CN102597173A - 具有原位co2捕集的合成燃料和化学品生产 - Google Patents

具有原位co2捕集的合成燃料和化学品生产 Download PDF

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CN102597173A
CN102597173A CN2010800481730A CN201080048173A CN102597173A CN 102597173 A CN102597173 A CN 102597173A CN 2010800481730 A CN2010800481730 A CN 2010800481730A CN 201080048173 A CN201080048173 A CN 201080048173A CN 102597173 A CN102597173 A CN 102597173A
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carbonaceous fuel
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L-S·樊
F·李
L·曾
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Ohio State University Research Foundation
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Abstract

提供了具有原位CO2捕集的用于燃料和化学品生产的新型基于氧化还原的系统。使用一种或多种化学中间体的氧化还原系统通常与经间接费-托合成、直接氢化或热解生产液体燃料结合使用。所述氧化还原系统用以产生用于液体燃料和化学品生产的富氢物流和/或CO2和/或热。将来自液体燃料和化学品合成的副产物燃料和/或蒸汽的一部分用作用于所述氧化还原系统的原料的一部分。

Description

具有原位CO2捕集的合成燃料和化学品生产
本发明通常涉及具有原位CO2捕集的用于合成燃料和化学产品生产的系统和方法。通常使用一种或多种化学中间体的氧化还原(redox)系统，并结合以经间接CO2氢化、直接氢化或热解生产液体燃料。
包括原油、天然气和煤炭的化石燃料提供超过85％的现今能源供应。这些化石燃料通常在由最终消费者利用之前转变成诸如电力和液体运输燃料的载体。电力主要由诸如煤炭、天然气和核的相对充足的能源生产。相比之下，液体运输燃料几乎专门由原油获得，其供应在多变的价格下相对不稳定。在日益增加的能量需要和对于来自化石燃料应用的碳排放的伴随担忧之下，需要来自诸如煤炭、生物质和油页岩的更充裕资源的可承受的合成运输燃料。为了解决环境问题，下一代合成燃料生产方法需要能够捕集在该工艺中产生的污染物。这些污染物包括CO2、硫化合物和汞，等等。
合成燃料通过重整和费托(Fischer-Tropsch，“F-T”)方案由诸如天然气的气态燃料生产。诸如煤炭、生物质和石油焦的固体燃料可通过间接液化(气化-水煤气变换-费托)、直接液化或热解转化为合成燃料。然而，这些系统比石油精炼方法资本更密集。此外，其能量转化效率比较低。
合成燃料也可经生物化学路径由生物质产生。然而，利用大量工业用水。此外，生物化学方法对原料具有严格需求。
所有上述方法都包括CO2排放。从这些方法捕集CO2与显著的能量损耗相关且因此降低工艺效率。
本发明的实施方案提供在高效率和有效CO2捕集下由天然存在的碳质燃料源生产合成燃料的供选方案。
