JP2010514658A - 多成分系触媒を用いた石油ベースの熱中性改質方法 - Google Patents
多成分系触媒を用いた石油ベースの熱中性改質方法 Download PDFInfo
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- JP2010514658A JP2010514658A JP2009544097A JP2009544097A JP2010514658A JP 2010514658 A JP2010514658 A JP 2010514658A JP 2009544097 A JP2009544097 A JP 2009544097A JP 2009544097 A JP2009544097 A JP 2009544097A JP 2010514658 A JP2010514658 A JP 2010514658A
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- catalyst
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- hydrogen
- reforming
- heat
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- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 1
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Abstract
Description
白金族金属は、1つ以上の金属、例えばロジウムまたはロジウム化合物およびその混合物を含む、2つまたは3つの金属として使用することができる。さらに、周期表のVIIB族由来の金属酸化物は、液体炭化水素供給燃料の熱中性改質の効果を高めるために使用することができる。
当該処理は、多成分系触媒上で、気化された液体炭化水素、空気/酸素および蒸気に接触させることを含む。本発明の当該処理は、広い範囲の実施条件(operating conditions)で実行されることができる。作業条件のレベルは、使用される供給燃料と、求められる変換のレベルにより決定される。
(1)供給された酸素すべての消費および燃焼反応の高熱の生成により、炭化水素燃料の完全な酸化ができる。
(2) 酸化反応によって生成される熱を消費し、真実の熱中性改質を提供する、本来吸熱性である蒸気改質反応は、非常に活発である。
(3) 検知できる失活のない、非常に長い活性期間を有する。
(4) 非常に高い割合の合成ガス変換において、イソオクタンからディーゼルにおよぶ液体炭化水素を処理することができる。
本発明の処理は、軽質のナフサやLPGのような、軽質の原油フラクションと同じく、低硫黄中間留分原油フラクション(例えば重質のナフサ、灯油、ディーゼル)からの水素リッチであるガスを生成するために用いられる。当該処理は、前述の多成分系触媒を使用する。
炭化水素供給原料は、天然ガスやそのコンデンセート(condensate)を含む、メタン、エタン、プロパン、ブタンまたはそれらの混合物のような単純な炭化水素(single hydrocarbon)や、軽質のナフサ、重質のナフサ、ケロシン、ディーゼルのような様々な原油フラクションとすることができる。
合成ガス(一酸化炭素+水素)生成、Fisher-Tropsch法を用いた炭化水素の液体への変換(HTL)、メタノールの生成、水素化処理(hydroprocessing)のための水素供給燃料、様々なアプリケーションのための高純度水素提供、特殊化学品の製造、および、プロトン交換膜燃料電池(PEMFC)、 固体電解質型燃料電池(SOFC)および溶融炭酸塩型燃料電池(MCFC)を使用する100Wから数MWまでの範囲の能力を有する燃料電池アプリケーションとしての液化炭化水素燃料の改質を含む、広範囲のアプリケーションに適用することができる。これらのシステムは、小規模商品、家庭用品用熱電供給システムおよび燃料電池自動車に適用することができる。
ガスはマスフロー・コントローラーを介して供給し;液体燃料は精密HPLCポンプによって送り込まれた。反応器のチューブは直径12.6mmで、ヘインズ230合金で作成されていた。3つの領域を有する電気炉(その温度は温度調節器によって監視および制御された)で、反応器システムを加熱した。
生成物収集部は、圧力調整バルブ、気体−液体セパレーター、液面(liquid-level)調節器および生成物タンクから構成された。
十分な量の水が生成物タンクに溜まった後、炭化水素の供給が始められた。様々なO2/C比率が使用された。反応器中の温度は、数秒でおよそ800℃-900℃まで上昇した。実験は、定常状態に到達した後、2時間行われた。ガスサンプルは集められ、2つのガスクロマトグラフで分析された。一方はTCDを備えており、そして他方はFIDを備えていた。パーセント変換および生成ガス成分はGCの結果から計算された。
1.炭化水素変換
2.水素の収量
3.選択性(H2/(CO+CO2))
