CN111246940A - Co2转化的催化组合物 - Google Patents
Co2转化的催化组合物 Download PDFInfo
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Abstract
本发明涉及一种催化组合物,其包含至少7种不同的元素和基质组分,所述元素选自由元素周期表的第二至第六周期与第一至第十六族的交集所限定的元素组成的组,其中排除了锝。还提供了使用该催化组合物的方法。
Description
技术领域
本发明涉及用于将CO2转化为合成气和烃化合物的方法以及催化组合物。
背景技术
化石燃料已在能源的产生中一直起着重要的作用。在过去的几十年中,能源消耗不断增加。因此,对化石燃料的依赖性增强,并且能源的产生导致温室气体CO2向大气中的释放显著增加。体积范围为数十亿吨的CO2排放到大气中,而且这一趋势还在继续增加。同时,越来越多的证据表明,这种人为的CO2排放至少部分地影响了气候和天气的变化,例如突然变化的条件,例如洪水和干旱。此外,在炼铁和混凝土生产过程中会散发大量的CO2。因此,非常需要将经济增长与基于化石燃料的能源生产以及由此引起的CO2排放脱钩。这样可以避免可能无法逆转的潜在危险气候和天气变化。已经进行了多次尝试来捕获和利用二氧化碳,但是它们缺乏效率和/或要求苛刻的条件以获得很少反应性CO2的充分转化。
减少CO2的一种合适方法表示将CO2转化为有用的化学物质。的确,这可能是一方面减少全球排放并在另一方面生产有价值的产品的最佳方法之一。CO2代表着丰富而宝贵的碳源,可以替代使用化石燃料来使用。这可能会潜在导致温室气体CO2的显著减少,从而消除气候和天气的不良变化。
如今,化石燃料仍然占世界能源的80%以上。此外,化学工业大量使用化石燃料,因为95%的有机类化学品均来自化石燃料等不可再生资源。完整的化学工业分支机构完全依靠化石原材料,即石油化学和合成聚合物工业。迫切需要主要依靠化石燃料向非化石或至少少消耗化石燃料的资源转变化学和能源工业。这也是现成的CO2作为合成燃料、基础化学品和其它化学产品来源日益重要的原因。最重要的是,使用CO2作为碳源可以减少人为的CO2排放量。利用CO2可以减少相关排放的过程基本上是CO2捕获和随后的(长期)存储,例如通过矿化或随后使用捕获的CO2作为碳源。后者还减少了使用化石燃料作为基础化合物的碳源的需求。CO2利用领域的主要重点在于开发有效的化学方法以捕集和随后使用CO2。寻求以更低的成本、更低的材料消耗或废物产生而更有效的催化剂。需要开发高效的催化剂,该催化剂允许在进一步用于合成的合成燃料或基础化学品的生产中转化来自工业烟道气(例如水泥、钢铁或其它耗能行业)的优选未纯化的含CO2的气流。非常令人欢迎的结果是,这将减少目前对化石燃料的依赖。因此,将CO2直接转化为基础化学品或化学构件非常重要,因为这可以开发更可持续、更容易获得的碳源,例如CO2。
对于良好的产率和加速的反应,优化了用于CO2利用的许多催化剂,从而改善了CO2利用的过程。但是,开发需要较少纯化或未纯化CO2流,能够耐受典型烟道气中的氮、水、SOx和NOx化合物,并且在低CO2浓度下也有效的催化剂将特别有利。由于直接使用来自工业过程的可变组成的CO2流的能力,而无需在使用它们之前对气流进行纯化,因此可以在整个过程中实现显著的经济和环境改善。
甲烷是天然气的主要成分,并且由于其有利的低碳氢比以及其在可能的最终用途中的多功能性,其作为化石燃料的重要性得到了提高。除石油和煤炭外,它还是能源领域和作为化学领域原料的用于加热的全球第三大使用矿物燃料。此外,它越来越多地用作运输燃料。甲烷是在含镍或钌的金属催化剂存在下,在较高温度(300℃至700℃)下由CO2或CO和H2通过Sabatier反应合成的,并且可直接供入天然气网络中,其中它可以部分替代化石甲烷。可以使用现有的天然气基础设施(管道网络、存储设施和最终使用设备),而无需进行进一步修改。使用H2减少二氧化碳需要廉价有效的氢源。昂贵或费力的生产H2的方法大大降低了将CO2或CO转化为合成燃料以及基础或结构性化学品的收益。目前有多种可用于制氢的不同技术,例如水电解,然而这是昂贵的。因此,生产H2的廉价有效方法至关重要。从经济和生态的观点来看,非常需要开发一种有效的催化剂,该催化剂能够热还原稀释和未纯化的CO2流,例如热还原为合成燃料以及将水蒸气热还原为H2,并因此,通过简单廉价的催化剂体系来促进将CO2直接转化为增值化学品,而无需昂贵的单独电解水,从而将CO2直接转化为增值化学品。
DE 10 2006 035 893描述了一种用于将燃烧产物转化为CO并且随后通过将由电解产生的H2加入甲醇和其它氢碳化合物中的方法。
