公开(公告)号：US07238803B2

公开(公告)日：2007-07-03

申请号：US10883822

申请日：2004-07-06

申请人： Masashi Yokota ,  Yoshinori Kobayashi ,  Masaru Kitamura

发明人： Masashi Yokota ,  Yoshinori Kobayashi ,  Masaru Kitamura

IPC分类号： C07D201/04

CPC分类号： C07D201/04 ,  Y02P20/52

摘要： ε-Caprolactam is produced by the method comprising the step of introducing a gas comprising cyclohexanone oxime into a layer of solid catalyst particles through a plurality of holes of a gas diffusion plate so that the solid catalyst particles are brought into contact with the gas, while fluidizing the catalyst layer, wherein the holes have an average diameter of about 3 mm or smaller. In accordance with the production method, ε-caprolactam can be produced from a raw material gas comprising cyclohexanone oxime with a high conversion of cyclohexanone oxime and a high selectivity to ε-caprolactam.

摘要翻译： ε-己内酰胺通过包括以下步骤的方法制备：包括环己酮肟的气体通过气体扩散板的多个孔引入固体催化剂颗粒层中，使得固体催化剂颗粒与气体接触，同时 使催化剂层流化，其中孔的平均直径为约3mm或更小。 根据制造方法，ε-己内酰胺可以由包含环己酮肟的高转化率和对ε-己内酰胺的高选择性的环己酮肟的原料气体制备。

公开(公告)号：US07060645B2

公开(公告)日：2006-06-13

申请号：US11165538

申请日：2005-06-24

申请人： Masahiro Hoshino ,  Masaru Kitamura ,  Keisuke Sugita

发明人： Masahiro Hoshino ,  Masaru Kitamura ,  Keisuke Sugita

IPC分类号： B01J29/40 ,  C07D201/04

CPC分类号： C07D201/04 ,  B01J29/035 ,  B01J37/06 ,  B01J2229/38 ,  B01J2229/40 ,  C01B37/02

摘要： The present invention provides a method for manufacturing a zeolite comprising following steps of: (1): calcining crystals obtained by hydrothermal synthesis reaction of a silicon compound; (2): contact treating a calcined product obtained by the step (1) with an aqueous solution including an amine and/or a quaternary ammonium compound; (3): calcining a treated product obtained by the step (2); and (4): contact treating the calcined product obtained by the step (3) with an aqueous solution including ammonia and/or an ammonium salt. According to the present invention, a method is also provided wherein ε-caprolactam is manufactured by Beckmann rearrangement reaction of cyclohexanone oxime in a gaseous phase in the presence of the zeolite manufactured by the above-described method.

摘要翻译： 本发明提供一种制造沸石的方法，包括以下步骤：（1）：煅烧通过硅化合物的水热合成反应获得的晶体; （2）：用包含胺和/或季铵化合物的水溶液接触步骤（1）得到的煅烧产物; （3）：煅烧通过工序（2）得到的处理物; 和（4）：用包含氨和/或铵盐的水溶液接触处理由步骤（3）获得的煅烧产物。 根据本发明，还提供了一种方法，其中ε-己内酰胺通过在通过上述方法制造的沸石存在下，在气相中通过环己酮肟的贝克曼重排反应制造。

公开(公告)号：US07026474B2

公开(公告)日：2006-04-11

申请号：US11055101

申请日：2005-02-11

申请人： Keisuke Sugita ,  Masaru Kitamura ,  Masahiro Hoshino

发明人： Keisuke Sugita ,  Masaru Kitamura ,  Masahiro Hoshino

IPC分类号： C07D201/04

CPC分类号： B01J38/08 ,  B01J29/90 ,  B01J38/12 ,  B01J38/66 ,  C07D201/04 ,  Y02P20/52 ,  Y02P20/584

摘要： A method for producing ε-caprolactam and a method for reactivating a zeolite catalyst for the production are provided. In the reactivation step, a zeolite catalyst is allowed to contact a gas containing a carboxylic acid, water and a compound selected from ammonia and amines. In accordance with the present invention, the catalytic activities of a zeolite catalyst used for the Beckmann rearrangement reaction of cyclohexanone oxime can be effectively restored. Consequently, ε-caprolactam may be produced with a high production yield for a long period of time by reusing the catalyst by the method described above.

