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1. 发明申请

US20130217897A1 VPO CATALYST WITH LOW VANADIUM OXIDATION STATE FOR MALEIC ANDHYDRIDE PRODUCTION (D#81,745) 审中-公开
标题翻译：具有低氧化钒氧化态的VPO催化剂用于马来酸酐生产（D＃81,745）
公开(公告)号：US20130217897A1
公开(公告)日：2013-08-22
申请号：US13821050
申请日：2011-08-24
申请人： Zhiping Shan , Michael J. Mummey , William S. Frazee , Bennie A. Horrell
发明人： Zhiping Shan , Michael J. Mummey , William S. Frazee , Bennie A. Horrell
IPC分类号： B01J27/198 , C07D307/60
CPC分类号： B01J27/198 , B01J27/199 , B01J35/002 , B01J35/026 , B01J35/1014 , B01J37/16 , C07C51/215 , C07D307/60 , C07C57/145
摘要： An oxidation catalyst comprising vanadium, phosphorus, and oxygen having average vanadium valence less than about 4.10, and a method of preparing such catalyst, is provided. The catalyst has side crush strength of at least about 5 lbs. and improved yield of maleic anhydride from n-butane between about 1% and about 6% absolute. The catalyst is formed by exposing a conventional active VPO catalyst having average vanadium valence between about 4.10 and about 4.40 to an organic solvent having a dielectric constant between about 5 and about 55 under conditions that facilitate an oxidation-reduction reaction, reducing the valence of the vanadium below 4.10.
摘要翻译：提供了包含钒值低于约4.10的钒，磷和氧的氧化催化剂及其制备方法。催化剂具有至少约5磅的侧面压碎强度。并从正丁烷提高约1％至约6％绝对值的马来酸酐产率。催化剂是通过在有助于进行氧化还原反应的条件下将平均钒价在约4.10至约4.40之间的常规活性VPO催化剂暴露于介电常数介于约5至约55之间的有机溶剂而形成的，钒低于4.10。

2. 发明授权

US5877331A Prevention of catalyst attrition and tar formation in manufacture of maleic anhydride 失效
公开(公告)号：US5877331A
公开(公告)日：1999-03-02
申请号：US968172
申请日：1997-11-12
申请人： Michael J. Mummey , Robert A. Keppel , A. Lamar Reeves
发明人： Michael J. Mummey , Robert A. Keppel , A. Lamar Reeves
IPC分类号： B01J8/00 , B01J8/06 , B01J27/198 , C07C51/215 , C07D307/60
CPC分类号： C07C51/215 , B01J23/002 , B01J27/198 , B01J8/006 , B01J8/0085 , B01J8/067 , B01J2208/00088 , B01J2208/00212 , B01J2208/00274 , B01J2208/0069 , B01J2523/00 , Y10S502/523
摘要： Improved methods and apparatus for manufacture of maleic anhydride by catalytic oxidation of n-butane or other hydrocarbon having four carbon atoms in a straight chain over a fixed catalyst bed comprising a phosphorus vanadium oxide catalyst. Movement of catalyst bodies with respect to each other and with respect to the walls of the reaction chamber is restrained so as to prevent the catalyst bodies from abrading against each other or the reactor chamber walls in a manner that would cause formation of catalyst fines. Methods and apparatus are also provided for removal of fines from a fixed catalyst bed. The methods of the invention are effective to prevent loss of catalyst from a tubular reactor, and to control degradation of solvent absorbent in a process in which maleic anhydride is separated from the reaction gas by absorption into such a solvent.

