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1. 发明授权

US09714205B2 Process for direct synthesis of (meth)acrolein from ethers and/or acetals 有权
公开(公告)号：US09714205B2
公开(公告)日：2017-07-25
申请号：US15300444
申请日：2015-03-26
申请人： Arkema France
发明人： Jean-Luc Dubois
IPC分类号： C07C45/38 , C07C45/37 , B01J23/00 , B01J23/04 , B01J23/881 , B01J35/02 , B01J35/10
CPC分类号： C07C45/38 , B01J23/002 , B01J23/04 , B01J23/881 , B01J23/8872 , B01J35/0006 , B01J35/023 , B01J35/08 , B01J35/1019 , B01J35/1042 , B01J35/1061 , B01J37/0203 , B01J37/0223 , B01J37/04 , B01J2523/00 , C07C45/37 , C07C47/22 , B01J2523/15 , B01J2523/41 , B01J2523/48 , B01J2523/68 , B01J2523/842
摘要： The subject matter of the present invention is a process for direct synthesis of (meth)acrolein from a reactive mixture comprising at least one compound chosen from ethers, acetals or hemiacetals derived from linear alcohols comprising from 1 to 3 carbon atoms. Examples of compounds are dimethyl ether, diethyl ether, methyl ethyl ether, dimethoxymethane, diethoxymethane, dipropoxymethane, 1,1-dimethoxyethane or 1,1-diethoxyethane. The process of the invention comprises two successive phases: oxidation then aldol condensation, which can be carried out in the presence of a solid oxidation catalyst chosen from molybdenum-based catalysts and optionally of an aldol condensation catalyst. These two phases are carried out in a reaction system comprising a single reactor or optionally two reactors in cascade.

2. 发明申请

US20160185698A1 Methods for Preparing Methacrolein from t-Butanol 有权
标题翻译：从叔丁醇制备甲基丙烯醛的方法
公开(公告)号：US20160185698A1
公开(公告)日：2016-06-30
申请号：US14959576
申请日：2015-12-04
申请人： Shanghai HuaYi Acrylic Acid Co., Ltd. , Shanghai HuaYi New Material Co., Ltd.
发明人： Xiaoqi Zhao , Ge Luo , Yong Chen , Chunhua Qin , Tonghao Wu , Yan Zhuang , Jianxue Ma , Xiaodong Chu , Jinhua Ji
IPC分类号： C07C45/37 , B01J23/888
CPC分类号： C07C45/37 , B01J23/002 , B01J23/8885 , B01J35/023 , B01J35/026 , B01J37/0009 , B01J37/038 , B01J2523/00 , B01J2523/15 , B01J2523/54 , B01J2523/68 , B01J2523/69 , B01J2523/842 , B01J2523/845 , B01J2523/847 , B01J2523/41 , B01J2523/48 , C07C47/22
摘要： A method for preparing methacrolein from t-butanol, specifically a method for preparing methacrolein by using t-butanol as a starting material, is disclosed, comprising passing the starting material through a fixed bed reactor filled with catalyst, wherein the fixed bed reactor is divided to n reaction zones from the inlet of the starting material to the outlet of the starting material and each zone is filled with catalysts of different catalytic activities; wherein the catalytic activity of the catalyst in the first reaction zone is higher than the catalytic activity of the catalyst in the second reaction zone, and the catalytic activity of the catalyst is gradually increased from the second reaction zone to the last reaction zone; and n is an integer between 3 to 10.
摘要翻译：公开了一种由叔丁醇制备甲基丙烯醛的方法，特别是以叔丁醇为起始原料制备甲基丙烯醛的方法，包括使原料通过填充有催化剂的固定床反应器，其中固定床反应器被分开从原料入口到原料出口的n个反应区，并且每个区填充有不同催化活性的催化剂; 其中所述催化剂在所述第一反应区中的催化活性高于所述第二反应区中所述催化剂的催化活性，并且所述催化剂的催化活性从所述第二反应区逐渐增加到所述最后反应区; n为3〜10的整数。

