EP4196557A1 - Procédé et installation de production d'essence à partir d'une charge contenant du goudron - Google Patents

Procédé et installation de production d'essence à partir d'une charge contenant du goudron

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Publication number
EP4196557A1
EP4196557A1 EP21763291.8A EP21763291A EP4196557A1 EP 4196557 A1 EP4196557 A1 EP 4196557A1 EP 21763291 A EP21763291 A EP 21763291A EP 4196557 A1 EP4196557 A1 EP 4196557A1
Authority
EP
European Patent Office
Prior art keywords
stream
unit
hydrogen
producing
process according
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.)
Pending
Application number
EP21763291.8A
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German (de)
English (en)
Inventor
Erik BEK-PEDERSEN
Søren Selde ENEVOLDSEN
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.)
Topsoe AS
Original Assignee
Haldor Topsoe AS
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Filing date
Publication date
Application filed by Haldor Topsoe AS filed Critical Haldor Topsoe AS
Publication of EP4196557A1 publication Critical patent/EP4196557A1/fr
Pending legal-status Critical Current

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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
    • C10G65/046—Treatment of hydrocarbon oils by two or more hydrotreatment processes only plural serial stages only including only refining steps at least one step being an aromatisation step
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
    • C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
    • C01B3/32—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air
    • C01B3/34—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents
    • 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
    • C10G63/00—Treatment of naphtha by at least one reforming process and at least one other conversion process
    • C10G63/02—Treatment of naphtha by at least one reforming process and at least one other conversion process plural serial stages only
    • C10G63/04—Treatment of naphtha by at least one reforming process and at least one other conversion process plural serial stages only including at least one cracking step
    • 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
    • C10G69/00—Treatment of hydrocarbon oils by at least one hydrotreatment process and at least one other conversion process
    • C10G69/02—Treatment of hydrocarbon oils by at least one hydrotreatment process and at least one other conversion process plural serial stages only
    • C10G69/08—Treatment of hydrocarbon oils by at least one hydrotreatment process and at least one other conversion process plural serial stages only including at least one step of reforming naphtha
    • C10G69/10—Treatment of hydrocarbon oils by at least one hydrotreatment process and at least one other conversion process plural serial stages only including at least one step of reforming naphtha hydrocracking of higher boiling fractions into naphtha and reforming the naphtha obtained
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/02—Processes for making hydrogen or synthesis gas
    • C01B2203/0205—Processes for making hydrogen or synthesis gas containing a reforming step
    • C01B2203/0227—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step
    • C01B2203/0233—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step the reforming step being a steam reforming step
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/02—Processes for making hydrogen or synthesis gas
    • C01B2203/0205—Processes for making hydrogen or synthesis gas containing a reforming step
    • C01B2203/0227—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step
    • C01B2203/0244—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step the reforming step being an autothermal reforming step, e.g. secondary reforming processes
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/04—Integrated processes for the production of hydrogen or synthesis gas containing a purification step for the hydrogen or the synthesis gas
    • C01B2203/042—Purification by adsorption on solids
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/06—Integration with other chemical processes
    • C01B2203/063—Refinery processes
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/06—Integration with other chemical processes
    • C01B2203/063—Refinery processes
    • C01B2203/065—Refinery processes using hydrotreating, e.g. hydrogenation, hydrodesulfurisation
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/08—Methods of heating or cooling
    • C01B2203/0805—Methods of heating the process for making hydrogen or synthesis gas
    • C01B2203/0811—Methods of heating the process for making hydrogen or synthesis gas by combustion of fuel
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/08—Methods of heating or cooling
    • C01B2203/0805—Methods of heating the process for making hydrogen or synthesis gas
    • C01B2203/0811—Methods of heating the process for making hydrogen or synthesis gas by combustion of fuel
    • C01B2203/0816—Heating by flames
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/08—Methods of heating or cooling
    • C01B2203/0805—Methods of heating the process for making hydrogen or synthesis gas
    • C01B2203/085—Methods of heating the process for making hydrogen or synthesis gas by electric heating
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P30/00—Technologies relating to oil refining and petrochemical industry
    • Y02P30/20—Technologies relating to oil refining and petrochemical industry using bio-feedstock

Definitions

  • the present invention relates to a process and plant for producing a high-quality gasoline from a tar-containing feedstock, the process and plant comprising one or more hydroprocessing stages which include hydrotreating and hydrocracking for producing diesel and naphtha, and subsequent aromatization of the naphtha, thereby also producing a light hydrocarbon gas as a liquid petroleum gas (LPG),from which a hydrogen stream is produced and which may be used in the process.
