JP4512365B2 - 原位置触媒再生/活性化法 - Google Patents
原位置触媒再生/活性化法 Download PDFInfo
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- JP4512365B2 JP4512365B2 JP2003543737A JP2003543737A JP4512365B2 JP 4512365 B2 JP4512365 B2 JP 4512365B2 JP 2003543737 A JP2003543737 A JP 2003543737A JP 2003543737 A JP2003543737 A JP 2003543737A JP 4512365 B2 JP4512365 B2 JP 4512365B2
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- catalyst
- hcs
- regeneration
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
- C10G2/00—Production of liquid hydrocarbon mixtures of undefined composition from oxides of carbon
- C10G2/30—Production of liquid hydrocarbon mixtures of undefined composition from oxides of carbon from carbon monoxide with hydrogen
- C10G2/32—Production of liquid hydrocarbon mixtures of undefined composition from oxides of carbon from carbon monoxide with hydrogen with the use of catalysts
- C10G2/33—Production of liquid hydrocarbon mixtures of undefined composition from oxides of carbon from carbon monoxide with hydrogen with the use of catalysts characterised by the catalyst used
- C10G2/331—Production of liquid hydrocarbon mixtures of undefined composition from oxides of carbon from carbon monoxide with hydrogen with the use of catalysts characterised by the catalyst used containing group VIII-metals
- C10G2/332—Production of liquid hydrocarbon mixtures of undefined composition from oxides of carbon from carbon monoxide with hydrogen with the use of catalysts characterised by the catalyst used containing group VIII-metals of the iron-group
-
- 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
- B01J23/90—Regeneration or reactivation
- B01J23/94—Regeneration or reactivation of catalysts comprising metals, oxides or hydroxides of the iron group metals or copper
-
- 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
- B01J23/90—Regeneration or reactivation
- B01J23/96—Regeneration or reactivation of catalysts comprising metals, oxides or hydroxides of the noble metals
-
- 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
- B01J38/00—Regeneration or reactivation of catalysts, in general
- B01J38/04—Gas or vapour treating; Treating by using liquids vaporisable upon contacting spent catalyst
- B01J38/10—Gas or vapour treating; Treating by using liquids vaporisable upon contacting spent catalyst using elemental hydrogen
-
- 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
- B01J38/00—Regeneration or reactivation of catalysts, in general
- B01J38/04—Gas or vapour treating; Treating by using liquids vaporisable upon contacting spent catalyst
- B01J38/12—Treating with free oxygen-containing gas
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
- C10G2/00—Production of liquid hydrocarbon mixtures of undefined composition from oxides of carbon
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
- C10G2/00—Production of liquid hydrocarbon mixtures of undefined composition from oxides of carbon
- C10G2/30—Production of liquid hydrocarbon mixtures of undefined composition from oxides of carbon from carbon monoxide with hydrogen
