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61. 发明申请

US20070260084A1 Industrial Process for Production of High-Purity Diaryl Carbonate 审中-公开
公开(公告)号：US20070260084A1
公开(公告)日：2007-11-08
申请号：US11661611
申请日：2005-10-17
申请人： Shinsuke Fukuoka , Hironori Miyaji , Hiroshi Hachiya , Kazuhiko Matsuzaki
发明人： Shinsuke Fukuoka , Hironori Miyaji , Hiroshi Hachiya , Kazuhiko Matsuzaki
IPC分类号： C07C69/96 , B01D3/14 , C07C68/08
CPC分类号： B01D3/146 , B01D3/009 , C07C68/06 , C07C68/065 , C07C68/08 , C08G64/307 , Y02P20/127 , Y02P20/582 , C07C69/96
摘要： It is an object of the present invention to provide a specific process that enables a high-purity diaryl carbonate that can be used as a raw material of a high-quality and high-performance polycarbonate to be produced stably for a prolonged period of time on an industrial scale of not less than 1 ton/hr using as a starting material a reaction mixture containing an alkyl aryl carbonate obtained through a transesterification reaction between a dialkyl carbonate and an aromatic monohydroxy compound. Although there have been various proposals regarding processes for the production of reaction mixtures containing aromatic carbonates by means of a reactive distillation method or the like, these have all been on a small scale and short operating time laboratory level, and there have been no disclosures on a specific process or apparatus enabling mass production on an industrial scale from such a reaction mixture of a high-purity diaryl carbonate that can be used as a raw material of a high-quality and high-performance polycarbonate. According to the present invention, there is provided a specific process that enables a high-purity diaryl carbonate substantially not containing intermediate boiling point by-products or high boiling point by-products and important as a raw material of a high-quality and high-performance polycarbonate to be produced stably for a prolonged period of time on an industrial scale of not less than 1 ton/hr by taking as a starting material a reaction mixture containing an alkyl aryl carbonate that has been obtained through a transesterification reaction between a dialkyl carbonate and an aromatic monohydroxy compound and subjecting this starting material to a transesterification reaction using a reactive distillation column, and then subjecting a high boiling point reaction mixture obtained from the bottom of the reactive distillation column to separation/purification by distillation using a high boiling point material separating column A, a diaryl carbonate purifying column B and an intermediate boiling point material separating column C in this order, wherein each of these three columns comprises a specified continuous multi-stage distillation column, the high-purity diaryl carbonate being obtained as a side cut component from said purifying column B.

62. 发明申请

US20070219387A1 Industrial Process for Producing an Aromatic Carbonate 审中-公开
标题翻译：生产芳香族碳酸酯的工业方法
公开(公告)号：US20070219387A1
公开(公告)日：2007-09-20
申请号：US11631862
申请日：2005-07-11
申请人： Shinsuke Fukuoka , Hiroshi Hachiya , Kazuhiko Matsuzaki
发明人： Shinsuke Fukuoka , Hiroshi Hachiya , Kazuhiko Matsuzaki
IPC分类号： C07C69/96
CPC分类号： B01D3/146 , C07C68/06 , C07C68/08 , Y02P20/127 , C07C69/96
摘要： It is an object of the present invention to provide, for the case of continuously producing aromatic carbonates containing a diaryl carbonate as a main product by taking an alkyl aryl carbonate containing specific amounts of a dialkyl carbonate and an aromatic monohydroxy compound as a starting material, in which said alkyl aryl carbonate is obtainable through a transesterification reaction between a dialkyl carbonate and an aromatic monohydroxy compound, using a continuous multi-stage distillation column in which a catalyst is present, and continuously feeding the starting material into the continuous multi-stage distillation column, a specific process that enables the diaryl carbonate to be produced with high selectivity and high productivity stably for a prolonged period of time on an industrial scale of not less than 1 ton per hour. Although there have been various proposals regarding processes for the production of aromatic carbonates by means of a reactive distillation method, these have all been on a small scale and short operating time laboratory level, and there have been no disclosures whatsoever on a specific process or apparatus enabling mass production on an industrial scale. According to the present invention, there is provided a specified continuous multi-stage distillation column, and there is also provided a specific process that enables a diaryl carbonate to be produced with high selectivity and high productivity stably for a prolonged period of time on an industrial scale of not less than 1 ton per hour from an alkyl aryl carbonate containing specific amounts of the dialkyl carbonate and the aromatic monohydroxy compound.
摘要翻译：本发明的目的是提供以含碳酸二烷基酯和芳族单羟基化合物作为起始原料的碳酸烷基芳基酯连续制备含有碳酸二芳基酯作为主要成分的芳族碳酸酯的情况，其中所述烷基芳基碳酸酯可通过碳酸二烷基酯和芳族单羟基化合物之间的酯交换反应获得，使用其中存在催化剂的连续多级蒸馏塔，并将原料连续进料到连续多级蒸馏柱，其特征在于能够以不低于1吨/小时的工业规模长时间稳定地以高选择性和高生产率生产碳酸二芳基酯。尽管通过反应性蒸馏法已经有关于生产芳族碳酸酯的方法的各种建议，但这些都是在小规模和短的操作时间实验室水平上，并且在具体方法或装置上没有公开任何内容实现工业规模的批量生产。根据本发明，提供了一种特定的连续多级蒸馏塔，并且还提供了一种能够在工业上长时间稳定地以高选择性和高生产率制备碳酸二芳基酯的具体方法含有特定量的碳酸二烷基酯和芳族单羟基化合物的碳酸烷基芳基酯不小于1吨/小时。

