CN113329969A - 制备甲醇合成气的方法 - Google Patents
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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 27
- 238000003786 synthesis reaction Methods 0.000 title claims abstract description 27
- 238000000034 method Methods 0.000 title claims abstract description 21
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 claims abstract description 55
- 229910002092 carbon dioxide Inorganic materials 0.000 claims abstract description 33
- 239000001569 carbon dioxide Substances 0.000 claims abstract description 26
- 238000002407 reforming Methods 0.000 claims abstract description 23
- 238000000629 steam reforming Methods 0.000 claims abstract description 23
- 238000002360 preparation method Methods 0.000 claims abstract description 4
- 239000007789 gas Substances 0.000 claims description 23
- 238000006243 chemical reaction Methods 0.000 claims description 9
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 claims description 8
- 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
- 239000003546 flue gas Substances 0.000 claims description 3
- 238000009420 retrofitting Methods 0.000 claims description 2
- 239000004215 Carbon black (E152) Substances 0.000 claims 1
- 230000003009 desulfurizing effect Effects 0.000 claims 1
- 239000002912 waste gas Substances 0.000 claims 1
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 16
- 238000004519 manufacturing process Methods 0.000 description 7
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 3
- 239000000203 mixture Substances 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
- 239000000126 substance Substances 0.000 description 2
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 1
- 238000002453 autothermal reforming Methods 0.000 description 1
- -1 components Chemical compound 0.000 description 1
- 238000005265 energy consumption Methods 0.000 description 1
- 239000010970 precious metal Substances 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
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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
- C01B3/38—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
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- 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
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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
- 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
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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
- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/06—Integration with other chemical processes
- C01B2203/061—Methanol production
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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
- 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
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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
- 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
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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
- 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
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- 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
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Abstract
制备甲醇合成气的方法，其将含有二氧化碳的进料的两步转化和蒸汽转化平行组合。
Description
本申请涉及甲醇合成气的制备。更特别地，本发明将两步转化与蒸汽转化平行组合。
通常通过蒸汽转化或蒸汽转化与氧气转化的组合来进行利用天然气进料对合成气(例如用于甲醇合成)的生产。
蒸汽转化的主要反应(针对甲烷给出)是：
且氧气转化(针对甲烷给出)：
其它烃发生类似的反应。任何转化通常伴随着水煤气变换反应：
连续实施蒸汽转化(也称为SMR)和氧气转化(也称为自热转化或简称ATR)被称为两步转化。
蒸汽转化和两步转化的更多细节可以在文献中找到。
来自两步转化的产物气体包含氢气、一氧化碳和二氧化碳、以及通常包括甲烷和蒸汽的其它组分。
甲醇合成气优选具有对应于1.90-2.20或更优选略高于2(例如2.00-2.10)的所谓的模数（module）(M=(H2-CO2)/(CO+CO2))的组成。
两步转化产生上述优选的化学计量模数。
在化学工业中，越来越希望减少二氧化碳的排放和/或在化学产品的生产中利用二氧化碳作为进料或一部分的进料。
在甲醇合成气的制备中采用或设计有两步转化的现有甲醇装置或新建甲醇装置中，由于两步转化生产用于甲醇生产的化学计量正确的合成气，使得向转化过程中添加二氧化碳受限制或没有可能，因此不选择使用二氧化碳作为至少一部分的转化进料。
我们已发现了通过将两步转化与平行于该两步转化布置的蒸汽转化步骤组合来利用二氧化碳生产甲醇合成气的方法，其中在平行的蒸汽转化步骤中使用二氧化碳作为一部分的转化进料。
因此，一方面，本发明提供制备甲醇合成气的方法，其包括以下步骤：
(a)提供包含烃和蒸汽的第一进料；
(b)提供包含烃、蒸汽和二氧化碳的第二进料；
