EP1151060A1 - Production de distillats a faible teneur en soufre et en aromatiques - Google Patents

Production de distillats a faible teneur en soufre et en aromatiques

Info

Publication number
EP1151060A1
EP1151060A1 EP99966004A EP99966004A EP1151060A1 EP 1151060 A1 EP1151060 A1 EP 1151060A1 EP 99966004 A EP99966004 A EP 99966004A EP 99966004 A EP99966004 A EP 99966004A EP 1151060 A1 EP1151060 A1 EP 1151060A1
Authority
EP
European Patent Office
Prior art keywords
liquid
reaction
stream
reaction stage
stage
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.)
Withdrawn
Application number
EP99966004A
Other languages
German (de)
English (en)
Other versions
EP1151060A4 (fr
Inventor
Edward Stanley Ellis
Henry Jung
William Ernest Lewis
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.)
ExxonMobil Technology and Engineering Co
Original Assignee
ExxonMobil Research and Engineering Co
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 ExxonMobil Research and Engineering Co filed Critical ExxonMobil Research and Engineering Co
Publication of EP1151060A1 publication Critical patent/EP1151060A1/fr
Publication of EP1151060A4 publication Critical patent/EP1151060A4/fr
Withdrawn legal-status Critical Current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
    • 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
    • C10G65/04—Treatment of hydrocarbon oils by two or more hydrotreatment processes only plural serial stages only including only refining steps
    • C10G65/08—Treatment of hydrocarbon oils by two or more hydrotreatment processes only plural serial stages only including only refining steps at least one step being a hydrogenation of the aromatic hydrocarbons

