CN110944938A - 用于制备合成气的方法 - Google Patents
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- 230000015572 biosynthetic process Effects 0.000 title claims abstract description 25
- 238000003786 synthesis reaction Methods 0.000 title claims abstract description 25
- 238000000034 method Methods 0.000 title claims abstract description 11
- 238000002453 autothermal reforming Methods 0.000 claims abstract description 32
- 239000004215 Carbon black (E152) Substances 0.000 claims abstract description 31
- 229930195733 hydrocarbon Natural products 0.000 claims abstract description 31
- 150000002430 hydrocarbons Chemical class 0.000 claims abstract description 31
- 238000005868 electrolysis reaction Methods 0.000 claims abstract description 12
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 9
- 239000007789 gas Substances 0.000 claims description 73
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 claims description 24
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 claims description 20
- 238000000629 steam reforming Methods 0.000 claims description 20
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 claims description 16
- 229910052739 hydrogen Inorganic materials 0.000 claims description 15
- 239000001257 hydrogen Substances 0.000 claims description 15
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims description 13
- 229910002092 carbon dioxide Inorganic materials 0.000 claims description 13
- 239000001569 carbon dioxide Substances 0.000 claims description 9
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 6
- 239000001301 oxygen Substances 0.000 claims description 6
- 229910052760 oxygen Inorganic materials 0.000 claims description 6
- 239000000203 mixture Substances 0.000 claims description 5
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 claims description 4
- 229910002091 carbon monoxide Inorganic materials 0.000 claims description 3
- 150000002431 hydrogen Chemical class 0.000 claims description 3
- 239000003345 natural gas Substances 0.000 claims description 3
- 238000011144 upstream manufacturing Methods 0.000 claims description 3
- WWYNJERNGUHSAO-XUDSTZEESA-N (+)-Norgestrel Chemical compound O=C1CC[C@@H]2[C@H]3CC[C@](CC)([C@](CC4)(O)C#C)[C@@H]4[C@@H]3CCC2=C1 WWYNJERNGUHSAO-XUDSTZEESA-N 0.000 claims description 2
