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1. 发明授权

US06225251B1 Catalyst efficiency for supported metallocene catalyst 有权
标题翻译：负载金属茂催化剂的催化剂效率
公开(公告)号：US06225251B1
公开(公告)日：2001-05-01
申请号：US09304974
申请日：1999-05-04
申请人： Edwar S. Shamshoum , Margarito Lopez , B. Raghava Reddy , Theodore G. Harris
发明人： Edwar S. Shamshoum , Margarito Lopez , B. Raghava Reddy , Theodore G. Harris
IPC分类号： B01J3100
CPC分类号： C08F10/00 , C08F4/61912 , C08F4/61927 , Y10S526/943 , C08F4/61916
摘要： The invention provides a polymerization process with improved catalyst activity of a metallocene catalyst supported on silica treated with MAO, a process for supporting a metallocene compound on silica treated with MAO, a metallocene catalyst supported on silica treated with MAO within a certain temperature range and a process for making a metallocene catalyst supported on silica treated with MAO. The invention includes supporting the metallocene compound on a MAO-treated silica at a temperature of below 0° C. The supported catalyst is activated with an aluminum alkyl. The catalyst may be prepolymerized in a tubular reactor prior to being introduced into the polymerization reaction zone.
摘要翻译：本发明提供了一种聚合方法，其具有改进的催化剂活性，其负载在用MAO处理的二氧化硅上的茂金属催化剂，用MAO处理的二氧化硅上负载茂金属化合物的方法，负载在一定温度范围内用MAO处理的二氧化硅上的茂金属催化剂和制备用MAO处理的二氧化硅上负载的茂金属催化剂的方法。本发明包括在低于0℃的温度下在MAO处理的二氧化硅上负载茂金属化合物。负载的催化剂用烷基铝活化。催化剂可以在引入聚合反应区之前在管式反应器中预聚合。

2. 发明授权

US5968864A Catalyst efficiency for supported metallocene catalyst 失效
标题翻译：负载金属茂催化剂的催化剂效率
公开(公告)号：US5968864A
公开(公告)日：1999-10-19
申请号：US772667
申请日：1996-12-20
申请人： Edwar S. Shamshoum , Margarito Lopez , B. Raghava Reddy , Theodore G. Harris
发明人： Edwar S. Shamshoum , Margarito Lopez , B. Raghava Reddy , Theodore G. Harris
IPC分类号： C08F4/02 , C08F4/619 , C08F4/6192 , C08F4/64 , C08F4/642 , C08F10/00
CPC分类号： C08F10/00 , C08F4/61912 , C08F4/61927 , Y10S526/943
摘要： The invention provides a process for making a metallocene catalyst supported on silica treated with MAO. The invention includes supporting the metallocene compound on a MAO-treated silica at a temperature of below 0.degree. C. The supported catalyst is activated with an aluminum alkyl. The catalyst may be prepolymerized in a tubular reactor prior to being introduced into the polymerization reaction zone.
摘要翻译：本发明提供一种制备负载在用MAO处理的二氧化硅上的茂金属催化剂的方法。本发明包括在低于0℃的温度下在MAO处理的二氧化硅上负载金属茂化合物。负载型催化剂用烷基铝活化。催化剂可以在引入聚合反应区之前在管式反应器中预聚合。

3. 发明授权

US06201081B1 Catalyst efficiency for supported metallocene catalyst 有权
公开(公告)号：US06201081B1
公开(公告)日：2001-03-13
申请号：US09305135
申请日：1999-05-04
申请人： Edwar S. Shamshoum , Margarito Lopez , B. Raghava Reddy , Theodore G. Harris
发明人： Edwar S. Shamshoum , Margarito Lopez , B. Raghava Reddy , Theodore G. Harris
IPC分类号： C08F442
CPC分类号： C08F10/00 , C08F4/61912 , C08F4/61927 , Y10S526/943 , C08F4/61916
摘要： The invention provides a polymerization process with improved catalyst activity of a metallocene catalyst supported on silica treated with MAO, a process for supporting a metallocene compound on silica treated with MAO, a metallocene catalyst supported on silica treated with MAO within a certain temperature range and a process for making a metallocene catalyst supported on silica treated with MAO. The invention includes supporting the metallocene compound on a MAO-treated silica at a temperature of below 0° C. The supported catalyst is activated with an aluminum alkyl. The catalyst may be prepolymerized in a tubular reactor prior to being introduced into the polymerization reaction zone.

