JP4855011B2 - 酸化物イオン伝導体および酸素分離膜並びに炭化水素の酸化用反応装置 - Google Patents
酸化物イオン伝導体および酸素分離膜並びに炭化水素の酸化用反応装置 Download PDFInfo
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- JP4855011B2 JP4855011B2 JP2005237957A JP2005237957A JP4855011B2 JP 4855011 B2 JP4855011 B2 JP 4855011B2 JP 2005237957 A JP2005237957 A JP 2005237957A JP 2005237957 A JP2005237957 A JP 2005237957A JP 4855011 B2 JP4855011 B2 JP 4855011B2
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- cerium oxide
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- 239000001301 oxygen Substances 0.000 title claims description 246
- 229910052760 oxygen Inorganic materials 0.000 title claims description 246
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 title claims description 206
- 239000012528 membrane Substances 0.000 title claims description 133
- 238000000926 separation method Methods 0.000 title claims description 131
- 239000010416 ion conductor Substances 0.000 title claims description 27
- AHKZTVQIVOEVFO-UHFFFAOYSA-N oxide(2-) Chemical compound [O-2] AHKZTVQIVOEVFO-UHFFFAOYSA-N 0.000 title claims description 23
- 229930195733 hydrocarbon Natural products 0.000 title claims description 12
- 150000002430 hydrocarbons Chemical class 0.000 title claims description 12
- 238000007254 oxidation reaction Methods 0.000 title description 9
- 239000004215 Carbon black (E152) Substances 0.000 title description 8
- 230000003647 oxidation Effects 0.000 title description 5
- 229910000420 cerium oxide Inorganic materials 0.000 claims description 60
- BMMGVYCKOGBVEV-UHFFFAOYSA-N oxo(oxoceriooxy)cerium Chemical compound [Ce]=O.O=[Ce]=O BMMGVYCKOGBVEV-UHFFFAOYSA-N 0.000 claims description 57
- 150000001875 compounds Chemical class 0.000 claims description 38
- -1 oxygen ion Chemical class 0.000 claims description 36
- 229910052791 calcium Inorganic materials 0.000 claims description 5
- 229910052688 Gadolinium Inorganic materials 0.000 claims description 2
- 229910052772 Samarium Inorganic materials 0.000 claims description 2
- 230000001590 oxidative effect Effects 0.000 claims description 2
- 239000003054 catalyst Substances 0.000 description 62
- 239000007789 gas Substances 0.000 description 55
- 230000009467 reduction Effects 0.000 description 40
- 230000006798 recombination Effects 0.000 description 31
- 238000005215 recombination Methods 0.000 description 31
- 238000010494 dissociation reaction Methods 0.000 description 25
- 230000005593 dissociations Effects 0.000 description 25
- 239000002245 particle Substances 0.000 description 22
- 230000005540 biological transmission Effects 0.000 description 18
- 239000000843 powder Substances 0.000 description 17
- CPLXHLVBOLITMK-UHFFFAOYSA-N Magnesium oxide Chemical compound [Mg]=O CPLXHLVBOLITMK-UHFFFAOYSA-N 0.000 description 16
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 14
- 239000013078 crystal Substances 0.000 description 13
- 239000000463 material Substances 0.000 description 12
- 230000007423 decrease Effects 0.000 description 11
- 239000010936 titanium Substances 0.000 description 11
- 238000010304 firing Methods 0.000 description 10
- 230000000052 comparative effect Effects 0.000 description 9
- 230000000694 effects Effects 0.000 description 9
- 238000004519 manufacturing process Methods 0.000 description 9
- 238000000034 method Methods 0.000 description 9
- 239000000395 magnesium oxide Substances 0.000 description 8
- 230000002093 peripheral effect Effects 0.000 description 8
- 230000002829 reductive effect Effects 0.000 description 8
- 239000002002 slurry Substances 0.000 description 8
- 239000000919 ceramic Substances 0.000 description 7
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 description 6
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 6
