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WO2025061932A1 - Procédé de préparation de gaz de synthèse à partir d'une charge de départ liquide - Google Patents

Procédé de préparation de gaz de synthèse à partir d'une charge de départ liquide Download PDF

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Publication number
WO2025061932A1
WO2025061932A1 PCT/EP2024/076419 EP2024076419W WO2025061932A1 WO 2025061932 A1 WO2025061932 A1 WO 2025061932A1 EP 2024076419 W EP2024076419 W EP 2024076419W WO 2025061932 A1 WO2025061932 A1 WO 2025061932A1
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WIPO (PCT)
Prior art keywords
range
feed stream
stream
weight
organic compounds
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English (en)
Inventor
Andre BADER
Martin Gall
Simon Wachter
Pawel CZAJKA
Martin Graebner
Andreas Richter
Olaf Schulze
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BASF SE
Bergakademie Freiberg
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BASF SE
Bergakademie Freiberg
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Publication of WO2025061932A1 publication Critical patent/WO2025061932A1/fr
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    • 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
    • C01B3/36—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 using oxygen or mixtures containing oxygen as gasifying agents
    • 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
    • C01B3/50—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
    • C10J3/46—Gasification of granular or pulverulent flues in suspension
    • C10J3/466—Entrained flow 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
    • C01B2203/02—Processes for making hydrogen or synthesis gas
    • C01B2203/025—Processes for making hydrogen or synthesis gas containing a partial oxidation step
    • C01B2203/0255—Processes for making hydrogen or synthesis gas containing a partial oxidation step containing a non-catalytic partial oxidation 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
    • C01B2203/04—Integrated processes for the production of hydrogen or synthesis gas containing a purification step for the hydrogen or the synthesis gas
    • C01B2203/0465—Composition of the impurity
    • C01B2203/0475—Composition of the impurity the impurity being carbon dioxide
    • 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
    • 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
    • C01B2203/12—Feeding the process for making hydrogen or synthesis gas
    • C01B2203/1276—Mixing of different feed components
    • 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
    • C01B2203/14—Details of the flowsheet
    • C01B2203/148—Details of the flowsheet involving a recycle stream to the feed of the process for making hydrogen or synthesis gas
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J2300/00—Details of gasification processes
    • C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
    • C10J2300/0903—Feed preparation
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J2300/00—Details of gasification processes
    • C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
    • C10J2300/0953—Gasifying agents
    • C10J2300/0959—Oxygen
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J2300/00—Details of gasification processes
    • C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
    • C10J2300/0953—Gasifying agents
    • C10J2300/0969—Carbon dioxide
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J2300/00—Details of gasification processes
    • C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
    • C10J2300/0953—Gasifying agents
    • C10J2300/0973—Water
    • C10J2300/0976—Water as steam
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J2300/00—Details of gasification processes
    • C10J2300/16—Integration of gasification processes with another plant or parts within the plant
    • C10J2300/164—Integration of gasification processes with another plant or parts within the plant with conversion of synthesis gas
    • C10J2300/1656—Conversion of synthesis gas to chemicals

Definitions

  • the present invention relates to a process for preparing syngas (also known as synthesis gas) via partial oxidation reaction of one or more organic compounds, wherein at least a portion of the one or more organic compounds are provided in liquid form, and wherein the partial oxidation is preferably carried out without using a catalyst.
  • syngas also known as synthesis gas
  • syngas comprises H2 and CO, wherein one or both of CO2 and H2O can be comprised as well.
  • syngas can be prepared having a specific H2 to CO molar ratio. Preparation of syngas is typically done by partial oxidation of an organic compound in the presence of one or more of O2 and steam. CO2 can be generated as side-product and it can be separated from a product stream. Separated CO2 can also be recycled into the preparation process.
  • WO 2015/090575 A1 generally relates to a method and device for producing syngas.
  • WO 2022/200532 A1 relates to a method for producing a synthesis gas mixture containing hydrogen and carbon monoxide by means of non-catalytic partial oxidation of hydrocarbons in the presence of oxygen and carbon dioxide, in which method at least a reactant gas containing hydrocarbons, a reactant gas containing oxygen, and a reactant gas containing carbon dioxide are fed into a partial oxidation reactor and are reacted at a temperature in the range of 1200 to 1550 °C to obtain a product gas mixture containing hydrogen, carbon monoxide and carbon dioxide, with at least a portion of the carbon dioxide being separated off from the product gas mixture and fed back into the partial oxidation reactor.
  • the method is characterized in that the carbon dioxide fed into the partial oxidation reactor contains additional, imported carbon dioxide, with a product gas mixture having a molar ratio of hydrogen to carbon monoxide in the range of 0.8:1 to 1.6:1 being obtained in the partial oxidation reactor.