- C10G2/32—Production of liquid hydrocarbon mixtures of undefined composition from oxides of carbon from carbon monoxide with hydrogen with the use of catalysts
- C10G2/33—Production of liquid hydrocarbon mixtures of undefined composition from oxides of carbon from carbon monoxide with hydrogen with the use of catalysts characterised by the catalyst used
- C10G2/331—Production of liquid hydrocarbon mixtures of undefined composition from oxides of carbon from carbon monoxide with hydrogen with the use of catalysts characterised by the catalyst used containing group VIII-metals
- C10G2/333—Production of liquid hydrocarbon mixtures of undefined composition from oxides of carbon from carbon monoxide with hydrogen with the use of catalysts characterised by the catalyst used containing group VIII-metals of the platinum-group
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- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Organic Chemistry (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Oil, Petroleum & Natural Gas (AREA)
- Materials Engineering (AREA)
- General Chemical & Material Sciences (AREA)
- Catalysts (AREA)
- Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
- Production Of Liquid Hydrocarbon Mixture For Refining Petroleum (AREA)
Description
1.触媒復活手段を含有し得る作動中のHCSプロセスから、炭化水素合成触媒の一部を除去する工程;
2.触媒から、プロセスの反応物と生成物を除去する工程;
3.触媒を再生環境に曝露する工程;および
4.触媒を触媒還元のためにHCSプロセスの環境に再導入する工程、
を含んでなる。
TiO2担体上の「新鮮」Co−Re触媒を活性化し、フィッシャー−トロプシュ反応器に入れた。反応器が作動してから2、3日後に取り出した実験早期試料、および実験サイクルのずっと後期に取り出した実験後期試料という、2つの試料を取り出した。各試料とも乾燥箱に取り出し、不活性条件下、高温トルエンでワックスを抽出した。
水素雰囲気下、高温条件(1200kPa、400℃で8時間)で「新鮮」(非活性化)触媒を還元(活性化)した。次に、触媒をH2/CO比2.1、200℃、20.25バールで作動するフィッシャー−トロプシュ合成反応器に入れた。非特許文献3に見られるものと同様の動力学モデルを用いて、反応条件の違いに関して調整した触媒生産性(転化されたCOのモル数/触媒容量)を測定することによって、触媒活性を決定した。図2に、この触媒の相対活性レベルを報告してある。予想通り、この「新鮮」高温還元触媒の活性レベルは、平均して12.0より僅かに低い。
「新鮮」触媒の初期水素還元を、低温復活条件(220℃、2000kPaで12時間)で行ったことを除いて、実施例2と同じ実験を行った。実施例2と同様に、触媒をフィッシャー−トロプシュ反応器(同じ作動条件)に入れ、相対活性を測定した。この触媒の相対活性は図3に報告してある。この触媒の相対活性は、5.0〜5.5の範囲にある。これらの結果は明らかに、「新鮮」触媒の低温還元は、許容し得るHCS活性レベルまで触媒を活性化しなかったことを証明している。
実施例2と同じ方法で調製された触媒試料を、フィッシャー−トロプシュ反応器の実験早期に、作動しているその反応器から不活性条件下に抽出した。この試料を、実施例2と同じフィッシャー−トロプシュ条件で作動している固定床反応器に入れた。およそ4日後、H2気流下に触媒からワックスをストリッピングし、ガス混合物(窒素中1%O2)中、20気圧で酸化した。この再生手順に続いて、フィッシャー−トロプシュ反応を続けたまま、20.25バールのH2圧下、触媒を200℃で12時間還元した。およそ5.5日後、同様のワックス除去処理を実施し、同じ方法で触媒を再生した(ただし、再還元は12気圧のH2圧下、400℃で8時間行った)。相対活性値を図4に示してある。
Claims (8)
- 失活化した炭化水素合成触媒を再活性化するための方法であって、
(1)炭化水素合成(HCS)反応器から失活化した触媒の一部を除去し、前記除去された触媒を再生容器へ移す工程;
(2)前記除去された触媒を再生容器中で300℃超で作動する酸化的環境からなる再生環境に付し、再生触媒を形成する工程;および
(3)前記再生触媒を、150〜320℃の範囲の温度、5.5〜42.0バールの範囲の圧力、100〜40,000V/時間/Vの範囲の合成ガスに関する時間当たりのガス空間速度のHCSプロセス条件で作動するHCS反応器に導入する工程からなり、
その際、前記再生触媒が導入されるHCS反応器は、さらに、HCSプロセスの低活性領域においてH2流の全体または一部を使用する触媒復活手段を含み、それにより、前記再生触媒は、前記触媒復活手段を通過すると、150〜320℃の範囲の温度で前記触媒復活手段のH2流の全体または一部中で再活性化されることを特徴とする触媒の再活性化方法。 - 前記触媒は、周期律表第VIII族金属よりなる群から選択される少なくとも1種の金属を成分として有するか、またはその化合物であることを特徴とする請求項1に記載の触媒の再活性化方法。
- 前記触媒は、Fe、Ni、CoおよびRuよりなる群から選択される少なくとも1種の金属を成分として有するか、またはその化合物であることを特徴とする請求項1に記載の触媒の再活性化方法。
- 前記触媒は、周期律表第VIII族金属よりなる群から選択される少なくとも1種の金属を成分として有するか、またはその化合物である第1の触媒金属、および周期律表第VIIa族元素またはVIII族元素よりなる群から選択される少なくとも1種の元素を成分として有するか、またはその化合物である第2の触媒金属を有するバイメタル触媒であることを特徴とする請求項1に記載の触媒の再活性化方法。
