CN101304093A - Low temperature solid-oxide fuel battery three-in-one component MEA and preparation thereof - Google Patents

Low temperature solid-oxide fuel battery three-in-one component MEA and preparation thereof Download PDF

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CN101304093A
CN101304093A CNA2007100112609A CN200710011260A CN101304093A CN 101304093 A CN101304093 A CN 101304093A CN A2007100112609 A CNA2007100112609 A CN A2007100112609A CN 200710011260 A CN200710011260 A CN 200710011260A CN 101304093 A CN101304093 A CN 101304093A
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electrolyte
transition zone
preparation
negative electrode
mea
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CN101304093B (en
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程谟杰
杨敏
董永来
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Dalian Institute of Chemical Physics of CAS
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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
    • 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 three-in-one component MEA of a low temperature solid oxide fuel cell and a preparation thereof, which comprises an anode substrate, an electrolyte diaphragm layer and a cathode, wherein, a perovskite-type oxide transition layer is arranged between the electrolyte diaphragm layer and the cathode. Under the same condition, the performance of the low temperature solid oxide fuel cell prepared by using the method can be increased by more than 30 percent compared with the cell that has no diaphragm layer added.

Description

A kind of low temperature solid-oxide fuel battery three-in-one component MEA and preparation thereof
Technical field
The present invention relates to field of solid oxide fuel, is a kind of high-performance low-temperature solid oxide fuel cell with the perovskite composite oxide transition layer structure (working temperature 500-650 ℃) three-in-one component MEA and preparation method thereof specifically.
Background technology
Solid Oxide Fuel Cell is the energy conversion device that chemical energy is directly changed into electric energy, adopt structure of whole solid state, characteristics with generating efficiency height, applied range are desirable dispersion generatings and concentrate power station technology, also can be applied to vehicle accessory power supply, compact power etc.In order to reduce manufacturing cost, improve reliability, shorten start-up time, the operating temperature of Solid Oxide Fuel Cell is reduced to the emphasis that 500-650 ℃ low-temperature solid oxide fuel cell becomes domestic and international research and development.But present employed low-temperature cathode material is as Ba xSr 1-xCo yFe 1-yO 3(BSCF) (0＜x＜1,0＜y＜1), Sm xSr 1-xCoO 3(SSC) (0＜x＜1) etc., its sintering activity is higher, and under negative electrode sintering temperature usually (1100-1200 ℃), very easily densified sintering product and reduce the porosity of negative electrode hinders the diffusion transmission and the electrical catalyze reduction activity of oxygen.Can keep certain porosity though reduce its sintering temperature, it is firm to cause negative electrode to combine with electrolyte simultaneously, very easily peels off; Interface resistance between negative electrode and the electrolyte increases.The low-temperature solid oxide fuel cell of 20 microns electrolyte thickness that present cell preparation technology obtains, its Ohmic resistance reaches 0.2 Ω cm 2-0.45 Ω cm 2, therefore influence the power output of battery to a great extent far above the theoretical value of electrolyte Ohmic resistance.Under the low-temperature operation condition, the interface resistance between electrolyte and the negative electrode has become one of principal element that influences the low-temperature solid oxide fuel cell performance.
Summary of the invention
In order to solve in the low-temperature solid oxide fuel cell the bigger problem of interface resistance between the electrolyte and negative electrode, the object of the present invention is to provide a kind of low-temperature solid oxide fuel cell with the perovskite composite oxide transition layer structure and preparation method thereof, by between electrolyte and negative electrode, introducing the transition zone that one deck is made of perovskite Composite Oxides Materials, promote effective contact the between electrolyte and the negative electrode, reduce the interface resistance between electrolyte/negative electrode, thereby effectively improve the power output of battery.
For reaching above purpose, the technical solution used in the present invention is:
A kind of low-temperature solid oxide fuel cell (working temperature 500-650 ℃) three-in-one component MEA comprises anode substrate, and electrolyte membrance layer and negative electrode are provided with the perovskite composite oxide transition zone between electrolyte membrance layer and negative electrode; Promptly a side that contacts with negative electrode at dielectric film adds the transition zone that one deck perovskite Composite Oxides Materials constitutes, and by material, thickness and the sintering temperature of regulating this transition zone, promotes effective contact the between electrolyte and the negative electrode, reduces interface resistance.
