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1. 发明授权

US4377718A Process for producing p-xylene 失效
标题翻译：生产对二甲苯的方法
公开(公告)号：US4377718A
公开(公告)日：1983-03-22
申请号：US285464
申请日：1981-07-21
申请人： Kimihiko Sato , Tokuji Sakai , Yasuo Yamasaki , Tamio Onodera , Koji Sumitani
发明人： Kimihiko Sato , Tokuji Sakai , Yasuo Yamasaki , Tamio Onodera , Koji Sumitani
IPC分类号： B01J29/00 , C07C1/00 , C07C2/86 , C07C15/08 , C07C67/00 , C07C2/68
CPC分类号： C07C2/864 , C07C2/865 , C07C2529/44 , Y02P20/52 , Y02P20/584
摘要： In a process for producing p-xylene which comprises catalytically methylating toluene with a methylating agent in the gaseous phase, the improvement wherein(a) said methylation is carried out continuously in a multi-stage reaction system consisting of a plurality of separate series-connected fixed catalyst layers without separating the resulting xylenes in an intermediate stage,(b) said toluene is fed together with hydrogen gas into only the first-stage fixed catalyst layer and passed successively through the subsequent fixed catalyst layers, the amount of toluene fed being such that the total weight hourly space velocity of toluene is from 1 to 300 hr.sup.-1,(c) said methylating agent is fed into each of said fixed catalyst layers, if desired together with hydrogen gas, the amount of the methylating agent fed into each catalyst layer being 0.01/t moles to 1/t moles, in which t is the number of methyl groups in the methylating agent, per mole of toluene fed into the first-stage catalyst layer, and the total amount of the methylating agent fed into all of the catalyst layers being within the range of 0.1/t moles to 2/t moles, in which t is as defined, per mole of toluene fed into the first-stage catalyst layer, and(d) each fixed catalyst layer is filled with a catalyst composed of a crystalline aluminosilicate containing magnesium oxide or lanthanide oxide.
摘要翻译：在一种生产对二甲苯的方法中，其包括在气相中用甲基化剂甲苯化甲苯，其中（a）所述甲基化在多级反应体系中连续进行，所述多级反应体系由多个单独的串联固定的催化剂层，而不在中间阶段分离所得的二甲苯，（b）将所述甲苯与氢气一起进入第一级固定催化剂层，并依次通过随后的固定催化剂层，进料的甲苯的量甲苯的总重小时空速为1〜300小时-1，（c）如果需要，将所述甲基化剂与氢气一起进料到每个所述固定催化剂层中，将甲基化剂加入到每个催化剂层为每摩尔进料到第一阶段催化剂中的甲苯为0.01 / t摩尔至1 / t摩尔，其中t为甲基化剂中的甲基数并且进料到所有催化剂层中的甲基化剂的总量在0.1 / t摩尔至2 / t摩尔的范围内，其中t定义为每摩尔进料到第一阶段催化剂中的甲苯层，并且（d）每个固定的催化剂层填充有由含有氧化镁或镧系元素氧化物的结晶硅铝酸盐组成的催化剂。

