公开(公告)号：US08524895B2

公开(公告)日：2013-09-03

申请号：US12501699

申请日：2009-07-13

Applicant: Tung-Han Tsai ,  Pin-To Yao ,  Cheng-Fa Hsieh

Inventor： Tung-Han Tsai ,  Pin-To Yao ,  Cheng-Fa Hsieh

IPC: C07D201/04 ,  C07D223/10

CPC classification number: C07D201/04 ,  C07D223/10

Abstract: The present invention provides a method for preparing amides, in which an amino acid ionic liquid is used as both a reaction medium and a catalyst to catalyze Beckman rearrangement of a ketoxime, so as to produce an amide. In the method, the rearrangement is conducted by catalyzing a ketoxime with an amino acid ionic liquid having the asymmetric property at a moderate reaction temperature during a short reaction time, so as to produce an amide without adding other catalysts such as concentrate sulfuric acid. The method has advantages such as avoiding corrosion in equipments with pipelines, the high conversion rate of ketoximes and the high selectivity of amides.

Abstract translation: 本发明提供了一种制备酰胺的方法，其中使用氨基酸离子液体作为反应介质和催化贝克曼重排酮肟的催化剂，以产生酰胺。 在该方法中，通过在短的反应时间内在适度的反应温度下用具有不对称性质的氨基酸离子液体催化酮肟进行重排，从而在不加入其它催化剂如浓硫酸的情况下生成酰胺。 该方法具有避免管道设备腐蚀，酮肟转化率高，酰胺选择性高等优点。

公开(公告)号：US08367865B2

公开(公告)日：2013-02-05

申请号：US12627681

申请日：2009-11-30

Applicant: Tung-Han Tsai ,  Cheng-Fa Hsieh ,  Chi-Yuan Chen

Inventor： Tung-Han Tsai ,  Cheng-Fa Hsieh ,  Chi-Yuan Chen

IPC: C07C231/04 ,  B01J31/04

CPC classification number: C07C231/10 ,  B01J31/0201 ,  B01J31/0202 ,  B01J31/0209 ,  B01J31/0217 ,  B01J31/0218 ,  B01J31/0222 ,  B01J31/0238 ,  B01J31/0247 ,  B01J31/0251 ,  B01J31/0279 ,  B01J31/0285 ,  C07B43/06 ,  C07C229/24 ,  C07D201/04 ,  C07D223/10

Abstract: The present invention provides a catalyst composition for preparing an amide, including an amino acid ionic liquid having a cation of formula (I) and an anion selected from the group consisting of an inorganic acid group, an organic acid group and a combination thereof, wherein the numbers of the anion and the cation are such that the amino acid ionic liquid is electroneutral; and a Bronsted acid. The present invention also provides a method for preparing an amide in the presence of the catalyst composition, and the method has advantages such as decreasing viscosity of ionic liquid, and increasing conversion rate of ketoximes and selectivity of amides.

Abstract translation: 本发明提供一种制备酰胺的催化剂组合物，其包括具有式（I）的阳离子的氨基酸离子液体和选自无机酸基，有机酸基及其组合的阴离子，其中 阴离子和阳离子的数量使得氨基酸离子液体是电中性的; 和布朗斯台德酸。 本发明还提供了在催化剂组合物存在下制备酰胺的方法，该方法具有降低离子液体的粘度，提高酮肟的转化率和酰胺选择性的优点。

公开(公告)号：US20120277468A1

公开(公告)日：2012-11-01

申请号：US13345089

申请日：2012-01-06

Applicant: Ya-Ping Chen ,  Cheng-Fa Hsieh ,  Pin-To Yao ,  Chien-Chang Chiang

Inventor： Ya-Ping Chen ,  Cheng-Fa Hsieh ,  Pin-To Yao ,  Chien-Chang Chiang

IPC: B01J21/06 ,  C07C249/04

CPC classification number: C01B37/005 ,  B01J29/89 ,  C01B39/085 ,  C01B39/087 ,  C07C249/04 ,  C07C251/44

Abstract: The present invention provides a titanium-silicalite molecular sieve and a method for preparing the same. The method includes the steps of preparing a mixture of a titanium source, a silicon source, a transition metal source, a template agent and water; heating the mixture to form a gel mixture; heating the gel mixture in a water bath; and calcining the gel mixture after the gel mixture in the water bath to form the titanium-silicalite molecular sieve. The present invention further provides a method for preparing cyclohexanone oxime by using the titanium-silicalite molecular sieve as the catalyst which results in high conversion rate, high selectivity and high usage efficiency of hydrogen peroxide.

