JP2004203737A - 炭化水素類を部分酸化して水素と一酸化炭素を製造する方法 - Google Patents
炭化水素類を部分酸化して水素と一酸化炭素を製造する方法 Download PDFInfo
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Abstract
【解決手段】炭化水素類を部分酸化して水素と一酸化炭素を製造する方法であって、これによって前記部分酸化が、セリアコーティング・ジルコニア・モノリス担体上またはその中に担持されたニッケル、コバルト、鉄、プラチナ、パラジウム、イリジウム、レニウム、ルテニウム、ロジウム、オスミウム及びそれらの組合せからなる群から選択される遷移金属から本質的になる還元金属触媒と、炭化水素含有供給材料ガスと酸素含有供給材料ガスと水素との混合物とを接触させることによって、約10℃程度の低い温度またはそれ以上で開始する、前記方法。
【選択図】図1
Description
・最小急冷様式では、合成ガスを急冷することによって合成ガスから最大熱回収が可能であり、炭素が形成する傾向が軽減する。
・最大急冷様式では、100℃〜150℃に合成ガスを冷却させることが可能であり、これは熱回収が望ましくない場合には、低い資本コスト解決を示す。
・部分急冷様式では、下流での処理、たとえばCOの大部分をH2に転換させるための水−ガスシフト反応に好適な温度まで合成ガスを冷却させることが可能である。
1.最初に所望の流速で天然ガスを導入する。
2.天然ガスのフローがその所望の設定値に到達したら、水素の注入を開始する。これは安全面から重要であり、酸素を添加する前に天然ガスが多い状態に維持する。
3.次いで酸素フローを開始する。
4.通常、全フローの約0.5〜4%のH2フローを10〜30秒間維持する。
5.反応の開始は、触媒温度が>400℃に急上昇することにより示される。開始を実施してから、ほんの短時間の水素の注入時間が必要なことを示すその設定値に酸素フローが到達する。
1.最初に所望の流速で天然ガスと二酸化炭素とを導入する。
2.天然ガスと二酸化炭素のフローがその所望の設定値に到達したら、水素の注入を開始する。
3.次いで酸素フローを開始する。
4.通常、全フローの約0.5〜4%のH2フローを10〜30秒間維持する。
5.反応の開始は、触媒温度が>400℃に急上昇することにより示される。
1インチ(25.4mm)当たり45個の孔、直径0.7インチ(17.8mm)及び長さ0.39インチ(9.91mm)のジルコニアモノリスを最初に20重量%セリアでコーティングし、次いで金属ロジウム2重量%で含浸させて金属触媒を製造した。詳細な製造法は、米国特許出願番号第10/143,705号に知見することができる。金属触媒モノリスを含有する反応器を10℃で60分間、窒素ガスでパージした。
実施例1に記載の如く、金属触媒を製造した。同量のロジウム金属をセリアコーティングジルコニア担体に充填した。
モノリス担体をジルコニアで製造した以外には、実施例1に記載の如く金属触媒を製造した。実施例1に記載のセリアコーティングを使用せずに、同量の金属ロジウムをジルコニア担体に充填した。
線速度及び空間速度の効果を比較するために、二種類の直径(0.7インチ(17.8mm)と1インチ(25.4mm))の実施例1に記載の如きモノリス触媒を使用した。同一触媒容積ベースで結果を比較するために、0.7インチ(17.8mm)直径×0.39インチ(9.91mm)厚さの4枚重ね触媒ディスクでのデータを、2つの1インチ(25.4mm)×0.39インチ(9.91mm)のモノリス触媒の結果と比較した。実施例1と同じ開始手順に従って、64%メタンと34%酸素とを含有する供給材料混合物を反応器内に通した。ここでは空間速度は、触媒モノリス容積により分割された全供給材料ガスフロー速度として定義し、線速度は、触媒モノリスの断面積により分割された全供給ガスフロー速度として定義する。表1は、同一空間速度と同一反応条件において、線速度が上昇すると、メタン転換率が上昇し、H2及びCO選択性が良くなった。他方、同一線速度に関しては、空間速度が低いと、メタン転換率が高く、メタンスリップ(slip)がかなり低かった。言い換えれば、触媒モノリスのL/Dアスペクト比が高くなると、部分酸化反応の性能が高くなった。
実施例1で使用したのと同一金属触媒を使用して、実施例1に記載のものと同一手順に従って部分酸化反応を開始した。炭素対酸素比1.75でメタンと酸素と、二酸化炭素0〜約30容積%とを含有するガス混合物とを、モノリス触媒を含有する反応器に供給した。この混合物は、反応を開始するのに使用した混合物とは異なっていた。この供給材料混合物を150,000/時間の空間速度で供給した。吸熱逆ガスシフト反応により、反応温度は1020℃から750℃に低下した。典型的な生成物ガスは、39%水素、33%一酸化炭素、13.1%二酸化炭素、1.3%メタンと12.6%水を含んでいた。メタンと二酸化炭素の転換比は、生成物中の測定濃度から計算した。この結果は、以下の図5A及び5Bに示されている。供給材料ガス混合物を300℃に予熱すると、CH4とCO2の両方の転換率がやや上昇した。転換率の測定は、元素物質バランスから計算した。
