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公开(公告)号：US07473814B2
公开(公告)日：2009-01-06
申请号：US10517212
申请日：2003-06-04
申请人： Jean-Marie Basset , Philippe Bres , Christophe Coperet , Barry Martin Maunders , Daravong Soulivong , Mostafa Taoufik , Jean Thivolle-Cazat
发明人： Jean-Marie Basset , Philippe Bres , Christophe Coperet , Barry Martin Maunders , Daravong Soulivong , Mostafa Taoufik , Jean Thivolle-Cazat
IPC分类号： C07C2/00
CPC分类号： C07C2/76 , C07C2531/12 , Y10S585/943 , C07C9/06
摘要： The invention relates to a process for producing ethane comprising contacting methane with a metal catalyst selected from metal hydrides, metal organic compounds and mixtures thereof. It also relates to a process for the conversion of methane to carbon-containing products comprising contacting methane with a metal catalyst comprising at least one metal, Me, chosen from the lanthanides, the actinides and the metals from Groups 2 to 12 of the Periodic Table of the Elements, so as to produce ethane in a proportion of at least 65%, especially at least 98% or 99% by weight with respect to carbon-containing products formed in the process. The process can be a single-step process, preferably carried out under conditions involving a non-oxidative catalytic coupling of methane, in particular under operating conditions maintained substantially constant, preferably continuously, during the ethane production, e.g. at a temperature ranging from −30° C. to +80° C., preferably from 20° C. to 500° C., under a total absolute pressure ranging from 10−3 to 100 MPa, preferably from 0.1 to 50 MPa. The metal catalyst may be chosen from metal catalysts supported on and preferably grafted to a solid support. One of the main advantages of the present invention is to produce ethane with a very high selectivity.
摘要翻译： 本发明涉及一种生产乙烷的方法，包括使甲烷与选自金属氢化物，金属有机化合物及其混合物的金属催化剂接触。 它还涉及将甲烷转化为含碳产物的方法，包括使甲烷与包含至少一种金属的金属催化剂接触，所述金属催化剂选自镧系元素，锕系元素和元素周期表第2至12族中的金属 的元素，以便相对于在该方法中形成的含碳产品，以至少65重量％，特别是至少98重量％或99重量％的比例制备乙烷。 该方法可以是单步骤方法，优选在涉及甲烷的非氧化催化偶合的条件下进行，特别是在乙烷生产期间，优选连续保持基本上恒定的操作条件下，例如乙烷生产。 在-30℃至+ 80℃，优选20℃至500℃的温度下，在绝对压力范围为10-3-100MPa，优选0.1-50MPa的温度下进行。 金属催化剂可以选自负载在并优选接枝到固体载体上的金属催化剂。 本发明的主要优点之一是以非常高的选择性生产乙烷。
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公开(公告)号：US20050272966A1
公开(公告)日：2005-12-08
申请号：US10517212
申请日：2003-06-04
申请人： Jean-Marie Basset , Philippe Bres , Christophe Coperet , Barry Maunders , Daravong Soulivong , Mostafa Taoufik , Jean Thivolle-Cazat
发明人： Jean-Marie Basset , Philippe Bres , Christophe Coperet , Barry Maunders , Daravong Soulivong , Mostafa Taoufik , Jean Thivolle-Cazat
CPC分类号： C07C2/76 , C07C2531/12 , Y10S585/943 , C07C9/06
摘要： The invention relates to a process for producing ethane comprising contacting methane with a metal catalyst selected from metal hydrides, metal organic compounds and mixtures thereof. It also relates to a process for the conversion of methane to carbon-containing products comprising contacting methane with a metal catalyst comprising at least one metal, Me, chosen from the lanthanides, the actinides and the metals from Groups 2 to 12 of the Periodic Table of the Elements, so as to produce ethane in a proportion of at least 65%, especially at least 98% or 99% by weight with respect to carbon-containing products formed in the process. The process can be a single-step process, preferably carried out under conditions involving a non-oxidative catalytic coupling of methane, in particular under operating conditions maintained substantially constant, preferably continuously, during the ethane production, e.g. at a temperature ranging from −30° C. to +80° C., preferably from 20° C. to 500° C., under a total absolute pressure ranging from 10−3 to 100 MPa, preferably from 0.1 to 50 MPa. The metal catalyst may be chosen from metal catalysts supported on and preferably grafted to a solid support. One of the main advantages of the present invention is to produce ethane with a very high selectivity.
