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WO2015180845A1 - Procédé d'élimination d'impuretés métalliques de fractions lourdes d'hydrocarbures - Google Patents

Procédé d'élimination d'impuretés métalliques de fractions lourdes d'hydrocarbures Download PDF

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Publication number
WO2015180845A1
WO2015180845A1 PCT/EP2015/025026 EP2015025026W WO2015180845A1 WO 2015180845 A1 WO2015180845 A1 WO 2015180845A1 EP 2015025026 W EP2015025026 W EP 2015025026W WO 2015180845 A1 WO2015180845 A1 WO 2015180845A1
Authority
WO
WIPO (PCT)
Prior art keywords
hydrocarbon fraction
metal
hydrocarbon
metals
diatomaceous earth
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.)
Ceased
Application number
PCT/EP2015/025026
Other languages
German (de)
English (en)
Inventor
Gerhard Birke
Roberta Olindo
Giuseppe CUSATI
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Air Liquide SA
LAir Liquide SA pour lEtude et lExploitation des Procedes Georges Claude
Original Assignee
Air Liquide SA
LAir Liquide SA pour lEtude et lExploitation des Procedes Georges Claude
Priority date (The priority date 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 date listed.)
Filing date
Publication date
Application filed by Air Liquide SA, LAir Liquide SA pour lEtude et lExploitation des Procedes Georges Claude filed Critical Air Liquide SA
Publication of WO2015180845A1 publication Critical patent/WO2015180845A1/fr
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

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
    • C10G31/00—Refining of hydrocarbon oils, in the absence of hydrogen, by methods not otherwise provided for
    • C10G31/08—Refining of hydrocarbon oils, in the absence of hydrogen, by methods not otherwise provided for by treating with water
    • 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
    • B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
    • B01J20/02—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material
    • B01J20/10—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising silica or silicate
    • B01J20/14—Diatomaceous earth
    • 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
    • C10G25/00—Refining of hydrocarbon oils in the absence of hydrogen, with solid sorbents
    • C10G25/06—Refining of hydrocarbon oils in the absence of hydrogen, with solid sorbents with moving sorbents or sorbents dispersed in the oil
    • 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
    • C10G31/00—Refining of hydrocarbon oils, in the absence of hydrogen, by methods not otherwise provided for
    • C10G31/06—Refining of hydrocarbon oils, in the absence of hydrogen, by methods not otherwise provided for by heating, cooling, or pressure treatment
    • 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
    • C10G31/00—Refining of hydrocarbon oils, in the absence of hydrogen, by methods not otherwise provided for
    • C10G31/09—Refining of hydrocarbon oils, in the absence of hydrogen, by methods not otherwise provided for by filtration
    • 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
    • C10G31/00—Refining of hydrocarbon oils, in the absence of hydrogen, by methods not otherwise provided for
    • C10G31/10—Refining of hydrocarbon oils, in the absence of hydrogen, by methods not otherwise provided for with the aid of centrifugal force
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D15/00—Separating processes involving the treatment of liquids with solid sorbents; Apparatus therefor
    • 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
    • C10G2300/10—Feedstock materials
    • C10G2300/1022—Fischer-Tropsch products
    • 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
    • C10G2300/20—Characteristics of the feedstock or the products
    • C10G2300/201—Impurities
    • C10G2300/205—Metal content