  • LPG liquid petroleum gas
  • the quality of gasoline is highly dependent on the resistance to engine knocking due to compression ignition of the fuel in engines running on the gasoline. This quality is measured by the so-called octane number, originating from isooctane being considered the ideal gasoline hydrocarbon.
  • octane number originating from isooctane being considered the ideal gasoline hydrocarbon.
  • a pure iso-octane defines the gasoline as having the octane number 100, while a pure n-heptane defines the octane number 0. It would be desirable to produce a gasoline having a research octane number (RON) of at least 85, such as 90 or higher.
  • gasoline is a complex hydrocarbon mixture and e.g. aromatics contribute to higher knock-resistance, while saturated alkanes, especially when having a linear structure, have a higher propensity to knocking. Therefore, naphtha hydrocarbon mixtures are less valuable if the aromatic content is very low.
  • Naphtha having insufficient octane number may be upgraded by catalytic reforming process, which typically involves alkylation of aromatics to increase the octane number.
  • Applicant’s US 9,752,080 discloses the use of LPG from a downstream Fischer- Tropsch (FT) process as feed to a steam reforming process for producing synthesis gas required in the FT-process.
  • FT Fischer- Tropsch
  • WO 2015/075315 A1 discloses the use of LPG or naphtha in a hydrogen producing plant which is integrated in a process for producing hydrocarbons from a renewable feedstock.
  • US 3,871,993 describes a process for converting virgin naphtha to a high-octane liquid gasoline product and LPG without hydrogen consumption by increasing the aromatics content of the naphtha via the use of zeolite such as ZSM-5 which may be modified with metals.
  • WO 2016/054316 A1 discloses a process or plant for producing aromatic compounds, particularly a product rich in BTX (benzene, toluene, xylene) from gas condensates (wide boiling range condensates) having a low content of aromatics e.g. up to 40 wt% or up to 15 wt% (Table 1).
  • the process includes the use of a hydroprocessing reactor, an aromatization reactor and a hydrogen extraction unit such as pressure swing adsorption unit (PSA unit). From the PSA unit, a LPG stream is withdrawn.
  • PSA unit pressure swing adsorption unit
  • Applicant’s co-pending European patent application EP 20162995.3 describes the production of renewable hydrocarbon products such as renewable naphtha in a process including production of hydrogen in a hydrogen producing unit which may use such renewable naphtha as part of the hydrocarbon feedstock.
  • the prior art is silent about a process or plant for converting a feedstock originating from a tar-containing feedstock into a hydrocarbon product boiling in the gasoline boiling range by hydrotreating and hydrocracking, and at the same time producing a light hydrocarbon gas as LPG for use in the production of hydrogen which may be used in the process or plant.
  • a process for producing a hydrocarbon product boiling in the gasoline boiling range comprising the steps of: i) converting a tar-containing feedstock such as coke oven tar (COT) by one or more hydroprocessing stages into a hydrocarbon product boiling at above 30°C, including a naphtha stream; wherein said one or more hydroprocessing stages comprise a hydrotreating and hydrocracking step, followed by a separation stage for thereby producing said naphtha stream; ii) upgrading said naphtha stream by passing said naphtha stream through an aromatization stage comprising contacting the naphtha stream with a catalyst, preferably a catalyst comprising an aluminosilicate zeolite, thereby producing said hydrocarbon product boiling in the gasoline boiling range and a separate light hydrocarbon gas stream as a liquid petroleum gas (LPG) stream; iii) passing at least a portion of said LPG stream to a hydrogen producing unit for producing a hydrogen stream;
  • a tar-containing feedstock such as coke oven
  • the hydrocarbon product boiling at above 30°C comprises said naphtha, diesel and lube base stock (base oil for lubes).
  • stage and “step” may be used interchangeably.
  • hydrocarbon product boiling in the gasoline boiling range means boiling in the range 30-210°C.
