公开(公告)号：US06960279B2

公开(公告)日：2005-11-01

申请号：US10139524

申请日：2002-05-06

Applicant: James T. Merrill

Inventor： James T. Merrill

IPC: C07C7/04 ,  C07C7/20 ,  C07C15/46 ,  C08F2/42 ,  C08F12/00 ,  B01D3/34 ,  C07C7/05 ,  C09K3/00

CPC classification number: C07C7/20 ,  C08F2/40 ,  C08F112/08 ,  C07C15/46 ,  C07C15/44 ,  C08F2/38 ,  C08F2/42

Abstract: Disclosed is the observation that 7-aryl-quinone methides and 4-tert-butylcatechol, when used in combination in a vinyl aromatic monomer to inhibit polymerization,do not inhibit polymerization to the same extend as each would if used separately. Stated another way, a phenomenon has been observed that when these two compounds are used together, they can, to a large extent, render each other unable to inhibit polymerization in a vinyl aromatic monomer. Also disclosed are methods of preventing adverse results of this interaction when undesired and a method of using this interaction to prepare a reactive vinyl aromatic monomer having a concentration of 4-tert-butylcatechol that would otherwise inhibit polymerization. The invention is disclosed to be useful with the production and storage of any vinyl aromatic monomer and is disclosed to be particularly useful with the production and storage of styrene monomer.

Abstract translation: 公开的观察结果是，7-芳基 - 醌甲基化物和4-叔丁基邻苯二酚在乙烯基芳族单体中组合用于抑制聚合时不抑制聚合反应至相同的延伸，如同分别使用的那样。 换句话说，已经观察到当这两种化合物一起使用时，它们可以在很大程度上彼此不能抑制乙烯基芳族单体中的聚合。 还公开了防止这种相互作用的不利结果的方法，以及使用该相互作用制备具有4-叔丁基儿茶酚浓度的反应性乙烯基芳族单体的方法，否则其将抑制聚合。 公开了本发明可用于任何乙烯基芳族单体的生产和储存，并且被公开用于苯乙烯单体的生产和储存特别有用。

公开(公告)号：US06864399B2

公开(公告)日：2005-03-08

申请号：US10193792

申请日：2002-07-12

Applicant: James T. Merrill ,  James R. Butler

Inventor： James T. Merrill ,  James R. Butler

IPC: B01J29/70 ,  C07C2/66

CPC classification number: B01J29/7007 ,  B01J2229/42 ,  C07C2/66 ,  C07C2521/08 ,  C07C2529/70 ,  Y02P20/544 ,  Y02P20/584 ,  C07C15/073

Abstract: The alkylation of benzene-containing feedstock over a zeolite beta alkylation catalyst which is formulated with a silica binder and has an average regeneration coefficient of at least 95% for at least three regenerations. The alkylation reaction is carried out in the liquid phase or supercritical region with a C2-C4 alkylating agent, specifically ethylene. The catalyst exhibits a regeneration coefficient of at least 95% after ethylation of the benzene with ethylene at a benzene/ethylene mole ratio of less than 10. The ethylation of benzene occurs at an initial designated primary activity. The operation of the reaction zone is continued until the activity of the catalyst for the ethylation of benzene decreases by a value of at least 0.1% and not more 1% from the initial designated primary activity. The operation of the reaction for alkylation is terminated and a regeneration procedure is instituted in which the catalyst is regenerated in an oxidizing environment at an average temperature of no more than 500° C. At the conclusion of the regeneration procedure, the operation of the alkylation zone is reinstituted with the reaction zone again operated under conditions as described above followed by regeneration.

Abstract translation: 在沸石β烷基化催化剂上的含苯原料的烷基化，其用二氧化硅粘合剂配制，并且对至少三次再生具有至少95％的平均再生系数。 烷基化反应在液相或超临界区域用C2-C4烷基化剂，特别是乙烯进行。 苯与乙烯在苯/乙烯摩尔比小于10的乙醚化后，催化剂表现出至少95％的再生系数。苯的乙基化发生在初始指定的主要活性。 反应区的操作继续进行，直到苯的乙基化催化剂的活性从初始指定的主要活性降低至少0.1％且不超过1％的值。 终止烷基化反应的操作，并且在不超过500℃的平均温度下在氧化环境中再生催化剂的再生步骤。在再生过程结束时，烷基化操作 区域被重新配置，反应区域再次在如上所述的条件下操作，随后再生。

