公开(公告)号：US08242304B2

公开(公告)日：2012-08-14

申请号：US13048537

申请日：2011-03-15

申请人： Fumiya Zaima ,  Nobuo Namiki ,  Hideaki Fujita ,  Masato Inari

发明人： Fumiya Zaima ,  Nobuo Namiki ,  Hideaki Fujita ,  Masato Inari

IPC分类号： C07C51/16 ,  C07C51/255

CPC分类号： C07C51/47 ,  C07C63/24

摘要： A method for producing isophthalic acid, comprising: subjecting a m-phenylene compound and a molecular-oxygen-containing gas to liquid-phase oxidation reaction in the presence of a catalyst comprising a heavy metal compound and a bromine compound, and hydrous acetic acid having a water content of 1 to 15 mass %, to thereby yield a slurry; regulating the temperature of the slurry to 35 to 140° C., to thereby precipitate isophthalic acid; removing the isophthalic acid through solid-liquid separation, to thereby recover a mother liquor; and recovering the catalyst from the mother liquor by following steps (1) to (4) as described.

摘要翻译： 一种间苯二甲酸的制造方法，其特征在于，在含有重金属化合物和溴化合物的催化剂的存在下，使间亚苯基化合物和含分子氧气体进行液相氧化反应， 水含量为1〜15质量％，由此得到浆料; 将浆料的温度调节至35〜140℃，由此沉淀间苯二甲酸; 通过固液分离除去间苯二甲酸，从而回收母液; 并按照如上所述的步骤（1）至（4）从母液中回收催化剂。

公开(公告)号：US08236982B2

公开(公告)日：2012-08-07

申请号：US13048644

申请日：2011-03-15

申请人： Fumiya Zaima ,  Masato Inari ,  Hideaki Fujita ,  Nobuo Namiki

发明人： Fumiya Zaima ,  Masato Inari ,  Hideaki Fujita ,  Nobuo Namiki

IPC分类号： C07C51/16 ,  C07C51/255

CPC分类号： C07C51/47 ,  B01J45/00 ,  B01J49/50 ,  C07C63/26

摘要： A method for producing terephthalic acid comprising: subjecting a p-phenylene compound to a liquid-phase oxidation reaction by the use of a molecular-oxygen-containing gas in the presence of a catalyst at least containing a heavy metal compound and a bromine compound, and hydrous acetic acid having a water content of 1 to 15 mass %, to thereby yield a slurry; regulating the temperature of the slurry to 35 to 140° C., to thereby cause terephthalic acid to precipitate; removing the terephthalic acid through solid-liquid separation, to thereby recover a mother liquor; and recovering the catalyst from the mother liquor through a series of operations (1) to (4), as described, for reusing at least a portion of the catalyst in the liquid-phase oxidation reaction.

摘要翻译： 一种对苯二甲酸的制造方法，其特征在于，在至少含有重金属化合物和溴化合物的催化剂的存在下，通过使用含分子氧的气体对对亚苯基化合物进行液相氧化反应， 水含量为1〜15质量％的含水乙酸，得到浆料; 将浆料的温度调节至35至140℃，从而使对苯二甲酸沉淀; 通过固液分离除去对苯二甲酸，从而回收母液; 并通过如上所述的一系列操作（1）至（4）从母液中回收催化剂，用于在液相氧化反应中重新使用至少一部分催化剂。

公开(公告)号：US20110213180A1

公开(公告)日：2011-09-01

申请号：US13048537

申请日：2011-03-15

申请人： Fumiya ZAIMA ,  Nobuo Namiki ,  Hideaki Fujita ,  Masato Inari

发明人： Fumiya ZAIMA ,  Nobuo Namiki ,  Hideaki Fujita ,  Masato Inari

IPC分类号： C07C51/255

CPC分类号： C07C51/47 ,  C07C63/24

摘要： A method for producing isophthalic acid, comprising: subjecting a m-phenylene compound and a molecular-oxygen-containing gas to liquid-phase oxidation reaction in the presence of a catalyst comprising a heavy metal compound and a bromine compound, and hydrous acetic acid having a water content of 1 to 15 mass %, to thereby yield a slurry; regulating the temperature of the slurry to 35 to 140° C., to thereby precipitate isophthalic acid; removing the isophthalic acid through solid-liquid separation, to thereby recover a mother liquor; and recovering the catalyst from the mother liquor by following steps (1) to (4) as described.