- 238000002156 mixing Methods 0.000 claims description 2
- 238000002407 reforming Methods 0.000 abstract description 10
- 238000004519 manufacturing process Methods 0.000 abstract description 8
- 239000003054 catalyst Substances 0.000 description 4
- 238000006243 chemical reaction Methods 0.000 description 4
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 2
- 229910052799 carbon Inorganic materials 0.000 description 2
- 238000002485 combustion reaction Methods 0.000 description 2
- 229910002090 carbon oxide Inorganic materials 0.000 description 1
- 238000006555 catalytic reaction Methods 0.000 description 1
- -1 components Chemical compound 0.000 description 1
- 238000006477 desulfuration reaction Methods 0.000 description 1
- 230000023556 desulfurization Effects 0.000 description 1
- 239000012528 membrane Substances 0.000 description 1
- 239000005518 polymer electrolyte Substances 0.000 description 1
- 238000002360 preparation method Methods 0.000 description 1
- 238000010926 purge Methods 0.000 description 1
- 238000000746 purification Methods 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
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Abstract
本发明涉及通过将水的电解、烃原料的自热重整和热交换重整相结合来制备合成气的方法。
Description
本申请涉及合成气的制备。更具体地，本发明在制备含有氢气和碳氧化物的合成气时结合了水的电解、烃原料的自热重整和热交换重整。
用天然气进料生产例如用于甲醇合成的合成气通常通过蒸汽重整进行。
蒸汽重整的主要反应是(针对甲烷)：
蒸汽重整通常伴随着水煤气变换反应：
蒸汽重整可以例如通过管式重整器(也称为蒸汽甲烷重整器，SMR)和自热重整(ATR)的组合来完成，其也称为一次和二次重整或两步重整。或者，可以使用独立的SMR或独立的ATR来制备合成气。
ATR反应器的主要元件是包含在耐火衬里压力壳内的燃烧器、燃烧室和催化剂床。在ATR反应器中，亚化学计量量的氧气使烃进料进行部分氧化或燃烧，然后在蒸汽重整催化剂的固定床中发生部分燃烧的烃进料流的蒸汽重整。由于高温，在燃烧室中也发生一定程度的蒸汽重整。蒸汽重整反应伴随着水煤气变换反应。通常，就蒸汽重整和水煤气变换反应而言，气体在ATR反应器出口处处于平衡或接近平衡。出口气体的温度通常为850至1100℃。ATR的更多细节和完整描述可以在现有技术中找到，例如“Studies in Surface Scienceand Catalysis,Vol.152,“Synthesis gas production for FT synthesis”；Chapter 4,p.258-352,2004”。
无论使用独立的SMR、两步重整还是独立的ATR，产品气体都将包含氢气、一氧化碳和二氧化碳以及通常包括甲烷和蒸汽的其他组分。
甲醇合成气优选的组成对应于所谓的模数(M＝(H2-CO2)/(CO+CO2))为1.90-2.20或更优选略高于2(例如2.00-2.10)。
对于独立的ATR，ATR出口气体中的模数通常低于当合成气用于甲醇生产时的期望值。这可以例如通过从来自甲醇合成回路的吹扫气中除去二氧化碳或回收氢气来进行纠正。在这两种情况下，甲醇回路效率均低于如果用于甲醇回路的合成气具有如上所述的略高于2的模数时所获得的效率。
此外，可以通过与ATR串联或并联布置的热交换重整器来补充ATR。
在串联方案中，将一部分或全部烃原料引导至其中发生蒸汽重整的热交换重整器。剩余部分的烃原料可以绕过热交换重整器，并被引导至自热重整器。通常，离开串联连接的热交换重整器的气体将在650-800℃的温度下处于平衡或接近平衡。然后将来自串联连接的热交换重整器的出口气体与未在热交换重整器中进行蒸汽重整的任何烃进料一起引导至ATR。一部分或全部的来自ATR的出口气体在热交换重整器中用作热源，其通过热交换驱动吸热的蒸汽重整反应。