Definitions

  • the present invention relates to a process for hydroprocessing a hydrotreated liquid distillate stream to produce a stream exceptionally low in sulfur as well as aromatics.
  • a hydrotreated distillate stream is further hydrotreated in a co-current reaction zone wherein the reaction product is passed to a separation drum wherein a vapor product is collected overhead and a liquid product is passed to an aromatics saturation zone countercurrent to the flow of hydrogen treat gas.
  • Hydrotreating or in the case of sulfur removal, hydrodesulfurization, is well known in the art and usually requires treating the petroleum streams with hydrogen in the presence of a supported catalyst at hydrotreating conditions.
  • the catalyst is typically comprised of a Group NI metal with one or more Group VIII metals as promoters on a refractory support.
  • Hydrotreating catalysts which are particularly suitable for hydrodesulfurization and hydrodenitrogenation generally contain molybdenum or tungsten on alumina promoted with a metal such as cobalt, nickel, iron, or a combination thereof.
  • Cobalt promoted molybdenum on alumina and nickel promoted molybdenum on alumina catalysts are most widely used when the limiting specifications are hydrodesulfurization. while nickel promoted molybdenum on alumina catalysts are the most widely used for hydrodenitrogenation and partial aromatic saturation.
  • One such configuration is a countercurrent design wherein the feedstock flows downward through successive catalyst beds counter to upflowing treat gas, which is typically a hydrogen containing treat-gas.
  • upflowing treat gas typically a hydrogen containing treat-gas.
  • the downstream catalyst beds, relative to the flow of feed can contain high performance, but otherwise more sulfur sensitive catalysts because the upflowing treat gas carries away heteroatom components such as H 2 S and ⁇ H 3 that are deleterious to the sulfur and nitrogen sensitive catalysts.
  • While such countercurrent reactors have commercial potential, they never-the-less are susceptible to flooding. That is, where upflowing treat gas and gaseous products impede the downward flow of feed. Such flooding tendency is increased with increases in treat gas rate.
  • Two types of process schemes are commonly employed to achieve substantial hydrodesulfurization (HDS)/ aromatics saturation (ASAT) of distillate fuels and both are operated at relatively high pressures.
  • One is a single stage process using Ni Mo or Ni/W sulfide catalysts operating at pressures in excess of 800 psig. To achieve high levels of saturation pressures in excess of 2,000 psig are required.
  • the other is a two stage process in which the feed is first processed over Co/Mo, Ni/Mo or Ni/W sulfide catalyst at moderate pressure to reduce heteroatom levels while little aromatics saturation is observed. After the first stage the product is stripped to remove H 2 S, NH 3 and light hydrocarbons. The first stage product is then reacted over a Group VIII metal hydrogenation catalyst at elevated pressure to achieve aromatics saturation.
  • the two stage processes are typically operated between 600 and 1,500 psig.
  • a two stage process for hydroprocessing a hydrotreated distillate feedstock which process comprises:
  • the liquid phase stream, before it passes through said second reaction stage is contacted with a vapor to strip dissolved gases from the liquid phase.
  • the figure hereof shows multiple reaction vessels of the present invention showing separation of the liquid phase product from the vapor phase product and further processing of the liquid phase product stream in an aromatics saturation stage.
  • Feedstocks suitable for being treated by the present invention are those petroleum based feedstocks boiling in the distillate range and above and which have previously been hydrotreated to reduce the sulfur and nitrogen levels.
  • Typical sulfur levels in such hydrotreated distillates are in the range of less than about 3,000 wppm. more preferably to less than about 1 ,000 wppm, most preferably to less than about 500 wppm sulfur, ideally to less than about 350 wppm.
  • Non-limiting examples of such feeds include diesel fuels, jet fuels, heating oils, and lubes.
  • Such feeds typically have a boiling range from about 150 to about 600°C, preferably from about 175 to about 400°C. It is highly desirable for the refiner to upgrade these types of feedstocks by removing as much of the sulfur as possible, as well as to saturate aromatic compounds.
  • the process of the present invention can be better understood by a description of a preferred embodiment illustrated by Figure 1 hereof.
  • the current invention offers an improvement over the prior art by using only once through hydrogen treat gas.
  • the first reaction stage Rl is a hydrotreating stage to further reduce the level of sulfur and nitrogen
  • the second reaction stage R2 is an aromatics saturation stage.
  • the hydrogen reacts with the impurities to convert them to H 2 S, NH 3 and water vapor, which are removed as part of the vapor effluent, and it also saturates olefins and aromatics.
  • Miscellaneous reaction vessel internals, valves, pumps, thermocouples, and heat transfer devices etc. are not shown for simplicity.
  • FIG. 1 shows reaction vessel Rl which contains reaction zones 10a and 10b, each of which is comprised of a bed of hydrotreating catalyst, although only a single or more than two reaction zones can be employed. It is preferred that the catalyst be in the reactor as a fixed bed, although other types of catalyst arrangements can be used, such as slurry or ebullating beds. Downstream of each reaction zone is a non-reaction zone 12 a and 12b. The non-reaction zone is typically void of catalyst, that is, it will be an empty section in the vessel with respect to catalyst. Although not shown, there may also be provided a liquid distribution means upstream of each reaction stage.
  • liquid distribution means is believed not to limit the practice of the present invention, but a tray arrangement is preferred, such as sieve trays, bubble cap trays, or trays with spray nozzles, chimneys, tubes, etc.
  • a vapor-liquid mixing device (not shown) can also be employed in non-reaction zone 12a for the purpose of introducing a quench fluid (liquid or vapor) for temperature control.
  • the feedstream is fed to reaction vessel Rl via line 10 along with a hydrogen-containing treat gas via line 12.
  • the hydrogen-containing treat gas is cascaded from reaction stage R2.
  • Make up hydrogen-containing treat gas can also be added via line 14. It is preferred that the rate of intoduction of treat gas be less than or equal to 3 times the chemical hydrogen consumption of the reactions in both stages, more preferably less than about 2 times, and most preferably less than about 1.5 times.
  • the feedstream and hydrogen-containing treat gas pass, cocurrently, through the one or more reaction zones of reaction vessel Rl , which represents the first reaction stage wherein the feedstream is further hydrotreated to remove substantially all of the heteroatoms from the feedstream. It is preferred that the first reaction stage contain a Co-Mo, or Ni- Mo, on refractory support catalyst, and a downstream reaction stage contain a Ni-Mo on refractory support catalyst.
  • hydrotreating refers to processes wherein a hydrogen-containing treat gas is used in the presence of a suitable catalyst which is primarily active for the removal of heteroatoms, such as sulfur, and nitrogen, and for some hydrogenation of aromatics.
  • Suitable hydrotreating catalysts for use in the present invention are any conventional hydrotreating catalyst and includes those which are comprised of at least one Group VIII metal, preferably Fe, Co and Ni, more preferably Co and/or Ni, and most preferably Co; and at least one Group VI metal, preferably Mo and W, more preferably Mo, on a high surface area support material, preferably alumina.
