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公开(公告)号：US5877331A
公开(公告)日：1999-03-02
申请号：US968172
申请日：1997-11-12
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.
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2.发明授权Prevention of catalyst attrition and tar formation in manufacture of maleic anhydride 有权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
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。
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公开(公告)号：US5773382A
公开(公告)日：1998-06-30
申请号：US775938
申请日：1997-01-03
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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公开(公告)号：US6005121A
公开(公告)日：1999-12-21
申请号：US58029
申请日：1998-04-10
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。
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公开(公告)号：US5734066A
公开(公告)日：1998-03-31
申请号：US835152
申请日：1992-02-13
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。
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公开(公告)号：US5641722A
公开(公告)日：1997-06-24
申请号：US306489
申请日：1994-09-15
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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7.发明授权
公开(公告)号：US5168090A
公开(公告)日：1992-12-01
申请号：US812252
申请日：1991-12-20
申请人： Jerry R. Ebner , Robert A. Keppel
发明人： Jerry R. Ebner , Robert A. Keppel
IPC分类号： B01J19/30 , B01J27/198 , B01J35/00 , B01J35/02 , C07C51/215 , C07C51/25 , C07C51/31
CPC分类号： B01J19/30 , B01J23/002 , B01J27/198 , B01J35/026 , B01J35/1004 , C07C51/215 , C07C51/25 , C07C51/252 , C07C51/313 , B01J2219/30242 , B01J2219/30296 , B01J2219/30475 , B01J2523/00 , B01J35/0026
摘要： Shaped oxidation catalyst structures containing catalytic material comprised of mixed oxides of vanadium and phosphorus which are useful for the production of maleic anhydride via the partial oxidation of nonaromatic hydrocarbons, particularly n-butane, in the vapor phase with molecular oxygen or a molecular oxygen-containing gas are provided. Such structures are characterized by exhibiting (a) a geometric volume of from about 30 percent to about 67 percent of that exhibited by the void space-free solid geometric form, (b) an external geometric surface area/geometric volume ratio of at least about 20 cm.sup.-1, (c) a bulk density of from about 0.4 g/cm.sup.3 to about 1.4 g/cm.sup.3, and (d) a mechanical resistance sufficient to maintain substantially the structural integrity of the shaped structure under handling and use conditions.
摘要翻译： 包含由钒和磷的混合氧化物组成的催化材料的成形氧化催化剂结构，其可用于通过在分子氧或含分子氧的气相中部分氧化非芳族烃，特别是正丁烷来生产马来酸酐 提供气体。 这种结构的特征在于显示（a）无空隙空间固体几何形状所显示的几何体积的几何体积约为30％至约67％，（b）外部几何表面积/几何体积比为至少约 20cm-1，（c）约0.4g / cm 3至约1.4g / cm 3的堆积密度，和（d）足以在处理和使用条件下基本上保持成形结构的结构完整性的机械阻力。
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8.发明授权Process for the preparation of iron/lithium -promoted catalysts for the production of maleic anhydride 失效用于制备用于生产马来酸酐的铁/锂 - 催化剂的方法
公开(公告)号：US4670415A
公开(公告)日：1987-06-02
申请号：US791977
申请日：1985-10-28
IPC分类号： B01J27/198 , C07C51/215 , C07C51/25 , B01J27/185 , C07D307/34
CPC分类号： C07C51/252 , B01J23/002 , B01J27/198 , C07C51/215 , C07C51/25 , B01J2523/00
摘要： Iron/lithium promoted phosphorus-vanadium-oxygen catalysts for the production of maleic anhydride are prepared by contacting a substantially tetravalent vanadium-containing compound and a phosphorus-containing compound and a promoter component containing each of iron and lithium in a substantially anhydrous alcohol medium in the presence of anhydrous hydrogen chloride to form an iron/lithium promoted phosphorus-vanadium-oxygen catalyst precursor. The catalyst precursor is recovered, dried, roasted, formed into structures if structures are desired, and calcined.
摘要翻译： 通过使基本上四价的含钒化合物和含磷化合物和含有铁和锂的助催化剂组分在基本上无水的醇介质中接触来制备用于生产马来酐的铁/锂促进的磷 - 钒 - 氧催化剂 存在无水氯化氢以形成铁/锂促进的磷 - 钒 - 氧催化剂前体。 将催化剂前体回收，干燥，焙烧，如果需要结构，则形成结构并煅烧。
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公开(公告)号：US4632915A
公开(公告)日：1986-12-30
申请号：US791655
申请日：1985-10-28
IPC分类号： B01J27/198 , C07B61/00 , C07C51/215 , C07C51/25 , B01J27/185 , C07D307/34
CPC分类号： C07C51/252 , B01J23/002 , B01J27/198 , C07C51/215 , C07C51/25 , B01J2523/00
摘要： Catalysts useful for the partial oxidation of nonaromatic hydrocarbons, particularly n-butane, with molecular oxygen or an oxygen-containing gas in the vapor phase to produce maleic anhydride are provided which comprise phosphorus, vanadium, and oxygen and a promoter component containing each of iron and lithium.
摘要翻译： 提供了用于在气相中分子氧或含氧气体部分氧化非芳族烃，特别是正丁烷以产生马来酸酐的催化剂，其包含磷，钒和氧，以及含有各自的铁的促进剂组分 和锂。
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10.发明授权
公开(公告)号：US4567158A
公开(公告)日：1986-01-28
申请号：US566361
申请日：1983-12-28
申请人： James T. Wrobleski , James W. Edwards , Charles R. Graham , Robert A. Keppel , Harold Raffelson
发明人： James T. Wrobleski , James W. Edwards , Charles R. Graham , Robert A. Keppel , Harold Raffelson
IPC分类号： B01J27/198 , C07C51/215 , C07C51/25 , C07C51/31 , B01J27/14 , C07D307/34
CPC分类号： B01J23/002 , B01J27/198 , C07C51/215 , C07C51/25 , C07C51/252 , C07C51/313 , B01J2523/00
摘要： Phosphorus-vanadium mixed oxide oxidation catalysts are prepared by introducing a substantially pentavalent vanadium-containing compound and a pentavalent phosphorus-containing compound into an alcohol medium capable of reducing the vanadium to a valence state less than +5 in the presence of an alcohol-modifying agent to form a phosphorus-vanadium mixed oxide catalyst precursor. The catalyst precursor is recovered, dried, formed into desired structures, and calcined at temperatures from about 250.degree. C. to about 600.degree. C. The catalysts are highly effective in that they exhibit a weight/weight productivity of at least 70 grams of maleic anhydride per kilogram of catalyst per hour.
摘要翻译： 磷钒混合氧化物氧化催化剂是通过将基本上五价含钒的化合物和五价含磷化合物引入到能够在醇改性的存在下将钒还原成低于+5的价态的醇介质中来制备的 以形成磷钒混合氧化物催化剂前体。 将催化剂前体回收，干燥，形成所需的结构，并在约250℃至约600℃的温度下煅烧。催化剂非常有效，因为它们表现出至少70克马来酸的重量/重量产率 酸酐每小时每千克催化剂。
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