在热交换重整器的并联方案中，将一部分烃原料引导至ATR，并且将剩余的烃原料和/或第二烃原料引导至热交换重整器。
引导至ATR和热交换重整器的原料可以具有不同的组成，例如不同的蒸汽/碳比。
在并联概念的热交换重整器中，进行蒸汽重整。一部分或全部的来自ATR的出口气体在热交换重整器中用作热源，其通过热交换驱动吸热的蒸汽重整反应。
在热交换重整器中离开催化剂的气体可以任选地与一部分或全部的来自ATR的出口气体混合，然后将后者用作热源。或者，可以将来自热交换重整器的出口气体和来自ATR的出口气体在热交换重整器的下游进行混合。
热交换重整器可替代地被称为气体加热重整器，而热交换重整可以被称为气体加热重整。
我们已经发现，当将热交换重整、ATR与水和/或蒸汽的电解结合在一起时，昂贵的ASU在合成气的制备中将是多余的。
因此，本发明提供了一种用于制备合成气的方法，其包括以下步骤：
(a)通过水和/或蒸汽的电解来制备单独的含氢气的流和单独的含氧气的流；
(b)提供烃原料；
(c1)将与一部分或全部的离开步骤(d)的经自热重整的气体为间接传热关系的一部分来自步骤(b)的烃原料和/或第二烃原料进行蒸汽重整，并且将经热交换蒸汽重整的气流与步骤(d)下游的经自热重整的气体混合；或者
(c2)将与一部分或全部的离开步骤(d)的经自热重整的气体为间接传热关系的一部分或全部的来自步骤(b)的烃原料热交换蒸汽重整为经热交换蒸汽重整的气体，并将所述经热交换蒸汽重整的气体引入到步骤(d)中的自热重整器中；
(d)通过用至少一部分来自步骤(a)的单独的含氧气的流使至少一部分来自步骤(b)的烃原料或至少一部分来自步骤(c2)的经热交换蒸汽重整的气体进行自热重整，在自热重整器中提供用于步骤(c1)或步骤(c2)的经自热重整的气体；
(e)将至少一部分来自步骤(a)的单独的含氢气的流引入到步骤(c1)下游的混合的经热交换重整的气体和经自热重整的气体中，或引入到步骤(c2)下游的经自热重整的气体中，以获得包含氢气、一氧化碳和二氧化碳的合成气；
(f)取出合成气。
在串联的热交换方案中，将一部分或全部烃原料引导至其中进行蒸汽重整的热交换重整器。烃原料的剩余部分可以绕过热交换重整器并被引导至自热重整器。
通常，离开串联的热交换重整器的气体在550-800℃的温度下将处于平衡或接近平衡。然后将来自串联的热交换重整器的出口气体引导至ATR。一部分或全部的来自ATR的出口气体通过热交换被用作热交换重整器中的热源，以驱动吸热的蒸汽重整反应。
在热交换重整器的并联方案中，将一部分烃原料和/或第二烃原料引导到ATR，将剩余的烃原料和/或第二烃原料引导到热交换重整器。
在并联概念的热交换重整器中，一部分或全部的来自ATR的出口气体通过热交换被用作热交换重整器中的热源，以驱动吸热的蒸汽重整反应。
离开热交换重整器中的催化剂的气体可以任选地与一部分或全部的来自ATR的出口气体混合，然后将后者用作热源。或者，可以将来自热交换重整器的出口气体和来自ATR的出口气体在热交换重整器的下游混合。
通往ATR和热交换重整器的原料可以具有不同的组成，例如不同的蒸气/碳比。
无论使用热交换重整器的并联还是串联概念，原则上都可以调节运行参数，步骤(e)中添加的来自电解装置的氢气的量以及热交换重整器的设计，以提供为1.9-2.2，优选2.0-2.1的期望值的模数M，特别是当使用合成气制备甲醇时。
通常，适用于本发明的热交换重整器和ATR的原料包括原样的或经预重整和/或脱硫的天然气、甲烷、LNG、石脑油或它们的混合物。
可以调节氢气的添加量，使得当氢气与由重整步骤产生的工艺气体混合时，获得期望的M值(在1.90至2.20之间，或者优选地在2.00至2.10之间)。
在一些情况下，来自电解步骤的氢气的量可能太高而不能提供在期望范围内的模数。在这种情况下，一部分氢气可以用于其他方式。
或者，可以通过向烃原料和/或合成气和/或在自热重整器的上游添加基本上纯的二氧化碳，而将模数另外调节至期望的值。
因此，在本发明的一个实施方案中，将基本上纯的二氧化碳添加到自热重整器上游或步骤(c1)或(c2)下游或步骤(d)下游的烃原料中。
在上述所有情况下，原料都可以在初始如上所述进行纯化(包括脱硫)和绝热预重整步骤。
烃原料可进一步包含氢气和/或蒸汽以及其他组分。
可以通过本领域已知的各种方式进行电解，例如通过基于固体氧化物的电解或通过碱性电池或聚合物电池(PEM)进行的电解。
如果用于电解的动力(至少部分地)是由可持续来源产生的，则减少来自装置的每单位所生产的产品的二氧化碳排放。
本发明可进一步用于生产用于其他应用的合成气，其中期望增加进料气中的氢气浓度并且其中通过电解有利地生产制备合成气所需的一部分氧气。
Claims (6)
1.用于制备合成气的方法，其包括以下步骤：
(a)通过水和/或蒸汽的电解来制备单独的含氢气的流和单独的含氧气的流；
(b)提供烃原料；
(c1)将与一部分或全部的离开步骤(d)的经自热重整的气体为间接传热关系的一部分来自步骤(b)的烃原料和/或第二烃原料进行蒸汽重整，并且将经热交换蒸汽重整的气流与步骤(d)下游的经自热重整的气体混合；或者
