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1.发明授权
公开(公告)号：US5792890A
公开(公告)日：1998-08-11
申请号：US792033
申请日：1997-02-03
申请人： Pei-Shing Eugene Dai , Laurence Darrel Neff , Kyle Lee Preston , Rei-Yu Judy Hwan , John Frederick Knifton
发明人： Pei-Shing Eugene Dai , Laurence Darrel Neff , Kyle Lee Preston , Rei-Yu Judy Hwan , John Frederick Knifton
摘要： A tertiary butyl alcohol charge stock contaminated with from about 0.5 to about 2 wt. % of corrosive oxygen-containing impurities, including peroxides and formates, is passed through an oxygenates decomposition reactor containing a bed of a basic zeolite catalyst to decompose the peroxides and oxygen-containing impurities, including peroxides and formates, and to dehydrate a portion of the tertiary butyl alcohol to form isobutylene and water to form a substantially less-corrosive tertiary butyl alcohol feedstock that is substantially free from oxygen-containing impurities, including formates that is suitable for reaction with methanol in a methyl tertiary butyl ether etherification reactor to form a methyl tertiary butyl ether etherification reaction product from which methyl tertiary butyl ether can be recovered.
摘要翻译： 叔丁醇装料被约0.5至约2wt。 含有过氧化物和甲酸盐的含腐蚀性含氧杂质的％通过含有碱性沸石催化剂床的含氧化合物分解反应器，以分解过氧化物和含氧杂质，包括过氧化物和甲酸盐，并使部分 叔丁醇形成异丁烯和水，以形成基本上不含氧的杂质的基本上较低腐蚀性的叔丁醇原料，包括适用于在甲基叔丁基醚醚化反应器中与甲醇反应形成甲基 可以回收甲基叔丁基醚的叔丁基醚醚化反应产物。
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2.发明授权
公开(公告)号：US5811597A
公开(公告)日：1998-09-22
申请号：US703269
申请日：1996-08-26
申请人： Rei-Yu Judy Hwan , Mark Elliott Taylor , John Frederick Knifton , Melvin Ernest Stockton , John Ronald Sanderson
发明人： Rei-Yu Judy Hwan , Mark Elliott Taylor , John Frederick Knifton , Melvin Ernest Stockton , John Ronald Sanderson
摘要： Methyl tertiary butyl ether is prepared from contaminated TBA by reactively distilling the contaminated TBA in a reactive distillation column to provide a lower boiling isobutylene fraction and a higher boiling aqueous TBA fraction, by distilling the higher boiling aqueous TBA fraction to provide a lower boiling TBA fraction, by charging the lower boiling isobutylene fraction, the lower boiling tertiary butyl alcohol fraction and methanol to an etherification reactor to form an etherification reaction product, by distilling the etherification reaction product to provide a lower boiling fraction containing isobutylene, methanol and methyl tertiary butyl ether by charging the lower boiling fraction to a finishing reactor to react the isobutylene and methanol contained therein to from additional MTBE and by recovering MTBE from the etherification reaction product and the isobutylene conversion product.
