CN101981163A - 从气体物流中分离甲烷的方法 - Google Patents

从气体物流中分离甲烷的方法 Download PDF

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CN101981163A
CN101981163A CN2009801115372A CN200980111537A CN101981163A CN 101981163 A CN101981163 A CN 101981163A CN 2009801115372 A CN2009801115372 A CN 2009801115372A CN 200980111537 A CN200980111537 A CN 200980111537A CN 101981163 A CN101981163 A CN 101981163A
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hydrogen
gas
logistics
gas stream
methane
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CN101981163B (zh
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P·K·拉曼
F·S·劳
E·T·罗宾逊
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Shunguan Investment Co., Ltd
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Greatpoint Energy Inc
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    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J2300/00—Details of gasification processes
    • C10J2300/18—Details of the gasification process, e.g. loops, autothermal operation
    • C10J2300/1853—Steam reforming, i.e. injection of steam only
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25J—LIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2205/00—Processes or apparatus using other separation and/or other processing means
    • F25J2205/40—Processes or apparatus using other separation and/or other processing means using hybrid system, i.e. combining cryogenic and non-cryogenic separation techniques
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25J—LIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2205/00—Processes or apparatus using other separation and/or other processing means
    • F25J2205/80—Processes or apparatus using other separation and/or other processing means using membrane, i.e. including a permeation step
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25J—LIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2215/00—Processes characterised by the type or other details of the product stream
    • F25J2215/02—Mixing or blending of fluids to yield a certain product
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F25—REFRIGERATION OR COOLING; COMBINED HEATING AND REFRIGERATION SYSTEMS; HEAT PUMP SYSTEMS; MANUFACTURE OR STORAGE OF ICE; LIQUEFACTION SOLIDIFICATION OF GASES
    • F25J—LIQUEFACTION, SOLIDIFICATION OR SEPARATION OF GASES OR GASEOUS OR LIQUEFIED GASEOUS MIXTURES BY PRESSURE AND COLD TREATMENT OR BY BRINGING THEM INTO THE SUPERCRITICAL STATE
    • F25J2245/00—Processes or apparatus involving steps for recycling of process streams
    • F25J2245/02—Recycle of a stream in general, e.g. a by-pass stream

Abstract

提供将碳质组合物催化转化成包含甲烷的气体物流的方法。此外，该方法生成富氢气体物流，和任选富一氧化碳气体物流，它们可以混合或单独用作后继催化气化过程的能源。

Description

从气体物流中分离甲烷的方法
发明领域
本发明涉及将碳质原料催化转化成包含在气体物流中的多种气体产物以及从该气体物流中分离甲烷的方法。特别地，本发明涉及将碳质原料催化转化成包含在气体物流中的多种气体产物以及将甲烷与一氧化碳和氢以如下方式分离的方法：所述方式使得氢和一氧化碳可再循环用于该催化气化法。
发明背景