  • hydrotreating catalyst supports include zeolites, amorphous silica-alumina, and titania-alumina Noble metal catalysts can also be employed, preferably when the noble metal is selected from Pd and Pt. It is within the scope of the present invention that more than one type of hydrotreating catalyst be used in the same reaction vessel.
  • the Group VIII metal is typically present in an amount ranging from about 2 to 20 wt.%, preferably from about 4 to 12%.
  • the Group VI metal will typically be present in an amount ranging from about 5 to 50 wt.%, preferably from about 10 to 40 wt.%, and more preferably from about 20 to 30 wt.%. All metals weight percents are on support.
  • on support we mean that the percents are based on the weight of the support. For example, if the support were to weigh 100 g. then 20 wt.% Group VIII metal would mean that 20 g. of Group VIII metal was on the support.
  • Typical hydrotreating temperatures range from about 100°C to about 400°C with pressures from about 50 psig to about 3,000 psig, preferably from about 50 psig to about 2,500 psig.
  • a combined liquid phase and vapor phase product stream exit reaction vessel Rl via line 16 and into separation zone S wherein a liquid phase product stream is separated from a vapor phase product stream.
  • the liquid phase product stream will typically be one that has components boiling in the range from about 150°C to about 650°C, but will not have a boiling range greater than the feedstream.
  • the vapor phase product stream is collected overhead via line 20.
  • the liquid reaction product from separation zone S is passed to reaction vessel R2 via line 20 and is passed downwardly through the reaction zones 22a and 22b of reaction stage R2.
  • said liquid reaction product stream Prior to being passed downwardly through reaction stage R2, said liquid reaction product stream can first be contacted in a stripping zone to remove entrapped vapor components from the liquid stream.
  • the liquid product stream flows through the stripping zone, it is contacted by upflowing hydrogen-containing treat gas under conditions effective for transferring at least a portion of the feed impurities in the vapor into the liquid.
  • the contacting means comprises any known vapor- liquid contacting means, such as rashig rings, bed saddles, wire mesh, ribbon, open honeycomb, gas-liquid contacting trays, such as bubble cap trays and other devices, etc.
  • Fresh hydrogen-containing treat gas is introduced into reaction stage R2 via line 24 and is is passed in an upward direction counter to the flow of liquid reaction product.
  • the introduction of clean treat gas (gas substantially free of H 2 S and NH 3 ) allows reaction stage R2 to be operated more efficiently owing to a reduction in the activity suppression effects on the catalyst exerted by H 2 S and NH 3 and an increase in H 2 partial pressure.
  • This type of two stage operation is particularly attractive for very deep removal of sulfur and nitrogen or when a more sensitive catalyst (i.e., hydrocracking, aromatic saturation, etc) is used in the second reactor.
  • Another advantage of the present invention is that the treat gas rate is relatively low compared with more conventional processes. The use of relatively low treat gas rates is primarily due to the use of previously hydrotreated distillate feedstocks. Further efficiencies are gained by not requiring recycle of treat gas.
  • the liquid/vapor separation step (S) may be a simple flash or may involve the addition of stripping steam or gas to improve the removal of H 2 S and NH 3 .
  • the liquid stream and treat gas are passed countercurrent to each other through one or more catalyst beds, or reaction zones, 22a and 22b.
  • the reulting liquid product stream exits reaction stage R2 via line 26, and a hydrogen- containing vapor product stream exits reaction stage R2 and is cascaded to reaction stage Rl .
  • Reaction stage R2 also contains non reaction zones 23a and 23b following each reaction zones.
  • the catalyst in this second reaction stage is an aromatic saturation catalyst.
  • lines 30 and 32 can carry kerosene which can be used as a quench fluid.
  • a unsaturated feedstock can also be introduced into the first reaction stage via line 28. The degree of unsaturation can be up to about 50 wt.%.
  • reaction stages used in the practice of the present invention are operated at suitable temperatures and pressures for the desired reaction.
  • typical hydroprocessing temperatures will range from about 40°C to about 450°C at pressures from about 50 psig to about 3,000 psig, preferably 50 to 2,500 psig.
  • hydroprocessing and in the context of the invention the terms “hydrogen” and “hydrogen-containing treat gas " are synonymous and may be either pure hydrogen or a hydrogen-containing treat gas which is a treat gas stream containing hydrogen in an amount at least sufficient for the intended reaction, plus other gas or gasses (e.g., nitrogen and light hydrocarbons such as methane) which will not adversely interfere with or affect either the reactions or the products.
  • gas or gasses e.g., nitrogen and light hydrocarbons such as methane
  • Impurities, such as H2S and NH3 are undesirable and, if present in significant amounts, will normally be removed from the treat gas. before it is fed into the reactor.
  • the treat gas stream introduced into a reaction stage will preferably contain at least about 50 vol. %. more preferably at least about 75 vol. % hydrogen, and most preferably at least 95 vol.
  • Non-limiting examples of aromatic hydrogenation catalysts include nickel, cobalt-molybdenum, nickel-molybdenum, and nickel-tungsten.
  • Noble metal containing catalysts can also be used.
  • Non-limiting examples of noble metal catalysts include those based on platinum and/or palladium, which is preferably supported on a suitable support material, typically a refractory oxide material such as alumina, silica, alumina-silica, kieselguhr, diatomaceous earth, magnesia, and zirconia. Zeolitic supports can also be used. Such catalysts are typically susceptible to sulfur and nitrogen inhibition or poisoning.
  • the aromatic saturation stage is preferably operated at a temperature from about 40°C to about 400°C, more preferably from about 200°C to about 350°C, at a pressure from about 100 psig to about 3,000 psig, preferably from about 200 psig to about 1 ,200 psig, and at a liquid hourly space velocity (LHSV) of from about 0.3 V/V/Hr. to about 10 V/V/Hr, preferably from about 1 to 5 V/V/Hr.
  • LHSV liquid hourly space velocity
  • the liquid phase in the reaction vessels used in the present invention will typically consist primarily of the higher boiling point components of the feed.
  • the vapor phase will typically be a mixture of hydrogen-containing treat gas, heteroatom impurities like H 2 S and NH 3 , and vaporized lower-boiling components in the fresh feed, as well as light products of hydroprocessing reactions. If the vapor phase effluent still requires further hydroprocessing, it can be passed to a vapor phase reaction stage containing additional hydroprocessing catalyst and subjected to suitable hydroprocessing conditions for further reaction. Alternatively, the hydrocarbons in the vapor phase products can be condensed via cooling of the vapors, with the resulting condensate liquid being recycled to either of the reaction stages, if necessary. It is also within the scope of the present invention that a feedstock which already contains adequately low levels of heteroatoms be fed directly into the reaction stage for aromatic saturation and/or cracking