2. 发明授权

US4524055A Crystalline aluminosilicate zeolite and process for production thereof 失效
标题翻译：结晶硅铝酸盐沸石及其生产方法
公开(公告)号：US4524055A
公开(公告)日：1985-06-18
申请号：US468381
申请日：1983-02-22
申请人： Tamio Onodera , Tokuji Sakai , Yasuo Yamasaki , Koji Sumitani
发明人： Tamio Onodera , Tokuji Sakai , Yasuo Yamasaki , Koji Sumitani
IPC分类号： C07C4/08 , B01J20/18 , B01J29/00 , B01J29/40 , B01J29/44 , C01B39/04 , C01B39/38 , C07B61/00 , C07C1/00 , C07C4/18 , C07C5/27 , C07C6/12 , C07C67/00 , C01B33/28 , B01J29/28
CPC分类号： C07C6/12 , B01J29/40 , B01J29/44 , C01B39/38 , C07C5/2708 , C07C2529/06 , Y10S423/22
摘要： A novel crystalline aluminosilicate zeolite characterized by having(a) a silica/alumina mole ratio in the range of from 10 to 100,(b) X-ray lattice distances d shown in Table A in the specification, and(c) a (cyclohexane/n-hexane) adsorption ratio of at least 0.7. This crystalline aluminosilicate zeolite is useful, for example, as a catalyst in the isomerization reaction or transalkylation reaction of alkylbenzenes or alkylnaphthalenes, and can be prepared by heating a crystalline aluminosilicate zeolite ZSM-5 having a silica/alumina mole ratio of from 20 to 300 at a temperature between 80.degree. C. and 250.degree. C. in an aqueous solution containing 0.1 to 1 g, per gram of the ZSM-5 zeolite, of an alkali metal hydroxide.
摘要翻译：其特征在于：（a）二氧化硅/氧化铝的摩尔比为10〜100，（b）本说明书中的表A所示的X射线晶格距离d，（c）a（环己烷 /正己烷）吸附比至少为0.7。该结晶硅铝酸盐沸石可用作例如烷基苯或烷基萘异构化反应或烷基转移反应中的催化剂，并可通过加热二氧化硅/氧化铝摩尔比为20至300的结晶硅铝酸盐沸石ZSM-5 在含有0.1至1g每克ZSM-5沸石的碱金属氢氧化物的水溶液中在80℃至250℃之间的温度下进行。

3. 发明授权

US4954326A Preparation of crystalline aluminosilicate zeolite, and its product 失效
标题翻译：结晶硅铝酸盐沸石及其制品的制备
公开(公告)号：US4954326A
公开(公告)日：1990-09-04
申请号：US380723
申请日：1989-07-12
申请人： Tamio Onodera , Tokuji Sakai , Yasuo Yamasaki , Koji Sumitani
发明人： Tamio Onodera , Tokuji Sakai , Yasuo Yamasaki , Koji Sumitani
IPC分类号： B01J20/18 , B01J29/00 , B01J29/70 , C01B39/38 , C07B61/00 , C07C1/00 , C07C4/18 , C07C6/12 , C07C15/00 , C07C15/08 , C07C15/24 , C07C67/00
CPC分类号： C07C6/126 , C01B39/38 , C07C4/18 , C07C2529/06 , Y02P20/52
摘要： A process for producing a crystalline aluminosilicate zeolite characterized by having (a) a silica/alumina mole ratio of from 10 to 100, (b) X-ray lattice distances d shown in Table A of the specification, and (c) a specific n-hexane adsorption, under limited measuring conditions, of at least 0.07 g/g, which comprises maintaining a silica source, an alumina source, and a zeolite selected from zeolites ZSM-5 and zeolites having said characteristics, in an aqueous solution containing 1 to 200 millimoles, per gram of said zeolite, of an alkali metal hydroxide under such temperature, pressure and time conditions as to produce a crystalline aluminosilicate zeolite; and a crystalline aluminosilicate zeolite characterized by having aforesaid properties (a) to (c) and (d) a (2-methylpentane/cyclohexane) adsorption ratio of from 1.1 to 1.6.
摘要翻译：一种结晶性硅铝酸盐沸石的制造方法，其特征在于，（a）二氧化硅/氧化铝摩尔比为10〜100，（b）本说明书的表A所示的X射线晶格距离d，（c）在有限的测量条件下，己烷吸附至少为0.07g / g，其包括将二氧化硅源，氧化铝源和选自沸石ZSM-5的沸石和具有所述特征的沸石在含有1至在这样的温度，压力和时间条件下，产生结晶铝硅酸盐沸石的碱金属氢氧化物，每克所述沸石200毫摩尔; 其特征在于上述性质（a）〜（c）和（d）（2-甲基戊烷/环己烷）吸附比为1.1〜1.6。