考虑到许多因素，如更高的能源价格和环境考虑，由较低燃料价值的碳质原料，如生物质、煤和石油焦生产增值气体产物受到新的关注。例如在US3828474、US3998607、US4057512、US4092125、US4094650、US4204843、US4468231、US4500323、US4541841、US4551155、US4558027、US4606105、US4617027、US4609456、US5017282、US5055181、US6187465、US6790430、US6894183、US6955695、US2003/0167961A1、US2006/0265953A1、US2007/000177A1、US2007/083072A1、US2007/0277437A1和GB1599932中公开了此类材料的催化气化以制造甲烷和其它增值气体。
较低燃料价值的碳质原料在上述参考资料中所述的条件下的反应通常产生粗产物气体和炭。该粗产物气体典型包含一定量的粒子，将其从该气体物流中除去以产生气体流出物。这种气体流出物典型含有气体的混合物，包括但不限于，甲烷、二氧化碳、氢、一氧化碳、硫化氢、氨、未反应的水蒸气、夹带的细粒和其它污染物，如COS。通过本领域已知的方法，可以处理该气体流出物以除去二氧化碳、硫化氢、水蒸气、夹带的细粒、COS和其它污染物，从而产生包含甲烷、一氧化碳和氢的净化的气体物流。可任选在氢分离前的某时刻除去或转化一氧化碳以产生包含甲烷和氢的净化的气体物流。
对于一些用途，回收富含甲烷的气体物流可能是合意的。在一些情况下，回收几乎完全包含甲烷的气体物流可能更加合意。在这样的情况下，该净化的气体物流必须经过额外加工以除去几乎所有氢，和如果存在的话，一氧化碳。另一方面，氢和氢与一氧化碳的混合物(“合成气”)可用作能源或原材料源。
在一些情况下，如在本发明的情况下，可能合意的是，收集氢和任选一氧化碳并使它们作为后继催化气化过程的原材料或能源再循环。因此，仍然需要能够有效回收甲烷以及能够回收一氧化碳和氢的分离气体物流的方法。
附图说明
图1描绘了阐述碳质原料气化的连续法的方框图，其中该方法包括甲烷与氢和任选一氧化碳分离以及氢和一氧化碳再循环用于该催化气化法。
发明内容
在第一方面中，本发明提供将碳质原料转化成包含在气体物流中的多种气体产物以及从该气体物流中分离氢和甲烷的方法，该方法包括下列步骤：(a)向气化反应器供应碳质原料；(b)在该气化反应器中在水蒸气和气化催化剂存在下、在合适的温度和压力下使该碳质原料反应形成包含甲烷、氢、一氧化碳、二氧化碳和一种或多种另外的气态副产物的第一气体物流；(c)从所述第一气体物流中除去极大部分的二氧化碳和极大部分的所述一种或多种另外的气态副产物以产生包含甲烷、氢和任选一氧化碳的第二气体物流；(d)从所述第二气体物流中至少部分分离氢以形成富氢气体物流和贫氢气体物流，其中该贫氢气体物流包含甲烷、任选一氧化碳和最多大约4摩尔％氢；其中，如果该贫氢气体物流的热值小于950btu/scf(折干计算)和如果该贫氢气体物流包含1000ppm或更多的一氧化碳：(1)从该贫氢气体物流中至少部分分离一氧化碳以形成(i)富一氧化碳气体物流和(ii)热值为至少950btu/scf(折干计算)的富甲烷气体物流；或(2)将该贫氢气体物流中的一氧化碳至少部分甲烷化以形成富甲烷气体物流。
在第二方面中，本发明提供将碳质原料转化成包含在气体物流中的多种气体产物以及从该气体物流中分离氢和甲烷的方法，该方法包括下列步骤：(a)向反应器供应第一碳质原料；(b)在该反应器中在氧存在下、在合适的温度和压力下至少部分燃烧所述第一碳质原料以生成(i)热能和(ii)包含氢、一氧化碳和二氧化碳的燃烧气体物流；(c)利用来自所述第一碳质原料的燃烧的热能生成水蒸气；(d)将至少一部分所述水蒸气、至少一部分所述燃烧气体物流、第二碳质原料和气化催化剂引入气化反应器；(e)在该气化反应器中在水蒸气和气化催化剂存在下在合适的温度和压力下使所述第二碳质原料反应形成包含甲烷、氢、一氧化碳、二氧化碳和一种或多种另外的气态副产物的第一气体物流；(f)从所述第一气体物流中除去极大部分的二氧化碳和极大部分的所述一种或多种气态副产物以产生包含甲烷、氢和任选一氧化碳的第二气体物流；(g)从所述第二气体物流中至少部分分离氢以形成富氢气体物流和贫氢气体物流，其中该贫氢气体物流包含甲烷、任选一氧化碳和最多大约4摩尔％氢；其中，如果该贫氢气体物流的热值小于950btu/scf(折干计算)和如果该贫氢气体物流包含1000ppm或更多的一氧化碳：(1)从该贫氢气体物流中至少部分分离一氧化碳以形成(i)富一氧化碳气体物流和(ii)热值为至少950btu/scf(折干计算)的富甲烷气体物流；或(2)将该贫氢气体物流中的一氧化碳至少部分甲烷化以形成富甲烷气体物流。
详述
本发明涉及将碳质原料转化成包含在气体物流中的多种气体产物以及将甲烷与该气体物流中的其它气体产物分离的方法。本发明提供以允许回收氢气体物流和任选单独的一氧化碳气体物流的方式分离甲烷的方法。尽管本发明的方法可用于多种气化法，但该方法在希望回收基本纯的甲烷气体物流和基本纯的氢气体物流的情况中特别有用。由此，该氢可用作能源或原材料，或可以与受控量的一氧化碳混合产生针对所需用途定制的合成气。本发明特别提供连续催化气化法，其产生管道级甲烷并且也回收氢和任选一氧化碳以便在该催化气化法中再循环。
可以例如利用共有US2007/0000177A1、US2007/0083072A1、US2007/0277437A1和US2009/0048476A1；和美国专利申请序号Nos.12/234,012(2008年9月19日提交)和12/234,018(2008年9月19日提交)中公开的催化气化技术的任何发展实施本发明。
此外，可以与各自在2008年12月28日提交的下列美国专利申请的主题联合实施本发明：序号No.12/342,554，名为“CATALYTIC GASIFICATION PROCESS WITH RECOVERY OF ALKALIMETAL FROM CHAR”；序号No.12/342,565，名为“PETROLEUM COKE COMPOSITIONS FOR CATALYTIC GASIFICATION”；序号No.12/342,578，名为“COAL COMPOSITIONS FOR CATALYTIC GASIFICATION”；序号No.12/342,596，名为“PROCESSES FOR MAKING SYNTHESIS GAS AND SYNGAS-DERIVED PRODUCTS”；序号No.12/342,608，名为“PETROLEUM COKE COMPOSITIONS FOR CATALYTIC GASIFICATION”；序号No.12/342,628，名为“PROCESSES FOR MAKING SYNGAS-DERIVED