  • US 10435295 relates to a method of preparing liquid fuels from syngas, the method particularly comprising: providing a waste conversion reactor having a decomposition chamber wherein waste materials comprising organic and inorganic waste is pyrolyzed to produce a high temperature syngas from said organic material and slag from decomposition of said inorganic waste; said waste conversion reactor comprising a submerged arc furnace or plasma torch furnace which supplies heat to the decomposition chamber for pyrolysis and decomposition of said organic and inorganic waste materials; and introducing said syngas to a liquid fuel synthesis system comprising one or more synfuel conversion reactors wherein said syngas is converted into liquid fuel.
  • one or more effluent stream from said synfuel conversion reactor comprising water, carbon dioxide and tail gas can be introduced into said waste conversion reactor.
  • US 2016/0362355 A1 relates to preparation of an oil product of gasoline.
  • the product contains hydrocarbon compound ranged as a gasoline composition.
  • the purification process of dimethyl ether (DME) used can reduce the feed rate for obtaining a smaller reactor with cost down.
  • Carbon dioxide (CO2) can be separated to be recycled back to the gasifier to be reused, archived or used otherwise for improves global environment.
  • CO2 can be reacted with hydrocarbons, water vapor, etc. through a high-temperature plasma torch to generate a synthesis gas (syngas) of carbon monoxide (CO) and hydrogen (H2) for regulating a hydrogen/ carbon ratio of a biomass- or hydrocarbon-synthesized compound and helping subsequent chemical synthesis reactions.
  • the final gasoline production has a high yield, a high octane rate, low nitrogen and sulfur pollution and a highly 'green' quality.
  • WO 2021/180482 A1 discloses a process for the production of synthesis gas by gasification, preferably by plasma gasification, of carbon-containing material using a gasification gas comprising at least 2 mol% carbon dioxide, and optionally at least one gas selected from steam, oxygen, hydrogen, methane and air, wherein external energy obtained from electric power is supplied in the gasification step and wherein exhaust gas of the process comprising carbon dioxide is at least partially recycled back into the gasification step.
  • the invention proposes a process for production of synthesis gas downstream products, wherein the synthesis gas is produced by the process and used as an intermediate product in a downstream synthesis process.
  • US 2022/234889 A1 relates to a method to control syngas composition by reactor temperature.
  • a method of producing syngas including partial oxidization of a hydro- carbonaceous feedstock material, wherein partial oxidation is carried out at specific reaction conditions.
  • EP 3878807 A1 relates to a process for the production of synthesis gas via allothermic gasification with controlled carbon dioxide reduction.
  • a process for the production of synthesis gas by gasification of carbon-containing material is disclosed therein.
  • a feed stream comprising one or more organic compounds in a liquid phase can be used for preparing a syngas.
  • CO2 which can be generated as side-product can be recycled into the process.
  • addition of O2 and H2O can be reduced.
  • recycled CO2 can be used for spraying the one or more organic compounds into the reaction zone.
  • the present invention relates to a process for preparing syngas, the process comprising
  • from 0 to 50 weight-%, more preferably from 0 to 40 weight-%, more preferably from 0 to 30 weight-%, more preferably from 0 to equal to or smaller than 20 weight-%, of the one or more organic compounds consist of O.
  • the one or more organic compounds comprised in the liquid phase are selected from the group consisting of pyrolysis oils, heating oils, vacuum residues, preferably vacuum distillation residues, crude oil residues, heavy crude oils, extra heavy crude oils, tar sand bitumen, visbreaker bottom residues, deasphalter bottom residues, C5 asphalthene fraction, preferably C5 asphalthene, high viscous residues, bio oils, fuel oils, pyrolysis gasolines, tire pyrolysis oils (TPO), waste oils, used oils, and mixtures thereof, wherein the one or more organic compounds preferably are pyrolysis oils.
  • the one or more organic compounds comprised in the liquid phase are selected from the group consisting of pyrolysis oils, heating oils, vacuum residues, preferably vacuum distillation residues, crude oil residues, heavy crude oils, extra heavy crude oils, tar sand bitumen, visbreaker bottom residues, deasphalter bottom residues, C5 asphalthene fraction, preferably C5 asphalthene, high viscous residues, bio oils, fuel oils, pyrolysis gasolines, tire pyrolysis oils (TPO), waste oils, used oils, and mixtures thereof
  • the pyrolysis oils are preferably obtained from pyrolysis of one or more of biomass, plastic waste, and mixed plastic waste, preferably mixed plastic waste, wherein the mixed plastic waste preferably comprises optionally shredded waste tires, wherein the mixed plastic waste more preferably comprises one or more of polyethylenes, polypropylenes, polyisoprenes, polyethylene terephthalates, polystyrenes, copolymers of one or more thereof, block polymers of one
  • the one or more organic compounds comprised in the liquid phase are selected from the group consisting of pyrolysis oils, heating oils, vacuum residues, preferably vacuum distillation residues, crude oil residues, heavy crude oils, extra heavy crude oils, tar sand bitumen, visbreaker bottom residues, deasphalter bottom residues, C5 asphalthene fraction, preferably C5 asphalthene, high viscous residues, bio oils, fuel oils, pyrolysis gasolines, tire pyrolysis oils (TPO), waste oils, used oils, and mixtures thereof
  • the heating oils are selected from the group consisting of (Ci-Cioo)hydrocarbons, preferably (C5-Cso)hy- drocarbons, more preferably (Cio-C6o)hydrocarbons, more preferably (Cn-C4o)hydrocarbons, more preferably (Ci2-C25)hydrocarbons, more preferably (Ci3-C2i)hydrocarbons,
  • the heating oils have a boiling point in the range of from 100 to 1 ,000 °C, more preferably in the range of from 150 to 750 °C, more preferably in the range of from 200 to 500 °C, more preferably in the range of from 225 to 375 °C, more preferably in the range of from 250 to 350 °C, preferably at a pressure in the range of from 0.99 to 1 .01 bara.