本发明的实施方案通常涉及具有原位CO2捕集的用于燃料和化学品生产的新型基于氧化还原的系统。使用一种或多种化学中间体的氧化还原系统通常与经间接费-托合成、直接氢化或热解生产液体燃料结合使用。所述氧化还原系统用以产生用于液体燃料和化学品生产的富氢物流和/或CO2和/或热。将来自液体燃料和化学品合成的副产物燃料和/或蒸汽的一部分用作用于所述氧化还原系统的原料的一部分。
鉴于以下详述将更全面地理解由本发明的实施方案提供的额外特征和优势。
当结合以下附图阅读时，可更好地理解本发明的说明性实施方案的以下详述，其中类似结构用类似附图标记表示且其中：
图1说明利用碳质原料的间接重整/气化与费-托合成的组合的合成液体燃料生产实施方案。
图2为说明间接重整/气化与费-托合成的集成的另一实施方案的示意图。
图3说明基于铁氧化物的气态燃料间接重整/气化系统与费-托合成的集成的另一实施方案。在该情况下使用煤炭和煤炭气化单元以生产合成气燃料。在该系统中也可直接使用甲烷和烃。或者，可安装重整器以代替气化单元(气化器)来转化烃燃料。
图4说明使用基于铁氧化物的固体燃料间接气化系统与费-托合成的集成的另一实施方案。除了生物质和煤炭以外，在该系统中还可使用其他固体燃料，诸如石油焦、沥青砂、油页岩和废物衍生的燃料。
图5说明使用吸附剂强化的重整/水煤气变换系统与费-托合成的集成的另一实施方案。在该系统中可使用气态燃料，诸如合成气和轻质烃。
图6为显示在直接煤炭变液体子系统与间接碳质燃料重整/气化子系统之间的集成的另一实施方案的示意图。吸附剂强化的重整/水煤气变换系统也可用以代替基于氧化还原的间接重整/气化子系统。
图7显示用于生物油合成的在生物质热解器与间接碳质燃料重整/气化子系统之间的集成的另一实施方案。
图8为说明用于生物油合成的在生物质热解器与间接碳质燃料重整/气化子系统之间的集成方案的另一实施方案。
图9说明在煤炭/生物质粉末向上流动且金属氧化物复合材料向下流动的逆流移动床中用于粉煤/生物质转化的额外还原器设计。
图9(a)说明用于粉煤和生物质转化的移动床还原器设计；图9(b)说明用于煤炭注入和转化的潜在设计。
本发明的实施方案通常涉及在极低碳排放和改进的能量转化效率下将碳质燃料转化为合成燃料的系统和方法。这类系统和方法通常包括间接燃料重整/气化子系统和液体燃料合成子系统。
基于经其生产合成燃料的技术，本发明的各种实施方案通常可归为三类，即，与间接燃料重整/气化子系统集成的间接合成燃料生产、与间接重整/气化子系统集成的直接合成燃料生产和与间接燃料燃烧子系统集成的直接热解系统。以下说明书分别论述这三类。
策略上与间接燃料重整/气化子系统集成的间接合成燃料生产系统通常由图1-5表示。
经气化/重整接着进行费-托合成将诸如煤炭和天然气的碳质燃料间接转化为合成液体燃料已沿用已久。然而，这些方法由于气化/重整步骤的极大不可逆性和费-托合成反应的高度放热性质及与热回收和利用相关的低效率而效率低下。此外，如果捕集在该工艺中产生的碳，则将引起显著的能量损耗。另外，间接合成燃料生产系统为资本高度密集型的。
关于能量安全和CO2排放的日益增加的担忧对间接合成燃料生产系统的环境和经济可接受性二者产生了严重怀疑。为了降低间接液体燃料合成系统的成本和碳足迹，非常需要伴随着CO2捕集的工艺能量转化效率的显著改进。本发明的实施方案策略上集成间接气化/重整子系统与费-托子系统以实现以下效果：1)降低总合成燃料生产系统的不可逆性；2)改进能量转化效率；和3)捕集在该工艺中产生的CO2。
根据一方面，诸如煤炭、生物质、石油焦、合成气、天然气、特稠油、石蜡和油页岩的碳质燃料首先在一种或多种化学中间体的辅助下转化为CO2和H2的单独物流。H2和一部分CO2随后在费-托合成反应器中反应以生产合成燃料和化学品。剩余CO2以浓缩形式获得且可容易地封存。与CO和H2相反，在费-托反应器中CO2和H2的转化降低F-T反应的放热性。此外，该方案潜在地降低气化/重整步骤的吸热性。因此，可降低总工艺的不可逆性。此外，由放热F-T反应器生产的蒸汽可容易地用于在气化/重整子系统中的氢气产生。虽然在二十世纪九十年代研究CO2和H2用于F-T合成，但用于由碳质燃料生产CO2和H2的方法和在本文所述的CO2/H2产生子系统之间的独特集成方案为新颖的。
