CN102610841A - Single-cavity solid oxide fuel cell with controlled gas flow direction - Google Patents
Single-cavity solid oxide fuel cell with controlled gas flow direction Download PDFInfo
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- CN102610841A CN102610841A CN2012100854031A CN201210085403A CN102610841A CN 102610841 A CN102610841 A CN 102610841A CN 2012100854031 A CN2012100854031 A CN 2012100854031A CN 201210085403 A CN201210085403 A CN 201210085403A CN 102610841 A CN102610841 A CN 102610841A
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- 239000000446 fuel Substances 0.000 title claims abstract description 37
- 239000007787 solid Substances 0.000 title abstract description 21
- 239000007789 gas Substances 0.000 claims abstract description 68
- 239000002737 fuel gas Substances 0.000 claims abstract description 5
- 238000003487 electrochemical reaction Methods 0.000 claims abstract description 3
- 239000003792 electrolyte Substances 0.000 claims description 19
- 239000008246 gaseous mixture Substances 0.000 claims description 19
- 239000000203 mixture Substances 0.000 claims description 12
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 claims description 6
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 claims description 6
- 229910052760 oxygen Inorganic materials 0.000 claims description 5
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 4
- 229910002204 La0.8Sr0.2MnO3 Inorganic materials 0.000 claims description 4
- 239000003085 diluting agent Substances 0.000 claims description 4
- 229910052751 metal Inorganic materials 0.000 claims description 4
- 239000002184 metal Substances 0.000 claims description 4
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 claims description 4
- 229910052697 platinum Inorganic materials 0.000 claims description 4
- 239000000126 substance Substances 0.000 claims description 4
- 150000001335 aliphatic alkanes Chemical class 0.000 claims description 3
- 229910052786 argon Inorganic materials 0.000 claims description 3
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 3
- 229910000420 cerium oxide Inorganic materials 0.000 claims description 3
- LNTHITQWFMADLM-UHFFFAOYSA-N gallic acid Chemical compound OC(=O)C1=CC(O)=C(O)C(O)=C1 LNTHITQWFMADLM-UHFFFAOYSA-N 0.000 claims description 3
- 229910052746 lanthanum Inorganic materials 0.000 claims description 3
- FZLIPJUXYLNCLC-UHFFFAOYSA-N lanthanum atom Chemical compound [La] FZLIPJUXYLNCLC-UHFFFAOYSA-N 0.000 claims description 3
- 239000003915 liquefied petroleum gas Substances 0.000 claims description 3
- BMMGVYCKOGBVEV-UHFFFAOYSA-N oxo(oxoceriooxy)cerium Chemical compound [Ce]=O.O=[Ce]=O BMMGVYCKOGBVEV-UHFFFAOYSA-N 0.000 claims description 3
- 239000001301 oxygen Substances 0.000 claims description 3
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 2
- 229910002127 La0.6Sr0.4Co0.2Fe0.8O3 Inorganic materials 0.000 claims description 2
- 229910002806 Sm0.2Ce0.8O1.9 Inorganic materials 0.000 claims description 2
- 239000001307 helium Substances 0.000 claims description 2
- 229910052734 helium Inorganic materials 0.000 claims description 2
- SWQJXJOGLNCZEY-UHFFFAOYSA-N helium atom Chemical compound [He] SWQJXJOGLNCZEY-UHFFFAOYSA-N 0.000 claims description 2
- 229910052742 iron Inorganic materials 0.000 claims description 2
- 239000003595 mist Substances 0.000 claims description 2
- 239000003345 natural gas Substances 0.000 claims description 2
- 229910052759 nickel Inorganic materials 0.000 claims description 2
- 229910052757 nitrogen Inorganic materials 0.000 claims description 2
- 230000000087 stabilizing effect Effects 0.000 claims description 2
- 230000005611 electricity Effects 0.000 abstract description 11
- 230000003647 oxidation Effects 0.000 abstract description 4
- 238000007254 oxidation reaction Methods 0.000 abstract description 4
- 238000005245 sintering Methods 0.000 description 34
- 238000005507 spraying Methods 0.000 description 26
- 210000004027 cell Anatomy 0.000 description 18
- 239000012528 membrane Substances 0.000 description 18
- 238000002360 preparation method Methods 0.000 description 16
- 239000010453 quartz Substances 0.000 description 14
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N silicon dioxide Inorganic materials O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 14
- 239000011230 binding agent Substances 0.000 description 9
- 238000001125 extrusion Methods 0.000 description 9
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 9
- 239000003708 ampul Substances 0.000 description 8
- 238000005520 cutting process Methods 0.000 description 8