Abstract translation: 本发明提供钛 - 硅沸石分子筛及其制备方法。 该方法包括制备钛源，硅源，过渡金属源，模板剂和水的混合物的步骤; 加热混合物以形成凝胶混合物; 在水浴中加热凝胶混合物; 并在凝胶混合物中在水浴中煅烧凝胶混合物以形成钛 - 硅沸石分子筛。 本发明还提供了通过使用钛 - 硅沸石分子筛作为催化剂制备环己酮肟的方法，其导致过氧化氢的高转化率，高选择性和高使用效率。

公开(公告)号：US20120184733A1

公开(公告)日：2012-07-19

申请号：US13332834

申请日：2011-12-21

Applicant: Tung-Han Tsai ,  Cheng-Fa Hsieh ,  Hung-Hung Hseuh ,  Chien-Chuan Shih

Inventor： Tung-Han Tsai ,  Cheng-Fa Hsieh ,  Hung-Hung Hseuh ,  Chien-Chuan Shih

IPC: C07D201/04 ,  B01J31/02

CPC classification number: C07D201/04 ,  B01J31/0237 ,  B01J31/0244 ,  B01J2231/52 ,  C07C231/10 ,  Y02P20/584 ,  C07C233/07 ,  C07C233/05

Abstract: The present invention provides a method for preparing an amide. The method includes the steps of performing in a reactor including a catalyst composition having a nitrogen-containing heterocyclic compound and sulfuric acid Beckman rearrangement of a ketoxime to form a product stream having the amide, wherein a molar ratio of the nitrogen-containing heterocyclic compound to the sulfuric acid is from 1:1 to 1:8; and separating an organic phase having the amide and an aqueous phase having the catalyst composition from the product stream. The present invention facilitates the regeneration of the catalyst composition with low water content, so as to increase the conversion rate of a ketoxime and the selectivity of an amide.

Abstract translation: 本发明提供一种制备酰胺的方法。 该方法包括以下步骤：在包括具有含氮杂环化合物的催化剂组合物和酮肟的硫酸贝克曼重排反应器的反应器中进行，以形成具有酰胺的产物流，其中含氮杂环化合物与 硫酸为1:1至1:8; 并从产物流中分离出具有酰胺的有机相和具有催化剂组成的水相。 本发明有助于低水含量的催化剂组合物的再生，从而提高酮肟的转化率和酰胺的选择性。

公开(公告)号：US20090324480A1

公开(公告)日：2009-12-31

申请号：US12459784

申请日：2009-07-08

Applicant: Shu-Hung Yang ,  Cheng-Fa Hsieh ,  Yi-Bau Hung

Inventor： Shu-Hung Yang ,  Cheng-Fa Hsieh ,  Yi-Bau Hung

IPC: C01B21/14

CPC classification number: C01B21/1418

Abstract: Provided is a method for manufacturing hydroxylamine. In this method, an aqueous reaction medium containing acidic buffer agent and nitrate ions in the presence of a limited amount of metal impurities such as Fe or Cu is introduced into a hydroxylamine synthesis reactor in the presence of catalyst to proceed hydroxylamine synthesis by reduction of nitrate ions with hydrogen gas as reducing agent in the aqueous reaction medium to produce hydroxylamine. The reaction is processed in the aqueous reaction medium with a limited amount of metal impurities or even without metal impurities, such that the selection rate of the hydroxylamine product is increased.