PRODUCTS”；序号No.12/342,663，名为“CARBONACEOUS FUELS AND PROCES SES FOR MAKING AND USING THEM”；序号No.12/342,715，名为“CATALYTIC GASIFICATION PROCESS WITH RECOVERY OF ALKALIMETAL FROM CHAR”；序号No.12/342,736，名为“CATALYTIC GASIFICATION PROCESS WITH RECOVERY OF ALKALI METAL FROM CHAR”；序号No.12/343,143，名为“CATALYTIC GASIFICATION PROCESS WITH RECOVERY OF ALKALI METAL FROM CHAR”；序号No.12/343,149，名为“STEAM GENERATING SLURRY GASIFIER FOR THE CATALYTIC GASIFICATION OF A CARBONACEOUS FEEDSTOCK”；和序号No.12/343,159，名为“CONTINUOUS PROCESSES FOR CONVERTING CARBONACEOUS FEEDSTOCK INTO GASEOUS PRODUCTS”。
此外，可以与各自在2008年2月27日提交的下列美国专利申请的主题联合实施本发明：序号No.12/395,293，名为“PROCESSES FOR MAKING ABSORBENTS AND PROCESSES FOR REMOVING CONTAMINANTS FROM FLUIDS USING THEM”；序号No.12/395,309，名为“STEAM GENERATION PROCESSES UTILIZING BIOMASS FEEDSTOCKS”；序号No.12/395,320，名为“REDUCED CARBON FOOTPRINT STEAM GENERATION PROCESSES”；序号No.12/395,330，名为“PROCESS AND APPARATUS FOR THE SEPARATION OF METHANE FROM A GASSTREAM”；序号No.12/395,344，名为“SELECTIVE REMOVAL AND RECOVERY OF ACID GASES FROM GASIFICATION PRODUCTS”；序号No.12/395,348，名为“COAL COMPOSITIONS FOR CATALYTIC GASIFICATION”；序号No.12/395,353，名为“COAL COMPOSITIONS FOR CATALYTIC GASIFICATION”；序号No.12/395,372，名为“CO-FEED OF BIOMASS AS SOURCE OF MAKEUP CATALYSTS FOR CATALYTIC COAL GASIFICATION”；序号No.12/395,381，名为“COMPACTOR-FEEDER”；序号No.12/395,385，名为“CARBONACEOUS FINES RECYCLE”；序号No.12/395,429，名为“BIOMASS CHAR COMPOSITIONS FOR CATALYTIC GASIFICATION”；序号No.12/395,433，名为“CATALYTIC GASIFICATION PARTICULATE COMPOSITIONS”；和序号No.12/395,447，名为“BIOMASS COMPOSITIONS FOR CATALYTIC GASIFICATION”。
也可以与和其同时提交的美国专利申请序号No.__/____,____(代理人案号no.FN-0033，名为“SOUR SHIFT PROCESS FOR THE REMOVAL OF CARBON MONOXIDE FROM A GAS STREAM”)的主题联合实施本发明。
如果没有另行指明，本文中提到的所有出版物、专利申请、专利和其它参考资料，包括但不限于上文提及的那些，就像充分阐述一样明确地出于各种目的全文经此引用并入本文。
除非另行规定，本文所用的所有技术和科学术语具有与本发明所属领域的普通技术人员的通常理解相同的含义。在冲突的情况下，以本说明书，包括定义为准。
除非明文指明，商标以大写体显示。
尽管在本发明的实践或测试中可以使用与本文所述的那些类似或等效的方法和材料，但本发明中描述了合适的方法和材料。
除非另行指明，所有百分比、份数、比率等按重量计。
在量、浓度或其它值或参数作为范围或一系列上限和下限值给出时，这被理解为明确公开由任何一对任何上和下范围界限形成的所有范围，无论是否独立公开这些范围。在本文中列举数值范围时，除非另行指明，该范围旨在包括其端点和在该范围内的所有整数和分数。无意将本发明的范围限制于在规定某范围时列举的具体数值。
当使用术语“大约”描述数值或范围的端点时，本发明应被理解为包括所提到的所述具体数值或端点。
本文所用的术语“包含”、“包括”、“具有”或它们的任何其它变体旨在涵盖非排他性的包含。例如，包含一系列要素的工艺、方法、制品或装置不一定仅限于这些要素，而是可包括未明确列举的或此类工艺、方法、制品或装置所固有的其它要素。此外，除非明确作出相反的指示，“或”是指可兼性的“或”而非排他性的“或”。例如，下列任一项都满足条件A或B：A真(或存在)且B假(或不存在)，A假(或不存在)且B真(或存在)，A和B都真(或存在)。
本文中使用“某”和“某个”描述各种要素和组分仅是为方便起见和给出本发明的一般含义。这种描述应被解释为包括一或至少一，单数也包括复数，除非明显看出无意如此。
本文中的材料、方法和实施例仅用于举例说明，且除非明确规定，它们不是限制性的。
气化法
本发明的气体回收法在将碳质原料，如石油焦、液体石油残渣、沥青质、生物质和/或煤转化成可燃气体，如甲烷的集成气化法中特别有用。
用于此类方法的气化反应器典型地在适度高的压力和温度下运行，要求在保持原料的所需温度、压力和流速的同时将碳质材料(即原料)引入该气化反应器的反应区。本领域技术人员熟悉用于向高压和/或高温环境提供原料的进料系统，包括星形加料器、螺旋进料器、旋转活塞和闭锁料斗。应该理解的是，该进料系统可包括会交替使用的两个或更多个压力平衡元件，如闭锁料斗。
由原料制备操作向该催化气化器提供催化的原料，所述催化的原料通常包含如下论述的碎碳质材料和气化催化剂的颗粒组合物。在一些情况下，该催化的原料可以在比催化气化器的运行压力高的压力条件下制备。因此，该催化的原料可以在不进一步加压的情况下直接送入催化气化器。
可以使用若干催化气化器的任一种。合适的气化器包括逆流固定床、并流固定床、流化床、气流床(entrained flow)和移动床反应器。在前面并入的US6955695中公开了用于气化液体进料，如液体石油残渣的催化气化器。