摘要翻译： 本发明涉及一种生产乙烷的方法，包括使甲烷与选自金属氢化物，金属有机化合物及其混合物的金属催化剂接触。 它还涉及将甲烷转化为含碳产物的方法，包括使甲烷与包含至少一种金属的金属催化剂接触，所述金属催化剂选自镧系元素，锕系元素和元素周期表第2至12族中的金属 的元素，以便相对于在该方法中形成的含碳产品，以至少65重量％，特别是至少98重量％或99重量％的比例制备乙烷。 该方法可以是单步骤方法，优选在涉及甲烷的非氧化催化偶合的条件下进行，特别是在乙烷生产期间，优选连续保持基本上恒定的操作条件下，例如乙烷生产。 在-30℃至+ 80℃，优选20℃至500℃的温度范围内，在绝对压力范围为10 -3至100MPa， 优选为0.1〜50MPa。 金属催化剂可以选自负载在并优选接枝到固体载体上的金属催化剂。 本发明的主要优点之一是以非常高的选择性生产乙烷。
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3.发明申请Metallic compound fixed to a support, method for production and use of said compound in hydrocarbon metathesis reactions 审中-公开固定在载体上的金属化合物，在烃复分解反应中生产和使用所述化合物的方法公开(公告)号：US20070129584A1
公开(公告)日：2007-06-07
申请号：US10550628
申请日：2004-03-24
申请人： Jean-Marie Basset , Christophe Coperet , Daravong Soulivong , Mostafa Taoufik , Jean Thivolle-Cazat
发明人： Jean-Marie Basset , Christophe Coperet , Daravong Soulivong , Mostafa Taoufik , Jean Thivolle-Cazat
CPC分类号： C07C6/10 , B01J31/121 , B01J37/0209 , B01J37/18 , C07C2521/04 , C07C2531/12 , C08L61/06
摘要： The invention relates to a supported metal compound, comprising a support made from aluminium oxide to which a tungsten hydride is grafted. The support may be selected from the homogeneous supports with a composition based on aluminum oxide and from heterogeneous supports made from aluminium oxide with aluminum oxide essentially on the surface of said support. The support may in particular comprise aluminium oxide, mixed aluminium oxides and modified aluminium oxides particularly comprising one or more elements of groups 15 to 17 of the periodic table of the elements, such as phosphorus, sulphur, fluorine or chlorine. A support made from porous, non-porous or mesoporous aluminas is preferred. The degree of oxidation of the tungsten may have a value of from 2 to 6. The tungsten atom is generally bonded to one or several hydrogen atoms and optionally to one or several hydrocarbon groups. According to the invention, the compound may be prepared by a dispersion step and grafting of a tungsten organometallic precursor to the support made from aluminium oxide then hydrogenation of the resulting product. The product may be used as catalyst in reactions of cleavage and recombination of hydrocarbons, particularly in hydrocarbon metathesis reactions most particularly of alkanes. The product has a surprising, extremely high catalytic activity in this type of reaction and in particular, a high selectivity for the formation of n-alkanes with relation to iso-alkanes.
