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1.发明授权Structurally modified alumina supports, and heat transfer solids for high temperature fluidized bed reactions 失效结构改性的氧化铝载体和用于高温流化床反应的传热固体
公开(公告)号：US5395406A
公开(公告)日：1995-03-07
申请号：US60371
申请日：1993-05-11
CPC分类号： B01J35/0006 , B01J23/002 , B01J23/02 , B01J2523/00
摘要： A structurally modified alumina useful as a catalyst support, or heat transfer solid for fluidized bed synthesis gas processing. A Group IIA metal, or metals, particularly magnesium and barium, is composited with a particulate alumina to provide a catalyst support, or alumina heat transfer solid, having increased resistance to sintering and agglomeration; properties which promote defluidization of the bed in conducting fluidized bed reactions at high temperatures. The particles of preference are represented by formulas (1) and (2), a composite particle being represented by formula (1), as follows:M.sub.x Al.sub.2 O.sub.3+x (1)with the core of the particle being represented by formula (2), as follows:M.sub.y Al.sub.2 O.sub.3+y (2)where in formulas (1) and (2) M is a Group IIA metal, x is a number ranging from about 0.01 to about 0.4 and is representative of the number of moles of the metal M per mole of Al.sub.2 O.sub.3 y is a number equal to or greater than zero, and x is greater than y.
摘要翻译： 用作催化剂载体的结构改性氧化铝，或用于流化床合成气处理的传热固体。 IIA族金属或金属，特别是镁和钡与颗粒氧化铝复合以提供具有增加的耐烧结和附聚性能的催化剂载体或氧化铝传热固体; 促进床在高温下进行流化床反应的流化的性质。 优选的颗粒由式（1）和（2）表示，复合颗粒由式（1）表示，如下：颗粒的核心由式（2）表示的M x Al 2 O 3 + x（1） 如下：MyAl2O3 + y（2）其中式（1）和（2）中的M是IIA族金属，x是约0.01至约0.4的数，代表每个金属M的摩尔数 摩尔的Al 2 O 3 y是等于或大于零的数，x大于y。
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2.发明授权High surface purity heat transfer solids for high temperature fluidized bed reactions 失效高表面纯度的传热固体用于高温流化床反应
公开(公告)号：US5360778A
公开(公告)日：1994-11-01
申请号：US60378
申请日：1993-05-11
CPC分类号： C01B3/44 , B01J8/008 , C01B13/145 , C01F7/02 , C01F7/46 , C01P2002/85 , C01P2004/50 , C01P2004/61 , C01P2006/80 , Y02P20/52
摘要： High surface purity heat transfer solids are formed, suitably by washing and treating particulate refractory inorganic solids, notably alumina, which contains as impurities up to about 0.5 wt. % silicon and/or up to about 500 wppm boron, with an acid, or dilute acid solution sufficient to reduce the concentration of silicon and boron in the outer peripheral surface layer of the particles, e.g., as measured inwardly toward the center of a particle to a depth of about 50 .ANG. using X-ray photoelectron spectroscopy, to no greater than about 5 atom percent silicon and boron, preferably about 2 atom percent silicon and boron, based on the total number of cations within said outer peripheral surface layer, thereby reducing the tendency of said particles to sinter and agglomerate in the conversion of said hydrocarbon to hydrogen and carbon monoxide in a fluidized bed synthesis gas operation vis-a-vis particles otherwise similar except that the particles are not treated with the acid. The tendency of the particles to sinter and agglomerate is further reduced by the additional removal of sodium, iron, calcium, and titanium impurities from the outer peripheral surface layer of the particles. Preferably the latter named impurities, or impurities other than silicon and boron, are reduced to a concentration below about 20 atom %, more preferably to a concentration below about 15 atom %, in the outer surface layer of the particles.