- 239000011777 magnesium Substances 0.000 description 6
- 239000011533 mixed conductor Substances 0.000 description 6
- 239000000203 mixture Substances 0.000 description 6
- 239000002994 raw material Substances 0.000 description 6
- 238000012360 testing method Methods 0.000 description 6
- 229910052782 aluminium Inorganic materials 0.000 description 5
- 230000015572 biosynthetic process Effects 0.000 description 5
- 238000006243 chemical reaction Methods 0.000 description 5
- 238000005259 measurement Methods 0.000 description 5
- 238000000465 moulding Methods 0.000 description 5
- 239000011148 porous material Substances 0.000 description 5
- 230000008569 process Effects 0.000 description 5
- 238000011084 recovery Methods 0.000 description 5
- 238000003786 synthesis reaction Methods 0.000 description 5
- 239000000654 additive Substances 0.000 description 4
- 239000000446 fuel Substances 0.000 description 4
- 150000002500 ions Chemical class 0.000 description 4
- 238000002156 mixing Methods 0.000 description 4
- PXHVJJICTQNCMI-UHFFFAOYSA-N nickel Substances [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 4
- 150000002926 oxygen Chemical class 0.000 description 4
- 239000012466 permeate Substances 0.000 description 4
- 239000000047 product Substances 0.000 description 4
- 229910002431 Ce0.8Gd0.2O1.9 Inorganic materials 0.000 description 3
- 229910002138 La0.6Sr0.4CoO3 Inorganic materials 0.000 description 3
- 230000009471 action Effects 0.000 description 3
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical group [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 3
- 230000008901 benefit Effects 0.000 description 3
- DRVWBEJJZZTIGJ-UHFFFAOYSA-N cerium(3+);oxygen(2-) Chemical class [O-2].[O-2].[O-2].[Ce+3].[Ce+3] DRVWBEJJZZTIGJ-UHFFFAOYSA-N 0.000 description 3
- 239000011248 coating agent Substances 0.000 description 3
- 238000000576 coating method Methods 0.000 description 3
- 238000010586 diagram Methods 0.000 description 3
- 238000001035 drying Methods 0.000 description 3
- 239000007788 liquid Substances 0.000 description 3
- 229910052749 magnesium Inorganic materials 0.000 description 3
- 229910052759 nickel Inorganic materials 0.000 description 3
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 3
- 238000005498 polishing Methods 0.000 description 3
- 229910052712 strontium Inorganic materials 0.000 description 3
- 229910018072 Al 2 O 3 Inorganic materials 0.000 description 2
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 2
- 229910002439 Ce0.8Sm0.2O1.9 Inorganic materials 0.000 description 2
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 2
- FYYHWMGAXLPEAU-UHFFFAOYSA-N Magnesium Chemical group [Mg] FYYHWMGAXLPEAU-UHFFFAOYSA-N 0.000 description 2
- 230000000996 additive effect Effects 0.000 description 2
- 229910052784 alkaline earth metal Inorganic materials 0.000 description 2
- 150000001342 alkaline earth metals Chemical class 0.000 description 2
- 229910052788 barium Inorganic materials 0.000 description 2
- 239000011230 binding agent Substances 0.000 description 2
- 229910052796 boron Inorganic materials 0.000 description 2
- HSJPMRKMPBAUAU-UHFFFAOYSA-N cerium(3+);trinitrate Chemical compound [Ce+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O HSJPMRKMPBAUAU-UHFFFAOYSA-N 0.000 description 2
- 230000008859 change Effects 0.000 description 2
- 239000002131 composite material Substances 0.000 description 2
- 239000000470 constituent Substances 0.000 description 2
- 229910052802 copper Inorganic materials 0.000 description 2
- 238000009792 diffusion process Methods 0.000 description 2
- 229910052739 hydrogen Inorganic materials 0.000 description 2
- 239000001257 hydrogen Substances 0.000 description 2
