WO2015016599A1 - 고체 산화물 연료전지 및 이의 제조방법 - Google Patents
고체 산화물 연료전지 및 이의 제조방법 Download PDFInfo
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- WO2015016599A1 WO2015016599A1 PCT/KR2014/006980 KR2014006980W WO2015016599A1 WO 2015016599 A1 WO2015016599 A1 WO 2015016599A1 KR 2014006980 W KR2014006980 W KR 2014006980W WO 2015016599 A1 WO2015016599 A1 WO 2015016599A1
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- glass frit
- electrolyte
- precursor
- fuel cell
- solid oxide
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- 239000000446 fuel Substances 0.000 title claims abstract description 62
- 239000007787 solid Substances 0.000 title claims abstract description 46
- 238000000034 method Methods 0.000 title claims abstract description 30
- 238000004519 manufacturing process Methods 0.000 title abstract description 8
- 239000011521 glass Substances 0.000 claims description 88
- 239000003792 electrolyte Substances 0.000 claims description 87
- 239000002243 precursor Substances 0.000 claims description 54
- 239000000463 material Substances 0.000 claims description 25
- 238000010304 firing Methods 0.000 claims description 23
- 238000005245 sintering Methods 0.000 claims description 13
- 229910015902 Bi 2 O 3 Inorganic materials 0.000 claims description 11
- 229910004298 SiO 2 Inorganic materials 0.000 claims description 11
- 229910018072 Al 2 O 3 Inorganic materials 0.000 claims description 8
- 229910021193 La 2 O 3 Inorganic materials 0.000 claims description 7
- 229910010413 TiO 2 Inorganic materials 0.000 claims description 7
- 229910007472 ZnO—B2O3—SiO2 Inorganic materials 0.000 claims description 7
- 229910052760 oxygen Inorganic materials 0.000 claims description 7
- 238000002844 melting Methods 0.000 claims description 6
- 230000008018 melting Effects 0.000 claims description 6
- 229910044991 metal oxide Inorganic materials 0.000 claims description 6
- 150000004706 metal oxides Chemical class 0.000 claims description 6
- -1 B 2 O 3 Inorganic materials 0.000 claims description 5
- 238000010345 tape casting Methods 0.000 claims description 5
- 230000009477 glass transition Effects 0.000 claims description 4
- MRELNEQAGSRDBK-UHFFFAOYSA-N lanthanum(3+);oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[La+3].[La+3] MRELNEQAGSRDBK-UHFFFAOYSA-N 0.000 claims description 4
- RVTZCBVAJQQJTK-UHFFFAOYSA-N oxygen(2-);zirconium(4+) Chemical compound [O-2].[O-2].[Zr+4] RVTZCBVAJQQJTK-UHFFFAOYSA-N 0.000 claims description 4
- 229910001928 zirconium oxide Inorganic materials 0.000 claims description 4
- ODINCKMPIJJUCX-UHFFFAOYSA-N calcium oxide Inorganic materials [Ca]=O ODINCKMPIJJUCX-UHFFFAOYSA-N 0.000 claims description 3
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims description 2
- QVQLCTNNEUAWMS-UHFFFAOYSA-N barium oxide Inorganic materials [Ba]=O QVQLCTNNEUAWMS-UHFFFAOYSA-N 0.000 claims description 2
- 229910000416 bismuth oxide Inorganic materials 0.000 claims description 2
- 229910000420 cerium oxide Inorganic materials 0.000 claims description 2
- 239000002131 composite material Substances 0.000 claims 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 claims description 2
- 238000001035 drying Methods 0.000 claims description 2
- YEXPOXQUZXUXJW-UHFFFAOYSA-N lead(II) oxide Inorganic materials [Pb]=O YEXPOXQUZXUXJW-UHFFFAOYSA-N 0.000 claims description 2
- BMMGVYCKOGBVEV-UHFFFAOYSA-N oxo(oxoceriooxy)cerium Chemical compound [Ce]=O.O=[Ce]=O BMMGVYCKOGBVEV-UHFFFAOYSA-N 0.000 claims description 2
- 238000007650 screen-printing Methods 0.000 claims description 2
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 claims description 2
- 239000000126 substance Substances 0.000 claims 2
- 238000001878 scanning electron micrograph Methods 0.000 description 19
- 230000000052 comparative effect Effects 0.000 description 11
- 239000012528 membrane Substances 0.000 description 8
- 229910052712 strontium Inorganic materials 0.000 description 6
- 239000001301 oxygen Substances 0.000 description 5
- 229910001233 yttria-stabilized zirconia Inorganic materials 0.000 description 5