  • the one or more organic compounds have a lower heating value in the range of from 20 to 60 MJ/kg, more preferably in the range of from 30 to 50 MJ/kg. It is preferred that from 90 to 100 weight-%, more preferably from 95 to 100 weight-%, more preferably from 99 to 100 weight-%, of the gaseous phase comprised in the first feed stream prepared in (i) consist of CO2.
  • the first feed stream prepared in (i) has a weight ratio, organic com- pounds:CC>2, of the one or more organic compounds to CO2 of equal to or greater than 1 :5, more preferably in the range of from 1 :5 to 1 ,000:1 , more preferably in the range of from 1 :5 to 500:1 , more preferably in the range of from 1 :5 to 100:1 , more preferably in the range of from 1 :5 to 50:1 , more preferably in the range of from 1 :1 to 25:1 , more preferably in the range of from 2:1 to 20:1 , more preferably in the range of from 5:1 to 15:1.
  • the first feed stream prepared in (i) displays a multiphase flow regime, more preferably a two phase flow regime.
  • the first feed stream prepared in (i) displays a dispersed flow regime, a plug flow regime, a slug flow regime, a wavy flow regime, a stratified flow regime, an annular flow regime or a mist flow regime, preferably a dispersed flow regime, wherein the first feed stream prepared in (i) preferably displays a horizontal flow.
  • the first feed stream prepared in (i) displays a churn flow regime, an annular flow regime, a bubbly flow regime, a slag flow regime, or a mist flow regime, preferably an annular flow regime or a mist flow regime, more preferably a mist flow regime, wherein the first feed stream prepared in (i) preferably displays a vertical flow.
  • the liquid phase of the first feed stream prepared in (i) has a viscosity in the range of from 20 to 6,000 mPas, mor preferably in the range of from 100 to 5,000 mPas, wherein the viscosity is preferably determined according to Reference Example 1 .
  • the first feed stream prepared in (i) has a temperature in the range of from 50 to 220 °C, more preferably in the range of from 80 to 190 °C, more preferably in the range of from 110 to 160 °C.
  • the first feed stream prepared in (i) has a pressure in the range of from 5 to 80 bara, more preferably in the range of from 35 to 60 bara, more preferably in the range of from 42 to 52 bara.
  • the first feed stream prepared in (i) has a mass flow rate in the range of from 100 to 20,000 kg/h, more preferably in the range of from 3,000 to 17,000 kg/h, more preferably in the range of from 5,000 to 15,000 kg/h, more preferably in the range of from 6,000 to 14,000 kg/h.
  • the second feed stream prepared in (ii) comprises steam, wherein the second feed stream prepared in (ii) more preferably has a weight ratio, O2:steam, of O2, calculated as elemental O2, to steam, calculated as H2O, in the range of from 1 :10 to 100:1 , more preferably in the range of from 1 :1 to 61 :1.
  • the second feed stream prepared in (ii) has a temperature in the range of from 25 to 400 °C, more preferably in the range of from 50 to 300 °C, more preferably in the range of from 90 to 250 °C.
  • the second feed stream prepared in (ii) has a pressure in the range of from 5 to 80 bara, more preferably in the range of from 35 to 60 bara, more preferably in the range of from 40 to 52 bara.
  • the second feed stream prepared in (ii) has a mass flow rate in the range of from 100 to 20,000 kg/h, more preferably in the range of from 3,000 to 17,000 kg/h, more preferably in the range of from 5,000 to 15,000 kg/h, more preferably in the range of from 6,000 to 14,000 kg/h.
  • mixing in (iii) is conducted by spraying of the first feed stream and of the second feed stream, forming droplets and optionally liquid fragments of the liquid phase.
  • mixing in (iii) comprises
  • mixing in (iii) comprises (iii.1) and (iii.2) as defined herein, it is preferred that mixing in (iii.1) is conducted by spraying of the mixed feed stream, forming droplets and optionally liquid fragments of the liquid phase.
  • mixing in (iii) comprises (iii.1) and (iii.2) as defined herein
  • feeding the mixed feed stream in the reaction zone is conducted by spraying of the mixed feed stream, forming droplets and optionally liquid fragments of the liquid phase.
