JP2006523002A - セリア系電解質の高密度化 - Google Patents
セリア系電解質の高密度化 Download PDFInfo
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- 239000003792 electrolyte Substances 0.000 title claims abstract description 109
- CETPSERCERDGAM-UHFFFAOYSA-N ceric oxide Chemical compound O=[Ce]=O CETPSERCERDGAM-UHFFFAOYSA-N 0.000 title claims abstract description 19
- 229910000422 cerium(IV) oxide Inorganic materials 0.000 title claims abstract description 19
- 238000000280 densification Methods 0.000 title description 10
- 150000001768 cations Chemical class 0.000 claims abstract description 124
- 238000004519 manufacturing process Methods 0.000 claims abstract description 20
- 238000000034 method Methods 0.000 claims description 44
- 239000000758 substrate Substances 0.000 claims description 29
- 238000005245 sintering Methods 0.000 claims description 26
- 229910052751 metal Inorganic materials 0.000 claims description 25
- 239000002184 metal Substances 0.000 claims description 25
- 230000008569 process Effects 0.000 claims description 14
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 11
- 239000001301 oxygen Substances 0.000 claims description 11
- 229910052760 oxygen Inorganic materials 0.000 claims description 11
- 239000000446 fuel Substances 0.000 claims description 6
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 3
- 239000000463 material Substances 0.000 claims description 2
- 230000002194 synthesizing effect Effects 0.000 claims description 2
- 238000007792 addition Methods 0.000 description 14
- 239000008188 pellet Substances 0.000 description 12
- 230000003647 oxidation Effects 0.000 description 8
- 238000007254 oxidation reaction Methods 0.000 description 8
- 239000012300 argon atmosphere Substances 0.000 description 6
- 230000000694 effects Effects 0.000 description 6
- 239000012535 impurity Substances 0.000 description 6
- 238000011109 contamination Methods 0.000 description 5
- 239000011888 foil Substances 0.000 description 5
- 239000000843 powder Substances 0.000 description 5
- 230000002411 adverse Effects 0.000 description 4
- 238000006243 chemical reaction Methods 0.000 description 4
- 238000012545 processing Methods 0.000 description 4
- 229910001220 stainless steel Inorganic materials 0.000 description 4
- 229910052723 transition metal Inorganic materials 0.000 description 4
- -1 transition metal cations Chemical class 0.000 description 4
- 229910002484 Ce0.9Gd0.1O1.95 Inorganic materials 0.000 description 3
- 229910052804 chromium Inorganic materials 0.000 description 3
- 239000007789 gas Substances 0.000 description 3
- 229910052742 iron Inorganic materials 0.000 description 3
- 230000009467 reduction Effects 0.000 description 3
- 125000002091 cationic group Chemical group 0.000 description 2
- 230000008859 change Effects 0.000 description 2