  • naphtha means a hydrocarbon product boiling in the range 30-160°C.
  • diesel means a hydrocarbon product boiling in the range 120-360°C, for instance 160-360°C.
  • lube base stock means a hydrocarbon product boiling at above 390°C.
  • boiling in a given range shall be understood as a hydrocarbon mixture of which at least 80 wt% boils in the stated range.
  • light hydrocarbon gas means a gas mixture comprising C1-C4 gases, in particular methane, ethane, propane, butane; the light hydrocarbon gas may also comprise i-C3, i-C4 and unsaturated C3-C4 olefins.
  • a particular light hydrocarbon gas is LPG as defined below.
  • LPG liquid/liquified petroleum gas, which is a gas mixture mainly comprising propane and butane, i.e. C3-C4; LPG may also comprise i-C3, i-C4 and unsaturated C3-C4 such as C4-olefins.
  • the separate light hydrocarbon gas stream is a liquid petroleum gas (LPG) stream.
  • LPG liquid petroleum gas
  • said hydrocarbon product boiling in the gasoline boiling range has at least 20 wt% aromatics in C5+, such as 20-50 wt% aromatics in C5+, and an octane number (Research Octane Number, RON) of at least 85, such as 90 or 95.
  • octane number Research Octane Number, RON
  • high quality gasoline is a hydrocarbon product in accordance with these specifications.
  • RON is measured according to ASTM D-2699.
  • step i) comprises a hydrotreating and hydrocracking step for thereby enabling deep sulfur and nitrogen removal, aromatic saturation and optional hydrocarbon product property improvement, followed by a separation stage for thereby producing said naphtha stream.
  • a hydrotreating and hydrocracking step for thereby enabling deep sulfur and nitrogen removal, aromatic saturation and optional hydrocarbon product property improvement, followed by a separation stage for thereby producing said naphtha stream.
  • an LPG stream may also be produced, as well as other hydrocarbon products such as diesel.
  • a tar-containing feedstock is particularly high in aromatics.
  • coke oven tar may have at least 25 wt% aromatics, such as up to 50 wt% or 60 wt% aromatics.
  • the present invention counter-intuitively, purposely subjects this feedstock to hydrotreatment and hydrocracking steps which inevitably reduce the content of aromatic compounds, compounds which according to the invention are necessary for providing a higher RON and thereby high-quality gasoline.
  • the process of the invention thus surprisingly reduces the amount of aromatics and later increases the amount of aromatics in order to obtain high quality gasoline along with a significant amount of light hydrocarbon gas, particularly LPG.
  • the material catalytically active in hydrotreating typically comprises an active metal (sulfided base metals such as nickel, cobalt, tungsten and/or molybdenum, but possibly also either elemental noble metals such as platinum and/or palladium) and a refractory support (such as alumina, silica or titania, or combinations thereof).
  • active metal sulfurided base metals such as nickel, cobalt, tungsten and/or molybdenum, but possibly also either elemental noble metals such as platinum and/or palladium
  • a refractory support such as alumina, silica or titania, or combinations thereof.
  • HDT conditions involve a temperature in the interval 250-400°C, a pressure in the interval 30-150 bar, and a liquid hourly space velocity (LHSV) in the interval 0.1-2, optionally together with intermediate cooling by quenching with cold hydrogen, feed or product
  • LHSV liquid hourly space velocity
  • a hydrodewaxing (HDW) stage may also be conducted.
  • the material catalytically active in HDW typically comprises an active metal (either elemental noble metals such as platinum and/or palladium or sulfided base metals such as nickel, cobalt, tungsten and/or molybdenum), an acidic support (typically a molecular sieve showing high shape selectivity, and having a topology such as MOR, FER, MRE, MWW, AEL, TON and MTT) and a refractory support (such as alumina, silica or titania, or combinations thereof).
  • an active metal either elemental noble metals such as platinum and/or palladium or sulfided base metals such as nickel, cobalt, tungsten and/or molybdenum
  • an acidic support typically a molecular sieve showing high shape selectivity, and having a topology such as MOR, FER, MRE, MWW, AEL, TON
  • Isomerization conditions involve a temperature in the interval 250-400°C, a pressure in the interval 20-100 bar, and a liquid hourly space velocity (LHSV) in the interval 0.5-8.
