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1.发明申请Cross-metathesis reaction of functionalized and substituted olefins using group 8 transition metal carbene complexes as metathesis catalysts 审中-公开使用第8族过渡金属卡宾络合物作为复分解催化剂的官能化和取代的烯烃的交错复分解反应公开(公告)号：US20070155975A1
公开(公告)日：2007-07-05
申请号：US11559399
申请日：2006-11-13
申请人： Robert Grubbs , Arnab Chatterjee , Tae-Lim Choi , Steven Godberg , Jennifer Love , John Morgan , Daniel Sanders , Matthias Scholl , F. Toste , Tina Trnka
发明人： Robert Grubbs , Arnab Chatterjee , Tae-Lim Choi , Steven Godberg , Jennifer Love , John Morgan , Daniel Sanders , Matthias Scholl , F. Toste , Tina Trnka
IPC分类号： C07F9/02 , C07F5/02 , C07F7/00 , C07C31/34 , C07C205/02 , C07C319/02
CPC分类号： C07F9/40 , C07C6/04 , C07C17/275 , C07C29/40 , C07C29/46 , C07C41/14 , C07C45/69 , C07C67/293 , C07C67/297 , C07C67/343 , C07C67/475 , C07C201/12 , C07C319/20 , C07C2531/22 , C07C2601/14 , C07C2601/16 , C07C2603/74 , C07D263/14 , C07D317/12 , C07D317/20 , C07D317/24 , C07F7/1892 , C07F9/4015 , C07F15/0046 , C07C25/13 , C07C47/21 , C07C69/007 , C07C69/78 , C07C69/732 , C07C69/56 , C07C321/14 , C07C69/16 , C07C69/533 , C07C69/145 , C07C69/157 , C07C69/18 , C07C205/06 , C07C33/483
摘要： The invention pertains to the use of Group 8 transition metal carbene complexes as catalysts for olefin cross-metathesis reactions. In particular, ruthenium and osmium alkylidene complexes substituted with an N-heterocyclic carbene ligand are used to catalyze cross-metathesis reactions to provide a variety of substituted and functionalized olefins, including phosphonate-substituted olefins, directly halogenated olefins, 1,1,2-trisubstituted olefins, and quaternary allylic olefins. The invention further provides a method for creating functional diversity using the aforementioned complexes to catalyze cross-metathesis reactions of a first olefinic reactant, which may or may not be substituted with a functional group, with each of a plurality of different olefinic reactants, which may or may not be substituted with functional groups, to give a plurality of structurally distinct olefinic products. The methodology of the invention is also useful in facilitating the stereoselective synthesis of 1,2-disubstituted olefins in the cis configuration.
摘要翻译： 本发明涉及第8族过渡金属卡宾络合物用作烯烃交叉复分解反应的催化剂。 特别地，用N-杂环卡宾配体取代的钌和锇亚烷基配合物用于催化交叉复分解反应以提供各种取代和官能化的烯烃，包括膦酸酯取代的烯烃，直接卤代烯烃， 三取代烯烃和季烯丙烯烯烃。 本发明还提供了一种使用上述配合物来催化可能或可能不被官能团取代的第一种烯属反应物与多种不同的烯属反应物中的每一种的交叉复分解反应的方法， 或可以不被官能团取代，得到多个结构不同的烯烃产物。 本发明的方法还可用于促进顺式构型中的1,2-二取代烯烃的立体选择性合成。
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2.发明授权Synthesis of functionalized and unfunctionalized olefins via cross and ring-closing metathesis 有权通过交叉和闭环复分解合成官能化和非官能化烯烃公开(公告)号：US06794534B2
公开(公告)日：2004-09-21
申请号：US09891144
申请日：2001-06-25
IPC分类号： C07C6952
CPC分类号： C07D303/22 , C07B37/00 , C07C45/673 , C07C45/69 , C07C45/72 , C07C67/293 , C07C67/343 , C07C201/12 , C07C231/12 , C07C259/06 , C07C315/04 , C07D263/22 , C07D263/24 , C07D309/12 , C07D309/30 , C07D315/00 , C07D317/12 , C07D319/12 , C07D319/14 , C07D321/08 , C07D413/12 , C07C49/597 , C07C317/14 , C07C233/09 , C07C233/11 , C07C205/06 , C07C205/56
摘要： The invention is directed to the cross-metathesis and ring-closing metathesis reactions between geminal disubstituted olefins and terminal olefins, wherein the reaction employs a Ruthenium or Osmium metal carbene complex. Specifically, the invention relates to the synthesis of &agr;-functionalized or unfunctionalized olefins via intermolecular cross-metathesis and intramolecular ring-closing metathesis using a ruthenium alkylidene complex. The catalysts preferably used in the invention are of the general formula wherein: M is ruthenium or osmium; X and X1 are each independently an anionic ligand; L is a neutral electron donor ligand; and, R, R1R6, R7, R8, and R9 are each independently hydrogen or a substituent selected from the group consisting of C1-C20 alkyl, C2-C20 alkenyl, C2-C20 alkynyl, aryl, C1-C20 carboxylate, C1-C20 alkoxy, C2-C20 alkenyloxy, C2-C20 alkynyloxy, aryloxy, C2-C20 alkoxycarbonyl, C1-C20 alkylthio, C1-C20 alkylsulfonyl and C1-C20 alkylsulfinyl.