Definitions

  • the invention relates to a process for the removal of metals from high-boiling hydrocarbon fractions, in particular for the separation of catalyst-derived nickel, cobalt and aluminum impurities from the primary products of a hydrocarbon synthesis, for example by the Fischer-Tropsch process.
  • Hydrocarbons may be obtained as synthesis products from chemical catalytic processes, such as the Fischer-Tropsch process, the bases of which have been extensively described in the literature, e.g. In Ullmann 's Encyclopedia of Industrial Chemistry, Sixth Edition, 1998 Electronic Release, keyword “Coal Liquefaction", Chapter 2.2 “Fischer-Tropsch Synthesis”.
  • a modern process variant represents the conversion of synthesis gas in a suspension of the solid, fine-grained catalyst in the liquid product hydrocarbons (so-called slurry process).
  • highly active catalysts are used which contain as active components metals, for example cobalt, on a support material, for example aluminum oxide, as described in US Pat. No. 4,801,573.
  • German Patent DE 1212662 describes a process for treating hydrocarbon oils to remove metallic impurities which are detrimental to the catalysts used in their conversions.
  • it is proposed to treat the contaminated hydrocarbon oils with a solution of hydrogen fluoride in an organic solvent, whereby the metals are converted into a sparingly soluble precipitate, which can be subsequently separated by a mechanical separation method.
  • This avoids the problems described above in the treatment of a two-phase mixture of hydrocarbon phase and aqueous phase.
  • a disadvantage is the use of highly reactive, gaseous hydrogen fluoride for the preparation of the treatment solution for reasons of safety at work and handling.
  • 4,518,484 discloses a process for treating metal-containing hydrocarbon feed streams comprising the steps of: (a) contacting the hydrocarbon feed streams in an extraction zone with at least one hydrocarbon solvent having from 2 to 10 carbon atoms per molecule under supercritical conditions in the presence of a hydrocarbon solvent Organophosphorus-based depleting agent, (b) discharging a top product from the extraction zone containing the largely metal-free hydrocarbons and a bottom product containing the solvent-laden metal.
  • a disadvantage is the complex process control, in particular the setting of supercritical conditions to consider.
  • the subject of the patent application DE 10201 1013470 A1 is a method and means for the removal of metal impurities from hydrocarbon fractions, as obtained, for example, as a product of the Fischer-Tropsch synthesis using suspended catalyst.
  • the feed hydrocarbon fraction is treated with a demetallizing agent comprising at least one sulfur source and at least one basic compound under anhydrous conditions.
  • the metals to be removed are obtained as a precipitate, which can be easily separated by a mechanical separation process, for example filtration.
  • the present invention is therefore based on the object to provide a simple method for the removal of metal contaminants from high-boiling hydrocarbon fractions, which is characterized by a simple process control, and which can be carried out without the use of substances with high risk potential.
  • the object of the invention results essentially from the features of claim 1 by a process for producing a metal-poor hydrocarbon fraction, wherein the metals in the hydrocarbon fraction are chemically bound or dispersed in the hydrocarbon fraction in colloidal or finely dispersed form, comprising the following steps:
  • the object of the invention is achieved essentially with the features of claim 2 by a process for producing a metal-poor hydrocarbon fraction, wherein the metals in the hydrocarbon fraction are chemically bound or dispersed in colloidal or finely dispersed form in the hydrocarbon fraction, comprising the following steps:
  • the feed hydrocarbon fraction must be present in liquid form.
  • Waxy hydrocarbons such as those obtained, for example, as products of the Fischer-Tropsch process, may need to be melted before treatment.
  • the metals are completely removed from the hydrocarbon fraction by treating the hydrocarbon fraction with powdered kieselguhr at temperatures above at least 85 ° C., followed by the subsequent separation of the metal-loaded kieseigur, if the mass ratios of Diatomaceous earth to the total metal content in the hydrocarbon fraction.
  • the method step according to claim 1. (c) or 2. (c) using the filtration. It is also possible to use the centrifugation or decantation; however, the filtration offers an optimum in terms of effort and achieved separation efficiency.
  • the process according to the invention is particularly preferably carried out using pulverulent silica gel whose particle size is less than 40 ⁇ .
  • the stirring speed in process step (b) was the same in all experiments and was constantly 350 revolutions per minute. It is also possible to use other, preferably higher, stirring speeds as long as they ensure intensive mixing of the liquid mixture. If necessary, then the required treatment time must be adjusted in order to achieve the desired degree of metal separation. Suitable periods of time may be determined by routine experimentation. All experiments were carried out in an autoclave with an internal volume of 300 ml.
  • Example 2 Analogously to Example 1, 100 g of a hydrocarbon mixture (wax fraction from the Fischer-Tropsch synthesis with a metal content of 367 ppm by weight (aluminum, nickel and cobalt) were melted at 85 ° C. and initially charged in an autoclave by X-ray fluorescence analysis (RFA) with the method Uniquant 2. The melted wax was then heated to 220 ° C and then 0.25 g of powdered diatomaceous earth with a particle size smaller than 40 ⁇ (Celite 577) was added, the mixture stirred for a further 5 min and The filtrate, which corresponded to the purified hydrocarbon mixture, was analyzed. Analysis of the hydrocarbon fraction showed that only 69% of the metals were removed from the hydrocarbon fraction. The metal separation in this comparative example was therefore insufficient.
  • RFA X-ray fluorescence analysis
  • the invention provides a process for the removal of metal contaminants from hydrocarbon fractions which, compared with the processes known in the prior art, is distinguished by its simplicity of apparatus and by the absence of additional, in particular process-foreign, extractants. Furthermore, it is advantageous that only substances with negligible or low hazard potential are used and the use of substances with high hazard potential, such as hydrogen fluoride, is avoided.