63. 发明授权

US07658817B2 Industrial evaporation apparatus 有权
标题翻译：工业蒸发装置
公开(公告)号：US07658817B2
公开(公告)日：2010-02-09
申请号：US11666464
申请日：2005-11-29
申请人： Shinsuke Fukuoka , Hiroshi Hachiya , Kazuhiko Matsuzaki
发明人： Shinsuke Fukuoka , Hiroshi Hachiya , Kazuhiko Matsuzaki
IPC分类号： B01D1/00 , B01D1/30
CPC分类号： B01D1/22 , C08G63/785 , C08G63/90 , C08G64/205 , C08G64/406 , Y10S159/37
摘要： An industrial evaporation apparatus having a specified structure in which there are guides that do not themselves have a heat source, a flow path controlling member having a function of making the liquid fed onto a perforated plate from a liquid receiving port flow mainly from a peripheral portion toward a central portion of the perforated plate is provided in a liquid feeding zone, and formula (1) to (5), or formula (1) to (10), or formula (1) to (12), are satisfied.
摘要翻译：具有特定结构的工业蒸发装置，其中存在不具有热源的导向件，具有使从液体接收口供给到多孔板上的液体主要从周边部分流出的功能的流路控制构件设置在供液区域中，并且满足公式（1）至（5）或式（1）至（10）或式（1）至（12）。

64. 发明申请

US20090326257A1 Process for industrially producing dialkyl carbonate and diol 审中-公开
标题翻译：工业生产碳酸二烷基酯和二醇的方法
公开(公告)号：US20090326257A1
公开(公告)日：2009-12-31
申请号：US11991251
申请日：2006-11-30
申请人： Shinsuke Fukuoka , Hironori MIyaji , Hiroshi Hachiya , Kazuhiko Matsuzaki
发明人： Shinsuke Fukuoka , Hironori MIyaji , Hiroshi Hachiya , Kazuhiko Matsuzaki
IPC分类号： C07C69/96 , C07C31/18 , B01D3/14
CPC分类号： C07C68/065 , B01D3/009 , B01D3/143 , B01D3/32 , Y02P20/127 , C07C69/96
摘要： It is an object of the present invention to provide a specific process that enables dialkyl carbonates and diols to be produced on an industrial scale of not less than 2 ton/hr and not less than 1.3 ton/hr respectively with high selectivity and high productivity stably for a prolonged period of time through a reactive distillation system of taking cyclic carbonates and aliphatic monohydric alcohols as starting materials, continuously feeding the starting materials into a continuous multi-stage distillation column in which a catalyst is present, and carrying out reaction and distillation simultaneously in the column. Although there have been many proposals regarding processes for the production of the dialkyl carbonates and the diols through a reactive distillation method, these have all been on a small scale and short operating time laboratory level, and there have been no disclosures whatsoever on a specific process or apparatus enabling mass production on an industrial scale. According to the present invention, there are provided a specific continuous multi-stage distillation column having a specified structure, and a production process using this continuous multi-stage distillation column, in which the dialkyl carbonates and the diols can be produced on an industrial scale of not less than 2 ton/hr and not less than 1.3 ton/hr respectively each with a selectivity of not less than 95%, preferably not less than 97%, more preferably not less than 99%, with a high yield stably for not less than 1000 hours, preferably not less than 3000 hours, more preferably not less than 5000 hours.
摘要翻译：本发明的目的是提供能够以高选择性和高生产率稳定地以不低于2吨/小时且不低于1.3吨/小时的工业规模生产碳酸二烷基酯和二醇的具体方法通过将环状碳酸酯和脂肪族一元醇作为起始原料的反应性蒸馏系统延长一段时间，将原料连续供给到其中存在催化剂的连续多级蒸馏塔中，同时进行反应和蒸馏在列中。虽然通过反应性蒸馏法生产碳酸二烷基酯和二醇的方法有许多建议，但这些都是在小规模和操作时间短的实验室水平上，并没有公开任何关于具体方法或能够在工业规模上批量生产的设备。根据本发明，提供了具有特定结构的特定连续多级蒸馏塔和使用该连续多级蒸馏塔的生产方法，其中可以以工业规模生产碳酸二烷基酯和二醇不低于2吨/小时，不低于1.3吨/小时，选择性不低于95％，优选不低于97％，更优选不低于99％，稳定性高，不高于99％小于1000小时，优选不小于3000小时，更优选不小于5000小时。