图1通常涉及基于氧化还原的气化/重整子系统和F-T子系统的集成方案。在该构型中，碳质燃料间接气化/重整成CO2和H2的两种单独物流。随后将这两种物流冷却并引入F-T子系统以生产液体燃料。在该工艺中的反应(未被配平)包括：
MeOx+CxHyOz→CO2+H2O+MeOy(反应器1)
MeOy+H2O→MeOz+H2(反应器2，y＜z≤x)
MeOz+O2→MeOx(反应器3，任选的)
CO2+H2→-(CH2)-+H2O(CO2氢化)
在此，CxHyOz通常是指碳质燃料。Me为可由碳质燃料还原且随后由蒸汽或空气氧化的金属或金属混合物。这类金属包括Fe、Co、In、Mn、Sn、Zn、Cu、W及其组合。
反应器1通常在400-1200℃和1.01×105Pa-8.10×106Pa(1-80atm)下操作。反应器2在比反应器1低0-300℃的温度下操作。反应器3，其是任选的，取决于金属的类型和系统构造，在比反应器1高0-400℃的温度下操作。在优选的实施方案中，反应器1在600-900℃下操作。气化/重整子系统在1.01×105Pa-3.04×106Pa(1-30atm)下操作。
在某些实施方案中，反应器1为吸热的。来自反应器1的被还原固体的一部分直接送到反应器3中以便用含氧气体氧化。在反应器3中释放的热用以补偿在反应器1中需要的热。在反应器3中产生的额外热用以发电以支撑附加动力应用。来自反应器2的氢气的一小部分可用于燃料产品提质。
如图1中所示，碳质燃料接近反应器1的底部进料。在一个实施方案中，所述碳质燃料包括固体粒子，所述固体粒子通过在反应器1下部的锥形段中的气体悬浮，直至它们在向反应器1的顶部淘选之前被转化至少50％。富CO2气体和富H2气体分别由反应器1和反应器2生产。可能含有蒸汽的这些气态物流可在F-T合成之前冷凝。或者，这些气态物流可直接用于F-T合成。
F-T子系统在200-500℃和1.01×106Pa-8.10×107Pa(10-100atm)下操作。在一些实施方案中，进行来自气化/重整子系统的富CO2气体和富H2气体的压缩。
硫可存在于碳质燃料中，污染富CO2气体物流和富H2气体物流。一个或多个脱硫单元可用以清洗产物气体物流。在其中将基于铁的催化剂用于F-T合成的情况下，使用诸如CaO、ZnO等的固体吸附剂的高温吸附剂床可用以将硫污染物降到100ppm或更低的水平。当将诸如基于钴的F-T催化剂的耐硫性较低的催化剂用于F-T合成时，可使用额外脱硫步骤，诸如，使用MDEA、SELEXOL(商品名称)或Rectisol(商品名称)的脱硫步骤。在使用诸如低硫生物质或不含硫的天然气或合成气的低硫燃料的情况下，不需要脱硫单元。
图2说明另一工艺构造，其集成了基于氧化还原的气化/重整子系统和F-T子系统。在该构造中，使来自F-T子系统的未转化的燃料连同碳质燃料原料一起再循环回到反应器1中。通过这样做，将来自F-T子系统的副产物转化为H2和CO2，增加工艺的液体燃料产率和选择性。另外，由F-T子系统产生的蒸汽重新引导到气化/重整子系统的反应器2中，降低在该工艺中对蒸汽产生的需要。F-T和气化/重整子系统及其集成-再循环方案二者的产物和副产物的策略利用降低了总工艺的能量损耗，同时增加了所需产物，要么是化学品要么是合成液体燃料，的产率。在该工艺中产生的任何CO2可以容易地封存。因此，与常规煤炭变液体方案相比，该工艺的碳密集性显著较低且更有效。
