CN104779398A - Solid oxide fuel cell anode material and anode provided with same - Google Patents
Solid oxide fuel cell anode material and anode provided with same Download PDFInfo
- Publication number
- CN104779398A CN104779398A CN201510207032.3A CN201510207032A CN104779398A CN 104779398 A CN104779398 A CN 104779398A CN 201510207032 A CN201510207032 A CN 201510207032A CN 104779398 A CN104779398 A CN 104779398A
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- Prior art keywords
- anode
- fuel cell
- solid oxide
- oxide fuel
- titanium
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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
-
- 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
- H01M4/90—Selection of catalytic material
- H01M4/9016—Oxides, hydroxides or oxygenated metallic salts
- H01M4/9025—Oxides specially used in fuel cell operating at high temperature, e.g. SOFC
- H01M4/9033—Complex oxides, optionally doped, of the type M1MeO3, M1 being an alkaline earth metal or a rare earth, Me being a metal, e.g. perovskites
-
- 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
- H01M2004/8678—Inert electrodes with catalytic activity, e.g. for fuel cells characterised by the polarity
- H01M2004/8689—Positive electrodes
-
- 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 relates to a solid oxide fuel cell anode material and an anode provided with the same. The solid oxide fuel cell anode material is an A-site defect A and B site doped perovskite type strontium titanate oxide with a general formula being Al-x-zA'xB1-yB'yO3, wherein A is one or more of strontium, calcium and barium, A' is one or more of yttrium and lanthanide elements, B is one of titanium and chromium, and B' is one or more of manganese, ferrum, cobalt, nickel, scandium, vanadium and molybdenum; when B is titanium, B' also comprises chromium; when B is chromium, B' also comprises titanium; the chemical composition is 0<x<1, 0<=y<=0.5, and 0<z<=0.2. A solid oxide fuel cell adopting the anode material as the anode can directly use hydrocarbon fuel, is stable in structure under the reduction atmosphere, and has high conductivity and carbon and sulfur resistance.
Description
Technical field
The present invention relates to Solid Oxide Fuel Cell technical field, be specifically related to a kind of anode of solid oxide fuel cell material and there is its anode.
Background technology
(English is Solid Oxide Fuel Cell to Solid Oxide Fuel Cell, be abbreviated as SOFC) be a kind of all solid state power generating device by electrochemical reaction, the chemical energy in fuel being directly transformed into electric energy, be new and effective clean energy conversion device.SOFC has many advantages, such as: do not need to make electrode with noble metal; The broad applicability of fuel, namely hydrogen, carbon monoxide and hydrocarbon all can be used as fuel; There is higher energy transformation efficiency; Quick electrode reaction; Be only gas-particle two-phase system, eliminate the etching problem that liquid electrolyte produces; The high-quality waste gas given off can with gas turbine combined cycle, or cogeneration.SOFC has a wide range of applications field, and it is mainly applied and comprises distributed power station, family power station, vehicle accessory power supply, uninterrupted power supply and Military Power etc.The developmental research of SOFC and commercialization, receive the most attention of many countries in the world, generally has an optimistic view of the application prospect of SOFC in the world.The major obstacle that SOFC enters commercialized development is cost and the life-span of battery system.Flat solid oxide fuel cell, especially intermediate temperature solid oxide fuel cell (500 ~ 800 DEG C), forward position and the focus of Solid Oxide Fuel Cell research in the world at present, its the most outstanding advantage is ensureing high power density while, the alloys such as cheap stainless steel can be used as metallic interconnect materials, reduce the requirement to other materials such as sealings, the ceramic preparation technique of low cost can be adopted, be expected the manufacturing cost significantly reducing Solid Oxide Fuel Cell.
At present, NiO-YSZ (YSZ: yttria-stabilized zirconia) anode-supported intermediate temperature solid oxide fuel cell is widely used in recent years in the world.When directly using hydrocarbon for anode fuel, there is the shortcomings such as Sulfur tolerance is low, meeting carbon distribution in NiO-YSZ anode, so, H
2could as desirable anode fuel with reformation hydrocarbon gas.But gas reforming adds the complexity of SOFC electricity generation system, reduces generating efficiency, thus cost is caused to improve.In addition, can there is the problem such as oxidation-reduction stability difference, Ni particle agglomeration in NiO-YSZ at high temperature long-time running.Therefore, find and develop single-phase oxide material to replace the anode material of NiO-YSZ as anode-supported intermediate temperature solid oxide fuel cell, making it possess the advantage of NiO-YSZ, can reduce carbon distribution simultaneously, overcoming the problems such as nickel sintering and sulfur poisoning is urgent and necessity.
