WO2020148376A1 - Method for the preparation of methanol synthesis gas - Google Patents

Method for the preparation of methanol synthesis gas Download PDF

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Publication number
WO2020148376A1
WO2020148376A1 PCT/EP2020/051011 EP2020051011W WO2020148376A1 WO 2020148376 A1 WO2020148376 A1 WO 2020148376A1 EP 2020051011 W EP2020051011 W EP 2020051011W WO 2020148376 A1 WO2020148376 A1 WO 2020148376A1
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WIPO (PCT)
Prior art keywords
feed
synthesis gas
reformer
reforming
steam
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Ceased
Application number
PCT/EP2020/051011
Other languages
French (fr)
Inventor
Per Juul Dahl
Asad NAVID
Thomas Rostrup-Nielsen
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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Publication date
Application filed by Haldor Topsoe AS filed Critical Haldor Topsoe AS
Priority to AU2020208782A priority Critical patent/AU2020208782B2/en
Priority to CN202080009691.5A priority patent/CN113329969B/en
Publication of WO2020148376A1 publication Critical patent/WO2020148376A1/en
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

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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; Reversible storage of hydrogen
    • C01B3/02—Production of hydrogen; Production of gaseous mixtures containing hydrogen
    • C01B3/32—Production of hydrogen; Production of gaseous mixtures containing hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide or air
    • C01B3/34—Production of hydrogen; Production of gaseous mixtures containing hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide or air by reaction of hydrocarbons with gasifying agents
    • C01B3/38—Production of hydrogen; Production of gaseous mixtures containing hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide or air by reaction of hydrocarbons with gasifying agents using catalysts
    • C01B3/382—Processes with two or more reaction steps, of which at least one is catalytic, e.g. steam reforming and partial oxidation
    • C—CHEMISTRY; METALLURGY
    • C07—ORGANIC CHEMISTRY
    • C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C29/00—Preparation of compounds having hydroxy or O-metal groups bound to a carbon atom not belonging to a six-membered aromatic ring
    • C07C29/15—Preparation of compounds having hydroxy or O-metal groups bound to a carbon atom not belonging to a six-membered aromatic ring by reduction of oxides of carbon exclusively
    • C07C29/151—Preparation of compounds having hydroxy or O-metal groups bound to a carbon atom not belonging to a six-membered aromatic ring by reduction of oxides of carbon exclusively with hydrogen or hydrogen-containing gases
    • C07C29/1516—Multisteps
    • C07C29/1518—Multisteps one step being the formation of initial mixture of carbon oxides and hydrogen for synthesis
    • 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
    • C01B2203/0238—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step the reforming step being a carbon dioxide 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
    • C01B2203/06—Integration with other chemical processes
    • C01B2203/061—Methanol production
    • 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
    • C01B2203/1258—Pre-treatment of the feed
    • 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
    • C01B2203/141—At least two reforming, decomposition or partial oxidation steps in parallel
    • 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
    • C01B2203/142—At least two reforming, decomposition or partial oxidation steps in series
    • 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
    • Y02P20/00—Technologies relating to chemical industry
    • Y02P20/141—Feedstock

Definitions

  • the present application is directed to the preparation of methanol synthesis gas. More particular, the invention com bines two-step reforming and steam reforming in parallel.
  • Production of synthesis gas e.g. for the methanol synthesis with natural gas feed is typically carried out by steam re- forming or a combination of steam reforming and oxygen re forming .
  • the product gas from 2-step reforming comprises hydrogen, carbon monoxide, and carbon dioxide as well as other compo nents normally including methane and steam.
  • this invention provides in one aspect a method for the preparation of a methanol synthesis gas comprising the steps of
  • step (d) steam reforming the second feed in parallel with the two-step reforming process) in step (c)to a second synthe sis gas comprising hydrogen, carbon monoxide and carbon di oxide;
  • the content of carbon dioxide in the second feed is prefer ably controlled to obtain a module M of 1.6 to 2.6, prefer- ably between 1.85 to 2.35, in the second synthesis gas withdrawn from the steam reforming.
  • the methanol synthesis gas ob tained by the method according to the invention has a mod ule M of 1.6 to 2.6, preferably between 1.85 and 2.35.
  • the methanol synthesis gas is in a downstream step converted to a methanol prod uct .
  • the steam reforming in step (d) can be performed in a con ventional tubular reformer, a tubular reformer followed by an adiabatic reformer where carbon dioxide is added before and/or after the tubular reformer, a bayonet type reformer, a convective reformer or a tubular reformer where carbon dioxide is added into the reformer tubes after the feed has initially come into contact with the reforming catalyst.
  • a suitable reforming catalyst composition for use in the steam reforming depends on the amount of carbon dioxide added to the feed and the type of reformer used in the steam reforming. In most cases, a nickel catalyst is suffi cient, but for high carbon dioxide contents in the feed, noble metal catalysts may be required for some types of steam reformers.
  • the carbon dioxide for use in the method according to the invention can advantageously be obtained from flue or off- gasses, such as e.g. flue gas stemming from the burners in the steam reformers.
  • the feed composition it might be preferred to desulfurize the first feed upstream the two-step reforming and/or the second feed upstream the steam reforming.
  • An advantage of the method according to the invention is i.a. a reduced energy consumption and a reduced CO2 foot- print.
  • the invention is addi tional useful in increasing production capacity of existing methanol plants based on two step reforming in the produc- tion of methanol synthesis gas or other methanol plants where the reforming section generates a synthesis gas close to stoichiometric M about 2.
  • a further aspect of the invention is a method for revamping methanol synthesis gas plant, comprising adding a steam reformer in parallel to an existing two- step reforming section;