图3进一步说明更详细的工艺构造，其集成了基于铁氧化物的气化/重整子系统和F-T子系统。在该实施方案中，气化/重整子系统包括气化/重整单元和基于铁的氧化还原单元。固体燃料首先转化为气态燃料混合物。随后将气态燃料注入铁氧化物氧化还原系统的还原器中以便产生氢气和CO2。当气态燃料被高水平的硫污染时，可能需要热气清洗系统。三个反应器基于铁氧化物的氧化还原系统以与在Thomas的美国专利7,767,191号、Fan的PCT申请WO 2007082089号和Fan的PCT申请WO2010037011号中所公开类似的方式转化燃料。第一反应器(还原器)被构造以将碳质燃料氧化为CO2和蒸汽，同时还原基于金属氧化物的载氧体，使得金属的平均化合价小于1。在还原器中需要或产生的热由载氧体粒子提供或除去。第二反应器(氧化器)被构造以用蒸汽(部分)氧化被还原的载氧体的一部分。第三反应器(燃烧器)用空气燃烧来自氧化器中的被部分氧化的载氧体和来自还原器的被还原的载氧体的剩余部分。在铁氧化物氧化还原系统中的反应包括方程(未被配平)：
Fe2O3+燃料→Fe/FeO+CO2+H2O(Fe的平均化合价＜1)
(还原器)
Fe/FeO+H2O→Fe3O4+H2(氧化器)
Fe3O4+O2(空气)→Fe2O3(燃烧器)。
在一个实施方案中，将来自氧化器的所有氢气和来自还原器的一部分CO2引入费-托反应器中以产生烃的混合物。随后分离并精炼该烃混合物。将具有较低经济价值的那部分燃料混合物(例如，未转化的合成气、轻质烃和石脑油)送到还原器或气化器/重整器中以加强碳利用率。实质上，在燃料中的大部分碳被固定在最终合成燃料产物或以备在适度压缩之后封存的浓CO2物流中。因此，当将煤炭用作燃料(在CO2捕集和封存下)时，系统的净生命周期CO2排放可与基于石油的汽油和柴油相当。在将生物质和天然气用作燃料的情况下，净生命周期CO2排放低得多或甚至为负。在碳约束情形下，诸如煤炭/生物质、煤炭/天然气的原料组合可用于降低CO2排放，同时利用来源广泛的煤炭的优势。
F-T反应器产生大量蒸汽用于F-T冷却用途，且一部分蒸汽用于氧化器中以便产生氢气。在用一小部分副产物燃料补充燃烧或过度加热和与在该工艺中的高温排放气体物流热交换之后，剩余部分的蒸汽用于发电以满足附加能量需要。
载氧体包括具有布置在载体上的至少一种金属氧化物的多个陶瓷复合粒子。陶瓷复合粒子描述在Thomas的美国专利US 7,767,191号、Fan公开的PCT申请WO 2007082089号和Fan的PCT申请WO 2010037011号中。除了在Thomas中描述的粒子和粒子配方及合成方法以外，申请人在另一实施方案中开发了用以改进在本发明系统中使用的陶瓷复合粒子的性能和强度的新方法和载体材料。
所述新方法包括以下步骤：混合金属氧化物与以浆料形式的至少一种陶瓷载体材料、接着干燥、粒化和制粒。除了在现有出版物中描述的那些载体材料以外，陶瓷载体材料还包括氧化镁、斑脱土、橄榄石、高岭土和海泡石。橄榄石也用作烃转化的助剂。
图4说明其中基于铁的三反应器氧化还原系统将固体燃料直接转化为CO2和H2、接着进行费-托合成的实施方案。在该实施方案中，基于铁氧化物的载氧体被固体燃料还原。这后面是以与在图3中所示的实施方案类似的方式进行蒸汽再生和空气燃烧。
现在参看在图4的第一反应器(即，还原器)中的还原反应，该还原器利用诸如生物质、煤炭、焦油、油页岩、油砂、沥青砂、石蜡和焦炭的各种固体碳质燃料以还原含铁氧化物的陶瓷复合材料以产生被还原的金属和/或金属氧化物的混合物。除了固体碳质燃料以外，来自液体燃料合成子系统的副产物和未转化的燃料也在还原器中转化。可能的还原反应包括：
FeOx+燃料→FeOy+CO2+H2O
燃料+CO2→CO+H2