3. 发明授权

US08178720B2 Method for producing unsaturated aldehyde and unsaturated carboxylic acid 有权
标题翻译：不饱和醛和不饱和羧酸的制备方法
公开(公告)号：US08178720B2
公开(公告)日：2012-05-15
申请号：US12281694
申请日：2007-03-06
申请人： Masahide Kondo , Seiichi Kawato , Toru Kuroda
发明人： Masahide Kondo , Seiichi Kawato , Toru Kuroda
IPC分类号： C07C51/00 , C07C51/16
CPC分类号： C07C51/252 , B01J23/002 , B01J37/0009 , B01J37/0045 , B01J2523/00 , C07C45/35 , C07C45/37 , C07C51/235 , C07C47/22 , C07C57/04 , B01J2523/15 , B01J2523/27 , B01J2523/53 , B01J2523/54 , B01J2523/68 , B01J2523/842 , B01J2523/845
摘要： Disclosed is a method of a gas-phase catalytic oxidation reaction of propylene, isobutylene, or tertiary butanol with molecular oxygen in the presence of a catalyst to produce a corresponding unsaturated aldehyde and a corresponding unsaturated carboxylic acid, in which the catalyst can be used over a long period of time. Concretely, in the presence of the catalyst containing a complex oxide including molybdenum, bismuth and iron as essential components, at least one factor of a reaction pressure and a molar ratio of molecular oxygen to a raw material is controlled to change in such a way that a rate of reaction of the raw material is kept constant in the temperature range of from (TA−15)° C. to TA° C., when a boundary temperature of the activation energy of the catalyst is set to be TA° C.
摘要翻译：公开了在催化剂存在下丙烯，异丁烯或叔丁醇与分子氧的气相催化氧化反应的方法，以产生相应的不饱和醛和相应的不饱和羧酸，其中可以使用催化剂很长一段时间。具体地说，在含有包含钼，铋和铁作为必要成分的复合氧化物的催化剂的存在下，控制至少一个反应压力因子和分子氧与原料的摩尔比，以使其变化，使得当催化剂的活化能的边界温度设定为TA℃时，原料的反应速率在（TA-15）℃至TA℃的温度范围内保持恒定。

4. 发明申请

US20100069659A1 PROCESS FOR PRODUCING GEOMETRIC SHAPED CATALYST BODIES 有权
标题翻译：生产几何形状催化剂体的方法
公开(公告)号：US20100069659A1
公开(公告)日：2010-03-18
申请号：US12546883
申请日：2009-08-25
申请人： Andreas RAICHLE , Catharina Horstmann , Frank Rosowski , Klaus Joachim Muller-Engel , Holger Borchert , Gerhard Cox , Ulrich Cremer
发明人： Andreas RAICHLE , Catharina Horstmann , Frank Rosowski , Klaus Joachim Muller-Engel , Holger Borchert , Gerhard Cox , Ulrich Cremer
IPC分类号： C07C253/18 , B01J21/06 , C07C45/35
CPC分类号： C07C45/28 , B01J23/002 , B01J23/8885 , B01J35/0006 , B01J35/023 , B01J37/0036 , B01J37/0221 , B01J37/04 , B01J2523/00 , C07C45/35 , C07C45/37 , C07C51/252 , C07C253/26 , Y02P20/52 , C07C47/22 , C07C57/04 , B01J2523/13 , B01J2523/41 , B01J2523/54 , B01J2523/68 , B01J2523/69 , B01J2523/842 , B01J2523/845 , C07C255/08
摘要： A process for producing geometric shaped catalyst bodies K whose active material is a multielement oxide of stoichiometry [Bi1WbOx]a[Mo12Z1cZ2dFeeZ3fZ4gZ5nOy]1, in which a finely divided oxide Bi1WbOx with the particle size d50A1 and, formed from element sources, a finely divided intimate mixture of stoichiometry Mo12Z1cZ2dFeeZ3fZ4gZ5h with the particle size d50A2 are mixed in a ratio of a:1, this mixture is used to form shaped bodies and these are treated thermally, where (d50A1)0.7•(d90A1)1.5•(a)−1≧820.
摘要翻译：一种用于生产几何形状的催化剂体K的方法，其活性材料是化学计量[Bi1WbOx] a [Mo12Z1cZ2dFeeZ3fZ4gZ5nOy] 1的多元素氧化物，其中具有粒度d50A1的细分离氧化物Bi1WbOx，并且由元素源形成，化学计量比的混合物Mo12Z1cZ2dFeeZ3fZ4gZ5h以a：1的比例混合，该混合物用于形成成型体，热处理，其中（d50A1）0.7•（d90A1）1.5•（a）-1≧ 820。