摘要翻译： 通过在反应性蒸馏塔中反应性蒸馏被污染的TBA以提供较低沸点的异丁烯级分和较高沸点的TBA级分，通过蒸馏高沸点TBA级分来提供较低沸点的TBA级分，由受污染的TBA制备甲基叔丁基醚 通过将低沸点异丁烯级分，低沸点叔丁醇级分和甲醇加入到醚化反应器中以形成醚化反应产物，通过蒸馏醚化反应产物以提供含有异丁烯，甲醇和甲基叔丁基醚的低沸点馏分 通过将较低沸点馏分装入精整反应器以使其中所含的异丁烯和甲醇与另外的MTBE反应，并从醚化反应产物和异丁烯转化产物中回收MTBE。
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3.发明授权Two-stage etherification of tertiary butyl alcohol using second stage zeolite catalysts for the intermediate preparation of isobutylene 失效使用第二阶段沸石催化剂对二丁基二醇进行二阶段醚化，用于中间体制备异丁烯
公开(公告)号：US5856588A
公开(公告)日：1999-01-05
申请号：US774339
申请日：1996-12-30
IPC分类号： B01J29/00 , B01J29/08 , B01J29/85 , B01J37/26 , C07B61/00 , C07C41/09 , C07C43/04 , C07C41/00
CPC分类号： B01J29/005 , B01J29/084 , B01J29/85 , C07C41/09 , C07C41/42 , Y10S977/775 , Y10S977/896
摘要： Methyl tertiary butyl ether is prepared from tertiary butyl alcohol and methanol in a plural stage process by (a) reacting tertiary butyl alcohol with methanol in a primary MTBE reaction zone containing a cationic ion-exchange resin catalyst to form a primary reaction product, (b) fractionating the primary reaction product in a primary distillation zone to provide a first lighter, lower boiling distillation fraction comprising isobutylene, methanol and methyl tertiary butyl ether and a first heavier, higher boiling distillation fraction comprising methanol, tertiary butyl alcohol and water, c) contacting the first heavier distillation fraction in a second stage reactor containing a second stage acidic, fluoride-treated Y-zeolite having a silica:alumina ratio of 100:1 to 10:1 and a unit cell size of from 24.20 to 24.45 .ANG. or a fluoride-treated silicoaluminophosphate (SAPO) molecular sieve having a pore size of from 5 .ANG. to 8 .ANG., under conversion conditions including a temperature of from 20.degree. to 300.degree. C. and a pressure of from 0 to 1000 psig to form a second stage reaction product rich in isobutylene and also containing methyl tertiary butyl ether; and (d) converting the isobutylene to additional methyl tertiary butyl ether.
摘要翻译： （a）在含有阳离子离子交换树脂催化剂的初级MTBE反应区中使叔丁醇与甲醇反应形成初级反应产物（b），由叔丁醇和甲醇在多级方法中制备甲基叔丁基醚 ）在一级蒸馏区中分馏初级反应产物以提供包含异丁烯，甲醇和甲基叔丁基醚的第一种较轻的低沸点馏分和包含甲醇，叔丁醇和水的第一较重较高沸点馏分，c） 在第二级反应器中接触第一较重蒸馏馏分，该第二级反应器含有二氧化硅：氧化铝比为100:1至10:1的第二阶段酸性，氟化物处理的Y-沸石，以及单位晶胞尺寸为24.20至24.45ng / 氟化物处理的硅铝磷酸盐（SAPO）分子筛，其孔径为5至8安培姆，转化条件包括 温度为20-300℃，压力为0-1000psig，形成富含异丁烯并含甲基叔丁基醚的第二阶段反应产物; 和（d）将异丁烯转化成另外的甲基叔丁基醚。
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公开(公告)号：US5716896A
公开(公告)日：1998-02-10
申请号：US346449
申请日：1994-11-29
CPC分类号： C07C41/09
摘要： Disclosed is a method for producing alkyl tertiary alkyl ethers which comprises reacting t-butanol with an alkanol in the presence of a catalyst which exhibits extended life comprising .beta.-zeolite modified with one or more metals selected from the group consisting of Group IA and Group IIIB of the Periodic Table and continuously contacting said alkanol and t-butanol in a molar amount from about 10:1 to 1:10 over said zeolite catalyst at a temperature of about 20.degree. C. to about 250.degree. C. and a pressure of about atmospheric to about 1000 psig.
