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GB1563357A - Hydrogenation process - Google Patents

Hydrogenation process Download PDF

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Publication number
GB1563357A
GB1563357A GB5207476A GB5207476A GB1563357A GB 1563357 A GB1563357 A GB 1563357A GB 5207476 A GB5207476 A GB 5207476A GB 5207476 A GB5207476 A GB 5207476A GB 1563357 A GB1563357 A GB 1563357A
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process according
range
catalyst
fraction
hydrogenation
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GB5207476A
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BP PLC
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BP PLC
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    • CCHEMISTRY; METALLURGY
    • C10PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10GCRACKING 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
    • C10G47/00Cracking of hydrocarbon oils, in the presence of hydrogen or hydrogen- generating compounds, to obtain lower boiling fractions
    • C10G47/32Cracking of hydrocarbon oils, in the presence of hydrogen or hydrogen- generating compounds, to obtain lower boiling fractions in the presence of hydrogen-generating compounds
    • C10G47/34Organic compounds, e.g. hydrogenated hydrocarbons
    • CCHEMISTRY; METALLURGY
    • C10PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10GCRACKING 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
    • C10G65/00Treatment of hydrocarbon oils by two or more hydrotreatment processes only
    • C10G65/02Treatment of hydrocarbon oils by two or more hydrotreatment processes only plural serial stages only

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  • Chemical & Material Sciences (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • General Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Production Of Liquid Hydrocarbon Mixture For Refining Petroleum (AREA)