Described perovskite composite oxide is
(Ln 1-xA x) 1-yMn yO 3 ± δ, wherein Ln=La, Nd or Pr, A=Sr or Ca, 0＜x＜1,0＜y≤1,0≤δ＜1;
Ln 1-xSr xFe 1-yCo yO 3 ± δ, wherein Ln=La, Sm, Nd, Gd or Dy, 0＜x＜1,0＜y≤1,0≤δ＜1;
Ba xSr 1-xCo yFe 1-yO 3(BSCF), 0＜x＜1,0＜y＜1 wherein;
Or La 1-xSr xGa 1-yMg yO 3 ± δ, a kind of formation in 0＜x＜1,0＜y＜1,0＜δ＜1 wherein.
Described transition region thickness is controlled between 20 nanometers-5 micron, is preferably 30 nanometers-2 micron.
The manufacturing materials of described anode can be metal composite ceramal, and wherein metallic catalyst is Ni, Co, Cu, Rh, Fe, Pt, Pd, Mo and/or Ti; Oxide is Sm xCe 1-xO 2(SDC), Gd xCe 1-xO 2(GDC), Y xCe 1-xO 2(YDC), La xCe 1-xO 2(LDC), Y 2O 3Stable ZrO 2(YSZ) and/or Sc 2O 3Stable ZrO 2(ScSZ), 0＜x＜1 wherein; Its thickness can be 300 microns-1 millimeter;
The electrolyte membrance layer is Sm 2O 3, Gd 2O 3, Y 2O 3CeO Deng doped with rare-earth oxide 2Base electrolyte, it is in CeO 2Doping in the base is molar content 5-50%, and its synthetic method can adopt coprecipitation, hydrothermal synthesis method, citric acid method, firing method and glycine method; Method preparations such as the membrane layer that perovskite Composite Oxides Materials constitutes can adopt dry pressing, scrapes embrane method, silk screen print method, coating process, The tape casting, vapour deposition process, plasma spraying method, magnetron sputtering, its thickness is at the 10-60 micron;
Negative electrode can be made of or the composite cathode be made up of cathode material and electrolyte constitutes pure cathode material, and wherein, the weight percent content of cathode material is＞50%; Described cathode material is Ba xSr 1-xCo yFe 1-yO 3(BSCF) or Sm xSr 1-xCoO 3(SSC), 0＜x＜1,0＜y＜1 wherein, its thickness can be the 10-70 micron.
The preparation of three-in-one component MEA: can adopt conventional inoranic membrane preparation method to prepare anode substrate, electrolyte membrance layer and the negative electrode of MEA, adopt conventional inoranic membrane preparation method between electrolyte membrance layer and negative electrode, to introduce the perovskite composite oxide transition zone simultaneously, the perovskite composite oxide transition zone can be fine and close, it also can be porous, but its preparation temperature is lower than fine and close electrolyte membrance layer, general low 100-500 ℃, the sintering temperature of perovskite composite oxide transition zone is 1000-1400 ℃; The inoranic membrane preparation method of described routine is dry pressing, scrape embrane method, silk screen print method, coating process, The tape casting, vapour deposition process, plasma spraying or magnetron sputtering method.
Concrete as: prepare the anode assembly by common technology; The perovskite composite oxide buffer layer material of particle diameter in 2 nanometers to 0.1 micron evenly mixed with binding agent, be made into slurry, by The tape casting, silk screen print method, coating process it is prepared a side that contacts with negative electrode at electrolyte, or the perovskite composite oxide buffer layer material is prepared a side that contacts with negative electrode at electrolyte by methods such as vapour deposition process, plasma spraying, magnetron sputterings with it.The THICKNESS CONTROL of transition zone is between 20 nanometers-5 micron, and sintering temperature is controlled at 1000-1400 ℃, prepares negative electrode then on transition zone.By the low-temperature solid oxide fuel cell of this method preparation, but battery performance that do not add interlayer more the same than other conditions can improve more than 30%.
Excellent results of the present invention is:
By between low-temperature electrolytes and low-temperature cathode, introducing the surface texture that transition zone that one deck is made of perovskite Composite Oxides Materials improves electrolyte membrance, this transition zone was both combined closely with electrolyte, can embed again in the negative electrode, can promote contacting of electrolyte and negative electrode.
