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1. 发明授权

US07211203B2 Polymer electrolyte, proton conductive membrane and membrane-electrode assembly 有权
标题翻译：聚合物电解质，质子传导膜和膜 - 电极组件
公开(公告)号：US07211203B2
公开(公告)日：2007-05-01
申请号：US10768151
申请日：2004-02-02
申请人： Toshihiro Otsuki , Nagayuki Kanaoka , Masaru Iguchi , Naoki Mitsuta , Hiroshi Soma
发明人： Toshihiro Otsuki , Nagayuki Kanaoka , Masaru Iguchi , Naoki Mitsuta , Hiroshi Soma
IPC分类号： H01B1/00 , C08G63/44 , C01G18/77 , C01G63/00 , C01G12/00
CPC分类号： H01M8/1004 , C08G65/48 , C08G73/10 , C08G75/23 , C08G2650/02 , C08G2650/40 , C08L71/00 , C08L81/06 , C25B13/08 , H01M8/1025 , H01M8/1027 , H01M8/103 , H01M8/1032
摘要： Disclosed are a polymer electrolyte having improved hot water resistance and radical resistance, a proton conductive membrane comprising the polymer electrolyte, and a membrane-electrode assembly including the proton conductive membrane.The polymer electrolyte comprises at least one polymer selected from polyether, polyketone, polyetherketone, polysulfone, polyethersulfone, polyimide, polyetherimide, polybenzimidazole, polybenzothiazole, polybenzoxazole and the like. The polymer comprises a repeating structural unit with either or both of an aromatic ring and a heterocyclic ring, and a repeating structural unit represented by the formula (1): wherein X is a single bond, an electron-withdrawing group or an electron-donating group; R is a single bond, —(CH2)q— or —(CF2)q— where q ranges from 1 to 10; m is from 0 to 10; k is from 0 to 5; l is from 0 to 4; and k+1≧1.
摘要翻译：公开了具有改善的耐热水性和耐自由基性的聚合物电解质，包含聚合物电解质的质子传导膜和包括质子传导膜的膜 - 电极组件。聚合物电解质包含至少一种选自聚醚，聚酮，聚醚酮，聚砜，聚醚砜，聚酰亚胺，聚醚酰亚胺，聚苯并咪唑，聚苯并噻唑，聚苯并恶唑等的聚合物。聚合物包含具有芳环和杂环中的任一个或两者的重复结构单元和由式（1）表示的重复结构单元：其中X是单键，吸电子基团或给电子组; R是单键， - （CH 2 CH 2）q - 或 - （CF 2 CH 2）q - 其中 q范围从1到10; m为0〜10; k为0〜5; l为0〜4; 和k + 1> = 1。

2. 发明申请

US20050202299A1 Polymer electrolyte and proton conductive membrane 有权
标题翻译：聚合物电解质和质子传导膜
公开(公告)号：US20050202299A1
公开(公告)日：2005-09-15
申请号：US11074664
申请日：2005-03-09
申请人： Toshihiro Otsuki , Nagayuki Kanaoka , Masaru Iguchi , Naoki Mitsuta , Hiroshi Soma
发明人： Toshihiro Otsuki , Nagayuki Kanaoka , Masaru Iguchi , Naoki Mitsuta , Hiroshi Soma
IPC分类号： C08J5/22 , C08G61/00 , C25B9/00 , G01N27/00 , H01B1/06 , H01B1/12 , H01M8/02 , H01M8/10
CPC分类号： C08J5/2256 , C08J2365/02 , C08J2371/12 , H01B1/122 , H01M8/1025 , H01M8/1027 , H01M8/1032 , H01M8/1039
摘要： A solid polymer electrolyte includes a polymer having a sulfonic group and shows high proton conductivity in a wide range of temperatures and humidities and is excellent in hot water resistance and chemical stability. A proton conductive membrane is composed of the electrolyte. The polymer electrolyte includes a polymer having a structural unit represented by the following formula (1a) or (1b): wherein A is a divalent electron-withdrawing group, B is a divalent electron-donating group or a direct bond, Ar is an aromatic group, Z is an oxygen or a sulfur atom, X is a hydrogen or a fluorine atom, j is an integer of 1 or greater, k is an integer of from 1 to 4, l is an integer of from 0 to 10, m is an integer of from 1 to 10, and n is an integer of from 1 to 8.
摘要翻译：固体聚合物电解质包括具有磺酸基的聚合物，并且在宽的温度和湿度范围内显示出高质子传导性，并且耐热水性和化学稳定性优异。质子传导膜由电解质组成。聚合物电解质包括具有由下式（1a）或（1b）表示的结构单元的聚合物：其中A是二价吸电子基团，B是二价给电子基团或直接键合，Ar是芳族基团，Z为氧或硫原子，X为氢或氟原子，j为1以上的整数，k为1〜4的整数，l为0〜10的整数，m 为1〜10的整数，n为1〜8的整数。