摘要翻译： 本发明涉及一种载体金属化合物，其包括由氧化铝制成的载体，钨载体与其接枝。 载体可以选自具有基于氧化铝的组合物的均相载体和基本上在所述载体表面上由氧化铝与氧化铝制成的非均相载体。 该载体可以特别包括氧化铝，混合的氧化铝和改性的氧化铝，特别包括元素周期表中第15至17族元素的一种或多种元素，如磷，硫，氟或氯。 由多孔，无孔或中孔氧化铝制成的载体是优选的。 钨的氧化度可以具有2至6的值。钨原子通常与一个或几个氢原子键合，任选地与一个或多个烃基键合。 根据本发明，化合物可以通过分散步骤制备，并将钨有机金属前体接枝到由氧化铝制成的载体上，然后氢化所得产物。 该产物可用作烃的裂解和重组反应的催化剂，特别是在烷烃中的烃复分解反应中。 该产物在这种类型的反应中具有惊人的极高的催化活性，特别是与异烷烃相关的形成正烷烃的高选择性。
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4.发明授权公开(公告)号：US07378564B2
公开(公告)日：2008-05-27
申请号：US10502845
申请日：2003-01-22
申请人： Jean-Marie Basset , Christophe Coperet , Richard Pardy , Daravong Soulivong , John Glenn Sunley , Jean Thivolle-Cazat
发明人： Jean-Marie Basset , Christophe Coperet , Richard Pardy , Daravong Soulivong , John Glenn Sunley , Jean Thivolle-Cazat
IPC分类号： C07C6/08
CPC分类号： C07C6/10 , B01J21/08 , B01J31/121 , B01J37/0209 , C07C2531/12 , Y10S585/943
摘要： The present invention relates to a process for the manufacture of alkanes comprising a catalytic reaction resulting from contacting methane with at least one other starting alkane (I) in the presence of a metal compound (C) capable of catalysing a reaction for the splitting and/or recombination of a carbon-carbon bond and/or of a carbon-hydrogen bond and/or of a carbon-metal bond, which catalytic reaction results in the formation of at least one final alkane (II) having a number of carbon atoms equal to or greater than (2). In the process, the contacting operation is carried out under a methane partial pressure equal to or greater than 0.1 MPa, preferably in the range from 0.1 to 100 MPa. The metal compound (C) can be chosen from metal compounds supported on and dispersed over a solid support, metal compounds supported on and grafted to a solid support and non-supported metal compounds. Under these conditions, it was found that the yield of the catalytic reaction was improved, and that the catalytic stability and activity of the metal compound (C) over timer were greatly enhanced.
摘要翻译： 本发明涉及一种制备烷烃的方法，其包括由甲烷与至少一种其它起始烷烃（I）在能够催化分解和/或反应的反应的金属化合物（C）存在下使甲烷接触而产生的催化反应， 或碳 - 碳键和/或碳 - 氢键和/或碳 - 金属键的重组，该催化反应导致至少一个具有多个碳原子的最终烷烃（II）的形成相等 至（2）以上。 在该过程中，接触操作在等于或大于0.1MPa，优选在0.1至100MPa范围内的甲烷分压下进行。 金属化合物（C）可以选自负载在固体载体上并分散在固体载体上的金属化合物，负载在和接枝到固体载体上的金属化合物和非负载的金属化合物。 在这些条件下，发现催化反应的产率提高，金属化合物（C）超过定时器的催化稳定性和活性大大提高。
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5.发明申请公开(公告)号：US20050014987A1
公开(公告)日：2005-01-20
申请号：US10502845
申请日：2003-01-22
申请人： Jean-Marie Basset , Christophe Coperet , Richard Pardy , Daravong Soulivong , John Sunley , Jean Thivolle-Cazat
发明人： Jean-Marie Basset , Christophe Coperet , Richard Pardy , Daravong Soulivong , John Sunley , Jean Thivolle-Cazat
CPC分类号： C07C6/10 , B01J21/08 , B01J31/121 , B01J37/0209 , C07C2531/12 , Y10S585/943
摘要： The present invention relates to a process for the manufacture of alkanes comprising a catalytic reaction resulting from contacting methane with at least one other starting alkane (I) in the presence of a metal compound (C) capable of catalysing a reaction for the splitting and/or recombination of a carbon-carbon bond and/or of a carbon-hydrogen bond and/or of a carbon-metal bond, which catalytic reaction results in the formation of at least one final alkane (II) having a number of carbon atoms equal to or greater than (2). In the process, the contacting operation is carried out under a methane partial pressure equal to or greater than 0.1 MPa, preferably in the range from 0.1 to 100 MPa. The metal compound (C) can be chosen from metal compounds supported on and dispersed over a solid support, metal compounds supported on and grafted to a solid support and non-supported metal compounds. Under these conditions, it was found that the yield of the catalytic reaction was improved, ant that the catalytic stability and activity of the metal compound (C) over timer were greatly enhanced.
