EP0233169B2 - Verfahren zur Behandlung von Gasölen - Google Patents
Verfahren zur Behandlung von Gasölen Download PDFInfo
- Publication number
- EP0233169B2 EP0233169B2 EP87870016A EP87870016A EP0233169B2 EP 0233169 B2 EP0233169 B2 EP 0233169B2 EP 87870016 A EP87870016 A EP 87870016A EP 87870016 A EP87870016 A EP 87870016A EP 0233169 B2 EP0233169 B2 EP 0233169B2
- Authority
- EP
- European Patent Office
- Prior art keywords
- hydrocarbons
- feed
- silicalite
- process according
- catalyst
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Expired - Lifetime
Links
Classifications
-
- 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
- C10G45/58—Refining of hydrocarbon oils using hydrogen or hydrogen-generating compounds to change the structural skeleton of some of the hydrocarbon content without cracking the other hydrocarbons present, e.g. lowering pour point; Selective hydrocracking of normal paraffins
- C10G45/60—Refining of hydrocarbon oils using hydrogen or hydrogen-generating compounds to change the structural skeleton of some of the hydrocarbon content without cracking the other hydrocarbons present, e.g. lowering pour point; Selective hydrocracking of normal paraffins characterised by the catalyst used
- C10G45/64—Refining of hydrocarbon oils using hydrogen or hydrogen-generating compounds to change the structural skeleton of some of the hydrocarbon content without cracking the other hydrocarbons present, e.g. lowering pour point; Selective hydrocracking of normal paraffins characterised by the catalyst used containing crystalline alumino-silicates, e.g. molecular sieves
-
- 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
- C10G65/00—Treatment of hydrocarbon oils by two or more hydrotreatment processes only
- C10G65/02—Treatment of hydrocarbon oils by two or more hydrotreatment processes only plural serial stages only
- C10G65/12—Treatment of hydrocarbon oils by two or more hydrotreatment processes only plural serial stages only including cracking steps and other hydrotreatment steps
-
- 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
- C10G2300/00—Aspects relating to hydrocarbon processing covered by groups C10G1/00 - C10G99/00
- C10G2300/70—Catalyst aspects
-
- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F02—COMBUSTION ENGINES; HOT-GAS OR COMBUSTION-PRODUCT ENGINE PLANTS
- F02B—INTERNAL-COMBUSTION PISTON ENGINES; COMBUSTION ENGINES IN GENERAL
- F02B3/00—Engines characterised by air compression and subsequent fuel addition
- F02B3/06—Engines characterised by air compression and subsequent fuel addition with compression ignition
Definitions
- the present invention relates to a method for treating diesel fuel charges in order to be able to extract more valuable products than usual treatments.
- the present invention is relates to a particular combination of two treatments of diesel fuel charges in order to promote diesel and gasoline production.
- Heavy gas oils (vacuum distillation, VGO, or cut 370 to 540 ° C gas oils) were generally sent directly to the catalytic cracking unit in order to convert them into lighter hydrocarbons, highly recoverable; it is however desirable to try to make the best use of all the constituents gas oils, whether from atmospheric distillation or vacuum distillation. It was moreover realized during these last years, that it was possible to treat the gas oils before send them to catalytic cracking so as to recover many more recoverable products than by catalytic cracking alone.
- Gas oils can also be subjected to a process allowing to eliminate hydrocarbons waxy paraffinics. This leads to lowering the cloud point of gas oils.
- EP-A-0 070 125 describes a process for treating boiling hydrocarbons in the range of heavy diesel oils, in the presence of a catalyst consisting of a mixture comprising generally modified silicalite and a catalyst hydrogenation deposited on a support, Significant results of pour point reduction are obtained when the silicalite is modified with a catalytic metal of the palladium type.
- the present invention relates to a process for treating hydrocarbons boiling in the range of heavy gas oils to increase recovery of light hydrocarbons.
- the present invention also relates to a process for treating heavy gas oils in two steps to increase the production of diesel oil and gasoline compared to the quantity generally recoverable by catalytic cracking of the same charge.
- the present invention also relates to a method which makes it possible to treat hydrocarbons having a boiling point between about 370 ° C and 540 ° C so as to obtain a significant amount of variable light hydrocarbons.
