TW483876B - Ceramic material for use in the separation of oxygen from gas mixture - Google Patents
Ceramic material for use in the separation of oxygen from gas mixture Download PDFInfo
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- TW483876B TW483876B TW088104005A TW88104005A TW483876B TW 483876 B TW483876 B TW 483876B TW 088104005 A TW088104005 A TW 088104005A TW 88104005 A TW88104005 A TW 88104005A TW 483876 B TW483876 B TW 483876B
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- 229910010293 ceramic material Inorganic materials 0.000 title claims abstract description 14
- 239000000203 mixture Substances 0.000 title claims description 9
- 239000001301 oxygen Substances 0.000 title description 3
- 229910052760 oxygen Inorganic materials 0.000 title description 3
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 title description 2
- 238000000926 separation method Methods 0.000 title description 2
- 239000007789 gas Substances 0.000 title 1
- 229910052751 metal Inorganic materials 0.000 claims abstract description 11
- 239000002184 metal Substances 0.000 claims abstract description 11
- 150000002739 metals Chemical class 0.000 claims abstract description 4
- -1 lanthanide metals Chemical class 0.000 claims abstract description 3
- 229910052723 transition metal Inorganic materials 0.000 claims abstract description 3
- 150000003624 transition metals Chemical class 0.000 claims abstract description 3
- 229910000510 noble metal Inorganic materials 0.000 claims abstract 2
- 239000000463 material Substances 0.000 claims description 9
- 239000000919 ceramic Substances 0.000 claims description 5
- 230000002079 cooperative effect Effects 0.000 claims description 4
- 150000002500 ions Chemical class 0.000 claims description 4
- 229910052684 Cerium Inorganic materials 0.000 claims description 2
- 229910052779 Neodymium Inorganic materials 0.000 claims description 2
- 229910052777 Praseodymium Inorganic materials 0.000 claims description 2
- 229910000831 Steel Inorganic materials 0.000 claims description 2
- 229910052784 alkaline earth metal Inorganic materials 0.000 claims description 2
- 150000001342 alkaline earth metals Chemical class 0.000 claims description 2
- 230000000737 periodic effect Effects 0.000 claims description 2
- 239000010970 precious metal Substances 0.000 claims description 2
- 239000010959 steel Substances 0.000 claims description 2
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 claims 1
- 238000004519 manufacturing process Methods 0.000 claims 1
- 229910052719 titanium Inorganic materials 0.000 claims 1
- 239000010936 titanium Substances 0.000 claims 1
- 229910052747 lanthanoid Inorganic materials 0.000 abstract 1
- 239000000126 substance Substances 0.000 description 6
- 150000001875 compounds Chemical class 0.000 description 5
- 239000003054 catalyst Substances 0.000 description 3
- 238000000034 method Methods 0.000 description 3
- 239000000843 powder Substances 0.000 description 3
- DHMQDGOQFOQNFH-UHFFFAOYSA-N Glycine Chemical compound NCC(O)=O DHMQDGOQFOQNFH-UHFFFAOYSA-N 0.000 description 2
- 239000013078 crystal Substances 0.000 description 2
