JP2007153931A - 水素の製造方法、改質ガソリンの製造方法及び芳香族炭化水素の製造方法 - Google Patents
水素の製造方法、改質ガソリンの製造方法及び芳香族炭化水素の製造方法 Download PDFInfo
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- JP2007153931A JP2007153931A JP2005347196A JP2005347196A JP2007153931A JP 2007153931 A JP2007153931 A JP 2007153931A JP 2005347196 A JP2005347196 A JP 2005347196A JP 2005347196 A JP2005347196 A JP 2005347196A JP 2007153931 A JP2007153931 A JP 2007153931A
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- Prior art keywords
- naphtha
- hydrogen
- oil
- hydrocracking
- catalyst
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Classifications
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/70—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
- B01J23/76—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36
- B01J23/84—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36 with arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
- B01J23/85—Chromium, molybdenum or tungsten
- B01J23/88—Molybdenum
- B01J23/883—Molybdenum and nickel
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
- C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
- C01B3/22—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by decomposition of gaseous or liquid organic compounds
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Abstract
【解決手段】本発明は、第1の原料油又はその第1の原料油に由来する第2の原料油を、水素を含む雰囲気中、水素化分解触媒との接触により水素化分解して第1のナフサを得る水素化分解工程と、第1のナフサ又はその第1のナフサに由来する第2のナフサを接触改質して水素を得る接触改質工程とを有する水素の製造方法であって、第1の原料油は、沸点230℃以上の留分を含む動植物油に由来する油脂成分を含有するものであり、水素化分解触媒は、周期律表第6A族及び第8族に属する金属からなる群より選ばれる1種以上の金属と、酸性質を有する無機酸化物とを含有するものであり、第1のナフサは、沸点100〜120℃の留分を含むものである水素の製造方法を提供する。
【選択図】 なし
Description
(社)石油学会、「石油精製プロセス」、講談社、1999年3月20日発行、101〜119ページ
濃度5質量%のアルミン酸ナトリウム水溶液1kgに水ガラス3号を加えて70℃に保温した容器に入れた。濃度2.5%の硫酸アルミニウム水溶液1kgを70℃に保温した別の容器に入れ、上述のアルミン酸ナトリウム水溶液及び水ガラスの混合物に15分かけて滴下した。水ガラスの量は所定のシリカ含有量となるよう調整した。混合溶液のpHが6.9〜7.5になる時点を滴下の終点とし、得られたスラリー状生成物をフィルターに通して濾取し、ケーキ状のスラリーを得た。
第1の水素化触媒A(70mL)を充填した第1反応管(内径20mm)と、水素化分解触媒B(30mL)を充填した第2反応管(内径20mm)とを、この順で直列に固定床流通式反応装置に取り付けた後、ジメチルジサルファイドを加えた直留軽油(硫黄分3質量%)を用いて、触媒A及びBの触媒層平均温度300℃、水素分圧6MPa、LHSV1h−1、水素/油比200NL/Lの条件下で、4時間触媒の予備硫化を行った。予備硫化終了後、パーム油(15℃密度:0.916g/mL、酸素分:11.4質量%、10%留出点:588℃)及び中東系の減圧軽油留分(15℃密度:0.919g/mL、硫黄分:2.41質量%、窒素分:610質量ppm、10%留出点:344℃)を20:80の容量比で混合した第1の原料油を、触媒A及びBにおける反応温度400℃、水素圧力10.5MPa、LHSV0.7h−1の条件で通油して、水素化前処理及び水素化分解を行った。得られた生成油から、JIS−K2601「原油試験方法」のうち参考に記載される「理論段数15段の精留塔を使用した蒸留試験方法」に準拠した装置により、沸点範囲80〜145℃の留分(第1のナフサ)を分取した。得られた第1のナフサの性状は、パラフィン:98容量%、ナフテン:2容量%、アロマ:0容量%、硫黄分:1質量ppm未満、酸素分:45質量ppmであった。