- La Damanderesse unexpectedly found that by first submitting the hydrocarbon load boiling in the range of heavy gas oils to a treatment to remove paraffinic hydrocarbons waxy, by passing over a polymorphic crystalline silica of the unmodified silicalite type in appropriate conditions, and by subjecting the resulting charge to light hydrocracking, a production of light hydrocarbons, notably diesels and gasolines, in quantities clearly improved over what could reasonably be expected.
- the fillers used for the process of the invention are heavy gas oils, or distillation gas oils under vacuum (VGO), comprising the fraction of hydrocarbons having a boiling point of 370 to 540 ° C about. These charges may contain at most 25% of hydrocarbons having a boiling point below 370 ° C.
- VGO distillation gas oils under vacuum
- the process of the invention is particularly suitable for loads of heavy diesel containing large sulfur contents as high as 4% (by weight).
- a preferred application of the invention resides in the treatment of charges containing more than approximately 1% of sulfur.
- an unmodified silicalite that is to say a crystalline silica
- polymorph which has no exchange capacity compared to zeolites and which has not been modified by a catalytic metal.
- Aluminum can be present in these catalysts, but only in the form impurities from the starting materials and in particular from the source of silica used. The methods to obtain these materials are given in US Patent 4,061,724 to Grose and Flanigen.
- Silicalites are microporous materials prepared hydrothermally using a mixture reaction comprising tetrapropylammonium cations, alkali metal cations, water and a source of reactive silica.
- an unmodified silicalite having pores is used in the process of the invention. approximately 0.55 nm, and being in the form of crystallites of size less than 8 ⁇ m.
- the waxy paraffinic hydrocarbon removal step can be performed in any device comprising a reaction zone containing the silicalite type catalyst.
- the Applicant has surprisingly found that by directly submitting the charge resulting from the first step in a light hydrocracking, a final charge containing light hydrocarbons in much larger quantities than could be expected.
- the light hydrocracking reaction is carried out on a conventional light hydrocracking catalyst.
- a conventional light hydrocracking catalyst By way of example, there may be mentioned a Ni-Mo catalyst deposited on alumina and silica, prepared by incorporation of Ni and Mo in the form of oxide followed by drying and then by treatment with sweeping of a mixture of hydrogen and H 2 S (1-2% vol.) first at 200-250 ° C then up to 320-350 ° C.
- This catalyst can also be partially replaced by a Co-Mo catalyst deposited on alumina, prepared in a similar manner.
- these catalysts In their oxide form, these catalysts generally contain from 3 to 6% by weight of NiO or CoO, and from 10 to 20% by weight of MoO 3 ; they have a specific surface generally between 150 and 300 m 2 / g and the pore volume is generally between 0.3 and 0.6 ml / g. These catalysts are commercially available in oxide form.
- the reactions can be carried out in two reactors arranged in cascade and in temperature and pressure conditions which need not necessarily be identical, the Applicant found that both reactions could take place in the same reactor.
- different catalysts play a certain role in obtaining interesting results. This is how the The Applicant has found that 15 to 25% by volume of silicalite should be used, relative to the total catalyst and from 85 to 75% by volume of light hydrocracking catalyst.
- the catalysts can be arranged in several layers that can be surrounded by layers of inert materials.
- the two stages of the process in the same reactor, and the different catalysts are thus arranged in several beds, the first bed encountered being constituted by a polymorphic crystalline silica of the unmodified silicalite type.
- the charge is passed through the reaction zone containing the catalysts at a temperature between 350 and 450 ° C, and preferably between 380 and 420 ° C, under a pressure between atmospheric pressure and 80 bars, and preferably between 35 and 65 bars, and at an hourly space speed liquid (LHSV) between 0.1 and 20 I / I (calculated with respect to all the catalysts), preferably between 0.5 and 5 l / l.
- LHSV hourly space speed liquid
- hydrogen is introduced into the reaction zone, in an amount such that the hydrogen / hydrocarbons volume ratio is between 50 and 5000 and preferably between 250 and 1000 (the volume of hydrogen being measured in the gaseous state and under standard conditions).
- the hydrogen / hydrocarbons volume ratio is between 50 and 5000 and preferably between 250 and 1000 (the volume of hydrogen being measured in the gaseous state and under standard conditions).
- the gas recovered at the output from the reactor is generally recycled.
- part of the gas is permanently withdrawn recycles which is replaced by hydrogen.
