CN1239679C - 含硅石脑油的催化加氢处理方法 - Google Patents
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- CXQXSVUQTKDNFP-UHFFFAOYSA-N octamethyltrisiloxane Chemical compound C[Si](C)(C)O[Si](C)(C)O[Si](C)(C)C CXQXSVUQTKDNFP-UHFFFAOYSA-N 0.000 description 1
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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
- C10G45/00—Refining of hydrocarbon oils using hydrogen or hydrogen-generating compounds
- C10G45/02—Refining of hydrocarbon oils using hydrogen or hydrogen-generating compounds to eliminate hetero atoms without changing the skeleton of the hydrocarbon involved and without cracking into lower boiling hydrocarbons; Hydrofinishing
- C10G45/04—Refining of hydrocarbon oils using hydrogen or hydrogen-generating compounds to eliminate hetero atoms without changing the skeleton of the hydrocarbon involved and without cracking into lower boiling hydrocarbons; Hydrofinishing characterised by the catalyst used
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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
- C10G45/00—Refining of hydrocarbon oils using hydrogen or hydrogen-generating compounds
- C10G45/02—Refining of hydrocarbon oils using hydrogen or hydrogen-generating compounds to eliminate hetero atoms without changing the skeleton of the hydrocarbon involved and without cracking into lower boiling hydrocarbons; Hydrofinishing
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- 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
- C10G45/00—Refining of hydrocarbon oils using hydrogen or hydrogen-generating compounds
- C10G45/02—Refining of hydrocarbon oils using hydrogen or hydrogen-generating compounds to eliminate hetero atoms without changing the skeleton of the hydrocarbon involved and without cracking into lower boiling hydrocarbons; Hydrofinishing
- C10G45/04—Refining of hydrocarbon oils using hydrogen or hydrogen-generating compounds to eliminate hetero atoms without changing the skeleton of the hydrocarbon involved and without cracking into lower boiling hydrocarbons; Hydrofinishing characterised by the catalyst used
- C10G45/06—Refining of hydrocarbon oils using hydrogen or hydrogen-generating compounds to eliminate hetero atoms without changing the skeleton of the hydrocarbon involved and without cracking into lower boiling hydrocarbons; Hydrofinishing characterised by the catalyst used containing nickel or cobalt metal, or compounds thereof
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- C10G45/00—Refining of hydrocarbon oils using hydrogen or hydrogen-generating compounds
- C10G45/02—Refining of hydrocarbon oils using hydrogen or hydrogen-generating compounds to eliminate hetero atoms without changing the skeleton of the hydrocarbon involved and without cracking into lower boiling hydrocarbons; Hydrofinishing
- C10G45/04—Refining of hydrocarbon oils using hydrogen or hydrogen-generating compounds to eliminate hetero atoms without changing the skeleton of the hydrocarbon involved and without cracking into lower boiling hydrocarbons; Hydrofinishing characterised by the catalyst used
- C10G45/06—Refining of hydrocarbon oils using hydrogen or hydrogen-generating compounds to eliminate hetero atoms without changing the skeleton of the hydrocarbon involved and without cracking into lower boiling hydrocarbons; Hydrofinishing characterised by the catalyst used containing nickel or cobalt metal, or compounds thereof