燃料+H2O→CO+H2
FeOx+CO/H2→FeOy+CO2/H2O。
优选的总反应为：
Fe2O3+燃料→Fe/FeO+CO2+H2O。
具体地讲，在还原器中形成金属铁(Fe)。同时，含有至少80％CO2(干基)的排出物流由还原器产生。在优选的实施方案中，CO2浓度超过95％且可直接封存。
还原器的优选设计包括具有一级或多级的移动床反应器、多级流化床反应器、阶梯式反应器、旋转窑炉或本领域的普通技术人员已知提供逆流气固接触模式的任何合适的反应器或容器。在固体和气体之间的逆流流动模式用以加强气体和固体的转化。逆流流动模式使固体和气体两者的反混最小化。此外，该流动模式保持反应器的固体出口处于更具还原性的环境下，同时反应器的气体出口保持在更具氧化性的环境下。因此，气体转化和固体转化二者都被加强。
回头参看在图4中的第二反应器(即，氧化器)中的氧化反应，该氧化器使用由费-托冷却产生的蒸汽将来自还原器的含铁载氧体粒子的一部分转化到高氧化态。可能的反应包括：
Fe+H2O→FeO+CO/H2
3FeO+H2O→Fe3O4+CO/H2。
氧化器的优选设计也包括移动床反应器和提供逆流气固接触模式的其他反应器设计。优选逆流模式，以便实现高的蒸汽到氢气和CO2到CO的转化率。
回头参看在图4中的第三反应器(即，燃烧器)中的氧化反应，空气或其他含氧气体用以燃烧还原器固体产物的剩余部分和所有氧化器固体产物。在该燃烧器中可能的反应包括：
Fe/FeO/Fe3O4+O2→Fe2O3。
或者，将所有还原器载氧体产物引入氧化器中以与亚化学计量之量的蒸汽反应。随后将来自氧化器的基本所有被部分再生的载氧体引入燃烧器中。通过这样做，不需要使固体物流旁路通过。
燃烧器的优选反应器设计包括快速流化床反应器、携带床反应器、运输床反应器或机械输送系统。燃烧器的功能包括：将载氧体氧化到高氧化态；和使载氧体再循环到还原器的入口用于另一氧化还原循环。
所述燃烧器为高度放热的。在燃烧器中产生的热可用以补偿在还原器中需要的热。该热也可用以预热进料流和产生用于附加能量消耗的动力。从系统中排出的高压气态物流可用以驱动膨胀机用于气体压缩。
表1说明当将伊利诺斯#6煤炭和柳枝稷用作原料且合成柴油为产物时在工艺中的主要物流的质量流量。表2说明系统的能量平衡。
表1.用于由煤炭合成液体燃料的集成的重整/气化-费-托系统的质量平衡
Figure BDA0000156903850000091
表2.用于由煤炭合成液体燃料的集成的重整/气化-费-托系统的能量平衡
表3说明当将柳枝稷用作原料且合成柴油为产物时在工艺中的主要物流的质量流量和能量流量。
表3.用于由柳枝稷合成液体燃料的集成的重整/气化-费-托系统的质量平衡和能量平衡
Figure BDA0000156903850000093
虽然由表1-3中例示的情况对于原料、产物、重整/气化子系统和液体燃料生产系统的类型来说为具体的，但上述参数的选择具有极大自由度。例如，可将多种类型的固体燃料用作原料且可生产各种合成燃料产物。
图5以实施方案示意性说明，其中重整/气化子系统由吸附剂强化的重整/气化单元构成。在该实施方案中，钙基吸附剂强化的重整方法用作重整/水裂解区块。燃料，其可为碳质进料或来自液体燃料合成子系统的副产物，在CaO/Ca(OH)2吸附剂和由F-T反应器产生的蒸汽的存在下被重整/转变为H2：
CaO+燃料+H2O→CaCO3+H2。
废吸附剂随后在高温下使用来自系统的废热在煅烧炉中再生：
CaCO3→CaO+CO2。
使来自液体燃料合成子系统的副产物的一部分燃烧以提供用于煅烧反应的热。任选增加水合步骤以使吸附剂再活化。随后压缩并封存来自煅烧炉的浓缩的CO2。
由吸附剂强化的重整方案产生的氢气和一部分CO2随后用以产生合成燃料。在燃料合成之前需要压缩CO2物流。