该催化气化器中的压力典型可以为大约10至大约100atm(大约150至大约1500psig)。该气化反应器温度可以保持在至少大约450℃，或至少大约600℃，或至少大约900℃，或至少大约750℃，或大约600℃至大约700℃左右；并在至少大约50psig，或至少大约200psig，或至少大约400psig，至大约1000psig，或至大约700psig，或至大约600psig的压力。
用于该颗粒组合物的加压和反应的催化气化器中所用的气体包含水蒸气和任选氧或空气，并按需要根据本领域技术人员已知的方法供应给该反应器。
例如，可以由本领域技术人员已知的可向该反应器供应水蒸气的任何水蒸气锅炉向该催化气化器供应水蒸气。此类锅炉可以例如通过使用任何碳质材料，如粉煤、生物质等供能，包括但不限于，来自该颗粒组合物制备操作的废弃碳质材料(例如上述细粉)，来提供能量。也可以由连向燃气轮机的第二气化反应器供应水蒸气，其中来自该反应器的废气与水源热交换并产生水蒸气。或者，可以如之前并入的美国专利申请序号Nos.12/343,149、12/395,309和12/395,320中所述向该气化反应器提供水蒸气。
来自其它工艺操作的再循环的水蒸气也可用于向该催化气化器补充水蒸气。例如，在该催化的原料的制备中，当如下所述用流化床淤浆干燥器干燥已制浆的颗粒组合物时，可以将生成的水蒸气送入该催化气化反应器。
可通过以本领域技术人员已知的任何方法过热送入该气化反应器的水蒸气和再循环气体的气体混合物来提供该催化气化器可能所需的少量热输入。在一个方法中，可以将CO和H2的压缩再循环气体与水蒸气混合，且所得水蒸气/再循环气体混合物可通过与催化气化器流出物热交换随后在再循环气体炉中过热来进一步过热。
在该方法中可任选包括甲烷重整器以补充该再循环CO和H2物流和来自淤浆气化器的废气以确保向反应器供应充足的再循环气体，从而使反应净热尽可能接近中性(仅略微放热或吸热)，换言之，该催化气化器在基本热中性条件下运行。在这些情况下，可以如下所述由甲烷产物向该重整器供应甲烷。
该催化的原料在催化气化器中在所述条件下的反应提供来自该催化气化反应器的粗产物气体和炭。
典型地以连续或分批方式从该催化气化器中除去在该催化气化器工艺中制成的炭以便取样、吹扫和/或回收催化剂。除炭法是本领域技术人员公知的。可以使用例如EP-A-0102828教导的一种这样的方法。可以通过闭锁料斗系统从该催化气化反应器中定期取出炭，但是本领域技术人员已知其它方法。
通常，将来自该催化气化器的炭送往催化剂回收和再循环工艺。已经开发出从所述固体废料(purge)中回收碱金属的方法以降低原材料成本和使催化气化法的环境影响最小化。例如，该炭可以用再循环气体和水淬火并送往用于提取和再利用该碱金属催化剂的催化剂再循环操作。在US4459138以及之前并入的US4057512和US2007/0277437A1和之前并入的美国专利申请序号Nos.12/342,554、12/342,715、12/342,736和12/343,143中描述了特别有用的回收和再循环法。进一步工艺细节可参考这些文献。
在催化剂回收完成后，可以将基本不含气化催化剂的炭和回收的催化剂(溶液或固体形式)送往包含催化的原料制备法和淤浆原料制备法的原料制备操作。
碳质原料
本文所用的术语“碳质原料”包括碳源，典型地煤、石油焦、沥青质和/或液体石油残渣，但可宽泛地包括适用于气化的任何碳源，包括生物质。
本文所用的术语“石油焦”包括(i)在石油加工中获得的高沸点烃馏分的固体热分解产物(重质残渣-“残油petcoke”)和(ii)加工焦油砂的固体热分解产物(沥青砂或油砂-“焦油砂petcoke”)。此类碳化产物包括，例如，生焦、煅烧焦、针状焦和流化床石油焦。
残油petcoke可衍生自原油，例如，通过用于将强重力残留原油升级的焦化法，该石油焦含有灰分作为次要组分，典型地为该焦炭重量的大约1.0重量％或更少，更典型大约0.5重量％或更少。典型地，此类低灰分焦炭中的灰分主要包含金属，如镍和钒。
焦油砂petcoke可衍生自油砂，例如通过用于将油砂升级的焦化法。焦油砂petcoke含有灰分作为次要组分，典型为该焦油砂petcoke总重量的大约2重量％至大约12重量％，更典型大约4重量％至大约12重量％。典型地，此类高灰分焦炭中的灰分主要包含材料比如硅和/或铝的化合物。
该石油焦可包含该石油焦总重量的至少大约70重量％碳，至少大约80重量％碳，或至少大约90重量％碳。典型地，该石油焦包含该石油焦重量的少于大约20重量％的无机化合物。
本文所用的术语“沥青质”在室温下是芳族碳质固体，并可以衍生自例如原油和原油焦油砂的加工。
本文所用的术语“液体石油残渣”包括(i)在石油加工中获得的高沸点烃馏分的液体热分解产物(重质残渣-“残油液体石油残渣”)和(ii)加工焦油砂的液体热分解产物(沥青砂或油砂-“焦油砂液体石油残渣”)。该液体石油残渣在室温下是基本非固体；例如，其可呈现粘稠流体或淤渣形式。
残油液体石油残渣也可衍生自原油，例如，通过用于将强重力原油蒸馏残渣升级的方法。此类液体石油残渣含有灰分作为次要组分，典型为该残渣重量的大约1.0重量％或更少，更典型大约0.5重量％或更少。典型，此类低灰分残渣中的灰分主要包含金属，如镍和钒。
焦油砂液体石油残渣可衍生自油砂，例如通过用于将油砂升级的方法。焦油砂液体石油残渣含有灰分作为次要组分，典型为该残渣总重量的大约2重量％至大约12重量％，更典型大约4重量％至大约12重量％。典型地，此类高灰分残渣中的灰分主要包含材料比如硅和/或铝的化合物。
本文所用的术语“煤”是指泥炭、褐煤、次烟煤、烟煤、无烟煤或其混合物。在某些实施方案中，该煤具有总煤重量的按重量计小于大约85％，或小于大约80％，或小于大约75％，或小于大约70％，或小于大约65％，或小于大约60％，或小于大约55％，或小于大约50％的碳含量。在另一些实施方案中，该煤具有总煤重量的按重量计最多大约85％，或最多大约80％，或最多大约75％的碳含量。可用的煤的实例包括，但不限于，Illinois#6、Pittsburgh#8、Beulah(ND)、Utah Blind Canyon和Powder River Basin(PRB)煤。无烟煤、烟煤、次烟煤和褐煤可分别含有折干计算为煤总重量的大约10重量％，大约5至大约7重量％，大约4至大约8重量％和大约9至大约11重量％的灰分。但是，如本领域技术人员熟悉的那样，任何特定煤源的灰分含量取决于该煤的等级和来源。参见例如，Coal Data：A Reference，Energy Information Administration，Office of Coal，Nuclear，Electric and Alternate Fuels，U.S.Department of Energy，DOE/EIA-0064(93)，1995年2月。