- 238000002156 mixing Methods 0.000 description 7
- 238000000034 method Methods 0.000 description 6
- 239000000463 material Substances 0.000 description 4
- 239000003054 catalyst Substances 0.000 description 3
- 230000008021 deposition Effects 0.000 description 3
- 239000000843 powder Substances 0.000 description 3
- RTZKZFJDLAIYFH-UHFFFAOYSA-N Diethyl ether Chemical compound CCOCC RTZKZFJDLAIYFH-UHFFFAOYSA-N 0.000 description 2
- 229910000416 bismuth oxide Inorganic materials 0.000 description 2
- TYIXMATWDRGMPF-UHFFFAOYSA-N dibismuth;oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[Bi+3].[Bi+3] TYIXMATWDRGMPF-UHFFFAOYSA-N 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- 238000010438 heat treatment Methods 0.000 description 2
- 229910052739 hydrogen Inorganic materials 0.000 description 2
- 239000011812 mixed powder Substances 0.000 description 2
- 239000007800 oxidant agent Substances 0.000 description 2
- 230000001590 oxidative effect Effects 0.000 description 2
- SIWVEOZUMHYXCS-UHFFFAOYSA-N oxo(oxoyttriooxy)yttrium Chemical compound O=[Y]O[Y]=O SIWVEOZUMHYXCS-UHFFFAOYSA-N 0.000 description 2
- 239000000565 sealant Substances 0.000 description 2
- 238000012360 testing method Methods 0.000 description 2
- VGGSQFUCUMXWEO-UHFFFAOYSA-N Ethene Chemical compound C=C VGGSQFUCUMXWEO-UHFFFAOYSA-N 0.000 description 1
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 1
- FYYHWMGAXLPEAU-UHFFFAOYSA-N Magnesium Chemical compound [Mg] FYYHWMGAXLPEAU-UHFFFAOYSA-N 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 229910002091 carbon monoxide Inorganic materials 0.000 description 1
- 238000005266 casting Methods 0.000 description 1
- 230000015556 catabolic process Effects 0.000 description 1
- 230000003197 catalytic effect Effects 0.000 description 1
- 239000000919 ceramic Substances 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 238000010276 construction Methods 0.000 description 1
- 238000001816 cooling Methods 0.000 description 1
- 238000006731 degradation reaction Methods 0.000 description 1
- 229910001938 gadolinium oxide Inorganic materials 0.000 description 1
- 229940075613 gadolinium oxide Drugs 0.000 description 1
- CMIHHWBVHJVIGI-UHFFFAOYSA-N gadolinium(iii) oxide Chemical compound [O-2].[O-2].[O-2].[Gd+3].[Gd+3] CMIHHWBVHJVIGI-UHFFFAOYSA-N 0.000 description 1
- 239000003292 glue Substances 0.000 description 1
- 229930195733 hydrocarbon Natural products 0.000 description 1
- 150000002430 hydrocarbons Chemical class 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 229910052749 magnesium Inorganic materials 0.000 description 1
- 239000011777 magnesium Substances 0.000 description 1
- 231100000572 poisoning Toxicity 0.000 description 1
- 230000000607 poisoning effect Effects 0.000 description 1
- 238000003825 pressing Methods 0.000 description 1
- QQONPFPTGQHPMA-UHFFFAOYSA-N propylene Natural products CC=C QQONPFPTGQHPMA-UHFFFAOYSA-N 0.000 description 1
- 125000004805 propylene group Chemical group [H]C([H])([H])C([H])([*:1])C([H])([H])[*:2] 0.000 description 1
- 239000000376 reactant Substances 0.000 description 1
- 238000013112 stability test Methods 0.000 description 1
- 229910052712 strontium Inorganic materials 0.000 description 1
- CIOAGBVUUVVLOB-UHFFFAOYSA-N strontium atom Chemical compound [Sr] CIOAGBVUUVVLOB-UHFFFAOYSA-N 0.000 description 1
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Classifications
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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
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- Fuel Cell (AREA)
Abstract
The invention relates to the field of solid oxide fuel cells, specifically to a single-cavity solid oxide fuel cell with special configuration, which is a single-cavity solid oxide fuel cell with controlled flow direction of mixed gas formed by fuel gas and oxidation gas. The solid oxide fuel cell of the invention is a tubular solid oxide fuel cell or a tubular structure fuel cell composed of a sheet solid oxide fuel cell, a main body is composed of the solid oxide fuel cell (1), a support tube (3) and an outer sleeve (2), mixed gas of fuel-oxidiation gas enters a reactor, orderly flows through a cathode (1-1) of the fuel cell and an anode (1-3) of the solid oxide fuel cell to perform electrochemical reaction to generate electricity. According to the invention, the fuel cell has high open-circuit voltage and power density; volume of the reactor is small; and work temperature is 500-900 degrees centigrade; therefore, the fuel cell is suitable for being used as a portable power source.
