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    Method of preparing catalyst used for producing methacrylic acids
    2.
    发明授权
    Method of preparing catalyst used for producing methacrylic acids 失效
    制备甲基丙烯酸的催化剂的制备方法

    公开(公告)号：US5420091A

    公开(公告)日：1995-05-30

    申请号：US90278

    申请日：1993-07-13

    申请人： Toru Kuroda ,  Motomu Oh-Kita

    发明人： Toru Kuroda ,  Motomu Oh-Kita

    IPC分类号： B01J27/199 ,  C07B61/00 ,  C07C51/25 ,  C07C57/055 ,  B01J27/18 ,  B01J27/19

    CPC分类号： B01J23/002 ,  B01J27/199 ,  C07C51/252 ,  B01J2523/00

    摘要： A method of preparing a catalyst used for producing methacrylic acids through gas phase catalytic oxidation of methacrolein with molecular oxygen. The catalyst is represented by the formula:P.sub.a Mo.sub.b V.sub.c Ge.sub.d X.sub.e Y.sub.f Z.sub.g O.sub.hwherein P, Mo, V, Ge and O represent phosphorous, molybdenum, vanadium, germanium and oxygen, respectively; X represents at least one element selected from the group consisting of arsenic, antimony, bismuth, zirconium, tellurium, silver and boron; Y represents at lest one element selected from the group consisting of iron, copper, zinc, chromium, magnesium, tantalum, manganese, barium, gallium, cerium and lanthanum; Z represents at least one element selected from the group consisting of potassium, rubidium, cesium and thallium, and a, b, c, d, e, f, g and h represent the atomic ratios of the respective elements, and when b=12, then a=0.5-3, c=0.01-3, d=0.01-3, e=0-3, f=0-3, g=0.01-3, and h is the number of oxygen atoms necessary for satisfying the above atomic ratios of the respective components. The method includes providing an aqueous mixture containing at least P, Mo, V, Ge, X, Y and Z and removing water from the aqueous mixture, where the improvement comprises providing at least part of the Ge for the aqueous mixture by dissolving germanium dioxide in an aqueous solution of a hydroxide of an element represented by Z in the above formula. The catalyst prepared according to the method is remarkably elevated in activity in the methacrolein oxidation reaction and allows enhancement of the yield of methacrylic acid.

    摘要翻译： 一种制备用于通过甲基丙烯醛与分子氧的气相催化氧化生产甲基丙烯酸的催化剂的方法。 催化剂由下式表示：PaMobVcGedXeYfZgOh其中P，Mo，V，Ge和O分别表示磷，钼，钒，锗和氧; X表示选自砷，锑，铋，锆，碲，银和硼中的至少一种元素; Y代表选自铁，铜，锌，铬，镁，钽，锰，钡，镓，铈和镧中的一种元素; Z表示选自钾，铷，铯和铊中的至少一种元素，a，b，c，d，e，f，g和h表示各元素的原子比，当b = 12时 ，则a = 0.5-3，c = 0.01-3，d = 0.01-3，e = 0-3，f = 0-3，g = 0.01-3，h为满足 以上各成分的原子比。 该方法包括提供至少含有P，Mo，V，Ge，X，Y和Z的水性混合物，并从水性混合物中除去水，其中改进包括通过将二氧化锗溶解来提供含水混合物的至少一部分Ge 在上式中由Z表示的元素的氢氧化物的水溶液中。 根据该方法制备的催化剂在甲基丙烯醛氧化反应中的活性显着提高，并且可以提高甲基丙烯酸的产率。

    Process for preparing catalysts for producing methacrylic acid
    3.
    发明授权
    Process for preparing catalysts for producing methacrylic acid 失效
    制备甲基丙烯酸催化剂的方法

    公开(公告)号：US5102846A

    公开(公告)日：1992-04-07

    申请号：US598305

    申请日：1990-10-16

    申请人： Toru Kuroda ,  Motomu Oh-Kita ,  Kazuhiro Ishii

    发明人： Toru Kuroda ,  Motomu Oh-Kita ,  Kazuhiro Ishii

    IPC分类号： B01J23/885 ,  B01J27/199 ,  B01J35/10 ,  C07B61/00 ,  C07C51/25 ,  C07C57/055

    CPC分类号： B01J23/002 ,  B01J23/885 ,  B01J27/199 ,  C07C51/252 ,  B01J2523/00

    摘要： In a process for producing a catalyst having a composition represented by the following formula usable to produce methacrylic acid by the gas-phase catalytic oxidation of methacrolein with molecular oxygen,P.sub.a Mo.sub.b Cu.sub.c V.sub.d X.sub.e Y.sub.f Z.sub.g O.sub.hwherein P, Mo, Cu, V and O are phosphorus, molybdenum, copper, vanadium and oxygen, respectively, X is at least one element selected from the group consisting of arsenic, antimony, bismuth, germanium, zirconium, tellurium and silver, Y is at least one element selected from the group consisting of iron, zinc, chromium, magnesium, tantalum, manganese, barium, boron, gallium, cerium and lanthanum, Z is at least one element selected from the group consisting of potassium, rubidium, cesium and thallium, a, b, c, d, e, f, g and h are an atomic ratio of each element, and when b is 12, a is 0.5 to 3, c is 0.01 to 2, d is 0.01 to 3, e is 0.01 to 3, f is 0 to 3, g is 0.01 to 2 nd h is the number of oxygen atoms necessary to satisfy the valence of each component, an improvement comprising adding 0.05 to 1.0 mole of nitric acid based on 12 moles of a molybdenum atom to a slurry containing materials for the catalyst components. According to the present invention, a catalyst for gas-phase catalytic oxidation excellent in the conversion of methacrolein and selectivity for methacrylic acid is obtained.

