公开(公告)号：US4895680A

公开(公告)日：1990-01-23

申请号：US000247

申请日：1987-01-02

申请人： Paul E. Ellis, Jr. ,  James E. Lyons ,  Harry K. Myers, Jr.

发明人： Paul E. Ellis, Jr. ,  James E. Lyons ,  Harry K. Myers, Jr.

IPC分类号： B01J27/24 ,  B01J31/18 ,  C07C29/50 ,  C07C45/33 ,  C07C45/34 ,  C07C45/35 ,  C07C45/36

CPC分类号： B01J31/1815 ,  B01J27/24 ,  B01J31/1805 ,  B01J31/183 ,  C07C29/50 ,  C07C45/33 ,  C07C45/34 ,  C07C45/35 ,  C07C45/36 ,  C12C11/02 ,  B01J2531/025 ,  B01J2531/56 ,  B01J2531/57 ,  B01J2531/62 ,  B01J2531/64 ,  B01J2531/66 ,  B01J2531/72 ,  B01J2531/821 ,  B01J2531/822 ,  B01J2531/825 ,  B01J2531/827 ,  B01J2531/842 ,  B01J2531/845 ,  C07C2101/14

摘要： Hydrocarbon, and particularly lower molecular weight alkanes and cycloalkanes, may readily be oxidized with air or O.sub.2 to form such products as alcohols, ketones, and the like in high yields when there is employed as the catalyst a highly active nitride-activated metal coordination complex having the structure ##STR1## where M is a transition metal; " " is a ligand; and X is a nitride. Certain dimeric forms of the above catalyst are also employed herein. It has also been discovered that Group IV through VIII transition metal nitrides are also highly effective oxidation catalysts for lower molecular weight hydrocarbons such as alkanes.

摘要翻译： 当使用高活性氮化物活化的金属配位络合物作为催化剂时，烃，特别是低分子量烷烃和环烷烃可以容易地用空气或O 2氧化形成醇，酮等产物， 具有结构，其中M是过渡金属; “”是配体; X是氮化物。 上述催化剂的某些二聚体形式也用于本文。 还发现，IV族至VIII族过渡金属氮化物也是用于低分子量烃如烷烃的高效氧化催化剂。

公开(公告)号：US4613411A

公开(公告)日：1986-09-23

申请号：US803199

申请日：1985-12-02

申请人： Chao-Yang Hsu ,  Paul E. Ellis, Jr.

发明人： Chao-Yang Hsu ,  Paul E. Ellis, Jr.

IPC分类号： C07C41/58 ,  B01D3/36

CPC分类号： C07C41/58 ,  C07C41/56

摘要： Diethoxymethane (ethylal), prepared by reacting formaldehyde with ethanol, may be recovered from the product mixture in substantially pure form by first distilling off an azeotrope comprising ethanol and diethoxymethane, adding a selected solvent to the azeotrope which will form an azeotrope with the ethanol, distilling off said latter azeotrope and recovering the substantially pure diethoxymethane.

摘要翻译： 通过甲醛与乙醇反应制备的二乙氧基甲烷（乙基）可以从产物混合物中以基本上纯的形式回收，首先蒸馏出包含乙醇和二乙氧基甲烷的共沸物，向与乙醇形成共沸物的共沸物中加入选定的溶剂， 蒸馏掉后一种共沸物并回收基本上纯的二乙氧基甲烷。

公开(公告)号：US4542119A

公开(公告)日：1985-09-17

申请号：US598935

申请日：1984-04-11

申请人： Chao-Yang Hsu ,  Paul E. Ellis, Jr.

发明人： Chao-Yang Hsu ,  Paul E. Ellis, Jr.