摘要翻译： 一种间苯二甲酸的制造方法，其特征在于，在含有重金属化合物和溴化合物的催化剂的存在下，使间亚苯基化合物和含分子氧气体进行液相氧化反应， 水含量为1〜15质量％，由此得到浆料; 将浆料的温度调节至35〜140℃，由此沉淀间苯二甲酸; 通过固液分离除去间苯二甲酸，从而回收母液; 并按照如上所述的步骤（1）至（4）从母液中回收催化剂。

公开(公告)号：US20100016629A1

公开(公告)日：2010-01-21

申请号：US12518662

申请日：2007-12-07

申请人： Fumiya Zaima ,  Masato Inari ,  Hideaki Fujita ,  Nobuo Namiki

发明人： Fumiya Zaima ,  Masato Inari ,  Hideaki Fujita ,  Nobuo Namiki

IPC分类号： C07C51/265

CPC分类号： C07C51/47 ,  B01J45/00 ,  B01J49/50 ,  C07C63/26

摘要： The invention provides a method for producing terephthalic acid, characterized by including subjecting a p-phenylene compound to liquid-phase oxidation reaction by use of a molecular-oxygen-containing gas in the presence of a catalyst at least containing a heavy metal compound and a bromine compound, and hydrous acetic acid having a water content of 1 to 15 mass %, to thereby yield a slurry; regulating the temperature of the slurry to 35 to 140° C., to thereby cause terephthalic acid to precipitate; removing the terephthalic acid through solid-liquid separation, to thereby recover a mother liquor; and recovering the catalyst from the mother liquor through a series of the following steps (1) to (4) for reusing at least a portion of the catalyst in the liquid-phase oxidation reaction: (1) an adsorption step including regulating the ratio “amount by mole of bromide ions in the mother liquor/total amount by mole of heavy metal ions in the mother liquor” to 0.6 to 3, and then exposing the mother liquor to a pyridine-ring-containing chelate resin which has been heated to 35 to 140° C., so that the resin adsorbs catalyst-derived heavy metal ions and bromide ions, and also adsorbs a carboxylic acid mixture which has been by-produced through the liquid-phase oxidation reaction, (2) an elution step (A) of exposing hydrous acetic acid having a water content of 1 to 15 mass % to the pyridine-ring-containing chelate resin which has undergone the adsorption step, thereby yielding an eluate containing the by-produced carboxylic acid mixture, (3) an elution step (B) of exposing water or hydrous acetic acid having a water content of 20 mass % or more to the pyridine-ring-containing chelate resin which has undergone the elution step (A), thereby yielding an eluate containing catalyst-derived heavy metal ions and bromide ions, and (4) a displacement step of exposing hydrous acetic acid having a water content of 1 to 15 mass % to the pyridine-ring-containing chelate resin which has undergone the elution step (B), serving as a displacement liquid, thereby regenerating the resin.

公开(公告)号：US20110213181A1

公开(公告)日：2011-09-01

申请号：US13048644

申请日：2011-03-15

申请人： Fumiya ZAIMA ,  Masato Inari ,  Hideaki Fujita ,  Nobuo Namiki

发明人： Fumiya ZAIMA ,  Masato Inari ,  Hideaki Fujita ,  Nobuo Namiki

IPC分类号： C07C51/255

CPC分类号： C07C51/47 ,  B01J45/00 ,  B01J49/50 ,  C07C63/26

摘要： A method for producing terephthalic acid comprising: subjecting a p-phenylene compound to a liquid-phase oxidation reaction by the use of a molecular-oxygen-containing gas in the presence of a catalyst at least containing a heavy metal compound and a bromine compound, and hydrous acetic acid having a water content of 1 to 15 mass %, to thereby yield a slurry; regulating the temperature of the slurry to 35 to 140° C., to thereby cause terephthalic acid to precipitate; removing the terephthalic acid through solid-liquid separation, to thereby recover a mother liquor; and recovering the catalyst from the mother liquor through a series of operations (1) to (4), as described, for reusing at least a portion of the catalyst in the liquid-phase oxidation reaction.

摘要翻译： 一种对苯二甲酸的制造方法，其特征在于，在至少含有重金属化合物和溴化合物的催化剂的存在下，通过使用含分子氧的气体对对亚苯基化合物进行液相氧化反应， 水含量为1〜15质量％的含水乙酸，得到浆料; 将浆料的温度调节至35至140℃，从而使对苯二甲酸沉淀; 通过固液分离除去对苯二甲酸，从而回收母液; 并通过如上所述的一系列操作（1）至（4）从母液中回收催化剂，用于在液相氧化反应中重新使用至少一部分催化剂。