3. 发明授权

US5773382A High performance VPO catalyst and process of preparation thereof 失效
标题翻译：高性能VPO催化剂及其制备方法
公开(公告)号：US5773382A
公开(公告)日：1998-06-30
申请号：US775938
申请日：1997-01-03
申请人： Scott F. Mitchell , Robert A. Keppel , Michael J. Mummey
发明人： Scott F. Mitchell , Robert A. Keppel , Michael J. Mummey
IPC分类号： C07D307/60 , B01J27/198 , B01J35/00 , B01J35/10 , B01J37/00 , B01J37/08 , C07B61/00 , C07C51/21 , C07C51/215 , C07C51/25
CPC分类号： C07C51/252 , B01J23/002 , B01J27/198 , B01J37/0018 , C07C51/215 , C07C51/25 , B01J2523/00 , B01J35/0026 , B01J35/1014 , B01J35/108 , B01J37/08
摘要： An activated porous phosphorus/vanadium oxide catalyst adapted for the catalytic oxidation of a hydrocarbon to produce a carboxylic acid anhydride. The catalyst comprises a shaped body having a volume of at least about 0.02 cc, a phosphorus content of between about 1.05 and about 1.20, a B.E.T. surface area of at least about 15 m.sup.2 /g, an average vanadium oxidation state of between about 4.06 and about 4.3, a total pore volume of at least about 0.15 cc/g, a normalized apparent shaped body density of between about 1.0 and about 2.0 g/cc, and a crush strength of at least about 4 pounds. At least about 20% of the pore volume of the catalyst is constituted of pores having a diameter between about 0.1 and about 3.3 .mu.M, and at least about 40% of the pore volume is constituted of pores having a diameter of less than about 0.1 .mu.M. The catalyst is prepared by mixing a particulate phosphorus/vanadium oxide precursor with a pore modification agent to produce a modified catalyst precursor composition, forming the modified precursor composition into a predetermined shape, and removing the pore modification agent substantially at a temperature below 300.degree. C., preferably using air as a stripping gas.
摘要翻译：一种活化的多孔磷/氧化钒催化剂，适于催化氧化烃以产生羧酸酐。催化剂包括具有至少约0.02cc的体积，约1.05至约1.20的磷含量的成形体，B.E.T. 表面积至少约15m 2 / g，平均钒氧化态在约4.06与约4.3之间，总孔体积至少约0.15cc / g，归一化表观体密度在约1.0至约2.0之间 g / cc，压碎强度至少约4磅。催化剂的孔体积的至少约20％由直径在约0.1至约3.3μm之间的孔构成，并且至少约40％的孔体积由直径小于约0.1的孔构成通过将颗粒状磷/钒氧化物前体与孔改性剂混合以制备改性催化剂前体组合物，将改性前体组合物形成预定形状并基本上在低于下述温度下除去孔改性剂来制备催化剂 300℃，优选使用空气作为汽提气体。

4. 发明授权

US6046343A Prevention of catalyst attrition and tar formation in manufacture of maleic anhydride 有权
标题翻译：防止马来酸酐制造中的催化剂消耗和焦油形成
公开(公告)号：US6046343A
公开(公告)日：2000-04-04
申请号：US257633
申请日：1999-02-25
申请人： Michael J. Mummey , Robert A. Keppel , A. Lamar Reeves
发明人： Michael J. Mummey , Robert A. Keppel , A. Lamar Reeves
IPC分类号： B01J8/00 , B01J8/06 , B01J27/198 , C07C51/215 , C07D307/34
CPC分类号： C07C51/215 , B01J23/002 , B01J27/198 , B01J8/006 , B01J8/0085 , B01J8/067 , B01J2208/00088 , B01J2208/00212 , B01J2208/00274 , B01J2208/0069 , B01J2523/00 , Y10S502/523
摘要： Improved methods and apparatus for manufacture of maleic anhydride by catalytic oxidation of n-butane or other hydrocarbon having four carbon atoms in a straight chain over a fixed catalyst bed comprising a phosphorus vanadium oxide catalyst. Movement of catalyst bodies with respect to each other and with respect to the walls of the reaction chamber is restrained so as to prevent the catalyst bodies from abrading against each other or the reactor chamber walls in a manner that would cause formation of catalyst fines. Methods and apparatus are also provided for removal of fines from a fixed catalyst bed. The methods of the invention are effective to prevent loss of catalyst from a tubular reactor, and to control degradation of solvent absorbent in a process in which maleic anhydride is separated from the reaction gas by absorption into such a solvent.
摘要翻译：通过在包含磷钒氧化物催化剂的固定催化剂床上在直链中具有四个碳原子的正丁烷或其它烃的催化氧化来改进制备马来酸酐的方法和装置。催化剂体相对于反应室的壁的移动受到限制，以防止催化剂体以导致催化剂细粉的形成的方式彼此磨损或反应室壁。还提供了用于从固定催化剂床中除去细粒料的方法和装置。本发明的方法有效地防止催化剂从管式反应器中的损失，并且在通过吸收到这种溶剂中马来酸酐与反应气体分离的方法中来控制溶剂吸收剂的降解。