本文所用的术语“灰分”包括该碳源中存在的无机化合物。该灰分典型包括硅、铝、钙、铁、钒、和硫等的化合物。此类化合物包括无机氧化物，如二氧化硅、氧化铝、三氧化二铁等，也可能包括含有硅、铝、钙、铁和钒中的一种或多种的各种矿物质。术语“灰分”可用于表示气化前的碳源中存在的此类化合物，也可用于表示气化后的炭中存在的此类化合物。
负载催化剂的碳质原料
该碳质组合物通常载有一定量的碱金属化合物以促进水蒸气气化成甲烷。典型地，该组合物中碱金属化合物的量足以提供从大约0.01，或从大约0.02，或从大约0.03，或从大约0.04，到大约0.06，到大约0.07，或到大约0.08，或到大约0.1的碱金属原子/碳原子比率。此外，该碱金属典型地被加载到碳源上以实现按质量计是该碳质材料(例如煤和/或石油焦)的总灰分含量的大约3至大约10倍大的碱金属含量。
适合用作气化催化剂的碱金属化合物包括选自碱金属碳酸盐、碳酸氢盐、甲酸盐、草酸盐、氨化物、氢氧化物、乙酸盐、卤化物、硝酸盐、硫化物和多硫化物的化合物。例如，该催化剂可包含Na2CO3、K2CO3、Rb2CO3、Li2CO3、Cs2CO3、NaOH、KOH、RbOH或CsOH中的一种或多种，特别是碳酸钾和/或氢氧化钾。
本领域技术人员已知的任何方法可用于使一种或多种气化催化剂与该碳质组合物结合。此类方法包括，但不限于，与固体催化剂源混合和将该催化剂浸渍到该碳质固体上。可以使用本领域技术人员已知的几种浸渍方法来结合该气化催化剂。这些方法包括，但不限于，初湿含浸、蒸发浸渍、真空浸渍、浸泡浸渍和这些方法的组合。气化催化剂可通过用该催化剂的溶液(例如水溶液)制浆来浸渍到碳质固体中。
具有适用在气化反应器中的粒度的那部分颗粒碳质原料可随后通过本领域已知的，例如如之前并入的US4069304、US4092125、US4468231、US4551155和US5435940；和之前并入的美国专利申请序号Nos.12/234,012、12/234,018、12/342,565、12/342,578、12/342,608、12/343,159、12/342,578和12/342,596中公开的方法进一步加工，以例如浸渍一种或多种催化剂和/或助催化剂。
在之前并入的US2009/0048476A1中描述了适用于将煤颗粒与气化催化剂合并以提供催化的碳质原料的一种特定方法，其中该催化剂已通过离子交换与该煤颗粒结合。使通过离子交换机制进行的催化剂载量最大化(基于为煤专门开发的吸附等温线)，并控制留在湿颗粒上的附加催化剂，包括在孔隙内的那些，从而以受控方式获得总催化剂目标值。此类加载提供湿滤饼形式的催化的煤颗粒。负载该催化剂且脱水的湿煤饼典型地含有例如大约50％水分。如相关领域普通技术人员基于原料煤的特性容易确定的那样，通过控制溶液中催化剂组分的浓度以及接触时间、温度和方法，控制负载的催化剂总量。
在本发明的实施方案中，不需要使整个碳质原料负载气化催化剂。在一些实施方案中，只有一部分碳质原料负载气化催化剂。在此类实施方案中，该碳质原料(部分负载和部分无负载)可任选与气化催化剂干混。但是，在其他实施方案中，基本所有碳质原料负载气化催化剂。但是，在这些实施方案中，该负载的碳质原料可任选与一定量的气化催化剂干混。
该催化的原料可以储存以便将来使用或转移到进料操作中以引入到该气化反应器中。该催化的原料可根据本领域技术人员已知的任何方法输送至储存或进料操作，例如螺旋输送机或气动输送。
水蒸气产生
向该气化反应器供应的水蒸气可源自各种来源，包括商业气化反应器、含氧燃料燃烧器和锅炉。碳质原料的气化或燃烧反应产生大量热能。有利地，这种热能可用于接触任何类型的热交换器，所述热交换器也与水源接触，由此生成水蒸气。例如，本领域技术人员已知的任何锅炉都可向该反应器供应水蒸气。尽管任何水源都可用于产生水蒸气，但将已知锅炉系统中常用的水提纯和去离子(大约0.3-1.0microsiemens/cm)以减缓腐蚀过程。此类锅炉可以例如通过任何碳质材料，包括粉煤/粉状煤、生物质和来自原料制备操作的废弃碳质材料(例如上述细粉)的燃烧供能。来自碳质材料燃烧的热能加热该锅炉中的水，其最终转化成水蒸气(在大约700℉和3,200psi)。将该水蒸气从锅炉送入典型地位于该炉中位于运载燃烧气体的出口管处或附近的被加热的管。该水蒸气可经由被加热的导管送往气化反应器，其可用于干燥碳质原料，或其可被准备和送往发电用的水蒸气轮机。为避免该水蒸气在运输过程中的过度冷却，也可以在将该水蒸气输送至其终点之前将运载水蒸气用的被加热的导管过热(例如通过与热交换器接触)。在之前并入的美国专利申请序号Nos.12/395,309和12/395,320中描述了合适的水蒸气产生方法。
水蒸气也可以由与燃烧轮机连接的第二气化反应器供应，其废气接触与水源(其可包括如上所述的锅炉系统)接触的热交换器以产生水蒸气。
来自其它工艺操作的再循环的水蒸气也可用于向该反应器供应水蒸气。例如，当已制浆的碳质原料如本文所述用流化床淤浆干燥器干燥时，可以将经由气化生成的水蒸气送入该气化反应器。类似地，如之前并入的美国专利申请序号No.12/343,149中所述，可以由淤浆气化器直接生成水蒸气，该淤浆气化器由含水的碳质进料淤浆产生水蒸气和合成气。至少一部分该水蒸气也可用于驱动发电的水蒸气轮机。
粗产物气体的处理
离开该催化气化器的粗产物气体流出物可通过充当分离区的反应器的一部分，在此将太重以致无法被离开该反应器的气体夹带的粒子(即细粒)送回流化床。该分离区可包括用于从该气体中除去细粒和颗粒的一个或多个内旋风分离器或类似装置。通过该分离区并离开催化气化器的气体流出物通常含有CH4、CO2、H2和CO、H2S、NH3、未反应的水蒸气、夹带的细粒和其它污染物，如COS。
已从中除去细粒的气体物流可随后通过热交换器以冷却该气体，且回收的热可用于预热再循环气体和生成高压水蒸气。也可以通过任何合适的装置(如外旋风分离器，任选随后文丘里洗涤器)除去残留的夹带的细粒。可以加工该回收的细粒以回收碱金属催化剂，该催化剂随后送往淤浆原料制备过程或送回催化气化反应器，或如之前并入的美国专利申请序号No.12/395,385中所述直接再循环回原料制备。
将已从中除去细粒的气体物流送入任选包含用于除去COS(酸法(sour process))的COS水解反应器的气体提纯操作，并在热交换器中进一步冷却以回收残热。COS水解法是本领域技术人员已知的，例如参见US4100256。
在除去COS后，该气体物流通常含有CH4、CO2、H2、CO、H2S、NH3和水蒸气。这种气体物流可以在水洗涤器中进一步处理以回收氨，从而产生包含至少H2S、CO2、CO、H2和CH4的洗过的气体。
可以加工洗涤器水和酸法冷凝物以解吸和回收H2S、CO2和NH3；此类方法是本领域技术人员公知的。NH3典型地能够以水溶液(例如20重量％)形式回收。