(c2)将与一部分或全部的离开步骤(d)的经自热重整的气体为间接传热关系的一部分或全部的来自步骤(b)的烃原料热交换蒸汽重整为经热交换蒸汽重整的气体，并将所述经热交换蒸汽重整的气体引入到步骤(d)中的自热重整器中，以获得步骤(c2)中使用的经自热重整的气体；
(d)通过用至少一部分来自步骤(a)的单独的含氧气的流使至少一部分来自步骤(b)的烃原料或至少一部分来自步骤(c2)的经热交换蒸汽重整的气体进行自热重整，在自热重整器中提供用于步骤(c1)或步骤(c2)的经自热重整的气体；
(e)将至少一部分来自步骤(a)的单独的含氢气的流引入到步骤(c1)下游的混合的经热交换重整的气体和经自热重整的气体中，或引入到步骤(d)下游的经自热重整的气体中，以获得包含氢气、一氧化碳和二氧化碳的合成气；
(f)取出合成气。
2.根据权利要求2所述的方法，其中将基本上纯的二氧化碳添加到自热重整器上游或步骤(c1)或(c2)下游或步骤(d)下游的烃原料中。
3.根据权利要求1或2所述的方法，其中以这样的量添加基本上纯的二氧化碳：其使得在步骤(d)所制备的合成气中，模数M＝(H2-CO2)/(CO+CO2)为1.9至2.2，或优选2至2.1。
4.根据权利要求1至3中任一项所述的方法，其中烃原料包括原样的或经预重整和/或脱硫的天然气、甲烷、LNG、石脑油或它们的混合物。
5.根据权利要求1至4中任一项所述的方法，其中步骤(a)中的水和/或蒸汽的电解至少部分地由可再生能源提供动力。
6.根据权利要求1至5中任一项所述的方法，其中在进一步的步骤中，将步骤(f)中制备的合成气转化为甲醇产物。
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| WO2021083776A1 (en) * | 2019-10-28 | 2021-05-06 | Haldor Topsøe A/S | Green method for the preparation of synthesis gas |
| JP2023515191A (ja) * | 2020-02-28 | 2023-04-12 | トプソー・アクチエゼルスカベット | 合成ガスを製造するための方法 |
| EP3967654A1 (de) * | 2020-09-11 | 2022-03-16 | L'air Liquide, Société Anonyme Pour L'Étude Et L'exploitation Des Procédés Georges Claude | Verfahren und anlage zur herstellung von wasserstoff durch dampfreformierung und hochtemperaturelektrolyse |
| WO2023275049A1 (en) * | 2021-06-29 | 2023-01-05 | Topsoe A/S | Process and plant for producing methane or methanol from a solid renewable feedstock |
| US11649549B1 (en) | 2021-11-11 | 2023-05-16 | Pyrochem Catalyst Company | Oxidative reforming and electrolysis system and process for hydrogen generation |
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| US20200140273A1 (en) | 2020-05-07 |
| KR20200031644A (ko) | 2020-03-24 |
| IL271941A (en) | 2020-02-27 |
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| AU2018308860B2 (en) | 2023-04-27 |
| CA3069262A1 (en) | 2019-01-31 |
| WO2019020519A1 (en) | 2019-01-31 |
| UA127414C2 (uk) | 2023-08-16 |
| ES2960926T3 (es) | 2024-03-07 |
| KR102596309B1 (ko) | 2023-10-31 |
| AU2018308860A1 (en) | 2020-01-23 |
| EP3658496B1 (en) | 2023-08-30 |
| ZA201908217B (en) | 2022-03-30 |
| EP3658496A1 (en) | 2020-06-03 |
| IL271941B2 (en) | 2024-04-01 |
| PL3658496T3 (pl) | 2024-03-11 |
| CL2020000159A1 (es) | 2020-07-31 |
| BR112020001479A2 (pt) | 2020-07-21 |
| IL271941B1 (en) | 2023-12-01 |
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