1. the preparation technology of low-temperature solid oxide fuel cell of the present invention is simple, can adopt multiple masking technique.As: dry pressing, scrape embrane method, silk screen print method, coating process, The tape casting, vapour deposition process, plasma spraying or magnetron sputtering method.
2. adopt the Solid Oxide Fuel Cell of the present invention's preparation, can effectively reduce the interface resistance of battery under the low-temperature operation condition, improve battery efficiency.The present invention introduces perovskite composite oxide function transition zone between electrolyte and negative electrode, and the after baking by functional layer, promote effective contact the between electrolyte and the negative electrode, reduce the interface resistance between electrolyte/negative electrode, improve the contact strength between electrolyte/negative electrode, thereby effectively improve the power output of battery.
3. the present invention can be used for the Solid Oxide Fuel Cell of multiple configurations such as plate, cast.That described three-in-one component MEA can be used on is plate, in the Solid Oxide Fuel Cell of cast and other various configurations.
4. the present invention is applicable to multiple low-temperature solid oxide fuel cell application, as compact power, decentralized power s etc.
Description of drawings
Accompanying drawing 1 is the structural representation of the anode support type low-temperature solid oxide fuel cell of band perovskite composite oxide transition zone.
Embodiment
Embodiment 1
With LSM is the plate low-temperature solid oxide fuel cell of transition zone
Be illustrated in figure 1 as the structural representation of the anode support type low-temperature solid oxide fuel cell of band perovskite composite oxide transition zone, comprise anode substrate 1, cerium base electrolyte membrane layer 2, perovskite composite oxide transition zone 3 and negative electrode 4.It is two-in-one to prepare NiO-GDC/GDC by dry pressing, and wherein the GDC electrolyte adopts glycine method synthetic, and two-in-one 1420 ℃ were burnt altogether 4 hours, and obtained the anode assembly.Prepare the LSM transition zone that thickness is 500 nanometers by The tape casting in GDC electrolyte one side, dry, be lower than the roasting temperature 2 hours that burns 120 ℃ in electrolyte, obtain the LSM transition zone of porous.
Adopt coating process to prepare the BSCF-GDC composite cathode, wherein BSCF content 70%, 950 ℃ of roastings 2 hours.
With hydrogen is fuel gas, and air is an oxidant, 500-600 ℃ of test battery performance.Maximum power density reaches 0.392Wcm in the time of 500 ℃ -2, more the same than other conditions but battery performance that do not add transition zone improves 37.6%; Ohmic resistance is 0.276 Ω cm -2, more the same than other conditions but battery that do not add transition zone reduces by 33%.
Embodiment 2
With LSGM is the plate low-temperature solid oxide fuel cell of transition zone
It is two-in-one to prepare NiO-SDC/SDC by The tape casting, and wherein the SDC electrolyte adopts citric acid method synthetic, two-in-onely burns altogether 4 hours at 1450 ℃, obtains the anode assembly.Preparing thickness by The tape casting in SDC electrolyte one side is 0.75 micron LSGM transition zone, dries, and is being lower than the roasting temperature 2 hours that burns 200 ℃ in electrolyte, obtains the LSGM transition zone of porous.
Adopt silk screen print method to prepare the BSCF-SDC composite cathode, wherein BSCF content 70%, 950 ℃ of roastings 2 hours.
With hydrogen is fuel gas, and oxygen is oxidant, 500-600 ℃ of test battery performance.Maximum power density reaches 0.91Wcm in the time of 600 ℃ -2, more the same than other conditions but battery performance that do not add transition zone improves 58.5%.
Embodiment 3
With LSCF is the plate low-temperature solid oxide fuel cell of transition zone
To prepare plate NiO-GDC/GDC two-in-one and 1500 ℃ of roastings by rolling embrane method, adopting spraying process to prepare thickness in electrolyte one side is 500 nanometer LSCF transition zones, wherein GDC, LSCF material adopt the citric acid method preparation, being lower than the roasting temperature 1 hour that burns 200 ℃ in electrolyte, obtain all fine and close anode assembly of electrolyte and transition zone.
Adopt silk screen print method to prepare the BSCF-GDC composite cathode, wherein BSCF content 70%, 1000 ℃ of roastings 2 hours.
