JP6166345B2 - 石油化学製品を生成させる、統合された、原油の水素化処理、水蒸気熱分解、及びスラリー水素化処理 - Google Patents
石油化学製品を生成させる、統合された、原油の水素化処理、水蒸気熱分解、及びスラリー水素化処理 Download PDFInfo
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- JP6166345B2 JP6166345B2 JP2015501890A JP2015501890A JP6166345B2 JP 6166345 B2 JP6166345 B2 JP 6166345B2 JP 2015501890 A JP2015501890 A JP 2015501890A JP 2015501890 A JP2015501890 A JP 2015501890A JP 6166345 B2 JP6166345 B2 JP 6166345B2
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- C10G65/00—Treatment of hydrocarbon oils by two or more hydrotreatment processes only
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Description
本出願は、2012年3月20日に出願された米国仮特許出願第61/613,294号、及び2013年3月14日に出願された同第61/785,894号の優先権の利益を主張し、それらは、本出願において参照により援用される。
発明の分野
本発明は、石油化学製品、例えば軽質オレフィン及び芳香族を、原油を含む供給物から生成させる、統合された、水素化処理、水蒸気熱分解、及びスラリー水素化処理に関する。
低級オレフィン(すなわち、エチレン、プロピレン、ブチレン、及びブタジエン)、並びに芳香族(すなわち、ベンゼン、トルエン、及びキシレン)は、石油化学及び化学工業で広く使用されている基本的な中間体である。熱分解、又は水蒸気熱分解は、典型的には水蒸気の存在下で、そして酸素の非存在下で、これらの物質を形成する主要なタイプの処理である。水蒸気熱分解用の原料には、石油ガス及び蒸留物、例えばナフサ、ケロシン、及びガス油を挙げることができる。通常、これらの原料を入手するには限界があり、原油精製所において、高コストでエネルギー集約型の処理工程が必要である。
VAPB=体積平均したランキン度での沸点
であり、
sp.gr.=原料の比重
である。
統合された、水素化処理、水蒸気熱分解、及びスラリー水素化処理を含む処理フロー概略図を、図1に示す。統合システムは概して、選択的水素化処理ゾーン、水蒸気熱分解ゾーン、スラリー水素化処理ゾーン、及び生成物分離ゾーンを含む。
a. HDM区域での触媒は概して、約140〜240m2/gの表面積を有するガンマアルミナの担持体をベースにしたものである。この触媒は、非常に高い細孔体積、例えば、1cm3/g超を有するものとして最も良く言い表される。細孔サイズそのものは典型的には、圧倒的にマクロ多孔性である。このことが要求されるのは、触媒表面上に金属、そして随意にドーパントを取り込むために大容量を提供するためである。典型的には触媒表面上で活性な金属は、ニッケルとモリブデンの硫化物であって、そのが比Ni/Ni+Mo<0.15となるものである。ニッケルの濃度は、HDM触媒上ではその他の触媒よりも低く、これは、幾分かのニッケルとバナジウムが、除去の間に原料それ自体から堆積し、触媒として作用すると予想されるからである。使用するドーパントは、リン(例えば、参照により本明細書において援用される、米国特許公開第2005/0211603号を参照されたい)、ホウ素、ケイ素、及びハロゲンの一つ又は複数が可能である。触媒は、アルミナ押し出し物又はアルミナビーズの形態であってもよい。特定の実施形態では、金属の取り込みが床の頂部で30〜100%の間で変化するであろうことから、アルミナビーズを使用すると反応器中での触媒HDM床の非担持が容易になる。