摘要翻译： 适当地通过洗涤和处理颗粒耐火无机固体，特别是氧化铝来形成高表面纯度的热传递固体，其含有高达约0.5wt。 ％硅和/或高达约500wppm的硼，与酸或稀酸溶液相比足以降低颗粒外周表面层中硅和硼的浓度，例如向内朝向颗粒中心测量 基于所述外周表面层中的阳离子总数，使用X射线光电子能谱测量至约50AHZ的深度，不大于约5原子％的硅和硼，优选约2原子％的硅和硼，由此 降低了所述颗粒在流化床合成气操作中将所述烃转化为氢气和一氧化碳的过程中所述颗粒烧结和附聚的倾向，除了颗粒不用酸处理之外，颗粒否则相似。 通过从颗粒的外周表面层另外去除钠，铁，钙和钛杂质，进一步降低了颗粒烧结和附聚的倾向。 优选地，后者称为杂质或除了硅和硼之外的杂质，在颗粒的外表面层中被还原成低于约20原子％，更优选低于约15原子％的浓度。
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公开(公告)号：US5476877A
公开(公告)日：1995-12-19
申请号：US346973
申请日：1994-11-29
CPC分类号： B01J21/066 , B01J23/83 , C01B3/40 , C01B2203/1052 , C01B2203/1064 , C01B2203/1082 , Y02P20/52
摘要： A particulate, precalcined low silica content zirconia, especially one stabilizer with yttria, is useful as a catalyst support or as a heat transfer solids component for conducting chemical reactions at high temperature, in oxidizing, reducing or hydrothermal conditions, especially in syn gas operations. An admixture of precalcined particulate low silica content zirconia, particularly a low silica content yttria-stabilized zirconia, is employed in a preferred embodiment as a heat transfer solid, in concentrations ranging generally from about 10 wt. % to about 99.9 wt. % with a particulate catalyst notably a nickel-on-alumina catalyst, in concentration ranging generally from about 0. 1 wt. % to about 90 wt. %. Such an admixture provides a particularly useful catalytic contact mass in high temperature oxidizing, reducing and hydrothermal environments, notably in conducting synthesis gas generation operations. This type of bed promotes continuous, highly efficient heat and mass transfer within the reacting gas phase. The presence of the heat transfer solid as a bed component maintains excellent bed fluidization characteristics, suppressing the normal tendency of the catalyst to sinter or agglomerate; tendencies which promote defluidization of the bed. Moreover, the heat transfer particles of the bed are highly attrition resistant, and are chemically compatible with the catalyst particles of the admixture.
摘要翻译： 颗粒状预煅烧的低二氧化硅含量的氧化锆，特别是具有氧化钇的一种稳定剂，可用作催化剂载体或用作在高温，氧化，还原或水热条件下进行化学反应的传热固体组分，特别是在合成气操作中。 预先煅烧的颗粒状低二氧化硅含量的氧化锆，特别是低二氧化硅含量氧化钇稳定的氧化锆的混合物在优选的实施方案中用作传热固体，浓度通常为约10重量％ ％至约99.9wt。 ％的颗粒催化剂，特别是镍 - 氧化铝催化剂，其浓度范围通常为约0.1重量％ ％至约90wt。 ％。 这种混合物在高温氧化，还原和水热环境中特别是在进行合成气生成操作中提供特别有用的催化接触物质。 这种类型的床促进在反应气相内的连续，高效的热和质量传递。 作为床成分的传热固体的存在保持了优异的床流化特性，抑制了催化剂烧结或附聚的正常趋势; 促进床层流变的趋势。 此外，床的传热颗粒是高度耐磨性的，并且与混合物的催化剂颗粒化学相容。
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4.发明授权Synthesis gas from particulate catalysts, and admixtures of particulate catalysts and heat transfer solids 失效颗粒催化剂的合成气，颗粒催化剂和传热固体的混合物
公开(公告)号：US5348717A
公开(公告)日：1994-09-20
申请号：US60332
申请日：1993-05-11
CPC分类号： B01J37/04 , C01B3/40 , C01B3/44 , C01B31/18 , C01B2203/1052 , C01B2203/1064 , C01B2203/1082 , Y02P20/52
摘要： A process utilizing a particulate catalyst, or particulate catalyst admixed with particulate heat transfer solids for conducting high temperature fluidized bed syn gas operations. Hydrogen and carbon monoxide are produced from a low molecular weight hydrocarbon by contact thereof, at high temperature in the presence of oxygen, or steam and oxygen, with a fluidized bed comprising said particulate solids. In one of its forms, barium hexaluminate is employed as a heat transfer solid, in concentrations ranging generally from about 10 wt. % to about 99.9 wt. %, in admixture with a particulate catalyst containing a metal, or metals, component catalytic for the production of hydrogen and carbon monoxide from low molecular weight hydrocarbons contacted with a fluidized bed of the catalyst at high temperature hydrothermal conditions. The catalyst, suitably one having a barium hexaluminate carrier component, is employed in concentration ranging generally from about 0.1 wt. % to about 90 wt. %. Such an admixture provides a particularly useful catalytic contact mass for conducting fluidized bed synthesis gas generation operations. This type of bed promotes continuous, highly efficient heat and mass transfer within the reacting gas phase. The presence of the catalyst having a barium hexaluminate carrier component, or barium hexaluminate heat transfer solid as a bed component maintains excellent bed fluidization characteristics, suppressing the normal tendency of the catalyst to sinter or agglomerate; tendencies which promote defluidization of the bed. Moreover, the heat transfer particles of the bed are highly attrition resistant, and are chemically compatible with the catalyst particles of the admixture.