IPC分类号： B01J31/18 ,  B01J31/24 ,  C07C45/50 ,  B01J27/08 ,  B01J27/10

CPC分类号： C07C45/50 ,  B01J31/2409 ,  B01J2231/321 ,  B01J2531/828 ,  B01J31/1895

摘要： Olefins are hydroformylated with syngas in the presence of a novel organo metallic complex catalyst to form the corresponding aldehydes at high reaction rate and improved selectivity of linear aldehydes over branched aldehydes.The novel catalyst comprises an organo metallic complex formed from a mixture of:(1) platinum (II) acetylacetonate;(2) a Group IVB metal halide; and(3) a bidentate tertiary ligand of the formulaR.sub.1 R.sub.2 Q(CH.sub.2).sub.m QR.sub.3 R.sub.4 ; or ##STR1## wherein Q is arsenic, antimony, or phosphorus; and R.sub.1,R.sub.2,R.sub.3 and R.sub.4 are alkyl, alkoxyl, aryl, or aryloxyl groups, and may be the same or different; and m is an integer of from 3 to about 5; and n is an integer of from 2 to about 4.

摘要翻译： 烯烃在新的有机金属配合物催化剂存在下用合成气进行加氢甲酰化，以高反应速率形成相应的醛，并提高线性醛与分支醛的选择性。 新型催化剂包含由以下混合物形成的有机金属络合物：（1）乙酰丙酮铂（II）; （2）ⅣB族金属卤化物; 和（3）式R1R2Q（CH2）mQR3R4的二齿叔配体; 或其中Q是砷，锑或磷; 并且R 1，R 2，R 3和R 4是烷基，烷氧基，芳基或芳氧基，并且可以相同或不同; m为3〜5的整数; n为2〜4的整数。

公开(公告)号：US07504357B2

公开(公告)日：2009-03-17

申请号：US11805797

申请日：2007-05-24

申请人： Paulette N. Hazin ,  Paul E. Ellis, Jr.

发明人： Paulette N. Hazin ,  Paul E. Ellis, Jr.

IPC分类号： B01J23/00 ,  B01J21/00 ,  B01J20/00 ,  B01J31/00 ,  B01J37/00

CPC分类号： B01J23/002 ,  B01J23/08 ,  B01J23/18 ,  B01J23/20 ,  B01J23/28 ,  B01J23/30 ,  B01J23/31 ,  B01J23/686 ,  B01J37/0036 ,  B01J37/0045 ,  B01J37/009 ,  B01J37/0236 ,  B01J2523/00 ,  C07C51/215 ,  C07C253/24 ,  Y02P20/52 ,  C07C57/04 ,  C07C255/08 ,  B01J2523/18 ,  B01J2523/53 ,  B01J2523/55 ,  B01J2523/56 ,  B01J2523/68 ,  B01J2523/32 ,  B01J2523/54 ,  B01J2523/69 ,  B01J2523/19

摘要： A catalyst composition having the formula: Mo1VaSbbNbcMdOx wherein M is gallium, bismuth, silver or gold, a is 0.01 to 1, b is 0.01 to 1, c is 0.01 to 1, d is 0.01 to 1 and x is determined by the valence requirements of the other components. Other metals, such as tantalum, titanium, aluminum, zirconium, chromium, manganese, iron, ruthenium, cobalt, rhodium, nickel, platinum, boron, arsenic, lithium, sodium, potassium, rubidium, calcium, beryllium, magnesium, cerium, strontium, hafnium, phosphorus, europium, gadolinium, dysprosium, holmium, erbium, thulium, terbium, ytterbium, lutetium, lanthanum, scandium, palladium, praseodymium, neodymium, yttrium, thorium, tungsten, cesium, zinc, tin, germanium, silicon, lead, barium or thallium may also be components of the catalyst. This catalyst is prepared by co-precipitation of metal compounds which are calcined to form a mixed metal oxide catalyst that can be used for the selective conversion of an alkane to an unsaturated carboxylic acid in a one-step process.

摘要翻译： 具有下式的催化剂组合物：<？in-line-formula description =“In-line Formulas”end =“lead”？> Mo1VaSbbNbcMdOx <？in-line-formula description =“In-line Formulas”end =“tail” 其中M为镓，铋，银或金，a为0.01至1，b为0.01至1，c为0.01至1，d为0.01至1，x由其它组分的化合价要求确定。 其他金属如钽，钛，铝，锆，铬，锰，铁，钌，钴，铑，镍，铂，硼，砷，锂，钠，钾，铷，钙，铍，镁，铈，锶 铪，磷，铕，钆，镝，钬，铒，ium，铽，镱，镥，镧，钪，钯，镨，钕，钇，钍，钨，铯，锌，锡，锗，硅，铅 钡或铊也可以是催化剂的组分。 该催化剂通过共沉淀金属化合物制备，金属化合物被煅烧以形成可用于在一步法中将烷烃选择性转化为不饱和羧酸的混合金属氧化物催化剂。

