CN106660789A - 生产合成气物流的方法 - Google Patents
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Abstract
本发明提供一种生产合成气物流的方法,所述方法至少包括如下步骤:(a)提供含烃物流;(b)提供温度至少1000℃的含热固体物质的反应器;(c)在步骤(b)提供的含热固体物质的反应器中使步骤(a)提供的含烃物流裂化,从而至少获得C和H2;(d)从反应器中脱除含H2物流;(e)以大于0的H2O/CO2体积进料比在反应器中使步骤(c)获得的C转化,从而获得含CO/H2的物流;(f)从反应器中脱除含CO/H2的物流;(g)将步骤(d)脱除的含H2物流与步骤(f)脱除的含CO/H2物流组合,从而获得合成气物流。
Description
本发明涉及一种生产合成气物流的方法,特别是一种非催化方法。生产合成气物流的各种方法在本领域中是已知的。
在GB 2 265 382中公开了生产合成气的非催化方法的一个例子。
在GB 2 265 382中公开的方法的问题是所生产的合成气中H2与CO的比是固定的(3:1,即H2/CO的体积比为3.0)。该固定的H2/CO体积比不总是适合后续的处理如费-托反应。
GB 365 912(公开于1932年1月)涉及通过使烃通过固体燃料如煤的点火床层而由烃的干馏分解生产富氢可燃气。在本实施例中应用的通过燃料床的天然气含17.6%的C2H6、75.0%的CH4、0.4%的CO2、0.2%的O2和6.8%的N2,但不含硫醇。另外,使固体燃料床层点火燃烧以提供用于烃干馏分解的热。这意味着将消耗燃料床,并且当其不能提供烃分解所需的热时要进行更换。
EP 0 219 163 A2(公开于1987年4月)涉及一种生产含氢气体的方法,所述方法包括如下步骤:
(i)在不存在蒸汽的情况下通过与非流化的热固体物质接触而使含烃物质主要裂化为碳和含氢气体,并允许碳沉积在固体上;和
(ii)蒸汽气化在步骤(i)中形成的碳。
EP 0 219 163建议在将天然气用作方法的原料之前对其进行处理以脱除硫和/或无机物质。在EP 0 219 163中没有具体提到硫醇。另外,也没有提到在蒸汽气化步骤中应用任何二氧化碳将所形成的碳转化为一氧化碳。
本发明的一个目的是克服或减小在所产生的合成气中H2与CO固定比的问题,从而对于进一步处理如在费-托反应中有更多的选择。更一般地,本发明的一个目的是提供生产合成气物流的一种替代方法,特别是非催化方法,所述方法允许在所产生的合成气中获得灵活的H2/CO体积比。
本发明的另一个目的是提供生产合成气物流的一种替代方法,特别是非催化方法,所述方法应用可以长期使用而不消耗的固体物质床层。
本发明的又一个目的是提供一种可以处理含硫醇的含烃物流的方法,所述方法在转化含烃物流为合成气之前不需要进行胺处理或其它分离来脱除硫醇。
一个或多个上述或其它目的可以通过提供生产合成气物流的方法来实现,所述方法至少包括如下步骤:
(a)提供含烃物流;
(b)提供温度至少1000℃的含热固体物质的反应器;
(c)在步骤(b)提供的含热固体物质的反应器中使步骤(a)提供的含烃物流裂化,从而至少获得C和H2;
(d)从反应器中脱除含H2物流;
(e)以大于0的H2O/CO2体积进料比在反应器中使步骤(c)获得的C转化,从而获得含CO/H2的物流;
(f)从反应器中脱除含CO/H2的物流;
(g)将步骤(d)脱除的含H2物流与步骤(f)脱除的含CO/H2物流组合,从而获得合成气物流。
已经令人惊奇地发现本发明方法允许以令人惊奇的简单方式产生H2/CO体积比灵活的合成气物流。本发明的一个重要优点是可以应用CO2生产CO;基于在(裂化)催化剂上的碳形成,通常很难利用例如CH4‘重整’CO2为CO/H2。本发明的另一个优点是裂化不需要应用任何催化剂。其结果是,本发明方法也可以用于含H2S和硫醇化合物的含烃物流(在用于生产合成气的催化方法中通常需要脱除这些硫化物以防止催化剂中毒)。另外,本发明应用的含烃物流中烯烃和类似物的量不是很关键;含烃物流可以含有更多的会导致催化剂中毒的这些物质。另外,步骤(c)的裂化前,不需要昂贵的胺处理单元等来处理步骤(a)提供的物流以脱除任意的硫醇。
本发明的另一个优点是因为不需要高纯O2,因此不需要ASU(空气分离装置);这使得所述方法适合于在小规模操作中施用。
在步骤(a)中,提供含烃物流。这种含烃物流不以任何方式进行限制,和可以为天然气、伴生气、原油等。通常,所述含烃物流为含烃的气体物流,优选含至少30vol%的甲烷。
如上所述,本发明方法适合于包含一些催化方法生产合成气时不希望的杂质的含烃物流。因此,在本发明的优选实施方案中,步骤(a)提供的含烃物流包含至少10ppm的硫醇(例如但不限于甲硫醇(CH3SH)、乙硫醇(C2H5SH)和丙硫醇(C3H7SH)),优选至少为50ppm,更优选至少80ppm。另外,在本发明的另一个实施方案中,步骤(a)提供的含烃物流包含至少1.0vol%、至少2.0vol%、至少3.0vol%或甚至至少5.0vol%的烯烃。