b. 中間触媒を使用して、HDM及びHDSの機能間の移行を行うこともできる。それは、中間金属の担持、及び細孔サイズ分布を有する。HDM/HDS反応器中のこの触媒は、実質的にアルミナをベースにした担持体であり、これは押し出し物の形態をとり、随意にVI族(例えば、モリブデン及び/又はタングステン)の少なくとも一つの触媒金属、及び/又はVIII族(例えば、ニッケル及び/又はコバルト)の少なくとも一つの触媒金属である。触媒はまた、ホウ素、リン、ハロゲン及びケイ素から選択される随意に少なくとも一つのドーパントを含有する。物理的特性には、約140〜200m2/gの表面積、少なくとも0.6cm3/gの細孔体積、及び細孔12〜50nmの範囲のメソ細孔性の細孔が挙げられる。
c. HDS区域中の触媒は、ガンマアルミナをベースにした担持物質を有するものを含んでいてもよく、その典型的な表面積は、HDM範囲の高い方の端に近い、例えば約180〜240m2/gである。HDS用に要求されるこの高い表面積により、結果として、比較的小さい細孔体積、例えば1cm3/g未満が得られる。触媒は、VI族の元素の少なくとも一つ、例えば、モリブデンと、VIII族の元素の少なくとも一つ、例えばニッケルとを含有する。触媒はまた、ホウ素、リン、ケイ素及びハロゲンから選択される少なくともの一つのドーパントを含む。特定の実施形態では、コバルトを使用して、比較的高いレベルの脱硫を行う。活性相のための金属担持は、要求される活性が高いほど高く、Ni/Ni+Moのモル比が0.1〜0.3の範囲であり、(Co+Ni)/Moのモル比が0.25〜0.85の範囲にある。
d. 最終触媒(随意に第2の及び第3の触媒と置き換わり得る)は、原料の水素化(脱硫の主機能ではなく)を実行するように設計され、例えば、Appl.Catal.AGeneral、204(2000)251に記載のとおりである。触媒はまた、Niにより促進されることになり、担持体は、細孔の大きいガンマアルミナである。物理的特性には、HDM範囲の高い方の端に近い表面積、例えば、180〜240m2/gが挙げられる。この高い表面積がHDSに要求される結果、比較的小さい細孔体積、例えば、1cm3/g未満が得られる。
原料として原油を使用する、石油化学製品、例えばオレフィン及び芳香族の生成;
コークス前駆体を、初期の原油全体から顕著に除去し、これにより水蒸気熱分解ユニットの輻射コイルでのコークス形成が減少する;
付加される不純物、例えば金属、硫黄、及び窒素化合物もまた、出発供給物から顕著に除去し、これにより最終生成物の後処理を回避する、
をもたらすものである。
Claims (13)
- 原油を直接変換してオレフィン及び芳香族の石油化学製品を生成させる、統合された、水素化処理、水蒸気熱分解、及びスラリー水素化処理方法であって:
a. 原油を、減少した汚染物質の含有量、増加したパラフィン度、減少した鉱山局相関指標(Bureau of Mines Correlation Index)、そして増加した米国石油協会比重を有する、水素化処理したエフルエントを生成させるのに有効な条件下で水素の存在下で水素化処理すること;
b. 水素化処理したエフルエント及びスラリー処理生成物を、水蒸気熱分解ゾーン内で水蒸気の存在下、混合生成物流を生成させるのに有効な条件下で熱分解すること;
c. 前記水素化処理したエフルエント、前記水蒸気熱分解ゾーン内の加熱流、又は前記混合生成物流の一つ又は複数に由来する廃棄残油又はボトムを、スラリー水素化処理ゾーン中で処理して、スラリー処理生成物を生成させること;
d. 混合生成物流を分離すること;
e. ステップ(d)で回収した水素を精製して、それを水素化処理のステップに再循環させること;及び
f. オレフィン及び芳香族を、前記分離した混合生成物流から回収すること、を含む処理方法。 - 熱分解燃料油を、前記混合生成物流から回収し、ステップ(c)において分解される廃棄残油又はボトムの少なくとも一部分として使用することをさらに含む、請求項1に記載の統合処理方法。
- ステップ(a)からの前記水素化処理されたエフルエントを、気液分離ゾーンにおいて気相と液相に分離し、前記気相をステップ(b)において熱分解し、前記液相の少なくとも一部分を、ステップ(c)において処理することをさらに含む、請求項1に記載の統合処理方法。
- 前記気液分離ゾーンがフラッシュ分離装置である、請求項3に記載の統合処理方法。
- 気液分離ゾーンが、気相と液相を分離する、物理的、又は機械的装置である、請求項3に記載の統合処理方法。
- 請求項3に記載の統合処理方法であって、前記気液分離ゾーンが、吸入口に気液分離器を有するフラッシュ容器を含み、前記気液分離器が、
予備回転の構成要素であって、流入部分及び遷移部分を有し、前記流入部分は、前記水素化処理したエフルエントを受け入れる吸入口、及び曲線の導管を有する、予備回転の構成要素と、
