JP2017507779A - 高温二酸化炭素水和、高温二酸化炭素水和および改質の組合せ、ならびに/または改質のためのイットリウム含有触媒、ならびに高温二酸化炭素水和、高温二酸化炭素水和および改質の組合せ、ならびに/または改質のための方法 - Google Patents
高温二酸化炭素水和、高温二酸化炭素水和および改質の組合せ、ならびに/または改質のためのイットリウム含有触媒、ならびに高温二酸化炭素水和、高温二酸化炭素水和および改質の組合せ、ならびに/または改質のための方法 Download PDFInfo
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- JP2017507779A JP2017507779A JP2016557232A JP2016557232A JP2017507779A JP 2017507779 A JP2017507779 A JP 2017507779A JP 2016557232 A JP2016557232 A JP 2016557232A JP 2016557232 A JP2016557232 A JP 2016557232A JP 2017507779 A JP2017507779 A JP 2017507779A
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- Prior art keywords
- catalyst
- carbon dioxide
- reforming
- aluminum
- yttrium
- Prior art date
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- 239000003054 catalyst Substances 0.000 title claims abstract description 175
- 238000000034 method Methods 0.000 title claims abstract description 123
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 title claims abstract description 110
- 239000001569 carbon dioxide Substances 0.000 title claims abstract description 55
- 229910002092 carbon dioxide Inorganic materials 0.000 title claims abstract description 55
- 238000002407 reforming Methods 0.000 title claims abstract description 46
- 229910052727 yttrium Inorganic materials 0.000 title claims abstract description 41
- VWQVUPCCIRVNHF-UHFFFAOYSA-N yttrium atom Chemical compound [Y] VWQVUPCCIRVNHF-UHFFFAOYSA-N 0.000 title claims abstract description 33
- 230000036571 hydration Effects 0.000 title 4
- 238000006703 hydration reaction Methods 0.000 title 4
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims abstract description 74
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 claims abstract description 62
- 230000008569 process Effects 0.000 claims abstract description 59
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 claims abstract description 53
- 229910052782 aluminium Inorganic materials 0.000 claims abstract description 53
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims abstract description 48
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Abstract
Description
(i)アルミニウム供給源を、好ましくは溶液中で、より好ましくは水溶液中で用意する工程、
(ii)アルミニウム供給源とイットリウム含有化合物および銅、亜鉛、ニッケル、コバルトまたは鉄からなる群の少なくとも1種のさらなる金属塩とを接触させる工程、
(iii)工程(i)からのアルミニウム供給源と工程(ii)における物質とを完全に混合する工程、
(iv)混合物を乾燥する工程、