- 前記触媒は、Fe、Ni、CoおよびRuよりなる群から選択される少なくとも1種の金属を成分として有するか、またはその化合物である第1の触媒金属、並びにRe、Ru、PtおよびPdよりなる群から選択される少なくとも1種の元素を成分として有するか、またはその化合物である第2の触媒金属を有するバイメタル触媒であることを特徴とする請求項1に記載の触媒の再活性化方法。
- 前記触媒は、Coを成分として有するか、またはCo化合物である第1の触媒金属、並びにReおよびRuから選択される少なくとも1種の元素を成分として有するか、またはその化合物である第2の触媒金属を有するバイメタル触媒であることを特徴とする請求項1に記載の触媒の再活性化方法。
- 前記除去された触媒は、HCS反応器から前記再生環境に入る前に、その中に存在する反応物と生成物との少なくとも一部が除去されることを特徴とする請求項1に記載の触媒の再活性化方法。
- 前記反応物と生成物との少なくとも一部の除去は、H2ストリッピングにより達成されることを特徴とする請求項7に記載の触媒の再活性化方法。
Applications Claiming Priority (2)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
US10/054,228 US6900151B2 (en) | 2001-11-13 | 2001-11-13 | In situ catalyst regeneration/activation process |
PCT/US2002/032760 WO2003041860A2 (en) | 2001-11-13 | 2002-10-15 | In situ catalyst regeneration/activation process |
Related Child Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
JP2010058620A Division JP2010174248A (ja) | 2001-11-13 | 2010-03-16 | 原位置触媒再生/活性化法および炭化水素合成方法 |
Publications (2)
Publication Number | Publication Date |
---|---|
JP2005508739A JP2005508739A (ja) | 2005-04-07 |
JP4512365B2 true JP4512365B2 (ja) | 2010-07-28 |
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JP2003543737A Expired - Fee Related JP4512365B2 (ja) | 2001-11-13 | 2002-10-15 | 原位置触媒再生/活性化法 |
JP2010058620A Pending JP2010174248A (ja) | 2001-11-13 | 2010-03-16 | 原位置触媒再生/活性化法および炭化水素合成方法 |
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JP2010058620A Pending JP2010174248A (ja) | 2001-11-13 | 2010-03-16 | 原位置触媒再生/活性化法および炭化水素合成方法 |
Country Status (10)
Country | Link |
---|---|
US (1) | US6900151B2 (ja) |
EP (1) | EP1446226A2 (ja) |
JP (2) | JP4512365B2 (ja) |
CN (1) | CN100488634C (ja) |
AU (1) | AU2002335008B2 (ja) |
BR (1) | BR0214008A (ja) |
CA (1) | CA2466441C (ja) |
TW (1) | TWI231812B (ja) |
WO (1) | WO2003041860A2 (ja) |
ZA (1) | ZA200403504B (ja) |
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WO2008139407A2 (en) * | 2007-05-11 | 2008-11-20 | Sasol Technology (Proprietary) Limited | Catalysts |
US20090023822A1 (en) * | 2007-07-19 | 2009-01-22 | Tijm Peter J | Method for activating and regenerating catalyst for a fischer-tropsch synthesis reaction |
US8614158B2 (en) * | 2008-02-29 | 2013-12-24 | Schlumberger Technology Corporation | Fischer-trospch and oxygenate synthesis catalyst activation/regeneration in a micro scale process |
JP2009214013A (ja) * | 2008-03-11 | 2009-09-24 | Ihi Corp | フィッシャー・トロプシュ合成触媒の連続再生方法及び装置 |
US8293805B2 (en) * | 2008-05-29 | 2012-10-23 | Schlumberger Technology Corporation | Tracking feedstock production with micro scale gas-to-liquid units |
EA019045B1 (ru) | 2009-03-16 | 2013-12-30 | Сауди Бейсик Индастриз Корпорейшн | Катализатор никель/оксид лантана для получения синтез-газа |
US8227654B2 (en) | 2009-09-08 | 2012-07-24 | Exxonmobil Chemical Patents Inc. | Aromatic hydrocarbon purification method |
BR112012014717B1 (pt) | 2009-12-16 | 2019-11-12 | Shell Int Research | processo para regenerar uma ou mais partículas de catalisador de fischer-tropsch que compreendem cobalto |