Landscapes

  • Chemical & Material Sciences (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • General Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Analytical Chemistry (AREA)
  • Inorganic Chemistry (AREA)
  • Dispersion Chemistry (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Geochemistry & Mineralogy (AREA)
  • Production Of Liquid Hydrocarbon Mixture For Refining Petroleum (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)

Abstract

L'invention concerne un procédé d'élimination d'impuretés métalliques de fractions lourdes d'hydrocarbures, comme par exemple celles qui sont obtenues comme produit de la synthèse de Fischer-Tropsch à l'aide d'un catalyseur en suspension. Selon l'invention, la fraction d'hydrocarbure à traiter ajouté à l'état fondu, à une température minimale définie, à une quantité minimale définie de diatomite. Les métaux à éliminer sont liés par la diatomite et sont éliminés avec celle-ci du processus par filtration.
PCT/EP2015/025026 2014-05-26 2015-05-21 Procédé d'élimination d'impuretés métalliques de fractions lourdes d'hydrocarbures Ceased WO2015180845A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE102014107375.4 2014-05-26
DE102014107375.4A DE102014107375A1 (de) 2014-05-26 2014-05-26 Verfahren zur Metallentfernung aus hochsiedenden Kohlenwasserstofffraktionen

Publications (1)

Publication Number Publication Date
WO2015180845A1 true WO2015180845A1 (fr) 2015-12-03

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ID=53717972

Family Applications (1)

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PCT/EP2015/025026 Ceased WO2015180845A1 (fr) 2014-05-26 2015-05-21 Procédé d'élimination d'impuretés métalliques de fractions lourdes d'hydrocarbures

Country Status (2)

Country Link
DE (1) DE102014107375A1 (fr)
WO (1) WO2015180845A1 (fr)

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN108220924A (zh) * 2018-01-26 2018-06-29 中国科学院理化技术研究所 一种铜薄膜的制备方法

Citations (8)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US2651655A (en) * 1949-06-29 1953-09-08 Kellogg M W Co Treatment of hydrocarbon waxes
DE1212662B (de) 1962-05-09 1966-03-17 Universal Oil Prod Co Verfahren zum Entfernen metallischer und stickstoffhaltiger Verunreinigungen aus Kohlenwasserstoffoelen
US3947347A (en) * 1972-10-04 1976-03-30 Chevron Research Company Process for removing metalliferous contaminants from hydrocarbons
US4518484A (en) 1984-02-16 1985-05-21 Phillips Petroleum Company Metals removal with a light hydrocarbon and an organophosphorous compound
US4801573A (en) 1987-10-23 1989-01-31 501 Den Norske Stats Oljeslenskap A.S. Catalyst for production of hydrocarbons
WO1998027181A1 (fr) 1996-12-16 1998-06-25 Rentech, Inc. Dispositif separateur catalyseur/cire pour reacteur de fischer-tropsch a combustible en suspension
WO2006053350A1 (fr) 2004-11-10 2006-05-18 Sasol Technology (Pty) Ltd Traitement de courants d'hydrocarbures de masse molaire elevee
DE102011013470A1 (de) 2010-07-26 2012-01-26 L'Air Liquide, Société Anonyme pour l'Etude et l'Exploitation des Procédés Georges Claude Verfahren und Mittel zur Entfernung von Metallen aus hochsiedenden Kohlenwasserstofffraktionen

Family Cites Families (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4412914A (en) * 1981-08-10 1983-11-01 Ashland Oil, Inc. Endothermic removal of coke deposited on sorbent materials during carbo-metallic oil conversion
US6007705A (en) * 1998-12-18 1999-12-28 Exxon Research And Engineering Co Method for demetallating petroleum streams (LAW772)
US8778173B2 (en) * 2008-12-18 2014-07-15 Exxonmobil Research And Engineering Company Process for producing a high stability desulfurized heavy oils stream

Patent Citations (8)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US2651655A (en) * 1949-06-29 1953-09-08 Kellogg M W Co Treatment of hydrocarbon waxes
DE1212662B (de) 1962-05-09 1966-03-17 Universal Oil Prod Co Verfahren zum Entfernen metallischer und stickstoffhaltiger Verunreinigungen aus Kohlenwasserstoffoelen
US3947347A (en) * 1972-10-04 1976-03-30 Chevron Research Company Process for removing metalliferous contaminants from hydrocarbons
US4518484A (en) 1984-02-16 1985-05-21 Phillips Petroleum Company Metals removal with a light hydrocarbon and an organophosphorous compound
US4801573A (en) 1987-10-23 1989-01-31 501 Den Norske Stats Oljeslenskap A.S. Catalyst for production of hydrocarbons
WO1998027181A1 (fr) 1996-12-16 1998-06-25 Rentech, Inc. Dispositif separateur catalyseur/cire pour reacteur de fischer-tropsch a combustible en suspension
WO2006053350A1 (fr) 2004-11-10 2006-05-18 Sasol Technology (Pty) Ltd Traitement de courants d'hydrocarbures de masse molaire elevee
DE102011013470A1 (de) 2010-07-26 2012-01-26 L'Air Liquide, Société Anonyme pour l'Etude et l'Exploitation des Procédés Georges Claude Verfahren und Mittel zur Entfernung von Metallen aus hochsiedenden Kohlenwasserstofffraktionen

Non-Patent Citations (1)

* Cited by examiner, † Cited by third party
Title
"Ullmann's Encyclopedia of Industrial Chemistry", 1998

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN108220924A (zh) * 2018-01-26 2018-06-29 中国科学院理化技术研究所 一种铜薄膜的制备方法

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