Description

(54) HYDROGENATION PROCESS (71) We, THE BRITISH PETROLEUM COMPANY LIMITED, of Britannic House, Moor Lane, London EC2Y 9BU, a British Company, do hereby declare the invention, for which we pray that a patent may be granted to us, and the method by which it is to be performed, to be particularly described in and by the following statement:- The present invention relates to a process for the hydrogenation of unsaturated hydrocarbons and optionally cracking the hydrogenated derivatives.
The process is particularly suitable for treating polynuclear aromatic hydrocarbons contained in heavy petroleum fractions such as atmospheric residue, waxy distillate and vacuum residue.
In the operation of a typical oil refinery, crude oil is initially fed to a distillation unit in which it is separated at atmospheric pressure into benzine, naphtha, kerosine and gas oil. The residue from the atmospheric distillation unit, known as atmospheric residue, is composed of fractions boiling under atmospheric pressure at a temperature greater than 3500 C. This residue may either be used directly as a fuel oil or as a feedstock to a distillation unit operating under reduced pressure.
The distillate from the vacuum distillation unit, known as waxy distillate, vacuum distillate or vacuum gas oil may be used as a catalytic cracker feedstock or used in lubricating oil manufacture, whilst the residue, known as vacuum residue, may be used as a fuel oil component.
The naphtha fraction is particularly important since, amongst other reasons, directly or indirectly it is the source of benzene, toluene and xylene, known collectively as BTX, and indirectly the source of olefins via steam cracking. BTX is a valuable motor spirit component because of its high octane number and it is also in demand as chemical feedstock.
With increasing crude oil prices, it is becoming more necessary to increase the conversion of crude petroleum to high value products, particularly the conversion of heavier fractions and to minimise the production of relatively low value residues.
Our British Patent 1361671 claims a process for the production of olefins which process comprises hydrogenating a petroleum distillate feedstock containing aromatic hydrocarbons in the presence of a hydrogenation catalyst and hydrogen to at least partially saturate the aromatic hydrocarbons in the feedstock and thermally cracking directly the resulting hydrogenated product in the presence of steam.
We have now discovered a process for the hydrogenation of heavy petroleum fractions using a hydrogen donor instead of or as a partial replacement for hydrogen, which may be combined with a cracking process.
Thus according to the present invention there is provided a process for the hydrogenation of a petroleum fraction containing at least 25% by wt of materialboiling above 350"C, preferably at least 25% by wt of material boiling above 5500 C, which process comprises contacting the fraction at elevated temperature and pressure with a hydrogen donor and a catalyst comprising from 525% of a metal of Group VIA of the Periodic Table, i.e., Mo, W, or Cr, on a refractory support, the percentage being by weight of total catalyst.
The catalyst may be promoted by the addition of 1--10% by wt of an Iron Group metal, i.e., Fe, Co or Ni.
Suitable hydrogen donors include partially hydrogenated polycyclic aromatic compounds, such as tetralin, the preferred donor, and naphthenes, such as decalin.
The hydrogen donor is suitably present in amount 20:1 to 1:1 by wt of the feedstock, preferably in amount 4:1.
Particularly preferred feedstocks are atmospheric residues boiling above 350"C. Depending on the original crude oil source the feedstocks may contain 1 -8% by wt sulphur, 01% by wt nitrogen, 1W10,000 ppm by wt metals and 1-20% by wt asphaltenes.
The catalyst may be used in the sulphided or unsulphided form and under an inert atmosphere, e.g., nitrogen, or hydrogen.
The feedstock may, if desired, be given a preliminary treatment, to remove asphaltenes and/or metal compounds.
The hydrogenation process conditions may be chosen from the following ranges: Broad Range Preferred Range Temperature OC 100 - 400 250 - 350 Pressure bars(ga) 1 - 100 1 - 20 Space velocity v/v/hr 0.1 - 10 0.5 - 2 The catalyst percentages above are expressed as element per cent by wt of total catalyst, but the metals will normally be present as compounds, particularly the oxides or sulphides. Preferred combinations are cobalt and molybdenum, nickel and molybdenum, nickel and tungsten or nickel, cobalt and molybdenum. If two or more iron group metals are used the total iron group metal content should remain in the range 1--10% wt.
The refractory support may be one or more oxides of elements of Groups III or IV of the Periodic Table, particularly alumina, silica, or silica-alumina. A single oxide, particularly alumina, is preferred to limit side reactions. The alumina may contain up to 5% wt of silica or phosphate to stabilise it and/or give the required pore characteristics.
The method of preparation of the catalyst as regards the Iron Group metal, the croup VIA metal and the support may follow standard practice. Thus the metals may be added by simultaneous or sequential impregnation with suitable salt solutions, followed by drying, calcination, and, if necessary, pre-sulphiding.
Attention must be paid to both physical and chemical characteristics of the catalysts used. Microporous catalysts, with most of the surface area in pores with diameters less than 300A combine good activity with reasonable life. These catalysts show less tendency to pick up metals and asphaltenes present in the feed.
The hydrogenated material is more suitable for cracking to high value products than the unhydrogenated feedstock.
If an acidic catalyst support is employed then hydrogenation and cracking can occur in a one stage process over a single catalyst.