摘要翻译： 本发明涉及一种制备烷烃的方法，其包括由甲烷与至少一种其它起始烷烃（I）在能够催化分解和/或反应的反应的金属化合物（C）存在下使甲烷接触而产生的催化反应， 或碳 - 碳键和/或碳 - 氢键和/或碳 - 金属键的重组，该催化反应导致至少一个具有多个碳原子的最终烷烃（II）的形成相等 至（2）以上。 在该过程中，接触操作在等于或大于0.1MPa，优选在0.1至100MPa范围内的甲烷分压下进行。 金属化合物（C）可以选自负载在固体载体上并分散在固体载体上的金属化合物，负载在和接枝到固体载体上的金属化合物和非负载的金属化合物。 在这些条件下，发现催化反应的产率提高，催化稳定性和金属化合物（C）与定时器的活性大大提高。
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公开(公告)号：US06469225B1
公开(公告)日：2002-10-22
申请号：US09663941
申请日：2000-09-18
申请人： Jean-Marie Basset , Christophe Coperet , Laurent Lefort , Barry Martin Maunders , Olivier Maury , Guillaume Saggio , Jean Thivolle-Cazat
发明人： Jean-Marie Basset , Christophe Coperet , Laurent Lefort , Barry Martin Maunders , Olivier Maury , Guillaume Saggio , Jean Thivolle-Cazat
IPC分类号： C07C608
CPC分类号： C07C1/325 , Y10S585/931 , C07C9/00
摘要： A process for the manufacture of alkanes comprising a cross-metathesis reaction between at least one starting alkane (A) and one organometallic compound (B) fixed to an inorganic support and comprising a metal bonded to at least one hydrocarbon-comprising radical. The reaction leads to the formation of at least one other alkane (C) which is a higher or lower homologue of the starting alkane (A), by cleavage of the hydrocarbon-comprising radical with the metal of the organometallic compound (B) and recombination of the radical with at least one other radical originating from a cleavage of the starting alkane (A). The metal of the compound (B) preferably is selected from transition metals, lanthanides and actinides, and the hydrocarbon-comprising radical of the compound (B) preferably is selected from alkyl, alkylidene and alkylidyne radicals.
摘要翻译： 一种制备烷烃的方法，其包括至少一种起始烷烃（A）和一种固定到无机载体上的一种有机金属化合物（B）之间的交叉复分解反应，并包含与至少一种含烃基团结合的金属。 该反应通过用有机金属化合物（B）的金属裂解含有烃的自由基和复合的方式，形成起始烷烃（A）的较高或较低同系物的至少一种其它烷烃（C） 的基团与至少一种源自起始烷烃（A）的裂解的其它基团反应。 化合物（B）的金属优选选自过渡金属，镧系元素和锕系元素，化合物（B）的含烃基团优选选自烷基，亚烷基和亚烷基。
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公开(公告)号：US06727397B2
公开(公告)日：2004-04-27
申请号：US10040495
申请日：2002-01-09
申请人： Jean-Marie Basset , Christophe Coperet , Laurent Lefort , Barry Martin Maunders , Olivier Maury , Guillaume Saggio , Jean Thivolle-Cazat
发明人： Jean-Marie Basset , Christophe Coperet , Laurent Lefort , Barry Martin Maunders , Olivier Maury , Guillaume Saggio , Jean Thivolle-Cazat
IPC分类号： C07C608
CPC分类号： B01J37/0203 , C07C6/10 , C07C2531/12
摘要： The present invention relates to a process for manufacturing alkanes, comprising, as main stage, a reaction resulting from bringing methane into contact with at least one other starting alkane (A) in the presence of a catalyst based on a metal M capable of catalyzing a metathesis of alkanes. The reaction results in the formation of at least one or two final alkanes (B) having a number of carbon atoms less than or equal to that of the starting alkane (A) and at least equal to 2. Preferably the catalyst comprises a hydride of a metal M grafted to and dispersed over a solid support. The metal M may be chosen from transition metals, lanthanides and actinides. The present invention also relates to the use of a catalyst capable of catalyzing a metathesis of alkanes in 3 reaction resulting from bringing methane into contact with at least one other starting alkane (A).