3. 发明授权

US07381501B2 Polymer electrolyte and proton conductive membrane 有权
标题翻译：聚合物电解质和质子传导膜
公开(公告)号：US07381501B2
公开(公告)日：2008-06-03
申请号：US11074664
申请日：2005-03-09
申请人： Toshihiro Otsuki , Nagayuki Kanaoka , Masaru Iguchi , Naoki Mitsuta , Hiroshi Soma
发明人： Toshihiro Otsuki , Nagayuki Kanaoka , Masaru Iguchi , Naoki Mitsuta , Hiroshi Soma
IPC分类号： H01M10/08 , H01M6/18
CPC分类号： C08J5/2256 , C08J2365/02 , C08J2371/12 , H01B1/122 , H01M8/1025 , H01M8/1027 , H01M8/1032 , H01M8/1039
摘要： A solid polymer electrolyte includes a polymer having a sulfonic group and shows high proton conductivity in a wide range of temperatures and humidities and is excellent in hot water resistance and chemical stability. A proton conductive membrane is composed of the electrolyte. The polymer electrolyte includes a polymer having a structural unit represented by the following formula (1a) or (1b): wherein A is a divalent electron-withdrawing group, B is a divalent electron-donating group or a direct bond, Ar is an aromatic group, Z is an oxygen or a sulfur atom, X is a hydrogen or a fluorine atom, j is an integer of 1 or greater, k is an integer of from 1 to 4, l is an integer of from 0 to 10, m is an integer of from 1 to 10, and n is an integer of from 1 to 8.
摘要翻译：固体聚合物电解质包括具有磺酸基的聚合物，并且在宽的温度和湿度范围内显示出高质子传导性，并且耐热水性和化学稳定性优异。质子传导膜由电解质组成。聚合物电解质包括具有由下式（1a）或（1b）表示的结构单元的聚合物：其中A是二价吸电子基团，B是二价给电子基团或直接键合，Ar是芳族基团，Z为氧或硫原子，X为氢或氟原子，j为1以上的整数，k为1〜4的整数，l为0〜10的整数，m 为1〜10的整数，n为1〜8的整数。