公开(公告)号：US06222084B1

公开(公告)日：2001-04-24

申请号：US09289488

申请日：1999-04-09

Applicant: Ashim Kumar Ghosh ,  James T. Merrill ,  James R. Butler

Inventor： Ashim Kumar Ghosh ,  James T. Merrill ,  James R. Butler

IPC: C07C266

CPC classification number: C07C15/073 ,  C07C2/66 ,  C07C2529/08 ,  C07C2529/40

Abstract: Process for the production of ethylbenzene by alkylation over a silicalite alkylation catalyst with subsequent transalkylation of diethylbenzene with the alkylation catalyst and conditions selected to retard xylene production and also heavies production. Benzene and ethylene are applied to a multi-stage alkylation reaction zone having a plurality of series-connected catalyst beds containing silicalite of a predominantly monoclinic symmetry having a silica/alumina ratio of at least 275. Gas-phase ethylation of benzene is at a flow rate to provide a space velocity of benzene over the catalyst to produce a xylene concentration of about 600 ppm or less of the ethylbenzene content. Periodically the space velocity may be increased to a value which is greater than the space velocity associated with a minimum concentration of diethylbenzene in the alkylation product such that diethylbenzene production is enhanced while minimizing any attendant transalkylation reactions within the alkylation reaction zone. The alkylation reactor output is applied to an intermediate recovery zone for the separation and recovery of ethylbenzene with the recovery of a polyalkylated aromatic component which is supplied along with benzene to a transalkylation reaction zone for disproportionation to provide a reduced diethylbenzene content and an enhanced ethylbenzene content. A specific monoclinic silicalite alkylation catalyst has a silica/alumina ratio of at least 300 and has a crystal size of less than one micron.

Abstract translation: 通过在硅沸石烷基化催化剂上烷基化生产乙苯的方法，随后用烷基化催化剂对二乙基苯进行烷基转移和选择用于延迟二甲苯生产和重质生产的条件。 苯和乙烯被施加到多级烷基化反应区，该多级烷基化反应区具有多个串联连接的催化剂床，该催化剂床含有主要单斜对称的硅沸石，其二氧化硅/氧化铝比至少为275.苯的气相乙基化处于流动 速率以提供苯在催化剂上的空速，以产生约600ppm或更少的乙苯含量的二甲苯浓度。 定期地，空间速度可以增加到大于与烷基化产物中的二乙基苯的最小浓度相关联的空间速度的值，使得二苯基产生增强，同时最小化在烷基化反应区内的任何伴随的烷基转移反应。 将烷基化反应器输出应用于中间回收区，用于分离和回收乙苯，回收与苯一起供应的多烷基化芳族组分至用于歧化的烷基转移反应区，以提供还原的二乙苯含量和增强的乙苯含量 。 特定的单斜硅沸石烷基化催化剂具有至少300的二氧化硅/氧化铝比例，其晶体尺寸小于1微米。

公开(公告)号：US6057485A

公开(公告)日：2000-05-02

申请号：US193310

申请日：1998-11-17

Applicant: James T. Merrill ,  James R. Butler ,  Ashim Kumar Ghosh

Inventor： James T. Merrill ,  James R. Butler ,  Ashim Kumar Ghosh

IPC: B01J29/06 ,  C07B61/00 ,  C07C2/66 ,  C07C15/073 ,  C07C1/00 ,  C07C2/64 ,  C07C2/68

CPC classification number: C07C15/073 ,  C07C2/66 ,  C07C2529/035 ,  C07C2529/08

Abstract: Ethylbenzene is produced by alkylation over a split load of monoclinic silicalite alkylation catalysts having different silica/alumina ratios. A feedstock containing benzene and ethylene is applied to a multi-stage alkylation reaction zone having a plurality of series-connected catalyst beds. At least one catalyst bed contains a first monoclinic silicalite catalyst having a silica/alumina ratio of at least 275. At least one other catalyst bed contains a second monoclinic silicalite catalyst having a silica/alumina ratio of less than about 275. The alkylation reaction zone is operated at temperature and pressure conditions in which the benzene is in a gaseous phase to cause gas-phase alkylation of the aromatic substrate in the presence of the monoclinic silicalite catalysts to produce an alkylation product. The alkylation product is then withdrawn from the reaction zone for separation and recovery. The use of the split load of catalyst allows a higher purity ethylbenzene product to be produced at improved efficiencies than if only one of the catalysts were used by itself.