- 239000000446 fuel Substances 0.000 description 2
- 230000003647 oxidation Effects 0.000 description 2
- 238000007254 oxidation reaction Methods 0.000 description 2
- 238000000197 pyrolysis Methods 0.000 description 2
- 239000000243 solution Substances 0.000 description 2
- QTBSBXVTEAMEQO-UHFFFAOYSA-M Acetate Chemical compound CC([O-])=O QTBSBXVTEAMEQO-UHFFFAOYSA-M 0.000 description 1
- OYPRJOBELJOOCE-UHFFFAOYSA-N Calcium Chemical compound [Ca] OYPRJOBELJOOCE-UHFFFAOYSA-N 0.000 description 1
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 description 1
- WQZGKKKJIJFFOK-GASJEMHNSA-N Glucose Natural products OC[C@H]1OC(O)[C@H](O)[C@@H](O)[C@@H]1O WQZGKKKJIJFFOK-GASJEMHNSA-N 0.000 description 1
- 239000007864 aqueous solution Substances 0.000 description 1
- WQZGKKKJIJFFOK-VFUOTHLCSA-N beta-D-glucose Chemical compound OC[C@H]1O[C@@H](O)[C@H](O)[C@@H](O)[C@@H]1O WQZGKKKJIJFFOK-VFUOTHLCSA-N 0.000 description 1
- 229910052791 calcium Inorganic materials 0.000 description 1
- 239000011575 calcium Substances 0.000 description 1
- 239000010406 cathode material Substances 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 239000003792 electrolyte Substances 0.000 description 1
- 239000008103 glucose Substances 0.000 description 1
- 229960002449 glycine Drugs 0.000 description 1
- 235000013905 glycine and its sodium salt Nutrition 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- 230000002452 interceptive effect Effects 0.000 description 1
- 229910052746 lanthanum Inorganic materials 0.000 description 1
- FZLIPJUXYLNCLC-UHFFFAOYSA-N lanthanum atom Chemical compound [La] FZLIPJUXYLNCLC-UHFFFAOYSA-N 0.000 description 1
- 238000002356 laser light scattering Methods 0.000 description 1
- 229910001960 metal nitrate Inorganic materials 0.000 description 1
- 229910044991 metal oxide Inorganic materials 0.000 description 1
- 150000004706 metal oxides Chemical class 0.000 description 1
- SIWVEOZUMHYXCS-UHFFFAOYSA-N oxo(oxoyttriooxy)yttrium Chemical compound O=[Y]O[Y]=O SIWVEOZUMHYXCS-UHFFFAOYSA-N 0.000 description 1
- 239000002245 particle Substances 0.000 description 1
- 238000000634 powder X-ray diffraction Methods 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 230000009257 reactivity Effects 0.000 description 1
- 229910002076 stabilized zirconia Inorganic materials 0.000 description 1
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- H01M8/124—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the process of manufacturing or by the material of the electrolyte
- H01M8/1246—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the process of manufacturing or by the material of the electrolyte the electrolyte consisting of oxides
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Description
483876 經濟部智慧財產局員工消費合作社印製 A7 ---------B7_____ 五、發明説明（ί ) 發明領域 本發明關於一種陶瓷材料，特別是銘鈦礦(per〇vskite) 型陶瓷，用於製造傳導離子及/或電子的陶瓷產品。 相關技藝之描述 用於分離氧之隔膜的鈣鈦礦陶瓷材料，具有下列的一 般式： AxA’x，A”x”ByB，y，B，，y”03_5 其中 x+x’+x’^l， y + y’+y”=1，且 _1<δ<1 ， 係由美國專利第5,24〇,473號可得知。 上述美國專利的陶瓷材料，具有符合化學配比的鈣鈦 礦組成，其中Σχί和Σγί都是1。 本發明者已經發現：非化學配比的鈣鈦礦型陶瓷材料 ，其中Σα及/或Eyi小於1，與金屬或金屬氧化物支撐其 上，或者與此陶瓷材料相結合，其顯示穩定性有改善，並. 且反應性有降低。 再者，本發明者已經證實：A位置的空缺不足，導致 電子和離子的傳導性增加，這是因爲材料中的缺陷濃度增 加所致。 發明槪述 依照上面所示之沒有想到的發現，本發明提供一種鈣 _____3____ 本紙張尺度適用中國國家標準（CNS ) A4規格（210X297公釐） (請先閱讀背面之注意事項再本頁)