- 230000008901 benefit Effects 0.000 description 4
- 239000002001 electrolyte material Substances 0.000 description 4
- 229910021526 gadolinium-doped ceria Inorganic materials 0.000 description 4
- XEEYBQQBJWHFJM-UHFFFAOYSA-N iron Substances [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 4
- 229910052746 lanthanum Inorganic materials 0.000 description 4
- 239000010410 layer Substances 0.000 description 4
- 239000002245 particle Substances 0.000 description 4
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 3
- CETPSERCERDGAM-UHFFFAOYSA-N ceric oxide Chemical compound O=[Ce]=O CETPSERCERDGAM-UHFFFAOYSA-N 0.000 description 3
- 229910000422 cerium(IV) oxide Inorganic materials 0.000 description 3
- 239000001257 hydrogen Substances 0.000 description 3
- 229910052739 hydrogen Inorganic materials 0.000 description 3
- 229910052742 iron Inorganic materials 0.000 description 3
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 2
- 229910018921 CoO 3 Inorganic materials 0.000 description 2
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 2
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 description 2
- 229910052772 Samarium Inorganic materials 0.000 description 2
- 150000001875 compounds Chemical class 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 238000003487 electrochemical reaction Methods 0.000 description 2
- 239000007789 gas Substances 0.000 description 2
- 239000002346 layers by function Substances 0.000 description 2
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 2
- 239000010970 precious metal Substances 0.000 description 2
- 229910003099 (Y2O3)x(ZrO2)1−x Inorganic materials 0.000 description 1
- 229910019525 La0.6Sr0.4Co0.8Fe0.2O3 Inorganic materials 0.000 description 1
- 229910002204 La0.8Sr0.2MnO3 Inorganic materials 0.000 description 1
- KJTLSVCANCCWHF-UHFFFAOYSA-N Ruthenium Chemical compound [Ru] KJTLSVCANCCWHF-UHFFFAOYSA-N 0.000 description 1
- 241000968352 Scandia <hydrozoan> Species 0.000 description 1
- BQENXCOZCUHKRE-UHFFFAOYSA-N [La+3].[La+3].[O-][Mn]([O-])=O.[O-][Mn]([O-])=O.[O-][Mn]([O-])=O Chemical compound [La+3].[La+3].[O-][Mn]([O-])=O.[O-][Mn]([O-])=O.[O-][Mn]([O-])=O BQENXCOZCUHKRE-UHFFFAOYSA-N 0.000 description 1
- 239000000654 additive Substances 0.000 description 1
- 230000000996 additive effect Effects 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 239000003054 catalyst Substances 0.000 description 1
- 239000011195 cermet Substances 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 238000010344 co-firing Methods 0.000 description 1
- 229910017052 cobalt Inorganic materials 0.000 description 1
- 239000010941 cobalt Substances 0.000 description 1
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 description 1
- 230000007797 corrosion Effects 0.000 description 1
- 238000005260 corrosion Methods 0.000 description 1
- 239000013078 crystal Substances 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 230000002950 deficient Effects 0.000 description 1
- 239000012530 fluid Substances 0.000 description 1
- 150000002500 ions Chemical class 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 229910052759 nickel Inorganic materials 0.000 description 1
- PXHVJJICTQNCMI-UHFFFAOYSA-N nickel Substances [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 1
- 229910000480 nickel oxide Inorganic materials 0.000 description 1
- GNRSAWUEBMWBQH-UHFFFAOYSA-N oxonickel Chemical compound [Ni]=O GNRSAWUEBMWBQH-UHFFFAOYSA-N 0.000 description 1
- HJGMWXTVGKLUAQ-UHFFFAOYSA-N oxygen(2-);scandium(3+) Chemical compound [O-2].[O-2].[O-2].[Sc+3].[Sc+3] HJGMWXTVGKLUAQ-UHFFFAOYSA-N 0.000 description 1
- 229910052763 palladium Inorganic materials 0.000 description 1
- 239000012466 permeate Substances 0.000 description 1
- 229910052697 platinum Inorganic materials 0.000 description 1
- 238000010248 power generation Methods 0.000 description 1
- 238000010791 quenching Methods 0.000 description 1
- 230000000171 quenching effect Effects 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 238000006722 reduction reaction Methods 0.000 description 1