4. 发明授权

US07078121B2 Aromatic sulfonate derivative, polyarylene, sulfonated polyarylene and production method thereof, macromolecular solid electrolyte, and proton conductive membrane 有权
标题翻译：芳族磺酸衍生物，聚亚芳基，磺化聚亚芳基及其制备方法，大分子固体电解质和质子传导膜
公开(公告)号：US07078121B2
公开(公告)日：2006-07-18
申请号：US10734194
申请日：2003-12-15
申请人： Nagayuki Kanaoka , Masaru Iguchi , Naoki Mitsuta , Hiroshi Soma , Toshihiro Ohtsuki
发明人： Nagayuki Kanaoka , Masaru Iguchi , Naoki Mitsuta , Hiroshi Soma , Toshihiro Ohtsuki
IPC分类号： H01M8/10 , C08G61/10 , C08G61/12 , C08L65/00 , C08L65/02
CPC分类号： C07C309/67 , C08G61/02 , C08G61/10 , C08G2261/312 , C08K5/42 , C08L65/00 , C08L65/02 , H01B1/122 , H01M8/1025 , H01M8/1027 , H01M8/1032 , H01M8/1039 , H01M2300/0082 , Y02P70/56
摘要： Described herein is a production method of sulfonated polyarylene that is safe and enables easy control of the amount and position of sulfonic groups introduced in the polymer. The sulfonated polyarylene is also disclosed. The invention further provides a polyarylene and an aromatic sulfonate derivative that are suitably employed in the above production method. Also provided are a macromolecular solid electrolyte that comprises the sulfonated polyarylene, and a proton conductive membrane.The aromatic sulfonate derivative has the following formula (1): wherein X is a halogen atom other than fluorine, a —OSO3CH3 group or a —OSO3CF3 group; Y is a divalent organic group; A is —(CH2)m— or —(CF2)m— (wherein m is an integer of 1 to 10); and R is a C4-20 hydrocarbon group. The production method of sulfonated polyarylene comprises coupling polymerization of an aromatic compound that includes at least the aromatic sulfonate derivative of the formula (1) and hydrolysis of the resultant polyarylene.
摘要翻译：本文描述了磺化聚亚芳基的生产方法，它是安全的并且易于控制在聚合物中引入的磺酸基的量和位置。还公开了磺化聚亚芳基。本发明还提供了适用于上述制备方法的聚亚芳基和芳族磺酸酯衍生物。还提供了包含磺化聚亚芳基和质子传导膜的高分子固体电解质。芳香族磺酸酯衍生物具有下式（1）：其中X是除氟以外的卤素原子，-OSO 3 CH 3基团或-OSO < 3 3 3组; Y是二价有机基团; A是 - （CH 2 CH 2）m - 或 - （CF 2）m - （其中m是 1〜10的整数）并且R是C 4-20烃基。磺化聚亚芳基的制备方法包括至少包含式（1）的芳族磺酸酯衍生物和所得聚亚芳基的水解的芳族化合物的偶联聚合。

5. 发明授权

US07001929B2 Proton conductive membrane having improved thermal stability 有权
标题翻译：质子导电膜具有改善的热稳定性
公开(公告)号：US07001929B2
公开(公告)日：2006-02-21
申请号：US10641212
申请日：2003-08-15
申请人： Kohei Goto , Mayumi Kakuta , Fusazumi Masaka , Kiyonori Kita , Naoki Mitsuta , Masaru Iguchi , Hiroshi Soma , Nagayuki Kanaoka
发明人： Kohei Goto , Mayumi Kakuta , Fusazumi Masaka , Kiyonori Kita , Naoki Mitsuta , Masaru Iguchi , Hiroshi Soma , Nagayuki Kanaoka
IPC分类号： C08J5/20
CPC分类号： H01M10/0565 , H01M8/0289 , H01M8/1023 , H01M8/1025 , H01M8/1027 , H01M8/103 , H01M8/1032 , H01M8/1039 , H01M8/1051 , H01M8/1081 , Y02P70/56
摘要： The invention provides a proton conductive membrane excellent in heat resistance, which has sulfonic acid as ion exchange groups. The proton conductive membrane comprises a nitrogen-containing compound that can be mixed with water in arbitrary proportions and has a boiling point of not lower than 100. degree. C. and a proton conductive resin which has sulfonic acid ion-exchange groups, wherein the nitrogen-containing compound is contained in an amount of 0.5 to 10 parts by weight based on 100 parts by weight of the proton conductive resin.
摘要翻译：本发明提供了耐热性优异的质子传导膜，其具有作为离子交换基团的磺酸。质子传导膜包含可与任意比例的水混合并且沸点不低于100.度的含氮化合物。以及具有磺酸离子交换基团的质子传导性树脂，其中，相对于100重量份的质子传导性树脂，含氮化合物的含量为0.5〜10重量份。