  • LHSV liquid hourly space velocity
  • the material catalytically active in hydrocracking is of similar nature to the material catalytically active in isomerization, and it typically comprises an active metal (either elemental noble metals such as platinum and/or palladium or sulfided base metals such as nickel, cobalt, tungsten and/or molybdenum), an acidic support (typically a molecular sieve showing high cracking activity, and having a topology such as MFI, BEA and FAU) and a refractory support (such as alumina, silica or titania, or combinations thereof).
  • an active metal either elemental noble metals such as platinum and/or palladium or sulfided base metals such as nickel, cobalt, tungsten and/or molybdenum
  • an acidic support typically a molecular sieve showing high cracking activity, and having a topology such as MFI, BEA and FAU
  • a refractory support such as alumina, silica or titania
  • the difference to material catalytically active isomerization is typically the nature of the acidic support, which may be of a different structure (even amorphous silica-alumina) or have a different acidity e.g. due to silica:alumina ratio.
  • HCR conditions involve a temperature in the interval 250-400°C, a pressure in the interval 30-150 bar, and a liquid hourly space velocity (LHSV) in the interval 0.5-8, optionally together with intermediate cooling by quenching with cold hydrogen, feed or product
  • LHSV liquid hourly space velocity
  • the material catalytically active in HDA typically comprises an active metal (typically elemental noble metals such as platinum and/or palladium but possibly also sulfided base metals such as nickel, cobalt, tungsten and/or molybdenum) and a refractory support (such as amorphous silica-alumina, alumina, silica or titania, or combinations thereof).
  • active metal typically elemental noble metals such as platinum and/or palladium but possibly also sulfided base metals such as nickel, cobalt, tungsten and/or molybdenum
  • a refractory support such as amorphous silica-alumina, alumina, silica or titania, or combinations thereof.
  • HDA conditions involve a temperature in the interval 200-350°C, a pressure in the interval 20-100 bar, and a liquid hourly space velocity (LHSV) in the interval 0.5-8.
  • LHSV liquid hourly space velocity
  • Tar is a heavy hydrocarbonaceous liquid, which is often considered an undesirable byproduct from coal processing such as coal gasification, and there are significant costs and efforts associated with the disposal of surplus tar.
  • the present invention generates a high-quality gasoline by processing and upgrading an otherwise not very desirable industrial by-product.
  • coal gasification shall be understood as a process comprising coking processes, which destructively distill the coal feedstock, to produce coke with a high carbon content, a gas phase and a liquid phase, coal tar.
  • Such coal tar is characterized by a high presence of heteroatoms (especially nitrogen, sulfur and oxygen) as well as a high content of aromatics.
  • coal tar and coke oven tar may be used to indicate the source of the tar.
  • tar is typically a product of coal gasification.
  • coal tar and coke oven tar are used interchangeably throughout this application.
  • tar-containing feedstock may also include a product from the pyrolysis of tyres, e.g. waste tyres.
  • the tar-containing feedstock is a product from the pyrolysis of tires and which contains at least 45 wt% aromatics, for instance 50 wt% or higher, e.g. 50-75 wt%, preferably as measured by ASTM D-6591 or ASMT D-6729.
  • Pyrolysis as is well known in the art, means the thermal decomposition of a material, e.g. waste tyres, by exposure to high temperatures such as from 300°C up to 700°C, 800°C or-900°C in an inert atmosphere such as nitrogen.
  • the tar-containing feedstock is a coke oven tar containing at least 25 wt% aromatics, such as at least 30%, or at least 40 wt%, for instance 50 wt% or 60 wt%, preferably as measured by ASTM D-6591 or ASMT D-6729.
  • a significant amount of aromatics is present in the tar-containing feedstock.
  • the naphtha stream obtained as intermediate product is highly naphthenic.
  • this naphtha stream contains, preferably as measured by ASTM D-6729: at least 50 wt% naphthenes, such as at least 60 wt%, or at least 70 wt%, for instance 75 wt% or 80 wt; preferably less than 15 wt% n+i paraffins, for instance less than 12 wt% i-paraffins and less than 3 wt% n-paraffins; preferably less than 1 wt% olefins, for instance less than 0.5 wt% olefins; and for instance also below 10 wt% aromatics, such as 6 wt% or 4-5 wt%.