- 238000002407 reforming Methods 0.000 description 1
- 229910052707 ruthenium Inorganic materials 0.000 description 1
- KZUNJOHGWZRPMI-UHFFFAOYSA-N samarium atom Chemical compound [Sm] KZUNJOHGWZRPMI-UHFFFAOYSA-N 0.000 description 1
- FKTOIHSPIPYAPE-UHFFFAOYSA-N samarium(iii) oxide Chemical compound [O-2].[O-2].[O-2].[Sm+3].[Sm+3] FKTOIHSPIPYAPE-UHFFFAOYSA-N 0.000 description 1
- 241000894007 species Species 0.000 description 1
- 229910002076 stabilized zirconia Inorganic materials 0.000 description 1
- CIOAGBVUUVVLOB-UHFFFAOYSA-N strontium atom Chemical compound [Sr] CIOAGBVUUVVLOB-UHFFFAOYSA-N 0.000 description 1
- 239000002918 waste heat Substances 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
- RUDFQVOCFDJEEF-UHFFFAOYSA-N yttrium(III) oxide Inorganic materials [O-2].[O-2].[O-2].[Y+3].[Y+3] RUDFQVOCFDJEEF-UHFFFAOYSA-N 0.000 description 1
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- H01M8/028—Sealing means characterised by their material
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- C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
- C04B35/01—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics
- C04B35/48—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics based on zirconium or hafnium oxides, zirconates, zircon or hafnates
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Definitions
- the present specification relates to a solid oxide fuel cell and a method of manufacturing the same.
- Solid Oxide Fuel Cell called the 3rd generation fuel cell, is a fuel cell that uses solid oxide that can permeate oxygen or hydrogen ions as electrolyte.It was first operated by Bauer and Preis in 1937. It became. SOFCs operate at the highest temperatures (700 ° C. to 1000 ° C.) of existing fuel cells. Because all components are solid, the structure is simpler than other fuel cells, and there is no problem of electrolyte loss, replenishment and corrosion. It also operates at high temperatures, eliminating the need for precious metal catalysts and facilitating fuel supply through direct internal reforming. It also has the advantage that thermal combined cycle power generation using waste heat is possible because it emits hot gases. Because of these advantages, research on SOFC is being actively conducted with the aim of commercializing it at the beginning of the 21st century.
- a typical SOFC consists of an oxygen ion conductive electrolyte and an anode (cathode) and a fuel anode (anode) located on both sides thereof.
- Oxygen ions produced by the reduction reaction of oxygen in the cathode move through the electrolyte to the anode and react with hydrogen supplied to the anode to generate water.
- electrons are generated at the anode and electrons are consumed at the cathode.
- the basic principle of operation is to connect the two electrodes to each other to generate a current.
- 1 illustrates an example of an operation principle of a solid oxide fuel cell. That is, the current may be generated by the reaction of oxygen introduced through the cathode and hydrogen introduced through the anode.
- the air electrode and fuel electrode of SOFC should have high porosity, and the electrolyte provided between them should have a dense structure. Therefore, in order to prepare them, a pacing process is performed individually, and in particular, in the case of an electrolyte which should have a dense structure, the firing should be performed at a particularly high temperature. As a result, a warpage phenomenon occurs between the components according to the sintering temperature difference, and each component is fired separately, thereby increasing the process cost.
- the present specification provides a solid oxide fuel cell and a method of manufacturing the same that can solve the above problems.
- One embodiment of the present specification is an air electrode; Fuel electrode; And an electrolyte provided between the cathode and the anode, and at least one of the cathode, the anode, and the electrolyte includes a glass frit or a material derived from the glass frit.
