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1. 发明授权

US06808652B2 Modified ⊖-alumina-supported nickel reforming catalyst and its use for producing synthesis gas from natural gas 失效
标题翻译：改性⊖-氧化铝负载镍重整催化剂及其在天然气生产合成气中的应用
公开(公告)号：US06808652B2
公开(公告)日：2004-10-26
申请号：US10750756
申请日：2004-01-05
申请人： Sang-Eon Park , Ki-Won Jun , Hyun-Seog Roh , Seung-Chan Baek , Young-Sam Oh , Young-Soon Baek , Ri-Sang Choi , Taek-Yong Song
发明人： Sang-Eon Park , Ki-Won Jun , Hyun-Seog Roh , Seung-Chan Baek , Young-Sam Oh , Young-Soon Baek , Ri-Sang Choi , Taek-Yong Song
IPC分类号： C07C2700
CPC分类号： B01J21/066 , B01J21/04 , B01J23/78 , B01J23/83 , C01B3/40 , C01B2203/0233 , C01B2203/0244 , C01B2203/0261 , C01B2203/1052 , C01B2203/1082 , C01B2203/1241 , Y02P20/52
摘要： A modified ⊖-Al2O3-supported nickel reforming catalyst and its use for producing synthesis gas from natural gas, more specifically to a nickel reforming catalyst expressed by the following formula 1, having improved coke resistance, high-temperature catalysis stability and catalytic activity, which is prepared by coating nickel or mixture of nickel and cocatalyst (M1-M2-Ni) on a Al2O3 support modified with metal (M3-M4-ZrO2/⊖-Al2O3), and its use for producing synthesis gas from natural gas through steam reforming, oxygen reforming or steam-oxygen reforming, M1-M2-Ni/M3-M4-ZrO2/⊖-Al2O3 (1) wherein M1 is an alkali metal; each of M2 and M3 is an alkaline earth metal; and M4 is a IIIB element or a lanthanide.
摘要翻译：改性的⊖-Al 2 O 3负载的镍重整催化剂及其用于从天然气制备合成气的用途，更具体地说，涉及由下式1表示的镍重整催化剂，具有改善的耐焦性，高温催化稳定性和催化活性，通过在用金属（M3-M4-ZrO2 /⊖-Al2O3）改性的Al 2 O 3载体上涂覆镍或镍和助催化剂（M1-M2-Ni）的混合物制备，以及其用于通过蒸汽重整从天然气生产合成气的用途，氧气重整或蒸汽 - 氧气重整，其中M1是碱金属; M2和M3各自为碱土金属; M4是IIIB元素或镧系元素。

2. 发明授权

US06693060B2 Modified &thgr;-Al2O3-supported nickel reforming catalyst and its use for producing synthesis gas from natural gas 失效
标题翻译：改性的θ-Al2O3负载的镍重整催化剂及其从天然气生产合成气的用途
公开(公告)号：US06693060B2
公开(公告)日：2004-02-17
申请号：US10143669
申请日：2002-05-13
申请人： Sang-Eon Park , Ki-Won Jun , Hyun-Seog Roh , Seung-Chan Baek , Young-Sam Oh , Young-Soon Baek , Ri-Sang Choi , Taek-Yong Song
发明人： Sang-Eon Park , Ki-Won Jun , Hyun-Seog Roh , Seung-Chan Baek , Young-Sam Oh , Young-Soon Baek , Ri-Sang Choi , Taek-Yong Song
IPC分类号： B01J2340
CPC分类号： B01J21/066 , B01J21/04 , B01J23/78 , B01J23/83 , C01B3/40 , C01B2203/0233 , C01B2203/0244 , C01B2203/0261 , C01B2203/1052 , C01B2203/1082 , C01B2203/1241 , Y02P20/52
摘要： A modified &thgr;-Al2O3-supported nickel reforming catalyst and its use for producing synthesis gas from natural gas, more specifically to a nickel reforming catalyst expressed by the following formula 1, having improved coke resistance, high-temperature catalysis stability and catalytic activity, which is prepared by coating nickel or mixture of nickel and cocatalyst (M1—M2—Ni) on a &thgr;-Al2O3 support modified with metal (M3—M4—ZrO2/&thgr;-Al2O3), and its use for producing synthesis gas from natural gas through steam reforming, oxygen reforming or steam-oxygen reforming, M1—M2—Ni/M3—M4—ZrO2/&thgr;-Al2O3 (1) wherein M1 is an alkali metal, each of M2 and M3 is an alkaline earth metal; and M4 is a IIIB element or a lanthanide.
摘要翻译：改性的θ-Al 2 O 3负载的镍重整催化剂及其用于从天然气生产合成气的用途，更具体地说，涉及由下式1表示的镍重整催化剂，具有改善的耐焦性，高温催化稳定性和催化活性，通过在用金属（M3-M4-ZrO 2 /θ-Al 2 O 3）改性的θ-Al 2 O 3载体上涂覆镍或镍和助催化剂（M1-M2-Ni）的混合物制备，以及其用于从天然气生产合成气的用途蒸汽重整，氧气重整或蒸汽 - 氧气重整，其中M1是碱金属，M2和M3各自是碱土金属; M4是IIIB元素或镧系元素。