US9062569B2 (en) | 2010-10-29 | 2015-06-23 | General Electric Company | Systems, methods, and apparatus for regenerating a catalytic material |
WO2012084160A1 (en) | 2010-12-22 | 2012-06-28 | Saudi Basic Industries Corporation | Catalyst useful in fisher-tropsch synthesis |
CN103648639B (zh) | 2011-04-19 | 2016-10-12 | 沙特基础工业公司 | 碳负载的钴和钼催化剂 |
JP6120835B2 (ja) | 2011-07-08 | 2017-04-26 | サウジ ベーシック インダストリーズ コーポレイションSaudi Basic Industries Corporaiton | 改善された炭素担持コバルトおよびモリブデン触媒、ならびに低級アルコールを生成するためのその使用 |
EP2679568A1 (en) | 2012-06-25 | 2014-01-01 | Saudi Basic Industries Corporation | Process for production ethylene and propylene from syngas |
EP2866937A1 (en) | 2012-06-27 | 2015-05-06 | Saudi Basic Industries Corporation | Catalyst and process for the selective production of lower hydrocarbons c1-c5 from syngass with low methane and co2 production |
EP3027314A2 (en) | 2013-07-31 | 2016-06-08 | Saudi Basic Industries Corporation | Catalyst for conversion of synthesis gas |
CN107207969B (zh) | 2014-11-20 | 2019-05-07 | 沙索技术有限公司 | 费托合成 |
KR101890044B1 (ko) * | 2016-12-26 | 2018-08-20 | 한서대학교 산학협력단 | 중질유 또는 잔사유 수소화 처리 공정용 재생 촉매 및 이의 제조방법 |
CN108722426B (zh) * | 2017-04-19 | 2021-06-11 | 中国石油化工股份有限公司 | 催化剂及制备方法和应用以及催化剂前体还原活化方法以及低碳烯烃的制备方法 |
CN109331824A (zh) * | 2018-10-08 | 2019-02-15 | 德清原素高科生物技术有限公司 | 一种葡萄糖酸钠生产过程中的钯铋炭催化剂的再生工艺 |
CN109999729B (zh) * | 2019-04-26 | 2022-08-02 | 上海华畅环保设备发展有限公司 | 沸腾床加氢反应器中催化剂原位在线旋流活性恢复方法和装置 |
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-
2001
- 2001-11-13 US US10/054,228 patent/US6900151B2/en not_active Expired - Fee Related
-
2002
- 2002-10-15 CN CNB028224027A patent/CN100488634C/zh not_active Expired - Fee Related
- 2002-10-15 JP JP2003543737A patent/JP4512365B2/ja not_active Expired - Fee Related
- 2002-10-15 CA CA2466441A patent/CA2466441C/en not_active Expired - Fee Related
- 2002-10-15 AU AU2002335008A patent/AU2002335008B2/en not_active Ceased
- 2002-10-15 WO PCT/US2002/032760 patent/WO2003041860A2/en active IP Right Grant
- 2002-10-15 BR BR0214008-0A patent/BR0214008A/pt not_active IP Right Cessation
- 2002-10-15 EP EP02803155A patent/EP1446226A2/en not_active Withdrawn
- 2002-10-24 TW TW091124779A patent/TWI231812B/zh not_active IP Right Cessation
-
2004
- 2004-05-07 ZA ZA200403504A patent/ZA200403504B/en unknown
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2010
- 2010-03-16 JP JP2010058620A patent/JP2010174248A/ja active Pending
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Publication number | Publication date |
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US20030092781A1 (en) | 2003-05-15 |
JP2005508739A (ja) | 2005-04-07 |
CA2466441A1 (en) | 2003-05-22 |
CN1610582A (zh) | 2005-04-27 |
WO2003041860A2 (en) | 2003-05-22 |
JP2010174248A (ja) | 2010-08-12 |
TWI231812B (en) | 2005-05-01 |
CN100488634C (zh) | 2009-05-20 |
WO2003041860A3 (en) | 2003-12-31 |
US6900151B2 (en) | 2005-05-31 |
ZA200403504B (en) | 2005-05-19 |
BR0214008A (pt) | 2004-11-03 |
CA2466441C (en) | 2010-09-28 |
EP1446226A2 (en) | 2004-08-18 |
AU2002335008B2 (en) | 2007-07-19 |
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