- an exemplary embodiment of the present specification comprises the steps of preparing a cathode precursor; Preparing an electrolyte precursor; Preparing an anode precursor; Providing the electrolyte precursor between the cathode precursor and the anode precursor; And a firing step of simultaneously firing the cathode precursor, the electrolyte precursor, and the anode precursor, wherein at least one of the cathode precursor, the electrolyte precursor, and the anode precursor includes a glass frit. to provide.
- the solid oxide fuel cell according to the exemplary embodiment of the present specification may minimize the distortion at each interface of the cathode, the electrolyte, and the anode.
- the solid oxide fuel cell according to an exemplary embodiment of the present specification has an advantage that can be manufactured through one firing process.
- the solid oxide fuel cell according to the exemplary embodiment of the present specification may form an electrolyte having a dense structure despite the low temperature firing step.
- the solid oxide fuel cell according to the exemplary embodiment of the present specification has excellent process efficiency through the unification of the low temperature firing process and the firing step.
- FIG. 1 illustrates an example of an operation principle of a solid oxide fuel cell.
- FIG. 2 shows an SEM image according to Example 1.
- FIG. 3 shows an SEM image according to Example 2.
- FIG. 4 shows an SEM image according to Comparative Example 1.
- FIG. 5 shows an SEM image according to Example 3.
- FIG. 6 shows an SEM image according to Example 4.
- FIG. 8 shows an SEM image according to Example 5.
- FIG. 9 shows an SEM image according to Example 6.
- One embodiment of the present specification is an air electrode; Fuel electrode; And an electrolyte provided between the cathode and the anode, and at least one of the cathode, the anode, and the electrolyte includes a glass frit or a material derived from the glass frit.
- the glass frit or the material derived from the glass frit may be a sintering aid.
- the glass frit or the material derived from the glass frit of the present specification may serve to lower the sintering temperature during formation of the cathode, the anode, and / or the electrolyte.
- the glass frit of the present specification may serve to promote sintering and shorten the sintering time.
- the glass frit may be used without limitation as long as the glass frit is generally used.
- the glass frit may be an amorphous compound.
- the glass frit may refer to a powdery material that is ground as needed after melting and quenching the raw material of the amorphous compound.
- the glass frit is SiO 2 , B 2 O 3 , Al 2 O 3 , Bi 2 O 3 , PbO, CaO, BaO, LiO, MgO, Na 2 O, K 2 O, ZnO , MnO, ZrO 2 , V 2 O 5 , P 2 O 5 , Y 2 O 3 , SrO, GaO, Se 2 O 3 , TiO 2 and La 2 O 3 may include one or more selected from the group consisting of. have.
- the glass frit of the present specification may further include an additive in addition to the above configuration, and may be used without limitation as long as it is a general glass frit.
- the average particle diameter of the glass frit may be 500 nm or more and 20 ⁇ m or less.
- the firing temperature of the electrolyte can be smoothly lowered as a sintering aid. If it is less than the above range, the melting of the glass frit is too fast to cause a problem that the firing temperature can not be lowered sufficiently, if the above range is exceeded may cause a problem that can act as a defect area in the electrolyte.
- the glass transition temperature (Tg) of the glass frit may be 100 ° C to 800 ° C lower than the firing temperature of the solid oxide fuel cell.
- the glass transition temperature of the glass frit may mean a temperature at which a phase of the glass frit changes, which may mean a temperature at which the glass frit in a solid state changes to a liquid state.
- the glass frit is 100 ° C. to 800 ° C. lower than the firing temperature of the solid oxide fuel cell during firing for forming the solid oxide fuel cell. And / or may promote sintering of the precursor of the electrolyte and lower the sintering temperature.
- the glass transition temperature (Tg) of the glass frit may be 450 ° C or more and 900 ° C or less.
- the electrolyte may include the glass frit or a material derived from the glass frit.
- the glass frit may lower the sintering temperature of the electrolyte and may serve to reduce the sintering time.
- the electrolyte includes a glass frit or a material derived from the glass frit, and the electrolyte has a firing temperature of 1% to more than a state without a material derived from the glass frit or the glass frit. It may be 50% lower. Specifically, according to one embodiment of the present specification, the electrolyte may have a firing temperature of 1% to 15% lower than that of the glass frit or a material derived from the glass frit, or may be 5% to 10% lower. Can be.