65. 发明申请

US20090287014A1 PROCESS FOR PRODUCTION OF HIGH-PURITY DIARYL CARBONATE 有权
标题翻译：生产高纯度二氧化碳的方法
公开(公告)号：US20090287014A1
公开(公告)日：2009-11-19
申请号：US12508331
申请日：2009-07-23
申请人： Shinsuke FUKUOKA , Hironori Miyaji , Hiroshi Hachiya , Kazuhiko Matsuzaki
发明人： Shinsuke FUKUOKA , Hironori Miyaji , Hiroshi Hachiya , Kazuhiko Matsuzaki
IPC分类号： C07C69/76
CPC分类号： C08G64/307 , B01D3/009 , B01D3/146 , C07C68/06 , C07C68/08 , Y02P20/127 , Y02P20/582 , C07C69/96
摘要： An aromatic polycarbonate that is obtained by transesterification between a high-purity diphenyl carbonate and an aromatic dihydroxy compound. A specific industrially useful process for the production of a high-purity diaryl carbonate in which a diaryl carbonate having low contents of intermediate boiling point and high boiling point impurities is produced is disclosed. As a starting material, a reaction mixture containing an alkyl aryl carbonate obtained through a transesterification reaction between a dialkyl carbonate and an aromatic monohydroxy compound is used. The process in which separation by distillation is carried out uses three distillation columns in a specified order. Moreover, it is particularly preferable if a reactive distillation column and the three distillation columns, each of which has a specified structure, and the three distillation columns are each operated under specified distillation conditions.
摘要翻译：通过高纯度碳酸二苯酯和芳族二羟基化合物之间的酯交换获得的芳族聚碳酸酯。公开了一种生产具有低中值沸点和高沸点杂质含量的碳酸二芳基酯的高纯度碳酸二芳酯的具体的工业上有用的方法。作为起始原料，使用含有通过碳酸二烷基酯和芳族单羟基化合物之间的酯交换反应获得的碳酸烷基芳基酯的反应混合物。通过蒸馏进行分离的方法使用三个蒸馏塔以指定的顺序。此外，特别优选的是，反应性蒸馏塔和具有特定结构的三个蒸馏塔和三个蒸馏塔各自在规定的蒸馏条件下运行。