摘要翻译： 本发明涉及一种制备烷烃的方法，该方法主要包括在催化剂存在下使甲烷与至少一种其它起始烷烃（A）接触而产生的反应，所述催化剂基于能够催化一种 烷烃的复分解。 反应导致至少一种或两种具有小于或等于起始烷烃（A）的碳原子的最终烷烃（B）的形成，并且至少等于2.优选地，催化剂包含 金属M接枝并分散在固体支持物上。 金属M可以选自过渡金属，镧系元素和锕系元素。 本发明还涉及能够在使甲烷与至少一种其它起始烷烃（A）接触的情况下，在3反应中催化烷烃的复分解的催化剂的用途。
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公开(公告)号：US20080228020A1
公开(公告)日：2008-09-18
申请号：US11571602
申请日：2005-06-27
IPC分类号： C07C2/02
CPC分类号： C07C6/04 , C07C2531/12 , Y02P20/584 , C07C11/06
摘要： The invention relates to a method for converting ethylene into propylene consisting in reacting said ethylene with a supported metal compound comprising an aluminium oxide based support to which a tungsten hydride is grafted. Said reaction is carried out at a temperature ranging from 20 to 600° C., preferably between 50 and 350° C., at an absolute pressure ranging from 0.01 to 8 MPa, preferably between 0.01 and 1 MPa. A catalyst is regeneratable by introducing hydrogen at a temperature of 50-300° C.
摘要翻译： 本发明涉及一种将乙烯转化成丙烯的方法，该方法是使所述乙烯与负载型金属化合物反应，该金属化合物包含接枝有氢化钨的氧化铝基载体。 所述反应在20〜600℃，优选50〜350℃的温度下进行，绝对压力为0.01〜8MPa，优选为0.01〜1MPa。 催化剂可以通过在50-300℃的温度下引入氢气来再生
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9.发明授权Method for metathesis of compounds comprising an olefinic double bond, in particular olefins 失效包含烯属双键，特别是烯烃的化合物的复分解方法公开(公告)号：US07635794B2
公开(公告)日：2009-12-22
申请号：US11571395
申请日：2005-07-01
IPC分类号： C07C6/04
CPC分类号： C07C6/04 , C07C2521/04 , C07C2531/12 , C07C11/06
摘要： The invention relates to a method for metathesis of one or several reagents comprising a linear or branched hydrocarbon chain containing a double olefinic bond Csp2═Csp2 consisting in reacting said reagent or reagents with a supported metal compound comprising an aluminum oxide-based support to which a tungsten hydride is grafted. Typically, each said reagent or reagents comprises from 2 to 30 carbon atoms. The reagent can be embodied in the form of olefin. The inventive method can be used, for example for producing propylene from ethylene and butane.
摘要翻译： 本发明涉及一种一种或多种试剂的复分解方法，其包含含有双重烯键Csp2-Csp2的直链或支链烃链，所述双链烯烃键Csp2-Csp2使所述试剂或试剂与包含氧化铝基载体的负载金属化合物反应， 接枝氢化钨。 通常，每个所述试剂或试剂包含2至30个碳原子。 试剂可以以烯烃的形式实施。 本发明的方法可用于例如从乙烯和丁烷生产丙烯。
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公开(公告)号：US07638672B2
公开(公告)日：2009-12-29
申请号：US11571602
申请日：2005-06-27
IPC分类号： C07C6/04
CPC分类号： C07C6/04 , C07C2531/12 , Y02P20/584 , C07C11/06
摘要： The invention relates to a method for converting ethylene into propylene consisting in reacting said ethylene with a supported metal compound comprising an aluminium oxide based support to which a tungsten hydride is grafted. Said reaction is carried out at a temperature ranging from 20 to 600° C., preferably between 50 and 350° C., at an absolute pressure ranging from 0.01 to 8 MPa, preferably between 0.01 and 1 MPa. A catalyst is regeneratable by introducing hydrogen at a temperature of 50-300° C.
摘要翻译： 本发明涉及一种将乙烯转化成丙烯的方法，该方法是使所述乙烯与负载型金属化合物反应，该金属化合物包含接枝有氢化钨的氧化铝基载体。 所述反应在20〜600℃，优选50〜350℃的温度下进行，绝对压力为0.01〜8MPa，优选为0.01〜1MPa。 催化剂可以通过在50-300℃的温度下引入氢气来再生
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