可以在该方法的任何阶段通过并入酸气变换反应来从气体物流中除去一氧化碳。酸气变换涉及使水蒸气和CO在合适的条件下反应产生CO2和H2。在例如US7074373中详细描述了这种酸气变换法。在之前并入的美国专利申请序号No.__________(代理人案号no.FN-0033，名为“SOUR SHIFT PROCESS FOR THE REMOVAL OF CARBON MONOXIDE FROM A GAS STREAM”)中描述了其在催化气化法中的用途。该方法典型地包括加入水或利用该气体中所含的水，并使所得水-气体混合物在水蒸气重整催化剂上绝热反应。典型的水蒸气重整催化剂包括在耐热载体上的一种或多种第VIII族金属。该酸气变换可例如除去该处理的气体物流中的至少大约80％，或至少大约90％，或至少大约95％，或至少大约99％的CO。
在含CO的气体物流上进行酸气变换反应的方法和反应器在一般意义上是本领域技术人员公知的。合适的反应条件和合适的反应器可以随必须从该气体物流中脱除的CO的量而变。在一些实施方案中，该酸气变换可以在单一阶段中在从大约100℃，或从大约150℃，或从大约200℃，到大约250℃，或到大约300℃，或到大约350℃的温度范围内进行。在这些实施方案中，可以用本领域技术人员已知的任何合适的催化剂催化该变换反应。此类催化剂包括，但不限于，Fe2O3-基催化剂，如Fe2O3-Cr2O3催化剂，和其它基于过渡金属的和基于过渡金属氧化物的催化剂。在其他实施方案中，可以在多个阶段中进行该酸气变换。在一个具体实施方案中，在两个阶段中进行该酸气变换。这种两阶段法使用高温序列，随后低温序列。该高温变换反应的气体温度为大约350℃至大约1050℃。典型的高温催化剂包括，但不限于，任选与较少量的氧化铬结合的氧化铁。低温变换的气体温度为大约150℃至大约300℃，或大约200℃至大约250℃。低温变换催化剂包括，但不限于，可负载在氧化锌或氧化铝上的氧化铜。
通常用热交换器和水蒸气产生器进行水蒸气变换以便有效利用热能。利用这些构件的变换反应器是本领域技术人员公知的。在之前并入的US7074373中阐述了合适的变换反应器的一个实例，尽管本领域技术人员已知的其它设计也有效。
可以使用后继酸性气脱除过程通过物理吸收法——其涉及该气体的溶剂处理以产生净化的气体物流——从该洗过的气体物流中除去H2S和CO2。此类方法包括使洗过的气体与溶剂，如单乙醇胺、二乙醇胺、甲基二乙醇胺、二异丙基胺、二乙二醇胺、氨基酸钠盐的溶液、甲醇、或热碳酸钾等接触。一种方法能够涉及使用SELEXOL
Figure BPA00001232790200141
(UOP LLC，Des Plaines，IL USA)或RECTISOL
Figure BPA00001232790200142
(Lurgi AG，Frankfurt am Main，Germany)溶剂，其具有两个串列；各串列由H2S吸收剂和CO2吸收剂构成。含有H2S、CO2和其它污染物的该废溶剂可通过本领域技术人员已知的任何方法再生，包括使该废溶剂与水蒸气或其它解吸气接触以除去污染物或使该废溶剂通过解吸塔。可以将回收的酸性气送往硫回收加工；例如，可以通过本领域技术人员已知的任何方法，包括Claus法将来自酸性气脱除和酸水解吸的任何回收的H2S转化成元素硫。硫可以以熔融液体形式回收。可以将解吸过的水送往在催化的原料的制备中循环再利用。在之前并入的美国专利申请序号No.12/395,344中描述了从洗过的气体物流中除去酸性气的一种方法。
有利地，在该方法中，无论是在水蒸气产生中还是在催化气化中还是在两者中(和在任选的酸气变换中)生成的CO2，可回收用于后继使用或封存，从而能够极大降低碳足迹(与原料的直接燃烧相比)。在之前并入的美国专利申请序号Nos.12/395,309和12/395,320中描述了降低碳足迹的方法。
离开该气体提纯操作的所得净化的气体物流含有显著量的CH4和H2和任选CO，也可含有少量CO2和H2O。
根据本发明，这种净化的气体物流可进一步加工以提供氢与该气体物流中的其它气体产物的至少部分分离。这导致形成富氢气体物流和贫氢气体物流。该富氢气体物流包含至少大约70摩尔％，或至少大约80摩尔％，或至少大约90摩尔％，或至少大约97摩尔％氢气。在一些实施方案中，该富氢气体物流基本包含氢气，具有例如至少大约90摩尔％氢气。该贫氢气体物流至少包含甲烷。在一些实施方案中，该贫氢气体物流至少包含甲烷和一氧化碳，也可包含最多大约4摩尔％氢。
实施氢分离的各种方法是本领域技术人员已知的。此类方法包括深冷分离和基于膜的分离。对于该净化的气体物流不含显著量一氧化碳(例如少于大约1000ppm CO)的实施方案，可以通过如之前并入的美国专利申请序号No.12/395,330中所示的涉及形成甲烷水合物的方法实施该分离。
该贫氢气体物流至少包含甲烷。在一些实施方案中，该贫氢气体物流应具有至少950btu/scf(折干计算)的热值。例如，在一些实施方案中，该贫氢气体物流包含至少大约80摩尔％，或至少大约90摩尔％，或至少大约95摩尔％甲烷。但是，在一些实施方案中，该贫氢气体物流至少包含甲烷和一氧化碳和任选次要量的氢(通常大约4摩尔％或更少)。在一些这样的实施方案中，该脱氢气体包含至少大约1000ppm一氧化碳。在另一些实施方案中，该贫氢气体物流基本不含一氧化碳，具有例如少于大约1000ppm一氧化碳。
在该贫氢气体物流包含1000ppm或更多一氧化碳和该贫氢气体物流的热值小于950btu/scf(折干计算)的实施方案中，该贫氢气体物流中的甲烷和该贫氢气体物流中的一氧化碳可以至少部分彼此分离。甲烷和一氧化碳的这种部分分离产生至少富甲烷气体物流和富一氧化碳气体物流。该富甲烷气体物流包含至少大约80摩尔％，或至少大约90摩尔％，或至少大约95摩尔％甲烷。此外，在典型实施方案中，该富甲烷气体物流具有至少大约950btu/scf(折干计算)的热值。该富一氧化碳气体物流包含至少大约50摩尔％，或至少大约65摩尔％，或至少大约80摩尔％，或至少大约90摩尔％一氧化碳。
在该分离产生基本包含甲烷的富甲烷气体物流的本发明的实施方案中，该甲烷物流可以回收和用作高品质能源。例如，可以将该甲烷压缩和引入现有天然气管道系统中。或者，一部分该甲烷产物也可用作燃气轮机用的装置燃料。
在一些实施方案中，富甲烷气体物流(例如贫氢气体物流)如果含有显著量CO，可通过进行调整型甲烷化(trim methanantion)以降低CO含量来进一步富集甲烷。可以使用本领域技术人员已知的任何合适的方法和装置，包括例如US4235044中公开的方法和装置进行调整型甲烷化。