In recent years, containing the perofskite type oxide ABO of transition metal
3obtain special concern, the dissimilar ion of their 3 kinds of containing constitutes various and has the defect chemistry of potential use, wherein SrTiO
3it is Typical Representative.SrTiO
3material has good chemistry and mechanical stability in wide in range partial pressure of oxygen and temperature range, demonstrates defect chemistry by a relatively large margin and can control and regulate defect density and defect chemistry thereof by doping.Through finding the literature search of prior art, the patent that China Patent Publication No. CN 101964422A, name are called " Ca-Ti ore type anode of solid oxide fuel cell material ", describes by perovskite structure (ABO
3) oxide carry out A, B position doping a series of materials, this new material has good structural stability, electrical property, catalytic performance and carbon accumulation resisting ability, is applicable to the hydrocarbon fuels such as oxidizing of methylene.But needed raw material kind is too much, preparation cost improves and preparation process is easily made mistakes.The patent that China Patent Publication No. CN 101222059A, name are called " a kind of B position omission perovskite anode material for Solid Oxide Fuel Cell ", describing molecular formula is Y
0.08sr
0.92ti
1-xo
3wherein the B position omission perovskite anode material of x=0-0.05 may be used for Solid Oxide Fuel Cell, stable performance, has good chemical compatibility with electrolyte YSZ, LSGM, and drastically increase the ionic conductivity of material, thus improve the service behaviour of anode material.But it does not take into account A position defect, the space that conductivity is still improved.In addition, China Patent No. publication number CN 102731090A, name are called the patent of " a kind of Direct-Hydrocarbon Solid Oxide Fuel Cells anode material and preparation method thereof ", describe La, Cr codope strontium titanates anode material, it is high that it has ionic conductivity, with electrolyte YSZ, there is good chemical compatibility, may be used for Direct-Hydrocarbon Solid Oxide Fuel Cells and improve battery operated performance.But the polarization resistance of this anode material is higher, battery performance can be reduced again.Therefore, how searching out a kind of perofskite type oxide anode material further to meet the requirement of the requirement of SOFC anode, particularly oxidation-reduction stability and conductivity, is the problem needing now solution badly.
Summary of the invention
The object of the invention is in order to overcome carbon distribution, nickel sintering and the problem such as sulfur poisoning provide a kind of can directly use hydrocarbon fuel, under reducing atmosphere Stability Analysis of Structures and the perofskite type oxide possessing high conductivity, anti-carbon and sulfur tolerance to replace NiO-YSZ as anode of solid oxide fuel cell material and preparation method thereof.
The present invention is realized by following technical proposal:
According to a first aspect of the invention, provide a kind of anode of solid oxide fuel cell material, wherein, described anode of solid oxide fuel cell material general formula is A
1-x-za ＇
xb
1-yb ＇
yo
3a, B position doped perovskite type strontium titanates oxide of A position defect, wherein, A is one or more in strontium, calcium and barium; A ＇ is one or more in yttrium and lanthanide series; B is the one in titanium and chromium; B ＇ is one or more in manganese, iron, cobalt, nickel, scandium, vanadium, niobium and molybdenum; When B is titanium, in B ＇, also comprise chromium; When B is chromium, in B ＇, also comprise titanium; Chemical composition is 0 < x < 1,0≤y≤0.5,0 < z≤0.2.
According to a second aspect of the invention, a kind of anode with above-mentioned anode of solid oxide fuel cell material is provided.
Compared with the prior art, the substantive distinguishing features that has of the present invention and marked improvement are:
(1) can directly use hydrocarbon fuel, under reducing atmosphere Stability Analysis of Structures and the perofskite type oxide possessing high conductivity, anti-carbon and sulfur tolerance to replace NiO-YSZ, the problems such as carbon distribution, nickel sintering and sulfur poisoning can be overcome.
(2) diameter of particle synthesized by Via Polymeric Precursor Method, powders by glycine-nitrate process or spray drying process is less, specific area is larger, there is better chemical property, and sintering activity is higher, so be more suitable for as anode of solid oxide fuel cell material.