、1T 線 483876 A7 ___________B7 五、發明説日^' - 欽礦陶瓷材料，其具有下列的一般式：
AxA’x，A”x，，ByB ’y，B”y，，〇3-s 其中 A、 A’和a”每個爲選自鑭族金屬當中的—或多種金屬 ， B、 B和B”每個爲選自過渡金屬、3a族、gb族眚金屬 當中的一種金屬； χ+χ’+χ”<1 及/ 或 y+y’+y”<q， 而使。 較佳具體實施例的詳述 於本發明一特定具體實施例中，該材料具有下式的組 成：
LaaLnbMcGadM’e〇3-s 其中：
Lii爲Ce、Pr和Nd的組合’ 擇性地可再組合—*種 鋼系金屬； Μ爲至少一種鹼土金屬； Μ，爲選自週期表中 2a、3b、4b、：5b、6b、7b、8、lb 、2b、3a、4a族和8b族貴金屬當中至少一種金屬；以及 其中 a+b+c<l 及/或 d+e<l 使得a+b+c关d+e 〇 範例1 使用滴落熱解(drip pyrolysis)程序來製造一種陶瓷粉末 ___ 4________ 本紙張尺度適用中國國家標準（CNS ) A4規格（210X297公釐） (請先閱讀背面之注意事項再本頁) |裝- 木 -線 經濟部智慧財產局員工消費合作社印製 483876 A7 _____B7 五、發明説明（3 ) 。根據所提出的化學式，以所需的比例來混合金屬硝酸鹽 、醋酸鹽或碳酸鹽的水溶液。然後，把例如葡萄糖或胺基 醋酸等燃料加入上述的溶液，以便得到富含燃料的混合物 。剛配好的原料溶液滴入旋轉窯中熱解。所得的粉末使用 XRD、SEM、BET來定其特徵，而使用雷射光散射技術來 決定其顆粒大小的分布。 發現此粉末具有鈣鈦礦結構。 範例1的材料可以用做如SOFC陰極材料、氧化觸媒 和感測器，而所提出的化學式爲：
La〇.40?Ce〇 !24Nd〇 !2〇Pr〇 〇48Na〇.〇 1 5Ca〇 〇〇7Sr〇 27δΜπ〇.945〇3-δ 此化合物的粉末XRD線則列於表1。 (請先閱讀背面之注意事項再本頁)
、1T 經濟部智慧財產局員工消費合作社印製 表1 平面間距（A) 尖蜂強度（計數） '…相Μ強度：Ί 3.877 74 ----- 17.1 3.528 28 6.5 3.455 23 5.3 3.165 36 8.3 2.742 433 100 2.472 5 1.1 2.343 16 3.7 2.238 66 15.2 2.045 12 2.7 1.936 106 24.5 1.732 10 2.4 1.582 86 20 1.369 31 7.2 1.290 3 0.7 1.224 22 — 5.1 表1 :範例1化合物的XRD特徵。 本紙張尺度適用中國國家標準（CNS ) M規格（21〇'χ297公釐） 483876 A7 ______B7 五、發明説明（+ ) 範例2 另一種材料，其可以用於例如SOFC陰極、電子/離 子混合傳導性隔膜、氧化觸媒和感測器等用途，如範例1 所提到的方式合成。該材料的化學式爲： (La〇.7Sr〇_3)〇.9Fe〇.8Mn〇.2〇3-5 此種A位置空缺不足的鈣鈦礦化合物已證實：相較於 A/B=l的氧化釔穩定化之氧化锆，具有更佳的化學穩定性 。同時，此化合物顯現高的電子傳導性（120 S/cm，於 850°C的空氣中）。晶體結構則爲斜方六面體，其參數爲(以 六方晶系表示）：aH=5.52〇A，cH=13.51〇A。 範例3 另一種可以用於SOFC交互連接，以及例如磁流體動 力學(Magneto-Hydro_Dynamic，MHD)裝置中感測器和加熱 元件之電子陶瓷化合物的材料，則爲： L^0.508Ce〇.〇48Nd〇 166Pr〇.〇68Na〇.〇i3Ca〇.〇〇7Sr〇.i79Cr〇3-6 此剛合成的材料(於範例1所提到的程序之後），顯示 出根據表2的鈣鈦礦結構。 經濟部智慧財產局S工消費合作社印製 適 度 尺，張 紙 一本 辟
¾ 4 A 5 N |釐 公 483876 A7 B7 五、發明説明（<) 表2
冷壓出小九，並於1600QC燒結。於1000°C時’其導 電性和環境氣氛之關係如下： 50.5 S/cm (Ρ〇2=0·21 atm)，26.0 S/cm (P〇2=l(T16 atm)， 6_4 S/cm (P〇2=5 · 10·18 atm)。 經濟部智慧財產局員工消費合作社印製 範例4 另一種用於SOFC電解質、氧離子隔膜和觸媒的材料 ，根據範例1而合成。本範例的化學式則爲： La〇.54Ce〇.〇5Nd〇.i8Pr〇.〇7Sr〇 i5Ga〇 9Mn〇 !〇3.§ 雖然本發明已經以相關的特定具體實施例加以描述， 但是對於熟於此技藝者而言，很明顯的有許多其他的變化 、改良和其他用途。因此，本發明不宜以此特定的揭示所 限制，而僅由所附的申請專利範圍來設限。 適 度 尺 張 紙
I 釐 公
Claims (1)
- 483876六、申請專利範圍 1· 一種銘鈦礦陶瓷材料，其具有下列的一般式： AxA’x，A”x，，ByB，y，B”y，，〇3 δ (請先閲讀背面之注意事項再填寫本頁) 其中 A、 Α’和Α”每個爲選自鑭族金屬當中的一或多種金屬 ， B、 B’和B”每個爲選自過渡金屬、3a族、81)族貴金屬 當中的一種金屬； x+x’+x”^ 及/或 y+y，+y，，<l， 而使ΣχθΣγί。 2.如申請專利範圍第1項的陶瓷材料，其具有下式的 組成： L3,aLllbNIcG3,(jM，e〇3-6 其中 Ln爲Ce、Pr和Nd的組合，選擇性地可再組合一種 鋼系金屬， Μ爲至少一種鹼土金屬； Μ’爲選自週期表中 2a、3b、4b、5b、6b、7b、8、lb 經濟部智慧財產局員工消費合作社印製 、2b、3a、4a族和8b族貴金屬當中至少—種金屬；以及 其中 a+b+c<l 及/或 d+e<l 使得a+b+c关d+e 〇 3 _如申請專利範圍第1項的陶瓷材料，其具有下式的 組成： La〇.4〇7Ce〇.i24Nd〇.i2〇Pr〇.〇48Na〇.〇i5Ca0 〇〇?8γ〇 278Μη〇 945〇3_§ 1 本紙張尺度適用中國國家標準（CNS ) A4規格（210X297公嫠） 483876 A8 Βδ C8 D8 六、申請專利範圍 4.如申請專利範圍第1項的陶瓷衬料，其具有下式的 組成： (La0.7Sr0 3)〇 9Fe0.8Mn〇.2〇3_s。 5_如申請專利範圍第1項的陶瓷材料，其具有下式的 組成： La0.508Ce〇.〇48Nd0.166pr〇 〇68Na〇 013Ca0 0〇7Sr〇 i79Cr〇3_s。 6.如申請專利範圍第1項的陶瓷材料，其具有下式的 組成： (請先閱讀背面之注意事項再填寫本頁) La0.54Ce〇.〇5Nd〇.18pr〇 07Sr〇.15Ga。9Μη〇 。 7·如申請專利範圍第1至6項中任〜項的陶瓷材料， 其用於製造傳導離子及/或電子的材料。 -"· Γ 經濟部智慧財產局員工消費合作社印製 2 本紙張尺度適用中國國家標準（CNS ) Α4規格（210Χ297公釐）
