AU2020208782A1 - Method for the preparation of methanol synthesis gas - Google Patents
Method for the preparation of methanol synthesis gas Download PDFInfo
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- AU2020208782A1 AU2020208782A1 AU2020208782A AU2020208782A AU2020208782A1 AU 2020208782 A1 AU2020208782 A1 AU 2020208782A1 AU 2020208782 A AU2020208782 A AU 2020208782A AU 2020208782 A AU2020208782 A AU 2020208782A AU 2020208782 A1 AU2020208782 A1 AU 2020208782A1
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- Prior art keywords
- feed
- synthesis gas
- reformer
- reforming
- steam
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- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 title claims abstract description 87
- 230000015572 biosynthetic process Effects 0.000 title claims abstract description 33
- 238000003786 synthesis reaction Methods 0.000 title claims abstract description 33
- 238000000034 method Methods 0.000 title claims abstract description 21
- 238000002360 preparation method Methods 0.000 title claims abstract description 7
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 claims abstract description 51
- 229910002092 carbon dioxide Inorganic materials 0.000 claims abstract description 35
- 238000002407 reforming Methods 0.000 claims abstract description 31
- 238000000629 steam reforming Methods 0.000 claims abstract description 25
- 239000001569 carbon dioxide Substances 0.000 claims abstract description 24
- 239000007789 gas Substances 0.000 claims description 29
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 claims description 6
- 229930195733 hydrocarbon Natural products 0.000 claims description 6
- 150000002430 hydrocarbons Chemical class 0.000 claims description 6
- 229910002091 carbon monoxide Inorganic materials 0.000 claims description 5
- 239000001257 hydrogen Substances 0.000 claims description 5
- 229910052739 hydrogen Inorganic materials 0.000 claims description 5
- 125000004435 hydrogen atom Chemical class [H]* 0.000 claims description 5
- 239000003054 catalyst Substances 0.000 claims description 4
- 238000011144 upstream manufacturing Methods 0.000 claims description 4
- 229940000425 combination drug Drugs 0.000 claims description 2
- 229960004424 carbon dioxide Drugs 0.000 claims 7
- 239000004215 Carbon black (E152) Substances 0.000 claims 3
- 229940105305 carbon monoxide Drugs 0.000 claims 2
- 230000003009 desulfurizing effect Effects 0.000 claims 2
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 16
- 238000004519 manufacturing process Methods 0.000 description 6
- 241000196324 Embryophyta Species 0.000 description 5
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 3
- 238000006243 chemical reaction Methods 0.000 description 3
- 239000003345 natural gas Substances 0.000 description 3
- 239000001301 oxygen Substances 0.000 description 3
- 229910052760 oxygen Inorganic materials 0.000 description 3
- 239000000047 product Substances 0.000 description 3
- 239000000126 substance Substances 0.000 description 2
- 235000008694 Humulus lupulus Nutrition 0.000 description 1
- 244000025221 Humulus lupulus Species 0.000 description 1
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 1
- 230000002730 additional effect Effects 0.000 description 1
- 238000002453 autothermal reforming Methods 0.000 description 1
- 239000000306 component Substances 0.000 description 1
- 230000000875 corresponding effect Effects 0.000 description 1
- 238000005265 energy consumption Methods 0.000 description 1
- 239000003546 flue gas Substances 0.000 description 1
- 229910000510 noble metal Inorganic materials 0.000 description 1
- 230000036647 reaction Effects 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
Classifications
-
- 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
- C01B3/38—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 catalysts
- C01B3/382—Multi-step processes
-
- 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
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- 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)
- Hydrogen, Water And Hydrids (AREA)
- Organic Low-Molecular-Weight Compounds And Preparation Thereof (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 (9)
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.