  • the subsequent aromatization stage of the naphtha stream instead of e.g. simply using it directly as source of hydrogen in a hydrogen producing unit and rather focusing on diesel as the main product, results in a large amount of aromatics thereby increasing the octane number (RON) to at least 85, particularly 90 or higher, from as low as 50-60 in the naphtha stream, while at the same time, a significant amount of light hydrocarbon gas, particularly LPG, is also produced e.g. 30-50 wt% LPG.
  • the gasoline yield (C5+ yield) can also be obtained at desired levels e.g. 40-60 wt%.
  • the need for hydrogen in the process would typically be satisfied by using coke oven gas as hydrogen source or another external source.
  • coke oven gas there is a deficit of hydrogen, so the utilization of the light hydrocarbon gas, particularly LPG, for producing hydrogen in step iii) enables closing the hydrogen balance and even generate surplus hydrogen.
  • the naphtha stream being highly naphthenic, is thus segregated into low hydrogen high-octane aromatic naphtha and LPG with increased hydrogen density i.e. H:C-ratio and which is used for hydrogen production.
  • a high energy efficiency in the process and plant is thereby obtained whilst at the same time a high-quality gasoline product is obtained from the otherwise not very desirable industrial by-product (tar). Diesel produced in the process, and which normally is the desired hydrocarbon product, may also be used as part of the hydrocarbon product pool.
  • a simple and elegant solution to the creation of valuable products on the basis of a tar-containing feedstock is achieved, by enabling among other things a significant improvement, i.e. more than expected increase of the octane number (RON) of the naphtha stream.
  • RON octane number
  • the octane number (RON) of the high-quality gasoline, having at least 20-45 wt% aromatics, is 85 or higher, such as 90 or 95.
  • a significant amount of LPG is formed as an additional valuable product due to the dehydrogenation that happens when aromatics are formed, and which is then converted to hydrogen in a steam reforming process in the hydrogen producing unit.
  • the invention enables a simpler approach than e.g. catalytic reforming of the naphtha, since the aromatization stage can be conducted at milder conditions, with less expensive catalyst and less expensive process equipment. More specifically, there is no need for noble metals or rare earth metals on the catalyst, there is no chlorine, the catalytic reactor can be operated as a fixed-bed reactor operation and thus represents a much simpler solution than conventional catalytic reformers.
  • the process further comprises: iv) passing at least a portion of the hydrogen stream to any of the hydroprocessing stages of step i) and/or the aromatization stage of step ii).
  • the produced hydrogen stream may be used as make-up hydrogen to provide hydrogen during the production of the gasoline, thereby improving the energy efficiency of the overall process and plant.
  • all process and plant means the process and plant used to convert the tar-containing feedstock to the hydrocarbon product boiling in the gasoline boiling range in accordance with above steps i)-iv). It would be understood that this encompasses also any of the below embodiments.
  • the tar-containing feedstock is passed through an acid wash step prior to passing to said step i). This removes impurities in the feedstock which may be detrimental for i.a. downstream catalysts.
  • step i) comprises a conditioning step including the use of one or more guards, e.g. bed guards, for the removal of metals, removal of di-olefins, and removal of bulk sulfur and nitrogen.
  • guards e.g. bed guards
  • the catalyst in step (ii) is incorporated, e.g. supported, in an aluminosilicate zeolite, such as a catalyst incoroporated in a zeolite having a MFI structure, in particular ZSM-5, preferably Zn- ZSM-5, ZnP-ZSM-5, Ni-ZSM-5, or combinations thereof;
  • the temperature is in the range 300-500°C, such as 300-460°C or 300-420°C
  • the pressure is 1-30 bar such as 2-30 bar or 10-30 bar
  • hydrogen i.e. optionally, the aromatization is conducted in the presence of hydrogen.
  • the liquid hourly space velocity (LHSV) is in the interval 1-3, for instance 1.5-2.
  • MFI structure means a structure as assigned and maintained by the International Zeolite Association Structure Commission in the Atlas of Zeolite Framework Types, which is at http:// www.iza-structure.org/databases/ or for instance also as defined in “Atlas of Zeolite Framework Types”, by Ch. Baerlocher, L.B. McCusker and D.H. Olson, Sixth Revised Edition 2007.