(c)在两步蒸汽转化过程中将第一进料转化为包含氢气、一氧化碳和二氧化碳，模数M为2.05 +/- 0.2的第一合成气，其中模数M为(H2-CO2)/(CO+CO2)；
(d)与步骤(c)中的两步转化过程平行地将第二进料蒸汽转化为包含氢气、一氧化碳和二氧化碳的第二合成气；和
(e)采用第一合成气和第二合成气的组合作为甲醇合成的进料。
优选控制第二进料中二氧化碳的含量，以在从蒸汽转化排出的第二合成气中获得1.6至2.6，优选介于1.85至2.35之间的模数M。
作为实例，对于仅含有甲烷的天然气，作为蒸汽转化器的进料的天然气/CO2比率为3，这将导致M = 2的合成气离开蒸汽转化器，如以下所示，对于甲烷发生两个转化方程：
进一步优选的是，通过根据本发明的方法获得的甲醇合成气的模数M为1.6至2.6，优选介于1.85和2.35之间。
在本发明的一种实施方案中，在下游步骤中将甲醇合成气转化为甲醇产物。
可以在常规的管式转化器、后面有绝热转化器的管式转化器（其中在管式转化器之前和/或之后添加二氧化碳）、插管式（bayonet type）转化器、对流转化器或管式转化器（其中在进料开始与转化催化剂接触之后，将二氧化碳添加入转化器管中）中实施步骤(d)中的蒸汽转化。
用于在蒸汽转化中使用的合适的转化催化剂组合物取决于添加到进料中的二氧化碳的量和在蒸汽转化中使用的转化器的类型。在大多数情况下，镍催化剂是足够的，但是由于进料中二氧化碳含量高，一些类型的蒸汽转化器可能需要贵金属催化剂。
用于在根据本发明的方法中使用的二氧化碳可以有利地获得自烟道气或废气，例如源自蒸汽转化器中的燃烧器的烟道气。
取决于进料组成，可能优选在两步转化的上游将第一进料脱硫且/或在蒸汽转化的上游将第二进料脱硫。
根据本发明的方法的优点尤其是：减少了能量消耗并减少了二氧化碳足迹(footprint)。
如上文已经提及的，本发明另外可用于提高甲醇合成气的生产中基于两步转化的现有甲醇装置的生产能力或其中转化段产生接近于大约2的化学计量M的合成气的其它甲醇装置的生产能力。
因此，本发明的另外方面是改造甲醇合成气装置的方法，其包括：
添加平行于现有的两步转化段的蒸汽转化器；
将蒸汽转化段与二氧化碳源连接；和
将平行蒸汽转化段的出口管线与现有的两步转化段的出口管线连接，或者将平行蒸汽转化段的出口管线与甲醇合成装置中的现有甲醇反应器连接。
Claims (9)
1.制备甲醇合成气的方法，其包括以下步骤：
(a)提供包含烃和蒸汽的第一进料；
(b)提供包含烃、蒸汽和二氧化碳的第二进料，其中分子CO2/烃比率介于0.1和0.6之间，优选介于0.25和0.4之间；
(c)在两步蒸汽转化过程中将所述第一进料转化为包含氢气、一氧化碳和二氧化碳且模数M为2.05 +/- 0.2的第一合成气，其中M为(H2-CO2)/(CO+CO2)；
(d)与步骤(c)中的所述两步转化过程平行地将所述第二进料蒸汽转化为包含氢气、一氧化碳和二氧化碳的第二合成气；和
(e)采用所述第一合成气和所述第二合成气的组合作为甲醇合成的进料。
2.权利要求1所述的方法，其包括在所述两步蒸汽转化过程的上游将所述第一进料脱硫的另外步骤。
3.权利要求1或2所述的方法，其包括在管式蒸汽转化的上游将所述第二进料脱硫的另外步骤。
4.权利要求1至3中任一项所述的方法，其中所述第二合成气的模数M为1.6至2.6，优选介于1.85和2.35之间。
5.权利要求1至4中任一项所述的方法，其中所述甲醇合成气的模数M为1.9至2.2。
6.权利要求1至4中任一项所述的方法，其中所述第二进料中的二氧化碳获得自烟道气和/或废气且/或被输入到装置。
7.权利要求1至6中任一项所述的方法，其中在以下转化器中实施步骤(d)中的所述蒸汽转化：标准管式转化器；后面有绝热转化器的管式转化器，其中在所述管式转化器之前和/或之后添加二氧化碳；插管式转化器；对流转化器或管式转化器，其中在进料开始与转化催化剂接触之后将二氧化碳添加入转化器管中。
8.权利要求1至7中任一项所述的方法，其中在另外步骤中将所述甲醇合成气转化为甲醇产物。
9.改造甲醇合成气装置的方法，其包括：
添加平行于现有的两步转化段的蒸汽转化器；
将蒸汽转化段与二氧化碳源连接；和
将平行蒸汽转化段的出口管线与所述现有的两步转化段的出口管线连接，或者将平行蒸汽转化段的出口管线与所述甲醇合成装置中的现有甲醇反应器连接。
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| Application Number | Priority Date | Filing Date | Title |
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| 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 |
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| CN1071141A (zh) * | 1991-07-09 | 1993-04-21 | 帝国化学工业公司 | 合成气的生产方法 |
| CN105377798A (zh) * | 2013-04-26 | 2016-03-02 | 普莱克斯技术有限公司 | 使用基于氧转运膜的重整系统生产甲醇的方法和系统 |
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| US20160318824A1 (en) * | 2015-05-01 | 2016-11-03 | Velocys Technologies, Ltd. | Process for operating an integrated gas-to-liquids facility |
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| EA026825B1 (ru) * | 2011-10-26 | 2017-05-31 | Стамикарбон Б.В. Эктин Андер Те Нейм Оф Мт Инновейшн Сентр | Способ получения синтез-газа для производства метанола |
| DE102012112705A1 (de) * | 2012-12-20 | 2014-06-26 | L'Air Liquide, Société Anonyme pour l'Etude et l'Exploitation des Procédés Georges Claude | Verfahren zur Herstellung von Methanol aus Kohlendioxid |
| WO2016083434A1 (en) * | 2014-11-25 | 2016-06-02 | Haldor Topsøe A/S | A process for generation of synthesis gas by flue gas recycle |
| ES2961463T3 (es) * | 2017-07-25 | 2024-03-12 | Topsoe As | Método para la preparación de gas de síntesis |
| KR102596309B1 (ko) * | 2017-07-25 | 2023-10-31 | 토프쉐 에이/에스 | 합성 가스의 제조 방법 |
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| US20160318824A1 (en) * | 2015-05-01 | 2016-11-03 | Velocys Technologies, Ltd. | Process for operating an integrated gas-to-liquids facility |
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| Title |
|---|
| ROSTRUPNIELSEN, JR: "PRODUCTION OF SYNTHESIS GAS", 《CATALYSIS TODAY》, vol. 18, no. 4, pages 305 - 324 * |
| ROSTRUPNIELSEN, JR: "PRODUCTION OF SYNTHESIS GAS", CATALYSIS TODAY, vol. 18, no. 4, pages 305 - 324 * |
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| Publication number | Publication date |
|---|---|
| AU2020208917A1 (en) | 2021-06-17 |
| AU2020208782A1 (en) | 2021-06-10 |
| WO2020148376A1 (en) | 2020-07-23 |
| CN113677653A (zh) | 2021-11-19 |
| AR117826A1 (es) | 2021-08-25 |
| AR117827A1 (es) | 2021-08-25 |
| WO2020148378A1 (en) | 2020-07-23 |
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