- 229910052738 indium Inorganic materials 0.000 description 2
- 229910052742 iron Inorganic materials 0.000 description 2
- 229910052746 lanthanum Inorganic materials 0.000 description 2
- 239000011812 mixed powder Substances 0.000 description 2
- 239000003960 organic solvent Substances 0.000 description 2
- 229910052697 platinum Inorganic materials 0.000 description 2
- 239000003566 sealing material Substances 0.000 description 2
- 239000006104 solid solution Substances 0.000 description 2
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 1
- 229910052684 Cerium Inorganic materials 0.000 description 1
- 229910018921 CoO 3 Inorganic materials 0.000 description 1
- 229910020800 La-Sr-Co Inorganic materials 0.000 description 1
- 229910052581 Si3N4 Inorganic materials 0.000 description 1
- 229910004298 SiO 2 Inorganic materials 0.000 description 1
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 1
- GEIAQOFPUVMAGM-UHFFFAOYSA-N ZrO Inorganic materials [Zr]=O GEIAQOFPUVMAGM-UHFFFAOYSA-N 0.000 description 1
- 229910052783 alkali metal Inorganic materials 0.000 description 1
- 150000001340 alkali metals Chemical class 0.000 description 1
- 229910052786 argon Inorganic materials 0.000 description 1
- 229910002091 carbon monoxide Inorganic materials 0.000 description 1
- 230000015556 catabolic process Effects 0.000 description 1
- ZMIGMASIKSOYAM-UHFFFAOYSA-N cerium Chemical compound [Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce] ZMIGMASIKSOYAM-UHFFFAOYSA-N 0.000 description 1
- VYLVYHXQOHJDJL-UHFFFAOYSA-K cerium trichloride Chemical compound Cl[Ce](Cl)Cl VYLVYHXQOHJDJL-UHFFFAOYSA-K 0.000 description 1
- TYAVIWGEVOBWDZ-UHFFFAOYSA-K cerium(3+);phosphate Chemical compound [Ce+3].[O-]P([O-])([O-])=O TYAVIWGEVOBWDZ-UHFFFAOYSA-K 0.000 description 1
- VGBWDOLBWVJTRZ-UHFFFAOYSA-K cerium(3+);triacetate Chemical compound [Ce+3].CC([O-])=O.CC([O-])=O.CC([O-])=O VGBWDOLBWVJTRZ-UHFFFAOYSA-K 0.000 description 1
- GHLITDDQOMIBFS-UHFFFAOYSA-H cerium(3+);tricarbonate Chemical compound [Ce+3].[Ce+3].[O-]C([O-])=O.[O-]C([O-])=O.[O-]C([O-])=O GHLITDDQOMIBFS-UHFFFAOYSA-H 0.000 description 1
- MMXSKTNPRXHINM-UHFFFAOYSA-N cerium(3+);trisulfide Chemical compound [S-2].[S-2].[S-2].[Ce+3].[Ce+3] MMXSKTNPRXHINM-UHFFFAOYSA-N 0.000 description 1
- UNJPQTDTZAKTFK-UHFFFAOYSA-K cerium(iii) hydroxide Chemical compound [OH-].[OH-].[OH-].[Ce+3] UNJPQTDTZAKTFK-UHFFFAOYSA-K 0.000 description 1
- 238000005336 cracking Methods 0.000 description 1
- 238000006731 degradation reaction Methods 0.000 description 1
- 238000013461 design Methods 0.000 description 1
- 239000002270 dispersing agent Substances 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 238000011156 evaluation Methods 0.000 description 1
- 238000011049 filling Methods 0.000 description 1
- 229910052733 gallium Inorganic materials 0.000 description 1
- 238000004817 gas chromatography Methods 0.000 description 1
- 239000011521 glass Substances 0.000 description 1
- 238000005469 granulation Methods 0.000 description 1
- 230000003179 granulation Effects 0.000 description 1
- 150000002431 hydrogen Chemical class 0.000 description 1
- 230000002706 hydrostatic effect Effects 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-M hydroxide Chemical compound [OH-] XLYOFNOQVPJJNP-UHFFFAOYSA-M 0.000 description 1
- 229910052741 iridium Inorganic materials 0.000 description 1
- 229910052747 lanthanoid Inorganic materials 0.000 description 1
- 150000002602 lanthanoids Chemical class 0.000 description 1
- FZLIPJUXYLNCLC-UHFFFAOYSA-N lanthanum atom Chemical compound [La] FZLIPJUXYLNCLC-UHFFFAOYSA-N 0.000 description 1
- 229910052748 manganese Inorganic materials 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 239000003345 natural gas Substances 0.000 description 1