- C10G45/08—Refining of hydrocarbon oils using hydrogen or hydrogen-generating compounds to eliminate hetero atoms without changing the skeleton of the hydrocarbon involved and without cracking into lower boiling hydrocarbons; Hydrofinishing characterised by the catalyst used containing nickel or cobalt metal, or compounds thereof in combination with chromium, molybdenum, or tungsten metals, or compounds thereof
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- 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
- C10G49/00—Treatment of hydrocarbon oils, in the presence of hydrogen or hydrogen-generating compounds, not provided for in a single one of groups C10G45/02, C10G45/32, C10G45/44, C10G45/58 or C10G47/00
- C10G49/007—Treatment of hydrocarbon oils, in the presence of hydrogen or hydrogen-generating compounds, not provided for in a single one of groups C10G45/02, C10G45/32, C10G45/44, C10G45/58 or C10G47/00 in the presence of hydrogen from a special source or of a special composition or having been purified by a special treatment
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Abstract
一种催化加氢处理含硅化合物的烃原料的方法,该方法是在氢存在下,在加氢处理该原料的有效条件下,含硅化合物的烃原料与加氢处理催化剂进行接触,其改进之处包括往原料加0.01-10体积%水润湿加氢处理催化剂的步骤。
Description
发明领域
本发明涉及一种催化加氢处理含硅石脑油原料的方法。
发明背景
在每个现代精炼厂中都可见到催化重整装置及其相关的石脑油加氢处理装置。随着双金属重整催化剂的出现,要求重整装置原料中的硫和氮是非常低的,通常小于0.5ppm。石脑油加氢精制方法的直馏原料满足这些要求时,甚至使用低活性或再生的催化剂,达到3年以上循环时间都是不困难的。
因为相对于其他选择,延迟焦化装置较低的设备成本,所以该装置常常是选择用来提高残余油品质的系统。但是,延迟焦化装置产物可在下游设备中引起附加的加工困难,特别地,发现加氢装置和重整催化剂对硅沉积是很敏感的。例如,为防止在焦化塔中起泡沫而使用的硅油中的残余物在石脑油范围内被大量蒸馏出来,可能在下游石脑油加氢精制装置和重整设备中引起催化剂失活。
在远洋开采石油期间,在井中注入硅油时硅污染了石脑油。
在石脑油加氢处理催化剂上硅沉积之源可追溯到加到延迟焦化装置重残渣料的硅油,或可追溯到加到硅烷保压的硅油(Kellberg,L.Zeuthen,P.和Jakobsen,H.J.,因硅油生成硅胶而使HDT催化剂失活。使用29Si和13C CP/MAS NMR表征来自焦化装置石脑油HDT废催化剂,《催化杂志》(J.Catalysis),143,45-51(1993))。
因为生成气体,硅油(聚二甲基硅氧烷,PDMS)通常加到焦化塔中,以便抑制起泡沫。在焦化装置中,硅油通常裂解或分解生成变性的硅胶和碎片。这些硅胶和碎片主要在石脑油段中蒸馏出来,并且随焦化石脑油一起到达加氢处理装置。其他的焦化产物还会含有一些硅,但通常比石脑油产物中的浓度低。
加氢处理焦化石脑油时,二氧化硅的毒化作用是一个严重的问题。催化剂操作时间典型地取决于随原料加入硅的量和使用催化剂系统的“容许”硅量。在原料中没有硅的情况下,大多数石脑油加氢处理催化剂循环时间超过三年。硅呈带部分甲基化表面的硅胶形式从焦化石脑油沉积出来可使催化剂失活,并且使典型的HDS设备循环时间常常降低到一年以下。
通过选择适当的催化剂,设备循环时间可以大大延长超过大多数典型的石脑油加氢处理的催化剂。
硅的吸收取决于催化剂类型和加氢处理装置中的温度。提高温度导致污染物更高的吸收。
石脑油预处理反应器的典型条件是氢压力为20-50巴;平均反应器温度是50-400℃。严格的条件将取决于原料类型、所要求的脱硫程度和所要求的运行时间。离开反应器的石脑油含有可检测量的硅时,一般就达到运行终点。
对于精制装置来说,运行时间是非常重要考虑的一点。较短的运行时间因频繁更换催化剂和由于更换催化剂而延长的停工期(停运时间)带来高成本,因为石脑油生产减少,并且还往重整设备加料而导致收入损失。
本发明的总目的是通过改善加氢处理催化剂的硅容量,提高用于处理含硅原料的加氢处理反应器的操作时间。
发明概述
因此,本发明是一种催化加氢处理含硅化合物的烃原料的方法,该方法是在氢存在下,在加氢处理原料的有效条件下,含硅化合物的烃原料与加氢处理催化剂进行接触,其改进之处包括往原料加0.01-10体积%水润湿加氢处理催化剂的步骤。
优选地将水加到处理气体或石脑油原料,充分润湿加氢处理催化剂时,该催化剂上反应表面-OH物种数量随加氢处理催化剂中硅容量增加而增加。因此,有利地,以含有催化剂的原料体积计,水含量直到10%(体积)都可延长催化剂的操作时间。典型地,水浓度0.1-3%(体积)足够增加催化剂中的硅容量。
硅高度地分散在催化剂表面上,开始在表面上生成单层覆盖层。硅吸收量取决于催化剂的表面。表面积越大,在不变的催化剂金属载荷下,硅的吸收就越高。水不断流入催化剂将进一步增加在催化剂表面上积累的硅量。
在用于加氢处理石油馏分的加氢处理反应器中常常使用的催化剂,在多孔耐高温无机氧化物载体上通常含有至少一种金属。具有加氢处理活性的金属实例包括第VI-B和VIII族的金属,例如Co、Mo、Ni、W、Fe,而Co-Mo、Ni-Mo和Ni-W混合物是优选的。这些金属通常呈氧化物或硫化物形式。适合作载体的多孔材料的实例包括氧化铝、二氧化硅-氧化铝和氧化铝-二氧化钛,而氧化铝和二氧化硅-氧化铝是优选的。
催化剂上的活性金属可以采用一般的方法进行预硫化,或在使用前就地进行硫化。加氢处理反应器部分可以由一个或多个反应器组成。每个反应器有一个或多个催化剂床。加氢处理反应器的功能主要地是降低产生硫、氮和硅。由于脱硫反应和烯烃饱和反应的放热性质,输出温度一般高于输入温度。
实施例
实施例1
在环境压力下,使用通常的加氢处理催化剂进行试验。