4. 发明授权

US4485185A Catalyst composition 失效
标题翻译：催化剂组成
公开(公告)号：US4485185A
公开(公告)日：1984-11-27
申请号：US532305
申请日：1983-09-15
申请人： Tamio Onodera , Tokuji Sakai , Yasuo Yamasaki , Koji Sumitani
发明人： Tamio Onodera , Tokuji Sakai , Yasuo Yamasaki , Koji Sumitani
IPC分类号： B01J29/00 , B01J29/44 , B01J29/65 , B01J29/70 , B01J29/74 , C07B61/00 , C07C1/00 , C07C5/27 , C07C15/02 , C07C15/08 , C07C67/00 , B01J29/32
CPC分类号： B01J29/44 , C07C5/2724 , B01J29/65 , B01J29/70
摘要： A catalyst composition comprising (i) a crystalline aluminosilicate selected from the group consisting of zeolite ZSM-5, zeolite ZSM-11, zeolite ZSM-12, zeolite ZSM-35 and zeolite ZSM-38 and having a silica/alumina mole ratio of 20 to 1,000; and (ii) at least two metals which are (a) platinum and (b) at least one other metal selected from the group consisting of titanium, chromium, zinc, gallium, germanium, strontium, yttrium, zirconium, molybdenum, palladium, tin, barium, cerium, tungsten, osmium, lead, cadmium, mercury, indium, lanthanum and beryllium. This catalyst composition is useful particularly for the isomerization of aromatic hydrocarbons and reforming of naphtha.

5. 发明授权

US4320242A Process for selective dealkylation of alkyl-substituted aromatic hydrocarbons 失效
标题翻译：烷基取代芳烃选择性脱烷基化方法
公开(公告)号：US4320242A
公开(公告)日：1982-03-16
申请号：US118324
申请日：1980-02-04
申请人： Tamio Onodera , Tokuji Sakai , Yasuo Yamasaki , Koji Sumitani , Minekazu Sueoka
发明人： Tamio Onodera , Tokuji Sakai , Yasuo Yamasaki , Koji Sumitani , Minekazu Sueoka
IPC分类号： B01J29/00 , C07B61/00 , C07C1/00 , C07C4/18 , C07C15/02 , C07C67/00 , C07C4/12
CPC分类号： C07C4/18 , C07C2529/40 , C07C2529/44
摘要： In a process for dealkylating a hydrocarbon material containing at least one alkyl-substituted aromatic hydrocarbon having bonded to the aromatic ring at least one alkyl group with at least 2 carbon atoms in the gaseous phase in the presence of hydrogen using a hydro-dealkylation catalyst, the improvement wherein (a) said hydro-dealkylation catalyst is composed of a crystalline aluminosilicate having a silica/alumina mole ratio of from 20 to 200 and containing a noble metal selected from platinum, palladium, rhodium and iridium, and (b) said dealkylation is carried out at a temperature of 250.degree. C. to 420.degree. C. and a pressure of not more than 100 psig, thereby selectively removing said alkyl group containing at least 2 carbon atoms from said alkyl-substituted aromatic hydrocarbon.
摘要翻译：在使用氢 - 脱烷基化催化剂的氢气存在下，在气相中含有至少一个与芳环键合至少一个具有至少2个碳原子的烷基的烃基物质脱烷基化的方法中，其中（a）所述加氢脱烷基化催化剂由二氧化硅/氧化铝摩尔比为20-200的结晶硅铝酸盐和含有选自铂，钯，铑和铱的贵金属组成，和（b）所述脱烷基化在250℃至420℃的温度和不超过100psig的压力下进行，从而从所述烷基取代的芳烃中选择性除去含有至少2个碳原子的烷基。