  • spraying comprises applying a flow rate of the mixed feed stream in the range of from 100 to 1500 m 3 /h, more preferably in the range of from 200 to 1000 m 3 /h.
  • the mixed feed stream obtained in (iii) displays a multiphase flow regime, more preferably a two phase flow regime.
  • the mixed feed stream obtained in (iii) displays a dispersed flow regime, a plug flow regime, a slug flow regime, a wavy flow regime, a stratified flow regime, an annular flow regime or a mist flow regime, preferably a dispersed flow regime, wherein the mixed feed stream obtained in (iii) preferably displays a horizontal flow.
  • the mixed feed stream obtained in (iii) displays a churn flow regime, an annular flow regime, a bubbly flow regime, a slag flow regime, or a mist flow regime, preferably an annular flow regime or a mist flow regime, more preferably a mist flow regime, wherein the mixed feed stream obtained in (iii) preferably displays a vertical flow.
  • the mixed feed stream obtained in (iii) has a weight ratio, organic compounds ⁇ , of the one or more organic compounds to O2 in the range of from 0.10:1 to 2.00:1 , more preferably in the range of from 0.25:1 to 1.50:1.
  • the mixed feed stream obtained in (iii) has a weight ratio, CO2:O2, of CO2 to O2 in the range of from 1 :500 to 1 :10, more preferably in the range of from 1 :100 to 1 :5.0, more preferably in the range of from 1 :75 to 1 :2.0, more preferably in the range of from 1 :50 to 1 :1.5.
  • the mixed feed stream obtained in (iii) has a weight ratio, organic com- pounds:steam, of the one or more organic compounds to steam in the range of from 1 :1 to 100:1 , more preferably in the range of from 5:1 to 50:1 , more preferably in the range of from 7:1 to 41 :1 , more preferably in the range of from 20:1 to 25:1.
  • reacting in (iv) is conducted at a temperature in the range of from 1100 to 1500 °C, more preferably in the range of from 1200 to 1450 °C, more preferably in the range of from 1225 to 1425 °C.
  • reacting in (iv) is performed by gasification, more preferably entrained flow gasification (German “Flugstromvergasung”).
  • the mixed feed stream displays a retention time in the reaction zone in the range of from 1 to 10 s. It is preferred that the product stream obtained in (iv) comprises a molar fraction of CO in the range of from 0.30 to 0.95, more preferably in the range of from 0.40 to 0.90, more preferably in the range of from 0.45 to 0.88.
  • the product stream obtained in (iv) comprises a molar fraction of H2 in the range of from 0.05 to 0.60, more preferably in the range of from 0.10 to 0.50, more preferably in the range of from 0.20 to 0.50.
  • the process further comprises after (iv)
  • the process further comprises (v)
  • separating CO2 is performed by a CO2 scrubber or by CO2 absorption.
  • process further comprises (v), preferably (v) and (vi), it is preferred according to a first alternative that the process further comprises after (v), preferably after
  • the process further comprises (vii), it is preferred that from 1 to 100 weight- %, more preferably from 25 to 75 weight-%, more preferably from 40 to 60 weight-%, of the CO2 comprised in the first feed stream prepared in (i) consists of recycled CO2 from the stream comprising CO2 obtained in (v) or (vi).
  • process further comprises (v), preferably (v) and (vi)
  • process further comprises after (v), preferably after (vi)
  • the process further comprises (vii’)
  • from 1 to 100 weight- %, more preferably from 25 to 75 weight-%, more preferably from 40 to 60 weight-%, of the CO2 recycled to the first feed stream obtained from (vii’) consists of recycled CO2 from the stream comprising CO2 obtained in (v) or (vi).
  • the process further comprises after (iv), preferably after (v),
  • H2 added to the product stream obtained in (iv) or to the product stream being CO2 depleted obtained in (v) comprises one or more of H2 obtained from a pipeline, H2 obtained from a tank, H2 obtained from a different process, preferably from a process for preparing styrene, and H2 obtained from electrolysis, preferably from electrolysis using green power.
  • preparing the first feed stream in (i) comprises
  • the stream comprising one or more organic compounds prepared in (i.1 ) has a temperature in the range of from 10 to 350 °C, more preferably in the range of from 25 to 300 °C, more preferably in the range of from 50 to 200 °C, more preferably in the range of from 70 to 150 °C.
  • the stream comprising one or more organic compounds prepared in (i.1 ) has a pressure in the range of from 5 to 80 bara, more preferably in the range of from 35 to 60 bara, more preferably in the range of from 42 to 52 bara.
  • the stream comprising one or more organic compounds prepared in (i.1 ) has a mass flow rate in the range of from 100 to 20,000 kg/h, more preferably in the range of from 3,000 to 17,000 kg/h, more preferably in the range of from 5,000 to 15,000 kg/h, more preferably in the range of from 6,000 to 14,000 kg/h.
  • the stream comprising CO2 prepared in (i.2) has a temperature in the range of from 25 to 380 °C, more preferably in the range of from 40 to 360 °C, more preferably in the range of from 60 to 300 °C.