图6说明显示在直接液化子系统和重整/气化子系统之间的集成的实施方案。重整/气化子系统与在图1-5中例示的那些相同，即，可使用基于金属氧化物氧化还原的子系统和吸附剂强化的重整/气化子系统二者。液体燃料合成子系统包括单级或两级直接液化反应器和精炼系统。煤浆在催化剂以及来自重整/气化子系统的氢气存在下直接转化为烃。直接液化反应器的压力为5.05×106Pa-1.01×107Pa(50-100atm)且温度为400-650℃。燃料的轻质馏分和来自精炼系统的诸如重质残渣和炭的副产物用作用于重整/气化子系统的燃料。此外，在煤炭液化单元中产生的蒸汽也用于在重整/气化子系统中生产氢气。概括来讲，集成的系统使用来自液体燃料合成子系统的副产物以产生用于直接煤炭液化的氢气。此外，对于燃料产物中所期待的几乎所有的碳，自重整/气化子系统转化为富CO2的排出气体物流。所述富CO2的物流容易被封存。
图7说明其中存在在快速热解工艺和基于氧化还原的燃料燃烧工艺之间的集成的实施方案。生物质可经快速热解工艺转变为生物油。然而，快速热解需要有效控制生物质温度和显著的热输入。在该实施方案中，基于金属氧化物的两步氧化还原工艺用以提供用于热解器的热，同时捕集在该工艺中产生的碳副产物。
将金属氧化物用作氧气和热二者的载体。在第一单元(还原器)中，高温金属氧化物(600-1400℃)由来自热解器和精炼区块的残余碳和轻质部分还原：
MeOx+来自热解器和精炼区块的不想要的燃料→MeOy+CO2
该步骤大多为吸热的，离开还原器的热MeOy处于在400-750℃范围的温度下。
来自还原器的MeOy进入热解器中，在那里它提供热到生物质原料以便快速热解。MeOy可在热解器中被进一步还原为MeOz。离开热解器的MeOz的温度在300-650℃范围内。还原器和热解器可为移动床或流化床。对于热解器，优选流化床。
随后将来自热解器的MeOz引入氧化器中，其类似于关于图1-4描述的燃烧器单元。在该氧化器中，MeOz用诸如空气的含氧气体燃烧以再生为MeOx：
MeOz+O2→MeOx
氧化器的出口温度在600-1400℃范围内。氧化器的优选反应器设计包括快速流化床反应器、携带床反应器、运输床反应器或机械输送系统。用于氧化还原操作的优选金属包括但不限于Co、Fe、Cu、Ni、Mn和W。选择载体材料和金属以使得金属氧化物复合物对于焦油裂化没有非常高的催化活性。
图8说明生物质快速热解工艺和氧化还原工艺的集成的另一实施方案。在该实施方案中，金属氧化物复合物不直接接触生物质进料，即，热量间接提供到快速热解器。在该实施方案中，用于还原器的燃料又为来自生物质的快速热解的副产物和炭。该还原器还原来自氧化器的热金属氧化物：
MeOx+来自热解器和精炼区块的不想要的燃料→MeOy+CO2
该步骤常为吸热的，离开还原器的热MeOy处于在400-750℃范围的温度下。
被还原的MeOy随后进入氧化器，该氧化器优选为携带床、运输床或快速流化床反应器。该氧化器类似于在壳侧具有金属氧化物复合物和空气流动的管壳式换热器设计。空气将MeOy氧化回到MeOx。
MeOy+O2→MeOx
在该步骤中产生大量热。同时，也产生了高温排出空气。该还原器可为移动床或流化床。
具有少量残余氧气的富N2的排出空气可直接用于生物质进料并在快速热解器中传输以提供热。在某些实施方案中，可使用来自快速热解阶段的过量副产物燃料的额外燃烧步骤来在将高温富N2气体用于生物质进料和输送之前除去残余氧气。
将被粉碎的生物质引入热解器中，该热解器安装在氧化器内。由高温气体携带的被粉碎的生物质在切线方向上注入热解器中且由高温气体以旋流方式向上输送。离心力使得生物质接近于热解器/氧化器壁，热可经由该壁转移到生物质以便热解。该热解器为快速流化床、携带床或稀释运输床。