With hydrogen is fuel gas, and air is an oxidant, 500-600 ℃ of test battery performance.Maximum power density reaches 0.3Wcm in the time of 500 ℃ -2, more the same than other conditions but battery performance that do not add transition zone improves 31.2%.
Embodiment 4
With LSC is the plate low-temperature solid oxide fuel cell of transition zone
Press down at certain pressure and to make plate NiO-YDC anode, adopt The tape casting at its surface preparation YDC dielectric substrate, and burnt altogether 4 hours at 1450 ℃, wherein YDC adopts coprecipitation synthetic.At the LSC transition zone that YDC one side that bakes adopts sputtering method to prepare, thickness is 1 micron.
Adopt coating process to prepare the BSCF negative electrode, wherein BSCF content 100%, 1000 ℃ of roastings 2 hours.
With hydrogen is fuel gas, and air is an oxidant, 500-600 ℃ of test battery performance.Maximum power density reaches 0.95Wcm in the time of 600 ℃ -2, more the same than other conditions but battery performance that do not add transition zone improves 41.6%.
Embodiment 5
With BSCF is the cast low-temperature solid oxide fuel cell of transition zone
Adopt the method for extrusion molding to prepare NiO-GDC cast anode, adopt spraying process load one deck GDC dielectric substrate on anode, prepare plate-load dielectric film NiO-GDC/GDC at 1450 ℃ of co-sinterings, wherein dielectric film thickness is 20 microns.Then, surface sputtering one deck BSCF layer of GDC electrolyte membrance at room temperature, thickness is 200 nanometers.
Adopt silk screen print method to prepare the SSC negative electrode, wherein SSC content 100%, 1000 ℃ of roastings 2 hours.
With hydrogen is fuel gas, and air is an oxidant, 500-600 ℃ of test battery performance.Maximum power density reaches 0.5Wcm in the time of 600 ℃ -2, more the same than other conditions but battery performance that do not add transition zone improves 30.6%.

Claims (8)

1. low temperature solid-oxide fuel battery three-in-one component MEA, comprise anode substrate (1), electrolyte membrance layer (2) and negative electrode (4) is characterized in that: be provided with perovskite composite oxide transition zone (3) between electrolyte membrance layer (2) and negative electrode.
2. according to the described three-in-one component MEA of claim 1, it is characterized in that: described perovskite composite oxide is
(Ln 1-xA x) 1-yMn yO 3 ± δ, wherein Ln=La, Nd or Pr, A=Sr or Ca, 0＜x＜1,0＜y≤1,0≤δ＜1;
Ln 1-xSr xFe 1-yCo yO 3 ± δ, wherein Ln=La, Sm, Nd, Gd or Dy, 0＜x＜1,0＜y≤1,0≤δ＜1;
Ba xSr 1-xCo yFe 1-yO 3, 0＜x＜1,0＜y＜1 wherein;
Or La 1-xSr xGa 1-yMg yO 3 ± δ, a kind of formation in 0＜x＜1,0＜y＜1,0＜δ＜1 wherein.
3. according to the described three-in-one component MEA of claim 1, it is characterized in that: described transition zone (3) THICKNESS CONTROL is between 20 nanometers-5 micron.
4. according to the described three-in-one component MEA of claim 1, it is characterized in that: described transition zone (3) optimum thickness is controlled between 30 nanometers-2 micron.
5. according to the described three-in-one component MEA of claim 1, it is characterized in that: the preparation material of described anode is a metal composite ceramal, and wherein metallic catalyst is Ni, Co, Cu, Rh, Fe, Pt, Pd, Mo and/or Ti; Oxide is Sm xCe 1-xO 2, Gd xCe 1-xO 2, Y xCe 1-xO 2, La xCe 1-xO 2, Y 2O 3Stable ZrO 2And/or Sc 2O 3Stable ZrO 2, 0＜x＜1 wherein; Its thickness can be 200 microns-5 millimeters;
The electrolyte membrance layer is the CeO of doped with rare-earth oxide 2Base electrolyte, thickness are 10～100 microns;
Negative electrode can be made of or the composite cathode be made up of cathode material and electrolyte constitutes pure cathode material, and wherein, the weight percent content of cathode material is＞50%; Cathode material is Ba xSr 1-xCo yFe 1-yO 3Or Sm xSr 1-xCoO 3, 0＜x＜1,0＜y＜1 wherein, its thickness can be 10～70 microns.