在该分离产生基本包含氢的富氢气体物流的本发明的实施方案中，该氢气物流可以回收和用作能源和/或反应物。例如，该氢可用作氢基燃料电池的能源，或用在后继催化气化法中。在另一实例中，氢可以如之前并入的美国专利申请序号Nos.12/395,309和12/395,320中所述；或如之前并入的美国专利申请序号No.__________(代理人案号no.FN-0033，名为“SOUR SHIFT PROCESS FOR THE REMOVAL OF CARBON MONOXIDE FROM A GAS STREAM”)中所公开用作水蒸气产生法用的燃料。
在该分离产生基本包含一氧化碳的富一氧化碳气体物流的本发明的实施方案中，该一氧化碳物流可回收和用作燃料混合物的一部分(例如与氢一起)，或用在后继催化气化法中。该一氧化碳气体物流也可以如之前并入的12/395,309和12/395,320中所述；或如之前并入的美国专利申请序号No.__________(代理人案号no.FN-0033，名为“SOUR SHIFT PROCESS FOR THE REMOVAL OF CARBON MONOXIDE FROM A GAS STREAM”)中所公开与氢结合和用作水蒸气产生法用的燃料。
在本发明的一些实施方案中，该氢直接和/或经由如下论述的另一单元操作再循环回该催化气化器。
使用甲烷分离选项的连续气化法
本发明还提供连续催化气化法，其中使氢和任选一氧化碳再循环并用在该催化气化法中。
1.将碳质原料引入气化反应器
本发明的方法要求向气化反应器供应碳质原料和气体进料(包含水蒸气、一氧化碳和氢)。
上文描述了合适的气化反应器和碳质原料。在典型实施方案中，该碳质原料以颗粒形式提供，但是这不需要是所有实施方案中的情况。在典型实施方案中，该碳质原料载有合适的气化催化剂，或至少部分与合适的气化催化剂混合。上文描述了合适的催化剂。典型方法至少包括碳酸钾和/或氢氧化钾。
在一些实施方案中，也可以在与碳质原料的引入相同的步骤中将水蒸气引入该气化反应器。可通过本领域技术人员已知的任何合适的水蒸气产生法生成水蒸气。上文描述了合适的水蒸气产生法。
在一些实施方案中，也可以在与碳质原料的引入相同的步骤中将进料气体物流(除水蒸气外)引入该气化反应器。这种进料气体物流至少包含氢和一氧化碳，还可包括二氧化碳和水蒸气。该进料气体物流可以以各种方式生成。
在一些实施方案中，该进料气体物流包含在甲烷重整器中重整甲烷的产物。在某具体实施方案中，用于该甲烷重整的输入气体是碳质原料的催化气化的甲烷产物的一部分。该甲烷在甲烷重整器中反应产生至少包含一氧化碳和氢气的气体物流。包含CO和H2的这种气体物流可充当作为产物气体物流引入(即再循环到)该气化反应器中的再循环气体物流(与富氢气体物流合并)。
在一些实施方案中，该进料气体物流是燃烧反应产物。在某具体实施方案中，该燃烧反应在反应器(例如吹氧气化器或燃烧反应器)中发生。在氧存在下向该反应器供应碳质原料。该碳质原料可以是或不是颗粒形式，并可具有与用于该催化气化的碳质原料相同或不同的组成。该燃烧法典型产生至少包含CO、H2和CO2，和如果该燃烧法用于生成水蒸气，还包含H2O的所得气体物流。与富氢气体物流结合的该燃烧气体物流可充当作为进料气体物流引入该气化反应器的气体物流。
在一些实施方案中，该进料气体物流包含氢和任选一氧化碳，它们从前一催化气化过程的净化的气体物流中回收。在本文中描述了适用于分离和回收富氢气体物流和富一氧化碳气体物流的方法。
在该进料气体物流是燃烧反应产物的实施方案中，来自该燃烧反应的热能可用作上述水蒸气产生法的热源。
2.碳质原料的催化气化
在气化反应器中在进料气体物流(包括水蒸气)和气化催化剂存在下在合适的温度和压力下使碳质原料反应形成包含甲烷、氢、一氧化碳、二氧化碳和一种或多种另外的气体产物的气体物流。上文描述了催化气化，包括合适的反应器和反应条件。
3.CO2和其它气态副产物的脱除
可以从该气体物流中除去二氧化碳和其它气态副产物(例如硫化氢、氨等)。上文描述了适用于从该气体物流中除去这些气体的方法。该分离产生至少两个气体物流。一个气体物流基本包含氢、甲烷和一氧化碳中的一种或多种。在典型实施方案中，这一气体物流包含至少大约90摩尔％，或至少大约95摩尔％，或至少大约99摩尔％甲烷、氢和/或一氧化碳。这些气体在该气体物流中的相对比例可以随各种因素，包括气化条件和碳质原料的性质而变。另一气体物流包含二氧化碳。在一些实施方案中，可以回收和封存包含二氧化碳的气体物流以实现碳足迹降低。
4.从气体物流中分离氢
在除去CO2和其它气态副产物后，该气体物流包含氢、甲烷和任选一氧化碳。将氢至少部分与该气体物流中的其它气体产物分离。这种分离产生富氢气体物流和贫氢气体物流。该富氢气体物流包含至少大约70摩尔％，或至少大约80摩尔％，或至少大约90摩尔％，或至少大约97摩尔％氢气。在一些实施方案中，该富氢气体物流基本包含氢气，具有例如至少大约90摩尔％氢气。该贫氢气体物流至少包含甲烷。在一些实施方案中，该贫氢气体物流至少包含甲烷和一氧化碳，也可包含最多大约4摩尔％氢。
上文描述了从气体物流中分离氢的合适方式。
在一些实施方案中，该富氢气体物流可以在分离后回收。在此类实施方案中，本发明包括本领域技术人员已知的任何合适的气体回收方式。该回收方法和装置可以随用于实施分离的方式和分离后的所述富集的气体物流的所需用途等因素而变。
5.甲烷和一氧化碳的分离
该贫氢气体物流至少包含甲烷。例如，在一些实施方案中，该贫氢气体物流包含至少大约80摩尔％，或至少大约90摩尔％，或至少大约95摩尔％甲烷。但是，在一些实施方案中，该贫氢气体物流至少包含甲烷和一氧化碳。在一些这样的实施方案中，该脱氢气体包含至少大约1000ppm一氧化碳。在另一些实施方案中，该贫氢气体物流基本不含一氧化碳，具有例如小于大约1000ppm一氧化碳。
在该贫氢气体物流包含1000ppm或更多一氧化碳和该贫氢气体物流的热值小于950btu/scf(折干计算)的实施方案中，该贫氢气体物流中的甲烷和该贫氢气体物流中的一氧化碳可以至少部分相互分离。甲烷和一氧化碳的这种部分分离产生至少富甲烷气体物流和富一氧化碳气体物流。该富甲烷气体物流包含至少大约80摩尔％，或至少大约90摩尔％，或至少大约95摩尔％甲烷。此外，在典型实施方案中，该富甲烷气体物流具有至少大约950btu/scf(折干计算)的热值。该富一氧化碳气体物流包含至少大约50摩尔％，或至少大约65摩尔％，或至少大约80摩尔％一氧化碳。
上文描述了分离甲烷和一氧化碳的合适方式。
在一些实施方案中，该富甲烷气体物流和/或富一氧化碳气体物流可以在分离后回收。在此类实施方案中，本发明包括本领域技术人员已知的任何合适的气体回收方式。该回收方法和装置可以随例如用于实施分离的方式和分离后的所述富集的气体物流的所需用途等因素而变。例如，在该富甲烷气体物流基本包含甲烷的实施方案中，该富甲烷气体物流可通过在合适的加压装置中加压该气体和将该加压甲烷引入天然气管道网络来回收。
进一步工艺细节可参考之前并入的专利和出版物。
管道品质天然气