在步骤(b)中,提供温度至少1000℃的含热固体物质的反应器。本领域熟练技术人员很容易理解热固体物质可以在很宽范围内变化。作为一个例子,热固体物质为含任何所需形状和尺寸的耐热固体材料的固定床形式,如颗粒固体的固定砖块基质或填料床。在本发明方法中可以应用各种固体材料;合适的固体材料包括惰性陶瓷材料、耐高温氧化物(如氧化铝、氧化钇、氧化锆)、碳化硅、含碳物质、金属合金和金属化合物等。可以以各种方式使热固体物质温度升高。
在步骤(c)中,在步骤(b)中提供的含热固体物质的反应器中使步骤(a)提供的含烃物流裂化,从而至少获得C(碳)和H2(氢)。通常,步骤(c)获得的C沉积在反应器中的热固体物质上。
优选地,步骤(c)中含热固体物质的反应器处于至少1100℃的温度,优选至少1200℃,更优选至少1350℃,和至多1500℃,优选至多1400℃。通常,步骤(c)中的裂化在压力0.5-50bara下实施,优选为5-20bara。因为本领域熟练技术人员熟悉(非催化)裂化,在这里不再进一步详细讨论。
在步骤(d)中,从反应器中脱除含H2物流。优选地,在步骤(d)中从反应器中脱除的含H2物流包含至少1ppm的H2S,优选为至少2ppm,在步骤(g)中组合前至少部分脱除H2S,从而获得贫含H2S的含H2物流。优选地,所述贫含H2S的含H2物流包含少于0.1ppm的H2S。因为本领域熟练技术人员熟悉从物流中脱除H2S(例如应用分子筛、胺等),在这里不再进一步详细讨论。
另外,优选的是应用步骤(d)中从反应器中脱除的一部分含H2物流加热反应器,例如通过使其燃烧来进行。不用说,步骤(d)中从反应器中脱除的部分含H2物流也可以用于其它用途,如加氢处理、加氢裂化等。
在步骤(e)中,将步骤(c)获得的C在H2O/CO2(水/二氧化碳)体积进料比大于0的情况下在反应器中转化,从而获得含CO/H2的物流。本领域熟练技术人员将会理解在步骤(e)中获得的含CO/H2的物流为合成气物流;但为了不使步骤(e)获得的合成气物流与步骤(g)获得的(富H2)合成气物流混淆,步骤(e)获得的合成气物流在这里称作“含CO/H2的物流”。因为本领域熟练技术人员熟悉步骤(e)中发生的这类转化,在这里不再进一步详细讨论。通常,将含CO2的物流和/或蒸汽进料至反应器以在步骤(e)中获得所需的H2O/CO2体积比;在后一种情况下,H2O/CO2体积比也是H2O/CO2体积进料比。在一个特别优选的实施方案中,使含CO2的物流从工艺装置的其它地方循环或者由附近工艺装置作为废气物流获得;这有利地降低了总CO2排放量。替代或附加地,步骤(a)中提供的含烃物流包含CO2。
优选地,含热固体物质的反应器在步骤(e)中的温度为至少1000℃,优选至少1100℃,更优选至少1200℃,和至多1500℃,优选至多1400℃。另外,步骤(e)中的转化在压力0.5-50bara下实施,优选5-20bara。
另外,优选的是在步骤(e)中,将步骤(c)获得的C在反应器中在H2O/CO2体积进料比为至少0.0001下转化,所述体积进料比优选至少0.001、更优选至少0.5、甚至更优选至少0.9、仍甚至更优选至少1.2,和至多1000、优选至多100、更优选至多10、甚至更优选至多3.0、仍甚至更优选至多2.5和最优选至多2.2。优选地,在步骤(e)中使步骤(c)获得的C与蒸汽接触。
在步骤(f)中,从反应器中脱除含CO/H2的物流。
在步骤(g)中,使步骤(d)脱除的含H2物流与步骤(f)脱除的含CO/H2物流组合,从而获得合成气物流。通常,步骤(g)获得的合成气物流的H2/CO体积比为0.5-5.0,优选大于0.9和低于3.5。优选地,步骤(g)获得的合成气物流的H2/CO体积比为至少1.0和低于3.1,优选为至少1.6,更优选至少1.75,和优选至多2.2,更优选至多2.05。
下面通过如下非限定性实施例进一步描述本发明。
实施例
在这些计算实施例(应用由Outokumpu Research OY,Pori,Finland获得的HSC化学软件)中,应用含甲烷、氮气、0.01vol%(即100ppm)甲硫醇(CH3SH;通常在天然气中存在的硫醇)和0.01vol%(即100ppm)乙硫醇(C2H5SH)的天然气进料物流。
将上述天然气进料物流在含热固体物质的反应器中在高温下裂化,从而获得C(沉积在热固体物质上)和H2。从反应器中脱除含H2物流,并经受胺处理以脱除H2S(在反应器中通过转化CH3SH和C2H5SH为H2S、H2和C形成)。
上述天然气原料物流和所脱除的含H2物流的组成以及裂化条件在下表1中针对实施例1-8给出。
将所获得的C(作为热固体物质上的沉积物)在反应器中在具体的H2O/CO2体积比(通过注入CO2和H2O进行调节)下转化,从而获得含CO/H2的物流,随后从反应器中脱除该物流。随后将含CO/H2的物流与含H2的物流(参考表1)组合,从而获得合成气物流。在这些计算实施例中,假定这种含H2的物流包含约99vol%的H2。合成气物流的H2/CO体积比在下表2中给出。
下表2列出了一些实施例(实施例9-20),其中在反应器中利用不同的转化条件和/或待进料和待转化的物流的H2O/CO2体积进料比(通过H2O和CO2注入调节)。
本领域熟练技术人员将会很容易理解在不偏离本发明范围的情况下可以作许多调整。
Claims (10)
1.一种生产合成气物流的方法,所述方法至少包括如下步骤:
(a)提供含烃物流;
(b)提供温度至少1000℃的含热固体物质的反应器;
(c)在步骤(b)提供的含热固体物质的反应器中使步骤(a)提供的含烃物流裂化,从而至少获得C和H2;
(d)从反应器中脱除含H2物流;
(e)以大于0的H2O/CO2体积进料比在反应器中使步骤(c)获得的C转化,从而获得含CO/H2的物流;
(f)从反应器中脱除含CO/H2的物流;
(g)将步骤(d)脱除的含H2物流与步骤(f)脱除的含CO/H2物流组合,从而获得合成气物流。
2.权利要求1的方法,其中步骤(a)提供的含烃物流包含至少10ppm的硫醇,优选至少50ppm的硫醇,更优选至少80ppm。
3.权利要求1或2的方法,其中步骤(a)提供的含烃物流包含至少1.0vol%、至少2.0vol%、至少3.0vol%或甚至至少5.0vol%的烯烃。
4.前述权利要求任一项的方法,其中步骤(c)中含热固体物质的反应器处于至少1100℃的温度,优选至少1200℃,更优选至少1350℃,和至多1500℃,优选至多1400℃。
5.前述权利要求任一项的方法,其中步骤(d)中从反应器中脱除的含H2物流包含至少1ppm的H2S,优选至少2ppm,在步骤(g)中组合前至少部分脱除H2S。
6.前述权利要求任一项的方法,其中步骤(d)中从反应器中脱除的含H2物流的一部分用于加热反应器。
7.前述权利要求任一项的方法,其中步骤(e)中含热固体物质的反应器处于至少1000℃的温度,优选至少1100℃,更优选至少1200℃,和至多1500℃,优选至多1400℃。
8.前述权利要求任一项的方法,其中步骤(e)中在反应器中在H2O/CO2体积进料比为至少0.0001、优选至少0.9、更优选至少1.2和至多1000、优选至多3.0、更优选至多2.2下使步骤(c)获得的C转化。
9.前述权利要求任一项的方法,其中在步骤(e)中使步骤(c)获得的C与蒸汽接触。
10.前述权利要求任一项的方法,其中步骤(g)获得的合成气物流的H2/CO体积比为至少1.0和低于3.1,优选为至少1.6,更优选为至少1.75,和优选至多2.2,更优选至多2.05。
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PCT/EP2015/065332 WO2016005317A1 (en) | 2014-07-08 | 2015-07-06 | A method for producing a syngas stream |
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EP (1) | EP3166884B1 (zh) |
CN (1) | CN106660789B (zh) |
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GB365912A (en) * | 1930-04-30 | 1932-01-28 | Humphreys & Glasgow Ltd | Improvements in or relating to the manufacture of combustible gas rich in hydrogen |
US3864460A (en) * | 1973-07-12 | 1975-02-04 | Nrg Inc | Method for removing hydrogen sulfide from hydrocarbon gas streams without pollution of the atmosphere |
EP0219163A2 (en) * | 1985-10-09 | 1987-04-22 | Shell Internationale Researchmaatschappij B.V. | Process and apparatus for producing a hydrogen-containing gas |
US20020100216A1 (en) * | 2001-01-26 | 2002-08-01 | Piero Colombani | Production of hydrogen from a gaseous hydrocarbon and system used in said procedure |
US20040118047A1 (en) * | 2002-12-18 | 2004-06-24 | Choudhary Vasant Ramchandra | Process for the continuous production of carbon monoxide-free hydrogen from methane or methane-rich hydrocarbons |
US20050003247A1 (en) * | 2003-07-01 | 2005-01-06 | Ai-Quoc Pham | Co-production of hydrogen and electricity using pyrolysis and fuel cells |