Landscapes

  • 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)
  • Catalysts (AREA)

Abstract

L'invention concerne un procédé d'hydrotraitement d'un distillat liquide hydrotraité, consistant à introduire le flux d'alimentation dans une cuve (R1) de réaction via le conduit (10), ainsi qu'un gaz de traitement renfermant de l'hydrogène via le conduit (12). Le flux produit à phases liquide et vapeur combinées sort de la cuve (R1) de réaction via le conduit (16). Le flux produit en phase vapeur est collecté en tête de distillation via le conduit (20). Le produit de réaction liquide traverse la cuve (R2) de réaction via le conduit (20) puis, s'écoule vers le bas, à travers les zones de réaction (22a) et (22b) ou la zone de réaction (R2).
EP19990966004 1998-12-08 1999-12-07 Production de distillats a faible teneur en soufre et en aromatiques Withdrawn EP1151060A4 (fr)

Applications Claiming Priority (3)

Application Number Priority Date Filing Date Title
US11134598P 1998-12-08 1998-12-08
US111345P 1998-12-08
PCT/US1999/028790 WO2000034416A1 (fr) 1998-12-08 1999-12-07 Production de distillats a faible teneur en soufre et en aromatiques

Publications (2)

Publication Number Publication Date
EP1151060A1 true EP1151060A1 (fr) 2001-11-07
EP1151060A4 EP1151060A4 (fr) 2010-08-18

Family

ID=22337985

Family Applications (1)

Application Number Title Priority Date Filing Date
EP19990966004 Withdrawn EP1151060A4 (fr) 1998-12-08 1999-12-07 Production de distillats a faible teneur en soufre et en aromatiques

Country Status (5)

Country Link
EP (1) EP1151060A4 (fr)
JP (1) JP4785250B2 (fr)
AU (1) AU756565B2 (fr)
NO (1) NO20012800D0 (fr)
WO (1) WO2000034416A1 (fr)