DE 10 2009 014 728描述了在中等温度下在脉冲电化学能的支持下将CO2与CH4转化为合成气。但是,该过程被归类为使用CH4作为还原剂的重整过程,并且需要额外的电化学能。
DE 695 18 550描述了在Fe-K/Al2O3催化剂存在下用H2转化CO2以在1-100bar、200-500℃和500-20000h-1体积速度下生成C2+烃。但是,该反应需要存在单独产生的氢作为还原剂。
DE 698 10 493公开了一种特别是由合成气制造醇和烃的方法,并且涉及基于锰或镁以及另外的碱土金属或碱金属的金属催化剂,用于其中具有两个或更多个、特别是四个或更多个碳原子的分子通过一氧化碳和氢来提供的方法。由CO2产生合成气再次需要单独产生的氢气作为还原剂。
Steinfeld等人,energy&fuels,2012,26,7051-7059报告了太阳能驱动的热化学循环,涉及金属氧化物氧化还原反应,分解水和CO2以在远高于1000℃的温度下产生H2和CO,需要太阳能支持。
发明内容
本发明的目的是提供一种用于将CO2转化为合成气的高效催化剂,以及消除了现有技术催化剂的缺点的其它低分子有机化合物。还提供了使用催化剂的方法。
该目的通过根据权利要求1的催化组合物和根据权利要求6的方法来实现。另外的优选实施方式受从属权利要求的约束。
根据本发明的催化组合物包含至少七种不同的元素。元素选自由元素周期表的第二至第六周期与第一至第十六族的交集所定义的元素组成的组,其中排除了锝。周期的编号对应于当前IUPAC标准(于2017年7月生效)。催化组合物还包含基质组分,其中分散有催化剂。所述基质由与形成实际催化剂的至少七种不同元素不同的另外的组分形成。应当理解,在催化剂中,金属元素可以是元素形式,或者可以是化合物的形式,例如它们的氧化物,或者是元素形式的金属和金属化合物的混合物。
该催化剂是非均相催化剂,其能够在低于250℃的温度下转化浓缩的(CO2浓度≥90%)以及稀释的(CO2浓度≤5%)非纯化的CO2流。根据化学方程式,在存在水蒸气的情况下将CO2简单转化:CO2+H2O→CO+H2+CxHy+O2,其中x为1或2,并且y为4或6。
锝由于其放射性性质而被排除在外。锝的放射性性质以及锝本身的衰变可能导致催化成分发生不必要的变化。
在优选的实施方式中,基质是多孔基质。较高的孔隙率增加了表面重量比,因此增加了化合物与催化剂反应的接触表面。
在另一个优选的实施方式中,催化组合物的基质的表面重量比为至少40m2/g。特别优选较高的表面重量比,例如50m2/g或甚至60m2/g。
优选地,催化组合物的至少一种基质组分选自由以下组成的组:天然铝硅酸盐,合成铝硅酸盐,沸石,蛭石,活性炭,黑曜石,氧化钛,氧化铝及以上的混合物。更优选的是组分蛭石和黑曜石,以及它们的最优选混合物。天然存在的基质化合物,例如蛭石和黑曜石在其组成中也包含金属元素,例如镁(Mg)、铁(Fe)和铝(Al)。此外,它们几乎不可避免地包含一些杂质,例如其它金属元素。
在另一个实施方式中,催化组合物的至少7种元素选自由Al,C,Cd,Ce,Co,Cr,Cu,Eu,Fe,Gd,Mo,Mo,Na,Nd,Ni,O和Sm组成的组。同样,催化剂中的金属元素可以是元素形式,或它们可以是化合物的形式,例如它们的氧化物,或者是元素形式的金属和金属化合物的混合物。包含这些元素的组合的催化组合物在CO2转化中获得特别好的结果。
根据本发明的催化组合物在已达到约10000小时的其使用寿命时可以再生。催化组合物的再生通过在300℃或更高的温度下用干燥的气体蒸汽热处理一小时来实现。
由含CO2的气体制备合成气和烃化合物的方法包括以下步骤:首先,将含CO2的气体与水蒸气混合。其次,使含CO2的气体和水蒸气的混合物随后与根据本发明的催化组合物接触。通常,将催化组合物加热至所需的工艺温度。合成气是一种主要由氢气、一氧化碳和很通常一些二氧化碳组成的混合燃料。产生的烃化合物主要是甲烷和乙烷。
在优选的实施方式中,该方法在低于250℃的温度下,优选在100℃至180℃范围内,优选120℃至160℃范围内,并且更优选130℃至150℃范围内的温度下进行。该方法有利地在较低温度下进行,因为这降低了加热反应混合物和催化组合物所需的能量消耗。
在另一个实施方式中,该方法在低压下进行,优选在低于10bar,更优选在0.1至2bar范围内。在较低压力下进行反应简化了对所用设备装置的要求。
有利地,可以在根据本发明的方法中使用的含CO2气体的来源是多种多样的。含CO2气体的优选来源是燃烧过程的废气。也可以使用其它来源,例如发电厂或水泥厂的废气。最有利地,含CO2的气体可以是未纯化的废气。因此,不需要繁琐的纯化步骤,例如分离含硫或氮的化合物。