丹麦,Haldor Top soe A/S,销售的在高表面积γ-氧化铝上的TK-439,其HBET表面积为380米2/克,孔体积为0.6克/厘米3,曾显示具有很高的Si容量。
与就地干燥催化剂的硅容量相比,通过测量已在环境条件(新的)下与空气接触后的催化剂和预润湿催化剂的Si吸收容量,研究了H2O(表面-O-H基团存在)的影响。知道就地干燥的催化剂具有较低的表面-O-H基团密度。
让He鼓泡(100Nml/分)通过保持在T=0℃的Si-型探针分子六甲基二硅氧烷(HMDSi),测量了Si吸收容量,HMDSi的沸点是101℃,硅含量为17.2%。该气体含有约0.17体积%Si,余量为He。使用校正的质谱仪在线分析了HMDSi消耗。催化剂材料在两个不同的温度350℃和400℃进行处理。
上述试验的结果和条件汇集于表1。
表1
TK-439 | Si容量(毫摩尔/克) | 容量增加(%) |
在T=350℃测量的Si吸收容量 | ||
新的 | 0.71 | 22% |
干燥的 | 0.58 | |
在T=400℃测量的Si吸收容量 | ||
预润湿的 | 0.91 | 15% |
新的 | 0.79 |
实施例2
表2显示了把用水饱和的气流加入实施例1使用的原料时在400℃时的Si容量。气体组成接近于1.4体积%H2O和0.5体积%的HMDSi,平衡量He。
表2
TK-439 | Si容量(毫摩尔/克) | 容量增加(%) |
无H2O | 1.10 | 26 |
有H2O | 1.39 |
Claims (1)
1、一种催化加氢处理含硅化合物的烃原料的方法,该方法是在氢存在下,在加氢处理该原料的有效条件下,含硅化合物的烃原料与加氢处理催化剂进行接触,其特征在于所述加氢处理催化剂是经过往原料中加的水润湿的,所述的加水量为0.01-3体积%。
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CNB011385154A Expired - Fee Related CN1239679C (zh) | 2000-09-15 | 2001-09-15 | 含硅石脑油的催化加氢处理方法 |
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US (1) | US6576121B2 (zh) |
EP (1) | EP1188811B1 (zh) |
JP (1) | JP2002097476A (zh) |
CN (1) | CN1239679C (zh) |
AT (1) | ATE270702T1 (zh) |
DE (1) | DE60104176T2 (zh) |
ES (1) | ES2223692T3 (zh) |
RU (1) | RU2288939C2 (zh) |
ZA (1) | ZA200107449B (zh) |
Families Citing this family (22)
Publication number | Priority date | Publication date | Assignee | Title |
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DE4441105A1 (de) * | 1994-10-17 | 1996-04-18 | Venta Vertriebs Ag | Duftverdunster, insbesondere für Toiletten |
EP1664248B1 (en) * | 2003-09-03 | 2011-12-21 | Shell Internationale Research Maatschappij B.V. | Fuel compositions |
EP1925654A1 (en) | 2006-11-22 | 2008-05-28 | Haldor Topsoe A/S | Process for the catalytic hydrotreating of silicon containing hydrocarbon feedstock |
CN101343566B (zh) * | 2007-07-09 | 2012-08-29 | 中国石油化工股份有限公司 | 一种提高劣质石脑油加氢装置运转周期的方法 |
CN101343565B (zh) * | 2007-07-09 | 2011-12-21 | 中国石油化工股份有限公司 | 一种含硅馏分油加氢精制方法 |
BRPI0802431B1 (pt) | 2008-07-28 | 2017-02-07 | Petróleo Brasileiro S/A - Petrobras | processo de remoção de compostos de silício de correntes de hidrocarbonetos |
US20130319662A1 (en) * | 2012-05-29 | 2013-12-05 | Emilio Alvarez | Systems and Methods For Hydrotreating A Shale Oil Stream Using Hydrogen Gas That Is Concentrated From The Shale Oil Stream |
AU2014340644B2 (en) | 2013-10-22 | 2017-02-02 | Exxonmobil Upstream Research Company | Systems and methods for regulating an in situ pyrolysis process |
US9394772B2 (en) | 2013-11-07 | 2016-07-19 | Exxonmobil Upstream Research Company | Systems and methods for in situ resistive heating of organic matter in a subterranean formation |
AU2015350480A1 (en) | 2014-11-21 | 2017-05-25 | Exxonmobil Upstream Research Company | Mitigating the effects of subsurface shunts during bulk heating of a subsurface formation |
CN105038843B (zh) * | 2015-06-12 | 2017-06-23 | 中国石油大学(华东) | 一种柴油气相加氢脱硫工艺方法 |
CN106281729A (zh) * | 2015-06-23 | 2017-01-04 | 中国石油化工股份有限公司 | 一种可再生原料的加氢处理方法 |
CN106281728A (zh) * | 2015-06-23 | 2017-01-04 | 中国石油化工股份有限公司 | 一种制备喷气燃料的方法 |
CN108349853B (zh) | 2015-11-12 | 2022-03-15 | 沙特基础工业全球技术公司 | 生产芳烃和烯烃的方法 |
EP3394219A1 (en) | 2015-12-21 | 2018-10-31 | SABIC Global Technologies B.V. | Methods and systems for producing olefins and aromatics from coker naphtha |