- the content of the glass frit or the material derived from the glass frit may be 0.01 wt% or more and 10 wt% or less with respect to the total weight of the electrolyte.
- the content of the glass frit or the material derived from the glass frit is within the range, it is possible to improve the density of the electrolyte and to minimize side effects caused by the glass frit or the material derived from the glass frit in the electrolyte. Can be. Specifically, when the content exceeds the above range, a problem may occur in that the ionic conductivity of the electrolyte is lowered and a defective area may occur. In addition, when the content is less than the above range, there may be a problem that can not exhibit the effect of improving the density of the electrolyte by the glass frit or the material derived from the glass frit.
- the material derived from the glass frit may be a glass frit re-solidified after melting.
- the material derived from the glass frit may be included in the air electrode, the fuel electrode, and / or the electrolyte and undergo a sintering process to re-solidify the glass frit after melting.
- the material derived from the glass frit may include the electrolyte material in a process in which the glass frit is melted and mixed with the electrolyte material and then resolidified.
- the glass frit may be included in an electrolyte to constitute an electrolyte together with the electrolyte material in the electrolyte, and the glass frit may form the electrolyte in a more compact structure, and the electrolyte material It can play a role in making this tightly coupled.
- the glass frit is included in the electrolyte, and then becomes a fluid state during the sintering process, and may also be resolidified after moving to the anode and / or the cathode. That is, according to one embodiment of the present specification, the glass frit or a material derived from the glass frit may be included in the air electrode and / or the fuel electrode as well as the electrolyte.
- the porosity of the electrolyte may be 0% or more and 5% or less. Specifically, the closer the porosity of the electrolyte to 0%, the better the performance of the solid oxide fuel cell. This is because, when the movement of gas in the electrolyte occurs, the efficiency may be lowered.
- the solid oxide fuel cell may be manufactured by co-firing, distortion between interfaces may be minimized. That is, the bonding force of the joint surface of each structure can be excellent.
- the electrolyte may include a solid oxide having ion conductivity.
- the electrolyte is a composite metal oxide including one or more selected from the group consisting of zirconium oxide based, cerium oxide based, lanthanum oxide based, titanium oxide based, and bismuth oxide based materials. It may include. More specifically, the electrolyte may include yttria stabilized zirconia (YSZ), scandia stabilized zirconia (ScSZ), samaria doped ceria (SDC), and gadolinia doped ceria (GDC).
- YSZ yttria stabilized zirconia
- ScSZ scandia stabilized zirconia
- SDC samaria doped ceria
- GDC gadolinia doped ceria
- the YSZ is yttria stabilized zirconium oxide, and may be represented by (Y 2 O 3 ) x (ZrO 2 ) 1-x , and x may be 0.05 to 0.15.
- ScSZ is a Scandinavian stabilized zirconium oxide, which may be represented by (Sc 2 O 3 ) x (ZrO 2 ) 1-x , and x may be 0.05 to 0.15.
- the SDC is samarium dope ceria, and may be represented by (Sm 2 O 3 ) x (CeO 2 ) 1-x , and x may be 0.02 to 0.4.
- the GDC is gadolium dope ceria, and may be represented by (Gd 2 O 3 ) x (CeO 2 ) 1-x , and x may be 0.02 to 0.4.
- the thickness of the electrolyte may be 10 nm or more and 100 ⁇ m or less. More specifically, it may be 100 nm or more and 50 ⁇ m or less.
- the cathode may include a metal oxide.
- the cathode may be a metal oxide particle having a perovskite type crystal structure, (Sm, Sr) CoO 3 , (La, Sr) MnO 3 , (La, Sr) CoO 3 , (La, Sr) (Fe, Co) O 3 , (La, Sr) (Fe, Co, Ni) O 3 may include metal oxide particles, and the metal oxide may be used alone or in combination of two or more thereof. It may be included in the anode.
- the material for forming the air electrode may include a precious metal such as platinum, ruthenium, palladium.
- the air electrode may include La 0.8 Sr 0.2 MnO 3 (LSM), La 0.6 Sr 0.4 Co 0.8 Fe 0.2 O 3 (LSCF), and the like.