摘要翻译： 一种利用颗粒催化剂或与颗粒状传热固体混合的颗粒催化剂进行高温流化床合成气操作的方法。 氢和一氧化碳通过与低分子量烃在氧气或蒸气和氧气的存在下在高温下与其接触而产生，其中包含所述颗粒固体的流化床。 在其一种形式中，采用六铝酸钡作为传热固体，其浓度通常为约10wt。 ％至约99.9wt。 ％，与含有金属或金属的颗粒催化剂的混合物，催化剂用于在高温水热条件下与催化剂的流化床接触的低分子量烃生产氢气和一氧化碳。 合适地使用具有六铝酸钡载体组分的催化剂的浓度通常为约0.1重量％ ％至约90wt。 ％。 这种混合物提供用于进行流化床合成气产生操作的特别有用的催化接触物质。 这种类型的床促进在反应气相内的连续，高效的热和质量传递。 作为床成分的具有六铝酸钡载体成分或六铝酸钡传热固体的催化剂的存在保持了优异的床流化特性，抑制了催化剂烧结或附聚的正常趋势; 促进床层流变的趋势。 此外，床的传热颗粒是高度耐磨性的，并且与混合物的催化剂颗粒化学相容。
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5.发明授权High surface purity heat transfer solids for high temperature fluidized bed reactions 失效高表面纯度的传热固体用于高温流化床反应
公开(公告)号：US5496531A
公开(公告)日：1996-03-05
申请号：US276071
申请日：1994-07-15
CPC分类号： C01B3/44 , B01J8/008 , C01B13/145 , C01F7/02 , C01F7/46 , C01P2002/85 , C01P2004/50 , C01P2004/61 , C01P2006/80 , Y02P20/52
摘要： High surface purity heat transfer solids are formed, suitably by washing and treating particulate refractory inorganic solids, notably alumina, which contains as impurities up to about 0.5 wt. % silicon and/or up to about 500 wppm boron, with an acid, or dilute acid solution sufficient to reduce the concentration of silicon and boron in the outer peripheral surface layer of the particles, e.g., as measured inwardly toward the center of a particle to a depth of about 50 .ANG. using X-ray photoelectron spectroscopy, to no greater than about 5 atom percent silicon and boron, preferably about 2 atom percent silicon and boron, based on the total number of cations within said outer peripheral surface layer, thereby reducing the tendency of said particles to sinter and agglomerate in the conversion of said hydrocarbon to hydrogen and carbon monoxide in a fluidized bed synthesis gas operation vis-a-vis particles otherwise similar except that the particles are not treated with the acid. The tendency of the particles to sinter and agglomerate is further reduced by the additional removal of sodium, iron, calcium, and titanium impurities from the outer peripheral surface layer of the particles. Preferably the latter named impurities, or impurities other than silicon and boron, are reduced to a concentration below about 20 atom %, more preferably to a concentration below about 15 atom %, in the outer surface layer of the particles.