(v)混合物を低温焼成する工程、
(vi)成形または造形する工程、
(vii)混合物を高温焼成する工程。
本開示の目的では、本発明の触媒または触媒前駆体という用語は、高い割合のYAG相を有するイットリウム含有材料を含む。これは、本発明の触媒または触媒前駆体は、特定の実施形態において、二次相も含むことができることを意味する。YAG相という用語は、(i)立方晶イットリウム−アルミニウムガーネット構造を有するY3Al5O12(YAG)、(ii)斜方晶および/または六方晶イットリウムアルミニウムペロブスカイト構造を有するYAlO3(YAP)および/または(iii)単斜晶ペロブスカイト構造を有するY4Al2O9(YAM)を含む相を含む。触媒が二次相を含む場合、二次相の割合は、好ましくは0〜49質量%の範囲、より好ましくは1〜40質量%の範囲、さらに好ましくは3〜30質量%の範囲である。検討中の相が斜方晶または六方晶イットリウムアルミニウムペロブスカイト構造を有するYAlO3(YAP)である場合、斜方晶および六方晶イットリウムアルミニウムペロブスカイト構造が並んで存在することも可能である。
アルミニウム供給源として、原則としては、すべてのアルミニウム含有出発材料を使用することが可能であり、好ましいアルミニウム供給源は、擬ベーマイト、ベーマイト、ギブサイト、バイヤライト、ガンマ−酸化アルミニウム、シータ−酸化アルミニウム、マグネシウムヒドロタルサイト等のヒドロタルサイト、BK Guilini製の製品「Guifloc」等のコロイド状塩基性酸化アルミニウムおよび当業者に公知の他のコロイド状アルミニウム供給源、ならびにまたこれらの混合物の群から選択される。特に、Sasol製のとりわけ以下の製品:DisperalおよびすべてのDisperalグレード、Dispal、Pural、Puralox、Catalox、CatapalならびにまたすべてのPural MGグレードが包含される。
本発明の触媒または触媒前駆体を使用する方法の分野は、極めて広範であり、それゆえ触媒または触媒前駆体を使用する方法は、特に、接触改質のために、炭化水素または炭化水素含有化合物(cPOx)の部分的接触酸化のために、オートサーマル改質(ATR)のために、乾式改質(DryRef)のために、高温二酸化炭素水素化およびメタンの存在下における高温二酸化炭素水素化と炭化水素の改質の組合せのために、ならびにまた、特に合成ガスを製造するために適している。水素に加えて、供給流体ストリームは、有利には、CO2、CO、O2、CH4およびH2Oからなる群からの少なくとも1種のガスを含む。
(a.1)好ましくは、炭化水素、好ましくはメタンならびに任意に水素および/または二酸化炭素を含む供給ガスと、本発明の触媒または本発明の方法によって製造された触媒とを接触させる工程、
(a.2)反応器またはその中に存在する触媒を、接触させる間、500℃を超える、好ましくは700℃を超える、好ましくは800℃を超えるおよびより好ましくは850℃を超える温度の改質ガスで加熱する工程、
(a.3)1バールを超える、好ましくは5バールを超える、より好ましくは10バールを超える、特に好ましくは15バールを超えるおよびより特に好ましくは20バールを超えるプロセス圧力で反応を実施しながら、反応器を操作する工程、
(a.4)触媒を、そのGHSVが500から300000hr−1の範囲、好ましくは1500から200000hr−1の範囲、より好ましくは2000から150000hr−1の範囲およびより好ましくは2000から100000hr−1の範囲のガスストリームに曝露する工程
を含む方法を提供する。
55.976gのGilufloc 83(Giulini製;Al含量12.4質量%)を600mlガラスビーカーに秤量し、磁気撹拌機(50mm撹拌子、150rpm)で室温において撹拌した。53.306gの硝酸イットリウム(III)六水和物(Alfa Aesar製、純度99.9%)および6.679gの硝酸鉄(III)九水和物(Sigma Aldrich製、純度99.6%)を別のガラスビーカーに秤量し、必要な限り少ない(約100ml)DI水(イオン交換後導電率0.5micro Siemens)中で撹拌しながら(磁気撹拌機、50mm撹拌子、150rpm)溶解した。溶解後、該混合物を定量的にGilufloc 83中に撹拌しながら導入した。該ガラスビーカーをDI水ですすいだ。
Claims (13)
- イットリウムおよびアルミニウムを含み、立方晶ガーネット構造、斜方晶ペロブスカイト構造、六方晶ペロブスカイト構造および/または単斜晶ペロブスカイト構造からなる群からの少なくとも1種の構造を有することを特徴とする、少なくとも1種の結晶性材料を含む触媒または触媒前駆体であって、触媒は、Cu、Zn、Fe、Co、および/またはNiを含む、触媒または触媒前駆体。
- イットリウム含量が、15〜80mol%の範囲であり、アルミニウム含量が、10〜90mol%の範囲であり、Cu、Zn、Ni、Co、Feからなる群からの化学種の総含量は、0.01〜10mol%の範囲である、請求項1に記載の触媒または触媒前駆体。
- 結晶性材料中のイットリウムおよび/またはアルミニウム種の一部が、Cu、Zn、Ni、Co、Feからなる群からの少なくとも1種の化学種によって置き換えられている、請求項1または請求項2に記載の触媒または触媒前駆体。