然而,含CO2的气体也可以作为用其它气体如氮气、氧气、氩气和硫氧化物稀释的气体混合物进行反应。
在另一个实施方式中,利用含CO2气体的热能进行催化反应。例如,源自燃烧过程的废气的热能可以用于加热催化组合物以及产生水蒸气。此外,这种废气的热能也足以维持所需的过程温度。
有利地,用于将CO2转化为可燃气体的转化率大于30%,更优选大于50%,或甚至更优选大于95%。可燃气体是指在提供火源的情况下在氧化剂存在下燃烧的气体。可燃气体可包括甲烷,乙烷,乙炔,氢,丙烷和丙烯。
用于实施根据本发明的方法的装置包括用于将含CO2的气体引入反应系统的入口管和水入口管。它还包括用于生成水蒸气的可选加热装置。同时,加热装置还用于加热催化组合物。反应容器包含催化组合物,并且出口管用于排出反应产物。反应容器与入口管和出口管流动连接。
在优选的实施方式中,反应容器是单室反应器或活塞流反应器。
催化组合物可以布置在反应器中的单个区域中,或者可以布置在几个不同的区域中,其中这些不同的区域均包含相同的催化组合物,即相同的至少七种元素的其元素形式或化合物形式,例如其氧化物,并分散在同一基质中。这些区域优选地串联布置。
在另一个实施方式中,存在至少两种包含不同元素的催化组合物。这意味着催化组合物确实包含不同的至少七种元素,其呈元素形式或化合物形式(例如其氧化物),并且分散在基质中。当然,并非至少七种元素的所有都必须不同。在不同的催化组合物中,它可以仅仅是至少七种元素中的一种元素是不同的。这些不同的催化组合物例如在活塞流反应器中优选串联布置在不同的区域中。还可以串联布置两种以上的不同催化组合物。同样,每种催化组合物布置在不同的区域中,其中其分散在基质中。对于所有不同的催化组合物,基质优选是相同的。然而,不同催化组合物分散在其中的基质也可以不同。几种不同催化组合物的这种串联布置有利地允许提高转化效率并引导或影响转化的主要产物。
附图说明
下面参考附图中的示例性实施方式更详细地解释根据本发明的用于转化CO2的方法和用于实施该方法的装置,其中,仅示意性地:
图1示出了根据本发明的方法的流程图;
图2示出了用于执行根据本发明的方法的装置。
具体实施方式
图1示出了描述该方法的步骤的流程图。第一步,将水加热以产生水蒸气。然后将水蒸气与含CO2的气体混合,该混合物随后与加热的催化组合物接触。
图2示出了用于执行根据本发明的方法的装置。装置15包括加热器10,所述加热器10用于加热以规则间隔布置在活塞流反应器中不同区域中的催化组合物5。加热器10还用于加热从水桶8馈送到螺旋形管9的水。通过加热螺旋形管9中的水,产生水蒸气。排气管12收集用作含CO2气体的加热器10的排气,所述含CO2的气体借助于气泵1通过管2和3泵送,其中气流通过经由阀4连接到管道3的压力控制器6。在含CO2的气体进入活塞流反应器之前,它通过一个入口,在其中产生的水蒸气与含CO2的气体混合。在活塞流反应器中,含CO2的气体和水蒸气的混合物与加热的催化混合物接触。最后,包含产物化合物的反应混合物进入出口管11,在其中可以将其收集用于进一步纯化或使用。
在下面的实施例中,根据本发明的催化组合物被更详细地描述。以下实施例显示了不同的催化剂组成。测试所有催化组合物将废气中的CO2转化为合成气和/或烃的活性。催化组合物包含基质组分和催化剂组分。给定不同化合物的量为催化组合物的重量%。
实施例1 | 实施例2 | 实施例3 | 实施例4 | 实施例5 | |
Al<sub>2</sub>O<sub>3</sub> | 12.0 | 15.0 | 8.0 | 4.0 | 0.0 |
C | - | - | - | 10.0 | - |
Cd | - | - | - | 2.0 | 1.0 |
Ce | - | 5.0 | - | 3.0 | 2.0 |
Co | - | - | 10.0 | - | 10.0 |
Cr<sub>2</sub>O<sub>3</sub> | 8.0 | 8.0 | 4.0 | - | 3.0 |
Cu | 7.0 | 10.0 | 6.0 | 3.0 | 3.0 |
Eu | 0.5 | - | - | - | - |
FeO | - | 6.0 | - | - | - |
Fe<sub>2</sub>O<sub>3</sub> | - | - | - | - | 20.0 |
Fe<sub>3</sub>O<sub>4</sub> | - | - | - | 12.0 | - |
Gd | 1.5 | - | - | - | - |
MoO<sub>3</sub> | - | 16.0 | 3.0 | - | - |