5. 发明申请

US20090221847A1 METHOD FOR PRODUCING UNSATURATED ALDEHYDE AND UNSATURATED CARBOXYLIC ACID 有权
标题翻译：生产不饱和醛和不饱和羧酸的方法
公开(公告)号：US20090221847A1
公开(公告)日：2009-09-03
申请号：US12281694
申请日：2007-03-06
申请人： Masahide Kondo , Seiichi Kawato , Toru Kuroda
发明人： Masahide Kondo , Seiichi Kawato , Toru Kuroda
IPC分类号： C07C61/16 , C07C47/20
CPC分类号： C07C51/252 , B01J23/002 , B01J37/0009 , B01J37/0045 , B01J2523/00 , C07C45/35 , C07C45/37 , C07C51/235 , C07C47/22 , C07C57/04 , B01J2523/15 , B01J2523/27 , B01J2523/53 , B01J2523/54 , B01J2523/68 , B01J2523/842 , B01J2523/845
摘要： Disclosed is a method of a gas-phase catalytic oxidation reaction of propylene, isobutylene, or tertiary butanol with molecular oxygen in the presence of a catalyst to produce a corresponding unsaturated aldehyde and a corresponding unsaturated carboxylic acid, in which the catalyst can be used over a long period of time. Concretely, in the presence of the catalyst containing a complex oxide including molybdenum, bismuth and iron as essential components, at least one factor of a reaction pressure and a molar ratio of molecular oxygen to a raw material is controlled to change in such a way that a rate of reaction of the raw material is kept constant in the temperature range of from (TA-15)° C. to TA° C., when a boundary temperature of the activation energy of the catalyst is set to be TA° C.
摘要翻译：公开了在催化剂存在下丙烯，异丁烯或叔丁醇与分子氧的气相催化氧化反应的方法，以产生相应的不饱和醛和相应的不饱和羧酸，其中可以使用催化剂很长一段时间。具体地说，在含有包含钼，铋和铁作为必要成分的复合氧化物的催化剂的存在下，控制至少一个反应压力因子和分子氧与原料的摩尔比，以使其变化，使得当催化剂的活化能的边界温度设定为TA℃时，原料的反应速率在（TA-15）℃至TA℃的温度范围内保持恒定。