6. 发明申请

US20060127728A1 Membrane-electrode assembly for fuel cell 审中-公开
标题翻译：燃料电池用膜电极组件
公开(公告)号：US20060127728A1
公开(公告)日：2006-06-15
申请号：US11302346
申请日：2005-12-14
申请人： Toshihiro Otsuki , Nagayuki Kanaoka , Masaru Iguchi , Hiroshi Soma
发明人： Toshihiro Otsuki , Nagayuki Kanaoka , Masaru Iguchi , Hiroshi Soma
IPC分类号： H01M8/10
CPC分类号： B01D71/82 , B01D71/52 , B01D71/72 , B01D71/80 , C08G61/02 , C08G61/025 , C08G65/40 , C08G75/23 , C08G2261/3424 , H01M8/1025 , H01M8/1027 , H01M8/1032 , H01M8/1039
摘要： The present invention provides a membrane-electrode assembly for fuel cell which comprises a solid polymer electrolyte membrane comprising a specific polyarylene having a sulfonic acid group and has excellent creep resistance, power generation performance and durability against power generation under high-temperature environment. The membrane-electrode assembly is characterized in that a pair of electrodes each comprising a gas diffusing layer and a catalyst layer are joined to both sides of a solid polymer electrolyte membrane so that the catalyst layer side comes into contact with the membrane, said membrane comprises a sulfonated polyarylene comprising constituent unit represented by the following formula (1): wherein Y is a group represented by —C(CF3)2—, (CF2)i—, wherein i is an integer of 1 to 10, —SO— or —SO2—; Z is a divalent electron-donating group or a direct bond; Ar is an aromatic group having a substituent represented by —SO3H; m is an integer of 0 to 10; n is an integer of 0 to 10; and k is an integer of 1 to 4.
摘要翻译：本发明提供一种燃料电池用膜电极接合体，其包含具有磺酸基的特定聚亚芳基的固体高分子电解质膜，在高温环境下具有优异的抗蠕变性，发电性能和耐发电性。膜 - 电极组件的特征在于，在固体聚合物电解质膜的两面上接合包括气体扩散层和催化剂层的一对电极，使得催化剂层侧与膜接触，所述膜包含包含由下式（1）表示的构成单元的磺化聚亚芳基：其中Y是由-C（CF 3）2 - 表示的基团，（CF 3）其中i为1〜10的整数，-SO - 或-SO 2 - ; - Z是二价给电子基团或直接键; Ar是具有由-SO 3 H 3表示的取代基的芳香族基团; m为0〜10的整数。 n为0〜10的整数。 k为1〜4的整数。

7. 发明授权

US07030206B2 Polymer electrolyte and proton-conducting membrane 有权
标题翻译：聚合物电解质和质子传导膜
公开(公告)号：US07030206B2
公开(公告)日：2006-04-18
申请号：US10804228
申请日：2004-03-19
申请人： Nagayuki Kanaoka , Masaru Iguchi , Naoki Mitsuta , Hiroshi Sohma , Toshihiro Ohtsuki
发明人： Nagayuki Kanaoka , Masaru Iguchi , Naoki Mitsuta , Hiroshi Sohma , Toshihiro Ohtsuki
IPC分类号： C08G73/06 , C08G75/00 , H01M8/00
CPC分类号： H01M10/052 , H01M4/926 , H01M8/0289 , H01M8/1004 , H01M8/1025 , H01M8/1027 , H01M8/103 , H01M8/1032 , H01M10/0565
摘要： To provide a sulfonic acid group-containing polymer having improved hot water resistance and radical resistance (durability), a solid polymer electrolyte including the polymer, and a proton-conducting membrane including the electrolyte, the polymer electrolyte includes a sulfonated product of a polymer shown by the following general formula (I): wherein X, Y, and Z are bonded randomly, alternately, or in blocks, y represents an integer of two or more, and each of x and z represents an integer of zero or more, where x+z>2.
摘要翻译：为了提供具有改善的耐热水性和耐自由基性（耐久性）的含磺酸基聚合物，包含该聚合物的固体聚合物电解质和包含电解质的质子传导膜，聚合物电解质包括所示聚合物的磺化产物通过以下通式（I）表示：其中X，Y和Z随机，交替或以块形式键合，y表示2以上的整数，x和z分别表示0以上的整数， x + z> 2。

