JP5177474B2 - セラミックス薄板体 - Google Patents
セラミックス薄板体 Download PDFInfo
- Publication number
- JP5177474B2 JP5177474B2 JP2007020822A JP2007020822A JP5177474B2 JP 5177474 B2 JP5177474 B2 JP 5177474B2 JP 2007020822 A JP2007020822 A JP 2007020822A JP 2007020822 A JP2007020822 A JP 2007020822A JP 5177474 B2 JP5177474 B2 JP 5177474B2
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- JP
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- Prior art keywords
- thin plate
- layer
- thin
- electrode layer
- plate member
- Prior art date
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- 239000000919 ceramic Substances 0.000 title claims description 37
- 239000000446 fuel Substances 0.000 claims description 164
- 239000003792 electrolyte Substances 0.000 claims description 98
- 238000012937 correction Methods 0.000 claims description 89
- 239000007784 solid electrolyte Substances 0.000 claims description 60
- 239000000463 material Substances 0.000 claims description 49
- 238000010030 laminating Methods 0.000 claims description 16
- 239000000758 substrate Substances 0.000 claims description 7
- 239000007787 solid Substances 0.000 claims description 5
- 238000003475 lamination Methods 0.000 claims description 4
- 239000012528 membrane Substances 0.000 claims 1
- 238000000034 method Methods 0.000 description 59
- 230000035882 stress Effects 0.000 description 34
- 238000006243 chemical reaction Methods 0.000 description 20
- 230000004048 modification Effects 0.000 description 18
- 238000012986 modification Methods 0.000 description 18
- 230000000694 effects Effects 0.000 description 14
- 238000004519 manufacturing process Methods 0.000 description 12
- 239000011195 cermet Substances 0.000 description 10
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 10
- 238000010304 firing Methods 0.000 description 9
- 229910052845 zircon Inorganic materials 0.000 description 8
- GFQYVLUOOAAOGM-UHFFFAOYSA-N zirconium(iv) silicate Chemical compound [Zr+4].[O-][Si]([O-])([O-])[O-] GFQYVLUOOAAOGM-UHFFFAOYSA-N 0.000 description 8
- 230000008569 process Effects 0.000 description 7
- 238000005520 cutting process Methods 0.000 description 6
- 229910002075 lanthanum strontium manganite Inorganic materials 0.000 description 6
- MCMNRKCIXSYSNV-UHFFFAOYSA-N ZrO2 Inorganic materials O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 description 5
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 5
- 229910052697 platinum Inorganic materials 0.000 description 5
- 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 4
- 238000005452 bending Methods 0.000 description 4
- 239000011159 matrix material Substances 0.000 description 4
- 230000001737 promoting effect Effects 0.000 description 4
- FVROQKXVYSIMQV-UHFFFAOYSA-N [Sr+2].[La+3].[O-][Mn]([O-])=O Chemical compound [Sr+2].[La+3].[O-][Mn]([O-])=O FVROQKXVYSIMQV-UHFFFAOYSA-N 0.000 description 3
- 239000007789 gas Substances 0.000 description 3
- 239000001301 oxygen Substances 0.000 description 3
- 229910052760 oxygen Inorganic materials 0.000 description 3
- 229910052709 silver Inorganic materials 0.000 description 3
- 239000004332 silver Substances 0.000 description 3
- 230000008646 thermal stress Effects 0.000 description 3
- 229910001233 yttria-stabilized zirconia Inorganic materials 0.000 description 3
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 2
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 2
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 description 2
- KJTLSVCANCCWHF-UHFFFAOYSA-N Ruthenium Chemical compound [Ru] KJTLSVCANCCWHF-UHFFFAOYSA-N 0.000 description 2
- GMPSWULASZPKFN-UHFFFAOYSA-N [O-2].[Ce+3].[Pt+2] Chemical compound [O-2].[Ce+3].[Pt+2] GMPSWULASZPKFN-UHFFFAOYSA-N 0.000 description 2
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 2
- 238000009792 diffusion process Methods 0.000 description 2
- 230000002401 inhibitory effect Effects 0.000 description 2
- 229910052746 lanthanum Inorganic materials 0.000 description 2
- FZLIPJUXYLNCLC-UHFFFAOYSA-N lanthanum atom Chemical compound [La] FZLIPJUXYLNCLC-UHFFFAOYSA-N 0.000 description 2
- 229910002119 nickel–yttria stabilized zirconia Inorganic materials 0.000 description 2
- 239000011148 porous material Substances 0.000 description 2