6. 发明授权

US4695667A Novel crystalline aluminosilicate zeolites and process for production thereof 失效
标题翻译：新型结晶硅铝酸盐沸石及其生产方法
公开(公告)号：US4695667A
公开(公告)日：1987-09-22
申请号：US705631
申请日：1985-02-26
申请人： Koji Sumitani , Tokuji Sakai , Yasuo Yamasaki , Tamio Onodera
发明人： Koji Sumitani , Tokuji Sakai , Yasuo Yamasaki , Tamio Onodera
IPC分类号： B01J29/70 , B01J29/74 , C01B39/48 , C07C1/20 , C07C2/86 , C07C4/06 , C07C4/18 , C07C5/27 , C07C5/387 , C07C6/12
CPC分类号： B01J29/7023 , B01J29/7073 , B01J29/7446 , B01J29/7646 , B01J29/7846 , C01B39/48 , C07C1/20 , C07C2/864 , C07C4/06 , C07C4/18 , C07C5/2708 , C07C5/2775 , C07C5/387 , C07C6/123 , C07C6/126 , B01J2229/36 , C07C2529/06 , Y02P20/52
摘要： A novel crystalline aluminosilicate zeolite characterized by having a composition of the following general formula expressed in terms of the mole ratios of oxides in the anhydrous statexM.sub.2/n O.Al.sub.2 O.sub.3.ySiO.sub.2wherein M represents at least one cation having a valence of n, x is a number between 0.5 and 4, and y is a number of at least 10, and having a specific X-ray diffraction pattern. Said crystalline aluminosilicate zeolite can be produced by maintaining a mixture of a water-soluble alkali metal compound, an N,N,N,N',N',N'-hexamethyl-1,6-hexane diammonium compound, a compound capable of giving silica under the reaction conditions, a compound capable of giving alumina under the reaction conditions and water, at a temperature of at least 80.degree. C. for a period sufficient to form crystals, and is useful as a catalyst for, for example, transalkylation or alkylation reaction of toluene, isomerization of xylene, isomerization of ethylbenzene to xylenes, etc.
摘要翻译：一种新型的结晶硅铝酸盐沸石，其特征在于具有以无机状态的氧化物摩尔比表示的以下通式的组成：xM 2 / nO·Al 2 O 3·ySiO 2，其中M表示至少一个价数为n的阳离子，x为数为0.5〜4，y为10以上，具有特定的X射线衍射图。所述结晶硅铝酸盐沸石可以通过保持水溶性碱金属化合物，N，N，N，N'，N'，N'-六甲基-1,6-己烷二铵化合物，能够在反应条件下给予二氧化硅，在反应条件下能够得到氧化铝的化合物和水，在至少80℃的温度下足以形成晶体的时间，并且可用作例如烷基转移的催化剂或甲苯的烷基化反应，二甲苯异构化，乙苯异构化成二甲苯等。

7. 发明授权

US4557919A Production of crystalline zeolites 失效
标题翻译：生产结晶沸石
公开(公告)号：US4557919A
公开(公告)日：1985-12-10
申请号：US598691
申请日：1984-04-10
申请人： Koji Sumitani , Tokuji Sakai , Yasuo Yamasaki , Tamio Onodera
发明人： Koji Sumitani , Tokuji Sakai , Yasuo Yamasaki , Tamio Onodera
IPC分类号： B01J29/70 , B01J29/74 , C01B37/02 , C01B39/42 , C01B39/48 , C07C5/27 , C07C5/373 , C07D295/02 , C01B33/28
CPC分类号： C07D295/02 , B01J29/7034 , B01J29/7469 , C01B37/02 , C01B39/48 , C07C5/2791 , C07C5/373 , B01J2229/26 , B01J2229/42 , Y02P20/52
摘要： A process for producing a crystalline zeolite TPZ-12, which comprises maintaining a starting mixture at a temperature of at least 80.degree. C. for a period sufficient to produce zeolite crystals, said starting mixture consisting of(a) a substance capable of yielding silica under the reaction conditions,(b) a water-soluble alkali metal compound,(c) water, and(d) a diammonium compound represented by the following general formula ##STR1## wherein R.sub.1 and R.sub.2 are identical or different and each represents a hydrogen atom or an alkyl group having 1 to 4 carbon atoms, p and q are identical or different and each represents an integer of 4 or 5, n is 4, 5 or 6, and y represents an anion having a valence of m, and additionally, if desired,(e) a substance capable of yielding alumina under the reaction conditions,in the particular quantities.
摘要翻译：一种生产结晶沸石TPZ-12的方法，其包括将起始混合物在至少80℃的温度下保持足以产生沸石晶体的时间，所述起始混合物由（a）能够产生二氧化硅的物质在反应条件下，（b）水溶性碱金属化合物，（c）水和（d）由以下通式表示的二铵化合物：其中R 1和R 2相同或不同，表示氢原子或碳原子数1〜4的烷基，p和q相同或不同，分别表示4或5的整数，n表示4,5或6，y表示m为阴离子，另外，如果需要，（e）能够在反应条件下以特定量产生氧化铝的物质。