  • Zn-ZSM-5 means Zn incorporated in the zeolite ZSM-5, and includes Zn supported on ZSM-5. The same interpretation applies when using ZnP, or Ni.
  • step ii) comprises providing after said aromatization stage an isomerization stage, said aromatization stage producing a raw upgraded naphtha stream which is passed through said isomerization stage for thereby forming said hydrocarbon product boiling in the gasoline boiling range.
  • the above recited isomerization conditions may be used in this isomerization.
  • the process further comprises using a portion of a light hydrocarbon gas stream, e.g. a LPG stream, in particular the light hydrocarbon gas stream obtained in step ii), or a portion of the naphtha stream as heat exchanging medium for quenching said raw upgraded naphtha stream.
  • a light hydrocarbon gas stream e.g. a LPG stream, in particular the light hydrocarbon gas stream obtained in step ii
  • a portion of the naphtha stream as heat exchanging medium for quenching said raw upgraded naphtha stream.
  • the hydrogen producing unit comprises feeding a hydrocarbon feedstock such as natural gas.
  • a hydrocarbon feedstock such as natural gas.
  • the hydrogen producing unit apart from using the light hydrocarbon gas, LPG, as feedstock, may also use another hydrocarbon feedstock, such as natural gas.
  • a separate LPG stream is also formed which is also used as hydrocarbon feedstock in the hydrogen producing unit.
  • the naphtha stream and LPG stream in step i) are withdrawn from the same unit, such as a separation unit e.g. a distillation unit.
  • the hydrogen producing unit comprises subjecting said light hydrocarbon gas stream and said hydrocarbon feedstock to: cleaning in a cleaning unit, said cleaning unit preferably being a sulfur- chlorine-metal absorption or catalytic unit; optionally pre-reforming in a pre-reforming unit; catalytic steam methane reforming in a steam reforming unit; water gas shift conversion in a water gas shift unit; optionally carbon dioxide removal in a CO2- separator unit; and optionally hydrogen purification in a hydrogen purification unit.
  • cleaning unit preferably being a sulfur- chlorine-metal absorption or catalytic unit
  • catalytic steam methane reforming in a steam reforming unit water gas shift conversion in a water gas shift unit
  • optionally carbon dioxide removal in a CO2- separator unit optionally hydrogen purification in a hydrogen purification unit.
  • the hydrogen purification unit is a Pressure Swing Adsorption unit (PSA unit), said PSA unit producing an off-gas stream which is used as fuel in the steam reforming unit of the hydrogen producing unit, and/or in fired heaters in any of the hydroprocessing stages of step i), and or the aromatization stage of step ii), and/or for steam production.
  • PSA unit Pressure Swing Adsorption unit
  • This enables further reduction of hydrocarbon consumption, thereby improving energy consumption figures, i.e. higher energy efficiency, as PSA off-gas which otherwise will need to be burned off (flared), is expediently used in the process.
  • the steam reforming unit is: a convection reformer, preferably comprising one or more bayonet reforming tubes such as an HTCR reformer i.e. Topsoe bayonet reformer, where the heat for reforming is transferred by convection along with radiation; a tubular reformer i.e. conventional steam methane reformer (SMR), where the heat for reforming is transferred chiefly by radiation in a radiant furnace; autothermal reformer (ATR), where partial oxidation of the hydrocarbon feed with oxygen and steam followed by catalytic reforming; electrically heated steam methane reformer (e-SMR), where electrical resistance is used for generating the heat for catalytic reforming; or combinations thereof.
  • a convection reformer preferably comprising one or more bayonet reforming tubes such as an HTCR reformer i.e. Topsoe bayonet reformer, where the heat for reforming is transferred by convection along with radiation
  • a tubular reformer i.e. conventional steam methane reformer (S
  • the catalyst in the steam reforming unit is a reforming catalyst, e.g. a nickel-based catalyst.
  • the catalyst in the water gas shift reaction is any catalyst active for water gas shift reactions.
  • the said two catalysts can be identical or different.