Description
Technical field
The present invention relates to field of solid oxide fuel, be specifically related to the controlled single cavity SOFC of the special gas flow of a kind of configuration.
Background technology
The most initial notion of single cavity fuel cell (SCFC) is to equal proposition in 1961 by Eyraud, and it also is called as mixed reactant fuel cells.The operable electrolyte kind of SCFC has a lot, and the SC-SOFC that uses solid oxide electrolyte is wherein a kind of.Single cavity SOFC (Single Chamber Solid Oxide Fuel Cell; SC-SOFC) be a kind of SOFC of brand new; It is direct and oxidant premixed with fuel; The anode and cathode of battery is exposed in the same air cavity simultaneously; The battery of comparing this configuration with traditional fuel cell has more superiority: SC-SOFC is with the atmosphere of fuel-oxidant mixtures while as negative electrode and anode, just can omit in this battery system as the sealant that intercepts anode and cathode atmosphere, and the unmatched problem of thermal coefficient of expansion just can not exist yet between sealant in the operating process and the fuel cell module like this; Therefore SC-SOFC can be competent at heating and cooling process fast, utilizes the field to have certain application value in portable energy source; For SC-SOFC because air chamber is single, final one road source of the gas that only needs, simultaneously the anode and cathode of battery also can electrolytical with one side on, thereby make the configuration of fuel cell and preparation technology significantly to simplify, the reduction preparation cost.Based on above some, as long as the stability test of SC-SOFC is resolved, just assembled battery is more easily piled; In addition, on the anode of SC-SOFC, modify one deck when Shao etc. also find to be fuel with alkane and have highly active hydro carbons partial oxidation catalyst, oneself keeps the temperature that fuel cell just can utilize the catalytic exothermic of anode to react to realize battery; The structure of whole solid state of SC-SOFC can directly adopt liquid fuel such as low-carbon alcohols, ether etc. in addition, can realize the microminiaturization of SC-SOFC to a certain extent.
But SC-SOFC is because air inlet contacts anode and negative electrode simultaneously at present, CO, H that anode reaction produces
2, CO
2Can Poisoning cathode and can reduce the partial pressure of oxygen of negative electrode Deng gas, have that open circuit voltage is lower, performance is stable inadequately and area amplifies the back performance and obviously descends the degradation problem.
Summary of the invention
The objective of the invention is to collaborate in order to solve in existing single cavity SOFC anode and negative electrode atmosphere; Problems such as open circuit voltage is low, power density is not high, and a kind of controlled single cavity SOFC of gas flow that is configured as the basis with tubular type has been proposed.
Technical scheme of the present invention is: single cavity SOFC that a kind of gas flow is controlled; It is characterized in that forming by SOFC 1, outer tube 2 and stay pipe 3; SOFC 1 links together with stay pipe 3 upper ends, and fits together through seal 4 and outer tube 2; Two holes are arranged on the seal 4, and one of them hole is communicated with extraneous and outer tube 2 inside, as the inlet A of gas or export B; A hole is used for fixing stay pipe 3 ends at the center of seal 4, and the end of stay pipe 3 stretches out seal 4, as the outlet B of gas or the A that enters the mouth; SOFC 1 presents tubulose, is made up of for three layers negative electrode 1-1, electrolyte 1-2, anode 1-3; The gaseous mixture of the fuel-oxic gas of single cavity fuel cell passes through anode generation electrochemical reaction through negative electrode earlier again, and mist gets into system by the inlet A of gas, and B discharges system by outlet.
The configuration of preferred SOFC 1 is a kind of in anode support type, electrolyte-supporting type or the cathode support type; Its operating temperature is 500~900 ℃.