66. 发明申请

US20090156865A1 Industrial process for production of high-purity diol 有权
公开(公告)号：US20090156865A1
公开(公告)日：2009-06-18
申请号：US11991292
申请日：2006-12-28
申请人： Shinsuke Fukuoka , Hironori Miyaji , Hiroshi Hachiya , Kazuhiko Matsuzaki
发明人： Shinsuke Fukuoka , Hironori Miyaji , Hiroshi Hachiya , Kazuhiko Matsuzaki
IPC分类号： B01D3/22 , C07C31/20 , B01D3/34 , B01D3/14
CPC分类号： C07C29/80 , B01D3/008 , B01D3/009 , B01D3/20 , B01D3/22 , B01D3/32 , C07C29/128 , C07C68/065 , Y02P20/127 , C07C69/96 , C07C31/202
摘要： It is an object of the present invention to provide a specific apparatus and process for producing a high-purity diol by taking a cyclic carbonate and an aliphatic monohydric alcohol as starting materials, continuously feeding the starting materials into a continuous multi-stage distillation column A in which a catalyst is present, carrying out reactive distillation in the column A, continuously withdrawing a low boiling point reaction mixture AT containing a produced dialkyl carbonate and the aliphatic monohydric alcohol from an upper portion of the column A in a gaseous form, continuously withdrawing a high boiling point reaction mixture AB containing a produced diol from a lower portion of the column A in a liquid form, continuously feeding the high boiling point reaction mixture AB into a continuous multi-stage distillation column C, distilling off material having a lower boiling point than that of the diol contained in the high boiling point reaction mixture AB as a column top component CT and/or a side cut component CS so as to obtain a column bottom component CB, continuously feeding the column bottom component CB into a continuous multi-stage distillation column E, and obtaining the diol as a side cut component ES from a side cut outlet of the continuous multi-stage distillation column E. Moreover, it is an object to thus provide a specific industrial apparatus and industrial production process that are inexpensive and, for example, enable the high-purity diol to be produced in an amount of not less than 1 ton/hr stably for a prolonged period of time (e.g. not less than 1000 hours, preferably not less than 3000 hours, more preferably not less than 5000 hours). The above objects can be attained by using a continuous multi-stage distillation column E having a specified structure, and withdrawing a liquid component from the side cut outlet, which is installed at the bottom of a chimney tray having a specified structure installed in an enrichment section of the continuous multi-stage distillation column E.

67. 发明申请

US20090156853A1 Process for industrially producing dialkyl carbonate and diol 审中-公开
标题翻译：工业生产碳酸二烷基酯和二醇的方法
公开(公告)号：US20090156853A1
公开(公告)日：2009-06-18
申请号：US11991250
申请日：2006-12-06
申请人： Shinsuke Fukuoka , Hironori Miyaji , Hiroshi Hachiya , Kazuhiko Matsuzaki
发明人： Shinsuke Fukuoka , Hironori Miyaji , Hiroshi Hachiya , Kazuhiko Matsuzaki
IPC分类号： C07C68/06
CPC分类号： B01D3/009 , B01D3/32 , C07C68/065 , Y02P20/127 , C07C69/96
摘要： It is an object of the present invention to provide a specific process that enables a dialkyl carbonate and a diol to be produced on an industrial scale of not less than 2 ton/hr and not less than 1.3 ton/hr respectively with high selectivity and high productivity stably for a prolonged period of time through a reactive distillation system of taking a cyclic carbonate and an aliphatic monohydric alcohol as starting materials, continuously feeding the starting materials into a continuous multi-stage distillation column in which a catalyst is present, and carrying out reaction and distillation simultaneously in the column. Although there have been many proposals regarding processes for the production of the dialkyl carbonate and the diol through the reactive distillation method, these have all been on a small scale and short operating time laboratory level, and there have been no disclosures whatsoever on a specific process or apparatus enabling mass production on an industrial scale. According to the present invention, there is provided a production process using the continuous multi-stage distillation column having a specified structure that enables the dialkyl carbonate and the diol to be produced on an industrial scale of not less than 2 ton/hr and not less than 1.3 ton/hr respectively each with a high selectivity of not less than 95%, preferably not less than 97%, more preferably not less than 99%, stably for not less than 1000 hours, preferably not less than 3000 hours, more preferably not less than 5000 hours, wherein the starting materials are introduced into specified stages of the distillation column, and the starting material aliphatic monohydric alcohol has a specified composition. As a result, the above object can be attained easily.
摘要翻译：本发明的目的是提供一种能够以不低于2吨/小时并且不低于1.3吨/小时的工业规模生产碳酸二烷基酯和二醇的具有高选择性和高的特定方法通过以环状碳酸酯和脂肪族一元醇为起始原料的反应蒸馏系统，稳定地长时间稳定生产，将原料连续供给到存在催化剂的连续多级蒸馏塔中，并进行在柱中同时进行反应和蒸馏。虽然通过反应蒸馏法生产碳酸二烷基酯和二醇的方法有许多提案，但这些都是在规模小，操作时间短的实验室水平上，并没有公开任何关于具体方法或能够在工业规模上批量生产的设备。根据本发明，提供一种使用具有规定结构的连续多级蒸馏塔的制造方法，其能够以不低于2吨/小时的工业规模生产碳酸二烷基酯和二醇分别为不低于1000小时，优选不小于3000小时，更优选为不低于95％，优选不低于97％，更优选不低于99％的高选择性，优选为1.3吨/小时不少于5000小时，其中将原料引入蒸馏塔的特定阶段，原料脂族一元醇具有特定的组成。结果，可以容易地实现上述目的。