  • reforming catalysts are Ni/MgAI2O4, Ni/AI2O3, Ni/CaAI2O4, Ru/MgAI2O4, Rh/MgAI2O4, lr/MgAI2O4, Mo2C, Wo2C, CeO2, Ni/ZrO2, Ni/MgAI2O3, Ni/CaAI2O3, Ru/MgAI2O3, or Rh/MgAI2O3, a noble metal on an AI2O3 carrier, but other catalysts suitable for reforming are also conceivable.
  • the catalytically active material may be Ni, Ru, Rh, Ir, or a combination thereof, while the ceramic coating may be AI2O3, ZrO2, MgAI2O3, CaAI2O3, or a combination therefore and potentially mixed with oxides of Y, Ti, La, or Ce.
  • the maximum temperature of the reactor may be between 850-1300°C.
  • the pressure of the feed gas may be 15-180 bar, preferably about 25 bar.
  • Steam reforming catalyst is also denoted steam methane reforming catalyst or methane reforming catalyst.
  • the make-up hydrogen stream passes through a compressor section comprising a make-up compressor optionally also a recycle compressor, the make-up compressor also producing a hydrogen recycle stream which is added to the hydrogen producing unit, and/or to the cleaning unit of the hydrogen producing unit.
  • the invention is a plant, i.e. process plant, for producing a hydrocarbon product boiling in the gasoline boiling range, comprising:
  • hydroprocessing section arranged to receive a tar-containing feedstock, and optionally also for receiving a compressed hydrogen stream for producing a naphtha product; said hydroprocessing section comprising a hydrotreating unit and a hydrocracking unit;
  • an aromatization section comprising a reactor containing a catalyst, preferably a catalyst comprising an alumininosilicate zeolite, and arranged to receive said naphtha product for producing said hydrocarbon product boiling in the gasoline boiling range and a light hydrocarbon gas stream as a liquid petroleum gas (LPG) stream;
  • a catalyst preferably a catalyst comprising an alumininosilicate zeolite
  • HPU hydrogen producing unit
  • the sole figure shows a schematic flow diagram of the overall process/plant according to an embodiment of the invention.
  • a block flow diagram of the overall process/plant 10 is shown, where a tar-containing feedstock 12 such as a coke oven tar feed or a product from pyrolsysis of tyres e.g. waster tyres, is introduced to the hydroprocessing stage 110.
  • This stage or section 110 comprises a feed section and reactor section 110’ including a conditioning step or section including the use of one or more guards, e.g. bed guards, for the removal of metals, removal of di-olefins, and removal of bulk sulfur and nitrogen.
  • the stage or section 110 comprises also one or more hydrotreating (HDT) units (reactors) as well as one or more downstream hydrocracking (HCR) units, for thereby enabling deep sulfur and nitrogen removal and aromatic saturation.
  • An optional hydrocarbon product property improvement may also be provided.
  • Hydroprocessing stage or section 110 includes a separation stage 110” which produces hydrocarbon products in the form of naphtha stream 14 as an intermediate product, diesel 16 and a bottom product such as lube base stock (base oil for lubes) 18.
  • lube base stock base oil for lubes
  • an LPG stream 20 is also produced.
  • the naphtha stream 14 is then passed to aromatization stage 120 comprising a reactor containing a catalyst comprising an aluminosilicate zeolite, thereby increasing the aromatic content of the naphtha and significantly increasing the octane number in the resulting hydrocarbon product boiling in the gasoline boiling range 22, by forming a high-quality gasoline product having an octane number (RON) of 85 or higher, such as 90 or higher.
  • the aromatization stage may also include an isomerization stage (not shown).
  • a light hydrocarbon gas stream in particular LPG stream 24, is produced, which is then used as feed for the hydrogen producing unit 130, together with an optional separate hydrocarbon feedstock stream 26 such as natural gas used as make-up gas for the steam reforming in the hydrogen producing unit 130.
  • LPG stream 20 from the separation section 110” may also be added, as shown in the figure.
  • the LPG stream(s) may be mixed and then co-fed with the natural gas stream 26 to the hydrogen producing unit 130.
  • the hydrogen producing unit 130 comprises a first section 130’ which includes a cleaning unit such as sulfur-chlorine-metal absorption or catalytic unit, one or more prereformer units, steam reformer preferably a convection reformer (e.g. HTCR), and water gas shifting unit(s), as it is well known in the art of hydrogen production; none of these units are shown here.