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US7435335B1 (en) 1998-12-08 2008-10-14 Exxonmobil Research And Engineering Company Production of low sulfur distillates
US6328879B1 (en) * 1999-07-26 2001-12-11 Uop Llc Simultaneous hydroprocesssing of two feedstocks
AU2001251657B2 (en) * 2000-04-20 2006-05-18 Exxonmobil Research And Engineering Company Production of low sulfur distillates
MXPA03002517A (es) * 2000-09-26 2003-06-19 Uop Llc Proceso de hidrofisuracion.
US7247235B2 (en) 2003-05-30 2007-07-24 Abb Lummus Global Inc, Hydrogenation of middle distillate using a counter-current reactor
CN1313574C (zh) * 2003-05-31 2007-05-02 中国石油化工股份有限公司 一种柴油深度脱硫和脱芳烃工艺
EP1663467B1 (fr) 2003-08-18 2010-02-24 Shell Internationale Researchmaatschappij B.V. Dispositif de distribution
US7906013B2 (en) 2006-12-29 2011-03-15 Uop Llc Hydrocarbon conversion process
US7794585B2 (en) * 2007-10-15 2010-09-14 Uop Llc Hydrocarbon conversion process
US7790020B2 (en) * 2007-10-15 2010-09-07 Uop Llc Hydrocarbon conversion process to improve cetane number
US7799208B2 (en) * 2007-10-15 2010-09-21 Uop Llc Hydrocracking process
US7794588B2 (en) * 2007-10-15 2010-09-14 Uop Llc Hydrocarbon conversion process to decrease polyaromatics
US8999141B2 (en) 2008-06-30 2015-04-07 Uop Llc Three-phase hydroprocessing without a recycle gas compressor
US9279087B2 (en) 2008-06-30 2016-03-08 Uop Llc Multi-staged hydroprocessing process and system
US8008534B2 (en) 2008-06-30 2011-08-30 Uop Llc Liquid phase hydroprocessing with temperature management
US8518241B2 (en) 2009-06-30 2013-08-27 Uop Llc Method for multi-staged hydroprocessing
US8221706B2 (en) 2009-06-30 2012-07-17 Uop Llc Apparatus for multi-staged hydroprocessing
CN102041074B (zh) * 2009-10-16 2014-03-05 中国石油化工股份有限公司 深拔蒽油的加氢方法
CN102041078B (zh) * 2009-10-16 2014-03-05 中国石油化工股份有限公司 一种深拔蒽油加氢生产轻质燃料油的方法
CN102041075B (zh) * 2009-10-16 2014-03-05 中国石油化工股份有限公司 一种蒽油加氢方法
CN102041077B (zh) * 2009-10-16 2014-01-01 中国石油化工股份有限公司 一种深拔蒽油的加氢方法
CN102041079B (zh) * 2009-10-16 2014-03-05 中国石油化工股份有限公司 一种深拔蒽油的加氢转化方法
CN102041073B (zh) * 2009-10-16 2013-12-04 中国石油化工股份有限公司 蒽油的加氢裂化方法
CN101712887A (zh) * 2009-10-18 2010-05-26 何巨堂 一种烃氢化方法
GB201308244D0 (en) 2013-05-08 2013-06-12 Croda Int Plc Soil treatment
KR102304149B1 (ko) * 2013-05-20 2021-09-23 쉘 인터내셔날 리써취 마트샤피지 비.브이. 베이스 금속 촉매를 사용한 2단계 디젤 방향족 포화 공정
RU2671978C2 (ru) * 2013-05-20 2018-11-08 Шелл Интернэшнл Рисерч Маатсхаппий Б.В. Двухступенчатый способ насыщения ароматических соединений дизельного топлива, использующий промежуточное отпаривание, и катализатор на основе неблагородного металла
CN103695030B (zh) * 2013-12-18 2015-10-21 宁波金远东工业科技有限公司 煤焦油中的蒽油加氢制柴油的方法

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EP0553920A1 (fr) * 1992-01-24 1993-08-04 Shell Internationale Researchmaatschappij B.V. Procédé d'hydrotraitement

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US3846278A (en) * 1971-09-02 1974-11-05 Lummus Co Production of jet fuel
EP0553920A1 (fr) * 1992-01-24 1993-08-04 Shell Internationale Researchmaatschappij B.V. Procédé d'hydrotraitement

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See also references of WO0034416A1 *

Also Published As

Publication number Publication date
AU756565B2 (en) 2003-01-16
NO20012800L (no) 2001-06-07
JP2002531682A (ja) 2002-09-24
AU2165800A (en) 2000-06-26
WO2000034416A1 (fr) 2000-06-15
NO20012800D0 (no) 2001-06-07
EP1151060A4 (fr) 2010-08-18
JP4785250B2 (ja) 2011-10-05

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