6. 发明授权

US07579501B2 Composite oxide catalyst and method of producing the same 有权
标题翻译：复合氧化物催化剂及其制备方法
公开(公告)号：US07579501B2
公开(公告)日：2009-08-25
申请号：US11987877
申请日：2007-12-05
申请人： Isao Teshigahara , Nariyasu Kanuka , Tomoatsu Iwakura
发明人： Isao Teshigahara , Nariyasu Kanuka , Tomoatsu Iwakura
IPC分类号： C07C51/16 , C07C45/00
CPC分类号： C07C45/35 , B01J21/08 , B01J23/002 , B01J23/31 , B01J23/8876 , B01J35/1009 , B01J35/1014 , B01J35/1038 , B01J35/1042 , B01J35/108 , B01J37/0009 , B01J37/03 , B01J2523/00 , C07C45/34 , C07C45/37 , C07C51/252 , C07C47/22 , C07C57/04 , B01J2523/12 , B01J2523/13 , B01J2523/305 , B01J2523/3737 , B01J2523/41 , B01J2523/54 , B01J2523/68 , B01J2523/842 , B01J2523/845 , B01J2523/847 , B01J2523/22 , B01J2523/23 , B01J2523/27 , B01J2523/3712 , B01J2523/30 , B01J2523/37
摘要： A composite oxide catalyst for the oxidation of an olefin containing Mo and Bi as essential components, characterized in that it has a specific surface area of 5 to 25 m2/g and a pore volume of 0.2 to 0.7 cc/g, and has a pore diameter distribution wherein the volume of the pores having a pore diameter of 0.03 to 0.1 μm accounts for 30% or more of the total pore volume, the volume of the pores having a pore diameter of 0.1 to 1 μm accounts for 20% or more of the total pore volume, and the volume of the pores having a pore diameter of less than 0.03 μm is 10% or less of the total pore volume; a composite oxide catalyst for use in the vapor phase catalytic oxidation of acrolein or methacrolein or the like which comprises Mo, Bi and a halogen; either of the above two composite oxide catalysts which comprises Mo, Bi, Fe, Si and an element selected from alkali metals and thallium, and optionally Co, Ni, Mg, Ca, Zn, Ce, Sm, a halogen, B, P, As and W; a method for preparing any of the above composite catalysts; and a method for using any of the above composite oxide catalysts.
摘要翻译：一种用于氧化含有Mo和Bi的烯烃作为必要组分的复合氧化物催化剂，其特征在于其具有5至25m 2 / g的比表面积和0.2至0.7cc / g的孔体积，并且具有孔直径分布，其中孔径为0.03至0.1μm的孔的体积占总孔体积的30％或更多，孔径为0.1至1μm的孔的体积占20％或更多的孔径总细孔容积和孔径小于0.03μm的孔的体积为总孔体积的10％以下; 用于丙烯醛或甲基丙烯醛等的气相催化氧化的复合氧化物催化剂，其包含Mo，Bi和卤素; 上述两种复合氧化物催化剂，其包含Mo，Bi，Fe，Si和选自碱金属和铊的元素，以及任选的Co，Ni，Mg，Ca，Zn，Ce，Sm，卤素，B，P， As和W; 制备任何上述复合催化剂的方法; 以及使用上述复合氧化物催化剂的方法。

7. 发明申请

US20090062564A1 Method for Producing Methacrolein and/or Methacrylic Acid 有权
标题翻译：生产甲基丙烯醛和/或甲基丙烯酸的方法
公开(公告)号：US20090062564A1
公开(公告)日：2009-03-05
申请号：US12223494
申请日：2007-03-30
申请人： Tatsuhiko Kurakami , Toshitake Kojima , Yoshimasa Seo
发明人： Tatsuhiko Kurakami , Toshitake Kojima , Yoshimasa Seo
IPC分类号： C07C51/16 , C07C45/29
CPC分类号： C07C45/37 , B01J21/04 , B01J21/12 , B01J23/002 , B01J23/8876 , B01J23/8878 , B01J23/8885 , B01J35/0006 , B01J2523/00 , C07C51/23 , C07C51/252 , C07C47/22 , C07C57/04 , B01J2523/15 , B01J2523/54 , B01J2523/68 , B01J2523/842 , B01J2523/845
摘要： The present invention relates to a method for producing methacrolein and/or methacrylic acid characterized in that the catalyst filling length of a dehydration catalyst layer is 3 to 20% of the catalyst filling length of an oxidation catalyst layer in a method where raw material gas containing gaseous t-butanol is supplied to a fixed-bed multitubular reactor having a dehydration catalyst layer and an oxidation catalyst layer in this order, from the entrance for raw material gas toward the exit, to produce methacrolein and/or methacrylic acid by dehydration reaction and catalytic gas phase oxidation reaction, and the present invention can increase the conventional yield of approximately 80% to 81 to 82% even when a reaction bath temperature is relatively low (approximately 355° C.).
摘要翻译：本发明涉及甲基丙烯醛和/或甲基丙烯酸的制造方法，其特征在于，在含有原料气体的方法中，脱水催化剂层的催化剂填充长度为氧化催化剂层的催化剂填充长度的3〜20％将气态叔丁醇从原料气体入口向出口依次供给具有脱水催化剂层和氧化催化剂层的固定床多管反应器，通过脱水反应生成甲基丙烯醛和/或甲基丙烯酸，催化气相氧化反应，即使反应浴温度相对较低（约355℃），本发明也可将常规产率提高约80％至81％至82％。