  • a hydrogen purification unit, such as PSA unit 130” is optionally provided to further enrich the gas and produce a hydrogen stream 28.
  • Offgas 30 from the PSA unit (PSA off-gas) is used as fuel in the hydrogen producing unit, and in particular as fuel for a HTCR unit, more particularly the burner of the HTCR unit, as well as in the hydroprocessing stage 110.
  • the hydrogen stream 28 may be exported as a product and/or may be used as makeup hydrogen in the process.
  • the hydrogen stream 28 passes to a compressor section 140 which includes make-up gas compressor an optionally also a recycle compressor, not shown.
  • An optional hydrogen-rich stream (not shown) which may have been produced in the hydroprocessing stage 110 and makeup hydrogen stream 28 are then compressed by respectively the recycle compressor and the make-up compressor and used for adding hydrogen as make-up hydrogen stream 30 into the hydroprocessing stage 110, and optionally also (not shown) to the aromatization stage 120.
  • a hydrogen stream 32 is recycled to hydrogen production unit 130.

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  • Chemical & Material Sciences (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Organic Chemistry (AREA)
  • Engineering & Computer Science (AREA)
  • General Chemical & Material Sciences (AREA)
  • Health & Medical Sciences (AREA)
  • General Health & Medical Sciences (AREA)
  • Combustion & Propulsion (AREA)
  • Inorganic Chemistry (AREA)
  • Production Of Liquid Hydrocarbon Mixture For Refining Petroleum (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)

Abstract

La présente invention concerne un procédé et une installation de production de produit hydrocarboné en ébullition dans la plage d'ébullition de l'essence à partir d'une charge contenant du goudron, le procédé et l'installation comprenant un étage d'hydrotraitement qui comprend l'hydrotraitement et l'hydrocraquage pour produire du diesel et du naphta, et l'aromatisation subséquente du naphta, ce qui permet également de produire un gaz d'hydrocarbure léger sous la forme d'un gaz de pétrole liquide (GPL), à partir duquel un courant d'hydrogène est produit.
EP21763291.8A 2020-08-13 2021-08-12 Procédé et installation de production d'essence à partir d'une charge contenant du goudron Pending EP4196557A1 (fr)

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PCT/EP2021/072523 WO2022034181A1 (fr) 2020-08-13 2021-08-12 Procédé et installation de production d'essence à partir d'une charge contenant du goudron

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WO2024104980A1 (fr) * 2022-11-16 2024-05-23 Nynas Ab (Publ) Procédé de préparation d'une huile de base à partir d'huile de pyrolyse de pneu et huile de base pouvant être obtenue à l'aide du procédé

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US3871993A (en) 1974-03-29 1975-03-18 Mobil Oil Corp Upgrading the octane value of naphtha employing a crystalline aluminosilicate zeolite which has a high silica to alumina ratio wherein alumina is incorporated in the interstices of the zeolite crystal
DK162891A (da) 1991-09-23 1993-03-24 Haldor Topsoe As Fremgangsmaade og reaktor til gennemfoerelse af ikke-adiabatiske reaktioner.
AU6654298A (en) * 1997-02-18 1998-09-08 Exxon Chemical Patents Inc. Naphtha aromatization process
US9039790B2 (en) * 2010-12-15 2015-05-26 Uop Llc Hydroprocessing of fats, oils, and waxes to produce low carbon footprint distillate fuels
US9752080B2 (en) 2013-03-27 2017-09-05 Haldor Topsoe A/S Process for producing hydrocarbons
FI126812B (en) 2013-11-21 2017-05-31 Upm Kymmene Corp INTEGRATED PROCESS FOR THE PREPARATION OF HYDROCARBON
KR101956489B1 (ko) 2014-10-03 2019-03-08 사우디 아라비안 오일 컴퍼니 천연가스/셰일 가스 응축물로부터 방향족 생성을 위한 2-단계 공정
EP3574991A1 (fr) 2018-05-31 2019-12-04 Haldor Topsøe A/S Reformage à la vapeur chauffée par un chauffage à résistance

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CN116075478A (zh) 2023-05-05
AU2021324383A1 (en) 2023-02-23

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