68. 发明申请

US20090156759A1 Industrial process for production of high-quality aromatic polycarbonate 审中-公开
标题翻译：工业生产高品质芳纶聚碳酸酯的工艺
公开(公告)号：US20090156759A1
公开(公告)日：2009-06-18
申请号：US11991420
申请日：2006-11-22
申请人： Shinsuke Fukuoka , Hironori Miyaji , Hiroshi Hachiya , Kazuhiko Matsuzaki
发明人： Shinsuke Fukuoka , Hironori Miyaji , Hiroshi Hachiya , Kazuhiko Matsuzaki
IPC分类号： C08F2/01
CPC分类号： C07C68/06 , B01D3/009 , C08G64/307 , Y02P20/127 , C07C69/96
摘要： It is an object of the present invention to provide a specific process that enables a high-quality high-performance aromatic polycarbonate having excellent mechanical properties and no discoloration to be produced industrially in a large amount (e.g. not less than 1 ton/hr) stably for a prolonged period of time (e.g. not less than 1000 hours, preferably not less than 3000 hours, more preferably not less than 5000 hours) from a dialkyl carbonate and an aromatic dihydroxy compound. When producing the aromatic polycarbonate from the dialkyl carbonate and the aromatic dihydroxy compound, the above object can be attained by carrying out a process of the present invention which comprises the step of; (I) producing a diaryl carbonate using two reactive distillation columns each having a specified structure: (II) purifying the diaryl carbonate so as to obtain a high-purity diaryl carbonate: (III) subsequently producing an aromatic polycarbonate using a guide-contacting downflow type polymerization apparatus having a specified structure from a molten prepolymer obtained from an aromatic dihydroxy compound and the high-purity diaryl carbonate: and (IV) recycling by-produced aromatic monohydroxy compound into the step (I).
摘要翻译：本发明的目的是提供一种能够在工业上大量（例如不低于1吨/小时）稳定地产生具有优异的机械性能和无变色的高品质高性能芳族聚碳酸酯的具体方法从碳酸二烷基酯和芳族二羟基化合物的长时间（例如不小于1000小时，优选不小于3000小时，更优选不小于5000小时）。当从碳酸二烷基酯和芳族二羟基化合物制备芳族聚碳酸酯时，可以通过进行本发明的方法来实现上述目的，该方法包括以下步骤：（I）使用两个具有特定结构的反应性蒸馏塔制备碳酸二芳基酯：（II）纯化碳酸二芳基酯以获得高纯度碳酸二芳基酯;（III）随后使用引导接触下流产生芳族聚碳酸酯由芳族二羟基化合物和高纯度碳酸二芳基酯得到的熔融预聚物具有特定结构的聚合装置和（Ⅳ）将副产的芳族一羟基化合物再循环到工序（I）中。