- the fuel electrode may use cermet in which a material and nickel oxide mixed in the aforementioned electrolyte are mixed. Furthermore, the anode may further include activated carbon.
- the solid oxide fuel cell includes a stack including an interconnect connecting two or more unit cells to each other; A fuel supply unit supplying fuel to the stack; And an air supply unit supplying air to the stack, wherein the unit cell may include the solid oxide fuel cell.
- the anode may include an anode support layer (ASL) and an anode functional layer (AFL).
- AFL may be a porous membrane, which may be provided between the ASL and the electrolyte membrane. More specifically, the ASL may be a region in which an electrochemical reaction occurs in contact with the electrolyte membrane.
- the ASL serves as a support layer of the anode, and for this purpose, may be formed relatively thicker than AFL.
- the ASL allows fuel to reach the AFL smoothly. Excellent electrical conductivity can be formed.
- the cathode may include a cathode support layer (CSL) and a cathode functional layer (CFL).
- CSL cathode support layer
- CFL cathode functional layer
- the CFL may be a porous membrane, which may be provided between the CSL and the electrolyte. More specifically, the CSL may be a region in contact with the electrolyte membrane, in which an electrochemical reaction occurs.
- the CSL serves as a support layer of the cathode, and for this purpose, may be formed relatively thicker than the CFL.
- the CSL allows air to reach the CFL smoothly. Excellent electrical conductivity can be formed.
- the interconnect may include a fuel flow path through which fuel may move to each unit cell, and an air flow path through which air may move to each unit cell.
- the stack may be a stack of two or more unit cells.
- the interconnect may include a fuel flow path and an air flow path connecting each unit cell.
- each stack of unit cells is stacked in series, and a separator may be further provided between the unit cells to electrically connect them.
- the solid oxide fuel cell may be a flat plate, cylindrical or flat tube.
- One embodiment of the present specification comprises the steps of preparing a cathode precursor; Preparing an electrolyte precursor; Preparing an anode precursor; Providing the electrolyte precursor between the cathode precursor and the anode precursor; And a firing step of simultaneously firing the cathode precursor, the electrolyte precursor, and the anode precursor, wherein at least one of the cathode precursor, the electrolyte precursor, and the anode precursor includes a glass frit. to provide.
- the temperature of the firing step may be 800 ° C or more and 1,600 ° C or less. Specifically, according to one embodiment of the present specification, the temperature of the firing step may be 1,000 ° C or more and 1,400 ° C or less.
- the electrolyte precursor may be a glass frit.
- the firing step may include the step of re-solidifying the glass frit after melting.
- preparing the cathode precursor; Preparing the electrolyte precursor; And preparing the anode precursors may each independently include a step of forming a film using a tape casting method or a screen printing method and then drying the film.
- a cathode precursor, YSZ containing 5 wt% of La 2 O 3 -B 2 O 3 -BaO-TiO 2 -based glass frit as an electrolyte precursor, and an anode precursor were respectively formed by tape casting. And these were laminated sequentially. Furthermore, the laminated film was fired at a temperature of 1,350 ° C. to manufacture a solid oxide fuel cell. In addition, in order to examine the density of the electrolyte membrane of the manufactured solid oxide fuel cell, the cross section of the electrolyte was confirmed by an electron microscope (SEM).
- FIG. 2 shows an SEM image according to Example 1.
- a solid oxide fuel cell was manufactured in the same manner as in Example 1, except that the content of the glass frit was 10% by weight, and the cross section of the electrolyte was confirmed by an electron microscope (SEM).
- FIG. 3 shows an SEM image according to Example 2.
- a solid oxide fuel cell was prepared in the same manner as in Example 1, and the cross section of the electrolyte was confirmed by an electron microscope (SEM).
- FIG. 4 shows an SEM image according to Comparative Example 1.
- Air electrode precursor as the electrolyte precursor to form a film with a La 2 O 3 -B 2 O 3 -BaO-TiO 2 based glass frit using a YSZ anode and each tape casting a precursor comprising 5% by weight relative to the total electrolyte precursor These were laminated sequentially. Furthermore, the laminated film was fired at a temperature of 1250 ° C. to manufacture a solid oxide fuel cell. In addition, in order to examine the density of the electrolyte membrane of the manufactured solid oxide fuel cell, the cross section of the electrolyte was confirmed by an electron microscope (SEM).