公开(公告)号：US5880313A

公开(公告)日：1999-03-09

申请号：US139677

申请日：1998-08-25

申请人： Fumiya Zaima ,  Hideaki Fujita ,  Masami Matsumoto ,  Masato Inari

发明人： Fumiya Zaima ,  Hideaki Fujita ,  Masami Matsumoto ,  Masato Inari

IPC分类号： C07C51/265 ,  C07C51/16

CPC分类号： C07C51/265

摘要： A process for continuously producing an aromatic carboxylic acid comprising oxidizing an aromatic compound substituted with alkyl groups with molecular oxygen gas in the liquid phase in a solvent containing a lower aliphatic carboxylic acid in the presence of a catalyst comprising heavy metal compounds and a bromine compound, wherein a mother liquor which is obtained after removal of crystals from a reaction liquid of the liquid phase oxidation and contains heavy metal ions and bromine ion as catalyst components is brought into contact with a chelate resin of an anion exchange type to recover the catalyst components.The catalyst components are efficiently recovered, and auxiliary agents in an amount exceeding the equivalent amount and excessive labor are not necessary.

摘要翻译： 一种连续生产芳族羧酸的方法，包括在含有重金属化合物和溴化合物的催化剂存在下，在含有低级脂肪族羧酸的溶剂中，将在液相中的分子氧气用烷基取代的芳族化合物氧化， 其中将从液相氧化反应液中除去结晶并含有重金属离子和溴离子作为催化剂组分的母液与阴离子交换型螯合树脂接触以回收催化剂组分。 有效地回收催化剂组分，并且不需要超过相当量和过量劳动量的助剂。

公开(公告)号：US08247605B2

公开(公告)日：2012-08-21

申请号：US12374835

申请日：2007-07-19

申请人： Masato Inari ,  Fumiya Zaima

发明人： Masato Inari ,  Fumiya Zaima

IPC分类号： C07C51/42

CPC分类号： C07C51/42 ,  C07C51/43 ,  C07C63/24

摘要： A method of replacing a first dispersion medium in a starting slurry composed of the first dispersion medium and isophthalic acid crystals with a second dispersion medium. The starting slurry is tangentially fed to a vertically extending cylindrical portion of a cyclone-shaped nozzle disposed at an upper portion of a replacement tank of a dispersion medium replacement apparatus, from a tangential direction of the cylindrical portion. The fed starting slurry moves circularly along an inner wall of the cylindrical portion. The slurry circularly moving is then discharged from an opening which is disposed at a vertically lower end of the cylindrical portion and dispersed in a second dispersion medium which is fed from a lower portion of the replacement tank. The replaced slurry composed of isophthalic acid crystals and the second dispersion medium is mainly discharged from the lower portion of the replacement tank, and the first dispersion medium is mainly withdrawn from the upper portion of the replacement tank.

摘要翻译： 将由第一分散介质和间苯二甲酸晶体构成的起始浆料中的第一分散介质用第二分散介质置换的方法。 将起始浆料切向地供给到设置在分散介质置换装置的更换罐的上部处的旋转形喷嘴的垂直延伸的圆柱形部分，该圆筒部分从圆柱形部分的切线方向。 进料的起始浆料沿圆柱形部分的内壁圆周移动。 然后，从设置在圆筒部的垂直下端的开口排出循环移动的浆料，并分散在从更换槽的下部供给的第二分散介质中。 由间苯二甲酸晶体构成的替代浆料和第二分散介质主要从更换槽的下部排出，第一分散介质主要从更换罐的上部排出。

公开(公告)号：US20120328483A1

公开(公告)日：2012-12-27

申请号：US13587449

申请日：2012-08-16

申请人： Masato Inari ,  Fumiya Zaima

发明人： Masato Inari ,  Fumiya Zaima

IPC分类号： B01J19/26

CPC分类号： B01D9/0045 ,  C07C51/42 ,  C07C51/43

摘要： A method of replacing a first dispersion medium, in a starting slurry composed of the first dispersion medium and either terephthalic acid crystals or isophthalic acid crystals, with a second dispersion medium, and apparatus therefore. The starting slurry is tangentially fed to a vertically extending cylindrical portion of a cyclone-shaped nozzle disposed at an upper portion of a replacement tank of a dispersion medium replacement apparatus, from a tangential direction of the cylindrical portion, and moves circularly along an inner wall of the cylindrical portion. The slurry circularly moving is then discharged from an opening which is disposed at a vertically lower end of the cylindrical portion and dispersed in a second dispersion medium which is fed from a lower portion of the replacement tank.