- 触媒又は触媒前駆体が、立方晶ガーネット構造、斜方晶ペロブスカイト構造、六方晶ペロブスカイト構造、および/または単斜晶ペロブスカイト構造からなる群からの主要相に加えて、1〜49質量%の範囲の割合で存在する少なくとも1種の二次相を含む、請求項1から3のいずれか一項に記載の触媒または触媒前駆体。
- 触媒又は触媒前駆体が、2m2/gを超えるBET表面積を有する、請求項1から4のいずれか一項に記載の触媒または触媒前駆体。
- 主要相として立方晶イットリウムアルミニウムガーネットを含む、請求項1から5のいずれか一項に記載の触媒または触媒前駆体。
- Pt、Rh、Ru、Pd、Ir、Auからなる群からの少なくとも1種の貴金属含有助触媒を含む触媒または触媒前駆体であって、貴金属含有助触媒の含量が0.001〜5質量%の範囲である、請求項1から6のいずれか一項に記載の触媒または触媒前駆体。
- Ce、La、Pr、Tb、Nd、Euからなるカチオン種Iの群、またはMg、Ca、Sr、Ba、Ga、Be、Cr、Mnからなるカチオン種IIの群から選択される少なくとも1種のカチオン種を含む、請求項1から7のいずれか一項に記載の触媒または触媒前駆体。
- (i)アルミニウム供給源を用意する工程、
(ii)アルミニウム供給源を、銅、亜鉛、ニッケル、コバルトまたは鉄からなる群の少なくとも1種のさらなる金属塩及びイットリウム含有化合物に接触させる工程、
(iii)工程(ii)からのイットリウム含有化合物と接触している、工程(i)からのアルミニウム供給源を完全に混合する工程、
(iv)混合物を乾燥する工程、
(v)混合物を低温焼成する工程、
(vi)成形または造形する工程、
(vii)混合物を高温焼成する工程
を含む、請求項1から8のいずれか一項に記載の触媒または触媒前駆体を製造する方法。 - ポリ塩化アルミニウムを含む塩基性溶液または分散体、および/またはナノ粒子のアルミニウム含有出発材料が、アルミニウム供給源として使用される、請求項9に記載の方法。
- 金属塩が、工程(iii)における混合の間、溶融物の形態で存在する、請求項9または10に記載の方法。
- 請求項1から8のいずれか一項に記載の触媒または触媒前駆体を使用した、二酸化炭素水素化、二酸化炭素水素化および改質の組合せならびに/または炭化水素の改質のための方法であって、
(a.1)炭化水素、ならびに任意に水素および/または二酸化炭素を含む供給ガスと、本発明の触媒とを接触させる工程、
(a.2)供給ガスと、反応器中に存在する触媒との接触が、≧600℃の温度において行われる工程、
(a.3)接触の間の反応器中のプロセス圧力が≧1バールであり、その間本方法が実施される工程、
(a.4)反応器に供給される供給ストリームの改質ガスストリームのGHSVが500から100000hr−1の範囲である工程
を含む方法。 - メタンおよび二酸化炭素が、改質ガスストリーム中に存在し、メタン対二酸化炭素の比が、4:1から1:2の範囲である、請求項12に記載の炭化水素を改質する方法。
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WO2000016899A1 (en) * | 1998-09-21 | 2000-03-30 | The University Of Queensland | Catalysts and process for reforming of hydrocarbons |
WO2001028678A1 (en) * | 1999-10-18 | 2001-04-26 | Conoco, Inc. | Nickel-rhodium based catalysts and process for preparing synthesis gas |
WO2001036323A2 (en) * | 1999-11-17 | 2001-05-25 | Conoco Inc. | Cobalt-based catalysts and process for producing synthesis gas |
WO2002066403A1 (en) * | 2001-02-16 | 2002-08-29 | Conoco Inc. | Supported rhodium-spinel catalysts and process for producing synthesis gas |
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RU2016140372A (ru) | 2018-04-16 |
RU2016140372A3 (ja) | 2018-10-25 |
WO2015135968A1 (de) | 2015-09-17 |
TW201600170A (zh) | 2016-01-01 |
CN106102905A (zh) | 2016-11-09 |
EP3116826A1 (de) | 2017-01-18 |
EP3116826B1 (de) | 2018-07-04 |
CA2942587A1 (en) | 2015-09-17 |
US20170080407A1 (en) | 2017-03-23 |
KR20160133490A (ko) | 2016-11-22 |
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