- SEM electron microscope
- FIG. 5 shows an SEM image according to Example 3.
- a solid oxide fuel cell was manufactured in the same manner as in Example 3, except that the content of the glass frit was 10 wt%, and the cross section of the electrolyte was confirmed by an electron microscope (SEM).
- FIG. 6 shows an SEM image according to Example 4.
- a solid oxide fuel cell was prepared in the same manner as in Example 3, and the cross section of the electrolyte was confirmed by an electron microscope (SEM).
- a film was formed by using a tape casting method of a cathode electrode and a GDC and an anode precursor each containing 5 wt% of La 2 O 3 -B 2 O 3 -BaO-TiO 2 -based glass frit as an electrolyte precursor. These were laminated sequentially. Furthermore, the laminated film was fired at a temperature of 1350 ° C. to manufacture a solid oxide fuel cell. In addition, in order to examine the density of the electrolyte membrane of the manufactured solid oxide fuel cell, the cross section of the electrolyte was confirmed by an electron microscope (SEM).
- FIG. 8 shows an SEM image according to Example 5.
- a solid oxide fuel cell was manufactured in the same manner as in Example 5, except that the content of the glass frit was 10% by weight, and the cross section of the electrolyte was confirmed by an electron microscope (SEM).
- FIG. 9 shows an SEM image according to Example 6.
- a solid oxide fuel cell was manufactured in the same manner as in Example 5, and the cross section of the electrolyte was confirmed by an electron microscope (SEM).
- the cross section of the electrolyte which contains the glass frit and is calcined, has a dense structure, compared to the cross section of the electrolyte that is not calcined and contains the glass frit.
- Example 4 SEM image in Example 4, even if calcined at a temperature of 1250 °C, it can be seen that the electrolyte having a more compact structure than the comparative example 1 calcined at 1350 °C.
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Abstract
Description
Claims (16)
- 공기극; 연료극; 및 상기 공기극 및 상기 연료극 사이에 구비된 전해질을 포함하고,상기 공기극, 상기 연료극, 및 상기 전해질 중 적어도 하나는 글라스 프릿 또는 상기 글라스 프릿으로부터 유래되는 물질을 포함하는 고체 산화물 연료전지.
- 청구항 1에 있어서,상기 글라스 프릿 또는 상기 글라스 프릿으로부터 유래되는 물질은 소결 조제인 것인 고체 산화물 연료전지.
- 청구항 1에 있어서,상기 글라스 프릿은 SiO2, B2O3, Al2O3, Bi2O3, PbO, CaO, BaO, LiO, MgO, Na2O, K2O, ZnO, MnO, ZrO2, V2O5, P2O5, Y2O3, SrO, GaO, Se2O3, TiO2 및 La2O3으로 이루어진 군에서 선택되는 1종 이상을 포함하는 것인 고체 산화물 연료전지.
- 청구항 1에 있어서,상기 글라스 프릿은 ZnO-SiO2 계, ZnO-B2O3-SiO2 계, ZnO-B2O3-SiO2-Al2O3 계, Bi2O3-SiO2 계, Bi2O3-B2O3-SiO2 계, Bi2O3-B2O3-SiO2-Al2O3 계, Bi2O3-ZnO-B2O3-SiO2 계, Bi2O3-ZnO-B2O3-SiO2-Al2O3 계, 및 La2O3-B2O3-BaO-TiO2 계 글라스 프릿으로 이루어진 군에서 선택되는 1종 이상을 포함하는 것인 고체 산화물 연료전지.
- 청구항 1에 있어서,상기 글라스 프릿의 유리전이온도(Tg)는 450 ℃ 이상 900 ℃ 이하인 것인 고체 산화물 연료전지.
- 청구항 1에 있어서,상기 전해질은 상기 글라스 프릿 또는 상기 글라스 프릿으로부터 유래된 물질을 포함하는 것인 고체 산화물 연료전지.