Applications Claiming Priority (3)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| DKPA201900073 | 2019-01-18 | ||
| DKPA201900073 | 2019-01-18 | ||
| PCT/EP2020/051011 WO2020148376A1 (en) | 2019-01-18 | 2020-01-16 | Method for the preparation of methanol synthesis gas |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| AU2020208782A1 true AU2020208782A1 (en) | 2021-06-10 |
Family
ID=69174499
Family Applications (2)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| AU2020208782A Pending AU2020208782A1 (en) | 2019-01-18 | 2020-01-16 | Method for the preparation of methanol synthesis gas |
| AU2020208917A Pending AU2020208917A1 (en) | 2019-01-18 | 2020-01-16 | Method for the preparation of methanol synthesis gas |
Family Applications After (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| AU2020208917A Pending AU2020208917A1 (en) | 2019-01-18 | 2020-01-16 | Method for the preparation of methanol synthesis gas |
Country Status (4)
| Country | Link |
|---|---|
| CN (2) | CN113677653A (en) |
| AR (2) | AR117826A1 (en) |
| AU (2) | AU2020208782A1 (en) |
| WO (2) | WO2020148378A1 (en) |
Families Citing this family (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2022155425A1 (en) * | 2021-01-14 | 2022-07-21 | Bd Energy Systems, Llc | Low co2 emissions methanol process and production apparatus |
Family Cites Families (12)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1033267C (en) * | 1991-07-09 | 1996-11-13 | 帝国化学工业公司 | Synthesis gas production |
| GB9817526D0 (en) * | 1998-08-13 | 1998-10-07 | Ici Plc | Steam reforming |
| CA2357527C (en) * | 2001-10-01 | 2009-12-01 | Technology Convergence Inc. | Methanol recycle stream |
| WO2013013895A1 (en) * | 2011-07-25 | 2013-01-31 | Haldor Topsøe A/S | Process for production of synthesis gas |
| CN103889891B (en) * | 2011-10-26 | 2016-09-14 | 代表Mt创新中心的斯塔米卡邦有限公司 | Produce the method being used for producing the synthesis gas of methanol |
| DE102012112705A1 (en) * | 2012-12-20 | 2014-06-26 | L'Air Liquide, Société Anonyme pour l'Etude et l'Exploitation des Procédés Georges Claude | Process for producing methanol from carbon dioxide |
| US9115045B2 (en) * | 2013-04-26 | 2015-08-25 | Praxair Technology, Inc. | Method and system for producing methanol using an oxygen transport membrane based reforming system |
| EA201791153A1 (en) * | 2014-11-25 | 2017-11-30 | Хальдор Топсёэ А/С | METHOD FOR OBTAINING SYNTHESIS-GAS THROUGH THE RECYCLING OF GAS COMBUSTION PRODUCTS |
| US9637432B2 (en) * | 2014-12-17 | 2017-05-02 | Praxair Technology, Inc. | Method and system for producing methanol using partial oxidation |
| US9725385B2 (en) * | 2015-05-01 | 2017-08-08 | Velocys Technologies, Ltd. | Process for operating an integrated gas-to-liquids facility |
| CA3069262A1 (en) * | 2017-07-25 | 2019-01-31 | Haldor Topsoe A/S | Method for the preparation of synthesis gas |
| EP3658495B1 (en) * | 2017-07-25 | 2023-08-30 | Topsoe A/S | Method for the preparation of synthesis gas |
-
2020
- 2020-01-16 AU AU2020208782A patent/AU2020208782A1/en active Pending
- 2020-01-16 AU AU2020208917A patent/AU2020208917A1/en active Pending
- 2020-01-16 WO PCT/EP2020/051014 patent/WO2020148378A1/en active Application Filing
- 2020-01-16 AR ARP200100114A patent/AR117826A1/en unknown
- 2020-01-16 CN CN202080009622.4A patent/CN113677653A/en active Pending
- 2020-01-16 AR ARP200100115A patent/AR117827A1/en unknown
- 2020-01-16 CN CN202080009691.5A patent/CN113329969A/en active Pending
- 2020-01-16 WO PCT/EP2020/051011 patent/WO2020148376A1/en active Application Filing
Also Published As
| Publication number | Publication date |
|---|---|
| WO2020148376A1 (en) | 2020-07-23 |
| WO2020148378A1 (en) | 2020-07-23 |
| AU2020208917A1 (en) | 2021-06-17 |
| AR117826A1 (en) | 2021-08-25 |
| AR117827A1 (en) | 2021-08-25 |
| CN113329969A (en) | 2021-08-31 |
| CN113677653A (en) | 2021-11-19 |
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