(3) anode of solid oxide fuel cell material preparation method technique of the present invention is simple, is convenient to amplify and scale manufacture.
Accompanying drawing explanation
In order to be illustrated more clearly in the embodiment of the present invention or technical scheme of the prior art, be briefly described to the accompanying drawing used required in embodiment or description of the prior art below, apparently, accompanying drawing in the following describes is only some embodiments of the present invention, for those of ordinary skill in the art, under the prerequisite not paying creative work, other accompanying drawing can also be obtained according to these accompanying drawings.
Fig. 1 is the Sr adopting spray drying process to synthesize in embodiment 4
0.7la
0.2tiO
3the XRD figure of powder.
Embodiment
Below in conjunction with the accompanying drawing in the embodiment of the present invention, be clearly and completely described the technical scheme in the embodiment of the present invention, obviously, described embodiment is only the present invention's part embodiment, instead of whole embodiments.Based on the embodiment in the present invention, those of ordinary skill in the art, not making the every other embodiment obtained under creative work prerequisite, belong to the scope of protection of the invention.
Anode of solid oxide fuel cell material in the present invention can adopt known any suitable preparation method's preparation, as: solid-phase synthesis, Via Polymeric Precursor Method, powders by glycine-nitrate process and spray drying process etc.
Embodiment 1:
Solid-phase synthesis:
With SrCO
3, La
2o
3, Cr
2o
3, TiO
2for raw material, according to Sr
0.7la
0.2cr
0.8ti
0.2o
3stoichiometric proportion configuration mixture, be medium with alcohol, ball milling 24 hours in agate jar, after mixing, dries in 120 DEG C of baking ovens.Powder after drying is put in 1000 DEG C of calcinings 12 hours, uses alcohol ball milling after cooling 24 hours, 120 DEG C of oven dry, be again put in 1400 DEG C of calcinings 12 hours, pulverize with pulverizer after cold going, after crossing 250 mesh sieves, obtain Sr
0.7la
0.2cr
0.8ti
0.2o
3powder.
Embodiment 2:
Via Polymeric Precursor Method:
With Sr (NO
3)
2, hydration La (NO
3)
3, hydration Cr (NO
3)
3, Mn (NO
3)
2for raw material, according to Sr
0.4la
0.4cr
0.5mn
0.5o
3stoichiometric proportion be dissolved in deionized water and be mixed with solution A, appropriate citric acid and ethylene glycol are added deionized water for stirring to dissolving wiring solution-forming B completely simultaneously, B solution is mixed with solution A, wherein metal ion: citric acid: the mol ratio of ethylene glycol is 1:2:4.Be stirred to evenly and continue to add thermal agitation formation gel at 80 DEG C, then gel is put in 400 degree and makes resin carbonation in 2 hours, the porous foam shape product obtained is put in 1000 DEG C of calcinings 12 hours, uses alcohol ball milling after cooling 24 hours, 120 DEG C of oven dry, obtain Sr after crossing 200 mesh sieves
0.4la
0.4cr
0.5mn
0.5o
3powder.
Embodiment 3
Powders by glycine-nitrate process:
With Sr (NO
3)
2, hydration La (NO
3)
3, hydration Cr (NO
3)
3, Mn (NO
3)
2for raw material, according to Sr
0.55la
0.3cr
0.8mn
0.2o
3stoichiometric proportion be dissolved in deionized water, add appropriate glycine again to stir wiring solution-forming, wherein glycine: the mol ratio of metal ion is 2:1, add at 100 DEG C after thermal agitation forms wet gel and improve temperature to 250 DEG C, 1000 DEG C of calcinings 6 hours are placed in Deng collection precursor powder after burning, use alcohol ball milling after cooling 24 hours, 120 DEG C of oven dry, after crossing 200 mesh sieves, obtain Sr
0.55la
0.3cr
0.8mn
0.2powder.