4. 发明授权

US6114480A Process and catalyst for producing polyolefins having low molecular weight 失效
标题翻译：用于生产低分子量聚烯烃的方法和催化剂
公开(公告)号：US6114480A
公开(公告)日：2000-09-05
申请号：US635274
申请日：1996-04-19
申请人： Edwar S. Shamshoum , B. Raghava Reddy , Margarito Lopez
发明人： Edwar S. Shamshoum , B. Raghava Reddy , Margarito Lopez
IPC分类号： C08F4/64 , C08F4/619 , C08F4/6192 , C08F4/642 , C08F4/6592 , C08F10/00 , C08F110/02 , C08F110/06
CPC分类号： C08F10/00 , C08F110/02 , C08F110/06 , C08F4/61912 , C08F4/61927 , Y10S526/943
摘要： The invention provides a metallocene catalyst for use in preparing polyolefins having low molecular weight. The catalyst comprises a metallocene compound generally described by the formula R"(C.sub.5 R.sub.4) (H.sub.2 C.sub.5 C.sub.4 H.sub.4)MeQ.sub.p wherein (C.sub.5 R.sub.4) is a substituted cyclopentadienyl ring; (H.sub.2 C.sub.5 C.sub.4 H.sub.4) is an indenyl ring; (C.sub.5 R.sub.4) has one R substituent in a distal position which is at least as bulky as a t-butyl radical; R" is a structural bridge between the (C.sub.5 R.sub.4) and (H.sub.2 C.sub.5 C.sub.4 H.sub.4) rings to impart stereorigidity; Q is a hydrocarbyl radical, such as an alkyl, aryl, alkenyl, alkylaryl or arylalkyl radical having 1-20 carbon atoms or is a halogen; Me is a Group IIIB, IVB, VB, or VIB metal as positioned in the Periodic Table of Elements; and p is the valence of Me minus 2. This catalyst produces a crystalline or atactic polymer with a low molecular weight and narrow or broad molecular weight distribution depending upon the isomer(s) used in polymerization. A single threo-isomer produces isotactic polypropylene and a single erythro-isomer produces atactic polypropylene, both polymers having narrow molecular weight distribution. When the bridge between the substituted cyclopentadienyl and the indenyl rings is substituted such that four diastereomers are possible, the threo-isomers produce isotactic polypropylene with broad molecular weight distribution.
摘要翻译：本发明提供用于制备低分子量聚烯烃的茂金属催化剂。该催化剂包含一般由式R“（C5R4）（H2C5C4H4）MeQp描述的茂金属化合物，其中（C5R4）是取代的环戊二烯基环; （H2C5C4H4）是茚基环; （C5R4）在远端位置具有至少与叔丁基一样庞大的一个R取代基; R“是（C5R4）和（H2C5C4H4）环之间的结构桥，以赋予立体刚度; Q是烃基，例如具有1-20个碳原子的烷基，芳基，烯基，烷基芳基或芳基烷基，或者是卤素; Me是位于元素周期表中的IIIB，IVB，VB或VIB族金属; 并且p是Me的化合价减去2.该催化剂产生具有低分子量和窄或宽分子量分布的结晶或无规立构聚合物，这取决于聚合中使用的异构体。单一苏式异构体产生全同立构聚丙烯，单一的异构异构体产生无规聚丙烯，两种聚合物具有窄的分子量分布。当取代的环戊二烯基和茚基环之间的桥被取代使得四个非对映异构体是可能的时，苏式异构体产生具有宽分子量分布的全同立构聚丙烯。