Abstract translation: 通过在具有不同二氧化硅/氧化铝比的单斜晶硅沸石烷基化催化剂的分裂负载下烷基化来制备乙苯。 将含有苯和乙烯的原料施加到具有多个串联催化剂床的多级烷基化反应区。 至少一个催化剂床含有二氧化硅/氧化铝比至少为275的第一单斜晶硅沸石催化剂。至少一个其它催化剂床含有二氧化硅/氧化铝比小于约275的第二单斜硅沸石催化剂。烷基化反应区 在其中苯处于气相的温度和压力条件下操作，以在单斜硅沸石催化剂的存在下引起芳族底物的气相烷基化以产生烷基化产物。 然后将烷基化产物从反应区取出以进行分离和回收。 与仅使用一种催化剂本身一起使用的催化剂的分离负载的使用允许以提高的效率生产更高纯度的乙苯产物。

公开(公告)号：US20130225888A1

公开(公告)日：2013-08-29

申请号：US13863722

申请日：2013-04-16

Applicant: James R. Butler ,  Xin Xiao ,  James T. Merrill

Inventor： James R. Butler ,  Xin Xiao ,  James T. Merrill

IPC: C07C2/66

CPC classification number: C07C2/66 ,  B01J29/06 ,  B01J29/7057 ,  B01J2219/00006 ,  C07C6/126 ,  C07C7/12 ,  C07C15/073 ,  C07C2529/08 ,  C07C2529/70 ,  Y02P20/52 ,  Y02P20/584 ,  Y02P20/588 ,  C07C15/04

Abstract: Alkylation systems and methods of minimizing alkylation catalyst regeneration are described herein. The alkylation systems generally include a preliminary alkylation system adapted to receive an input stream including an alkyl aromatic hydrocarbon and contact the input stream with a preliminary alkylation catalyst disposed therein to form a first output stream. The preliminary alkylation catalyst generally includes a zeolite catalyst having a SiO2/Al2O3 ratio of less than about 25. The alkylation systems further include a first alkylation system adapted to receive the first output stream and contact the first output stream with a first alkylation catalyst disposed therein and an alkylating agent to form a second output stream.

Abstract translation: 本文描述了使烷基化催化剂再生最小化的烷基化系统和方法。 烷基化系统通常包括适于接收包含烷基芳族烃的输入流并将输入流与设置在其中的预置烷基化催化剂接触以形成第一输出流的初步烷基化系统。 初步烷基化催化剂通常包括SiO 2 / Al 2 O 3比小于约25的沸石催化剂。烷基化系统还包括适于接收第一输出流并将第一输出流与置于其中的第一烷基化催化剂接触的第一烷基化系统 和烷基化剂以形成第二输出流。

公开(公告)号：US08426662B2

公开(公告)日：2013-04-23

申请号：US13344390

申请日：2012-01-05

Applicant: James T. Merrill ,  Marcus Ledoux

Inventor： James T. Merrill ,  Marcus Ledoux

IPC: C07C2/66

CPC classification number: C07C2/66 ,  Y02P20/584 ,  C07C15/02

Abstract: Alkylation systems and methods of minimizing alkylation catalyst regeneration are discussed herein. The alkylation systems generally include a preliminary alkylation system adapted to receive an input stream including an alkyl aromatic hydrocarbon and contact the input stream with a first preliminary alkylation catalyst disposed therein to form a first output stream. The first preliminary alkylation catalyst generally includes a Y zeolite. The systems further include a first alkylation system adapted to receive the first output stream and contact the first output stream with a first alkylation catalyst disposed therein and an alkylating agent to form a second output stream.