6. according to the described three-in-one component MEA of claim 5, it is characterized in that: described rare earth oxide is Sm 2O 3, Gd 2O 3Or Y 2O 3, it is in CeO 2Doping in the base is a molar content 5～50%.
7. the preparation method of the described three-in-one component MEA of claim 1, it is characterized in that: can adopt conventional inoranic membrane preparation method to prepare the anode substrate of MEA, electrolyte membrance layer and negative electrode, adopt conventional inoranic membrane preparation method between electrolyte membrance layer and negative electrode, to introduce the perovskite composite oxide transition zone simultaneously, the perovskite composite oxide transition zone can be fine and close, it also can be porous, but its preparation temperature is lower than fine and close electrolyte membrance layer, general low 100-500 ℃, the sintering temperature of perovskite composite oxide transition zone is 1000-1400 ℃.
8. according to the preparation method of the described three-in-one component MEA of claim 7, it is characterized in that: the inoranic membrane preparation method of described routine is dry pressing, scrapes embrane method, silk screen print method, coating process, The tape casting, vapour deposition process, plasma spraying or magnetron sputtering method.
CN2007100112609A 2007-05-11 2007-05-11 Low temperature solid-oxide fuel battery three-in-one component MEA and preparation thereof Expired - Fee Related CN101304093B (en)

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CN103107342A (en) * 2013-01-22 2013-05-15 哈尔滨工业大学 One-dimensional nanofiber SSC (Sm(1-x)SrxCoO(3-delta)) cathode material, preparation method of the cathode material, composite cathode using cathode material and preparation method of composite cathode
CN103367763A (en) * 2013-07-11 2013-10-23 黑龙江大学 Method for preparing solid oxide fuel cell nanometer thin film cathode by magnetron sputtering method
CN104157893A (en) * 2013-05-13 2014-11-19 中国科学院大连化学物理研究所 Low temperature solid oxide fuel cell supported by porous metal and preparation method thereof
CN105734607A (en) * 2014-12-08 2016-07-06 中国科学院大连化学物理研究所 High temperature solid oxide electrolytic bath with double-layer composite interlayer
CN106876725A (en) * 2015-12-12 2017-06-20 中国科学院大连化学物理研究所 A kind of method for reducing cathode of solid oxide fuel cell calcining heat
CN107093744A (en) * 2017-04-17 2017-08-25 北京矿冶研究总院 Preparation method of low-temperature solid fuel cell
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CN103107342B (en) * 2013-01-22 2014-11-19 哈尔滨工业大学 Preparation method of one-dimensional nanofiber SSC based composite cathode
CN104157893A (en) * 2013-05-13 2014-11-19 中国科学院大连化学物理研究所 Low temperature solid oxide fuel cell supported by porous metal and preparation method thereof
CN104157893B (en) * 2013-05-13 2016-12-28 中国科学院大连化学物理研究所 Low-temperature solid oxide fuel cell that a kind of porous metals support and preparation method thereof
CN103367763A (en) * 2013-07-11 2013-10-23 黑龙江大学 Method for preparing solid oxide fuel cell nanometer thin film cathode by magnetron sputtering method
CN103367763B (en) * 2013-07-11 2015-06-03 黑龙江大学 Method for preparing solid oxide fuel cell nanometer thin film cathode by magnetron sputtering method
CN105734607A (en) * 2014-12-08 2016-07-06 中国科学院大连化学物理研究所 High temperature solid oxide electrolytic bath with double-layer composite interlayer
CN105734607B (en) * 2014-12-08 2018-11-27 中国科学院大连化学物理研究所 A kind of high-temperature solid oxide electrolytic cell with two-layer compound interlayer
CN106876725A (en) * 2015-12-12 2017-06-20 中国科学院大连化学物理研究所 A kind of method for reducing cathode of solid oxide fuel cell calcining heat
CN107093744A (en) * 2017-04-17 2017-08-25 北京矿冶研究总院 Preparation method of low-temperature solid fuel cell
CN109841846A (en) * 2017-11-29 2019-06-04 中国科学院大连化学物理研究所 A kind of method of modifying of cathode of solid oxide fuel cell

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