Preferred described electrolyte 1-2 is that the stabilizing zirconia material is (like the zirconia of stabilized with yttrium oxide; YSZ), the doped cerium oxide material is (like the gadolinium oxide doping of cerium oxide; The lanthanum gallate of GDC), mixing is (like the lanthanum gallate of strontium and magnesium doping; LSGM), (combination is to mix or the multilayer stack for the bismuth oxide of Yttrium oxide doping, a kind of or any several kinds combination in YSB) for the bismuth oxide that mixes; Described anode 1-3 is the mixture of any one or several kinds in electrolyte 1-2 and Ni, Pt, Ag, Ru, Fe or the Cu metal simple-substance, and wherein metal simple-substance accounts for the 10-90% of mixture gross mass.Preferred described negative electrode 1-1 is electrolyte 1-2 and La
0.8Sr
0.2MnO
3, La
0.6Sr
0.4Co
0.2Fe
0.8O
3, Ba
0.5Sr
0.5Co
0.8Fe
0.2O, La
2NiO
4, PrBaCoO
5, Pt, Ag-Sm
0.2Ce
0.8O
1.9Or Ag-La
0.8Sr
0.2MnO
3In any one or a few mixture, wherein electrolyte accounts for the 10-90% of mixture gross mass.
Preferred described fuel-oxic gas gaseous mixture is 0~80% diluent gas by accounting for the gaseous mixture volume fraction, account for the gaseous mixture volume fraction is the fuel gas of 10-90% and to account for the gaseous mixture volume fraction be that the oxidizing gas of 10-90% is formed; Wherein said diluent gas is nitrogen, argon gas or helium; Described fuel gas is alkane, alcohol, natural gas or liquefied petroleum gas; Described oxic gas is an air or oxygen.
The preparation process of single cavity SOFC that gas flow of the present invention is controlled is:
(1) monocell preparation
A kind of is the SOFC of tubular type, and its preparation method is to adopt mechanical means to prepare the cell support pipe, and stay pipe can be the male or female material, also can be electrolyte.After 1000-1400 ℃ sintering process, prepare remaining electrolyte or electrode again, finally obtain anode | electrolyte | cathode construction.
The tubular structure that monocell also can be made up of the sheet battery adopts traditional monocell preparation method, like dry pressing, curtain coating-spraying method etc.Use the ceramic glue that is fit to that the monocell that obtains is bonded together, form tubular structure.Also can adopt the series, parallel method to link together between the monocell.
(2) single cavity solid oxide fuel cell stack dress
Special structure design is adopted in the assembling of monocell of the present invention, and SOFC structure one end of tubulose is sealed on the stay pipe, and stay pipe and overall fuel cell are in being sealed in outer tube, and whole system has an air inlet and a gas outlet.
(3) single cavity fuel cell operation
When monocell of the present invention moved, fuel gas-oxic gas got into system simultaneously according to certain ratio, and gaseous mixture through negative electrode, passes through anode earlier again, discharged at last.The operating temperature of battery is between 500-900 ℃.Single cavity SOFC of the present invention also can increase the voltage of solid oxide fuel battery system through being composed in series the battery pack of a plurality of SOFCs like this.
Beneficial effect:
Single cavity SOFC of the present invention has particular structural, and promptly the gaseous mixture inlet air flow through anode behind the negative electrode, has avoided the atmosphere between anode and the negative electrode to collaborate mutually earlier to being controlled.But single cavity SOFC of the present invention has advantages such as high open circuit voltage, high power density and portable operation simultaneously, is suitable as portable power supplies and uses.
Description of drawings
Fig. 1 is the structural representation of monocell (1) among the present invention, and wherein 1-1 is a negative electrode, and 1-2 is an electrolyte, and 1-3 is an anode;
Fig. 2 is for flowing to the sketch map of controlled single cavity SOFC in the embodiment of the invention 1, wherein 1 is monocell, and 2 is outer tube, and 3 is stay pipe, and 4 is seal, and A is an air inlet, and B is the gas outlet.
Fig. 3 is for flowing to the sketch map of controlled single cavity SOFC in the embodiment of the invention 2, wherein 1 is monocell, and 2 is outer tube, and 3 is stay pipe, and A is an air inlet, and B is the gas outlet.
Fig. 4 is the cross section pattern SEM figure after the monocell test in the embodiment of the invention 9.