- 230000009467 reduction Effects 0.000 description 2
- 229910052707 ruthenium Inorganic materials 0.000 description 2
- 230000009466 transformation Effects 0.000 description 2
- OYPRJOBELJOOCE-UHFFFAOYSA-N Calcium Chemical compound [Ca] OYPRJOBELJOOCE-UHFFFAOYSA-N 0.000 description 1
- VYZAMTAEIAYCRO-UHFFFAOYSA-N Chromium Chemical compound [Cr] VYZAMTAEIAYCRO-UHFFFAOYSA-N 0.000 description 1
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 1
- 229910052581 Si3N4 Inorganic materials 0.000 description 1
- 229910052782 aluminium Inorganic materials 0.000 description 1
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 1
- 229910052791 calcium Inorganic materials 0.000 description 1
- 239000011575 calcium Substances 0.000 description 1
- 229910000420 cerium oxide Inorganic materials 0.000 description 1
- WEDXVUHOBZDVHR-UHFFFAOYSA-N cerium(3+) oxygen(2-) ruthenium(3+) Chemical compound [O-2].[Ce+3].[Ru+3].[O-2].[O-2] WEDXVUHOBZDVHR-UHFFFAOYSA-N 0.000 description 1
- 229910052804 chromium Inorganic materials 0.000 description 1
- 239000011651 chromium Substances 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
- 229910052963 cobaltite Inorganic materials 0.000 description 1
- 238000009826 distribution Methods 0.000 description 1
- 239000012530 fluid Substances 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 229910052742 iron Inorganic materials 0.000 description 1
- 229910000473 manganese(VI) oxide Inorganic materials 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- 229910052759 nickel Inorganic materials 0.000 description 1
- -1 oxygen ions Chemical class 0.000 description 1
- 229910052763 palladium Inorganic materials 0.000 description 1
- 229910002077 partially stabilized zirconia Inorganic materials 0.000 description 1
- 230000035699 permeability Effects 0.000 description 1
- 230000035939 shock Effects 0.000 description 1
- HBMJWWWQQXIZIP-UHFFFAOYSA-N silicon carbide Chemical compound [Si+]#[C-] HBMJWWWQQXIZIP-UHFFFAOYSA-N 0.000 description 1
- 229910010271 silicon carbide Inorganic materials 0.000 description 1
- HQVNEWCFYHHQES-UHFFFAOYSA-N silicon nitride Chemical compound N12[Si]34N5[Si]62N3[Si]51N64 HQVNEWCFYHHQES-UHFFFAOYSA-N 0.000 description 1
- 238000005549 size reduction 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
- 230000001629 suppression Effects 0.000 description 1
- 238000012360 testing method Methods 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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- H01M8/10—Fuel cells with solid electrolytes
- H01M8/12—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte
- H01M8/1213—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the electrode/electrolyte combination or the supporting material
- H01M8/122—Corrugated, curved or wave-shaped MEA
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B18/00—Layered products essentially comprising ceramics, e.g. refractory products
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- C04B37/001—Joining burned ceramic articles with other burned ceramic articles or other articles by heating directly with other burned ceramic articles
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- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/10—Fuel cells with solid electrolytes
- H01M8/12—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte
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- H01M8/1226—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the electrode/electrolyte combination or the supporting material characterised by the supporting layer
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- H01M8/12—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte
- H01M8/1286—Fuel cells applied on a support, e.g. miniature fuel cells deposited on silica supports
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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
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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
- Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
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- Y10T428/24—Structurally defined web or sheet [e.g., overall dimension, etc.]