Abstract translation: 提供了制备羟胺的方法。 在该方法中，在有限量的金属杂质如Fe或Cu的存在下，将酸性缓冲剂和硝酸根离子的含水反应介质在催化剂存在下引入羟胺合成反应器中以通过还原硝酸盐进行羟胺合成 离子与氢气作为还原剂在水性反应介质中产生羟胺。 反应在水性反应介质中用有限量的金属杂质或甚至没有金属杂质处理，使得羟胺产物的选择速率增加。

公开(公告)号：US08865892B2

公开(公告)日：2014-10-21

申请号：US13332834

申请日：2011-12-21

Applicant: Tung-Han Tsai ,  Cheng-Fa Hsieh ,  Hung-Hung Hseuh ,  Chien-Chuan Shih

Inventor： Tung-Han Tsai ,  Cheng-Fa Hsieh ,  Hung-Hung Hseuh ,  Chien-Chuan Shih

IPC: C07D201/04 ,  B01J31/02 ,  C07C231/10

CPC classification number: C07D201/04 ,  B01J31/0237 ,  B01J31/0244 ,  B01J2231/52 ,  C07C231/10 ,  Y02P20/584 ,  C07C233/07 ,  C07C233/05

Abstract: The present invention provides a method for preparing an amide. The method includes the steps of performing in a reactor including a catalyst composition having a nitrogen-containing heterocyclic compound and sulfuric acid Beckman rearrangement of a ketoxime to form a product stream having the amide, wherein a molar ratio of the nitrogen-containing heterocyclic compound to the sulfuric acid is from 1:1 to 1:8; and separating an organic phase having the amide and an aqueous phase having the catalyst composition from the product stream. The present invention facilitates the regeneration of the catalyst composition with low water content, so as to increase the conversion rate of a ketoxime and the selectivity of an amide.

Abstract translation: 本发明提供一种制备酰胺的方法。 该方法包括以下步骤：在包括具有含氮杂环化合物的催化剂组合物和酮肟的硫酸贝克曼重排反应器的反应器中进行，以形成具有酰胺的产物流，其中含氮杂环化合物与 硫酸为1:1至1:8; 并从产物流中分离出具有酰胺的有机相和具有催化剂组成的水相。 本发明有助于低水含量的催化剂组合物的再生，从而提高酮肟的转化率和酰胺的选择性。

公开(公告)号：US08540956B2

公开(公告)日：2013-09-24

申请号：US12748932

申请日：2010-03-29

Applicant: Pin-To Yao ,  Cheng-Fa Hsieh ,  Shih-Yao Chao ,  Yang-Min Liang

Inventor： Pin-To Yao ,  Cheng-Fa Hsieh ,  Shih-Yao Chao ,  Yang-Min Liang

IPC: C01B39/02 ,  C01B39/04

CPC classification number: C01B39/023 ,  B01J29/405 ,  C01B37/005 ,  C01B39/04

Abstract: The present invention provides a method for preparing large particles of titanium-silicalite molecular sieves. The method of the present invention includes the steps of preparing a dispersion solution of a primary crystalline molecular sieve; forming an aggregated particle solution by adding a flocculating agent and a coagulating agent into the dispersion solution; mixing the aggregated particle solution with a synthesis gel to form a mixture; and heat-treating the mixture. The average diameter of the titanium-silicalite molecular sieves in the present invention is more than 5 μm. In the preparation of cyclohexanone oxime using the molecular sieve of the present invention as the catalyst, the selectivity and conversion rate of cyclohexanone oxime are high, the usage of hydrogen peroxide is enhanced, and the catalyst is easy to be recovered.

Abstract translation: 本发明提供一种制备钛 - 硅沸石分子筛大颗粒的​​方法。 本发明的方法包括制备一级结晶分子筛的分散液的步骤; 通过向分散液中添加絮凝剂和凝结剂形成凝集颗粒溶液; 将聚集的颗粒溶液与合成凝胶混合以形成混合物; 并对该混合物进行热处理。 本发明中钛 - 硅沸石分子筛的平均直径大于5μm。 在使用本发明的分子筛作为催化剂的环己酮肟的制备中，环己酮肟的选择性和转化率高，过氧化氢的用途增加，催化剂容易回收。