Claims (15)
- 炭化水素類を部分酸化して水素と一酸化炭素を製造する方法であって、これによって前記部分酸化が、セリアコーティング・ジルコニア・モノリス担体上またはその中に担持されたニッケル、コバルト、鉄、プラチナ、パラジウム、イリジウム、レニウム、ルテニウム、ロジウム、オスミウム及びそれらの組合せからなる群から選択される遷移金属から本質的になる還元金属触媒と、炭化水素含有供給材料ガスと酸素含有供給材料ガスと水素との混合物とを接触させることによって、約10℃程度の低い温度またはそれ以上で開始する、前記方法。
- 前記水素の供給が連続的である、請求項1に記載の方法。
- 前記還元金属触媒が、セリアコーティング・ジルコニア・モノリス担体上またはその中に担持されたロジウム触媒であり、且つ前記混合物がさらに二酸化炭素を含む、請求項1に記載の方法。
- 前記混合物の圧力が約1.0barから約10.0barである、請求項1に記載の方法。
- 前記水素を前記供給材料ガス混合物中に注入する、請求項1または2に記載の方法。
- 前記水素を、前記炭化水素含有供給材料ガスと、前記酸素含有供給材料ガスとの添加の間に注入する、請求項1に記載の方法。
- 前記温度が10℃を超え100℃未満である、請求項1〜3のいずれか1項に記載の方法。
- 前記セリアコーティング・ジルコニア・モノリス担体がセリア約5重量%〜約30重量%である、請求項1〜3のいずれか1項に記載の方法。
- 前記水素の注入フローが約10〜約30秒である、請求項1に記載の方法。
- 前記水素が、前記供給材料ガスの全フローの約0.5容積%〜約4.0容積%の量で存在する、請求項1〜3のいずれか1項に記載の方法。
- 二酸化炭素の連続フローを前記供給材料ガスに添加することをさらに含む、請求項2に記載の方法。
- 前記二酸化炭素が約80容積%以下の量で前記供給材料ガス混合物中に存在する、請求項3に記載の方法。
- 前記部分酸化によって製造した水素対一酸化炭素の比が約2:1の水素対一酸化炭素である、請求項4に記載の方法。
- 前記セリアコーティング・ジルコニア・モノリス担体がセリア約5重量%〜約30重量%である、請求項1〜4のいずれか1項に記載の方法。
- 前記部分酸化を、容器、触媒物質を含浸させた少なくとも一つのセラミックフォームディスクと、少なくとも一つのブランクセラミックフォームディスクを含む反応器で実施する、請求項1〜4のいずれか1項に記載の方法。
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JP2009523688A (ja) * | 2006-01-20 | 2009-06-25 | イネオス ユーロープ リミテッド | 炭化水素及び酸素含有ガスを反応器内で触媒床と接触させる方法 |
JP2009263199A (ja) * | 2008-04-01 | 2009-11-12 | Air Water Inc | 一酸化炭素ガス発生装置および方法 |
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US7090826B2 (en) | 2006-08-15 |
SG135004A1 (en) | 2007-09-28 |
TW200417407A (en) | 2004-09-16 |
CA2450157A1 (en) | 2004-06-23 |
US20060204415A1 (en) | 2006-09-14 |
PL364198A1 (en) | 2004-06-28 |
CN100575247C (zh) | 2009-12-30 |
KR20040057953A (ko) | 2004-07-02 |
NO20035493L (no) | 2004-06-24 |
NZ529798A (en) | 2004-10-29 |
ZA200309254B (en) | 2004-05-26 |
AU2003264634A1 (en) | 2004-07-08 |
MY134650A (en) | 2007-12-31 |
EP1433746A2 (en) | 2004-06-30 |
NO20035493D0 (no) | 2003-12-10 |
CN1509980A (zh) | 2004-07-07 |
AU2003264634C1 (en) | 2009-01-29 |
EP1433746A3 (en) | 2008-03-26 |
PL203313B1 (pl) | 2009-09-30 |
TWI312294B (en) | 2009-07-21 |
AU2003264634B2 (en) | 2008-07-24 |
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