- Y10T428/24479—Structurally defined web or sheet [e.g., overall dimension, etc.] including variation in thickness
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- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- Life Sciences & Earth Sciences (AREA)
- Manufacturing & Machinery (AREA)
- Sustainable Energy (AREA)
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- Organic Chemistry (AREA)
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- Fixed Capacitors And Capacitor Manufacturing Machines (AREA)
- Measuring Oxygen Concentration In Cells (AREA)
- Laminated Bodies (AREA)
Description
(1/2)・O2+2e−→O2− (於:空気極層13) …(1)
H2+O2−→H2O+2e− (於:燃料極層12) …(2)
次に、第1実施形態に係る薄板体10の構造について詳細に説明する。前述したように、薄板体10は、平面視において正方形である。斜視図である図3に示したように、薄板体10の一辺の長さa及び同一辺に直交する他の辺の長さbは、5mm以上且つ200mm以下である。
次に、本発明の第1実施形態の変形例に係る薄板体40について説明する。薄板体40も、平面視において正方形である。斜視図である図6に示したように、薄板体40の一辺の長さa及び同一辺に直交する他の辺の長さbは、5mm以上且つ200mm以下である。
次に、第2実施形態に係る薄板体50の構造について詳細に説明する。薄板体50は、平面視において正方形である。斜視図である図9に示したように、薄板体50の一辺の長さa及び同一辺に直交する他の辺の長さbは、5mm以上且つ200mm以下である。
次に、第3実施形態に係る薄板体60の構造について詳細に説明する。薄板体60は、平面視において正方形である。斜視図である図12に示したように、薄板体60の一辺の長さa及び同一辺に直交する他の辺の長さbは、5mm以上且つ200mm以下である。
次に、本発明の第3実施形態の第1変形例に係る薄板体70について説明する。薄板体70も、平面視において正方形である。斜視図である図15に示したように、薄板体70の一辺の長さa及び同一辺に直交する他の辺の長さbは、5mm以上且つ200mm以下である。
次に、本発明の第3実施形態の第2変形例に係る薄板体80について説明する。薄板体80も、平面視において正方形である。斜視図である図18に示したように、薄板体80の一辺の長さa及び同一辺に直交する他の辺の長さbは、5mm以上且つ200mm以下である。
本発明に係る薄板体は、斜視図である図21に示した薄板体100であってもよい。図22は、図21において長さbの辺に平行な21−21線を含むとともに薄板体100の平面に垂直な平面に沿って薄板体100を切断した薄板体100の一部断面図である。薄板体100も平面視において正方形である。
1.薄肉部の厚さが5μm未満では熱応力により基板全体にクラックが入った。これは、薄肉部の厚さが5μm未満では反り矯正層95による反り矯正応力に基板が耐えられなかったことに基づくと思われる。
2.薄肉部の厚さが5μm以上であれば各種厚さの試験片が作成可能であったが、薄肉部の厚さが100μmを超えると基板の強度が十分であるため、薄肉部の変形(反り)による基板の反り低減の効果は確認されなかった。
3.厚肉部と薄肉部の厚さの差が300μmを超えると、薄肉部にクラックが入った。これは、厚肉部が十分な強度を有するために薄肉部の変形が抑制され、薄肉部と厚肉部の境界、即ち、薄肉部の端部に応力が集中したことに基づくと考えることができる。
1.薄肉部の厚さは、5μm以上且つ100μm以下であって、厚肉部と薄肉部の厚さの差は10μm以上且つ300μm以下が好ましい。
2.薄肉部の反り量が僅かであっても基板全体の変形抑制(反り抑制)に効果があるとともに、薄肉部の反り量が100μmを超えると、むしろ薄肉部の端部からクラックが導入され破壊に至ることがわかった。
Claims (21)
- 少なくともセラミックス層を含む焼成された薄板体であって、
それぞれの材質の熱膨張率が相違する2種以上の層が積層されてなる前記薄板体の部分である薄肉部と、少なくとも前記薄肉部を構成する層の全てを含む複数の層が積層されてなる前記薄肉部よりも厚さの大きい前記薄板体の部分である厚肉部と、を備え、
前記薄肉部は、前記薄板体の平面に垂直な方向に反った形状を有する薄板体。 - 請求項1に記載の薄板体であって、
前記薄肉部の厚さが5μm以上且つ100μm以下であり、前記厚肉部の厚さと前記薄肉部の厚さとの差が10μm以上且つ300μm以下である薄板体。 - 請求項2に記載の薄板体であって、
前記薄肉部は、1つ又は複数設けられ、