US8313718B2 (en) * | 2006-12-13 | 2012-11-20 | Dow Global Technologies Llc | Method and composition for removal of mercaptans from gas streams |
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GB2265382A (en) | 1992-03-23 | 1993-09-29 | Shell Int Research | Process for the non-catalytic production of hydrogen and/or carbon monoxide |
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- 2015-07-06 WO PCT/EP2015/065332 patent/WO2016005317A1/en active Application Filing
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- 2015-07-06 EP EP15732756.0A patent/EP3166884B1/en active Active
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Patent Citations (7)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
GB365912A (en) * | 1930-04-30 | 1932-01-28 | Humphreys & Glasgow Ltd | Improvements in or relating to the manufacture of combustible gas rich in hydrogen |
US3864460A (en) * | 1973-07-12 | 1975-02-04 | Nrg Inc | Method for removing hydrogen sulfide from hydrocarbon gas streams without pollution of the atmosphere |
EP0219163A2 (en) * | 1985-10-09 | 1987-04-22 | Shell Internationale Researchmaatschappij B.V. | Process and apparatus for producing a hydrogen-containing gas |
US20020100216A1 (en) * | 2001-01-26 | 2002-08-01 | Piero Colombani | Production of hydrogen from a gaseous hydrocarbon and system used in said procedure |
US20040118047A1 (en) * | 2002-12-18 | 2004-06-24 | Choudhary Vasant Ramchandra | Process for the continuous production of carbon monoxide-free hydrogen from methane or methane-rich hydrocarbons |
US20050003247A1 (en) * | 2003-07-01 | 2005-01-06 | Ai-Quoc Pham | Co-production of hydrogen and electricity using pyrolysis and fuel cells |
US8313718B2 (en) * | 2006-12-13 | 2012-11-20 | Dow Global Technologies Llc | Method and composition for removal of mercaptans from gas streams |
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US10125018B2 (en) | 2018-11-13 |
US20170166444A1 (en) | 2017-06-15 |
EP3166884B1 (en) | 2020-01-01 |
CN106660789B (zh) | 2019-08-20 |
AU2015286899A1 (en) | 2017-02-02 |
EP3166884A1 (en) | 2017-05-17 |
AU2015286899B2 (en) | 2017-11-30 |
WO2016005317A1 (en) | 2016-01-14 |
MY178326A (en) | 2020-10-08 |
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