公开(公告)号：US20080188681A1

公开(公告)日：2008-08-07

申请号：US11702395

申请日：2007-02-05

申请人： Wugeng Liang ,  Paul E. Ellis ,  Joseph R. Linzer

发明人： Wugeng Liang ,  Paul E. Ellis ,  Joseph R. Linzer

IPC分类号： C07C51/235 ,  B01J27/199 ,  C01B25/37

CPC分类号： B01J27/199 ,  B01J23/002 ,  B01J35/023 ,  B01J35/1009 ,  B01J35/1038 ,  B01J37/0036 ,  B01J37/03 ,  B01J37/04 ,  B01J2523/00 ,  C07C51/252 ,  C07C57/04 ,  B01J2523/15 ,  B01J2523/17 ,  B01J2523/305 ,  B01J2523/51 ,  B01J2523/53 ,  B01J2523/54 ,  B01J2523/55 ,  B01J2523/68

摘要： The invention is a supported or bound heteropoly acid catalyst composition, a method of making the catalyst composition and a process for the oxidation of saturated and/or unsaturated aldehydes to unsaturated carboxylic acids using the catalyst composition. The catalyst composition has a heteropoly acid component containing molybdenum, vanadium, phosphorus and cesium and support/binder having a surface area of about 0.1 m2/g to about 1.0 m2/g.The catalyst is made by dissolving compounds of the components of each of the heteropoly acid compounds in a solution, precipitating the heteropoly acid compounds, contacting the heteropoly acid compounds to form a catalyst precursor and calcining the catalyst precursor to form a heteropoly acid compound catalyst.Unsaturated aldehydes, such as methacrolein, may be oxidized in the presence of the heteropoly acid compound catalyst to produce an unsaturated carboxylic acid, such as methacrylic acid.

摘要翻译： 本发明是负载或结合的杂多酸催化剂组合物，制备催化剂组合物的方法和使用催化剂组合物将饱和和/或不饱和醛氧化成不饱和羧酸的方法。 催化剂组合物具有包含钼，钒，磷和铯的杂多酸组分和表面积为约0.1m 2 / g至约1.0m 2的载体/粘合剂， /G。 将各种杂多酸化合物的组分的化合物溶解在溶液中，沉淀杂多酸化合物，使杂多酸化合物接触形成催化剂前体并煅烧催化剂前体以形成杂多酸化合物催化剂来制备催化剂。 不饱和醛如甲基丙烯醛可在杂多酸化合物催化剂存在下被氧化，生成不饱和羧酸，如甲基丙烯酸。

公开(公告)号：US5990363A

公开(公告)日：1999-11-23

申请号：US175057

申请日：1993-12-29

申请人： Tilak Wijesekera ,  James E. Lyons ,  Paul E. Ellis, Jr.

发明人： Tilak Wijesekera ,  James E. Lyons ,  Paul E. Ellis, Jr.

IPC分类号： B01J27/24 ,  B01J31/18 ,  B01J31/22 ,  C07B61/00 ,  C07C27/00 ,  C07C29/132 ,  C07C29/50 ,  C07C31/02 ,  C07C31/10 ,  C07C45/33 ,  C07C45/34 ,  C07C45/35 ,  C07C45/36 ,  C07C45/53 ,  C07C51/215 ,  C07C51/235 ,  C07C51/245 ,  C07C51/25 ,  C07C51/265 ,  C07C409/16 ,  C07D487/22 ,  C07F15/02

CPC分类号： C07F15/025 ,  B01J27/24 ,  B01J31/1815 ,  C07C29/132 ,  C07C29/50 ,  C07C45/33 ,  C07C45/34 ,  C07C45/35 ,  C07C45/36 ,  C07C45/53 ,  C07C51/215 ,  C07C51/235 ,  C07C51/245 ,  C07C51/25 ,  C07C51/252 ,  C07C51/265 ,  C07D487/22 ,  B01J2531/025 ,  B01J2531/72 ,  B01J2531/821 ,  B01J2531/842 ,  B01J2531/845