Embodiment 4
Spray drying process:
With Sr (NO
3)
2, hydration La (NO
3)
3, tetraisopropyl titanate is raw material, according to Sr
0.7la
0.2tiO
3stoichiometric proportion by Sr (NO
3)
2with hydration La (NO
3)
3add in the deionized water solution containing appropriate nitric acid and hydrogen peroxide to be stirred to and dissolve completely, wherein the mol ratio of nitric acid and titanium ion is 5:1, the mol ratio of hydrogen peroxide and titanium ion is 2:1, and then add in solution tetraisopropyl titanate continue stirring obtain uniform mixed solution, solution is carried out spray drying treatment, the speed of spraying is 16.67ml/min, simultaneously dry temperature is 230 DEG C, the presoma obtained 1000 DEG C calcining 6 hours, use alcohol ball milling after cooling 24 hours, 120 DEG C of oven dry, obtain Sr after crossing 200 mesh sieves
0.7la
0.2tiO
3powder.With Sr
0.7la
0.2tiO
3for anode material, yttria-stabilized zirconia (YSZ) is electrolyte, La
0.6sr
0.4coO
3the positive electrode support solid oxide fuel cell be prepared into for cathode material maximum power density 800 DEG C time is 120mW/cm
2.
Fig. 1 is the Sr of spray drying process synthesis in the present embodiment
0.7la
0.2tiO
3the XRD figure of powder.
Embodiment 5
With embodiment 1, adopt solid-phase synthesis, with SrCO
3, Y
2o
3, TiO
2, Nb
2o
5for raw material, according to Sr
0.86y
0.08ti
0.9nb
0.1o
3stoichiometric proportion configuration mixture, be medium with alcohol, ball milling 24 hours in agate jar, after mixing, dries in 120 DEG C of baking ovens.Powder after drying is put in 1000 DEG C of calcinings 12 hours, uses alcohol ball milling after cooling 24 hours, 120 DEG C of oven dry, be again put in 1400 DEG C of calcinings 12 hours, pulverize with pulverizer after cold going, after crossing 250 mesh sieves, obtain Sr
0.86y
0.08ti
0.9nb
0.1o
3powder.
Embodiment 6
With embodiment 2, adopt Via Polymeric Precursor Method, with Sr (NO
3)
2, Y (NO
3)
3, hydration Cr (NO
3)
3, Mn (NO
3)
2for raw material, according to Sr
0.86y
0.08cr
0.8mn
0.2o
3stoichiometric proportion be dissolved in deionized water and be mixed with solution A, appropriate citric acid and ethylene glycol are added deionized water for stirring to dissolving wiring solution-forming B completely simultaneously, B solution is mixed with solution A, wherein metal ion: citric acid: the mol ratio of ethylene glycol is 1:4:16, be stirred to evenly and continue to add thermal agitation formation gel at 80 DEG C, then gel is put in 400 degree and makes resin carbonation in 2 hours, the porous foam shape product obtained is put in 1000 DEG C of calcinings 12 hours, use alcohol ball milling after cooling 24 hours, 120 DEG C of oven dry, obtain Sr after crossing 200 mesh sieves
0.88y
0.08cr
0.8mn
0.2o
3powder.
Embodiment 7
With embodiment 3, adopt powders by glycine-nitrate process, with Sr (NO
3)
2, Y (NO
3)
3, hydration Cr (NO
3)
3, Mn (NO
3)
2for raw material, according to Sr
0.874y
0.076cr
0.5mn
0.5o
3stoichiometric proportion be dissolved in deionized water, add appropriate glycine again to stir wiring solution-forming, wherein glycine: the mol ratio of metal ion is 2:1, add at 100 DEG C after thermal agitation forms wet gel and improve temperature to 250 DEG C, 1000 DEG C of calcinings 6 hours are placed in Deng collection precursor powder after burning, use alcohol ball milling after cooling 24 hours, 120 DEG C of oven dry, after crossing 200 mesh sieves, obtain Sr
0.874y
0.076cr
0.5mn
0.5o
3powder.
Embodiment 8
With embodiment 4, adopt spray drying process, with Sr (NO
3)
2, Y (NO
3)
3, tetraisopropyl titanate, hydration Cr (NO
3)
3for raw material, according to Sr
0.86y
0.08ti
0.8cr
0.2o
3stoichiometric proportion by Sr (NO
3)
2, Y (NO
3)
3with hydration Cr (NO
3)
3add in the deionized water solution containing appropriate nitric acid and hydrogen peroxide to be stirred to and dissolve completely, wherein the mol ratio of nitric acid and titanium ion is 5:1, the mol ratio of hydrogen peroxide and titanium ion is 2:1, and then add in solution tetraisopropyl titanate continue stirring obtain uniform mixed solution, solution is carried out spray drying treatment, the speed of spraying is 8.5ml/min, simultaneously dry temperature is 220 DEG C, the presoma obtained 1000 DEG C calcining 6 hours, use alcohol ball milling after cooling 24 hours, 120 DEG C of oven dry, obtain Sr after crossing 200 mesh sieves
0.86y
0.08ti
0.8cr
0.2o
3powder.