8. 发明授权

US08114552B2 Electrode structure for polymer electrolyte fuel cell comprising sulfonated polyarylene-based polymer and method for manufactuing same 有权
标题翻译：包含磺化聚亚芳基聚合物的聚合物电解质燃料电池的电极结构及其制造方法
公开(公告)号：US08114552B2
公开(公告)日：2012-02-14
申请号：US11723436
申请日：2007-03-20
申请人： Yuichiro Hama , Masaru Iguchi , Junichi Yano , Nagayuki Kanaoka , Naoki Mitsuta
发明人： Yuichiro Hama , Masaru Iguchi , Junichi Yano , Nagayuki Kanaoka , Naoki Mitsuta
IPC分类号： H01M8/10
CPC分类号： H01M4/8828 , H01M4/8807 , H01M4/8882 , H01M4/92 , H01M4/926 , H01M8/1004 , H01M8/1025 , H01M8/1039 , Y02P70/56
摘要： There is provided an electrode structure for a polymer electrolyte fuel cell having excellent power generation performance and excellent durability and a method for manufacturing the same. Also provided is a polymer electrolyte fuel cell including the electrode structure and an electrical apparatus and a transport apparatus using the polymer electrolyte fuel cell. The electrode structure includes a polymer electrolyte membrane 2 sandwiched between a pair of electrode catalyst layers 1, 1 containing carbon particles supporting catalyst particles. The polymer electrolyte membrane 2 is made of a sulfonated polyarylene-based polymer. The sulfonated polyarylene-based polymer has an ion exchange capacity in the range of 1.7 to 2.3 meq/g, and the polymer contains a component insoluble in N-methylpyrrolidone in an amount of 70% or less relative to the total amount of the polymer, after the polymer is subjected to heat treatment for exposing it under a constant temperature atmosphere of 12° C. for 200 hours. A catalyst paste containing catalyst particles and a polymer electrolyte is coated on a sheet-like support 6 and dried to form an electrode catalyst layer 1 containing a solvent in an amount in the range of 0.5% or less by weight of the total membrane. The electrode catalyst layers 3, 3 are thermally transferred and joined on both sides of the polymer electrolyte membrane 1.
摘要翻译：提供了具有优异的发电性能和优异的耐久性的用于聚合物电解质燃料电池的电极结构及其制造方法。还提供了包括电极结构的聚合物电解质燃料电池和使用聚合物电解质燃料电池的电气设备和输送设备。电极结构包括夹在包含支持催化剂颗粒的碳颗粒的一对电极催化剂层1,1之间的聚合物电解质膜2。高分子电解质膜2由磺化聚亚芳基系聚合物构成。磺化聚亚芳基系聚合物的离子交换容量为1.7〜2.3meq / g，聚合物中含有不溶于N-甲基吡咯烷酮的成分相对于聚合物总量为70％以下，在聚合物经受热处理以使其在12℃的恒温气氛下暴露200小时。将含有催化剂颗粒和聚合物电解质的催化剂浆料涂覆在片状载体6上并干燥，形成含有溶剂总量为0.5重量％以下的溶剂的电极催化剂层1。电极催化剂层3,3在高分子电解质膜1的两面热转印并接合。

9. 发明申请

US20100190088A1 MEMBRANE ELECTRODE ASSEMBLY AND POLYMER ELECTROLYTE FUEL CELL THEREWITH 有权
标题翻译：膜电极组件和聚合物电解质燃料电池
公开(公告)号：US20100190088A1
公开(公告)日：2010-07-29
申请号：US12752941
申请日：2010-04-01
申请人： Nagayuki KANAOKA , Naoki Mitsuta , Yuichiro Hama , Ryoichiro Takahashi , Hiroshi Souma , Masaru Iguchi , Yoichi Asano
发明人： Nagayuki KANAOKA , Naoki Mitsuta , Yuichiro Hama , Ryoichiro Takahashi , Hiroshi Souma , Masaru Iguchi , Yoichi Asano
IPC分类号： H01M8/10
CPC分类号： H01M8/1032 , H01M4/8605 , H01M4/92 , H01M4/926 , H01M8/1004 , H01M8/1025 , H01M8/1027 , H01M8/1048 , H01M8/1081 , Y02P70/56
摘要： A membrane electrode assembly for a polymer electrolyte fuel cell has superior power generation characteristics under low humidity conditions and superior starting characteristics under low temperature conditions. In the membrane electrode assembly for a polymer electrolyte fuel cell in which a polymer electrolyte membrane is disposed between a pair of electrodes containing a catalyst, the polymer electrolyte membrane has a polymer segment A having an ion conductive component and a polymer segment B not having an ion conductive component. Furthermore, in the case in which the polymer electrolyte membrane is immersed in water at 90° C. for 30 minutes, absorbed water which exhibits a thawing temperature of from −30 to 0° C. is in a range from 0.01 to 3.0 g per 1 g of the polymer.
摘要翻译：用于聚合物电解质燃料电池的膜电极组件在低湿度条件下具有优异的发电特性，并且在低温条件下具有优异的起动特性。在其中聚合物电解质膜设置在包含催化剂的一对电极之间的聚合物电解质燃料电池的膜电极组件中，聚合物电解质膜具有具有离子传导性成分的聚合物链段A和不具有离子传导元件。此外，在将聚合物电解质膜浸渍在90℃的水中30分钟的情况下，解冻温度为-30〜0℃的吸收水为0.01〜3.0g 1g聚合物。