US10253272B2 (en) | 2017-06-02 | 2019-04-09 | Uop Llc | Process for hydrotreating a residue stream |
RU2693380C1 (ru) * | 2018-12-20 | 2019-07-02 | Федеральное государственное бюджетное учреждение науки "Федеральный исследовательский центр "Институт катализа им. Г.К. Борескова Сибирского отделения Российской академии наук" (ИК СО РАН) | Способ очистки дизельного топлива от соединений кремния |
WO2020171965A1 (en) * | 2019-02-22 | 2020-08-27 | Exxonmobil Research And Engineering Company | Hydroprocessing feedstocks having silicon content |
FR3117886A1 (fr) | 2020-12-21 | 2022-06-24 | IFP Energies Nouvelles | Procede de captation de silicium en absence d’hydrogene |
FR3117893A1 (fr) | 2020-12-21 | 2022-06-24 | IFP Energies Nouvelles | Procede de rejuvenation de masse de captation de silicium |
FR3117887A1 (fr) | 2020-12-21 | 2022-06-24 | IFP Energies Nouvelles | Procede de captation de silicium a faible vitesse spatiale horaire |
US20220235284A1 (en) * | 2021-01-27 | 2022-07-28 | Phillips 66 Company | Decreasing refinery fouling and catalyst deactivation |
Family Cites Families (6)
Publication number | Priority date | Publication date | Assignee | Title |
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US4196102A (en) * | 1975-12-09 | 1980-04-01 | Chiyoda Chemical Engineering & Construction Co., Ltd. | Catalysts for demetallization treatment of _hydrocarbons supported on sepiolite |
US4176047A (en) * | 1978-04-10 | 1979-11-27 | Continental Oil Company | Removal of organic compounds from coker gasoline |
US4645587A (en) * | 1984-12-07 | 1987-02-24 | Union Oil Company Of California | Process for removing silicon compounds from hydrocarbon streams |
US5173173A (en) * | 1990-09-28 | 1992-12-22 | Union Oil Company Of California | Trace contaminant removal in distillation units |
US5118406A (en) * | 1991-04-30 | 1992-06-02 | Union Oil Company Of California | Hydrotreating with silicon removal |
FR2764213B1 (fr) * | 1997-06-10 | 1999-07-16 | Inst Francais Du Petrole | Catalyseur d'hydrotraitement de charges hydrocarbonees dans un reacteur a lit fixe |
-
2001
- 2001-08-31 AT AT01120960T patent/ATE270702T1/de not_active IP Right Cessation
- 2001-08-31 DE DE2001604176 patent/DE60104176T2/de not_active Expired - Lifetime
- 2001-08-31 ES ES01120960T patent/ES2223692T3/es not_active Expired - Lifetime
- 2001-08-31 EP EP01120960A patent/EP1188811B1/en not_active Expired - Lifetime
- 2001-09-10 ZA ZA200107449A patent/ZA200107449B/xx unknown
- 2001-09-10 US US09/950,523 patent/US6576121B2/en not_active Expired - Lifetime
- 2001-09-14 RU RU2001125150/04A patent/RU2288939C2/ru not_active IP Right Cessation
- 2001-09-14 JP JP2001279481A patent/JP2002097476A/ja active Pending
- 2001-09-15 CN CNB011385154A patent/CN1239679C/zh not_active Expired - Fee Related
Also Published As
Publication number | Publication date |
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ZA200107449B (en) | 2002-08-05 |
EP1188811B1 (en) | 2004-07-07 |
DE60104176D1 (de) | 2004-08-12 |
US6576121B2 (en) | 2003-06-10 |
CN1348979A (zh) | 2002-05-15 |
JP2002097476A (ja) | 2002-04-02 |
RU2288939C2 (ru) | 2006-12-10 |
EP1188811A1 (en) | 2002-03-20 |
ES2223692T3 (es) | 2005-03-01 |
DE60104176T2 (de) | 2004-11-18 |
ATE270702T1 (de) | 2004-07-15 |
US20020056665A1 (en) | 2002-05-16 |
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