Fig. 5 is the sketch map after the monocell assembling in the embodiment of the invention 11.
Embodiment
Method involved in the present invention comprises but is not limited to the material in following examples.
Embodiment 1: with NiO and YSZ mixing and water adding and binding agent pugging, mechanical extrusion molding obtains anode support tube, and stay pipe is 1100 ℃ of sintering after super-dry.Prepare one deck YSZ electrolytic thin-membrane in the anode-supported surface through spraying method, electrolytic thin-membrane obtains half-cell behind 1400 ℃ of sintering.Sintering is 1100 ℃ behind half-cell surface spraying preparation one deck LSM electrode, obtains monocell.As shown in Figure 2, elargol uses seal (cutting ferrule) that solid oxide fuel cell stack is loaded in outer tube as current collector on the cathode of solid oxide fuel cell surfaces coated; Have two holes on the seal cutting ferrule; A hole is communicated with extraneous and outer tube inside, is air inlet A, and a hole is used for fixing the stay pipe end; The stay pipe end is gas outlet B, and device places tube furnace to be heated to 750 ℃.During external gas circuit, gas is crossed outer tube cathode earlier, passes through interior tube anode again, earlier feeding H
2With the anode reduction, it is 40% that reduction back Ni accounts for the anode mass fraction, feeds CH again
4And O
2Gaseous mixture (volume ratio 3: 1) just can generate electricity, and the monocell open circuit voltage is 0.92V in the time of 750 ℃, and the monocell maximum power density is 214mW/cm
2
Embodiment 2: the YSZ powder is added water and binding agent pugging, and mechanical extrusion molding obtains the electrolyte-supported pipe, and stay pipe is 1400 ℃ of sintering after super-dry.Prepare one deck anode NiO-YSZ in the electrolyte-supported surface through spraying method, anode film obtains half-cell behind 1300 ℃ of sintering.Sintering is 1100 ℃ behind half-cell inner surface spraying preparation one deck LSM-YSZ (mass fraction of LSM is 70%) electrode, obtains monocell.As shown in Figure 3, elargol uses cutting ferrule (seal) that solid oxide fuel cell stack is loaded in outer tube as current collector on the cathode of solid oxide fuel cell surfaces coated; Have two holes on the seal cutting ferrule; A hole is communicated with extraneous and outer tube inside, is gas outlet B, and a hole is used for fixing the stay pipe end; The stay pipe end is air inlet A, and device places tube furnace to be heated to 650 ℃.During external gas circuit, gas through interior tube cathode, passes through outer tube anode earlier again, earlier feeding H
2With the anode reduction, it is 60% that reduction back Ni accounts for the anode mass fraction, feeds propylene and air Mixture (volume ratio 1.5: 1) again and just can generate electricity, and the monocell open circuit voltage is 0.98V in the time of 750 ℃, and the monocell maximum power density is 65mW/cm
2
Embodiment 3: the SDC powder is added water and binding agent pugging, and mechanical extrusion molding obtains the electrolyte-supported pipe, and stay pipe is 1400 ℃ of sintering after super-dry.Prepare layer of Ni O-SDC anode at electrolyte-supported body inner surface through spraying method, anode film obtains half-cell behind 1300 ℃ of sintering.Sintering is 1100 ℃ behind half-cell outer surface spraying preparation one deck LSCF-SDC (mass fraction of LSCF is 40%) electrode, obtains monocell.The monocell cathode surface is coated elargol as current collector, and one is encapsulated on the quartz ampoule then, and anode and negative electrode are drawn wiring with silver-colored line respectively.Use cutting ferrule that solid oxide fuel cell stack is loaded in outer tube, have two holes on the cutting ferrule, a hole is communicated with extraneous inner with outer tube; Be air inlet A; A hole is used for fixing the stay pipe end, and the stay pipe end is gas outlet B, and device places tube furnace to be heated to 800 ℃.During external gas circuit, gas through outer tube cathode, passes through interior tube anode earlier again, feeds H earlier
2With the anode reduction, it is 30% that reduction back Ni accounts for the anode mass fraction, feeds CH again
4And O
2And N
2Gaseous mixture (volume ratio 1: 1: 1) just can generate electricity, and the monocell open circuit voltage is 0.95V in the time of 650 ℃, and the monocell maximum power density is 54mW/cm
2