Mo<sub>3</sub>O<sub>7</sub> | 10.0 | - | - | 3.0 | - |
NaOH | - | - | - | 8.0 | - |
Nd | - | - | 2.0 | - | - |
Ni | 5.0 | - | - | - | 10.0 |
NiO | 5.0 | 10.0 | 18.0 | 5.0 | - |
Sm | 1.0 | - | 2.0 | - | 1.0 |
黑曜石 | 25.0 | 30.0 | 47.0 | 30.0 | - |
蛭石 | 25.0 | - | - | 20.0 | 50.0 |
随后将实施例编号1-5的催化组合物置于活塞流反应器中,并测试它们在将含CO2的气流转化为合成气和/或其它烃化合物中的催化活性。将反应器加热至140℃。将含CO2的气体和水蒸气在反应器中混合,然后与催化组合物接触。在出口管处收集气流样品,并然后进行分析。
在其它实验中,还发现了各种浓度的其它反应产物。这些额外的产物例如但不限于甲醇,乙醇,乙炔,苯和甲醛。
Claims (15)
1.一种催化组合物,其包含:形成催化剂的至少7种不同的元素,所述元素选自由元素周期表的第二至第六周期与第一至第十六族的交集所限定的元素组成的组,其中排除了锝;以及基质组分,其中分散有所述催化剂。
2.根据权利要求1所述的催化组合物,其中所述基质是多孔基质。
3.根据权利要求1或2中任一项所述的催化组合物,其中所述基质的表面重量比为至少40m2/g。
4.根据前述权利要求中任一项所述的催化组合物,其中至少一种基质组分选自由以下组成的组:天然铝硅酸盐、合成铝硅酸盐、沸石、蛭石、活性炭、黑曜石、氧化钛、氧化铝及以上的混合物。
5.根据权利要求1至4中任一项所述的催化组合物,其中至少7种元素选自由Al、C、Cd、Ce、Co、Cr、Cu、Eu、Fe、Gd、Mo、Mo、Na、Nd、Ni、O和Sm组成的组。
6.一种用于从含CO2的气体制备合成气和烃化合物的方法,其包括以下步骤:将所述含CO2的气体与水蒸气混合,并随后使混合物与根据权利要求1至5中任一项所述的催化组合物接触。
7.根据权利要求6所述的方法,其中所述方法在低于250℃的温度下进行,优选在100℃至180℃的范围内,优选120℃至160℃的范围内,并且最优选130℃至150℃的范围内的温度下进行。
8.根据权利要求6或7中任一项所述的方法,其中所述方法在低压下进行,优选在低于10bar,更优选在0.1至2bar的范围内进行。
9.根据权利要求6至8中任一项所述的方法,其中所述含CO2气体是燃烧的废气。
10.根据权利要求6至8中任一项所述的方法,其中所述含CO2气体是发电厂、熔炼厂或水泥厂的废气。
11.根据权利要求6至8中任一项所述的方法,其中所述含CO2的气体是未纯化的废气。
12.根据权利要求6至8中任一项所述的方法,其中将所述含CO2气体的热能用于进行催化反应。
13.根据权利要求6至8中任一项所述的方法,其用于将CO2转化为可燃气体,其中转化率大于30%,更优选大于50%,或甚至更优选大于95%。
14.一种用于执行根据权利要求6至13中任一项所述的方法的装置,其包括:含CO2气体的入口管、水入口管、用于产生水蒸气并加热催化组合物的加热装置、包含所述催化组合物的反应容器、以及用于排出反应产物的出口管,其中所述反应容器与所述入口管和所述出口管流动连接。
15.根据权利要求14所述的装置,其中所述反应容器是单室反应器或活塞流反应器。
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EP17020309.5 | 2017-07-14 | ||
EP17020309.5A EP3427821A1 (en) | 2017-07-14 | 2017-07-14 | Catalytic composition for co2 conversion |
PCT/EP2018/069321 WO2019012160A1 (en) | 2017-07-14 | 2018-07-16 | CATALYTIC COMPOSITION FOR CO2 CONVERSION |
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EP (2) | EP3427821A1 (zh) |
JP (1) | JP2020526392A (zh) |
CN (1) | CN111246940A (zh) |
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KR0169188B1 (ko) | 1995-07-31 | 1999-03-20 | 강박광 | 탄화수소의 제조방법 |