5. 发明授权

US06376418B1 Process and catalyst for producing polyolefins having low molecular weight 失效
标题翻译：用于生产低分子量聚烯烃的方法和催化剂
公开(公告)号：US06376418B1
公开(公告)日：2002-04-23
申请号：US09559775
申请日：2000-04-27
申请人： Edwar S. Shamshoum , B. Raghava Reddy , Margarito Lopez
发明人： Edwar S. Shamshoum , B. Raghava Reddy , Margarito Lopez
IPC分类号： B01J3100
CPC分类号： C08F10/00 , C08F4/61912 , C08F4/61927 , C08F110/02 , C08F110/06 , Y10S526/943 , C08F2500/02 , C08F2500/03
摘要： The invention provides a metallocene catalyst for use in preparing polyolefins having low molecular weight. The catalyst comprises a bridged metallocene in which one of the cyclopentadienyl rings is substituted in a substantially different manner from the other ring. The catalyst comprises a metallocene compound generally described by the formula R″(C5R4)(R′2C5C4R′4)MeQp wherein (C5R4) is a substituted cyclopentadienyl ring; (R′2C5C4R′4n) is an indenyl ring or substituted indenyl ring; each R and R′ is hydrogen or hydrocarbyl radical having from 1-20 carbon atoms, a halogen, an alkoxy, and alkoxy alkyl or an alkylamino radical, each R and R′ may be the same or different; (C5R4) has one R substituent in a distal position which is at least as bulky as a t-butyl radical; R″ is a structural bridge between the (C5R4) and (R′2C5C4R′4) rings to impart stereorigidity; Q is a hydrocarbyl radical, such as an alkyl, aryl, alkenyl, alkylaryl or arylalkyl radical having 1-20 carbon atoms or is a halogen; Me is a Group IIIB, IVB, VB, or VIB metal as positioned in the Periodic Table of Elements; and p is the valence of Me minus 2.
摘要翻译：本发明提供用于制备低分子量聚烯烃的茂金属催化剂。该催化剂包括其中一个环戊二烯基环以与另一个环基本不同的方式被取代的桥连茂金属。该催化剂包含一般由式R“（C5R4）（R'2C5C4R'4）MeQp描述的茂金属化合物，其中（C5R4）是取代的环戊二烯基环; （R'2C5C4R'4n）是茚基环或取代的茚基环; 每个R和R'是氢或具有1-20个碳原子的烃基，卤素，烷氧基和烷氧基烷基或烷基氨基，每个R和R'可以相同或不同; （C5R4）在远端位置具有至少与叔丁基一样庞大的一个R取代基; R“是（C5R4）和（R'2C5C4R'4）环之间的结构桥，以赋予立体刚度; Q是烃基，例如具有1-20个碳原子的烷基，芳基，烯基，烷基芳基或芳基烷基，或者是卤素; Me是位于元素周期表中的IIIB，IVB，VB或VIB族金属; 而p是Me的价数减去2。