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5.发明授权公开(公告)号：US07115540B2
公开(公告)日：2006-10-03
申请号：US10669485
申请日：2003-09-24
申请人： Joseph Broun Powell , Paul Richard Weider , John Frederick Knifton , Kevin Dale Allen , Lynn Henry Slaugh , Juan Pedro Arhancet
发明人： Joseph Broun Powell , Paul Richard Weider , John Frederick Knifton , Kevin Dale Allen , Lynn Henry Slaugh , Juan Pedro Arhancet
CPC分类号： B01J31/2471 , B01J31/1805 , B01J31/1815 , B01J31/183 , B01J31/20 , B01J31/24 , B01J31/28 , B01J2231/321 , B01J2531/025 , B01J2531/16 , B01J2531/80 , B01J2531/82 , B01J2531/821 , B01J2531/824 , B01J2531/828 , B01J2531/845 , C07C29/16 , Y02P20/584 , C07C31/205
摘要： This invention is a process for synthesizing aliphatic 1,3-diols in one step by hydroformylation and hydrogenation of oxirane, carbon monoxide, and hydrogen employing a catalyst comprising a cobalt carbonyl compound and a cocatalyst metal compound ligated with a ligand in a ligand to cocatalyst metal atom molar ratio in the range of 0.2:1.0 to 0.6:1.0, optionally in the presence of a promoter, where recovery of product is preferably accomplished via water extraction of a diol rich phase from the bulk reaction mixture. The process modifications can, particularly in combination, be beneficial with respect to product recovery, catalyst recycle, and overall economics of a one-step process for producing aliphatic 1,3-diols.
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6.发明授权One-step production of 1,3-propanediol from ethylene oxide and syngas with a catalyst with a N-heterocyclic ligand 失效从环氧乙烷和合成气一步生产1,3-丙二醇与催化剂与N-杂环配体公开(公告)号：US06903044B2
公开(公告)日：2005-06-07
申请号：US10298866
申请日：2002-11-18
申请人： John Frederick Knifton , Talmadge Gail James , Kevin Dale Allen , Paul Richard Weider , Joseph Broun Powell , Lynn Henry Slaugh , Timothy Williams
发明人： John Frederick Knifton , Talmadge Gail James , Kevin Dale Allen , Paul Richard Weider , Joseph Broun Powell , Lynn Henry Slaugh , Timothy Williams
IPC分类号： B01J31/28 , B01J31/18 , B01J31/20 , C07B61/00 , C07C29/16 , C07C29/44 , C07C31/20 , B01J31/00
CPC分类号： C07C29/16 , B01J31/181 , B01J31/1815 , B01J31/183 , B01J31/20 , B01J31/28 , B01J2231/48 , B01J2531/0208 , B01J2531/025 , B01J2531/821 , B01J2531/845 , Y02P20/52 , C07C31/205
摘要： Disclosed is a new catalyst composition comprising a bimetallic Co—Ru catalyst complexed with a N-heterocylcic ligand that is effective, economical, and provides improvements in oxidative stability in the one step synthesis of 1,3-propanediol (1,3-PDO) from ethylene oxide and synthesis gas. For example, cobalt-ruthenium-2,2′-bipyrimidine, 2,2′-dipyridyl, or 2,4,6-tripridyl-s-triazine catalyst precursors in cyclic ether solvents, such as 1,3-dioxolane, 1,4-dioxolane, 1,4-dioxane, and 2-ethyl-2-methyl-1,3-dioxolane, provide good yields of 1,3-PDO in a one step synthesis.