Abstract translation: 本文讨论了使烷基化催化剂再生最小化的烷基化系统和方法。 烷基化系统通常包括适于接收包含烷基芳族烃的输入流并将输入流与设置在其中的第一初步烷基化催化剂接触以形成第一输出流的初步烷基化系统。 第一初步烷基化催化剂通常包括Y沸石。 所述系统还包括适于接收第一输出流并将第一输出流与设置在其中的第一烷基化催化剂接触的第一烷基化系统和烷基化剂以形成第二输出流。

公开(公告)号：US07569741B2

公开(公告)日：2009-08-04

申请号：US11412244

申请日：2006-04-26

Applicant: James R. Butler ,  James T. Merrill

Inventor： James R. Butler ,  James T. Merrill

IPC: C07C7/10

CPC classification number: C07C15/46 ,  C07C13/28 ,  C07C15/44 ,  C07C2601/16

Abstract: Methods and systems for petrochemical feedstream purification are described herein. The methods generally include providing a petrochemical feedstock, wherein the petrochemical feedstock includes a concentration of polar impurities, contacting the petrochemical feedstock with a washing agent to remove at least a portion of the polar impurities therefrom, separating the washing agent from the petrochemical feedstock to form a purified feedstock and passing the purified feedstock to a petrochemical process. In one embodiment, the petrochemical feedstock includes benzene and the washing agent includes water.

Abstract translation: 本文描述了石油化学原料流净化的方法和系统。 所述方法通常包括提供石油化学原料，其中石油化学原料包括极性杂质的浓度，使石油化学原料与洗涤剂接触以从其中除去至少一部分极性杂质，从洗涤剂与石油化学原料分离形成 纯化的原料并将纯化的原料送至石化工艺。 在一个实施方案中，石油化学原料包括苯，洗涤剂包括水。

公开(公告)号：US06781024B2

公开(公告)日：2004-08-24

申请号：US10074173

申请日：2002-02-12

Applicant: James R. Butler ,  James T. Merrill ,  Adrian M. Jacobsen

Inventor： James R. Butler ,  James T. Merrill ,  Adrian M. Jacobsen

IPC: C07G5367

CPC classification number: C07C5/333 ,  B01F5/06 ,  B01J8/0292 ,  B01J8/0453 ,  B01J8/065 ,  B01J2208/00061 ,  B01J2208/00212 ,  B01J2208/00548 ,  B01J2208/0084 ,  B01J2208/00849 ,  Y10S585/922 ,  Y10S585/923 ,  Y10S585/924 ,  C07C15/44 ,  C07C15/46

Abstract: Process for the catalytic dehydrogenation of a C2 or C3 alkyl aromatic in which a feedstock containing the alkyl aromatic and steam is supplied into the inlet of a tubular reactor containing a dehydrogenation catalyst. Within the reactor, the feedstock flows through at least a portion of the reactor along a spiral flow path extending longitudinally of the reactor. The resulting vinyl aromatic product is then recovered from a downstream or outlet section of the reactor. The spiral flow path through which the feedstock is passed is located at least adjacent the inlet side of the reactor and at least a portion of the spiral flow path contains a particulate dehydrogenation catalyst. The spiral flow path may extend throughout a major portion of the elongated tubular reactor and may contain a particulate dehydrogenation catalyst in a substantial portion there. The feedstock containing the alkyl aromatic and steam is supplied into a plurality of tubular reactors located within the interior of a dehydrogenation reactor vessel and is arranged in a parallel relationship in which the tubular reactors are spaced laterally from one another and from the interior wall of the reaction vessel.

Abstract translation: 将含有烷基芳族和蒸汽的原料供给到含有脱氢催化剂的管式反应器的入口中的C2或C3烷基芳族化合物的催化脱氢方法。 在反应器内，原料沿着反应器纵向延伸的螺旋流动路径流过反应器的至少一部分。 然后从反应器的下游或出口部分回收得到的乙烯基芳族化合物。 原料通过的螺旋流动路径至少位于反应器的入口侧，螺旋流路的至少一部分含有颗粒脱氢催化剂。 螺旋流动路径可以延伸穿过细长管式反应器的主要部分，并且可以在其中大部分含有颗粒状脱氢催化剂。 将含有烷基芳族化合物和蒸汽的原料供给到位于脱氢反应器容器内部的多个管式反应器中并且以平行关系排列，其中管式反应器彼此横向间隔开， 反应容器

公开(公告)号：US06380449B1

公开(公告)日：2002-04-30

申请号：US09718601

申请日：2000-11-22

Applicant: James R. Butler ,  James T. Merrill ,  Adrian M. Jacobsen

Inventor： James R. Butler ,  James T. Merrill ,  Adrian M. Jacobsen

IPC: C07C5367

CPC classification number: B01J8/065 ,  B01F5/06 ,  B01J8/0292 ,  B01J8/0453 ,  B01J2208/00061 ,  B01J2208/00212 ,  B01J2208/00548 ,  B01J2208/0084 ,  B01J2208/00849 ,  C07C5/333 ,  Y10S585/921 ,  Y10S585/922 ,  Y10S585/923 ,  Y10S585/924 ,  C07C15/46