  • preparing the first feed stream in (i) comprises (i.1), (i.2) and (i.3)
  • the stream comprising CO2 prepared in (i.2) has a pressure in the range of from 5 to 80 bara, more preferably in the range of from 35 to 60 bara, more preferably in the range of from 42 to 52 bara.
  • the stream comprising CO2 prepared in (i.2) has a mass flow rate in the range of from 100 to 20,000 kg/h, more preferably in the range of from 3,000 to 17,000 kg/h, more preferably in the range of from 5,000 to 15,000 kg/h, more preferably in the range of from 6,000 to 14,000 kg/h.
  • the stream comprising CO2 comprises one or more of CO2 recycled from (vii), CO2 recycled from (vii’), CO2 obtained from a different process for preparing syngas, CO2 obtained from a tank, CO2 obtained from a pipeline from another plant.
  • the second feed stream prepared in (ii) comprises steam, wherein preparing the second feed stream in (ii) comprises
  • the second feed stream prepared in (ii) comprises steam
  • preparing the second feed stream in (ii) comprises (ii.1 ), (ii.2) and (ii.3) as defined herein
  • the stream comprising O2 prepared in (ii.1 ) has a temperature in the range of from 25 to 400 °C, more preferably in the range of from 60 to 250 °C, more preferably in the range of from 120 to 190 °C.
  • the second feed stream prepared in (ii) comprises steam
  • preparing the second feed stream in (ii) comprises (ii.1 ), (ii.2) and (ii.3) as defined herein
  • the stream comprising O2 prepared in (ii.1 ) has a pressure in the range of from 5 to 80 bara, more preferably in the range of from 35 to 60 bara, more preferably in the range of from 42 to 52 bara.
  • the second feed stream prepared in (ii) comprises steam
  • preparing the second feed stream in (ii) comprises (ii.1 ), (ii.2) and (ii.3) as defined herein
  • the stream comprising O2 prepared in (ii.1 ) has a mass flow rate in the range of from 100 to 20,000 kg/h, more preferably in the range of from 3,000 to 17,000 kg/h, more preferably in the range of from 5,000 to 15,000 kg/h, more preferably in the range of from 6,000 to 14,000 kg/h.
  • the second feed stream prepared in (ii) comprises steam
  • preparing the second feed stream in (ii) comprises (ii.1 ), (ii.2) and (ii.3) as defined herein
  • the stream comprising steam prepared in (ii.2) has a temperature in the range of from 200 to 500 °C, more preferably in the range of from 300 to 450 °C, more preferably in the range of from 350 to 425 °C.
  • the second feed stream prepared in (ii) comprises steam
  • preparing the second feed stream in (ii) comprises (ii.1 ), (ii.2) and (ii.3) as defined herein
  • the stream comprising steam prepared in (ii.2) has a pressure in the range of from 5 to 80 bara, more preferably in the range of from 35 to 60 bara, more preferably in the range of from 42 to 52 bara.
  • the second feed stream prepared in (ii) comprises steam
  • preparing the second feed stream in (ii) comprises (ii.1 ), (ii.2) and (ii.3) as defined herein
  • the stream comprising steam prepared in (ii.2) has a mass flow rate smaller than 6,000 kg/h, more preferably smaller than 3,000 kg/h, more preferably smaller than 1 ,500 kg/h, more preferably smaller than 1 ,000 kg/h.
  • the molar ratio, CO2(product stream):CO2(mixed stream), of CO2 comprised in the product stream obtained in (iv) to CO2 comprised in the mixed stream obtained in (iii) is less than 1 :1.
  • the product stream obtained in (iv) or the product stream being CO2 depleted obtained in (v) has a volume ratio, H2:CO, of H2 to CO in the range of from 0.1 :1 to 1.5:1 , more preferably in the range of from 0.3:1 to 1.3:1 , more preferably in the range of from 0.4:1 to 1.1 :1.
  • the invention further relates to a method, preferably according to the method described herein, comprising the step:
  • the monomer is a di- or polyol, preferably butandiol, aldehyde, preferably formaldehyde, di- or polyisocyanate, preferably methylene diphenyl diisocyanate (MDI), polymeric methylene diphenyl diisocyanate (pMDI), toluene diisocyanate (TDI), hexamethylenediisocyanate (HDI) or isophoronediisocyanate (IPDI), amide, preferably caprolactam, alkene, preferably styrene, ethene and norbornene, alkyne, (di)ester, preferably methyl methacrylate, mono or diacid, preferably adipic acid or terephthalic acid, diamine, preferably hexamethylenediamine, nonanediamine, or sulfones, preferably 4, 4'-dichlorodiphenyl sulfone.