    Method for packing with catalyst for synthesis of unsaturated aldehyde and unsaturated carboxylic acid
    4.
    发明授权
    Method for packing with catalyst for synthesis of unsaturated aldehyde and unsaturated carboxylic acid 失效
    用于合成不饱和醛和不饱和羧酸的催化剂填充的方法

    公开(公告)号：US5892108A

    公开(公告)日：1999-04-06

    申请号：US852162

    申请日：1997-05-06

    申请人： Tohru Shiotani ,  Miezi Sugiyama ,  Toru Kuroda ,  Motomu Oh-Kita

    发明人： Tohru Shiotani ,  Miezi Sugiyama ,  Toru Kuroda ,  Motomu Oh-Kita

    IPC分类号： B01J23/88 ,  B01J19/30 ,  B01J23/887 ,  C07B61/00 ,  C07C27/12 ,  C07C45/32 ,  C07C45/35 ,  C07C45/37 ,  C07C45/38 ,  C07C47/22 ,  C07C51/235 ,  C07C51/25 ,  C07C57/05 ,  C07C51/16

    CPC分类号： C07C45/37 ,  B01J23/002 ,  B01J23/887 ,  B01J23/8876 ,  C07C45/32 ,  C07C45/35 ,  C07C51/252 ,  B01J2523/00

    摘要： A method for packing of catalyst, which comprises mixing, into a shaped catalyst containing at least molybdenum and iron, used in the gas-phase catalytic oxidation of propylene, isobutylene, tert-butyl alcohol or methyl tert-butyl ether with molecular oxygen to synthesize an unsaturated aldehyde and an unsaturated carboxylic acid both corresponding to the raw material used, metal-made Raschig rings as auxiliary packing material having a bulk volume of 0.3-3.5 times that of the shaped catalyst and a packing density of 0.5-1.5 kg/l, and packing the resulting mixture into a fixed bed type reactor; and a process for producing an unsaturated aldehyde and an unsaturated carboxylic acid, which comprises subjecting propylene, isobutylene, tert-butyl alcohol or methyl tert-butyl ether to gas-phase catalytic oxidation using molecular oxygen, in a fixed bed type reactor wherein a catalyst is packed by the above method.

    摘要翻译： 一种包装催化剂的方法，其包括将至少含有钼和铁的成形催化剂混合，用于丙烯，异丁烯，叔丁醇或甲基叔丁基醚与分子氧的气相催化氧化以合成 对应于所使用的原料的不饱和醛和不饱和羧酸，金属制的拉西奇环作为本体体积为成形催化剂的0.3-3.5倍的辅助包装材料，填充密度为0.5-1.5kg / l 并将所得混合物包装到固定床型反应器中; 以及制造不饱和醛和不饱和羧酸的方法，其包括在固定床型反应器中使丙烯，异丁烯，叔丁醇或甲基叔丁基醚用分子氧进行气相催化氧化，其中催化剂 由上述方法包装。

    Process for producing methacrylic acid
    6.
    发明授权
    Process for producing methacrylic acid 失效
    生产甲基丙烯酸的方法

    公开(公告)号：US5093521A

    公开(公告)日：1992-03-03

    申请号：US376062

    申请日：1989-07-06

    申请人： Motomu Oh-Kita ,  Toru Kuroda ,  Yutaka Kinoshita ,  Kazuhiro Ishii

    发明人： Motomu Oh-Kita ,  Toru Kuroda ,  Yutaka Kinoshita ,  Kazuhiro Ishii

    IPC分类号： B01J27/199 ,  B01J27/24 ,  C07B61/00 ,  C07C51/25 ,  C07C57/055

    CPC分类号： C07C51/252 ,  B01J23/002 ,  B01J27/199 ,  B01J2523/00

    摘要： A process for producing methacrylic acid which includes subjecting methacrolein to gaseous phase catalytic oxidation using molecular oxygen and a catalyst represented by the general formula:P.sub.a Mo.sub.b V.sub.c Fe.sub.d Ce.sub.e (NH.sub.4).sub.f X.sub.g Y.sub.h Z.sub.i O.sub.jwherein P, Mo, V, Fe, Ce, NH.sub.4 and O represent phosphorus, molybdenum, vanadium, iron, cerium, ammonium group and oxygen, respectively; X represents at least one element selected from the group consisting of copper, zinc, bismuth, chromium, magnesium, silver, tantalum and lanthanum; Y represents at least one element selected from the group consisting of arsenic, antimony, zirconium, barium, manganese, germanium and tellurium; Z represents at least one element selected from the group consisting of potassium, rubidum, cesium and thallium; a, b, c, d, e, g, h, i and j each represents an atomic ratio of each element, and b is 12, a is in a range of 0.5-3, c is in a range of 0.01-3, d is in a range of 0.01-2, e is in a range of 0.01-2, g is in a range of 0.01-3, h is in a range of 0.01-3, i is in a range of 0.01-2 and j is the number of oxygen atoms taken to satisfy the valence requirements stoichiometrically; f represents a number of ammonium groups and is in a range of 0.1-3.6.