摘要： The invention comprises a method for the oxidation of alkanes to alcohols and for decomposition of hydroperoxides to alcohols utilizing new compositions of matter, which are metal complexes of porphyrins. Preferred complexes have hydrogen, haloalkyl or haloaryl groups in meso positions, two of the opposed meso atoms or groups being hydrogen or haloaryl, and two of the opposed meso atoms or groups being hydrogen or haloalkyl, but not all four of the meso atoms or groups being hydrogen. Other preferred complexes are ones in which all four of the meso positions are substituted with haloalkyl groups and the beta positions are substituted with halogen atoms. A new method of synthesizing porphyrinogens is also disclosed.

摘要翻译： 本发明包括使用作为卟啉的金属络合物的物质的新组合物将烷烃氧化成醇并将氢过氧化物分解成醇的方法。 优选的络合物在中间位置具有氢，卤代烷基或卤代芳基，两个相对的内消旋原子或基团是氢或卤代芳基，两个相对的内消旋原子或基团是氢或卤代烷基，但不是全部四个中子原子或基团 是氢。 其它优选的络合物是其中全部四个中间位置被卤代烷基取代并且β位被卤素原子取代的络合物。 还公开了一种合成卟啉原体的新方法。

公开(公告)号：US5817881A

公开(公告)日：1998-10-06

申请号：US902931

申请日：1997-07-30

申请人： Paul E. Ellis ,  James E. Lyons ,  Harry K. Myers, Jr. ,  Shahid N. Shaikh

发明人： Paul E. Ellis ,  James E. Lyons ,  Harry K. Myers, Jr. ,  Shahid N. Shaikh

IPC分类号： B01J23/881 ,  B01J27/188 ,  C07C29/50 ,  C07C45/33

CPC分类号： C07C29/50 ,  B01J23/881 ,  B01J27/188 ,  C07C45/33

摘要： Alkanes are catalytically oxidized in air or oxygen using iron-substituted polyoxoanions (POAs) of the formula: H.sub.e-z �(n-C.sub.4 H.sub.9).sub.4 N!.sub.z (XM.sub.11 M'O.sub.39).sup.-eThe M' (e.g., iron(III)/iron(II)) reduction potential of the POAs is affected by selection of the central atom X and the framework metal M, and by the number of tetrabutyl-ammonium groups. Decreased Fe(III)/Fe(II) reduction potential has been found to correlate to increased oxidation activity.

摘要翻译： 烷烃在空气或​​氧气中使用下式的铁取代的聚氧阴离子（POA）催化氧化：He-z [（n-C4H9）4N] z（XM11M'O39）-e M'（例如铁（III）/ 铁（II））还原电位受中心原子X和骨架金属M的选择以及四丁基铵基团的数量的影响。 已经发现Fe（III）/ Fe（II）还原电位的降低与增加的氧化活性相关。

公开(公告)号：US5705685A

公开(公告)日：1998-01-06

申请号：US565206

申请日：1995-10-31

申请人： James E. Lyons ,  Paul E. Ellis, Jr. ,  Swati Karmakar ,  Shahid N. Shaikh

发明人： James E. Lyons ,  Paul E. Ellis, Jr. ,  Swati Karmakar ,  Shahid N. Shaikh

IPC分类号： B01J27/186 ,  B01J23/24 ,  B01J27/188 ,  C07B61/00 ,  C07C51/215 ,  C07C51/225 ,  C07C57/05 ,  C07C51/16

CPC分类号： B01J27/188 ,  B01J23/24 ,  C07C51/215

摘要： Alkanes are converted to unsaturated carboxylic acids by contacting an alkane with an oxidizing agent and a heteropolyacid or polyoxoanion comprising (1) at least 9 atoms of a first framework metal or metals comprising molybdenum, tungsten or vanadium or combinations thereof and (2) 1 to 3 atoms of a second framework metal or metals comprising zinc or a transition metal different from the first framework metal.