摘要翻译： 公开了一种新的催化剂组合物，其包含与N-杂环配体络合的双金属Co-Ru催化剂，该双金属Co-Ru催化剂有效，经济，并且在一步合成1,3-丙二醇（1,3-PDO）中提供氧化稳定性的改善， 来自环氧乙烷和合成气。 例如，在环醚溶剂中的钴 - 钌-2,2'-联嘧啶，2,2'-二吡啶基或2,4,6-三苯基-s-三嗪催化剂前体，如1,3-二氧戊环， 4-二氧戊环，1,4-二恶烷和2-乙基-2-甲基-1,3-二氧戊环，在一步合成中可提供1,3-PDO的良好产率。
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公开(公告)号：US06545190B2
公开(公告)日：2003-04-08
申请号：US09963068
申请日：2001-09-25
IPC分类号： C07C2700
CPC分类号： C07C29/16 , Y02P20/582 , Y02P20/584 , C07C31/205
摘要： Disclosed is a one step hydroformylation process for preparing a 1,3-diol, comprising the reaction of an oxirane with syngas at hydroformylation conditions in an inert solvent in the presence of a hydroformylation catalyst comprising a ruthenium (+1)-phosphine bidentate: cobalt (−1) complex, wherein the ligated metal is ruthenium, under conditions which preferably upon completion of the oxirane/syngas reaction cause a phase separation of the reaction mixture into a solvent phase which is rich in catalyst and a second phase which is rich in the 1,3-diol, recycling the phase rich in catalyst directly to the hydroformylation reaction for further reaction with previously unreacted starting materials, thus permitting valuable hydroformylation catalyst to be recycled without degradation or exposure to downstream processing and recovering the 1,3-diol from the second phase rich in 1,3-diol.
摘要翻译： 公开了一种用于制备1,3-二醇的一步加氢甲酰化方法，其包括在加氢甲酰化条件下，在惰性溶剂中，在加氢甲酰化催化剂存在下，环氧乙烷与合成气的反应，所述加氢甲酰化催化剂包含钌（+1） - 膦二齿：钴 （-1）络合物，其中连接的金属是钌，在优选在完成环氧乙烷/合成气反应的条件下，使反应混合物相分离成富含催化剂的溶剂相和富含 该1,3-二醇将富含催化剂的相直接再循环到加氢甲酰化反应中以进一步与先前未反应的起始原料反应，从而允许有价值的加氢甲酰化催化剂再循环而不降解或暴露于下游加工并回收1,3-二醇 从第二阶段富含1,3-二醇。
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公开(公告)号：US06518466B2
公开(公告)日：2003-02-11
申请号：US09957279
申请日：2001-09-20
申请人： John Frederick Knifton , Lynn Henry Slaugh , Paul Richard Weider , Talmadge Gail James , Joseph Broun Powell , Kevin Dale Allen , Timothy Scott Williams
发明人： John Frederick Knifton , Lynn Henry Slaugh , Paul Richard Weider , Talmadge Gail James , Joseph Broun Powell , Kevin Dale Allen , Timothy Scott Williams
IPC分类号： C07C2700
CPC分类号： B01J31/2409 , B01J31/20 , B01J31/24 , B01J31/2414 , B01J31/248 , B01J2231/48 , B01J2531/821 , B01J2531/845 , C07C29/16 , Y02P20/52 , Y02P20/584 , C07C31/205
摘要： The invention provides a process for an improved oxirane hydroformylation catalyst, the improved oxirane hydroformylation catalyst, and a one step process for preparing a 1,3-diol in the presence of such a catalyst. One process for preparing the hydroformylation catalyst involves: a) forming a complex (A) by contacting a ruthenium(0) compound with a ditertiary phosphine ligand; and b) forming a complex (B) by subjecting complex (A) to a redox reaction with a cobalt(0) carbonyl compound. This catalyst is used in a one step hydroformylation process for preparing a 1,3-diol, comprising the reaction of an oxirane with syngas at hydroformylation conditions in an inert solvent in the presence of the above hydroformylation catalyst where recovery of product is preferably accomplished via phase separation of a diol rich phase from the bulk reaction liquor.
