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1. 发明授权

US06262210B1 Process for producing aromatic carbonates 有权
标题翻译：芳香族碳酸酯的制备方法
公开(公告)号：US06262210B1
公开(公告)日：2001-07-17
申请号：US09445982
申请日：1999-12-15
申请人： Masahiro Tojo , Kazuhiro Oonishi , Kyosuke Komiya
发明人： Masahiro Tojo , Kazuhiro Oonishi , Kyosuke Komiya
IPC分类号： C08F12400
CPC分类号： C07C68/06 , C07C69/96
摘要： A process for producing aromatic carbonates, which comprises transesterifying, in the presence of a metal-containing catalyst, a starting material selected from a dialkyl carbonate, an alkyl aryl carbonate and a mixture thereof with a reactant selected from an aromatic monohydroxy compound, an alkyl aryl carbonate and a mixture thereof, characterized in that: at least one type of catalyst-containing liquid is taken out, wherein the catalyst-containing liquid is selected from a portion of a high boiling point reaction mixture obtained by the above transesterification and containing the desired aromatic carbonate and the metal-containing catalyst, and a portion of a liquid catalyst fraction obtained by separating the desired aromatic carbonate from the high boiling point reaction mixture, wherein each portion contains (A) high boiling point substance having a boiling point higher than the boiling point of the produced aromatic carbonate and (B) the metal-containing catalyst; (C) a functional substance capable of reacting with at least one component selected from high boiling point substance (A) and metal-containing catalyst (B) is added to the taken-out catalyst-containing liquid; and the (B)/(C) reaction product is recycled to the reaction system, while withdrawing the (A)/(C) reaction product. By the process of the present invention, the desired aromatic carbonates having high purity can be produced stably for a prolonged period of time.
摘要翻译：一种制备芳族碳酸酯的方法，其包括在含金属的催化剂存在下，将选自碳酸二烷基酯，碳酸烷基芳基酯及其混合物的起始原料与选自芳族单羟基化合物，烷基芳基碳酸酯及其混合物，其特征在于：取出至少一种含催化剂的液体，其中含催化剂的液体选自通过上述酯交换反应获得的高沸点反应混合物的一部分，并含有所需的芳族碳酸酯和含金属的催化剂，以及通过从高沸点反应混合物中分离所需的芳族碳酸酯而得到的液体催化剂馏分的一部分，其中每一部分含有（A）沸点高于所生成的芳族碳酸酯的沸点和（B）含金属的催化剂; （C）能够与选自高沸点物质（A）和含金属催化剂（B）中的至少一种成分反应的功能性物质加入到含有催化剂的液体中; 并且（B）/（C）反应产物在回收（A）/（C）反应产物的同时循环到反应体系中。通过本发明的方法，可以长时间稳定地制备具有高纯度的所需芳族碳酸酯。