Embodiment 4: the LSM powder is added water and binding agent pugging, and mechanical extrusion molding obtains the cathode branch stay tube, and stay pipe is 1100 ℃ of sintering after super-dry.Prepare one deck YSZ electrolytic thin-membrane at LSM supporter outer surface through spraying method, electrolytic thin-membrane obtains half-cell behind 1300 ℃ of sintering.Sintering is 1300 ℃ behind half-cell outer surface spraying preparation one deck CuO-YSZ anode, obtains monocell.The monocell cathode surface is coated elargol as current collector, and one is encapsulated on the quartz ampoule then, and anode and negative electrode are drawn wiring with silver-colored line respectively.Use cutting ferrule that solid oxide fuel cell stack is loaded in outer tube, have two holes on the cutting ferrule, a hole is communicated with extraneous inner with outer tube; Be gas outlet B; A hole is used for fixing the stay pipe end, and the stay pipe end is air inlet A, and device places tube furnace to add and reheats to 750 ℃.During external gas circuit, gas feeds through interior tube cathode earlier, passes through outer tube anode again, earlier feeding H
2With the anode reduction, it is 50% that reduction back Cu accounts for the anode mass fraction, feeds CH again
4And O
2Gaseous mixture (volume ratio 2: 1) just can generate electricity, and the monocell open circuit voltage is 0.98V in the time of 800 ℃, and the monocell maximum power density is 326mW/cm
2
Embodiment 5: with Fe
2O
3With YSZ mixing and water adding and binding agent pugging, mechanical extrusion molding obtains anode support tube, and stay pipe is 1100 ℃ of sintering after super-dry.Prepare one deck YSZ electrolytic thin-membrane in the anode-supported surface through spraying method, electrolytic thin-membrane obtains half-cell behind 1400 ℃ of sintering.Half-cell is used H under 700 ℃ of heating
2Reduction, reduction back behind half-cell surface spraying preparation one deck LSM-YSZ (mass fraction of LSM accounts for 35%) electrode at N
2Sintering is 1100 ℃ under the atmosphere, obtains monocell.The monocell cathode surface is coated elargol as current collector, and one is encapsulated on the quartz ampoule then, and anode and negative electrode are drawn wiring with silver-colored line respectively.SOFC places tube furnace to be heated to 750 ℃ in being sealed in quartz socket tube.During external gas circuit, gas is earlier through the outer tube sintering.Prepare one deck YSZ electrolytic thin-membrane in the anode-supported surface through spraying method, electrolytic thin-membrane obtains half-cell behind 1400 ℃ of sintering.The half-cell surface uses thick the reburning of spraying method deposition one deck SDC electrolyte to tie 1300 ℃.Sintering is 1000 ℃ behind SDC surface spraying preparation one deck BSCF electrode, obtains monocell.The monocell cathode surface is coated elargol as current collector, and one is encapsulated on the quartz ampoule then, and anode and negative electrode are drawn wiring with silver-colored line respectively.Monocell is sealed in the quartz socket tube again, places tube furnace to add 750 ℃.During external gas circuit, gas is crossed outer tube cathode earlier, passes through interior tube anode again, earlier feeding H
2With the anode reduction, it is 30% that reduction back Fe accounts for the anode mass fraction, feeds CH again
4And O
2Gaseous mixture (volume ratio 2: 1) just can generate electricity, and the monocell open circuit voltage is 0.92V in the time of 750 ℃, and the monocell maximum power density is 362mW/cm
2
Embodiment 7: with NiO and YSZ mixing and water adding and binding agent pugging, mechanical extrusion molding obtains anode support tube, and stay pipe is 1100 ℃ of sintering after super-dry.Prepare one deck YSZ electrolytic thin-membrane in the anode-supported surface through spraying method, electrolytic thin-membrane obtains half-cell behind 1400 ℃ of sintering.Thick 1300 ℃ of the knots of reburning of spraying method deposition one deck SDC electrolyte are used on half-cell surface, and the half-cell that makes use hydrogen reducing under 700 ℃ temperature, and the NiO of anode is reduced into Ni, and to account for the anode mass fraction be 70% to Ni after the reduction.Prepare one deck BSCF electrode in the spraying of SDC surface afterwards, last N
2Sintering is 1000 ℃ under the atmosphere, obtains monocell.The monocell cathode surface is coated elargol as current collector, and one is encapsulated on the quartz ampoule then, and anode and negative electrode are drawn wiring with silver-colored line respectively.Monocell is sealed in the quartz socket tube again, places tube furnace to be heated to 750 ℃.During external gas circuit, gas through outer tube cathode, passes through interior tube anode earlier again, directly feeds CH
4And air Mixture (volume ratio 1: 2) just can be generated electricity.