摘要翻译： 提供了制备ε-己内酰胺的方法和用于再生催化剂的方法。 在再活化步骤中，使沸石催化剂与含有羧酸，水和选自氨和胺的化合物的气体接触。 根据本发明，可以有效地恢复用于环己酮肟的贝克曼重排反应的沸石催化剂的催化活性。 因此，通过上述方法重新使用催化剂，可以长期生产ε-己内酰胺。

公开(公告)号：US5315039A

公开(公告)日：1994-05-24

申请号：US981472

申请日：1992-11-25

申请人： Hiroshi Kajikuri ,  Masaru Kitamura ,  Yasuhiko Higashio

发明人： Hiroshi Kajikuri ,  Masaru Kitamura ,  Yasuhiko Higashio

IPC分类号： C07C249/14 ,  C07C251/44 ,  C07C209/82

CPC分类号： C07C249/14

摘要： Thermal decomposition of cycloalkanone oximes is inhibited by allowing nitrogen-containing compounds represented by the following formula (1) to coexist with the cycloalkanone oximes:NR.sub.1 R.sub.2 R.sub.3 (1)(wherein R.sub.1, R.sub.2 and R.sub.3 each represents a hydrogen atom or a lower alkyl group).

摘要翻译： 通过使由下式（1）表示的含氮化合物与环烷酮肟共存：NR1R2R3（1）（其中R1，R2和R3各自表示氢原子或低级烷基），可以抑制环烷酮肟的热分解， 。

公开(公告)号：US4717770A

公开(公告)日：1988-01-05

申请号：US19921

申请日：1987-02-27

申请人： Hiroshi Sato ,  Kenichi Hirose ,  Masaru Kitamura ,  Hideto Tojima ,  Norio Ishii

发明人： Hiroshi Sato ,  Kenichi Hirose ,  Masaru Kitamura ,  Hideto Tojima ,  Norio Ishii

IPC分类号： C07B61/00 ,  B01J25/00 ,  B01J29/06 ,  B01J31/00 ,  B01J31/12 ,  C07D201/04

CPC分类号： C07D201/04 ,  Y02P20/52

摘要： .epsilon.-caprolactam is prepared by gas phase catalytic synthesis where cyclohexanone oxime is brought into contact with a crystalline zeolite, for example, aluminosilicate zeolite or metallosilicate zeolite having a constraint index of 1-12 which has been surface treated with an organometallic compound represented by the general formula: R.sub.4-n MX.sub.n wherein R which may be identical or different represent an alkyl group of 1-6 carbon atoms or phenyl group, M represnets Si or Ge, X represents Cl or an alkoxy group of 1-6 carbon atoms and n represents 1 or 2.

摘要翻译： ε-己内酰胺通过气相催化合成法制备，其中环己酮肟与结晶沸石接触，例如具有1-12的约束指数的铝硅酸盐沸石或金属硅酸盐沸石，其已经用由下式表示的有机金属化合物 通式R4-nMXn其中R可相同或不同，表示1-6个碳原子的烷基或苯基，M表示Si或Ge，X表示C1或1-6个碳原子的烷氧基，n表示 1或2。

公开(公告)号：US07071360B2

公开(公告)日：2006-07-04

申请号：US10105321

申请日：2002-03-26

申请人： Yasumoto Shimazu ,  Kanji Kuwahara ,  Masaru Kitamura

发明人： Yasumoto Shimazu ,  Kanji Kuwahara ,  Masaru Kitamura

IPC分类号： C07C249/00

CPC分类号： B01D1/065 ,  C07C249/14 ,  C07C2601/14 ,  C07C251/44

摘要： A method is provided for evaporating cyclohexanone oxime in which cyclohexanone oxime is evaporated using a falling-film evaporator with wetting the evaporation surface of the evaporator well with the cyclohexanone oxime at a pressure of less than about 1060 Torr with a falling rate of the cyclohexanone oxime of about 170 kg/hour or more per one meter around the circumference of evaporation surface at the lowest part of the evaporator. In this method, the cyclohexanone oxime is evaporated efficiently with little decomposition thereof, while preventing the plugging of the pipes of the evaporator and continuously carrying out the operation of the evaporator for a long period of time.

公开(公告)号：US20060004194A1

公开(公告)日：2006-01-05

申请号：US11165538

申请日：2005-06-24

申请人： Masahiro Hoshino ,  Masaru Kitamura ,  Keisuke Sugita

发明人： Masahiro Hoshino ,  Masaru Kitamura ,  Keisuke Sugita

IPC分类号： B01J29/40 ,  C07D201/04

CPC分类号： C07D201/04 ,  B01J29/035 ,  B01J37/06 ,  B01J2229/38 ,  B01J2229/40 ,  C01B37/02

摘要： The present invention provides a method for manufacturing a zeolite comprising following steps of: (1): calcining crystals obtained by hydrothermal synthesis reaction of a silicon compound; (2): contact treating a calcined product obtained by the step (1) with an aqueous solution including an amine and/or a quaternary ammonium compound; (3): calcining a treated product obtained by the step (2); and (4): contact treating the calcined product obtained by the step (3) with an aqueous solution including ammonia and/or an ammonium salt. According to the present invention, a method is also provided wherein ε-caprolactam is manufactured by Beckmann rearrangement reaction of cyclohexanone oxime in a gaseous phase in the presence of the zeolite manufactured by the above-described method.