8. 发明申请

US20070073084A1 Method of producing unsaturated acid in fixed-bed catalytic partial oxidation reactor with high efficiency 有权
标题翻译：固定床催化部分氧化反应器高效生产不饱和酸的方法
公开(公告)号：US20070073084A1
公开(公告)日：2007-03-29
申请号：US11483752
申请日：2006-07-10
申请人： Kyoung Ha , Boo Woo , Jun Ko , Seong Kang , Seok Choi , Young Kim
发明人： Kyoung Ha , Boo Woo , Jun Ko , Seong Kang , Seok Choi , Young Kim
IPC分类号： B01J8/04 , C07C51/16 , C07C51/235
CPC分类号： C07C45/34 , B01J8/0453 , B01J8/0457 , B01J8/067 , B01J2208/00212 , B01J2208/0053 , B01J2208/025 , B01J2219/0004 , C07C45/35 , C07C45/36 , C07C45/37 , C07C51/215 , C07C51/252 , C07C47/21 , C07C47/22 , C07C57/04
摘要： Disclosed is a process for producing unsaturated aldehydes and/or unsaturated acids from olefins or alkanes in a fixed bed shell-and-tube heat exchanger-type reactor by catalytic vapor phase oxidation. A heat exchanger-type reactor for use in such a process is also disclosed. In the process, at least one of the first-step reaction zone and the second-step reaction zone is divided into two or more shell spaces by at least one partition; each of the divided shell spaces is independently heat-controlled; a heat transfer medium in the first shell space of the first-step reaction zone or the first shell space of the second-step reaction zone has a temperature ranging from the lowest active temperature of a catalyst layer packed in a reaction tube corresponding to the first shell space of the first-step reaction zone or the first shell space of the second-step reaction zone to [the lowest active temperature+20° C.], when referring to the two or more shell spaces corresponding to the first-step reaction zone sequentially as the first shell space of the first-step reaction zone, the second shell space of the first-step reaction zone, . . . , the nth shell space of the first-step reaction zone, and the two or more shell spaces corresponding to the second-step reaction zone sequentially as the first shell space of the second-step reaction zone, the second shell space of the second-step reaction zone, . . . , the nth shell space of the second-step reaction zone; and the first shell space of the first-step reaction zone or the first shell space of the second-step reaction zone is controlled in such a manner that the first shell space provides a reactant conversion contribution per length as defined in Equation 1 or 2 of 1.2˜2.5.
摘要翻译：公开了一种通过催化气相氧化在固定床管壳式热交换器型反应器中由烯烃或烷烃生产不饱和醛和/或不饱和酸的方法。还公开了一种用于这种方法的热交换器型反应器。在该过程中，至少一个第一步骤反应区和第二步反应区被至少一个隔板分成两个或多个壳层空间; 每个分开的壳空间是独立的热控制的; 在第一步骤反应区的第一壳体空间或第二阶段反应区的第一壳体空间中的传热介质的温度范围从填充在对应于第一步骤的反应管的反应管中的催化剂层的最低活性温度当提及对应于第一步反应的两个或多个壳层空间时，第一步反应区的壳体空间或第二步反应区的第一壳空间为[最低活性温度+ 20℃] 作为第一步反应区的第一壳空间，第一步反应区的第二壳空间。。。，第一步反应区的第n个第<！ - SIPO - >壳空间，以及对应于第二步反应区的两个或多个壳层空间依次作为第二步反应区的第一壳空间，第二步反应区的第二个壳体空间。。。，第二步反应区的第n个壳空间; 并且以这样的方式控制第一步骤反应区或第二阶段反应区的第一壳层空间的第一壳层空间，使得第一壳空间提供如式1或2中定义的每个长度的反应物转化贡献 1.2〜2.5。