Thus according to a modification of the invention there is provided a process for the hydrogenation and cracking of a petroleum fraction containing at least 25% by wt of material boiling above 3500 C, preferably at least 25% by wt of material boiling above 5500 C, which process comprises contacting the fraction at elevated temperature and pressure with a hydrogen donor and a catalyst comprising from 1-1 0% by wt of an Iron Group metal, i.e., Fe,Co or Ni, and from 525% by wt of a metal of Group VIA, i.e., Mo, W or Cr, on a refractory acidic support, all percentages being in weight of total catalyst.
Suitable acidic catalysts include silica-alumina, zeolites and alumina or silicaalumina treated with a halide such as fluorine.
The cracked products include useful chemicals such as benzene, toluene and xylene, naphthalene and substituted naphthalenes. The naphthalenes and substituted naphthalenes are potential hydrogen donors and can be hydrogenated to donors in a separate step and recycled to the hydrogenation/cracking stage together with unconverted donor.
Thus according to a further feature of the present invention there is provided a process for the production of BTX from a petroleum fraction containing at least 25% by wt of material boiling above 3500C, preferably at least 25% of material boiling above 5500 C, which process comprises (a) contacting the fraction at elevated temperature and pressure with a hydrogen donor and a catalyst comprising from 1--10% by wt of an Iron Group metal as hereinbefore defined and from 525% by weight of a metal of Group VIA as hereinbefore defined on a refractory acidic support, all percentages being by weight of total catalyst, (b) fractionating the reaction product into a top fraction containing BTX, a middle fraction containing unconverted donor and potential donor and a bottom residual fraction, (c) removing the BTX and residue fractions as products, (d) selectively hydrogenating the middle fraction and (e) recycling the selectively hydrogenated fraction as hydrogen donor to Stage (a).
Suitable selective hydrogenation catalysts include Groups VIA and/or VIII metal catalysts such as Cr2OJAI203, CoMo/Al2O3, NiMo/Al2O3 and Group IB metal catalysts such as Cu/Al2O3.
If the feedstock has not been demetallised, by careful choice of the support for the catalyst in Stage (a) it is possible to influence the properties of the residue from this stage. It is possible to use a demetallising catalyst support, e.g., wide pore SiOAl2O3 which will give a demetallised residue of low metal content, but an unregenerably catalyst. On the other hand if a regenerable catalyst is desired this can be achieved by using a support which does not remove metallic contaminants from the residue, e.g., a microporous basic alumina.
Demetallised residue can be further treated, e.g., by coking to produce coke and a range of lighter products.
The invention is illustrated with reference to the following Examples.
Example 1.
The first table shows that of the Group VIA and Group VIII promoted catalysts, WOJAI203 has the highest activity in'the oxide form. The catalysts are charged in the ratio 1 to 2 parts of tetralin containing about 9% phenanthrene and heated to 3000C for 15 hours in a stirred autoclave. The products are analysed by GLC and include hydrogenated phenanthrenes, substituted naphthalenes, naphthalene itself, decalin, a variety of light aromatics as well as unconverted reactants.
TABLE 1 Activities and Selectivities of Group VIA Catalysts at 3000C Cr2O3Y MoO3/ W03 / Catalyst Alp03 Al203 Awl 202 CoMo NiMo Atmosphere N2 N2 N2 N2 N2 % Phenanthrene conversion 17.0 12.2 89.6 30.7 32.7 Naphthalene % wt 3.7 8.2 8.5 22.8 13.6 Tetralin loss % wt 3.6 8.0 9.3 22.7 13.5 Example 2.
Hydrogen donation can be catalysed also by sulphided catalysts under hydrogen. Table 2 summarises the results and shows good conversion of phenanthrene over the unpromoted Group VIA catalysts.
TABLE 2 Activity and Selectivity of Sulphided Group VIA Catalysts at 3000C Catalyst Mo/A 1203 W/AI203 NiMo CoMo Atmosphere H2 H2 H2 H2 % Phenanthrene conversion 72.9 85.9 51.0 61.3 Naphthalene 6Xc wt 10.9 4.1 13.8 15.3 Tetralin loss % wt 10.1 7.1 10.0 10.6 Example 3.
Table 3 gives details of the results when an oxidic NiW catalyst is supported on bases of increasing acidity.
TABLE 3 Activity and Selectivity of Oxidic NiW Catalysts on Acidic Supports Catalyst SiO2 /Al293 F-SiO2 /Al2O3 Y-Zeolite Atmosphere N2 N2 N2 % Phenanthene conversion 62.4 87.1 84.8 Naphthalene 7E wt 11.0 12.8 12.4 Tetralin loss % wt 16.1 20.9 41.1 The conversion of phenanthrene is high and hydrogen donation is the main reaction. However it can be seen that more tetralin is lost than naphthalene formed. This occurs because tetralin is cracked to BTX over these acidic supports.
The products of reaction for one support F-SiO2Al2O3 are shown in detail in Table 4.
TABLE 4 Products from Phenanthrene Conversion on F-SiO2/Al2O3 Catalysts
Catalyst NiW/F-SiO2/Al2O3 W/F-SiO2/Al2Oa Feed Phenanthrene % wt 8.5 8.5 Products Benzene 5.9 3.5 Toluene 1.6 0.8 Xylenes 0.6 0.9 Butyl benzenes - 1.6 Methyl naphthalene-s 0.4 0.3 Subset naphthalenes 1.9 1.9 Trmsdecalin 5.9 3.6 Cis-decalin 1.6 1.8 Tetralin 63.1 70.7 Naphthalene 12.8 9.5 Butyl-di-hydro-naphthalene 1.6 1.0 9 ::10-di-hydro-phenanthrene 1.0 1.3 Teflahydro-phenanthrene 1.7 1.8 Octhydrophenanthrene 0.8 1.2 Phenanthrene 1.1 1.0 In both cases about 7.5% phenanthrene has been converted partly to various hydrogenated derivatives (3.5 to 4.5% wt) and partly to naphthalene derivatives formed by cracking the hydrogenated products (3.0 to 3.5% wt). Large amounts of tetralin have been removed, 30 to 35%, part to decalin (5 to 7%) part to naphthalene by hydrogen transfer (10 to 13% and part to light aromatics (7 to 8%).
The potential hydrogen donor capacity of the system is made up of tetralin, decalin and naphthalenes which in principle can be rehydrogenated to donors in a separate step. The sum of these components is 87% and 89%, very close to the original amount of tetralin present allowing for dilution by light products. Thus the net reaction in this example is the conversion of phenanthrene partly to hydrogenated derivatives and partly to BTX. The yield of aromatics is about 50% on phenanthrene consumed.