2. 发明授权

US5872275A Process for the producing of aromatic carbonate 失效
标题翻译：芳香族碳酸酯的制造方法
公开(公告)号：US5872275A
公开(公告)日：1999-02-16
申请号：US913883
申请日：1997-09-24
申请人： Kyosuke Komiya , Masahiro Tojo , Shinsuke Fukuoka
发明人： Kyosuke Komiya , Masahiro Tojo , Shinsuke Fukuoka
IPC分类号： C07C68/06
CPC分类号： C07C68/06
摘要： Disclosed is a process for producing an aromatic carbonate which comprises transesterifying, in the presence of a metal-containing catalyst, a starting material selected from the group consisting of a dialkyl carbonate, an alkyl aryl carbonate and a mixture thereof with a reactant selected from the group consisting of an aromatic monohydroxy compound, an alkyl aryl carbonate and a mixture thereof, wherein the transesterification is conducted while maintaining a weight ratio (WR) of at least one aromatic group-containing substance selected from the group consisting of a specific aromatic polyhydroxy compound and a residue thereof to the metal of the metal-containing catalyst at 2.0 or less, wherein the weight ratio (WR) is measured with respect to a catalyst-containing liquid-phase mixture in a system for the transesterification, and wherein the aromatic group-containing substance originates from the starting material, the reactant and/or a by-product of the transesterification. According to the process of the present invention, the transesterification reaction can be conducted without suffering disadvantageous phenomena, such as the deposition of the catalyst from the catalyst-containing liquid-phase mixture and the adhesion of the deposited catalyst to the inner walls of the reactor, pipes and the like, so that the desired aromatic carbonate can be produced stably for a prolonged period of time.
摘要翻译： PCT No.PCT / JP96 / 02734 Sec。 371日期：1997年9月24日 102（e）1997年9月24日PCT PCT 1996年9月20日PCT公布。公开号WO97 / 11049 日期1997年3月27日公开是一种生产芳族碳酸酯的方法，其包括在含金属的催化剂存在下，将选自碳酸二烷基酯，碳酸烷基芳基酯及其混合物的起始原料与选自芳族单羟基化合物，碳酸烷基芳基酯及其混合物的反应物，其中进行酯交换反应，同时保持至少一种含芳族基团的物质的重量比（WR），所述至少一种含芳族基团的物质选自特定的芳香族多羟基化合物及其残留物的含金属催化剂的金属为2.0以下，其中，在酯交换反应体系中，相对于含催化剂的液相混合物测定重量比（WR）并且其中所述含芳族基团的物质源自所述起始材料，所述反应物和/或所述酯的副产物通知。根据本发明的方法，可以进行酯交换反应而不会产生不利现象，例如来自含催化剂的液相混合物的催化剂沉积和沉积的催化剂粘附到反应器的内壁，管等，使得所需的芳族碳酸酯可以长时间稳定地制备。

3. 发明授权

US06479689B1 Process for continuously producing dialkyl carbonate and diol 有权
标题翻译：连续生产碳酸二烷基酯和二醇的方法
公开(公告)号：US06479689B1
公开(公告)日：2002-11-12
申请号：US09857980
申请日：2001-06-11
申请人： Masahiro Tojo , Kazuhiro Oonishi
发明人： Masahiro Tojo , Kazuhiro Oonishi
IPC分类号： C07C6996
CPC分类号： C07C41/16 , C07C29/1285 , C07C68/065 , C07C69/96 , C07C43/11 , C07C31/20 , C07C31/202 , C07C31/205 , C07C31/207
摘要： A method for continuously producing a dialkyl carbonate and a diol, comprising: (1) continuously feeding a cyclic carbonate and an aliphatic monohydric alcohol to a continuous multi-stage distillation column, and continuously effecting a transesterification between the cyclic carbonate and the aliphatic monohydric alcohol in the presence of a transesterification catalyst in the distillation column, while continuously withdrawing a low boiling point mixture in a gaseous form containing the produced dialkyl carbonate and the unreacted aliphatic monohydric alcohol from an upper portion of the distillation column and continuously withdrawing a high boiling point mixture in a liquid form containing the produced diol and the unreacted cyclic carbonate from a lower portion of the distillation column, and (2) continuously feeding the high boiling point mixture withdrawn from the lower portion of the distillation column to a continuous etherification reactor, to thereby effect a continuous etherification reaction between the unreacted cyclic carbonate and a part of the produced diol and produce a chain ether and carbon dioxide, while continuously withdrawing the resultant etherification reaction mixture containing the remainder of the diol produced in step (1) and the produced chain ether from the continuous etherification reactor, wherein the etherification reaction mixture has a cyclic carbonate content of from 0 to 10−2 in terms of the weight ratio of the cyclic carbonate to the diol.
摘要翻译：一种连续生产碳酸二烷基酯和二醇的方法，包括：（1）连续地向连续多级蒸馏塔中加入环状碳酸酯和脂肪族一元醇，并连续进行环状碳酸酯与脂肪族一元醇的酯交换反应在蒸馏塔中存在酯交换催化剂的同时，从蒸馏塔的上部连续取出含有生成的碳酸二烷基酯和未反应的脂族一元醇的气态的低沸点混合物，并连续地抽出高沸点含有生成的二醇的液体形式的混合物和来自蒸馏塔下部的未反应的环状碳酸酯，和（2）将从蒸馏塔的下部排出的高沸点混合物连续供给至连续醚化反应器，从而实现连续的等级在未反应的环状碳酸酯和一部分所生成的二醇之间进行裂解反应，并产生链状醚和二氧化碳，同时连续地将所得到的醚化反应混合物从步骤（1）中产生的剩余的二醇和所产生的链乙醚从连续醚化反应器，其中醚化反应混合物的环状碳酸酯含量以环状碳酸酯与二醇的重量比计为0至10-2。