摘要翻译： 本发明涉及孪生二取代的烯烃和末端烯烃之间的交叉复分解和闭环复分解反应，其中该反应采用钌或锇金属卡宾络合物。 具体地，本发明涉及通过分子间交叉复分解和使用亚烷基钌络合物的分子内闭合复分解来合成α-官能化或未官能化的烯烃。 本发明优选使用的催化剂是通式为：M为钌或锇; X和X 1各自独立地为阴离子配体; L为中性给电子体配位体; 并且R 1，R 1，R 6，R 7，R 8和R 9各自独立地为氢或选自C 1 -C 20烷基，C 2 -C 20烯基 ，C 2 -C 20炔基，芳基，C 1 -C 20羧酸酯，C 1 -C 20烷氧基，C 2 -C 20链烯氧基，C 2 -C 20炔氧基，芳氧基，C 2 -C 20烷氧基羰基，C 1 -C 20烷硫基，C 1 -C 20烷基磺酰基和C 1 -C 20烷基亚磺酰基。
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公开(公告)号：US06803429B2
公开(公告)日：2004-10-12
申请号：US10114674
申请日：2002-04-01
IPC分类号： C08F444
CPC分类号： C07C67/343 , B01J31/18 , B01J31/2226 , B01J31/2273 , B01J31/24 , B01J31/2404 , B01J2231/543 , B01J2531/80 , B01J2531/821 , B01J2540/32 , C07C6/06 , C07C45/68 , C07C51/353 , C07C67/475 , C07C2531/22 , C07C47/21 , C07C49/203 , C07C57/13 , C07C69/587 , C07C69/757 , C07C69/74 , C07C69/602
摘要： A catalytic method is provided for a ring-opening cross-metathesis reaction between a cycloolefinic substrate and a second olefinic reactant, wherein the catalyst used is a transition metal alkylidene complex substituted with an N-heterocyclic carbene ligand. The substrates are selected so that the rate of the cross-metathesis reaction of the second olefinic reactant, kCM, is greater than or equal to the rate of the ring-opening metathesis reaction, kRO. In this way, the predominant ROCM product is a monomer, dimer, and/or oligomer, but not a polymer. The invention additionally provides for selective production of an end-differentiated olefinic product, using trisubstituted cycloolefins as substrates and/or a subsequent cross-metathesis reaction following an initial ROCM step. The cycloolefinic substrates include low-strain olefins such as cyclohexene as well as higher strain olefins such as cyclooctene.
摘要翻译： 提供了用于环烯基底物和第二烯属反应物之间的开环交叉复分解反应的催化方法，其中使用的催化剂是被N-杂环卡宾配体取代的过渡金属亚烷基络合物。 选择底物使得第二烯属反应物的交叉复分解反应速率kCM大于或等于开环复分解反应速率（kRO）。 以这种方式，主要的ROCM产物是单体，二聚体和/或低聚物，但不是聚合物。 本发明另外提供了在初始ROCM步骤之后使用三取代的环烯烃作为底物和/或随后的交叉复分解反应来选择性生产末端分解的烯烃产物。 环烯烃底物包括低应变烯烃如环己烯以及较高级烯烃如环辛烯。
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4.发明授权公开(公告)号：US07034096B2
公开(公告)日：2006-04-25
申请号：US10371196
申请日：2003-02-19
申请人： Tae-Lim Choi , Choon Woo Lee , Hyunjin M. Kim , Robert H. Grubbs
发明人： Tae-Lim Choi , Choon Woo Lee , Hyunjin M. Kim , Robert H. Grubbs
CPC分类号： C07F7/1892 , B01J31/2265 , C08G61/08
摘要： This invention relates generally to synthetic procedures that include the step of ring-opening metathesis of cyclic olefins and reaction with an acyclic diene co-reactant to produce olefin macrocycles by ring expansion, or alternatively. The ring expansion of the cyclic olefin is provided by three types of sequential olefin metathesis (ring-opening, cross, and ring-closing olefin metathesis). More particularly, the invention pertains to synthesis of olefin macrocycles via olefin metathesis reactions using a Group 8 transition metal complex as the metathesis catalyst. Macrocycles provided herein have a variety of uses in the pharmaceutical, biomedical, organic synthesis and chemical industries, such as the production of crown ethers that are useful as metal complexing species.
摘要翻译： 本发明一般涉及合成方法，其包括环烯烃的开环复分解步骤和与无环二烯共反应物反应以通过环扩展产生烯烃大环化合物的步骤。 环烯烃的环扩展由三种顺序烯烃复分解（开环，交叉和闭环烯烃复分解）提供。 更具体地，本发明涉及通过使用第8族过渡金属络合物作为复分解催化剂的烯烃复分解反应合成烯烃大环化合物。 本文提供的大环在药物，生物医学，有机合成和化学工业中具有多种用途，例如可用作金属络合物质的冠醚的生产。
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公开(公告)号：US06987154B2
公开(公告)日：2006-01-17
申请号：US10371195
申请日：2003-02-19
IPC分类号： C08F4/44
CPC分类号： C07F7/1892 , B01J31/2265 , C08G61/08
摘要： This invention relates generally to synthetic procedures that include the step of ring-opening metathesis of cyclic olefins and reaction with an acyclic diene co-reactant to produce regularly repeating A,B-alternating olefin polymers. The A,B-alternating polymers are produced by varying reaction conditions and/or reactant proportions and using only two types of olefin metathesis (ring-opening and cross) to provide regularly repeating ABAB . . . etc. polymers via ring-opening metathesis polymerization (ROMP). More particularly, the invention pertains to synthesis of A,B-alternating olefin polymers via olefin metathesis reactions using a Group 8 transition metal complex as the metathesis catalyst. Polymers provided herein have utility in a variety of fields, including not only polymer chemistry per se, but also in the pharmaceutical, biomedical, and packaging industries where the structure and properties of polymers need to be tightly controlled.
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