Claims (12)

WHAT WE CLAIM IS:
1. A process for the hydrogenation of a petroleum fraction containing at least 25% by wt of material boiling above 350"C which process comprises contacting the fraction at elevated temperature and pressure with a hydrogen donor and a catalyst comprising from 525% by wt of a metal of Group VIA of the Periodic Table.
2. A process according to Claim 1 wherein the petroleum fraction contains at least 25% by wt of material boiling above 5500C.
3. A process according to either of the preceding claims wherein the catalyst is promoted by the addition of 1--10% by wt of an Iron Group metal.
4. A process according to any of the preceding claims wherein the hydrogen donor is a partially hydrogenated polycyclic aromatic compound or a naphthene.
5. A process according to any of the preceding claims wherein the hydrogen donor is present in amount 20:1 to 1:1 by wt of the feedstock.
6. A process according to Claim I wherein hydrogenation is effected under a temperature in the range 1000--4000C, a pressure in the range 1--100 bars (ga) and a space velocity in the range 0.1-10 v/v/hr.
7. A process according to Claim 6 wherein hydrogenation is effected under a temperature in the range 2500--350"C, a pressure in the range 1-20 bars (ga) and a space velocity in the range 0.5-2 v/v/hr.
8. A process according to any of the preceding claims wherein the catalyst is supported on a refractory acidic material and cracking is effected in addition to hydrogenation.
9. A process according to Claim 8 wherein the refractory acidic support is silica-alumina, a zeolite or halogenated alumina.
10. A process for the production of benzene, toluene and xylene from a petroleum fraction containing at least 25% by wt of material boiling above 350"C which process comprises (a) hydrogenating and cracking the feedstock by a process according to either Claims 8 or 9, (b) fractionating the reaction product into a top fraction containing BTX, a middle fraction containing unconverted donor and potential donor and a bottom residual fraction, (c) removing the BTX and residue fractions as products, (d) selectively hydrogenating the middle fraction, and (e) recycling the selectively hydrogenated fraction as hydrogen donor to Stage (a).
11. A process according to Claim 1 as hereinbefore described with reference to the Examples.
12. Products whenever prepared by a process according to any of the preceding claims.
GB5207476A 1977-12-13 1977-12-13 Hydrogenation process Expired GB1563357A (en)

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Application Number Priority Date Filing Date Title
GB5207476A GB1563357A (en) 1977-12-13 1977-12-13 Hydrogenation process

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Application Number Priority Date Filing Date Title
GB5207476A GB1563357A (en) 1977-12-13 1977-12-13 Hydrogenation process

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Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US7157401B2 (en) 2002-10-17 2007-01-02 Carnegie Mellon University Catalyst for the treatment of organic compounds
US7387712B2 (en) 2002-10-17 2008-06-17 Carnegie Mellon University Catalytic process for the treatment of organic compounds
US8039652B2 (en) 2004-06-15 2011-10-18 Carnegie Mellon University Methods for producing biodiesel

Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US7157401B2 (en) 2002-10-17 2007-01-02 Carnegie Mellon University Catalyst for the treatment of organic compounds
US7387712B2 (en) 2002-10-17 2008-06-17 Carnegie Mellon University Catalytic process for the treatment of organic compounds
US7625832B2 (en) 2002-10-17 2009-12-01 Carnegie Mellon University Catalyst for the treatment of organic compounds
US8039652B2 (en) 2004-06-15 2011-10-18 Carnegie Mellon University Methods for producing biodiesel

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Legal Events

Date Code Title Description
PS Patent sealed
PCNP Patent ceased through non-payment of renewal fee
732 Registration of transactions, instruments or events in the register (sect. 32/1977)