Embodiment 8: according to 1: 1 mixing and water adding and binding agent pugging, mechanical extrusion molding obtains anode support tube with NiO and YSZ, and stay pipe is 1100 ℃ of sintering after super-dry.Prepare one deck YSZ electrolytic thin-membrane in the anode-supported surface through spraying method, electrolytic thin-membrane obtains half-cell behind 1400 ℃ of sintering.Sintering is 1100 ℃ behind half-cell surface spraying preparation one deck LSM electrode, obtains monocell.The monocell cathode surface is coated elargol as current collector, and one is encapsulated on the quartz ampoule then, and anode and negative electrode are drawn wiring with silver-colored line respectively.Monocell is sealed in the quartz socket tube again, places tube furnace to be heated to 850 ℃.During external gas circuit, gas through outer tube cathode, passes through interior tube anode earlier again, and the anode inlet end is placed the catalyst of little amount of N i-YSZ mixed powder as methane-anode part oxidation, feeds CH again
4And O
2Gaseous mixture (volume ratio 3: 1) just can generate electricity, and the monocell open circuit voltage is 0.96V in the time of 700 ℃, and the monocell maximum power density is 457mW/cm
2
Embodiment 9: according to 3: 1 mixing and water addings and binding agent pugging, mechanical extrusion molding obtains anode support tube with NiO and YSZ, and stay pipe is 1100 ℃ of sintering after super-dry.Prepare one deck YSZ electrolytic thin-membrane in the anode-supported surface through spraying method, electrolytic thin-membrane obtains half-cell behind 1400 ℃ of sintering.The half-cell surface is used spraying method deposition one deck SDC electrolyte to reburn and is tied 1300 ℃.Sintering is 1000 ℃ behind SDC surface spraying preparation one deck BSCF electrode, obtains monocell.The monocell cathode surface is coated elargol as current collector, and one is encapsulated on the quartz ampoule then, and anode and negative electrode are drawn wiring with silver-colored line respectively.Monocell is sealed in the quartz socket tube again, places tube furnace to be heated to 750 ℃.During external gas circuit, gas through outer tube cathode, passes through interior tube anode earlier again, and the anode inlet end is placed the catalyst of little amount of N i-YSZ mixed powder as methane-anode part oxidation, feeds liquefied petroleum gas, argon gas and O again
2Gaseous mixture (volume ratio 2: 1: 1) just can generate electricity, and the monocell open circuit voltage is 0.99V in the time of 750 ℃, and the monocell maximum power density is 423mW/cm
2Cross section pattern SEM figure after the monocell test is as shown in Figure 4.
Embodiment 10: with NiO and SDC mixing and water adding and binding agent pugging, mechanical extrusion molding obtains anode support tube, and stay pipe is 1100 ℃ of sintering after super-dry.Prepare one deck SDC electrolytic thin-membrane in the anode-supported surface through spraying method, electrolytic thin-membrane obtains half-cell behind 1400 ℃ of sintering.Half-cell is used H under 700 ℃ temperature
2Reduction, it is 70% that reduction back Ni accounts for the anode mass fraction, the reduction back is spraying preparation one deck BSCF electrode on the half-cell surface, afterwards at N
2Sintering is 1000 ℃ under the atmosphere, obtains monocell.The monocell cathode surface is coated elargol as current collector, and one is encapsulated on the quartz ampoule then, and anode and negative electrode are drawn wiring with silver-colored line respectively.Monocell is sealed in the quartz socket tube again, places tube furnace to be heated to 750 ℃.During external gas circuit, gas through outer tube cathode, passes through interior tube anode earlier again, directly feeds ethene and air Mixture (volume ratio 1: 1) and just can generate electricity, and the monocell open circuit voltage is 0.98V in the time of 500 ℃, and the monocell maximum power density is 54mW/cm
2