  • MDI
  • the polymer is and/or the polymer product comprises polyamide (PA), preferably PA 6 or PA 66, polyisocyanate polyaddition product, preferably polyurethane (PU), thermoplastic polyurethane (TPU), polyurea or polyisocyanurate (PIR), low-density polyethylene (LDPE), high-density polyethylene (HDPE), polyethylene (PE), polypropylene (PP), polyvinyl chloride (PVC), polyvinyl acetate (PVA), polystyrene (PS), poly acrylonitrile butadiene styrene (ABS), poly styrene acrylonitrile (SAN), poly acrylate styrene acrylonitrile (ASA), polytetrafluoroethylene (PTFE), poly(methyl acrylate) (PM A), poly(methyl methacrylate) (PM MA), polybutadiene (BR, PBD), poly(cis-1 ,4-isoprene), polyamide (PA),
  • the polymer and/or the polymer product is/are or is/are a part of:
  • cylinder head cover a part of a car, preferably cylinder head cover, engine cover, housing for charge air cooler, charge air cooler flap, intake pipe, intake manifold, connector, gear wheel, fan wheel, cooling water box, housing, housing part for heat exchanger, coolant cooler, charge air cooler, thermostat, water pump, radiator, fastening part, part of battery system for electromobility, dashboard, steering column switch, seat, headrest, center console, transmission component, door module, A, B, C or D pillar cover, spoiler, door handle, exterior mirror, windscreen wiper, windscreen wiper protection housing, decorative grill, cover strip, roof rail, window frame, sunroof frame, antenna panel, headlight and taillight, engine cover, cylinder head cover, intake manifold, airbag, cushion, or coating;
  • - a cloth, preferably shirt, trousers, pullover, boot, shoe, shoe sole, tight or jacket;
  • an electrical part preferably electrical or electronic passive or active component, circuit board, printed circuit board, housing component, foil, line, switch, plug, socket, distributor, relay, resistor, capacitor, inductor, bobbin, lamp, diode, LED, transistor, connector, regulator, integrated circuit (IC), processor, controller, memory, sensor, microswitch, microbutton, semiconductor, reflector housing for light-emitting diodes (LED), fastener for electrical or electronic component, spacer, bolt, strip, slide-in guide, screw, nut, film hinge, snap hook (snap- in), or spring tongue;
  • LED light-emitting diodes
  • a consumer, agricultural product or pharmaceutical product preferably tennis string, climbing rope, bristle, brush, artificial grass, 3D printing filament, grass trimmer, zipper, hook and loop fastener, paper machine clothing, extrusion coating, fishing line, fishing net, offshore line and rope, vial, syringe, ampoule, bottle, sliding element, spindle nut, chain conveyor, plain bearing, roller, wheel, gear, roller, ring gear, screw and spring dampers, hose, pipeline, cable sheathing, socket, switch, cable tie, fan wheel, carpet, box or bottle for cosmetics, mattress, cushion, insulation, detergent, dishwasher tabs or powder, shampoo, body wash, shower gel, soap, fertilizer, fungicide, or pesticide;
  • a packaging for the food industry preferably mono- or multi-layer blown film, cast film (mono- or multi-layer), biaxially stretched film, or laminating film; or
  • the content of the feedstock in the product stream comprising H2 and CO, monomer, polymer or polymer product is 1 weight-% or more, preferably 2 weight-% or more, more preferably 5 weight-% or more, more preferably 15 weight-% or more, more preferably 30 weight-% or more, more preferably 40 weight-% or more, more preferably 60 weight-% or more, more preferably 80 weight-% or more, more preferably 90 weight-% or more, more preferably 95 weight-% or more; and/or wherein the content of the feedstock in the product stream comprising H2 and CO, monomer, polymer or polymer product is 100 weight-% or less, preferably 95 weight-% or less, more preferably 90 weight-% or less, more preferably 50 weight-% or less, more preferably 25 weight-% or less, more preferably 10 weight-% or less; and
  • the content of C stemming from the product stream comprising H2 and CO which is contained in the monomer, polymer or polymer product is 1 weight-% or more, wherein C is calculated as the element, preferably 2 weight-% or more, more preferably 5 weight-% or more, more preferably 15 weight-% or more, more preferably 30 weight-% or more, more preferably 40 weight-% or more, more preferably 60 weight-% or more, more preferably 80 weight-% or more, more preferably 90 weight-% or more, more preferably 95 weight-% or more; and/or wherein the content of C stemming from the product stream comprising H2 and CO which is contained in the monomer, polymer or polymer product is 100 weight-% or less, wherein C is calculated as the element, preferably 95 weight-% or less, more preferably 90 weight-% or less, more preferably 50 weight-% or less, more preferably 25 weight-% or less, more preferably 10 weight-% or less; and preferably wherein the content is determined
  • Process for preparing syngas comprising (i) preparing a first feed stream comprising a liquid phase and a gaseous phase, wherein the liquid phase comprises one or more organic compounds, and wherein the gaseous phase comprises CO2;
  • the one or more organic compounds comprised in the liquid phase are selected from the group consisting of pyrolysis oils, heating oils, vacuum residues, preferably vacuum distillation residues, crude oil residues, heavy crude oils, extra heavy crude oils, tar sand bitumen, visbreaker bottom residues, deasphalter bottom residues, C5 asphalthene fraction, preferably C5 asphalthene, high viscous residues, bio oils, fuel oils, pyrolysis gasolines, tire pyrolysis oils (TPO), waste oils, used oils, and mixtures thereof, wherein the one or more organic compounds preferably are pyrolysis oils.