69. 发明申请

US20090105494A1 Industrial process for production of dialkyl carbonate and diol 审中-公开
公开(公告)号：US20090105494A1
公开(公告)日：2009-04-23
申请号：US11991371
申请日：2006-12-20
申请人： Shinsuke Fukuoka , Hironori Miyaji , Hiroshi Hachiya , Kazuhiko Matsuzaki
发明人： Shinsuke Fukuoka , Hironori Miyaji , Hiroshi Hachiya , Kazuhiko Matsuzaki
IPC分类号： C07C68/08
CPC分类号： B01D3/009 , B01D3/32 , C07C68/065 , C07C68/08 , Y02P20/127 , Y02P20/582 , C07C69/96
摘要： It is an object of the present invention, when producing a dialkyl carbonate and a diol industrially in a large amount (e.g. not less than 2 ton/hr for the dialkyl carbonate and not less than 1.3 ton/hr for the diol) through a reactive distillation system of taking a cyclic carbonate and an aliphatic monohydric alcohol as starting materials, continuously feeding the starting materials into a continuous multi-stage distillation column in which a catalyst is present, and carrying out reaction and distillation simultaneously in the column, is to provide a specific process that enables the dialkyl carbonate and the diol to be produced each with high selectivity and high productivity stably for a prolonged period of time (e.g. not less than 1000 hours, preferably not less than 3000 hours, more preferably not less than 5000 hours), and moreover enables the dialkyl carbonate produced to be separated out and purified stably for a prolonged period of time with high efficiency. It has been discovered that by carrying out reactive distillation using a continuous multi-stage distillation column A having a specified structure, and subjecting a column top component AT thus obtained to separation by distillation using a continuous multi-stage distillation column B having a specified structure, a dialkyl carbonate of high purity (e.g. not less than 97%, preferably not less than 99%, more preferably not less than 99.9%, yet more preferably not less than 99.99%) and a diol can be produced each with a high selectivity of not less than 95%, preferably not less than 97%, more preferably not less than 99%, on an industrial scale of not less than 2 ton/hr, preferably not less than 3 ton/hr, more preferably not less than 4 ton/hr, for the dialkyl carbonate, and not less than 1.3 ton/hr, preferably not less than 1.95 ton/hr, more preferably not less than 2.6 ton/hr, for the diol, with a high yield stably for a prolonged period of time of not less than 1000 hours, preferably not less than 3000 hours, more preferably not less than 5000 hours, from a cyclic carbonate and an aliphatic monohydric alcohol.

70. 发明申请

US20090054676A1 Industrial process for separating out dialkyl carbonate 有权
公开(公告)号：US20090054676A1
公开(公告)日：2009-02-26
申请号：US11991073
申请日：2006-12-15
申请人： Shinsuke Fukuoka , Hironori Miyaji , Hiroshi Hachiya , Kazuhiko Matsuzaki
发明人： Shinsuke Fukuoka , Hironori Miyaji , Hiroshi Hachiya , Kazuhiko Matsuzaki
IPC分类号： C07C69/96 , C07C68/08 , B01J19/24
CPC分类号： C07C68/065 , B01D3/009 , B01D3/32 , C07C68/08 , Y02P20/127 , Y02P20/582 , C07C69/96
摘要： It is an object of the present invention to provide a specific apparatus and process for using a single distillation column on a low boiling point reaction mixture containing a large amount of a dialkyl carbonate and an aliphatic monohydric alcohol produced through a reactive distillation process of taking a cyclic carbonate and the aliphatic monohydric alcohol as starting materials, continuously feeding the starting materials into a continuous multi-stage distillation column in which a homogeneous catalyst is present, and carrying out reaction and distillation simultaneously in the column, so as to separate the low boiling point reaction mixture by distillation into a column top component BT having the aliphatic monohydric alcohol as a main component thereof and a column bottom component BB having the dialkyl carbonate as a main component thereof stably for a prolonged period of time industrially. Moreover, it is an object to provide such a specific apparatus and process that are inexpensive and enable the dialkyl carbonate to be separated out by distillation in an amount of, for example, not less than 2 ton/hr stably for a prolonged period of time (e.g. not less than 1000 hours, preferably not less than 3000 hours, more preferably not less than 5000 hours). It has been discovered that by using a single continuous multi-stage distillation column having a specified structure, from out of a dialkyl carbonate and a diol produced through a reactive distillation system from a cyclic carbonate and an aliphatic monohydric alcohol, a high-purity dialkyl carbonate of purity not less than 97%, preferably not less than 99%, more preferably not less than 99.9%, can be separated out by distillation on an industrial scale of not less than 2 ton/hr, preferably not less than 3 ton/hr, more preferably not less than 4 ton/hr, with a high yield stably for a prolonged period of time of not less than 1000 hours, preferably not less than 3000 hours, more preferably not less than 5000 hours.

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