前記薄板体の平面に垂直な方向に対する各薄肉部の正射影面積は、1mm2以上且つ100mm2以下であり、各薄肉部における反りの前記平面に垂直な方向の高さは、1μm以上且つ100μm以下である薄板体。 - 請求項3に記載の薄板体であって、
前記薄板体の平面に垂直な方向に対する各薄肉部の正射影形状は、円形、楕円形、正方形、又は長方形であり、前記円形の直径、前記楕円形の長径、前記正方形の1辺の長さ、又は前記長方形の長辺の長さは、10mm以下である薄板体。 - 請求項1乃至請求項4の何れか一項に記載の薄板体であって、
前記薄肉部及び前記厚肉部は、前記セラミックス層としての固体電解質層と、前記固体電解質層の一面に形成された燃料極層と、前記固体電解質層の他面に形成された空気極層とが積層されてなり、
前記厚肉部における何れか1つの層の厚さが、前記薄肉部における対応する層の厚さよりも大きい薄板体。 - 請求項5に記載の薄板体において、
前記厚肉部における前記固体電解質層の厚さが、前記薄肉部における前記固体電解質層の厚さよりも大きい薄板体。 - 請求項6に記載の薄板体において、
前記厚肉部における前記固体電解質層の厚さと、前記薄肉部における前記固体電解質層の厚さとの差は、10μm以上且つ300μm以下である薄板体。 - 請求項5に記載の薄板体において、
前記厚肉部における前記燃料極層の厚さが、前記薄肉部における前記燃料極層の厚さよりも大きい薄板体。 - 請求項8に記載の薄板体において、
前記厚肉部における前記燃料極層の厚さと、前記薄肉部における前記燃料極層の厚さとの差は、10μm以上且つ300μm以下である薄板体。 - 請求項1乃至請求項4の何れか一項に記載の薄板体であって、
前記薄肉部は、前記セラミックス層としての固体電解質層と、前記固体電解質層の一面に形成された燃料極層と、前記固体電解質層の他面に形成された空気極層とが積層されてなり、
前記厚肉部は、前記薄肉部を構成する前記固体電解質層、前記燃料極層、及び前記空気極層の積層体の表面に、熱膨張率の相違に起因して発生する前記薄板体の反りを低減するための層である反り矯正層が積層されてなる薄板体。 - 請求項10に記載の薄板体において、
前記反り矯正層として、前記燃料極層の表面に前記固体電解質層の熱膨張率よりも熱膨張率の小さい材質からなる層が積層されている薄板体。 - 請求項10に記載の薄板体において、
前記反り矯正層として、前記空気極層の表面に前記固体電解質層の熱膨張率よりも熱膨張率の大きい材質からなる層が積層されている薄板体。 - 請求項10に記載の薄板体において、
前記反り矯正層として、前記燃料極層の表面に前記固体電解質層の熱膨張率よりも熱膨張率の小さい材質からなる層が積層され、前記空気極層の表面に前記固体電解質層の熱膨張率よりも熱膨張率の大きい材質からなる層が積層されている薄板体。 - 請求項10に記載の薄板体において、
前記反り矯正層として、前記燃料極層の表面に前記燃料極層の熱膨張率よりも熱膨張率の小さい材質からなる層が積層されている薄板体。 - 請求項10に記載の薄板体において、
前記反り矯正層として、前記空気極層の表面に前記空気極層の熱膨張率よりも熱膨張率の大きい材質からなる層が積層されている薄板体。 - 請求項10に記載の薄板体において、
前記反り矯正層として、前記燃料極層の表面に前記燃料極層の熱膨張率よりも熱膨張率の小さい材質からなる層が積層され、前記空気極層の表面に前記空気極層の熱膨張率よりも熱膨張率の大きい材質からなる層が積層されている薄板体。 - 請求項1乃至請求項4の何れか一項に記載の薄板体であって、
前記薄肉部は、前記セラミックス層としての固体電解質層と、前記固体電解質層の一面に形成された燃料極層と、前記固体電解質層の他面に形成された空気極層とが積層されてなり、
前記厚肉部は、前記薄肉部を構成する前記固体電解質層、前記燃料極層、及び前記空気極層の積層体において、前記燃料極層の内部に、前記固体電解質層の熱膨張率よりも熱膨張率の小さい材質からなるとともに熱膨張率の相違に起因して発生する前記薄板体の反りを低減するための層である反り矯正層が埋設されてなる薄板体。 - 請求項17に記載の薄板体において、
前記厚肉部には、前記空気極層の表面に前記固体電解質層の熱膨張率よりも熱膨張率の大きい材質からなるとともに熱膨張率の相違に起因して発生する前記薄板体の反りを低減するための層である第2の反り矯正層が積層されている薄板体。 - 請求項1乃至請求項4の何れか一項に記載の薄板体であって、
前記薄肉部は、前記セラミックス層としての固体電解質層と、前記固体電解質層の一面に形成された燃料極層と、前記固体電解質層の他面に形成された空気極層とが積層されてなり、
前記厚肉部は、前記薄肉部を構成する前記固体電解質層、前記燃料極層、及び前記空気極層の積層体において、前記燃料極層の内部に、前記燃料極層の熱膨張率よりも熱膨張率の小さい材質からなるとともに熱膨張率の相違に起因して発生する前記薄板体の反りを低減するための層である反り矯正層が埋設されてなる薄板体。 - 請求項19に記載の薄板体において、
前記厚肉部には、前記空気極層の表面に前記空気極層の熱膨張率よりも熱膨張率の大きい材質からなるとともに熱膨張率の相違に起因して発生する前記薄板体の反りを低減するための層である第2の反り矯正層が積層されている薄板体。 - 請求項11乃至請求項20の何れか一項に記載の薄板体において、
前記各反り矯正層の厚さは、10μm以上且つ100μm以下である薄板体。
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