- 청구항 6에 있어서,상기 글라스 프릿 또는 상기 글라스 프릿으로부터 유래되는 물질의 함량은 상기 전해질 총중량에 대하여 0.01 중량% 이상 10 중량% 이하인 것인 고체 산화물 연료전지.
- 청구항 6에 있어서,상기 전해질은 상기 글라스 프릿 또는 글라스 프릿으로부터 유래되는 물질이 없는 상태보다 소성온도가 1 % 내지 50 % 더 낮은 것인 고체 산화물 연료전지.
- 청구항 1에 있어서,상기 글라스 프릿으로부터 유래되는 물질은 상기 글라스 프릿이 용융 후 재응고된 것인 고체 산화물 연료전지.
- 청구항 1에 있어서,상기 전해질의 공극률은 0 % 이상 5 % 이하인 것인 고체 산화물 연료전지.
- 청구항 1에 있어서,상기 전해질은 산화 지르코늄계, 산화 세륨계, 산화 란탄계, 산화 티타늄계, 산화 비스무스계물질로 이루어진 군에서 선택되는 1종 이상을 포함하는 복합 금속 산화물을 포함하는 것인 고체 산화물 연료전지.
- 청구항 1에 있어서,상기 고체산화물 연료전지는 평판형, 원통형 또는 평관형인 것인 고체산화물 연료전지.
- 공기극 전구체를 준비하는 단계;전해질 전구체를 준비하는 단계;연료극 전구체를 준비하는 단계;상기 공기극 전구체와 상기 연료극 전구체 사이에 상기 전해질 전구체를 구비하는 단계; 및상기 공기극 전구체, 상기 전해질 전구체 및 상기 연료극 전구체를 동시에 소성하는 소성 단계를 포함하고,상기 공기극 전구체, 상기 전해질 전구체 및 상기 연료극 전구체 중 적어도 하나는 글라스 프릿을 포함하는 고체 산화물 연료전지의 제조방법.
- 청구항 13에 있어서,상기 소성 단계의 온도는 800 ℃ 이상 1,600 ℃ 이하인 것인 고체 산화물 연료전지의 제조방법.
- 청구항 13에 있어서,상기 전해질 전구체는 글라스 프릿을 포함하는 것인 고체 산화물 연료전지의 제조방법.
- 청구항 13에 있어서,상기 공기극 전구체를 준비하는 단계; 상기 전해질 전구체를 준비하는 단계; 및 상기 연료극 전구체를 준비하는 단계는 각각 독립적으로, 테이프 캐스팅법 또는 스크린 프린팅법을 이용하여 막을 형성한 후 건조하는 단계를 포함하는 것인 고체 산화물 연료전지의 제조방법.
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JP2016525306A JP6240761B2 (ja) | 2013-07-31 | 2014-07-30 | 固体酸化物燃料電池およびその製造方法 |
US14/908,057 US9923213B2 (en) | 2013-07-31 | 2014-07-30 | Solid oxide fuel cell and method for manufacturing same |
US15/890,230 US10593966B2 (en) | 2013-07-31 | 2018-02-06 | Solid oxide fuel cell and method for manufacturing same |
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WO2016144067A1 (ko) * | 2015-03-06 | 2016-09-15 | 주식회사 엘지화학 | 전극의 제조방법, 이로 제조된 전극, 이를 포함하는 전극구조체, 연료전지 또는 금속공기이차전지, 상기 전지를 포함하는 전지모듈, 및 전극 제조용 조성물 |
KR20190044234A (ko) | 2017-10-20 | 2019-04-30 | 재단법인대구경북과학기술원 | 이중 도핑을 통해 고온안정성이 강화된 어븀-안정화 산화비스무트 (esb)계 전해질 |
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US10593966B2 (en) | 2020-03-17 |
US20180159149A1 (en) | 2018-06-07 |
US20160164114A1 (en) | 2016-06-09 |
US9923213B2 (en) | 2018-03-20 |
CN105409041B (zh) | 2018-11-09 |
JP2016525268A (ja) | 2016-08-22 |
JP6240761B2 (ja) | 2017-11-29 |
KR101672588B1 (ko) | 2016-11-03 |
CN105409041A (zh) | 2016-03-16 |
KR20150016118A (ko) | 2015-02-11 |
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