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1. 发明授权

US07473814B2 Process for converting methane into ethane 失效
标题翻译：将甲烷转化为乙烷的方法
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。

2. 发明申请

US20050272966A1 Process for converting methane into ethane 失效
标题翻译：将甲烷转化为乙烷的方法
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
IPC分类号： C07C2/76 , C07C6/08 , C07C9/06
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。

3. 发明申请

US20070129584A1 Metallic compound fixed to a support, method for production and use of said compound in hydrocarbon metathesis reactions 审中-公开
标题翻译：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
IPC分类号： C07C2/02 , B01J23/00
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。

4. 发明申请

US20100028735A1 PROCESS FOR CONVERTING METHANE INTO A HIGHER ALKANE MIXTURE 审中-公开
标题翻译：将甲烷转化为较高的烷烃混合物的方法
公开(公告)号：US20100028735A1
公开(公告)日：2010-02-04
申请号：US12448275
申请日：2007-12-18
申请人： Jean Marie Basset , Sudhakar Chakka , Daravong Soulivong , Mostafa Taoufik , Jean Thivolle-Cazat
发明人： Jean Marie Basset , Sudhakar Chakka , Daravong Soulivong , Mostafa Taoufik , Jean Thivolle-Cazat
IPC分类号： H01M8/04 , C07C2/76 , C01B3/02
CPC分类号： C07C6/10 , C07C2521/08 , C07C2531/12 , C07C9/10 , C07C9/14 , C07C9/08
摘要： The present invention relates to a process for converting methane into a higher alkane mixture, preferably a liquid alkane mixture, comprising (C3+) alkanes having 3 carbon atoms and more, preferably (C4+) alkanes having 4 carbon atoms, especially (C5+) alkanes having 5 carbon atoms and more. The process comprises:—a stage (1) comprising contacting methane with a metal catalyst (C1) capable of producing, in contact with alkane, reactions involving the splitting and recombining of C—C and/or C—H and/or C-metal bonds, so as to form by a non-oxidative methane coupling reaction a mixture (M1) comprising ethane and hydrogen,—preferably a stage (2) comprising fractionating the mixture (M1) so as to separate and to isolate the ethane, and—a stage (3) comprising, preferably simultaneously, (i) contacting the mixture (M1) or preferably the ethane isolated in stage (2) with a metal catalyst (C2) capable of producing, in contact with alkane, reactions involving the splitting and recombining of C—C and/or C—H and/or C-metal bonds, said catalyst being identical to or different from catalyst (C1), so as to form by simultaneous ethane self- and cross-metathesis reactions a mixture (M2) comprising methane and the higher alkane mixture, and (ii) fractionating the mixture (M2) so as to separate and to isolate said higher alkane mixture, preferably in liquid form, and particularly the methane which is preferably recycled into stage (1). The hydrogen produced in stage (1) is preferably separated and isolated in stage (2) and then used for various applications and stages, e.g. for producing thermal and/or electrical energies preferably employed to run the process.
摘要翻译：本发明涉及一种将甲烷转化成高级烷烃混合物，优选液态烷烃混合物的方法，该混合物包含具有3个碳原子的（C3 +）烷烃和更多（优选具有4个碳原子的（C4 +）烷烃），特别是（C5 +）烷烃，其具有 5个碳原子和更多。该方法包括：a阶段（1）包括使甲烷与能够与烷烃接触的金属催化剂（C1）接触涉及CC和/或CH和/或C - 金属键的分解和重组的反应，因此通过非氧化甲烷偶联反应形成包含乙烷和氢气的混合物（M1），优选地包括分级分离混合物（M1）以分离和分离乙烷的阶段（2）和阶段（ 3）优选同时包含（i）将阶段（2）中分离的混合物（M1）或优选乙烷与能够与烷烃接触的金属催化剂（C2）接触涉及CC的分解和重组的反应和/或CH和/或C - 金属键，所述催化剂与催化剂（C1）相同或不同，以便通过同时进行乙烷自身和交叉复分解反应形成包含甲烷和高级烷烃的混合物（M2）混合物，和（ii）分离混合物（M2）以分离并且优选分离所述高级烷烃混合物，优选液体形式，特别是优选循环到阶段（1）中的甲烷。在阶段（1）中产生的氢优选在阶段（2）中分离和分离，然后用于各种应用和阶段，例如，用于产生优选用于运行该过程的热能和/或电能。

5. 发明授权

US07378564B2 Process for manufacturing alkanes by reacting other alkanes with methane 失效
标题翻译：通过使其他烷烃与甲烷反应制备烷烃的方法
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。

6. 发明申请

US20050014987A1 Process for manufacturing alkanes by reacting other alkanes with methane 失效
标题翻译：通过使其他烷烃与甲烷反应制备烷烃的方法
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
IPC分类号： B01J21/08 , B01J31/12 , B01J37/02 , C07C6/10 , 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, 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。

7. 发明授权

US06660823B1 Modifying POSS compounds 失效
标题翻译：修饰POSS化合物
公开(公告)号：US06660823B1
公开(公告)日：2003-12-09
申请号：US09709783
申请日：2000-11-14
申请人： Joseph D. Lichtenhan , Frank J. Feder , Daravong Soulivong
发明人： Joseph D. Lichtenhan , Frank J. Feder , Daravong Soulivong
IPC分类号： C08G7738
CPC分类号： C07F7/21 , C07F7/0876 , C08G77/04 , C08G77/045 , C08G77/38
摘要： Method is provided for controlling the stereo chemistry of functionalities or X groups to exo or endo positions on a polyhedral oligomeric silsesquioxane (POSS) compound by adding certain reagents to said X groups to change one or more positions thereof to endo or exo. Also provided are the POSS species formed by the above inventive method. Method is also provided for inserting a ring substituent into a POSS compound. Also provided are the POSS species formed by such inventive method.
摘要翻译：提供了通过向所述X基团添加某些试剂以将其一个或多个位置改变为内切或外切来控制功能性或X基团在多面体低聚倍半硅氧烷（POSS）化合物上的内部或内部位置的立体化学性质的方法。还提供了通过上述发明方法形成的POSS种类。还提供了将环取代基插入POSS化合物的方法。还提供了通过这种创造性方法形成的POSS物种。