- 230000001627 detrimental effect Effects 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- 238000002474 experimental method Methods 0.000 description 2
- 229910052748 manganese Inorganic materials 0.000 description 2
- 239000012528 membrane Substances 0.000 description 2
- 230000005012 migration Effects 0.000 description 2
- 238000013508 migration Methods 0.000 description 2
- 239000000203 mixture Substances 0.000 description 2
- 239000007787 solid Substances 0.000 description 2
- OVSKIKFHRZPJSS-UHFFFAOYSA-N 2,4-D Chemical compound OC(=O)COC1=CC=C(Cl)C=C1Cl OVSKIKFHRZPJSS-UHFFFAOYSA-N 0.000 description 1
- 229910018072 Al 2 O 3 Inorganic materials 0.000 description 1
- 229910001030 Iron–nickel alloy Inorganic materials 0.000 description 1
- 239000000654 additive Substances 0.000 description 1
- 230000000996 additive effect Effects 0.000 description 1
- 150000001450 anions Chemical class 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- VNNRSPGTAMTISX-UHFFFAOYSA-N chromium nickel Chemical compound [Cr].[Ni] VNNRSPGTAMTISX-UHFFFAOYSA-N 0.000 description 1
- 239000011248 coating agent Substances 0.000 description 1
- 238000000576 coating method Methods 0.000 description 1
- 230000007423 decrease Effects 0.000 description 1
- 238000000151 deposition Methods 0.000 description 1
- 230000006866 deterioration Effects 0.000 description 1
- 238000009826 distribution Methods 0.000 description 1
- 238000000462 isostatic pressing Methods 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- 230000007246 mechanism Effects 0.000 description 1
- 229910000000 metal hydroxide Inorganic materials 0.000 description 1
- 150000004692 metal hydroxides Chemical class 0.000 description 1
- 229910044991 metal oxide Inorganic materials 0.000 description 1
- 150000004706 metal oxides Chemical class 0.000 description 1
- 238000003801 milling Methods 0.000 description 1
- 229910001120 nichrome Inorganic materials 0.000 description 1
- RJSRQTFBFAJJIL-UHFFFAOYSA-N niobium titanium Chemical compound [Ti].[Nb] RJSRQTFBFAJJIL-UHFFFAOYSA-N 0.000 description 1
- 238000005457 optimization Methods 0.000 description 1
- 238000013386 optimize process Methods 0.000 description 1
- 239000002245 particle Substances 0.000 description 1
- 230000001737 promoting effect Effects 0.000 description 1
- 230000001681 protective effect Effects 0.000 description 1
- 238000005204 segregation Methods 0.000 description 1
- 239000010935 stainless steel Substances 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 230000008719 thickening Effects 0.000 description 1
- 238000003466 welding Methods 0.000 description 1
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Abstract
Description
製造した電解質中の二価のカチオンの濃度を決定することと;
製造した電解質中の三価のカチオンの濃度を決定することと、前記二価のカチオンの濃度から三価のカチオンの調整された濃度を差し引いて二価のカチオンの有効濃度を出すことと
を含む、製造した電解質中の二価のカチオンの有効濃度の決定方法が提供される。三価のカチオンの悪影響のために、以下に記載するように、測定された濃度に5から10の間のファクターを掛ける必要がある。