4. 发明授权

US06346638B1 Process for continuous production of dialkyl carbonate and diol 有权
标题翻译：连续生产碳酸二烷基酯和二醇的方法
公开(公告)号：US06346638B1
公开(公告)日：2002-02-12
申请号：US09674769
申请日：2000-11-06
申请人： Masahiro Tojo , Kazuhiro Oonishi
发明人： Masahiro Tojo , Kazuhiro Oonishi
IPC分类号： C07C6806
CPC分类号： C07C29/1285 , C07C68/065 , Y02P20/52 , C07C69/96 , C07C31/202 , C07C31/20
摘要： A method for continuously producing a (A) dialkyl carbonate and a (B) diol, comprising continuously feeding a cyclic carbonate and an aliphatic monohydric alcohol to a continuous multi-stage distillation column to thereby effect a transesterification therebetween, thereby continuously producing a dialkyl carbonate and a diol, while continuously withdrawing a low boiling point mixture containing the produced dialkyl carbonate (A) in a gaseous form from an upper portion of the distillation column and continuously withdrawing a high boiling point mixture containing the produced diol (B) in a liquid form from a lower portion of the distillation column, wherein the transesterification is performed under conditions wherein: (a) the reaction pressure of the column bottom is 5×104 Pa or less; (b) the reaction temperature of the column bottom is in the range of from −20° C. to less than 60° C.; and (c) the distillation column has an F-factor in the range of from 0.2 to 5.0, the F-factor being represented by the following formula (1): F-factor=ug(&rgr;g)½ (1) wherein ug represents the gas velocity (m/s) in the distillation column and &rgr;g represents the gas density (kg/m3) in the distillation column.
摘要翻译：一种连续制备（A）碳酸二烷基酯和（B）二醇的方法，其包括将连续多级蒸馏塔连续供入环状碳酸酯和脂族一元醇，从而在其间进行酯交换，从而连续制备碳酸二烷基酯和二醇，同时从蒸馏塔的上部连续取出含有生成的碳酸二烷基碳酸酯（A）的低沸点混合物，并连续地将含有生成的二醇（B）的高沸点混合物在液体形成从蒸馏塔的下部，其中酯交换反应在以下条件下进行：（a）柱底的反应压力为5×10 4 Pa以下; （b）塔底的反应温度在-20℃至小于60℃的范围内; 和（c）蒸馏塔的F因子范围为0.2-5.0，F因子由下式（1）表示：其中ug代表蒸馏塔中的气体速度（m / s） rhog表示蒸馏塔中的气体密度（kg / m3）。