- 229910000480 nickel oxide Inorganic materials 0.000 description 1
- 238000005121 nitriding Methods 0.000 description 1
- 230000008520 organization Effects 0.000 description 1
- GNRSAWUEBMWBQH-UHFFFAOYSA-N oxonickel Chemical compound [Ni]=O GNRSAWUEBMWBQH-UHFFFAOYSA-N 0.000 description 1
- 229910052763 palladium Inorganic materials 0.000 description 1
- 230000000704 physical effect Effects 0.000 description 1
- 238000003825 pressing Methods 0.000 description 1
- 238000012545 processing Methods 0.000 description 1
- 230000001737 promoting effect Effects 0.000 description 1
- 230000009257 reactivity Effects 0.000 description 1
- 229910052703 rhodium Inorganic materials 0.000 description 1
- 229910052707 ruthenium Inorganic materials 0.000 description 1
- 150000003839 salts Chemical class 0.000 description 1
- 238000007493 shaping process Methods 0.000 description 1
- 229910052710 silicon Inorganic materials 0.000 description 1
- 239000010703 silicon Substances 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
- 239000000243 solution Substances 0.000 description 1
- 238000001179 sorption measurement Methods 0.000 description 1
- 239000007921 spray Substances 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 230000002194 synthesizing effect Effects 0.000 description 1
- 229910052719 titanium Inorganic materials 0.000 description 1
- 229910052720 vanadium Inorganic materials 0.000 description 1
- GPPXJZIENCGNKB-UHFFFAOYSA-N vanadium Chemical compound [V]#[V] GPPXJZIENCGNKB-UHFFFAOYSA-N 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
- 229910052727 yttrium Inorganic materials 0.000 description 1
Images
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- Separation Using Semi-Permeable Membranes (AREA)
- Compounds Of Iron (AREA)
- Oxygen, Ozone, And Oxides In General (AREA)
- Inorganic Compounds Of Heavy Metals (AREA)
Description
また、第3発明の炭化水素の酸化用反応装置の要旨とするところは、上記第2発明の酸素分離膜を用いたことにある。
また、前記第3発明によれば、上記のように高効率で耐久性に優れた酸素分離膜が用いられていることから、安価且つ高効率で耐久性の高い炭化水素の酸化用反応装置が得られる。
CH4+1/2O2 → CO+2H2 ・・・(1)
Claims (4)
- 一般式(La 1-x Sr x)(Tiy Fe 1-y)O3(但し、0<x<1、0<y<1)で表されるペロブスカイト化合物と、その結晶粒界および粒内の少なくとも一方に位置し且つCeO2-δ(但し、0≦δ<0.5)にSm,Gd,Caの少なくとも一種がドープされたセリウム酸化物とを、そのセリウム酸化物が前記ペロブスカイト化合物100重量部に対して1〜100重量部の範囲内の割合となるように含むことを特徴とする酸化物イオン伝導体。
- 前記セリウム酸化物は0.10〜1.00(S/cm)の範囲内の酸素イオン伝導度を備えたものである請求項1に記載の酸化物イオン伝導体。
- 請求項1または請求項2に記載の酸化物イオン伝導体を緻密な膜状としたことを特徴とする酸素分離膜。
- 請求項3に記載の酸素分離膜を用いた炭化水素の酸化用反応装置。
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CN105642131A (zh) * | 2014-11-13 | 2016-06-08 | 中国科学院大连化学物理研究所 | 一种纳米粒子稳定钙钛矿结构透氧膜的方法 |
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KR101579308B1 (ko) | 2008-02-25 | 2015-12-21 | 가부시키가이샤 노리타케 캄파니 리미티드 | 세라믹 제품 및 세라믹 부재의 접합 방법 |
JP5438607B2 (ja) * | 2010-06-30 | 2014-03-12 | 一般財団法人ファインセラミックスセンター | 金属酸化膜、酸素センサ、酸素透過膜及び固体酸化物燃料電池 |
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JPH11214014A (ja) * | 1998-01-28 | 1999-08-06 | Tokyo Gas Co Ltd | 固体電解質型燃料電池の空気極およびその作製方法 |
EP1452507B1 (en) * | 2001-11-09 | 2008-08-06 | Noritake Co., Limited | Oxygen ion conducting ceramic material and use thereof |
JP3876306B2 (ja) * | 2002-03-27 | 2007-01-31 | 独立行政法人産業技術総合研究所 | 混合伝導性酸化物 |
JP3574439B2 (ja) * | 2002-05-28 | 2004-10-06 | コリア インスティテュート オブ サイエンス アンド テクノロジー | 多孔性イオン伝導性セリア膜コーティングで三相界面が拡張された微細構造の電極およびその製造方法 |
JP2004292177A (ja) * | 2003-03-25 | 2004-10-21 | Toto Ltd | 固体電解質材料 |
JP2005279439A (ja) * | 2004-03-29 | 2005-10-13 | Noritake Co Ltd | 酸素分離膜エレメント、酸素製造方法、および反応器 |
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CN105642131A (zh) * | 2014-11-13 | 2016-06-08 | 中国科学院大连化学物理研究所 | 一种纳米粒子稳定钙钛矿结构透氧膜的方法 |
CN105642131B (zh) * | 2014-11-13 | 2019-06-18 | 中国科学院大连化学物理研究所 | 一种纳米粒子稳定钙钛矿结构透氧膜的方法 |
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