公开(公告)号：US20100063274A1

公开(公告)日：2010-03-11

申请号：US12501699

申请日：2009-07-13

Applicant: Tung-Han Tsai ,  Pin-To Yao ,  Cheng-Fa Hsieh

Inventor： Tung-Han Tsai ,  Pin-To Yao ,  Cheng-Fa Hsieh

IPC: C07D201/04 ,  C07D223/10

CPC classification number: C07D201/04 ,  C07D223/10

Abstract: The present invention provides a method for preparing amides, in which an amino acid ionic liquid is used as both a reaction medium and a catalyst to catalyze Beckman rearrangement of a ketoxime, so as to produce an amide. In the method, the rearrangement is conducted by catalyzing a ketoxime with an amino acid ionic liquid having the asymmetric property at a moderate reaction temperature during a short reaction time, so as to produce an amide without adding other catalysts such as concentrate sulfuric acid. The method has advantages such as avoiding corrosion in equipments with pipelines, the high conversion rate of ketoximes and the high selectivity of amides.

Abstract translation: 本发明提供了一种制备酰胺的方法，其中使用氨基酸离子液体作为反应介质和催化贝克曼重排酮肟的催化剂，以产生酰胺。 在该方法中，通过在短的反应时间内在适度的反应温度下用具有不对称性质的氨基酸离子液体催化酮肟进行重排，从而在不加入其它催化剂如浓硫酸的情况下生成酰胺。 该方法具有避免管道设备腐蚀，酮肟转化率高，酰胺选择性高等优点。

公开(公告)号：US07622420B1

公开(公告)日：2009-11-24

申请号：US12454962

申请日：2009-05-27

Applicant: Pin-To Yao ,  Chun-Kao Wang ,  Cheng-Fa Hsieh

Inventor： Pin-To Yao ,  Chun-Kao Wang ,  Cheng-Fa Hsieh

IPC: B01J23/00 ,  B01J23/38 ,  B01J23/40 ,  B01J23/42 ,  B01J23/44 ,  B01J23/54 ,  B01J23/56 ,  B01J23/60 ,  B01J23/62 ,  B01J23/64 ,  B01J23/644

CPC classification number: B01J23/624 ,  B01J23/62 ,  B01J23/66 ,  B01J27/1856 ,  C01B21/1418

Abstract: This invention provides a catalyst composition for preparing hydroxylamine, which comprises palladium, a platinum compound, a germanium compound and a carrier, wherein a halogen concentration of the composition is no more than 10 ppm. The catalyst composition is prevented from poisoning by halogens, and therefore the catalyst composition has high selectivity and catalytic activity. Further, the weight ratio of palladium and platinum in the catalyst composition ranges from 100:1 to 1000:1, such that the catalyst composition can be used to solve the commonly observed problem, i.e., decreased selectivity due to the excessive amount of platinum.

Abstract translation: 本发明提供一种用于制备羟胺的催化剂组合物，其包含钯，铂化合物，锗化合物和载体，其中组合物的卤素浓度不超过10ppm。 催化剂组合物不会被卤素中毒，因此催化剂组合物具有高选择性和催化活性。 此外，催化剂组合物中钯和铂的重量比为100:1-1000:1，使得催化剂组合物可用于解决普遍观察到的问题，即由于铂的过量引起的选择性降低。

公开(公告)号：US20070265471A1

公开(公告)日：2007-11-15

申请号：US11712690

申请日：2007-02-28

Applicant: Pin-To Yao ,  Cheng-Fa Hsieh ,  Ren-Hao Hsu

Inventor： Pin-To Yao ,  Cheng-Fa Hsieh ,  Ren-Hao Hsu

IPC: C07C239/08

CPC classification number: C01B21/1418

Abstract: A method for preparing hydroxylamine, comprising the steps of: (i) pretreating the acidic buffer solution with the compounds having a functional group represented by formula (I), thereby removing metal impurities from the acidic buffer solution; and (ii) reducing nitrate ions in the acidic buffer solution with hydrogen to give hydroxylamine in the presence of catalysts, According to the present invention the selectivity for reducing nitrate ions to give hydroxylamine can be significantly enhanced.

Abstract translation: 一种制备羟胺的方法，包括以下步骤：（i）用具有由式（I）表示的官能团的化合物预处理酸性缓冲溶液，从而从酸性缓冲溶液中除去金属杂质; 和（ii）用氢还原酸性缓冲溶液中的硝酸根离子，在催化剂存在下得到羟胺。根据本发明，可显着提高还原硝酸根离子以产生羟胺的选择性。