5. 发明授权

US6005121A High productivity process for the production of maleic anhydride 失效
标题翻译：用于生产马来酸酐的高生产率工艺
公开(公告)号：US6005121A
公开(公告)日：1999-12-21
申请号：US58029
申请日：1998-04-10
申请人： Jerry R. Ebner , Robert A. Keppel , Michael J. Mummey
发明人： Jerry R. Ebner , Robert A. Keppel , Michael J. Mummey
IPC分类号： B01J8/06 , B01J27/198 , B01J35/02 , C07C51/215 , C07C51/54 , C07C57/145 , C07D307/60
CPC分类号： C07C51/215 , B01J23/002 , B01J27/198 , B01J35/026 , B01J8/06 , B01J8/067 , B01J2208/00026 , B01J2208/00044 , B01J2208/0007 , B01J2208/00212 , B01J2208/00539 , B01J2208/00548 , B01J2523/00
摘要： An improved process for the manufacture of maleic anhydride by catalytic oxidation of a nonaromatic hydrocarbon having at least four carbon atoms in a straight chain, in which a gas containing oxygen and hydrocarbon is passed through a fixed catalyst bed in a tubular reactor. The activity of the catalyst bed is graded in such manner that the reactor can be operated at an initial (feed gas) hydrocarbon concentration of over 1.5% by volume, an integrated average temperature difference between gas and cooling fluid of at least about 15.degree. C. over that portion of the bed in which the gas temperature exceeds the cooling fluid temperature, and a productivity of at least about 5.0 lbs. maleic anhydride per hour, without the temperature difference between the gas and the cooling fluid exceeding 80.degree. C. at any point in the catalyst bed during the course of the reaction. Preferably, the catalyst activity and the gas permeability of the bed vary in the direction of gas flow so that both the catalyst activity and the pressure drop per unit distance are lower in a critical region, where the combination of temperature and hydrocarbon concentration could otherwise cause the reaction to proceed at an excessive rate, than they are in a region of low temperature and low hydrocarbon concentration. Significant and unexpected improvement in reactor performance is achieved by the combination of a graded catalyst charge and incorporation of a catalyst modifying organophosphorus compound in the hydrocarbon feed.
摘要翻译：通过在直链中具有至少四个碳原子的非芳族烃的催化氧化制备马来酐的改进方法，其中含有氧和烃的气体通过管式反应器中的固定催化剂床。催化剂床的活性以这样的方式分级，使得反应器可以以超过1.5体积％的初始（进料气体）烃浓度操作，气体和冷却流体之间的一体化平均温差为至少约15℃ 在其中气体温度超过冷却流体温度的床的那部分上，并且生产率至少约为5.0磅。马来酸酐/小时，在反应过程中，在催化剂床中的任何点处，气体和冷却流体之间的温差不超过80℃。优选地，床的催化剂活性和气体渗透性在气流方向上变化，使得催化剂活性和每单位距离的压降在临界区域较低，其中温度和烃浓度的组合可能会导致反应以比低温和低碳氢化合物浓度的区域高的速度进行。反应器性能的显着和意想不到的改进通过将分级催化剂装料和在烃进料中掺入催化剂改性有机磷化合物的组合来实现。

6. 发明授权

US4855459A Process for the production of maleic anhydride 失效
标题翻译：马来酸酐生产工艺
公开(公告)号：US4855459A
公开(公告)日：1989-08-08
申请号：US145795
申请日：1988-01-19
申请人： Michael J. Mummey
发明人： Michael J. Mummey
IPC分类号： C07D307/60 , B01J27/195 , C07B61/00 , C07C51/215
CPC分类号： C07C51/215
摘要： Maleic anhydride is produced by the catalytic vapor phase partial oxidation of a nonaromatic hydrocarbon having at least four carbon atoms in a straight chain with molecular oxygen or a molecular oxygen-containing gas in the presence of phosphorus-vanadium mixed oxide oxidation catalyst. The catalyst is diluted with an inert solid material in an amount sufficient to form a catalyst-inert solid material composition effective to stabilize the maleic anhydride yield such that the average yield decay is less than 0.30% of the established initial maleic anhydride yield per month over an extended period of sustained operations.