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公开(公告)号：US06468940B1
公开(公告)日：2002-10-22
申请号：US09957561
申请日：2001-09-20
申请人： John Frederick Knifton , Lynn Henry Slaugh , Paul Richard Weider , Talmadge Gail James , Joseph Broun Powell , Kevin Dale Allen , Timothy Scott Williams
发明人： John Frederick Knifton , Lynn Henry Slaugh , Paul Richard Weider , Talmadge Gail James , Joseph Broun Powell , Kevin Dale Allen , Timothy Scott Williams
IPC分类号： B01J3100
CPC分类号： B01J31/2409 , B01J31/20 , B01J31/24 , B01J31/2414 , B01J31/248 , B01J2231/48 , B01J2531/821 , B01J2531/845 , C07C29/16 , Y02P20/52 , Y02P20/584 , C07C31/205
摘要： The invention provides a process for an improved oxirane hydroformylation catalyst, the improved oxirane hydroformylation catalyst, and a one step process for preparing a 1,3-diol in the presence of such a catalyst. One process for preparing the hydroformylation catalyst involves: a) forming a complex (A) by contacting a ruthenium(0) compound with a ditertiary phosphine ligand; and b) forming a complex (B) by subjecting complex (A) to a redox reaction with a cobalt(0) carbonyl compound. This catalyst is used in a one step hydroformylation process for preparing a 1,3-diol, comprising the reaction of an oxirane with syngas at hydroformylation conditions in an inert solvent in the presence of the above hydroformylation catalyst where recovery of product is preferably accomplished via phase separation of a diol rich phase from the bulk reaction liquor.
摘要翻译： 本发明提供改进的环氧乙烷加氢甲酰化催化剂，改进的环氧乙烷加氢甲酰化催化剂的方法，以及在这种催化剂存在下制备1,3-二醇的一步法。 制备加氢甲酰化催化剂的一个方法包括：a）通过使钌（O）化合物与二膦配体接触形成络合物（A）; 和b）通过使复合物（A）与羰基钴（O）化合物进行氧化还原反应形成络合物（B）。 该催化剂用于制备1,3-二醇的一步加氢甲酰化方法，其包括在上述加氢甲酰化催化剂存在下，在惰性溶剂中，在加氢甲酰化条件下使环氧乙烷与合成气反应，其中产物的回收优选通过 富二醇相与本体反应液相分离。
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10.发明授权Reduction of the viscosity of reactive heavy byproducts during the production of 1,3-propanediol 失效在1,3-丙二醇生产过程中降低反应性重副产物的粘度公开(公告)号：US07276634B2
公开(公告)日：2007-10-02
申请号：US10676682
申请日：2003-10-01
申请人： John Frederick Knifton , Talmadge Gail James , Paul Richard Weider , Joseph Broun Powell , Edward Lewis Nielsen , Glenn Charles Komplin
发明人： John Frederick Knifton , Talmadge Gail James , Paul Richard Weider , Joseph Broun Powell , Edward Lewis Nielsen , Glenn Charles Komplin
IPC分类号： C07C27/10
CPC分类号： C07C45/58 , C07C29/141 , C07C31/205
摘要： The present invention is an improvement upon the process for the production of 1,3-propanediol wherein an aqueous solution of 3-hydroxy propanal is formed, catalyst, if any, used in said formation is removed from the solution, sodium hydroxide is added to the solution to neutralize any acid therein such that the pH is at least about 5, the neutralized aqueous solution is subjected to hydrogenation to produce a crude 1,3-propanediol mixture which is distilled to produce 1,3-propanediol, water, and reactive heavy components. The improvement on this process comprises replacing the sodium hydroxide with a hydroxide selected from the group consisting of ammonium hydroxide, alkali metal hydroxides other than sodium hydroxide, and alkaline earth metal hydroxides to reduce the viscosity of the reactive heavy components.
摘要翻译： 本发明是对生产1,3-丙二醇的方法的改进，其中形成3-羟基丙醛的水溶液，从该溶液中除去所述地层中使用的催化剂（如果有的话），将氢氧化钠加入 中和其中的任何酸使其pH至少约为5的溶液，中和的水溶液进行氢化以产生粗制的1,3-丙二醇混合物，其被蒸馏以产生1,3-丙二醇，水和反应性 重组件。 该方法的改进包括用选自氢氧化铵，氢氧化钠以外的碱金属氢氧化物和碱土金属氢氧化物的氢氧化物代替氢氧化钠，以降低反应性重组分的粘度。
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