電解質に付属した金属基板又は該基板上の酸化物層によって生成した蒸気から二価のカチオンを受け取ること;
基板材料中の三価のカチオンを二価のカチオンに還元すること;又は
製造の前又は間に二価のカチオンを電解質に特別に添加すること;
の1つ以上によって二価のカチオンの濃度を上昇させることを含む。
図1は、カチオンを0、1%及び2%添加したセリア系電解質ペレットの焼結特性を示し;
図2は、カチオンを0及び0.1%添加したセリア系電解質ペレットの焼結特性を示し;
図3は、金属箔で支持された厚膜のセル組立体の略図である。
[ME 2+]=[MA 2+]+[MI 2+]−Y[MI 3+] ・・・ (A)
Claims (33)
- 製造した電解質中の二価のカチオンの濃度を決定することと、
製造した電解質中の三価のカチオンの濃度を決定することと、
前記二価のカチオンの濃度から三価のカチオンの調整された濃度を差し引いて二価のカチオンの有効濃度を出すことと
を特徴とする、製造した電解質中の二価のカチオンの有効濃度の決定方法。 - 製造プロセスの完了前に電解質に加えられた二価のカチオンの濃度を、添加がない製造プロセスの後に電解質中に存在することが決定された二価のカチオンの濃度に加えることによって、前記製造した電解質中の二価のカチオンの濃度を決定することを特徴とする請求項1に記載の方法。
- 三価のカチオンを二価のカチオンに転換又は還元することによって、電解質中で二価のカチオンの少なくとも一部を生成させることを特徴とする請求項1又は2に記載の方法。
- 製造プロセスの間に三価のカチオンを二価のカチオンに転換又は還元することを特徴とする請求項3に記載の方法。
- 焼結炉中の酸素又は水の分圧を適切にコントロールすることによって、製造プロセスの間に三価のカチオンを二価のカチオンに転換又は還元することを特徴とする請求項4に記載の方法。
- 製造プロセスの完了前に電解質に二価のカチオンを加えることを特徴とする請求項1〜5のいずれかに記載の方法。
- 前記電解質中の二価のカチオンの少なくとも一部が、金属基板又は金属基板上の酸化物層から生成した蒸気を起源とすることを特徴とする請求項1〜6のいずれかに記載の方法。
- 二価のカチオンの有効濃度が0.01モル%以上0.1モル%以下になるように、前記カチオンの濃度をコントロールすることを特徴とする請求項1〜7のいずれかに記載の方法。
- 二価のカチオンの有効濃度を0.02モル%以上0.09モル%以下にすることを特徴とする請求項8に記載の方法。
- 二価のカチオンの有効濃度を0.03モル%以上0.08モル%以下にすることを特徴とする請求項9に記載の方法。
- 5から10の間の係数による通常の掛け算によって、決定された三価のカチオンの濃度を調整することを特徴とする請求項1〜10のいずれかに記載の方法。
- セリア系電解質を形成することと、
焼結された電解質中の二価のカチオンの濃度から三価のカチオンの調整された濃度を差し引いた値が0.01モル%から0.1モル%になるように、前記電解質を1200℃以下で焼結することと
を特徴とする、理論的に達成可能な密度の97%より高い密度を有するセリア系電解質の合成方法。 - 焼結プロセスの条件をコントロールして、電解質中の三価のカチオンの少なくとも一部を二価のカチオンに還元することを特徴とする請求項12に記載の方法。
- 焼結プロセスの条件をコントロールして適切な酸素又は水圧力を形成し、適切な量の三価のカチオンを二価のカチオンに還元することを特徴とする請求項13に記載の方法。
- 前記電解質を基板上に設け、該基板の材料を選択して、電解質中における二価のカチオンの濃度から三価のカチオンの調整された濃度を差し引いた値が要求される値になるようにすることを特徴とする請求項12,13又は14に記載の方法。
- 前記電解質と前記基板との間に電極を設けることを特徴とする請求項15に記載の方法。
- 焼結プロセスの前又は間に、前記電解質に二価のカチオンを加えることを特徴とする請求項12〜16のいずれかに記載の方法。
- 焼結された電解質中における二価のカチオンの濃度から三価のカチオンの調整された濃度を差し引いた値が0.02モル%以上0.09モル%以下であることを特徴とする請求項12〜17のいずれかに記載の方法。
- 焼結された電解質中における二価のカチオンの濃度から三価のカチオンの調整された濃度を差し引いた値が0.03モル%以上0.08モル%以下であることを特徴とする請求項18に記載の方法。
- 5から10の間の数による掛け算によって、前記三価のカチオンの濃度を調整することを特徴とする請求項12〜19のいずれかに記載の方法。
- 前記電解質を1100℃以下で焼結することを特徴とする請求項12〜20のいずれかに記載の方法。
- 前記電解質を1050℃以下で焼結することを特徴とする請求項21に記載の方法。
- 前記電解質を1000℃以下で焼結することを特徴とする請求項22に記載の方法。
- 前記電解質を厚膜として設けることを特徴とする請求項12〜23のいずれかに記載の方法。
- 理論的に達成可能な密度の97%より高い密度を有し、二価のカチオンの濃度から三価のカチオンの調整された濃度を差し引いた値が0.01モル%以上0.1モル%以下であることを特徴とする、セリア系電解質。
- 二価のカチオンの濃度から三価のカチオンの調整された濃度を差し引いた値が0.02モル%以上0.09モル%以下であることを特徴とする請求項25に記載の電解質。
- 二価のカチオンの濃度から三価のカチオンの調整された濃度を差し引いた値が0.03モル%以上0.08モル%以下であることを特徴とする請求項26に記載の電解質。
- 前記三価のカチオンの濃度が、5から10の間の数による掛け算によって調整されていることを特徴とする請求項25〜27のいずれかに記載の電解質。
- 前記電解質が、厚膜として設けられていることを特徴とする請求項25〜28のいずれかに記載の電解質。
- 基板と、電極と、請求項25〜29のいずれかに記載の電解質とを備えることを特徴とする半電池組立体。
- 請求項30に記載の半電池組立体と、第1の前記電極から見て電解質の反対側に設けられた他の電極とを備えることを特徴とする燃料電池。
- 第1の前記電極がアノードであり、前記他の電極がカソードであることを特徴とする請求項31に記載の燃料電池。
- 請求項30に記載の半電池組立体と、第1の前記電極から見て電解質の反対側に設けられた他の電極とを備えることを特徴とする酸素発生機。
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