制御されたサイクロン区域であって、
前記予備回転の構成要素に、前記曲線の導管及び前記サイクロン区域を通じて接続する吸入口、及び
気体が通過するサイクロン部材の上端にライザー区域を有するサイクロン区域と、を有し、
前記フラッシュ容器の底部分が、前記液相のすべて又は一部分をステップ(c)に移行させるのに先立って、前記液相の収集及び沈降ゾーンとしての役割を果たす処理方法。 - 請求項1に記載の統合処理方法であって、ステップ(b)がさらに、
水素化処理したエフルエントを、水蒸気熱分解ゾーンの対流区域において加熱すること、
前記加熱した水素化処理したエフルエントを、気相と液相に分離すること、
前記気相を、前記水蒸気熱分解ゾーンの熱分解区域に受け渡すこと、及び
前記液相を排出して、ステップ(c)において処理される前記廃棄残油又はボトムの少なくとも一部分として使用すること、を含む処理方法。 - 前記加熱した水素化処理したエフルエントを気相と液相に分離することを、物理的及び機械的分離に基づく気液分離器を用いて行う、請求項7に記載の統合処理方法。
- 前記加熱した水素化処理したエフルエントの気相と液相へ分離を、気液分離器を用いて行う、請求項8に記載の統合処理方法であって、前記気液分離器が、
予備回転の構成要素であって、流入部分及び遷移部分を有し、前記流入部分は、前記加熱した水素化処理したエフルエントを入れる吸入口、及び曲線の導管を有する、予備回転の構成要素と、
制御されたサイクロン区域であって、
前記予備回転の構成要素に、前記曲線の導管及び前記サイクロン区域を通じて接続する吸入口、及び
気相が通過するサイクロン部材の上端にライザー区域を有するサイクロン区域と、
液相のすべて又は一部分をステップ(c)に搬送するのに先立って、前記液相が通過する液体収集器/沈降区域と、を有する処理方法。 - 請求項1に記載の統合処理方法であって、
ステップ(d)が、
熱分解された混合生成物流を複数段の圧縮を用いて圧縮すること;
前記圧縮された、熱分解された混合生成物流を苛性処理に付して、硫化水素と二酸化炭素の含有量が減少した、熱分解された混合生成物流を生成させること;
硫化水素と二酸化炭素の含有量が減少した、前記熱分解された混合生成物流を圧縮すること;
硫化水素と二酸化炭素の含有量が減少した、前記圧縮された、熱分解された混合生成物流を脱水させること;
硫化水素と二酸化炭素の含有量が減少した、前記脱水した、圧縮された、熱分解された混合生成物流から、水素を回収すること;及び
オレフィン及び芳香族を、硫化水素と二酸化炭素の含有量が減少した、前記脱水した、圧縮された、熱分解された混合生成物流の残りから得ること;
を含み、そして
ステップ(e)が、硫化水素と二酸化炭素の含有量が減少した、前記脱水した、圧縮された、熱分解された混合生成物流から回収した水素を精製し、水素化処理ゾーンに再循環させることを含む処理方法。 - 硫化水素と二酸化炭素の含有量が減少した、前記脱水した、圧縮された、熱分解された混合生成物流から水素を回収することがさらに、個別にメタンを回収して、熱分解ステップにおいてバーナー及び/又はヒーターの燃料として使用することを含む、請求項10に記載の統合処理方法。
- 請求項3に記載の統合処理方法であって、さらに
前記水素化処理したエフルエントを高圧分離器中で分離して、ガス部分と液体部分を回収し、前記ガス部分は洗浄して、追加の水素源として水素化処理ゾーンに再循環させること、及び
前記高圧分離器から得られた液体部分を、低圧分離器中でガス部分と液体部分に分離することを含み、前記低圧分離器からの前記液体部分は、熱分解ステップへの供給物であり、前記低圧分離器からの前記ガス部分は、前記水蒸気熱分解ゾーンの後、ステップ(d)での分離の前で、前記混合生成物流と一つにする処理方法。 - 請求項3に記載の統合処理方法であって、さらに
前記水素化処理したエフルエントを高圧分離器中で分離して、ガス部分と液体部分を回収し、前記ガス部分は洗浄して、追加の水素源として水素化処理ゾーンに再循環させること、及び、
前記高圧分離器から得られた前記液体部分を、低圧分離器中でガス部分と液体部分に分離することを含み、前記低圧分離器に由来する前記液体部分は、前記気液分離ゾーンへの供給物であり、前記低圧分離器に由来する前記ガス部分を、前記水蒸気熱分解ゾーンの後、ステップ(d)での分離の前で、前記混合生成物流と一つにする処理方法。
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