5. 发明授权

US06472525B1 Hexaazaisowurtzitane derivative and method for producing the same 失效
标题翻译：六氮杂异纤锌矿型结构烷烃衍生物及其制造方法
公开(公告)号：US06472525B1
公开(公告)日：2002-10-29
申请号：US08737094
申请日：1997-05-16
申请人： Tamotsu Kodama , Masahiro Tojo , Masanori Ikeda
发明人： Tamotsu Kodama , Masahiro Tojo , Masanori Ikeda
IPC分类号： C07D25900
CPC分类号： C07D487/18 , C07D487/22
摘要： Disclosed is an acyl group-containing hexaazaisowurtzitane derivative represented by the following formula (I): W At Q(6−t), wherein t represents an integer of from 4 to 6, A independently represents an acyl group having 1 to 10 carbon atoms, each Q independently represents a hydrogen atom or an alkyl group having 1 to 10 carbon atoms, and W represents a hexavalent hexaazaisowurtzitane residue represented by the following formula (II): Also disclosed is a method for producing the above-mentioned acyl group-containing hexaazaisowurtzitane derivative. The acyl group-containing hexaazaisowurtzitane derivative of the present invention is useful as a precursor of a polynitrohexaazaisowurtzitane derivative which can be used not only as a material for explosives but also as an additive for propellants and explosives. The acyl group-containing hexaazaisowurtzitane derivative of the present invention is also useful as a raw material for producing a highly polar polymer, and as a polyfunctional crosslinking agent and an additive for polymers.
摘要翻译：公开了下式（I）表示的含酰基的六氮杂异纤锌矿型结构烷烃衍生物：W在Q（6-t）中，t表示4〜6的整数，A独立地表示碳原子数1〜10的酰基，各Q独立地表示氢原子或碳原子数1〜10的烷基，W表示由下式（II）表示的六价六氮杂异纤锌矿型结构烷烃残基：还公开了上述含酰基的六氮杂异纤锌矿型结构烷烃衍生物。本发明的含酰基的六氮杂异纤锌矿型结构烷烃衍生物可用作多硝基六氮杂异纤锌矿型结构烷烃衍生物的前体，其不仅可用作爆炸物质，而且可用作推进剂和爆炸物的添加剂。本发明的含酰基六氮杂异纤锌矿型结构烷烃衍生物也可用作高极性聚合物的生产原料，多官能交联剂和聚合物添加剂。

6. 发明授权

US07645896B2 Method for producing a dialkyl carbonate and a diol 有权
标题翻译：碳酸二烷基酯和二醇的制造方法
公开(公告)号：US07645896B2
公开(公告)日：2010-01-12
申请号：US10594671
申请日：2005-06-17
申请人： Masahiro Tojo , Hironori Miyaji
发明人： Masahiro Tojo , Hironori Miyaji
IPC分类号： C07C69/96
CPC分类号： C07C29/128 , C07C68/065 , C07C69/96 , C07C31/202
摘要： A method for producing a dialkyl carbonate and a diol, comprising: (a) effecting a transesterification reaction between a cyclic carbonate and an aliphatic monohydric alcohol in the presence of a transesterification catalyst, thereby obtaining a reaction mixture containing a product dialkyl carbonate and a product diol, (b) withdrawing a dialkyl carbonate-containing liquid from the reaction mixture, followed by separation of the dialkyl carbonate from the dialkyl carbonate-containing liquid, and (c) withdrawing a diol-containing liquid from the reaction mixture, followed by separation of the diol from the diol-containing liquid, wherein the cyclic carbonate contains a cyclic ether in an amount of from 0.1 to 3,000 ppm by weight, and the product dialkyl carbonate contains a carbonate ether of not more than 10,000 ppm by weight.
摘要翻译：一种碳酸二烷基酯和二醇的制造方法，包括：（a）在酯交换催化剂的存在下进行环状碳酸酯与脂肪族一元醇的酯交换反应，得到含有碳酸二烷基酯和产物的反应混合物二醇，（b）从反应混合物中取出含二烷基碳酸酯的液体，然后从含碳酸二烷基酯的液体中分离碳酸二烷基酯，和（c）从反应混合物中取出含二醇的液体，然后分离的二醇，其中所述环状碳酸酯含有0.1至3,000重量ppm的环醚，并且所述产物中的碳酸二烷基酯含有不大于10,000ppm重量的碳酸酯醚。