8. 发明授权

US4331822A Isomerization of xylene 失效
标题翻译：二甲苯异构化
公开(公告)号：US4331822A
公开(公告)日：1982-05-25
申请号：US133793
申请日：1980-03-25
申请人： Tamio Onodera , Tokuji Sakai , Yasuo Yamasaki , Koji Sumitani
发明人： Tamio Onodera , Tokuji Sakai , Yasuo Yamasaki , Koji Sumitani
IPC分类号： B01J29/00 , B01J29/44 , B01J29/65 , B01J29/70 , B01J29/74 , C07B61/00 , C07C1/00 , C07C5/27 , C07C15/02 , C07C15/08 , C07C67/00 , C07C5/22
CPC分类号： B01J29/44 , C07C5/2724 , B01J29/65 , B01J29/70
摘要： In a process for isomerization of xylenes which comprises contactng an aromatic hydrocarbon stock mainly containing xylene isomers not attaining a thermodynamic equilibrium composition with a catalyst composition containing a crystalline aluminosilicate at an elevated temperature in the vapor phase in the presence of hydrogen, the improvement wherein said catalyst composition comprises a crystalline aluminosilicate having a silica/alumina mole ratio of at least 10 and contains at least two metals which are (a) platinum and (b) at least one metal selected from the group consisting of titanium, chromium, zinc, gallium, germanium, strontium, yttrium, zirconium, molybdenum, palladium, tin, barium, cesium, cerium, tungsten, osmium, lead, cadmium, mercury, indium, lanthanum, beryllium, lithium and rubidium.
摘要翻译：在二甲苯异构化的方法中，其包括在氢气存在下，在蒸气相中在高温下接触主要含有二甲苯异构体的芳族烃原料而不能获得热力学平衡组合物，所述组合物含有结晶硅铝酸盐，所述催化剂组合物在气相中处于升高的温度，其中所述催化剂组合物包含具有至少10的二氧化硅/氧化铝摩尔比的结晶硅铝酸盐，并且包含至少两种金属，其为（a）铂和（b）至少一种选自钛，铬，锌，镓锗，锶，钇，锆，钼，钯，锡，钡，铯，铈，钨，锇，铅，镉，汞，铟，镧，铍，锂和铷。