Landscapes

  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Health & Medical Sciences (AREA)
  • General Health & Medical Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Combustion & Propulsion (AREA)
  • Inorganic Chemistry (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
  • Hydrogen, Water And Hydrids (AREA)

Abstract

Method for the preparation of methanol synthesis gas combining two-step reforming and steam reforming of a carbon dioxide containing feed in parallel.5

Description

Title: Method for the preparation of methanol synthesis gas
The present application is directed to the preparation of methanol synthesis gas. More particular, the invention com bines two-step reforming and steam reforming in parallel.
Production of synthesis gas e.g. for the methanol synthesis with natural gas feed is typically carried out by steam re- forming or a combination of steam reforming and oxygen re forming .
The principal reaction of steam reforming is (given for me thane) :
CH4 + H20 ¾ 3H2 + CO
And oxygen reforming (given for methane) :
CH4 + ½02 ¾ 2¾ + CO
Similar reactions occur for other hydrocarbons. Any reform ing is normally accompanied by the water gas shift reac tion :
CO + ¾0 ¾ C02 + H2
Performing steam reforming, also known as SMR, and oxygen reforming, also known as autothermal reforming or in short ATR, in series is known as two-step reforming. More details of steam reforming and 2-step reforming can be found in the literature.
The product gas from 2-step reforming comprises hydrogen, carbon monoxide, and carbon dioxide as well as other compo nents normally including methane and steam.
Methanol synthesis gas has preferably a composition corre sponding to a so-called module (M= (H2-C02 ) / (C0+C02 ) ) of 1.90-2.20 or more preferably slightly above 2 (eg.2.00-
2.10) .
2-step reforming produces the above mentioned preferred stoichiometric module.
It is an increasing desire in the chemical industry to re duce emission of carbon dioxide and/or to utilize carbon dioxide as feed or a part of the feed in the production of chemical products.
In existing or new methanol plants employing or designed with two-step reforming in the preparation of methanol syn thesis gas, use of carbon dioxide as at least a part of the reforming feed is not an option because two-step reforming produces the stoichiometric correct synthesis gas for the methanol production leaving limited or no possibility for adding carbon dioxide to the reforming process.
We have found a method for the production of methanol syn- thesis gas utilizing carbon dioxide by combining two-step reforming with a steam reforming step arranged in parallel to the two step reforming, where in the parallel steam re forming step carbon dioxide is used as part of the reform ing feed. Thus, this invention provides in one aspect a method for the preparation of a methanol synthesis gas comprising the steps of
(a) providing a first feed comprising hydrocarbons and steam;
(b) providing a second feed comprising hydrocarbons, steam and carbon dioxide;
(c) reforming the first feed in a two step steam reform ing process, to a first synthesis gas comprising hydrogen, carbon monoxide and carbon dioxide having a module M of 2.05 +/- 0.2, where M is (H2-C02 ) / (C0+C02 ) ;
(d) steam reforming the second feed in parallel with the two-step reforming process) in step (c)to a second synthe sis gas comprising hydrogen, carbon monoxide and carbon di oxide; and
(e) employing the first and second synthesis gas in combi nation thereof as feed for methanol synthesis.
The content of carbon dioxide in the second feed is prefer ably controlled to obtain a module M of 1.6 to 2.6, prefer- ably between 1.85 to 2.35, in the second synthesis gas withdrawn from the steam reforming.
As an example, for a natural gas containing only methane, a natural gas/C02 ratio of 3 as feed to a steam reformer will result in a synthesis gas outlet the steam reformer with M = 2 as shown by below two reforming equations take place for methane 3CH4 + 6H20 + C02 ¾ 12H2 + 4C02
3CH4 + 2¾0 + C02 ¾ 8H2 + 4CO
It is further preferred that the methanol synthesis gas ob tained by the method according to the invention has a mod ule M of 1.6 to 2.6, preferably between 1.85 and 2.35.
In an embodiment of the invention the methanol synthesis gas is in a downstream step converted to a methanol prod uct .
The steam reforming in step (d) can be performed in a con ventional tubular reformer, a tubular reformer followed by an adiabatic reformer where carbon dioxide is added before and/or after the tubular reformer, a bayonet type reformer, a convective reformer or a tubular reformer where carbon dioxide is added into the reformer tubes after the feed has initially come into contact with the reforming catalyst.
A suitable reforming catalyst composition for use in the steam reforming depends on the amount of carbon dioxide added to the feed and the type of reformer used in the steam reforming. In most cases, a nickel catalyst is suffi cient, but for high carbon dioxide contents in the feed, noble metal catalysts may be required for some types of steam reformers.
The carbon dioxide for use in the method according to the invention can advantageously be obtained from flue or off- gasses, such as e.g. flue gas stemming from the burners in the steam reformers.
Depending on the feed composition it might be preferred to desulfurize the first feed upstream the two-step reforming and/or the second feed upstream the steam reforming.
An advantage of the method according to the invention is i.a. a reduced energy consumption and a reduced CO2 foot- print.
As already mentioned hereinbefore, the invention is addi tional useful in increasing production capacity of existing methanol plants based on two step reforming in the produc- tion of methanol synthesis gas or other methanol plants where the reforming section generates a synthesis gas close to stoichiometric M about 2.
Accordingly, a further aspect of the invention is a method for revamping methanol synthesis gas plant, comprising adding a steam reformer in parallel to an existing two- step reforming section;
connecting the steam reforming section to a carbon dioxide source; and
connecting an outlet line of the parallel steam reforming section to an outlet line of the existing two-step reform ing section or connecting the outlet line of the parallel steam reforming section to an existing methanol reactor in the methanol synthesis plant.