6. 发明授权

US5807800A Process for producing stereospecific polymers 失效
标题翻译：制备立体有择聚合物的方法
公开(公告)号：US5807800A
公开(公告)日：1998-09-15
申请号：US798245
申请日：1997-02-11
申请人： Edwar S. Shamshoum , Margarito Lopez
发明人： Edwar S. Shamshoum , Margarito Lopez
IPC分类号： C08F4/02 , C08F4/602 , C08F4/639 , C08F4/6392 , C08F4/64 , C08F4/642 , C08F4/659 , C08F4/6592 , C08F10/06 , C08F12/04 , C08F12/08 , C08F14/06
CPC分类号： C08F10/06 , C08F10/00 , C08F110/06 , C08F12/04 , C08F4/63927 , Y10S526/943
摘要： Stereospecific catalysts and processes for the stereotactic polymerization of ethylenically unsaturated monomers, specifically C.sub.3 -C.sub.4 alpha olefins involving a molecular sieve supported metallocene catalyst comprising a stereospecific metallocene catalyst component and a co-catalyst component. The metallocene catalyst component incorporates a metallocene ligand structure having two sterically dissimilar cyclopentadienyl ring structures coordinated with the central transition metal atom. Both the metallocene catalyst component and the co-catalyst component are supported on a molecular sieve having an average effective pore size which is less than the kinetic diameter of at least one of said ring structures. This supported catalyst is contacted in a polymerization reaction zone with an ethylenically unsaturated monomer which contains 3 or more carbon atoms or which is a substituted vinyl compound under polymerization conditions to produce stereospecific polymerization of the monomer. The supported catalyst incorporates a molecular sieve support having an average effective pore size within the range of 5-10 angstroms. The metallocene component can be an unbalanced metallocene having a ligand structure in which stereorigidity is imparted by means of a structural bridge extending between dissimilar cyclopentadienyl groups, for example, a fluorenyl group, a cyclopentadienyl group, of a ligand which exhibits bilateral symmetry. The specific zeolite supports are zeolite Y, zeolite X, mordenite, and zeolite .beta.. Others include various zeolites of the ZSM substitutional series, including ZSM-5, ZSM-11, and ZSM-12.
摘要翻译：烯属不饱和单体的立体定向聚合的立体定向催化剂和方法，特别是涉及包含立体特异性金属茂催化剂组分和助催化剂组分的分子筛负载金属茂催化剂的C3-C4α烯烃。茂金属催化剂组分包含具有两个与中心过渡金属原子配位的空间不同的环戊二烯基环结构的茂金属配体结构。金属茂催化剂组分和助催化剂组分都被负载在平均有效孔径小于所述环结构中的至少一个的动力学直径的分子筛上。该聚合反应区中的负载型催化剂与含有3个以上碳原子的烯键式不饱和单体接触，或者在聚合条件下与取代的乙烯基化合物接触，生成单体的立体有择聚合。载体催化剂含有平均有效孔径在5-10埃范围内的分子筛载体。茂金属组分可以是具有配体结构的不平衡茂金属，其中立体刚性通过在不同的环戊二烯基之间延伸的结构桥，例如具有双侧对称性的配体的芴基，环戊二烯基。特定的沸石载体是沸石Y，沸石X，丝光沸石和β沸石。其他还包括ZSM替代系列的各种沸石，包括ZSM-5，ZSM-11和ZSM-12。

7. 发明授权

US5753785A Production of E-B copolymers with a single metallocene catalyst and a single monomer 失效
标题翻译：用单一茂金属催化剂和单一单体生产E-B共聚物
公开(公告)号：US5753785A
公开(公告)日：1998-05-19
申请号：US766075
申请日：1996-12-16
申请人： Baireddy Raghava Reddy , Edwar S. Shamshoum , Margarito Lopez
发明人： Baireddy Raghava Reddy , Edwar S. Shamshoum , Margarito Lopez
IPC分类号： C08F4/642 , C08F4/60 , C08F4/619 , C08F4/6192 , C08F4/622 , C08F4/659 , C08F4/6592 , C08F110/02 , C08F210/08 , C08F210/16 , C08F4/623 , C08F210/02
CPC分类号： C08F210/16 , C08F110/02 , C08F210/08 , C08F4/61927 , C08F4/61912 , Y10S526/943
摘要： A process of polymerizing ethylene with a catalyst using a single metallocene catalyst comprising a bridged metallocene compound having two cyclopentadienyl rings, one substituted with a bulky group in a distal position and one substituted such that a fused ring, substituted or unsubstituted, is formed, which produces a copolymer of ethylene. The metallocene catalyst promotes simultaneous oligomerization of a fraction of ethylene to form a comonomer in situ and copolymerization of the remaining ethylene and the comonomer to form a copolymer.
摘要翻译：使用包含具有两个环戊二烯基环的桥连金属茂化合物的单茂金属催化剂与一种催化剂聚合乙烯的方法，一个被远端位置的大体积取代，一个被取代成取代或未取代的稠环，其中产生乙烯的共聚物。金属茂催化剂促进一部分乙烯的同时低聚，原位形成共聚单体，并使剩余的乙烯和共聚单体共聚以形成共聚物。