9. 发明申请

US20040220429A1 Process and catalyst for production of formaldehyde from dimethyl ether 审中-公开
公开(公告)号：US20040220429A1
公开(公告)日：2004-11-04
申请号：US10861214
申请日：2004-06-03
申请人： Regents of the University of California
发明人： Haichao Liu , Enrique Iglesia
IPC分类号： C07C045/37
CPC分类号： B01J37/0201 , B01J23/22 , B01J23/28 , B01J35/0046 , C07C45/37 , C07C47/04
摘要： Dimethyl ether is converted to formaldehyde using a supported catalyst comprising molybdenum and/or vanadium oxides. The surface density of the oxide(s) ranges from greater than that for the isolated monomeric oxides upwards, so long as there is a substantial absence of bulk crystalline molybdenum and/or vanadium oxide(s). Conversion and selectivity to formaldehyde are improved as compared to data reported for known catalysts. Also disclosed is a supported catalyst comprising molybdenum and/or vanadium oxides wherein the support comprises one or more reducible metal oxides, preferably a layer or layers of one or more reducible metal oxides disposed on the surface of a particulate alumina or zirconia support.

10. 发明授权

US06346646B1 Process for producing methacrolein and methacrylic acid 有权
标题翻译：甲基丙烯醛和甲基丙烯酸的制备方法
公开(公告)号：US06346646B1
公开(公告)日：2002-02-12
申请号：US09463385
申请日：2000-01-27
申请人： Seigo Watanabe , Motomu Oh-Kita
发明人： Seigo Watanabe , Motomu Oh-Kita
IPC分类号： C07C5125
CPC分类号： C07C51/235 , B01J23/002 , B01J23/8876 , B01J2523/00 , C07C45/35 , C07C45/37 , C07C51/21 , C07C51/252 , C07C47/22 , C07C57/04 , B01J2523/15 , B01J2523/27 , B01J2523/53 , B01J2523/54 , B01J2523/68 , B01J2523/842 , B01J2523/845
摘要： A process for producing methacrolein and methacrylic acid by catalytically oxidizing isobutylene or tertiary butanol in the presence of a catalyst comprising a compound oxide containing molybdenum, bismuth and iron as the essential components, wherein a catalytic oxidation reaction is started at a temperature of (T−3)° C. or lower wherein T° C. is defined as the boundary temperature of activation energy of a reaction for obtaining methacrolein and methacrylic acid from isobutylene using said catalyst, the reaction is continued while the reaction temperature is increased as the activity of the catalyst decreases, and an activation treatment is conducted for the catalyst at least once before the reaction temperature exceeds the boundary temperature of activation energy.
摘要翻译：在含有以钼，铋和铁为主要成分的复合氧化物的催化剂存在下催化氧化异丁烯或叔丁醇的方法，其中催化氧化反应在（T- 3）℃或更低，其中T℃定义为使用所述催化剂从异丁烯获得异丁烯醛和甲基丙烯酸的反应的活化能的边界温度，反应继续，同时反应温度随着催化剂减少，并且在反应温度超过活化能的边界温度之前，对催化剂进行至少一次的活化处理。

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