Claims

Claims
1. A method for the preparation of a methanol synthesis gas comprising the steps of
(a) providing a first feed comprising hydrocarbon and steam;
(b) providing a second feed comprising hydrocarbon, steam and carbon dioxide, where the molecular CCh/hydrocarbon ra- tio is between 0.1 and 0.6, preferably between 0.25 and 0.4
(c) reforming the first feed in a two step steam reforming process to a first synthesis gas comprising hydrogen, car bon monoxide and carbon dioxide and having a module M of 2.05 +/- 0.2, where M is (H2-C02 ) / (C0+C02 ) ;
(d) steam reforming the second feed in parallel with the two-step reforming process in step (c) to a second synthesis gas comprising hydrogen, carbon monoxide and carbon diox ide; and
(e) employing the first and second synthesis gas in combi- nation thereof as feed for methanol synthesis.
2. The method of claim 1, comprising the further step of desulfurizing the first feed upstream the two step steam reforming process.
3. The method of claim 1 or 2, comprising the further step of desulfurizing the second feed upstream the tubular steam reforming.
4. The method of any one of claims 1 to 3, wherein the second synthesis gas has a module M of 1.6 to 2.6, prefera bly between 1.85 to 2.35.
5. The method of any one of claims 1 to 4, wherein the methanol synthesis gas has a module M of 1.9 to 2.2.
6. The method of any one of claim 1 to 4, wherein the carbon dioxide in the second feed is obtained from flue and/or off-gas and/or imported to plant.
7. The method of any one of claims 1 to 6, wherein the steam reforming in step (d) is performed in a standard tub ular reformer, a tubular reformer followed by an adiabatic reformer where carbon dioxide is added before and/or after the tubular reformer, a bayonet type reformer, a convective reformer or a tubular reformer where carbon dioxide is added into the reformer tubes after the feed has ini tially come into contact with the reforming catalyst.
8. The method of any one of claims 1 to 7, wherein the methanol synthesis gas is in a further step converted to a methanol product.
9. A method for revamping methanol synthesis gas plant, comprising
adding a steam reformer in parallel to an existing two-step reforming section;
connecting the steam reforming section to a carbon dioxide source; and
connecting an outlet line of the parallel steam reforming section to an outlet line of the existing two-step reform- ing section or connecting the outlet line of the parallel steam reforming section to an existing methanol reactor in the methanol synthesis plant.
PCT/EP2020/051011 2019-01-18 2020-01-16 Method for the preparation of methanol synthesis gas Ceased WO2020148376A1 (en)

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AU2020208782A AU2020208782B2 (en) 2019-01-18 2020-01-16 Method for the preparation of methanol synthesis gas
CN202080009691.5A CN113329969B (en) 2019-01-18 2020-01-16 Method for preparing methanol synthesis gas

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DKPA201900073 2019-01-18

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AR (2) AR117826A1 (en)
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Publication number Priority date Publication date Assignee Title
EP4277886A4 (en) * 2021-01-14 2025-01-15 BD Energy Systems, LLC LOW CO2 EMISSION METHANOL PRODUCTION PROCESS AND PRODUCTION DEVICE
EP4277729A4 (en) 2021-01-14 2024-12-18 BD Energy Systems, LLC Method and apparatus for improved efficiency and flue gas scrubbing in a fired heater using a condensing convection section
WO2026002653A1 (en) 2024-06-27 2026-01-02 Casale Sa Method for revamping a methanol plant and process for synthesis of methanol

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Publication number Publication date
AR117826A1 (en) 2021-08-25
AU2020208917A1 (en) 2021-06-17
AR117827A1 (en) 2021-08-25
CN113677653A (en) 2021-11-19
AU2020208917B2 (en) 2025-06-26
AU2020208782B2 (en) 2025-07-24
AU2020208782A1 (en) 2021-06-10
CN113329969A (en) 2021-08-31
CN113329969B (en) 2025-02-11
WO2020148378A1 (en) 2020-07-23

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