摘要翻译： 烷烃通过使烷烃与氧化剂和杂多酸或多氧阴离子接触而转化为不饱和羧酸，所述烷烃包含（1）至少9个原子的第一骨架金属或包含钼，钨或钒的金属或其组合，和（2）1至 3原子的第二骨架金属或包含不同于第一骨架金属的锌或过渡金属的金属。

公开(公告)号：US5663328A

公开(公告)日：1997-09-02

申请号：US672202

申请日：1996-06-27

申请人： Paul E. Ellis, Jr. ,  James E. Lyons

发明人： Paul E. Ellis, Jr. ,  James E. Lyons

IPC分类号： B01J31/18 ,  C07D487/22 ,  C07C29/50 ,  C07C31/12

CPC分类号： B01J31/1815 ,  B01J2231/70 ,  B01J2531/025 ,  B01J2531/16 ,  B01J2531/26

摘要： The invention provides novel catalyst compositions, useful in the oxidation of hydrocarbons with air or oxygen to form hydroxy-group containing compounds and in the decomposition of hydroperoxides to form hydroxy-group containing compounds. The catalysts comprise transition metal complexes of a porphyrin ring having 1 to 12 halogen substituents on the porphyrin ring, at least one of said halogens being in a meso position and/or the catalyst containing no aryl group in a meso position. The compositions are prepared by halogenating a transition metal complex of a porphyrin. In one embodiment, a complex of a porphyrin with a metal whose porphyrin complexes are not active for oxidation of hydrocarbons is halogenated, thereby to obtain a haloporphyrin complex of that metal, the metal is removed from the haloporphyrin complex to obtain the free base form of the haloporphyrin, and a metal such as iron whose porphyrin complexes are active for oxidation of hydrocarbons and for the decomposition of alkyl hydroperoxides is complexed with the free base to obtain an active catalyst for oxidation of hydrocarbons and decomposition of alkyl hydroperoxides.

摘要翻译： 本发明提供了新的催化剂组合物，其可用于用空气或氧气氧化烃以形成含羟基化合物，并在氢过氧化物的分解中形成含羟基化合物。 催化剂包括在卟啉环上具有1至12个卤素取代基的卟啉环的过渡金属络合物，所述卤素中的至少一个在中间位置和/或在中间位置不含芳基的催化剂。 通过卤化卟啉的过渡金属络合物制备组合物。 在一个实施方案中，卟啉与卟啉络合物对于烃的氧化不起作用的金属的络合物被卤化，从而获得该金属的卤卟啉络合物，从卤卟啉络合物中除去金属，得到游离碱形式 卤卟啉和卟啉配合物对烃的氧化和烷基氢过氧化物的分解具有活性的金属如铁，与游离碱络合，得到烃的氧化和烷基氢过氧化物的分解的活性催化剂。

公开(公告)号：US5395988A

公开(公告)日：1995-03-07

申请号：US223090

申请日：1994-04-04

申请人： Manoj V. Bhinde ,  James E. Lyons ,  Paul E. Ellis, Jr.

发明人： Manoj V. Bhinde ,  James E. Lyons ,  Paul E. Ellis, Jr.

IPC分类号： A62D3/00 ,  A62D3/37 ,  A62D101/28 ,  C07C29/132 ,  C07C31/12 ,  C07C35/08 ,  C07C45/53 ,  C07C407/00 ,  C07C29/00 ,  C07C33/22 ,  C07C35/14

CPC分类号： A62D3/37 ,  C07C29/132 ,  C07C31/12 ,  C07C35/08 ,  C07C407/003 ,  C07C45/53 ,  A62D2101/28 ,  C07C2101/14

摘要： Organic hydroperoxides are decomposed by drying a reaction mixture containing the organic hydroperoxide and an organic solvent and contacting the dried reaction mixture with a metal organic ligand catalyst under hydroperoxide decomposition conditions. An organic co-solvent for the hydroperoxide may also be used.

摘要翻译： 通过干燥含有机氢过氧化物和有机溶剂的反应混合物分解有机氢过氧化物，并在氢过氧化物分解条件下使干燥的反应混合物与金属有机配体催化剂接触。 也可以使用氢过氧化物的有机助溶剂。