本发明提供在某些实施方案中可以由碳质原料的催化气化产生管道品质天然气的方法。“管道品质天然气”典型地是指(1)在纯甲烷(其热值在标准大气条件下为1010btu/ft3)的热值的±5％内，和(2)不含水和有毒或腐蚀性污染物的天然气。在本发明的一些实施方案中，上述方法中所述的富甲烷气体物流满足这样的要求。
管道品质天然气可含有不同于甲烷的气体，只要所得气体混合物具有在1010btu/ft3的±5％内的热值并且既无毒又非腐蚀性。因此，富甲烷气体物流可包含热值小于甲烷并仍有资格作为管道品质天然气的气体，只要所述其它气体的存在不会将该气体物流的热值降至低于950btu/scf(折干计算)。因此，富甲烷气体物流可包含最多大约4摩尔％氢并仍充当管道品质天然气。一氧化碳的热值高于氢。因此，管道品质天然气可以在不降低该气体物流的热值的情况下含有甚至更高的CO百分比。适合用作管道品质天然气的富甲烷气体物流优选具有少于大约1000ppm CO。
实施例
下列实施例例证本发明的一个或多个具体实施方案。该实施例仅提供要求保护的本发明的一个或多个实施方案，且无论如何不是限制性的。
实施例1-使用甲烷分离选项的连续法
图1例证本发明涵盖的连续法的若干实施方案。可通过使用湿磨机将一定量的原料湿磨成细粒来制备原料。在研磨后，该原料应具有大约45微米至大约2500微米的粒度。该原料可以从研磨机中取出并引入催化剂加载单元(例如一个或多个淤浆槽)，在此可以将气化催化剂加载到该原料颗粒上。该加载的催化剂可包含从前一气化过程回收的催化剂和原始的补充催化剂的混合物。在将催化剂加载到原料颗粒上后，可以将该负载催化剂的原料引入气化反应器(1)。
该原料应该在气化反应器(1)中在水蒸气存在下转化成包含至少CH4、CO2、H2、CO、H2S、NH3、水蒸气和COS的多种气体产物。该COS可通过在水解反应器(未显示)中进行的水解过程除去。随后可通过在多单元洗涤器装置(作为笼统分离装置(2)的一部分显示)中洗涤该气体来除去氨。然后可以在酸性气脱除法中从该气体物流中基本除去CO2和H2S，该酸性气脱除法涉及使该气体物流在溶剂处理容器(作为笼统分离装置(2)的一部分显示)中暴露在溶剂中。此时，该气体物流应基本包含甲烷、一氧化碳和氢。
任选地，在酸性气脱除过程之前可以使用酸变换反应器(sour shift reactor)将基本所有CO(在水蒸气存在下)转化成CO2和H2。在这种情况下，在酸性气脱除过程后的气体物流应基本包含甲烷和氢。
可通过使该气体物流通过膜分离器(3)来将氢气基本与甲烷和一氧化碳分离。两个气体物流(8，9)离开膜分离器。一个气体物流应基本包含氢(8)。另一气体物流应基本包含甲烷和一氧化碳(9)。
该甲烷和一氧化碳可通过几种可用方式相互分离。在第一选项中，可以将该气体混合物引入深冷分离器(4)，其将该气体分离成基本包含甲烷的气体物流和基本包含一氧化碳的另一气体物流(7)。在第二选项中，可以将该气体混合物引入甲烷水合物分离器(5)，其将该气体分离成基本包含甲烷的气体物流和基本包含一氧化碳的另一气体物流(7)。在第三选项中，可以通过如上所述将该气体混合物引入trim甲烷化反应器来提纯该气体混合物。在上文中和在经此引用并入的临时申请中更详细描述了这些分离法的每一个。
该甲烷气体物流可回收和用于管道级天然气。该氢气体物流(8)可以与一氧化碳气体物流(6)合并和再循环到气化反应器中以用在后继催化气化过程中。

Claims (10)

1.用于将碳质原料转化成包含在气体物流中的多种气体产物且从该气体物流中分离氢和甲烷的方法，其特征在于该方法包括下列步骤：
(a)向气化反应器供应碳质原料；
(b)在该气化反应器中在水蒸气和气化催化剂存在下、在合适的温度和压力下使该碳质原料反应形成包含甲烷、氢、一氧化碳、二氧化碳和一种或多种另外的气态副产物的第一气体物流；
(c)从所述第一气体物流中除去极大部分的二氧化碳和极大部分的所述一种或多种另外的气态副产物以产生包含甲烷、氢和任选一氧化碳的第二气体物流；
(d)从所述第二气体物流中至少部分分离氢以形成富氢气体物流和贫氢气体物流，其中该贫氢气体物流包含甲烷、任选一氧化碳和最多大约4摩尔％氢；
其中，如果该贫氢气体物流的热值小于950btu/scf(折干计算)和如果该贫氢气体物流包含1000ppm或更多的一氧化碳，那么：(1)从该贫氢气体物流中至少部分分离一氧化碳以形成(i)富一氧化碳气体物流和(ii)热值为至少950btu/scf(折干计算)的富甲烷气体物流；或(2)将该贫氢气体物流中的一氧化碳至少部分甲烷化以形成富甲烷气体物流。
2.用于将碳质原料转化成包含在气体物流中的多种气体产物且从该气体物流中分离氢和甲烷的方法，其特征在于该方法包括下列步骤：
(a)向反应器供应第一碳质原料；
(b)在该反应器中在氧存在下、在合适的温度和压力下至少部分燃烧所述第一碳质原料以生成(i)热能和(ii)包含氢、一氧化碳和二氧化碳的燃烧气体物流；
(c)利用来自所述第一碳质原料的所述燃烧的热能生成水蒸气；
(d)将至少一部分所述水蒸气、至少一部分所述燃烧气体物流、第二碳质原料和气化催化剂引入气化反应器；
(e)在该气化反应器中在水蒸气和所述气化催化剂存在下在合适的温度和压力下使所述第二碳质原料反应形成包含甲烷、氢、一氧化碳、二氧化碳和一种或多种另外的气态副产物的第一气体物流；
(f)从所述第一气体物流中除去极大部分的二氧化碳和极大部分的所述一种或多种气态副产物以产生包含甲烷、氢和任选一氧化碳的第二气体物流；
(g)从所述第二气体物流中至少部分分离氢以形成富氢气体物流和贫氢气体物流，其中该贫氢气体物流包含甲烷、任选一氧化碳和最多大约4摩尔％氢；
其中，如果该贫氢气体物流的热值小于950btu/scf(折干计算)且如果该贫氢气体物流包含1000ppm或更多的一氧化碳，那么：(1)从该贫氢气体物流中至少部分分离一氧化碳以形成(i)富一氧化碳气体物流和(ii)热值为至少950btu/scf(折干计算)的富甲烷气体物流；或(2)将该贫氢气体物流中的一氧化碳至少部分甲烷化以形成富甲烷气体物流。
3.权利要求2的方法，其特征在于所述第一碳质原料为含水淤浆形式。
4.权利要求2或权利要求3的方法，其特征在于，在步骤(c)中，在所述反应器内生成水蒸气。
5.权利要求2的方法，其特征在于，在步骤(c)中，将热能转移至在与水接触时生成水蒸气的热交换器。
6.权利要求1-5任一项的方法，其特征在于所述第二气体物流包含一氧化碳，且所述贫氢气体物流包含至少大约1000ppm一氧化碳。
7.权利要求6的方法，其特征在于将所述贫氢气体物流中的一氧化碳至少部分甲烷化以形成富甲烷气体物流。
8.权利要求1-7任一项的方法，其特征在于所述气化催化剂是碱金属气化催化剂。
9.权利要求8的方法，其特征在于所述碱金属是钾。
10.权利要求1-9任一项的方法，其特征在于通过使所述第二气体物流通过氢膜分离器来分离氢。
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