8. 发明授权

US06432860B1 Supported metallocene catalysts 有权
标题翻译：负载金属茂催化剂
公开(公告)号：US06432860B1
公开(公告)日：2002-08-13
申请号：US09273819
申请日：1999-03-22
申请人： Edwar S. Shamshoum , Margarito Lopez
发明人： Edwar S. Shamshoum , Margarito Lopez
IPC分类号： B01J3100
CPC分类号： C08F10/06 , C08F4/025 , C08F4/65912 , C08F4/65927 , C08F12/04 , C08F110/06 , Y02P20/52 , Y10S526/943 , C08F4/65916 , C08F2500/16
摘要： Supported stereospecific catalysts and processes for the stereotactic propagation of a polymer chain derived from ethylenically unsaturated monomers which contain three or more carbon atoms or which are substituted vinyl compounds, such as styrene and vinyl chloride. One application is the stereospecific propagation of C3-C4 alpha olefins, particularly the polymerization of propylene to produce syndiotactic polypropylene over a supported metallocene catalyst comprising a stereospecific metallocene catalyst component incorporating a metallocene ligand structure having two sterically dissimilar cyclopentadienyl ring structures coordinated to the central transition metal atom. Both of the cyclopentadienyl groups are in a relationship with one another by virtue of bridge or substituent groups, which provide a stereorigid relationship relative to the coordinating transition metal atom to prevent rotation of said ring structures. The metallocene catalyst component and a co-catalyst component, an alumoxane or an alkyl aluminum, are supported on a particulate silica support comprising spheroidal silica particles having an average diameter within the range of 5-40 microns and an average effective pore size within the range of 50-350 angstroms. The particulate silica support contains at least 50 wt. % of the supported catalyst component within the pore volume of the silica support. The particles are preferably toroidal shaped, i.e. donut shaped.
摘要翻译：支持的立体定向催化剂和衍生自含有三个或更多个碳原子的乙烯基不饱和单体的聚合物链的立体定向增长的方法，或者是取代的乙烯基化合物如苯乙烯和氯乙烯。一种应用是C3-C4α烯烃的立体有择性扩增，特别是丙烯在负载金属茂催化剂下产生间同立构聚丙烯的聚合反应，该载体包含立体特异性金属茂催化剂组分，该催化剂组分含有具有两个与中心转移配位的空间不同的环戊二烯基环结构的茂金属配体结构金属原子。两个环戊二烯基通过桥或取代基相互关系，其提供相对于配位过渡金属原子的立体刚性关系以防止所述环结构的旋转。金属茂催化剂组分和助催化剂组分，铝氧烷或烷基铝负载在颗粒状二氧化硅载体上，所述颗粒二氧化硅载体包含平均直径在5-40微米范围内的平均直径范围的球形二氧化硅颗粒，并且平均有效孔径在该范围内 50-350埃。颗粒状二氧化硅载体含有至少50wt。负载的催化剂组分的百分比在二氧化硅载体的孔体积内。颗粒优选为环形，即环形。