- a 2.5 cm inside diameter reactor was filled with 20% by volume (i.e. 7 cm in height) of silicalite and 80% by volume (i.e. 28 cm in height) of Ni-Mo catalyst, all between two layers of inert material (each 40 cm high).
- a load of hydrocarbons was passed into the reactor in normal mode, the charge passing through successively silicalite, then Ni-Mo.
- the hydrogen from the refinery (called “pure” but containing about 85% hydrogen) at a partial hydrogen pressure of at least 40 bar.
- Example 2 The procedure described in Example 1 was repeated, replacing the Ni-Mo catalyst for half by a Co-Mo catalyst on alumina (commercially available under the name Ketjen 742) and for the other half by a catalyst. Ni-Mo on Al 2 O 3 / SiO 2 . The charge passed successively through the silicalite, the Co-Mo then the Ni-Mo.
- Example no Catalysts LHSV Conversion 1A silicalite / Ni-Mo 0.6 51.1 2 silicalite / Co-Mo / Ni-Mo 0.6 48.7 3A Ni-Mo / silicalite 0.6 50.8 C1 silicalite 3 5.6 C2 Ni-mo 0.6 34.9 C3 Ni-mo 0.75 26.9 1B silicalite / Ni-Mo 1.0 36.6 3B Ni-Mo / silicalite 1.0 30.7 C4 silicalite 5 5.0 C5 Ni-mo 1.0 24.7 C6 Ni-mo 1.25 19.3 1 C silicalite / Ni-Mo 1.5 21.8 3C Ni-Mo / silicalite 1.5 19.2 C7 silicalite 7.5 3.4 C8
- Example no. 1A C1 C3 Effluent composition (% by weight) hydrocarbons C 1 to C 4 7.17 2.99 1.45 section C 5 -180 ° C 14.18 3.19 7.58 180-250 ° C cut 9.01 2.28 7.79 cut 250-370 ° C 31.51 17.85 29.29 cutting 370 + ° C 38.13 73.69 53.89 Cutting properties 180-250 ° C density d 15/4 0.844 0.845 freezing point ⁇ -57 ° C -54 ° C cloud point ⁇ -45 ° C -45 ° C Cutting properties 250-370 ° C density d 15/4 0.893 0.884 freezing point -24 ° C - 4 ° C cloud point -27 ° C - 4 ° C cetane number 41.2 43.9
Claims (6)
- Verfahren zur Behandlung einer Beschickung von Kohlenwasserstoffen, das in dem Bereich von schweren Gasölen siedet, um leichte Kohlenwasserstoffe daraus zu extrahieren, umfassend ein leichtes Hydrocracken und eine Entfernung von paraffinischen wachsartigen Kohlenwasserstoffen, dadurch gekennzeichnet, daß es besteht aus(i) Aussetzen dieser Beschickung einer Entfernung paraffinischer wachsartiger Kohlenwasserstoffe, indem man die Beschickung über einen Katalysator, gebildet durch ein kristallines polymorphes Siliciumdioxid vom Typ nicht modifizierter Silicalit, unter angemessenen Bedingungen passieren läßt, um die paraffinischen wachsartigen Kohlenwasserstoffe zu cracken, dann(ii) Aussetzen der aus der ersten Stufe resultierenden Beschickung einem leichtem Hydrocracken über einem klassischen Katalysator für leichtes Hydrocracken und schließlich(iii) Gewinnen der Beschickung, die eine erhebliche Menge leichter Kohlenwasserstoffe umfaßt,
- Verfahren nach Anspruch 1, dadurch gekennzeichnet, daß die Beschickung mindestens 75% von Kohlenwasserstoffen mit einem Siedepunkt von 370 bis 540°C umfaßt.
- Verfahren nach einem der Ansprüche 1 oder 2, dadurch gekennzeichnet, daß die Beschickung 1 bis 4% von Schwefel enthält.
- Verfahren nach einem der Ansprüche 1 bis 3, dadurch gekennzeichnet, daß das Verfahren bei einer Temperatur von 350 bis 450°C, bei einem Druck von 1 bis 80 Bar und bei einer LHSV von 0,1 bis 20 in Anwesenheit von Wasserstoff in einer solchen Menge realisiert wird, daß das Volumenverhältnis H2/HC von 50 bis 5000 ist.
