electrolytic conductivity, S/cm；
H is electrolyte sheet thickness, unit cm；
R is bath resistance, unit Ω；
S is electrolyte sheet cross-sectional area, unit cm2。
Result shows, the molten salts compound intermediate temperature solid oxide fuel cell electrolyte that the present invention prepares, 700
DEG C time ionic conductivity be 0.022S/cm, when 800 DEG C, ionic conductivity reaches 0.026S/cm, and this shows that it can be as electrolysis
Matter is used for intermediate temperature solid oxide fuel cell.
The foregoing is only presently preferred embodiments of the present invention, all impartial changes done according to scope of the present invention patent with
Modify, all should belong to the covering scope of the present invention.
Claims (3)
1. a molten salts compound intermediate temperature solid oxide fuel cell electrolyte, it is characterised in that: described electrolyte
Composition is calculated as by mole percent: 80%Gd0.2Ce0.8O1.9-10%Li2CO3-10%Na2B4O7。
2. the side preparing molten salts as claimed in claim 1 compound intermediate temperature solid oxide fuel cell electrolyte
Method, it is characterised in that: specifically include following steps:
(1) Gd is prepared0.2Ce0.8O1.9；
(2) 8:1:1 weighs Gd respectively in molar ratio0.2Ce0.8O1.9、Li2CO3And Na2B4O7·10H2O, by three's machinery spheroidal graphite
3h so that it is mixing is abundant and uniform, then by mixed-powder after 600 ± 10 DEG C of pre-burnings 0.5 ± 0.1 hour, then at 800 ± 10
DEG C sintering 3 ± 0.1 hours, it is thus achieved that 80% Gd0.2Ce0.8O1.9-10%Li2CO3-10%Na2B4O7Powder；
(3) by step (two) gained 80% Gd0.2Ce0.8O1.9-10%Li2CO3-10%Na2B4O7Powder is put in mould,
Under the pressure of 300MPa, make a diameter of 13 ± 0.1mm, thickness is the disk of 0.5 ± 0.1mm, by disk with 3 DEG C per minute
Speed is heated to 1000 ± 10 DEG C, is incubated 3 ± 0.1 hours, obtains the compound intermediate temperature solid oxide fuel cell of molten salts
Electrolyte disk.
The preparation side of molten salts the most according to claim 2 compound intermediate temperature solid oxide fuel cell electrolyte
Method, it is characterised in that: the Gd described in step ()0.2Ce0.8O1.9Preparation method, specifically comprise the following steps that
1) Gd is pressed0.2Ce0.8O1.9Stoichiometric proportion weighs Ce (NO3)3·6H2O、Gd2O3, and press metal cation and citric acid
Mol ratio is that 1:1.5 weighs citric acid；
2) with the dust technology that mass concentration is 10%-15% by Gd2O3It is dissolved as nitrate；
3) by Ce (NO3)3·6H2O and citric acid add distilled water and dissolve；
4) by step 2) and step 3) gained solution pour into successively in Gadolinium trinitrate solution, and in solution, be added dropwise over mass concentration
For the ammonia of 15%-20%, to regulate solution ph for 7；
5) mixed solution that step 4) obtains is put into agitator is heated to 45 DEG C, be then maintained at continuous stirring at 45 DEG C,
And in whipping process, add ammonia, make the pH value of solution be maintained at 7, until forming gel；
6) gel is moved in evaporating dish, be placed on electric furnace heating, until occurring self-propagating combustion to form fluffy oxidate powder
End；
7) gained oxide powder is heated to 800 ± 10 DEG C, is incubated 3 ± 0.1 hours, then natural cooling, formed
Gd0.2Ce0.8O1.9Powder.
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN110257848A (en) * | 2019-06-10 | 2019-09-20 | 武汉大学 | Middle low-temperature oxidation methane is the melten salt electriochemistry method of hydrogen and carbon monoxide |
| CN110474036A (en) * | 2019-08-29 | 2019-11-19 | 桑顿新能源科技(长沙)有限公司 | Anode material of lithium battery and preparation method thereof, lithium battery anode, lithium battery and power supply unit |
| CN113782799A (en) * | 2021-10-14 | 2021-12-10 | 北京思伟特新能源科技有限公司 | CGO/ESB double-electrolyte-layer solid oxide electrolytic cell |
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|---|---|---|---|---|
| CN1269613A (en) * | 2000-02-16 | 2000-10-11 | 刘向荣 | Composite ceramic material for middle-temperature oxide fuel cell |
| CN104852070A (en) * | 2015-06-02 | 2015-08-19 | 福州大学 | Solid oxide fuel cell electrolyte as well as preparation method and application thereof |
| CN105655618A (en) * | 2016-01-08 | 2016-06-08 | 福州大学 | Solid-melt hybrid medium-temperature solid oxide fuel cell electrolyte |
-
2016
- 2016-09-30 CN CN201610868165.XA patent/CN106207238A/en active Pending
Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1269613A (en) * | 2000-02-16 | 2000-10-11 | 刘向荣 | Composite ceramic material for middle-temperature oxide fuel cell |
| CN104852070A (en) * | 2015-06-02 | 2015-08-19 | 福州大学 | Solid oxide fuel cell electrolyte as well as preparation method and application thereof |
| CN105655618A (en) * | 2016-01-08 | 2016-06-08 | 福州大学 | Solid-melt hybrid medium-temperature solid oxide fuel cell electrolyte |
Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN110257848A (en) * | 2019-06-10 | 2019-09-20 | 武汉大学 | Middle low-temperature oxidation methane is the melten salt electriochemistry method of hydrogen and carbon monoxide |
| CN110474036A (en) * | 2019-08-29 | 2019-11-19 | 桑顿新能源科技(长沙)有限公司 | Anode material of lithium battery and preparation method thereof, lithium battery anode, lithium battery and power supply unit |
| CN113782799A (en) * | 2021-10-14 | 2021-12-10 | 北京思伟特新能源科技有限公司 | CGO/ESB double-electrolyte-layer solid oxide electrolytic cell |
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