Embodiment 11: combine Fig. 5 to describe present case, use casting method to prepare the NiO-YSZ anode support, supporter is 1100 ℃ of sintering after super-dry.Prepare one deck YSZ electrolytic thin-membrane in the anode-supported surface through spraying method, electrolytic thin-membrane obtains half-cell behind 1400 ℃ of sintering.Sintering is 1100 ℃ behind half-cell surface spraying preparation one deck LSM electrode, obtains monocell.The monocell cathode surface is coated elargol as current collector, and through the mode among Fig. 5 dull and stereotyped monocell is sealed on the stay pipe, and anode is in inside, negative electrode externally, anode and negative electrode are drawn wiring with silver-colored line respectively.Monocell is sealed in the outer tube again, places tube furnace to be heated to 750 ℃.During external gas circuit, gas through external cathode, passes through anode earlier again, feeds H earlier
2With the anode reduction, it is 40% that reduction back Ni accounts for the anode mass fraction, is feeding CH
3OH and O
2Gaseous mixture (volume ratio 2: 1) just can generate electricity, and the monocell open circuit voltage is 0.88V in the time of 750 ℃, and the monocell maximum power density is 47mW/cm
2
Claims (6)
1. single cavity SOFC that gas flow is controlled; It is characterized in that forming by SOFC (1), outer tube (2) and stay pipe (3); SOFC (1) links together with stay pipe (3) upper end, and fits together through seal (4) and outer tube (2); Two holes are arranged on the seal (4), and one of them hole is communicated with extraneous and outer tube (2) inside, as the inlet (A) or the outlet (B) of gas; A hole is used for fixing stay pipe (3) end at the center of seal (4), and the end of stay pipe (3) stretches out seal (4), as the outlet (B) or the inlet (A) of gas; SOFC (1) presents tubulose, is made up of for three layers negative electrode (1-1), electrolyte (1-2), anode (1-3); The gaseous mixture of the fuel-oxic gas of single cavity fuel cell passes through anode generation electrochemical reaction through negative electrode earlier again, and mist is by inlet (A) the entering system of gas, by outlet (B) discharge system.
2. single cavity SOFC that gas flow according to claim 1 is controlled, the configuration that it is characterized in that SOFC (1) are a kind of in anode support type, electrolyte-supporting type or the cathode support type; Its operating temperature is 500~900 ℃.
3. single cavity SOFC that gas flow according to claim 1 is controlled; It is characterized in that described electrolyte (1-2) is any one the perhaps any several kinds combination in stabilizing zirconia, doped cerium oxide or the doped lanthanum gallate, combination is to mix or the multilayer stack.
4. single cavity SOFC that gas flow according to claim 1 is controlled; It is characterized in that the mixture of described anode (1-3) for any one or several kinds in electrolyte (1-2) and Ni, Pt, Ag, Ru, Fe or the Cu metal simple-substance, wherein metal simple-substance accounts for the 10-90% of mixture gross mass.
5. single cavity SOFC that gas flow according to claim 1 is controlled is characterized in that described negative electrode (1-1) is electrolyte (1-2) and La
0.8Sr
0.2MnO
3, La
0.6Sr
0.4Co
0.2Fe
0.8O
3, Ba
0.5Sr
0.5Co
0.8Fe
0.2O, La
2NiO
4, PrBaCoO
5, Pt, Ag-Sm
0.2Ce
0.8O
1.9Or Ag-La
0.8Sr
0.2MnO
3In any one or a few mixture, wherein electrolyte accounts for the 10-90% of mixture gross mass.
6. single cavity SOFC that gas flow according to claim 1 is controlled is characterized in that described fuel-oxic gas gaseous mixture is 0~80% diluent gas by accounting for the gaseous mixture volume fraction, to account for the gaseous mixture volume fraction be the fuel gas of 10-90% and to account for the gaseous mixture volume fraction be that the oxic gas of 10-90% is formed; Wherein said diluent gas is nitrogen, argon gas or helium; Described fuel gas is alkane, alcohol, natural gas or liquefied petroleum gas; Described oxic gas is an air or oxygen.
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CN105244523A (en) * | 2015-08-28 | 2016-01-13 | 山西大学 | Solid oxide fuel cell with anti-carbon function |
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JP2008251277A (en) * | 2007-03-29 | 2008-10-16 | Dainippon Printing Co Ltd | Single chamber type solid oxide fuel cell system |
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JP2008251277A (en) * | 2007-03-29 | 2008-10-16 | Dainippon Printing Co Ltd | Single chamber type solid oxide fuel cell system |
US20090162723A1 (en) * | 2007-12-20 | 2009-06-25 | Zhongliang Zhan | Integrated Single-Chamber Solid Oxide Fuel Cells |
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