或者，还原器可与热解器集成以将热从其外壁提供到热解器。在两种情况下，热解器在300-650℃之间操作，还原器在400-1300℃之间操作，且氧化器在450-1350℃之间操作。
在基于氧化还原的重整/气化子系统中的还原器的性能对于如在图1、2、3、4、6、7和8中所示的集成的实施方案的成功来说是重要的。除了在Fan的PCT申请WO 2007082089号和Fan的PCT申请WO 2010037011号中公开的设计以外，对用于转化固体燃料的还原器设计进行改进。
图9说明还原器的改进设计。在该设计中，大(0.5-10mm)且密度较大(＞1.5g/mL)的金属氧化物复合粒子从还原器的顶部进料。小(＜0.5mm)且密度较低(＜1.5g/mL)的被粉碎的生物质或煤炭或其他固体燃料进料到还原器的底部。被粉碎的煤炭或生物质由输送气体携带且在复合粒子的间隙之间向上流动，同时被转化。复合物粒子向下移动且在离开还原器之前被还原。

Claims (14)

1.由碳质燃料生产合成液体燃料的方法，其包括：
使用蒸汽和任选的含氧气体使所述碳质燃料间接气化并形成富二氧化碳气体和富氢气体的单独物流；和
使所述富氢气体和所述二氧化碳的一部分以CO2氢化反应进行反应以形成合成燃料。
2.权利要求1的方法，其中金属氧化物粒子用于所述间接气化反应中。
3.权利要求1的方法，其中所述蒸汽的至少一部分使用由所述CO2氢化步骤产生的热来生产。
4.权利要求1的方法，其中所述碳质燃料包括合成气、一氧化碳、富甲烷气体、轻质烃、液体碳质燃料、煤炭、生物质、沥青砂、油页岩、石油焦、重质液体烃、蜡以及它们的混合物。
5.权利要求1的方法，其中剩余的CO2在冷凝出水分之后被封存。
6.权利要求1的方法，其中所述合成液体燃料的至少一部分用作所述碳质燃料的进料。
7.权利要求2的方法，其中所述金属氧化物粒子包括铁和/或其氧化物。
8.权利要求2的方法，其中所述金属氧化物粒子含有载体材料，所述载体材料包括选自由以下各物组成的集合的陶瓷材料：Al、Ti、Zr、Y、Si、La、CR、Mg、Mn、Cu、Ca的氧化物；Si和Ti的碳化物；海泡石；斑脱土；和高岭土。
9.权利要求2的方法，其中所述金属氧化物粒子含有Fe2O3，且所述碳质燃料通过以下步骤间接气化：
在具有逆流气固接触模式的包括填料移动床的第一反应区中用所述碳质燃料还原含Fe2O3的粒子以使得铁的平均化合价小于1；
在包括逆流气固接触模式的第二反应区中用蒸汽至少部分地氧化含被还原的铁氧化物的粒子以产生富氢气体，以使得所述铁氧化物被至少部分地氧化成Fe2O4；和
在第三反应区中用含氧气体氧化所述含铁氧化物的粒子且使含被氧化的铁氧化物的粒子返回所述第一反应区。
10.权利要求9的方法，其中将选自CO2、H2O的气态物质或来自CO2氢化的气态燃料引入所述第一反应区的底部以加强所述铁氧化物粒子和所述碳质燃料二者的转化。
11.权利要求9的方法，其中所述碳质燃料包括固体碳质燃料粒子，所述固体碳质燃料粒子通过在所述第一反应区的下段中的气体悬浮，直至它们在向所述第一反应区的顶部淘选之前被转化至少50％。
12.权利要求1的方法，其中含氧化钙的CO2吸附剂用以辅助所述碳质燃料的间接气化。
13.由碳质燃料生产合成液体燃料的方法，其包括：
用富氢气体物流使固体碳质燃料直接液化；和
使任何未转化的固体碳质燃料间接气化以形成富氢气体和富CO2气体的单独物流。
14.由碳质燃料生产合成液体燃料的方法，其包括以下步骤：
用热的含金属氧化物的粒子使固体碳质燃料直接或间接热解以形成液体燃料；和
用含金属氧化物的粒子使所述未转化的固态碳质燃料间接燃烧或气化以产生热和富CO2的气体物流。
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