9. 发明授权

US06362125B1 Metallocene catalyst and catalyst system for producing polypropylene blend of iso and syndio-tactic polypropylene 有权
标题翻译：茂金属催化剂和催化剂体系，用于生产异丙烯和聚丙烯聚丙烯共混物
公开(公告)号：US06362125B1
公开(公告)日：2002-03-26
申请号：US09576405
申请日：2000-05-22
申请人： Edwar S. Shamshoum , Margarito Lopez , Ted G. Harris, III , Sehyun Kim
发明人： Edwar S. Shamshoum , Margarito Lopez , Ted G. Harris, III , Sehyun Kim
IPC分类号： B01J3100
CPC分类号： C08F10/06 , C08F4/65912 , C08F4/65927 , C08F110/06 , Y02P20/52 , Y10S526/943 , C08F4/65904 , C08F4/65916 , C08F2500/15 , C08F2500/16 , C08F2500/03 , C08F2500/06 , C08F2500/20
摘要： A polyolefin metallocene catalyst which includes two metallocene components, a stereorigid isospecific metallocene catalyst component and a stereorigid syndiospecific metallocene catalyst component, both of which are supported upon the same support. A method of forming a catalyst system includes contacting the above catalyst with a cocatalyst or Lewis acid. A method of polymerization includes contacting an olefin with the catalyst system.
摘要翻译：一种聚烯烃茂金属催化剂，其包含两种茂金属组分，一种立体刚性同分异构茂金属催化剂组分和一种立体刚性同分子特异性茂金属催化剂组分，两者均负载在相同的载体上。形成催化剂体系的方法包括使上述催化剂与助催化剂或路易斯酸接触。聚合方法包括使烯烃与催化剂体系接触。

10. 发明授权

US06855782B2 Process for producing stereospecific polymers 有权
标题翻译：制备立体有择聚合物的方法
公开(公告)号：US06855782B2
公开(公告)日：2005-02-15
申请号：US10114185
申请日：2002-04-02
申请人： Edwar S. Shamshoum , Margarito Lopez
发明人： Edwar S. Shamshoum , Margarito Lopez
IPC分类号： C08F4/02 , C08F4/60 , C08F4/6392 , C08F4/642 , C08F4/659 , C08F4/6592 , C08F10/06 , C08F12/04 , C08F110/06
CPC分类号： C08F10/06 , C08F4/025 , C08F4/65912 , C08F4/65927 , C08F12/04 , C08F110/06 , Y02P20/52 , Y10S526/943 , C08F4/65916 , C08F2500/16
摘要： Supported stereospecific catalysts and processes for the stereotactic propagation of a polymer chain derived from ethylenically unsaturated monomers which contain three or more carbon atoms or which are substituted vinyl compounds, such as styrene and vinyl chloride. One application is the stereospecific propagation of C3-C4 alpha olefins, particularly the polymerization of propylene to produce syndiotactic polypropylene over a supported metallocene catalyst comprising a stereospecific metallocene catalyst component incorporating a metallocene ligand structure having two sterically dissimilar cyclopentadienyl ring structures coordinated with the central transition metal atom. Both of the cyclopentadienyl groups are in a relationship with one another by virtue of bridge or substituent groups, which provide a stereorigid relationship relative to the coordinating transition metal atom to prevent rotation of said ring structures. The metallocene catalyst component and a co-catalyst component, an alumoxane or an alkyl aluminum, are supported on a particulate silica support comprising spheroidal silica particles having an average diameter within the range of 5-40 microns and an average effective pore size within the range of 50-350 angstroms. The particulate silica support contains at least 50 wt. % of the supported catalyst component within the pore volume of the silica support.
摘要翻译：支持的立体定向催化剂和衍生自含有三个或更多个碳原子的乙烯基不饱和单体的聚合物链的立体定向增长的方法，或者是取代的乙烯基化合物如苯乙烯和氯乙烯。一个应用是C3-C4α烯烃的立体特异性扩增，特别是丙烯在负载金属茂催化剂下聚合制备间同立构聚丙烯的方法，该催化剂包含立体特异性茂金属催化剂组分，该组分含有具有两个与中心转移配位的空间不同的环戊二烯基环结构的茂金属配体结构金属原子。两个环戊二烯基通过桥或取代基相互关系，其提供相对于配位过渡金属原子的立体刚性关系以防止所述环结构的旋转。金属茂催化剂组分和助催化剂组分，铝氧烷或烷基铝负载在颗粒状二氧化硅载体上，所述颗粒二氧化硅载体包含平均直径在5-40微米范围内的平均直径范围的球形二氧化硅颗粒，并且平均有效孔径在该范围内 50-350埃。颗粒状二氧化硅载体含有至少50wt。负载的催化剂组分的百分比在二氧化硅载体的孔体积内。

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