- Verfahren nach einem der Ansprüche 1 bis 4, dadurch gekennzeichnet, daß das Verfahren bei einer Temperatur von 380 bis 420°C, bei einem Druck von 35 bis 65 Bar und bei einer LHSV von 0,5 bis 5 in Anwesenheit von Wasserstoff in einer solchen Menge realisiert wird, daß das Volumenverhältnis H2/HC von 250 bis 1000 ist.
- Verfahren nach einem der Ansprüche 1 bis 5, dadurch gekennzeichnet, daß die Stufen (i) und (ii) durch aufeinanderfolgende Durchleitung über getrennten Betten von Katalysatoren in einem gleichen Reaktor realisiert werden.
Applications Claiming Priority (2)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
LU86288A LU86288A1 (fr) | 1986-02-03 | 1986-02-03 | Procede de traitement des gasoils |
LU86288 | 1986-02-03 |
Publications (4)
Publication Number | Publication Date |
---|---|
EP0233169A2 EP0233169A2 (de) | 1987-08-19 |
EP0233169A3 EP0233169A3 (en) | 1989-02-22 |
EP0233169B1 EP0233169B1 (de) | 1991-12-27 |
EP0233169B2 true EP0233169B2 (de) | 2001-08-29 |
Family
ID=19730635
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
EP87870016A Expired - Lifetime EP0233169B2 (de) | 1986-02-03 | 1987-02-03 | Verfahren zur Behandlung von Gasölen |
Country Status (5)
Country | Link |
---|---|
US (1) | US4810356A (de) |
EP (1) | EP0233169B2 (de) |
JP (1) | JP2879793B2 (de) |
DE (1) | DE3775426D1 (de) |
LU (1) | LU86288A1 (de) |
Families Citing this family (10)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US5385663A (en) * | 1992-06-18 | 1995-01-31 | Uop | Integrated hydrocracking-catalytic dewaxing process for the production of middle distillates |
RU2128681C1 (ru) * | 1993-10-08 | 1999-04-10 | Акцо Нобель Н.В. | Способ превращения парафинсодержащего углеводородного сырья |
US5690810A (en) * | 1994-11-14 | 1997-11-25 | Texaco Inc. | Single-step process to upgrade naphthas to an improved gasoline blending stock |
US6068757A (en) * | 1995-11-03 | 2000-05-30 | Coastal Eagle Point Oil Company | Hydrodewaxing process |
EP0920911A1 (de) * | 1997-12-05 | 1999-06-09 | Fina Research S.A. | Herstellung von Katalysatoren für die Olefinumsetzung |
US6461497B1 (en) | 1998-09-01 | 2002-10-08 | Atlantic Richfield Company | Reformulated reduced pollution diesel fuel |
CA2292314C (en) * | 1998-12-16 | 2007-02-06 | China Petrochemical Corporation | A process for producing diesel oils of superior quality and low solidifying point from fraction oils |
EP1061117A1 (de) * | 1999-06-16 | 2000-12-20 | Fina Research S.A. | Herstellung von Olefinen |
US20030070965A1 (en) * | 1999-11-01 | 2003-04-17 | Shih Stuart S. | Method for the production of very low sulfur diesel |
US7955401B2 (en) * | 2007-07-16 | 2011-06-07 | Conocophillips Company | Hydrotreating and catalytic dewaxing process for making diesel from oils and/or fats |
Citations (2)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
GB1443877A (en) † | 1973-06-15 | 1976-07-28 | Mobil Oil Corp | Catalytic dewaxing of gas oils |
US4309276A (en) † | 1980-04-28 | 1982-01-05 | Chevron Research Company | Hydrocarbon conversion with low-sodium silicalite |
Family Cites Families (23)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US3700585A (en) * | 1969-10-10 | 1972-10-24 | Mobil Oil Corp | Dewaxing of oils by shape selective cracking and hydrocracking over zeolites zsm-5 and zsm-8 |
US3654133A (en) | 1970-06-23 | 1972-04-04 | Universal Oil Prod Co | Dewaxed lubricating oil production |
US4061724A (en) * | 1975-09-22 | 1977-12-06 | Union Carbide Corporation | Crystalline silica |
US4229282A (en) * | 1979-04-27 | 1980-10-21 | Mobil Oil Corporation | Catalytic dewaxing of hydrocarbon oils |