酸化物換算で触媒質量に対し3質量%のニッケルと酸化物換算で触媒質量に対して18質量%のモリブデンをアルミナ担体に担持した市販触媒(比表面積:180m2/g)を70mL充填した反応管(内径20mm)を固定床流通式反応装置に取り付けた後、ジメチルジサルファイドを加えた直留軽油(硫黄分3質量%)を用いて、触媒層平均温度300℃、水素分圧3MPa、LHSV1h−1、水素/油比200NL/Lの条件下で、4時間触媒の予備硫化を行った。予備硫化後、直留ナフサ(初留点:90℃、終点:155℃、パラフィン:65容量%、ナフテン:25容量%、アロマ:10容量%、硫黄分:330質量ppm)と実施例2で得られた第1のナフサとを70:30の比率で混合したナフサ留分を、反応温度310℃、圧力2.5MPa、LHSV5h−1、水素/油比40NL/Lの条件で通油して第2の水素化処理を行った。生成油(第2のナフサ)の硫黄分は0.2質量ppm、酸素分は5質量ppm以下であった。
球状のγ−アルミナ500gに蒸留水500mLを加え、更に0.012mol/Lの濃度の塩化白金酸水溶液500mLと、0.020mol/Lの塩化第二スズに0.1N塩酸溶液を加え500mLとした水溶液とを加え、エバポレーターで水を蒸発させた。その後、得られた試料を120℃で10時間乾燥し、更に400℃で1時間焼成して接触改質用の触媒を得た。得られた触媒の窒素吸着法による比表面積は195m2/gであった。
実施例4で得られた接触改質用の触媒(30mL)を充填した反応管(内径20mm)を固定床流通式反応装置に取り付けた後、反応前処理として水素分圧2MPa、530℃の条件で還元前処理を実施した。その後、実施例3で得られた第2のナフサを、水分量を調整しながら通油して反応温度530℃で接触改質した。生成物の性状を表2に示す。なお、表2中、水素生成量は第1の原料油1Lに対するNLで表される。また、ベンゼン、トルエン、キシレンの収率はJIS−K2536−2「石油製品−成分試験方法(ガスクロマトグラフによる全成分の求め方)」に記載された方法によって測定された数値から算出した。更に、ここでいうリサーチオクタン価とは、JIS−K2280「オクタン価及びセタン価試験方法」により測定されるリサーチ法オクタン価を意味する。
第1のナフサを用いずに直留ナフサのみを通油して第2の水素化処理を行った以外は実施例3と同様にして、生成油を得た。得られた生成油の硫黄分は0.2質量ppm、酸素分は0.1質量ppmであった。
実施例4で得られた接触改質用の触媒(30mL)を充填した反応管(内径20mm)を固定床流通式反応装置に取り付けた後、反応前処理として水素分圧2MPa、530℃の条件で還元前処理を実施した。その後、比較例1で得られた生成油を、水分量を調整しながら通油して反応温度505℃で接触改質した。生成物の性状を表2に示す。
Claims (6)
- 第1の原料油又はその第1の原料油に由来する第2の原料油を、水素を含む雰囲気中、水素化分解触媒との接触により水素化分解して第1のナフサを得る水素化分解工程と、
前記第1のナフサ又はその第1のナフサに由来する第2のナフサを接触改質して水素を得る接触改質工程と、を有する水素の製造方法であって、
前記第1の原料油は、沸点230℃以上の留分を含む動植物油に由来する油脂成分を含有するものであり、
前記水素化分解触媒は、周期律表第6A族及び第8族に属する金属からなる群より選ばれる1種以上の金属と、酸性質を有する無機酸化物と、を含有するものであり、
前記第1のナフサは、沸点100〜120℃の留分を含むものである、
水素の製造方法。 - 前記接触改質工程よりも前に、前記第1のナフサを含有するナフサ留分を、水素を含む雰囲気中、第2の水素化触媒と接触させることにより、前記ナフサ留分よりも硫黄分及び酸素分を低減せしめた前記第2のナフサを得る水素化処理工程、を更に有し、
前記第2の水素化触媒は、周期律表第6A族及び第8族に属する金属からなる群より選ばれる1種以上の金属を含有するものであり、
前記第2のナフサは、硫黄分1.0質量ppm以下、かつ酸素分10質量ppm以下のものである、
請求項1記載の水素の製造方法。 - 前記水素化分解工程よりも前に、前記第1の原料油を、水素を含む雰囲気中、第1の水素化触媒と接触させて第2の原料油を得る水素化前処理工程、を更に有し、
前記第1の水素化触媒は、周期律表第6A族及び第8族に属する金属からなる群より選ばれる1種以上の金属を含有するものである、
請求項1又は2に記載の水素の製造方法。 - 前記水素化分解工程において水素化分解する条件が、水素圧力6〜20MPa、LHSV0.2〜1.5h−1、及び水素/油比200〜2000NL/Lである、請求項1〜3のいずれか一項に記載の水素の製造方法。
- 請求項1〜4のいずれか一項に記載の接触改質工程において改質ガソリンを得る改質ガソリンの製造方法。
- 請求項1〜4のいずれか一項に記載の接触改質工程において炭素数6〜8の芳香族炭化水素を得る芳香族炭化水素の製造方法。
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JPH0639588B2 (ja) * | 1989-03-22 | 1994-05-25 | 日揮株式会社 | 炭化水素の接触改質法 |
JPH04122790A (ja) * | 1990-09-14 | 1992-04-23 | Osaka Gas Co Ltd | 重質油の接触水素化分解方法 |
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