摘要翻译： 因此，在由第一分散介质和对苯二甲酸晶体或间苯二甲酸晶体构成的起始浆料中用第二分散介质代替第一分散介质的方法及装置。 起始浆料切向地供给到设置在分散介质置换装置的替换罐的上部的旋风形喷嘴的垂直延伸的圆柱形部分，从圆柱形部分的切线方向移动，并沿着内壁圆周移动 的圆柱形部分。 然后，从设置在圆筒部的垂直下端的开口排出循环移动的浆料，并分散在从更换槽的下部供给的第二分散介质中。

公开(公告)号：US08247604B2

公开(公告)日：2012-08-21

申请号：US12304415

申请日：2007-06-08

申请人： Masato Inari ,  Fumiya Zaima

发明人： Masato Inari ,  Fumiya Zaima

IPC分类号： C07C51/42

CPC分类号： C07C51/43 ,  B01D9/004 ,  B01D9/0045 ,  C07C51/47 ,  C07C63/26

摘要： A method of replacing a first dispersion medium in a starting slurry composed of the first dispersion medium and a terephthalic acid crystal with a second dispersion medium. The starting slurry is tangentially fed to a vertically extending cylindrical portion of a cyclone-shaped nozzle disposed at an upper portion of a replacement tank of a dispersion medium replacement apparatus, from a tangential direction of the cylindrical portion. The fed starting slurry moves circularly along an inner wall of the cylindrical portion. The slurry circularly moving is then discharged from an opening which is disposed at a vertically lower end of the cylindrical portion and dispersed in a second dispersion medium which is fed from a lower portion of the replacement tank. The replaced slurry composed of the terephthalic acid crystal and the second dispersion medium is mainly discharged from the lower portion of the replacement tank, and the first dispersion medium is mainly withdrawn from the upper portion of the replacement tank.

摘要翻译： 用第二分散介质代替由第一分散介质和对苯二甲酸晶体组成的起始浆料中的第一分散介质的方法。 将起始浆料切向地供给到设置在分散介质置换装置的更换罐的上部处的旋转形喷嘴的垂直延伸的圆柱形部分，该圆筒部分从圆柱形部分的切线方向。 进料的起始浆料沿圆柱形部分的内壁圆周移动。 然后，从设置在圆筒部的垂直下端的开口排出循环移动的浆料，并分散在从更换槽的下部供给的第二分散介质中。 由对苯二甲酸晶体和第二分散介质构成的替换浆料主要从更换槽的下部排出，第一分散介质主要从更换槽的上部排出。

公开(公告)号：US06268528B1

公开(公告)日：2001-07-31

申请号：US09432783

申请日：1999-11-03

申请人： Hiroshi Machida ,  Fumiya Zaima ,  Masato Inari ,  Hiroshi Watanabe ,  Emiko Yokose

发明人： Hiroshi Machida ,  Fumiya Zaima ,  Masato Inari ,  Hiroshi Watanabe ,  Emiko Yokose

IPC分类号： C07C5116

CPC分类号： C07C51/265 ,  C07C63/38

摘要： Dialkylnaphthalene is oxidized to naphthalenedicarboxylic acid in a lower aliphatic carboxylic acid solvent in the presence of a catalyst comprising a cobalt compound, a manganese compound and a bromine compound having an atomic ratio of manganese to cobalt of 0.03 to 0.5. The catalyst is supplied to the oxidation reaction zone so that the total amount of cobalt and manganese is 0.025 to 0.1 gram atom based on 1 gram mol of the dialkylnaphthalene. An oxidation product slurry is subjected to solid-liquid separation when the concentration of the naphthalenedicarboxylic acid in the slurry is 8 to 30% by weight. The process prevents the by-production of benzotricarboxylic acid such as trimellitic acid, thereby drastically reducing the incorporation of heavy metal complexes with trimellitic acid into naphthalenedicarboxylic acid crystals. The process optionally includes the addition of a polymer flocculant, this forming crystal aggregates with a large particle size and facilitating the separation of the crystals from the mother liquor.

摘要翻译： 在包含钴化合物，锰化合物和原子比为锰与钴的溴化合物的催化剂存在下，在低级脂族羧酸溶剂中将二烷基萘氧化成萘二羧酸为0.03〜0.5。 将催化剂供应到氧化反应区，使得钴和锰的总量基于1克摩尔的二烷基萘为0.025至0.1克原子。 当浆料中萘二甲酸的浓度为8〜30重量％时，氧化产物浆液进行固液分离。 该方法防止苯三甲酸如偏苯三酸的副产物，从而大大降低了与偏苯三酸的重金属络合物与萘二甲酸晶体的结合。 该方法任选地包括加入聚合物絮凝剂，这种形成晶体具有大粒径的聚集体并且有利于晶体与母液的分离。