Abstract: Process for the catalytic dehydrogenation of ethylbenzene in which a feedstock containing ethylbenzene and steam is supplied into the inlet of a tubular reactor containing a dehydrogehation catalyst. Within the reactor, the feedstock flows through at least a portion of the reactor along a spiral flow path extending longitudinally of the reactor. The resulting styrene product is then recovered from a downstream or outlet section of the reactor. The spiral flow path through which the feedstock is passed is located at least adjacent the inlet side of the reactor and at least a portion of the spiral flow path contains a particulate dehydrogenation catalyst. The spiral flow path may extend throughout a major portion of the elongated tubular reactor and may contain a particulate dehydrogenation catalyst in a substantial portion there.

Abstract translation: 乙苯的催化脱氢方法，其中将含有乙苯和蒸汽的原料供入含有脱氢化催化剂的管式反应器的入口。 在反应器内，原料沿着反应器纵向延伸的螺旋流动路径流过反应器的至少一部分。 然后从反应器的下游或出口部分回收得到的苯乙烯产物。 原料通过的螺旋流动路径至少位于反应器的入口侧，螺旋流路的至少一部分包含颗粒脱氢催化剂。 螺旋流动路径可以延伸穿过细长管式反应器的主要部分，并且可以在其中大部分含有颗粒状脱氢催化剂。

公开(公告)号：US5955642A

公开(公告)日：1999-09-21

申请号：US739564

申请日：1996-10-30

Applicant: James T. Merrill ,  James R. Butler

Inventor： James T. Merrill ,  James R. Butler

IPC: B01J29/06 ,  C07B61/00 ,  C07C2/66 ,  C07C5/13 ,  C07C5/27 ,  C07C6/12 ,  C07C9/22 ,  C07C15/02 ,  C07C15/073 ,  C07C1/00 ,  C07C2/64 ,  C07C2/68 ,  C07C5/22

CPC classification number: C07C15/02 ,  C07C2529/40 ,  C07C2529/70

Abstract: An alkylation/transalkylation process involving vapor phase alkylation of a benzene feedstock in a multi-stage alkylation zone having a plurality of series connected catalyst beds containing a pentasil aromatic alkylation catalyst, such as silicalite, coupled with intermediate separation and recirculation steps and liquid phase transalkylation over a transalkylation catalyst comprising a molecular sieve having a pore size greater than the pore size of the silicalite. The benzene containing feedstock is supplied to the multi-stage alkylation reaction zone along with a C.sub.2 -C.sub.4 alkylating agent operated under temperature and pressure conditions to maintain the benzene in the gas phase. Alkylated product is recovered from the alkylation zone and supplied to a benzene recovery zone for the separation of the benzene from the alkylation product. Benzene from the benzene recovery zone is recycled to the reaction zone. A higher boiling bottom fraction containing a mixture of monoalkylated and polyalkylated aromatic components is supplied to a secondary separation zone from which a monoalkylated aromatic component, e.g. ethylbenzene, is recovered overhead with a heavier polyalkylated aromatic recovered as a bottom fraction. The bottom fraction may be applied to a tertiary separation zone.

Abstract translation: 一种烷基化/烷基转移方法，涉及在多级烷基化区中苯原子气相烷基化的方法，该多级烷基化区具有多个串联连接的催化剂床，该催化剂床含有pentasil芳族烷基化催化剂，如硅沸石，加上中间分离和再循环步骤以及液相烷基转移 在包含具有大于硅沸石的孔径的孔径的分子筛的烷基转移催化剂上。 含苯原料与在温度和压力条件下运行的C2-C4烷基化剂一起供应到多级烷基化反应区，以保持苯在气相中。 从烷基化区回收烷基化产物，并将其供应至苯回收区，以将苯与烷基化产物分离。 苯从苯回收区循环到反应区。 将含有单烷基化和多烷基化芳族组分的混合物的较高沸点底部馏分供应到二级分离区，从其分离单烷基化芳族组分，例如， 乙苯，用作为底部馏分回收的较重的多烷基化芳烃塔顶回收。 底部馏分可以施加到第三分离区。