GB9720593D0 (en) | 1997-09-26 | 1997-11-26 | Exxon Chemical Patents Inc | Catalysts and processes using them |
DE10151559A1 (de) * | 2001-10-23 | 2003-04-30 | Basf Ag | Als Katalysator geeignete Masse |
US20050023190A1 (en) * | 2003-08-01 | 2005-02-03 | Welch Robert C. | Process to manufacture low sulfur fuels |
US7304011B2 (en) * | 2004-04-15 | 2007-12-04 | W.R. Grace & Co. -Conn. | Compositions and processes for reducing NOx emissions during fluid catalytic cracking |
WO2007021394A2 (en) * | 2005-08-18 | 2007-02-22 | Exxonmobil Chemical Patents Inc. | Catalytic conversion of oxygenates to olefins |
DE102006035893A1 (de) | 2006-07-31 | 2008-02-07 | Wolf, Bodo M., Dr. | Verfahren zur Wiederaufarbeitung von Verbrennungsprodukten fossiler Brennstoffe |
US20100174129A1 (en) * | 2006-12-29 | 2010-07-08 | Bauman Richard F | High throughput propylene from methanol catalytic process development method |
WO2008134484A2 (en) * | 2007-04-25 | 2008-11-06 | Hrd Corp. | Catalyst and method for converting natural gas to higher carbon compounds |
DE102009014728A1 (de) | 2009-03-25 | 2010-09-30 | Siemens Aktiengesellschaft | Verfahren zum Betreiben eines Fossilbrennstoff-Kraftwerks und Fossilbrennstoff-Kraftwerk mit vermindertem Kohlendioxidausstoß |
WO2012119958A1 (en) * | 2011-03-04 | 2012-09-13 | Antecy B.V. | Catalytic process for converting carbon dioxide to a liquid fuel or platform chemical |
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US9789470B2 (en) * | 2012-09-25 | 2017-10-17 | Haldor Topsoe A/S | Steam reforming catalyst and method of making thereof |
EP2769765A1 (en) * | 2013-02-22 | 2014-08-27 | Centre National De La Recherche Scientifique | Use of compositions obtained by calcing particular metal-accumulating plants for implementing catalytical reactions |
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JP2020526392A (ja) | 2020-08-31 |
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