4.触媒の失活が検出されない重質の燃料を改質する高い能力。例えば、本発明の触媒を用いたディーゼル変換は99%であったのに対し、4つの成分の従来技術の触媒を使用したディーゼル変換は64%であった。
Claims (16)
- 液体炭化水素燃料から水素リッチである合成ガスを生成するための熱中性改質処理であって、
a)炭化水素燃料、O2リッチであるガス、および蒸気の混合物を、Ni,La2O3,Ce2O3,Pt,ZrO2,RhおよびReを含む、燃焼と蒸気および/またはCo2の改質とが複合化される触媒からなる触媒床を含む反応器の内部領域に供給し、
b)前記燃料、前記O2リッチであるガス、および前記蒸気を、およそ380℃からおよそ480℃の範囲における温度に予備加熱し、
c)およそ800℃からおよそ900℃の反応温度に上昇させる発熱性の燃焼反応を引き起こし、且つ水素リッチである合成ガスを得るための炭化水素燃料の改質に十分な時間の吸熱性の蒸気改質反応を引き起こす、およそ30000h-1からおよそ70000h-1であるガスの時間ごとの空間速度で前記触媒床に前記予備加熱した混合物を接触させることを備える熱中性改質処理。 - 前記液体炭化水素燃料は、原油ベース燃料である請求項1に記載の熱中性改質処理。
- 前記液体原油ベース液体燃料は、イソオクタン、軽質ナフサ、重質ナフサ、ケロシン、およびディーゼルをからなる群から選択される請求項2に記載の熱中性改質処理。
- 前記ガスの時間ごとの空間速度は、およそ35000h-1からおよそ50000h-1である請求項1に記載の熱中性改質処理。
- 前記予備加熱の温度が、およそ410℃からおよそ420℃である請求項1に記載の熱中性改質処理。
- 前記発熱性の燃焼反応から生成された熱は、同一の前記触媒床における前記吸熱性の反応により中性化および相殺される請求項1に記載の熱中性処理。
- 前記反応は、外部からの熱が非供給で実行される請求項1に記載の熱中性処理。
- コークスが非形成である請求項1に記載の熱中性処理。
- 前記触媒は、硫黄分を200ppm以下で含有する供給燃料を改質できる請求項1に記載の熱中性処理。
- 97%以上の液体炭化水素の供給燃料が合成ガス(H2/CO/CO2/CH4)に変換される請求項3に記載の熱中性処理。
- 前記処理から生成された合成ガスは、水性ガスシフト且つ選択的酸化、メタン生成且つ膜技術、およびPSAからなる群から選択される水素の精製技術を用いて、高純度の水素を生成するためにさらに精製される請求項1に記載の熱中性処理。
- 水素リッチである合成ガスは、高い温度または低い温度の燃料電池が実装される自動車において、搭載型改質装置(on-board reformers)の燃料として用いられる請求項1に記載の熱中性処理。
- 前記水素リッチである合成ガスは、内燃機関のエンジンにおいて水素濃縮の燃料として用いられる請求項1に記載の熱中性処理。
- 前記水素リッチである合成ガスは、定置型出力設備アプリケーションにおいて用いられる請求項1に記載の熱中性処理。
- Ni、La2O3、Ce2O3、Pt、ZrO2、Rh、およびReを含む、熱中性改質処理において使用されるための触媒。
- 各成分の重量%について、Niが0.5から15%、Ce2O3が0.5から10%、La2O3が0.5から5%、Ptが0.1から2%、ZrO2 が0.5から3%、Rhが0.1から2%、およびReが0.1から2%である請求項15に記載の触媒。
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US7700005B2 (en) | 2010-04-20 |
EA200900890A1 (ru) | 2010-04-30 |
NO20092485L (no) | 2009-09-22 |
JP5276010B2 (ja) | 2013-08-28 |
US8008226B2 (en) | 2011-08-30 |
CN101679155B (zh) | 2013-11-06 |
KR20090123853A (ko) | 2009-12-02 |
EP2104657A4 (en) | 2016-03-09 |
EP2104657A2 (en) | 2009-09-30 |
EA015806B1 (ru) | 2011-12-30 |
BRPI0719620A2 (pt) | 2018-01-23 |
US20080152572A1 (en) | 2008-06-26 |
US20100216633A1 (en) | 2010-08-26 |
WO2008082589A3 (en) | 2008-08-28 |
EP2104657B1 (en) | 2018-07-04 |
WO2008082589A8 (en) | 2009-08-13 |
WO2008082589A2 (en) | 2008-07-10 |
NO343573B1 (no) | 2019-04-08 |
KR101419567B1 (ko) | 2014-07-15 |
WO2008082589A9 (en) | 2008-10-09 |
CN101679155A (zh) | 2010-03-24 |
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