10. 发明申请

US20070166594A1 Electrode structure for polymer electrolyte fuel cell and method for manufacturing the same 有权
标题翻译：聚合物电解质燃料电池的电极结构及其制造方法
公开(公告)号：US20070166594A1
公开(公告)日：2007-07-19
申请号：US11723436
申请日：2007-03-20
申请人： Yuichiro Hama , Masaru Iguchi , Junichi Yano , Nagayuki Kanaoka , Naoki Mitsuta
发明人： Yuichiro Hama , Masaru Iguchi , Junichi Yano , Nagayuki Kanaoka , Naoki Mitsuta
IPC分类号： H01M8/10 , H01M4/96 , H01M4/88 , B05D5/12
CPC分类号： H01M4/8828 , H01M4/8807 , H01M4/8882 , H01M4/92 , H01M4/926 , H01M8/1004 , H01M8/1025 , H01M8/1039 , Y02P70/56
摘要： There is provided an electrode structure for a polymer electrolyte fuel cell having excellent power generation performance and excellent durability and a method for manufacturing the same. Also provided is a polymer electrolyte fuel cell including the electrode structure and an electrical apparatus and a transport apparatus using the polymer electrolyte fuel cell. The electrode structure includes a polymer electrolyte membrane 2 sandwiched between a pair of electrode catalyst layers 1, 1 containing carbon particles supporting catalyst particles. The polymer electrolyte membrane 2 is made of a sulfonated polyarylene-based polymer. The sulfonated polyarylene-based polymer has an ion exchange capacity in the range of 1.7 to 2.3 meq/g, and the polymer contains a component insoluble in N-methylpyrrolidone in an amount of 70% or less relative to the total amount of the polymer, after the polymer is subjected to heat treatment for exposing it under a constant temperature atmosphere of 12° C. for 200 hours. A catalyst paste containing catalyst particles and a polymer electrolyte is coated on a sheet-like support 6 and dried to form an electrode catalyst layer 1 containing a solvent in an amount in the range of 0.5% or less by weight of the total membrane. The electrode catalyst layers 3, 3 are thermally transferred and joined on both sides of the polymer electrolyte membrane 1.
摘要翻译：提供了具有优异的发电性能和优异的耐久性的用于聚合物电解质燃料电池的电极结构及其制造方法。还提供了包括电极结构的聚合物电解质燃料电池和使用聚合物电解质燃料电池的电气设备和输送设备。电极结构包括夹在包含支持催化剂颗粒的碳颗粒的一对电极催化剂层1,1之间的聚合物电解质膜2。高分子电解质膜2由磺化聚亚芳基系聚合物构成。磺化聚亚芳基系聚合物的离子交换容量为1.7〜2.3meq / g，聚合物中含有不溶于N-甲基吡咯烷酮的成分相对于聚合物总量为70％以下，在聚合物经受热处理以使其在12℃的恒温气氛下暴露200小时。将含有催化剂颗粒和聚合物电解质的催化剂浆料涂覆在片状载体6上并干燥以形成含有溶剂的总量为0.5重量％以下的溶剂的电极催化剂层1。电极催化剂层3,3在高分子电解质膜1的两面热转印并接合。

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