  • the pyrolysis oils are preferably obtained from pyrolysis of one or more of biomass, plastic waste, and mixed plastic waste, preferably mixed plastic waste, wherein the mixed plastic waste preferably comprises optionally shredded waste tires, wherein the mixed plastic waste more preferably comprises one or more of polyethylenes, polypropylenes, polyisoprenes, polyethylene terephthalates, polystyrenes, copolymers of one or more thereof, block polymers of one or more thereof, graft copolymers of one or more thereof, and mixtures of two or more thereof.
  • heating oils are selected from the group consisting of (Ci-Cioo)hydrocarbons, preferably (C5-C8o)hydrocarbons, more preferably (Cio-C6o)hydrocarbons, more preferably (Cn-C4o)hydrocarbons, more preferably (C12- C25)hydrocarbons, more preferably (Ci3-C2i)hydrocarbons, preferably (Ci4-C2o)hydrocar- bons.
  • the heating oils are selected from the group consisting of (Ci-Cioo)hydrocarbons, preferably (C5-C8o)hydrocarbons, more preferably (Cio-C6o)hydrocarbons, more preferably (Cn-C4o)hydrocarbons, more preferably (C12- C25)hydrocarbons, more preferably (Ci3-C2i)hydrocarbons, preferably (Ci4-C2o)hydrocar- bons.
  • heating oils have a boiling point in the range of from 100 to 1 ,000 °C, preferably in the range of from 150 to 750 °C, more preferably in the range of from 200 to 500 °C, more preferably in the range of from 225 to 375 °C, more preferably in the range of from 250 to 350 °C, preferably at a pressure in the range of from 0.99 to 1 .01 bara.
  • 100:1 more preferably in the range of from 1 :5 to 50:1 , preferably in the range of from 1 :1 to 25:1 , more preferably in the range of from 2:1 to 20:1 , more preferably in the range of from 5:1 to 15:1.
  • liquid phase of the first feed stream prepared in (i) has a viscosity in the range of from 20 to 6,000 mPas, preferably in the range of from 100 to 5,000 mPas, wherein the viscosity is preferably determined according to Reference Example 1 .
  • spraying comprises applying a flow rate of the mixed feed stream in the range of from 100 to 1500 m 3 /h, preferably in the range of from 200 to 1000 m 3 /h.
  • (iv) comprises a molar fraction of H2 in the range of from 0.05 to 0.60, preferably in the range of from 0.10 to 0.50, more preferably in the range of from 0.20 to 0.50.
  • H2 added to the product stream obtained in (iv) or to the product stream being CO2 depleted obtained in (v) comprises one or more of H2 obtained from a pipeline, H2 obtained from a tank, H2 obtained from a different process, preferably from a process for preparing styrene, and H2 obtained from electrolysis, preferably from electrolysis using green power.
  • preparing the first feed stream in (i) comprises
  • any one of embodiments 53 to 55 wherein the stream comprising one or more organic compounds prepared in (i.1) has a mass flow rate in the range of from 100 to 20,000 kg/h, preferably in the range of from 3,000 to 17,000 kg/h, more preferably in the range of from 5,000 to 15,000 kg/h, more preferably in the range of from 6,000 to 14,000 kg/h.
  • the process of any one of embodiments 53 to 56, wherein the stream comprising CO2 prepared in (i.2) has a temperature in the range of from 25 to 380 °C, preferably in the range of from 40 to 360 °C, more preferably in the range of from 60 to 300 °C.
  • the stream comprising CO2 comprises one or more of CO2 recycled from (vii), CO2 recycled from (vii’), CO2 obtained from a different process for preparing syngas, CO2 obtained from a tank, CO2 obtained from a pipeline from another plant.