摘要翻译： 适当地通过洗涤和处理颗粒耐火无机固体，特别是氧化铝来形成高表面纯度的热传递固体，其含有高达约0.5wt。 ％硅和/或高达约500wppm的硼，与酸或稀酸溶液相比足以降低颗粒外周表面层中硅和硼的浓度，例如向内朝向颗粒中心测量 基于所述外周表面层中的阳离子总数，使用X射线光电子能谱测量至约50AHZ的深度，不大于约5原子％的硅和硼，优选约2原子％的硅和硼，由此 降低了所述颗粒在流化床合成气操作中将所述烃转化为氢气和一氧化碳的过程中所述颗粒烧结和附聚的倾向，除了颗粒不用酸处理之外，颗粒否则相似。 通过从颗粒的外周表面层另外去除钠，铁，钙和钛杂质，进一步降低了颗粒烧结和附聚的倾向。 优选地，后者称为杂质或除了硅和硼之外的杂质，在颗粒的外表面层中被还原成低于约20原子％，更优选低于约15原子％的浓度。
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公开(公告)号：US5395813A
公开(公告)日：1995-03-07
申请号：US60334
申请日：1993-05-11
CPC分类号： B01J21/066 , B01J23/83 , C01B3/40 , C01B2203/1052 , C01B2203/1064 , C01B2203/1082 , Y02P20/52
摘要： A particulate, precalcined low silica content zirconia, especially one stabilized with yttria, is useful as a catalyst support or as a heat transfer solids component for conducting chemical reactions at high temperature, in oxidizing, reducing or hydrothermal conditions, especially in syn gas operations. An admixture of precalcined particulate low silica content zirconia, particularly a low silica content yttria-stabilized zirconia, is employed in a preferred embodiment as a heat transfer solid, in concentrations ranging generally from about 10 wt. % to about 99.9 wt. %, with a particulate catalyst, notably a nickel-on-alumina catalyst, in concentration ranging generally from about 0.1 wt. % to about 90 wt. %. Such an admixture provides a particularly useful catalytic contact mass in high temperature oxidizing, reducing and hydrothermal environments, notably in conducting synthesis gas generation operations. This type of bed promotes continuous, highly efficient heat and mass transfer within the reacting gas phase. The presence of the heat transfer solid as a bed component maintains excellent bed fluidization characteristics, suppressing the normal tendency of the catalyst to sinter or agglomerate; tendencies which promote defluidization of the bed. Moreover, the heat transfer particles of the bed are highly attrition resistant, and are chemically compatible with the catalyst particles of the admixture.
摘要翻译： 颗粒状预煅烧的低二氧化硅含量的氧化锆，特别是用氧化钇稳定的氧化锆，可用作催化剂载体或用作在高温，氧化，还原或水热条件下进行化学反应的传热固体组分，特别是在合成气操作中。 预先煅烧的颗粒状低二氧化硅含量的氧化锆，特别是低二氧化硅含量氧化钇稳定的氧化锆的混合物在优选的实施方案中用作传热固体，浓度通常为约10重量％ ％至约99.9wt。 ％的颗粒催化剂，特别是镍 - 氧化铝催化剂，其浓度通常为约0.1wt。 ％至约90wt。 ％。 这种混合物在高温氧化，还原和水热环境中特别是在进行合成气生成操作中提供特别有用的催化接触物质。 这种类型的床促进在反应气相内的连续，高效的热和质量传递。 作为床成分的传热固体的存在保持了优异的床流化特性，抑制了催化剂烧结或附聚的正常趋势; 促进床层流变的趋势。 此外，床的传热颗粒是高度耐磨性的，并且与混合物的催化剂颗粒化学相容。
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7.发明授权High performance alumina heat transfer solids for high temperature fluidized bed synthesis gas reactions 失效高性能氧化铝传热固体用于高温流化床合成气反应
公开(公告)号：US5360777A
公开(公告)日：1994-11-01
申请号：US60395
申请日：1993-05-11
CPC分类号： C10J3/12 , B01J21/04 , C10J3/463 , C10J2300/0986 , C10J2300/0993 , Y02P20/52
摘要： Alumina heat transfer solids are admixed with a catalyst, or catalysts, and used in conducting high temperature fluidized bed reactions, particularly in a process for the production of hydrogen and carbon monoxide from a low molecular weight hydrocarbon by contact with a fluidized bed of catalyst and said heat transfer solids at high temperature in the presence of oxygen, or steam, or both oxygen and steam. The particulate heat transfer solids are characterized as having a performance index, PI, greater than 20, preferably greater than 40, as characterized by the formula PI=[(i).times.(ii).times.(iii).times.(iv)].sup.-1 where (i) the peripheral outer surface of the particle contains
摘要翻译： 将氧化铝传热固体与催化剂或催化剂混合，并用于进行高温流化床反应，特别是在通过与催化剂流化床接触从低分子量烃生产氢气和一氧化碳的方法中， 所述传热固体在高温下在氧气或蒸汽，氧气和蒸汽两者的存在下。 颗粒传热固体的特征在于具有大于20，优选大于40的性能指数PI，其特征在于PI = [（i）x（ii）x（iii）x（iv）] -1 其中（i）颗粒的周边外表面含有<5原子％（Si + B）作为杂质，和（ii）<20原子％的Na，Fe，Ca和Ti作为杂质，其中（Si + B）足以在工艺条件下迁移并污染颗粒的外表面层。 此外，（iii）颗粒的堆积密度范围为约1.2g / cc至约2.5g / cc，和（iv）颗粒的Davison磨损指数不大于约12。
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公开(公告)号：US5143647A
公开(公告)日：1992-09-01
申请号：US711697
申请日：1991-06-07
CPC分类号： B01J8/1809 , B01J8/24 , B01J8/32 , C01B3/44 , B01J2208/00716
摘要： Start-up procedure for FBSG process involving starting up under oxidizing conditions with Al.sub.2 O.sub.3 (no Ni) particles in the bed and the switching to reducing conditions prior to adding Ni/Al.sub.2 O.sub.3 catalyst. This procedure will prevent catalyst particle agglomeration.