9. 发明授权

US4300014A Process for isomerization of xylene 失效
标题翻译：二甲苯异构化方法
公开(公告)号：US4300014A
公开(公告)日：1981-11-10
申请号：US204018
申请日：1980-11-04
申请人： Yasuo Yamasaki , Tokuji Sakai , Tamio Onodera , Kiji Sumitani
发明人： Yasuo Yamasaki , Tokuji Sakai , Tamio Onodera , Kiji Sumitani
IPC分类号： B01J23/32 , B01J23/90 , B01J29/44 , B01J29/90 , B01J38/12 , B01J38/20 , C07B61/00 , C07C1/00 , C07C5/27 , C07C15/08 , C07C67/00 , C07C5/24
CPC分类号： B01J29/90 , B01J23/32 , B01J29/44 , C07C5/2724 , Y02P20/52 , Y02P20/584
摘要： A process for isomerizing xylenes, which comprisescontacting an aromatic hydrocarbon feedstock containing mainly a xylene isomeric mixture containing ethylbenzene with a catalyst of a palladium-containing crystalline aluminosilicate in the vapor phase in the presence of hydrogen to continuously isomerize xylenes and simultaneously de-ethylate the ethylbenzene selectively;interrupting the isomerization reaction;introducing an oxygen-containing gas into a bed of the catalyst in which coke has been deposited during the isomerization reaction, to contact the catalyst with the oxygen-containing gas;burning off the coke deposits on the catalyst with the oxygen-containing gas by gradually increasing the temperature of introduction of the oxygen-containing gas from not more than 200.degree. C. to a temperature in the range of 330.degree. to 390.degree. C. with no part of the catalyst bed exceeding a maximum temperature of 400.degree. C. while controlling the hot spot temperature of the catalyst bed not to exceed 50.degree. C. throughout the burn-off period;reducing in hydrogen the catalyst from which the burnable coke deposits have been removed at least partly;andthereafter resuming the isomerization reaction in the presence of the regenerated catalyst.
摘要翻译：异构化二甲苯的方法，其包括在氢气存在下使主要含有乙苯的二甲苯异构体混合物的芳族烃原料与气相中的含钯结晶硅铝酸盐的催化剂接触，以连续异构化二甲苯，同时使二甲苯脱乙基化乙苯选择性; 中断异构化反应; 在异构化反应期间将含氧气体引入已经沉积焦炭的催化剂床中，以使催化剂与含氧气体接触; 通过逐渐将含氧气体的引入温度从不高于200℃升温到330℃至390℃的温度，用含氧气体燃烧催化剂上的焦炭沉积物，在整个燃烧期间，催化剂床的热点温度不超过50℃，催化剂床的任何部分超过最高温度400℃。减少氢气，至少部分地将可燃焦炭沉积物从其中除去的催化剂; 然后在再生催化剂存在下恢复异构化反应。

10. 发明授权

US4709088A Process for producing 2,6-naphthalene-dicarboxylic acid 失效
标题翻译： 2,6-萘二羧酸的制备方法
公开(公告)号：US4709088A
公开(公告)日：1987-11-24
申请号：US883479
申请日：1986-07-15
申请人： Isao Hirose , Tamio Amemiya , Tokuji Sakai
发明人： Isao Hirose , Tamio Amemiya , Tokuji Sakai
IPC分类号： C07C51/265 , C07C51/16 , C07C51/23
CPC分类号： C07C51/265
摘要： A process for producing 2,6-naphthalenedicarboxylic acid which comprises oxidizing 2,6-diisopropylnaphthalene or its oxidation product as a starting material with molecular oxygen in a reaction medium containing at least 50% by weight of an aliphatic monocarboxylic acid having not more than 3 carbon atoms in the presence of an oxidation catalyst comprising (A) at least one heavy metal element selected from the group consisting of cobalt and manganese, and (B) bromine element, the 2,6-diisopropylnaphthalene and/or its oxidation product being used in a proportion of 0.1 to 5 moles per gram-atom of the heavy metal element of the oxidation catalyst.
摘要翻译：一种生产2,6-萘二羧酸的方法，其包括在反应介质中将2,6-二异丙基萘或其氧化产物作为起始原料用分子氧氧化，所述反应介质含有至少50重量％的不超过3重量％的脂肪族单羧酸在包含（A）至少一种选自钴和锰的重金属元素和（B）溴元素的氧化催化剂的存在下，使用2,6-二异丙基萘和/或其氧化产物的氧化催化剂每克原子的氧化催化剂的重金属元素为0.1-5摩尔。

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