    Process for the preparation of catalyst used in the production of unsaturated carboxylic acids
    8.
    发明授权
    Process for the preparation of catalyst used in the production of unsaturated carboxylic acids 失效
    制备用于生产不饱和羧酸的催化剂的方法

    公开(公告)号：US4891347A

    公开(公告)日：1990-01-02

    申请号：US795820

    申请日：1985-11-07

    申请人： Motomu Oh-Kita ,  Kazuhiro Ishii ,  Masaaki Kato ,  Masao Kobayashi

    发明人： Motomu Oh-Kita ,  Kazuhiro Ishii ,  Masaaki Kato ,  Masao Kobayashi

    IPC分类号： B01J27/19 ,  C07B61/00 ,  C07C51/00 ,  C07C51/235 ,  C07C51/25 ,  C07C57/055 ,  C07C67/00

    CPC分类号： C07C51/252 ,  B01J27/19

    摘要： The present invention provides a process for the preparation of a catalyst used in the production of unsaturated carboxylic acids such as methacrylic acid by the gas phase catalytic oxidation of the corresponding unsaturated aldehydes such as methacrolein. Said catalyst is composed of a multi-component composition containing at least phosphorus, molybdenum and antimony. The present invention has attained an improved in its catalytic performance such as conversion rate, selectivity, single-pass yield etc. by using antimony trioxide with average particle size of no more than 0.2 micron as a starting material upon preparing said catalyst.

    摘要翻译： 本发明提供了通过气相催化氧化相应的不饱和醛如甲基丙烯醛，制备用于生产不饱和羧酸如甲基丙烯酸的催化剂的方法。 所述催化剂由至少含有磷，钼和锑的多组分组合物组成。 本发明在制备所述催化剂时，通过使用平均粒径不超过0.2微米的三氧化锑作为起始材料，在其催化性能如转化率，选择性，单程产率等方面得到了改进。

    Carrier-supported catalyst for the synthesis of unsaturated aldehydes and unsaturated carboxylic acids and process for preparing the same
    10.
    发明授权
    Carrier-supported catalyst for the synthesis of unsaturated aldehydes and unsaturated carboxylic acids and process for preparing the same 失效
    用于合成不饱和醛和不饱和羧酸的载体载体催化剂及其制备方法

    公开(公告)号：US5532199A

    公开(公告)日：1996-07-02

    申请号：US359430

    申请日：1994-12-20

    申请人： Seigo Watanabe ,  Motomu Oh-Kita

    发明人： Seigo Watanabe ,  Motomu Oh-Kita

    IPC分类号： B01J23/31 ,  B01J23/887 ,  B01J35/06 ,  B01J37/02 ,  C07C45/35 ,  C07C45/37 ,  C07C51/25

    CPC分类号： C07C45/37 ,  B01J23/002 ,  B01J23/31 ,  B01J23/8876 ,  B01J35/06 ,  C07C45/35 ,  C07C51/252 ,  B01J2523/00 ,  B01J37/0223

    摘要： A carrier-supported catalyst for the synthesis of unsaturated aldehydes and unsaturated carboxylic acids, comprising a catalyst active substance comprising at least molybdenum and bismuth as its components, glass fiber having an average diameter in a range of more than 5 .mu.m and not more than 200 .mu.m and an average length in a range of from 50 .mu.m to 1 mm, which is used as a carrier assistant in an amount of 0.5-50% by weight based on the catalyst active substance, and a carrier. The carrier-supported catalyst of this invention suffers no release or fall-off of the catalyst active substance from the carrier even if the catalyst supporting rate is increased. It also has high mechanical strength and is helpful for providing the objective product in a high yield. Further, the carrier-supported catalyst preparation process of this invention is capable of producing a carrier-supported catalyst having excellent mechanical strength and enabling high-yield production of an objective product, with ease and good reproducibility.

    摘要翻译： 用于合成不饱和醛和不饱和羧酸的载体负载催化剂，其包含至少包含钼和铋作为其组分的催化剂活性物质，平均直径在5μm以上且不大于 200μm，平均长度为50μm〜1mm，作为载体助剂，其用量为催化剂活性物质的0.5〜50wt％，载体为载体。 本发明的载体负载型催化剂即使催化剂支持率提高，也不会使催化剂活性物质从载体中释放或脱落。 它还具有很高的机械强度，有助于以高产量提供目标产品。 此外，本发明的载体负载型催化剂制备方法能够以容易且良好的再现性制造具有优异的机械强度且能够高产率生产目标产物的载体负载型催化剂。