Compared with the prior art, the substantive distinguishing features that has of the present invention and marked improvement are:
(1) can directly use hydrocarbon fuel, under reducing atmosphere Stability Analysis of Structures and the perofskite type oxide possessing high conductivity, anti-carbon and sulfur tolerance to replace NiO-YSZ, the problems such as carbon distribution, nickel sintering and sulfur poisoning can be overcome.
(2) diameter of particle synthesized by Via Polymeric Precursor Method, powders by glycine-nitrate process or spray drying process is less, specific area is larger, there is better chemical property, and sintering activity is higher, so be more suitable for as anode of solid oxide fuel cell material.
(3) anode of solid oxide fuel cell material preparation method technique of the present invention is simple, is convenient to amplify and scale manufacture.
More than show and describe general principle of the present invention, principal character and advantage of the present invention.The technical staff of the industry should understand; the present invention is not restricted to the described embodiments; what describe in above-described embodiment and specification just illustrates principle of the present invention; the present invention also has various changes and modifications without departing from the spirit and scope of the present invention, and these changes and improvements all fall in the claimed scope of the invention.Application claims protection range is defined by appending claims and equivalent thereof.
Claims (2)
1. an anode of solid oxide fuel cell material, is characterized in that, described anode of solid oxide fuel cell material general formula is A
1-x-za ＇
xb
1-yb ＇
yo
3a, B position doped perovskite type strontium titanates oxide of A position defect, wherein, A is one or more in strontium, calcium and barium; A ＇ is one or more in yttrium and lanthanide series; B is the one in titanium and chromium; B ＇ is one or more in manganese, iron, cobalt, nickel, scandium, vanadium, niobium and molybdenum; When B is titanium, in B ＇, also comprise chromium; When B is chromium, in B ＇, also comprise titanium; Chemical composition is 0 < x < 1,0≤y≤0.5,0 < z≤0.2.
2. one kind comprises the anode of anode of solid oxide fuel cell material as claimed in claim 1.
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|---|---|---|---|
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ID=53620739
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Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN108063272A (en) * | 2017-12-13 | 2018-05-22 | 叶芳 | A kind of fuel cell modified electrode material and preparation method thereof |
| CN109301297A (en) * | 2018-11-15 | 2019-02-01 | 中国矿业大学(北京) | A kind of composite ceramic powder and composite solid oxide fuel cell prepared therefrom |
| CN110302791A (en) * | 2019-04-29 | 2019-10-08 | 南京工业大学 | A kind of electrolysis water catalyst of unconventional Local Structure and preparation method thereof |
| CN114855203A (en) * | 2022-05-20 | 2022-08-05 | 南京理工大学 | Application of perovskite LSCM material in solid oxide electrolytic cell |
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| CN101964422A (en) * | 2009-07-24 | 2011-02-02 | 中国矿业大学(北京) | Perovskite type solid oxide fuel cell anode material |
| CN102731090A (en) * | 2012-06-29 | 2012-10-17 | 华南师范大学 | Anode material of direct-hydrocarbon solid oxide fuel cell and preparation method thereof |
| CN104078687A (en) * | 2013-03-25 | 2014-10-01 | 中国科学院物理研究所 | Anode material containing alkali metal or alkaline-earth metal element of solid oxide fuel cell and preparation method and application thereof |
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| CN108063272A (en) * | 2017-12-13 | 2018-05-22 | 叶芳 | A kind of fuel cell modified electrode material and preparation method thereof |
| CN109301297A (en) * | 2018-11-15 | 2019-02-01 | 中国矿业大学(北京) | A kind of composite ceramic powder and composite solid oxide fuel cell prepared therefrom |
| CN109301297B (en) * | 2018-11-15 | 2021-06-22 | 中国矿业大学(北京) | Composite ceramic powder and composite solid oxide fuel cell prepared from same |
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| CN114855203A (en) * | 2022-05-20 | 2022-08-05 | 南京理工大学 | Application of perovskite LSCM material in solid oxide electrolytic cell |
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