  • the second feed stream prepared in (ii) comprises steam, wherein preparing the second feed stream in (ii) comprises (ii.1) preparing a stream comprising O2; (11.2) preparing a stream comprising steam;
  • polyamide PA
  • PA polyamide
  • PA polyamide
  • TPU thermoplastic polyurethane
  • any one of embodiments 70 to 73 wherein the content of the feedstock in the product stream comprising H2 and CO, monomer, polymer or polymer product is 1 weight-% or more, preferably 2 weight-% or more, more preferably 5 weight-% or more, more preferably 15 weight-% or more, more preferably 30 weight-% or more, more preferably 40 weight-% or more, more preferably 60 weight-% or more, more preferably 80 weight-% or more, more preferably 90 weight-% or more, more preferably 95 weight-% or more; and/or wherein the content of the feedstock in the product stream comprising H2 and CO, monomer, polymer or polymer product is 100 weight-% or less, preferably 95 weight-% or less, more preferably 90 weight-% or less, more preferably 50 weight-% or less, more preferably 25 weight-% or less, more preferably 10 weight-% or less; and preferably wherein the content is determined based on identity preservation and/or segregation and/or mass balance and/or book
  • any one of embodiments 70 to 73 wherein the content of C stemming from the product stream comprising H2 and CO which is contained in the monomer, polymer or polymer product is 1 weight-% or more, wherein C is calculated as the element, preferably 2 weight-% or more, more preferably 5 weight-% or more, more preferably 15 weight-% or more, more preferably 30 weight-% or more, more preferably 40 weight-% or more, more preferably 60 weight-% or more, more preferably 80 weight-% or more, more preferably 90 weight-% or more, more preferably 95 weight-% or more; and/or wherein the content of C stemming from the product stream comprising H2 and CO which is contained in the monomer, polymer or polymer product is 100 weight-% or less, wherein C is calculated as the element, preferably 95 weight-% or less, more preferably 90 weight- % or less, more preferably 50 weight-% or less, more preferably 25 weight-% or less, more preferably 10 weight-% or less;
  • the unit bara refers to an absolute pressure of 10 5 Pa.
  • Viscosity was measured at 20°C according to the standard method DIN EN ISO 3219:1994 using a “Brookfield RV”-type laboratory viscosimeter employing spindles #4 or #5 at 100 revolutions per minute.
  • the prepared streams were mixed and reacted by gasification.

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  • Oil, Petroleum & Natural Gas (AREA)
  • Inorganic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Health & Medical Sciences (AREA)
  • General Health & Medical Sciences (AREA)
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Abstract

La présente invention concerne un procédé de préparation de gaz de synthèse, le procédé comprenant : (i) la préparation d'un premier flux d'alimentation comprenant une phase liquide et une phase gazeuse, la phase liquide comprenant un ou plusieurs composés organiques, et la phase gazeuse comprenant du CO2 ; (ii) la préparation d'un second flux d'alimentation comprenant de l'O2 et éventuellement de la vapeur d'eau ; (iii) le mélange du premier flux d'alimentation et du second flux d'alimentation ; (iv) la réaction du flux d'alimentation mélangé obtenu à l'étape (iii) dans une zone de réaction, l'obtention d'un flux de produit comprenant de l'H2, du CO, éventuellement du CO2, et éventuellement de l'H2O, le ou les composés organiques comprenant du C, de l'H, et éventuellement un ou plusieurs éléments parmi l'O, le S, et le N.
PCT/EP2024/076419 2023-09-22 2024-09-20 Procédé de préparation de gaz de synthèse à partir d'une charge de départ liquide Pending WO2025061932A1 (fr)

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Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2015090575A1 (fr) 2013-12-16 2015-06-25 Ralf Spitzl Procédé et dispositif de production de gaz de synthèse
US20160362355A1 (en) 2015-06-12 2016-12-15 Institute of Nuclear Energy Research, Atomic Energy Council, Executive Yuan, R.O.C. Method of Fabricating Oil Product of Gasoline
US10435295B2 (en) 2016-12-01 2019-10-08 Thomas L Eddy Coupling an electric furnace with a liquid fuel synthesis process to improve performance when processing heterogeneous wastes
EP3878807A1 (fr) 2020-03-13 2021-09-15 Clariant International Ltd Procédé de production de gaz de synthèse par gazéification allothermique à réduction de dioxyde de carbone contrôlée
US20220234889A1 (en) 2021-01-25 2022-07-28 Bradley D. Damstedt Method to control syngas composition by reactor temperature
WO2022200532A1 (fr) 2021-03-26 2022-09-29 Basf Se Procédé de production d'un mélange de gaz de synthèse

Patent Citations (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2015090575A1 (fr) 2013-12-16 2015-06-25 Ralf Spitzl Procédé et dispositif de production de gaz de synthèse
US20160362355A1 (en) 2015-06-12 2016-12-15 Institute of Nuclear Energy Research, Atomic Energy Council, Executive Yuan, R.O.C. Method of Fabricating Oil Product of Gasoline
US10435295B2 (en) 2016-12-01 2019-10-08 Thomas L Eddy Coupling an electric furnace with a liquid fuel synthesis process to improve performance when processing heterogeneous wastes
EP3878807A1 (fr) 2020-03-13 2021-09-15 Clariant International Ltd Procédé de production de gaz de synthèse par gazéification allothermique à réduction de dioxyde de carbone contrôlée
WO2021180482A1 (fr) 2020-03-13 2021-09-16 Clariant International Ltd Procédé de production de gaz de synthèse par gazéification avec réduction contrôlée du dioxyde de carbone
US20220234889A1 (en) 2021-01-25 2022-07-28 Bradley D. Damstedt Method to control syngas composition by reactor temperature
WO2022200532A1 (fr) 2021-03-26 2022-09-29 Basf Se Procédé de production d'un mélange de gaz de synthèse

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