7. 发明申请

US20100076213A1 METHOD FOR PRODUCING A DIALKYL CARBONATE AND A DIOL 有权
标题翻译：碳酸二乙酯和二醇的生产方法
公开(公告)号：US20100076213A1
公开(公告)日：2010-03-25
申请号：US12626444
申请日：2009-11-25
申请人： Masahiro Tojo , Hironori Miyaji
发明人： Masahiro Tojo , Hironori Miyaji
IPC分类号： C07C69/96
CPC分类号： C07C29/128 , C07C68/065 , C07C69/96 , C07C31/202
摘要： A method for producing a dialkyl carbonate and a diol, comprising: (a) effecting a transesterification reaction between a cyclic carbonate and an aliphatic monohydric alcohol in the presence of a transesterification catalyst, thereby obtaining a reaction mixture containing a product dialkyl carbonate and a product diol, (b) withdrawing a dialkyl carbonate-containing liquid from the reaction mixture, followed by separation of the dialkyl carbonate from the dialkyl carbonate-containing liquid, and (c) withdrawing a diol-containing liquid from the reaction mixture, followed by separation of the diol from the diol-containing liquid, wherein the cyclic carbonate contains a cyclic ether in an amount of from 0.1 to 3,000 ppm by weight, and the product dialkyl carbonate contains a carbonate ether of not more than 10,000 ppm by weight.
摘要翻译：一种碳酸二烷基酯和二醇的制造方法，包括：（a）在酯交换催化剂的存在下进行环状碳酸酯与脂肪族一元醇的酯交换反应，得到含有碳酸二烷基酯和产物的反应混合物二醇，（b）从反应混合物中取出含二烷基碳酸酯的液体，然后从含碳酸二烷基酯的液体中分离碳酸二烷基酯，和（c）从反应混合物中取出含二醇的液体，然后分离的二醇，其中所述环状碳酸酯含有0.1至3,000重量ppm的环醚，并且所述产物中的碳酸二烷基酯含有不大于10,000ppm重量的碳酸酯醚。

8. 发明授权

US5847189A Method for continuously producing a dialkyl carbonate and a diol 失效
标题翻译：连续生产碳酸二烷基酯和二醇的方法
公开(公告)号：US5847189A
公开(公告)日：1998-12-08
申请号：US930700
申请日：1997-10-16
申请人： Masahiro Tojo , Shinsuke Fukuoka , Mamoru Kawamura
发明人： Masahiro Tojo , Shinsuke Fukuoka , Mamoru Kawamura
IPC分类号： C07C29/128 , C07C68/06
CPC分类号： C07C29/128 , C07C68/065
摘要： Disclosed is a method for continuously producing a dialkyl carbonate and a diol, comprising: (1) feeding a cyclic carbonate and an aliphatic monohydric alcohol to a continuous multi-stage distillation column, and effecting a transesterification in the presence of a catalyst in the multi-stage distillation column and/or at least one transesterification reactor which communicates fluid-tightly with the distillation column, while continuously withdrawing a low boiling point gaseous mixture containing the produced dialkyl carbonate from a upper portion of the distillation column and a high boiling point liquid mixture from a lower portion of the distillation column; and (2) continuously feeding water and the high boiling point mixture to a hydrolysis reactor, to thereby effect a continuous hydrolysis of the unreacted cyclic carbonate contained therein and produce a diol and carbon dioxide. By the method of the present invention, it becomes possible to produce a dialkyl carbonate and a high purity diol, with high productivity, even when the feedstock aliphatic monohydric alcohol contains a concomitant dialkyl carbonate.
摘要翻译： PCT No.PCT / JP96 / 03746 Sec。 371日期：1997年10月16日 102（e）日期1997年10月16日PCT 1996年12月20日PCT公布。公开号WO97 / 23445 日期1997年7月3日公开是一种连续生产碳酸二烷基酯和二醇的方法，包括：（1）向连续多级蒸馏塔中加入环状碳酸酯和脂肪族一元醇，并进行酯交换反应多级蒸馏塔中的催化剂和/或至少一种与蒸馏塔流体紧密连通的酯交换反应器，同时从蒸馏塔的上部连续抽出含有生成的碳酸二烷基碳酸酯的低沸点气态混合物，来自蒸馏塔下部的高沸点液体混合物; 和（2）将水和高沸点混合物连续供给到水解反应器中，从而使其中所含的未反应的环状碳酸酯的连续水解产生二醇和二氧化碳。通过本发明的方法，即使当原料脂族一元醇含有伴随的碳酸二烷基酯时，也可以以高生产率制备碳酸二烷基酯和高纯度二醇。