8. 发明授权

US6100417A Functionalizing olefin bearing silsesquioxanes 失效
标题翻译：官能化烯烃轴承倍半硅氧烷
公开(公告)号：US6100417A
公开(公告)日：2000-08-08
申请号：US387682
申请日：1999-08-31
申请人： Joseph D. Lichtenhan , Frank J. Feher , Daravong Soulivong
发明人： Joseph D. Lichtenhan , Frank J. Feher , Daravong Soulivong
IPC分类号： C07F7/21 , C07F2/08
CPC分类号： C07F7/21
摘要： Method is provided for reacting silsesquioxane resins or polyhedral oligomeric silsesquioxanes (POSS) bearing one or more olefinic groups with strong acids to cleave one or more olefin bonds of the olefinic groups to form POSS species of monomers or polymers having one or more functionalities suitable for reaction with a wide range of polymeric systems, to thus form new POSS derived compounds. Also provided are the new compounds so formed.
摘要翻译：提供了将含有一个或多个烯属基团的倍半硅氧烷树脂或多面体低聚倍半硅氧烷（POSS）与强酸反应以切割烯烃基团的一个或多个烯烃键以形成具有一个或多个适合于反应的官能团的单体或聚合物的POSS种类的方法具有广泛的聚合体系，从而形成新的POSS衍生化合物。还提供了如此形成的新化合物。

9. 发明授权

US06770724B1 Altering of poss rings 失效
标题翻译：改变可能的环
公开(公告)号：US06770724B1
公开(公告)日：2004-08-03
申请号：US09783719
申请日：2001-02-16
申请人： Joseph D. Lichtenhan , Timothy S. Haddad , Frank J. Feher , Daravong Soulivong
发明人： Joseph D. Lichtenhan , Timothy S. Haddad , Frank J. Feher , Daravong Soulivong
IPC分类号： C08G7706
CPC分类号： C07F7/21 , C07F7/0876 , C08G77/04 , C08G77/045 , C08G77/38
摘要： Method is provided for selectively opening rings of polyhedral oligomeric silsesquioxane (POSS) compounds to from functionalized derivatives thereof or new POSS species. Per the inventive method, the POSS compound is reacted with an acid to selectively cleave bonds in the POSS rings to add functionalities thereto for grafting, polymerization or catalysis, to thus form new familes of POSS derived compounds. Also provided are the new compounds so formed. Method is also provided for expanding rings of POSS compounds. Per the inventive method, a POSS compound is reacted with silane reagents to obtain an expanded POSS framework with added Si ring substituends to form new families of POSS compounds. Also provided are the new compounds so formed.
摘要翻译：提供了从其官能化衍生物或新的POSS物质选择性地打开多面体低聚倍半硅氧烷（POSS）化合物的环的方法。按照本发明的方法，POSS化合物与酸反应以选择性地切割POSS环中的键，以便为其接枝，聚合或催化添加官能团，从而形成新的POSS衍生化合物。还提供了如此形成的新化合物。还提供了扩展POSS化合物环的方法。根据本发明的方法，POSS化合物与硅烷试剂反应以获得具有添加的Si环取代基的扩展的POSS框架，以形成新的POSS化合物族。还提供了如此形成的新化合物。

10. 发明授权

US5942638A Method of functionalizing polycyclic silicones and the resulting compounds 失效
标题翻译：官能化多环硅氧烷和所得化合物的方法
公开(公告)号：US5942638A
公开(公告)日：1999-08-24
申请号：US003083
申请日：1998-01-05
申请人： Joseph D. Lichtenhan , Joseph J. Schwabb , Frank J. Feher , Daravong Soulivong
发明人： Joseph D. Lichtenhan , Joseph J. Schwabb , Frank J. Feher , Daravong Soulivong
IPC分类号： C07F7/08 , C07F7/21
CPC分类号： C07F7/21 , C07F7/0878
摘要： A synthetic process for the selective preparation of reactive polyhedral oligomeric silsesquioxanes (POSS) as well as polyhedral oligomeric silicate (POS) (spherosilicate) is provided. The method claimed herein employs metal catalyzed metathesis reactions for the selective reaction of .alpha.-olefin containing polyhedral oligomeric silsesquioxanes or silicates with olefinic reagents bearing functionalities useful for grafting reactions, polymerization chemistry and sol-gel processes. The use of metal catalyzed metathesis chemistry to form both linear or network polyhedral silsesquioxane polymers directly from .alpha.-olefin-containing polyhedral oligomeric silsesquioxanes is also described.
摘要翻译：提供了选择性制备反应性多面体低聚倍半硅氧烷（POSS）以及多面体低聚硅酸盐（POS）（硅藻土）的合成方法。本文所要求的方法使用金属催化的复分解反应，用于选择性反应含α-烯烃的多面体低聚倍半硅氧烷或硅酸盐与含有可用于接枝反应，聚合化学和溶胶 - 凝胶方法的官能团的烯属试剂。还描述了使用金属催化的复分解化学直接从含α-烯烃的多面体低聚倍半硅氧烷形成直链或网络多面体倍半硅氧烷聚合物。

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