摘要翻译： 本发明提供一种制造沸石的方法，包括以下步骤：（1）：煅烧通过硅化合物的水热合成反应获得的晶体; （2）：用包含胺和/或季铵化合物的水溶液接触步骤（1）得到的煅烧产物; （3）：煅烧通过工序（2）得到的处理物; 和（4）：用包含氨和/或铵盐的水溶液接触处理由步骤（3）获得的煅烧产物。 根据本发明，还提供了一种方法，其中ε-己内酰胺通过在通过上述方法制造的沸石存在下，在气相中通过环己酮肟的贝克曼重排反应制造。

公开(公告)号：US06265574B1

公开(公告)日：2001-07-24

申请号：US09500997

申请日：2000-02-09

申请人： Masaru Kitamura ,  Yasumoto Shimazu ,  Makoto Yako

发明人： Masaru Kitamura ,  Yasumoto Shimazu ,  Makoto Yako

IPC分类号： C07D20104

CPC分类号： B01J38/12 ,  B01J29/90 ,  C07D201/04 ,  Y02P20/52 ,  Y02P20/584 ,  Y02P20/588

摘要： A process for producing &egr;-caprolactam is provided which comprises the steps of subjecting cyclohexanone oxime to a gaseous phase Beckmann rearrangement reaction in a fluidized bed system using a solid catalyst and re-generating the catalyst, wherein said process comprises a step of treating the catalyst with an oxygen-containing gas at an elevated temperature in a re-generation step so that the nitrogen content of the catalyst falls within a range of 10 ppm to 2,500 ppm on its way to the reaction step from the re-generating step. According to the present invention, &egr;-caprolactam is produced with a high conversion or a high selectivity without interrupting the rearrangement reaction or the re-generation step.

摘要翻译： 提供了一种生产ε-己内酰胺的方法，其包括以下步骤：使用固体催化剂在流化床系统中使环己酮肟进行气相贝克曼重排反应并重新产生催化剂，其中所述方法包括处理催化剂的步骤 在再生步骤中在升高的温度下含有氧的气体，使得在从再生步骤到反应步骤的途中，催化剂的氮含量在10ppm至2,500ppm的范围内。 根据本发明，在不中断重排反应或重生步骤的情况下，以高转化率或高选择性生产ε-己内酰胺。

公开(公告)号：US5407881A

公开(公告)日：1995-04-18

申请号：US81101

申请日：1993-06-25

申请人： Masaru Kitamura ,  Shuzo Murata ,  Kazuya Tsuchimoto

发明人： Masaru Kitamura ,  Shuzo Murata ,  Kazuya Tsuchimoto

IPC分类号： B01J29/40 ,  B01J37/06 ,  B01J29/28 ,  B01J37/10

CPC分类号： B01J29/40 ,  B01J37/06 ,  B01J2229/26 ,  B01J2229/42

摘要： A process is disclosed wherein a zeolite molding having a high mechanical strength is produced by contacting a pentasil type zeolite molding with water.

摘要翻译： 公开了一种方法，其中具有高机械强度的沸石模制品是通过使pentasil型沸石模制件与水接触而产生的。

公开(公告)号：US5354859A

公开(公告)日：1994-10-11

申请号：US981476

申请日：1992-11-25

申请人： Hiroshi Ichihashi ,  Masaru Kitamura ,  Hiroshi Kajikuri ,  Eiji Tasaka

发明人： Hiroshi Ichihashi ,  Masaru Kitamura ,  Hiroshi Kajikuri ,  Eiji Tasaka

IPC分类号： B01J29/06 ,  C07D201/04

CPC分类号： B01J29/06 ,  C07D201/04 ,  Y02P20/52

摘要： .epsilon.-Caprolactam is prepared by bringing cyclohexanone oxime into contact in gas phase with solid catalysts such as a zeolite catalyst in the presence of at least one nitrogen-containing compound selected from the group consisting of ammonia, methylamines and .epsilon.-caprolactam.

摘要翻译： 在选自氨，甲胺和ε-己内酰胺的至少一种含氮化合物的存在下，使环己酮肟与气相与固体催化剂如沸石催化剂接触来制备ε-己内酰胺。