9. 发明授权

US5210268A Process for continuously producing an aromatic carbonate 失效
标题翻译：连续生产芳香碳酸盐的工艺
公开(公告)号：US5210268A
公开(公告)日：1993-05-11
申请号：US688588
申请日：1991-06-28
申请人： Shinsuke Fukuoka , Masahiro Tojo , Mamoru Kawamura
发明人： Shinsuke Fukuoka , Masahiro Tojo , Mamoru Kawamura
IPC分类号： C07C69/96 , B01D3/34 , C07C68/06
CPC分类号： C07C68/06
摘要： Disclosed is a process for producing an aromatic carbonate or aromatic carbonate mixture by a transesterification reaction between a starting material selected from a dialkyl carbonate, an alkyl aryl carbonate and a mixture thereof and a reactant selected from an aromatic hydroxy compound, an alkyl aryl carbonate and a mixture thereof, wherein the starting material and the reactant are continuously fed to a continuous multi-stage distillation column to effect a transesterification reaction therebetween in the presence of a catalyst in the distillation column, while continuously withdrawing the produced aromatic carbonate or aromatic carbonate mixture as a high boiling point product in a liquid form from a lower portion of the distillation column and continuously withdrawing the by-product as a low boiling point product in a gaseous form from an upper portion of the distillation column by distillation, thereby enabling the aromatic carbonate or aromatic carbonate mixture to be produced continuously. By the method of the present invention, an aromatic carbonate, which is useful as a material for the production of aromatic polycarbonates without using poisonous phosgene or as a material for the production of various isocyanates without using poisonous phosgene, can be produced not only at a high reaction rate but also in a high yield with a high selectivity.
摘要翻译： PCT No.PCT / JP90 / 01734 Sec。 371日期1991年6月28日 102（e）日期1991年6月28日PCT提交1990年12月28日PCT公布。出版物WO91 / 09832 日期：1991年7月11日。公开是通过在碳酸二烷基酯，碳酸烷基芳基酯和其混合物中选择的起始材料之间的酯交换反应和选自芳族羟基化合物，碳酸烷基芳基酯及其混合物，其中将起始原料和反应物连续加入到连续多级蒸馏塔中以在催化剂存在下在蒸馏塔中进行酯交换反应，同时连续地取出从蒸馏塔的下部产生作为液体形式的高沸点产物的芳族碳酸酯或芳族碳酸酯混合物，并从蒸馏塔的上部连续抽出作为气态形式的低沸点产物的副产物通过蒸馏，从而使芳族碳酸酯或芳族碳酸酯混合不断生产。通过本发明的方法，可以生产芳香族碳酸酯，其可用作不使用有毒光气制备芳族聚碳酸酯的材料或用于生产不使用有毒光气的各种异氰酸酯的材料，不仅在反应速度高，而且产率高，选择性高。

10. 发明授权

US5166393A Process for producing diaryl carbonate 失效
标题翻译：生产碳酸二芳酯的方法
公开(公告)号：US5166393A
公开(公告)日：1992-11-24
申请号：US771538
申请日：1991-10-07
申请人： Shinsuke Fukuoka , Ryoji Deguchi , Masahiro Tojo
发明人： Shinsuke Fukuoka , Ryoji Deguchi , Masahiro Tojo
IPC分类号： C07C68/06
CPC分类号： C07C68/06
摘要： A process for producing a diaryl carbonate in high yield and with high selectivity which comprises disproportionating an alkylaryl carbonate in the presence of a lead catalyst to produce a diaryl carbonate and a dialkyl carbonate and recovering the diaryl carbonate from the reaction products. Use of the lead catalyst is effective in avoiding corrosion problems normally caused by other catalyst systems.
摘要翻译：一种以高产率和高选择性制备碳酸二芳基酯的方法，包括在铅催化剂存在下歧化碳酸烷基芳基酯以制备碳酸二芳基酯和碳酸二烷基酯，并从反应产物中回收碳酸二芳基酯。使用铅催化剂有效地避免了通常由其他催化剂体系引起的腐蚀问题。

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