7. 发明授权

US5734066A Supression of autoignition in maleic anhydride production 失效
标题翻译：抑制马来酸酐生产中的自燃
公开(公告)号：US5734066A
公开(公告)日：1998-03-31
申请号：US835152
申请日：1992-02-13
申请人： Robert A. Keppel , Scott F. Mitchell , Michael J. Mummey
发明人： Robert A. Keppel , Scott F. Mitchell , Michael J. Mummey
IPC分类号： B01J27/198 , C07C51/215 , C07C51/225 , C07C57/145 , C07D307/60
CPC分类号： C07C51/215
摘要： An improved process for the manufacture of maleic anhydride by catalytic oxidation of n-butane in which the feed flow channel to the catalytic reactor contains an autoignition suppression agent containing acid sites or trivalent phosphorus as an ignition inhibiting component. The autoignition suppression agent may also be used in other gas/liquid containment envelopes for flammable mixtures of hydrocarbons and oxygen. A novel apparatus and method are disclosed for assessing the influence of system conditions on autoignition of hydrocarbon/oxygen mixtures.
摘要翻译：通过正丁烷的催化氧化制备马来酸酐的改进方法，其中向催化反应器的进料流动通道含有含有酸性位点或三价磷作为点火抑制组分的自燃抑制剂。自燃抑制剂也可以用于其它气体/液体容纳包封，用于可燃的烃和氧混合物。公开了一种用于评估系统条件对烃/氧混合物的自燃的影响的新颖的装置和方法。

8. 发明授权

US5641722A High performance VPO catalyst and process of preparation thereof 失效
标题翻译：高性能VPO催化剂及其制备方法
公开(公告)号：US5641722A
公开(公告)日：1997-06-24
申请号：US306489
申请日：1994-09-15
申请人： Scott F. Mitchell , Robert A. Keppel , Michael J. Mummey
发明人： Scott F. Mitchell , Robert A. Keppel , Michael J. Mummey
IPC分类号： C07D307/60 , B01J27/198 , B01J35/00 , B01J35/10 , B01J37/00 , B01J37/08 , C07B61/00 , C07C51/21 , C07C51/215 , C07C51/25
CPC分类号： C07C51/252 , B01J23/002 , B01J27/198 , B01J37/0018 , C07C51/215 , C07C51/25 , B01J2523/00 , B01J35/0026 , B01J35/1014 , B01J35/108 , B01J37/08
摘要： An activated porous phosphorus/vanadium oxide catalyst adapted for the catalytic oxidation of a hydrocarbon to produce a carboxylic acid anhydride. The catalyst comprises a shaped body having a volume of at least about 0.02 cc, a phosphorus content of between about 1.05 and about 1.20, a B.E.T. surface area of at least about 15 m.sup.2 /g, an average vanadium oxidation state of between about 4.06 and about 4.3, a total pore volume of at least about 0.15 cc/g, a normalized apparent shaped body density of between about 1.0 and about 2.0 g/cc, and a crush strength of at least about 4 pounds. At least about 20% of the pore volume of the catalyst is constituted of pores having a diameter between about 0.1 and about 3.3 .mu.M, and at least about 40% of the pore volume is constituted of pores having a diameter of less than about 0.1 .mu.M. The catalyst is prepared by mixing a particulate phosphorus/vanadium oxide precursor with a pore modification agent to produce a modified catalyst precursor composition, forming the modified precursor composition into a predetermined shape, and removing the pore modification agent substantially at a temperature below 300.degree. C., preferably using air as a stripping gas.
摘要翻译：一种活化的多孔磷/氧化钒催化剂，适于催化氧化烃以产生羧酸酐。催化剂包括具有至少约0.02cc的体积，约1.05至约1.20的磷含量的成形体，B.E.T. 表面积至少约15m 2 / g，平均钒氧化态在约4.06与约4.3之间，总孔体积至少约0.15cc / g，归一化表观体密度在约1.0至约2.0之间 g / cc，压碎强度至少约4磅。催化剂的孔体积的至少约20％由直径在约0.1至约3.3μm之间的孔构成，并且至少约40％的孔体积由直径小于约0.1的孔构成通过将颗粒状磷/钒氧化物前体与孔改性剂混合以制备改性催化剂前体组合物，将改性前体组合物形成预定形状并基本上在低于下述温度下除去孔改性剂来制备催化剂 300℃，优选使用空气作为汽提气体。

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