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| US (1) | US6150290A (zh) |
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| ES2204042T3 (es) * | 1998-10-07 | 2004-04-16 | Haldor Topsoe A/S | Material laminar ceramico. |
| JP3598956B2 (ja) | 2000-08-28 | 2004-12-08 | 日産自動車株式会社 | ガレート複合酸化物固体電解質材料とその製造方法 |
| JP2003007309A (ja) * | 2001-06-26 | 2003-01-10 | Nissan Motor Co Ltd | 電極材料、固体電解質型燃料電池及びガスセンサ |
| US7151067B2 (en) * | 2001-10-15 | 2006-12-19 | Nippon Steel Corporation | Porcelain composition, composite material comprising catalyst and ceramic, film reactor, method for producing synthetic gas, apparatus for producing synthetic gas and method for activating catalyst |
| US7303606B2 (en) | 2002-01-08 | 2007-12-04 | The Boc Group, Inc. | Oxy-fuel combustion process |
| AU2003291044A1 (en) * | 2002-11-15 | 2004-06-15 | Battelle Memorial Institute | Copper-substituted perovskite compositions for solid oxide fuel cell cathodes and oxygen reduction electrochemical devices |
| US20040214070A1 (en) * | 2003-04-28 | 2004-10-28 | Simner Steven P. | Low sintering lanthanum ferrite materials for use as solid oxide fuel cell cathodes and oxygen reduction electrodes and other electrochemical devices |
| US7157165B2 (en) * | 2003-11-18 | 2007-01-02 | Uchicago Argonne, Llc | Iron-based perovskite cathodes for solid oxide fuel cells |
| WO2010003926A1 (en) * | 2008-07-08 | 2010-01-14 | Technical University Of Denmark | Magnetocaloric refrigerators |
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| US3595809A (en) * | 1969-06-27 | 1971-07-27 | Gulf Research Development Co | Lanthanum chromium ferrite catalyst |
| US3885020A (en) * | 1971-10-28 | 1975-05-20 | Univ Southern California | Method of oxidizing hydrocarbons and oxygenated hydrocarbons to carbon dioxide and water |
| JPH06171950A (ja) * | 1992-12-02 | 1994-06-21 | Shin Etsu Chem Co Ltd | ランタンマンガナイト粉末の製造方法 |
| US5604048A (en) * | 1993-02-26 | 1997-02-18 | Kyocera Corporation | Electrically conducting ceramic and fuel cell using the same |
| RU2079935C1 (ru) * | 1994-11-16 | 1997-05-20 | Институт высокотемпературной электрохимии Уральского отделения РАН | Активный электрод для высокотемпературных электрохимических устройств с твердым электролитом |
| RU2104984C1 (ru) * | 1996-02-28 | 1998-02-20 | Санкт-Петербургский государственный технологический институт | Многокомпонентный резистивный материал и шихта для получения резистивного материала |
| US5759936A (en) * | 1996-03-21 | 1998-06-02 | Haldor Topsoe As | Lanthanide ceramic material |
| JP3087645B2 (ja) * | 1996-04-01 | 2000-09-11 | 株式会社村田製作所 | 負の急変抵抗温度特性を有する半導体磁器組成物 |
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| US6150290A (en) | 2000-11-21 |
| KR19990082774A (ko) | 1999-11-25 |
| JP2000001316A (ja) | 2000-01-07 |
| CA2267534C (en) | 2005-05-31 |
| NO991602L (no) | 1999-10-04 |
| CA2267534A1 (en) | 1999-10-01 |
| AU743211B2 (en) | 2002-01-24 |
| KR100365369B1 (ko) | 2003-01-15 |
| EP0947484A1 (en) | 1999-10-06 |
| RU2237039C2 (ru) | 2004-09-27 |
| NO991602D0 (no) | 1999-03-31 |
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