摘要翻译： FBSG工艺的启动程序涉及在氧化条件下在床中加入Al2O3（无Ni）颗粒并在添加Ni / Al2O3催化剂之前切换至还原条件。 该过程将防止催化剂颗粒聚集。
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9.发明授权High energy level in situ attrition and break up of catalyst to maintain bed fluidization during high temperature operations 失效高能量原位消耗和催化剂分解，以保持高温操作过程中的床流化
公开(公告)号：US5421842A
公开(公告)日：1995-06-06
申请号：US301209
申请日：1994-09-09
申请人： Robert H. Shabaker , Charles A. Euker, Jr. , Geoffrey R. Say , Gerald A. Wilcox , James H. Taylor , LeRoy R. Clavenna
发明人： Robert H. Shabaker , Charles A. Euker, Jr. , Geoffrey R. Say , Gerald A. Wilcox , James H. Taylor , LeRoy R. Clavenna
CPC分类号： C01B3/44 , B01J8/1872 , B01J8/388
摘要： A process for the in situ attrition and break up of an agglomerating, or agglomerated catalyst to maintain and control the fluidization characteristics of a bed wherein low molecular weight hydrocarbons, oxygen and steam are contacted with the bed to produce hydrogen and carbon monoxide via both partial oxidation and steam reforming reactions. The feeds are injected into the reaction zone with mechanical energy input sufficient to balance the intrinsic rate of agglomeration by fracturing and breaking apart in situ the agglomerated catalyst to maintain the fluidization characteristics of the bed throughout the cycle of operation.
摘要翻译： 一种用于原位磨损和聚集的催化剂分解以保持和控制床的流化特性的方法，其中低分子量烃，氧气和蒸汽与床接触以通过两部分产生氢气和一氧化碳 氧化和蒸汽重整反应。 将进料注入到反应区中，其机械能量输入足以通过压裂平衡凝固的固有速率并原位分解聚集的催化剂，以在整个操作循环中保持床的流化特性。
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10.发明授权Process for the elimination of silica and other impurities in fluidized bed syn gas production 失效在流化床合成气生产中消除二氧化硅和其他杂质的方法
公开(公告)号：US5421841A
公开(公告)日：1995-06-06
申请号：US301207
申请日：1994-09-06
IPC分类号： C01B3/44
CPC分类号： C01B3/44
摘要： A process for the production of syn gas (hydrogen and carbon monoxide) by reaction at high temperature between low molecular weight hydrocarbons, steam and oxygen in an impurities-containing refractory lined reaction zone. The lined reaction zone is pretreated with steam, or with steam and a reducing gas, e.g. a mixture of steam and hydrogen to leach out, react with, and transport the impurities, i.e., the reaction products of silica, or silica plus phosphorus or sulfur, or silica plus phosphorus and sulfur, from the reaction zone. Steam alone may be used to leach out, convert the silica to gaseous silicic acid, and remove same from the reaction zone; and then the hydrocarbons, steam and oxygen feeds are introduced into the reaction zone to produce syn gas.
摘要翻译： 通过在含杂质的耐火材料衬里反应区中的低分子量烃，蒸汽和氧气之间的高温反应生产合成气（氢气和一氧化碳）的方法。 衬里的反应区用蒸汽或蒸汽和还原气体例如预处理。 蒸汽和氢气的混合物从反应区浸出，反应和输送杂质，即二氧化硅或二氧化硅与磷或硫或二氧化硅加磷和硫的反应产物。 可以单独使用蒸汽浸出，将二氧化硅转化为气态硅酸，并从反应区除去; 然后将烃，蒸汽和氧气进料引入反应区以产生合成气。
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