US4419271A (en) * | 1979-10-15 | 1983-12-06 | Union Oil Company Of California | Hydrocarbon conversion catalyst |
US4292166A (en) * | 1980-07-07 | 1981-09-29 | Mobil Oil Corporation | Catalytic process for manufacture of lubricating oils |
US4428862A (en) * | 1980-07-28 | 1984-01-31 | Union Oil Company Of California | Catalyst for simultaneous hydrotreating and hydrodewaxing of hydrocarbons |
JPS5763134A (en) * | 1980-07-28 | 1982-04-16 | Union Oil Co | Simultaneous hydrogenation dewaxing and hydrogenation treatment method for hydrocarbon and catalyst used for said method |
US4347121A (en) * | 1980-10-09 | 1982-08-31 | Chevron Research Company | Production of lubricating oils |
US4325805A (en) * | 1980-12-18 | 1982-04-20 | Chevron Research Company | Lubricating oil stabilization |
US4361477A (en) * | 1981-04-17 | 1982-11-30 | Chevron Research Company | Stabilizing and dewaxing lube oils |
US4561967A (en) * | 1981-04-23 | 1985-12-31 | Chevron Research Company | One-step stabilizing and dewaxing of lube oils |
US4362653A (en) * | 1981-04-27 | 1982-12-07 | Uop Inc. | Hydrocarbon conversion catalyst |
US4428825A (en) * | 1981-05-26 | 1984-01-31 | Union Oil Company Of California | Catalytic hydrodewaxing process with added ammonia in the production of lubricating oils |
US4513090A (en) * | 1981-07-09 | 1985-04-23 | Exxon Research And Engineering Co. | Crystalline silica zeolite-containing catalyst |
US4443329A (en) * | 1981-07-09 | 1984-04-17 | Exxon Research And Engineering Co. | Crystalline silica zeolite-containing catalyst and hydrocarbon hydroprocesses utilizing the same |
US4394249A (en) * | 1981-08-03 | 1983-07-19 | Mobil Oil Corporation | Catalytic dewaxing process |
CA1203225A (en) * | 1981-08-07 | 1986-04-15 | Stephen M. Oleck | Two-stage hydrocarbon dewaxing hydrotreating process |
US4458024A (en) * | 1982-02-08 | 1984-07-03 | Mobil Oil Corporation | Process for hydrotreating petroleum residua and catalyst therefor |
US4490570A (en) * | 1982-02-22 | 1984-12-25 | Cosden Technology, Inc. | Method for para selective alkylation employing silicalite catalysts |
US4548705A (en) * | 1982-03-09 | 1985-10-22 | Union Oil Company Of California | Hydrocracking with catalytically active amorphous silica and zeolites |
US4599473A (en) * | 1983-12-19 | 1986-07-08 | Cosden Technology, Inc. | Process for para selective alkylation of aromatic hydrocarbons |
US4597854A (en) * | 1985-07-17 | 1986-07-01 | Mobil Oil Corporation | Multi-bed hydrodewaxing process |
-
1986
- 1986-02-03 LU LU86288A patent/LU86288A1/fr unknown
-
1987
- 1987-02-02 JP JP62020601A patent/JP2879793B2/ja not_active Expired - Lifetime
- 1987-02-03 US US07/010,223 patent/US4810356A/en not_active Expired - Lifetime
- 1987-02-03 DE DE8787870016T patent/DE3775426D1/de not_active Expired - Lifetime
- 1987-02-03 EP EP87870016A patent/EP0233169B2/de not_active Expired - Lifetime
Patent Citations (2)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
GB1443877A (en) † | 1973-06-15 | 1976-07-28 | Mobil Oil Corp | Catalytic dewaxing of gas oils |
US4309276A (en) † | 1980-04-28 | 1982-01-05 | Chevron Research Company | Hydrocarbon conversion with low-sodium silicalite |
Also Published As
Publication number | Publication date |
---|---|
EP0233169B1 (de) | 1991-12-27 |
EP0233169A2 (de) | 1987-08-19 |
US4810356A (en) | 1989-03-07 |
JP2879793B2 (ja) | 1999-04-05 |
LU86288A1 (fr) | 1987-09-10 |
JPS62246995A (ja) | 1987-10-28 |
EP0233169A3 (en) | 1989-02-22 |
DE3775426D1 (de) | 1992-02-06 |
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