3. 发明授权

US07417004B2 Catalyst for dimethyl ether synthesis and its preparation methods 失效
标题翻译：二甲醚合成催化剂及其制备方法
公开(公告)号：US07417004B2
公开(公告)日：2008-08-26
申请号：US10572707
申请日：2004-08-30
申请人： Ki-Won Jun , Hyun-Seog Roh , Jae-Woo Kim , Jeon Keun Oh , Jin Hwan Bang
发明人： Ki-Won Jun , Hyun-Seog Roh , Jae-Woo Kim , Jeon Keun Oh , Jin Hwan Bang
IPC分类号： B01J29/06
CPC分类号： B01J37/0009 , B01J29/06 , B01J29/18 , B01J29/40 , B01J29/7007 , B01J37/0018 , B01J2229/42 , C07C41/09 , C07C43/043
摘要： This invention relates to a catalyst for synthesis of dimethyl ether and its preparation methods. More specifically, this invention relates to a catalyst with improved formulation for a highly efficient synthesis of dimethyl ether via dehydration of methanol. These catalysts are composed of hydrophobic zeolites, cations selected from alkali metal, alkaline earth metal, or ammonium along with alumina, silica, or silica-alumina. The methods of manufacturing the catalyst of this invention include (a) combining hydrophobic zeolites and precursors of alkali or alkaline earth metal cations with pastes of inorganic binders (at least one selected from the group consisting of bohemites, silica sol, and clay) and calcining the mixture at high temperature; (b) combining particles, which are obtained by calcining the hydrophobic zeolites impregnated with precursors of alkali or alkaline earth metal cations, with pastes of inorganic binders (at least one selected from bohemites, silica sol, and clay) and calcining the mixture at high temperature; (c) combining hydrophobic zeolites with pastes of inorganic binders (at least one selected from the group consisting of bohemites, silica sol, and clay), calcining the mixture at high temperature, impregnating the calcined product with precursors of ammonium cations and calcining the mixture at high temperature. The catalysts of this invention provide significantly high yields of dimethyl ether because they do not result in the production of hydrocarbon side products and their high catalytic activities are maintained for a prolonged period of time.
摘要翻译：本发明涉及二甲醚合成催化剂及其制备方法。更具体地说，本发明涉及具有改进配方的催化剂，用于通过甲醇脱水高效合成二甲醚。这些催化剂由疏水性沸石，选自碱金属，碱土金属或铵以及氧化铝，二氧化硅或二氧化硅 - 氧化铝的阳离子组成。制备本发明的催化剂的方法包括（a）将疏水性沸石和碱金属或碱土金属阳离子的前体与无机粘合剂（至少一种选自由bohemites，硅溶胶和粘土组成的组）和煅烧混合物在高温下; （b）将通过煅烧浸渍有碱金属或碱土金属阳离子前体的疏水性沸石获得的颗粒与无机粘合剂（选自硼酸盐，硅溶胶和粘土中的至少一种）的浆料混合并在高温下煅烧该混合物温度; （c）将疏水性沸石与无机粘合剂（选自由bohemites，硅溶胶和粘土组成的组中选出的至少一种）的混合物组合，在高温下煅烧混合物，将煅烧产物与铵阳离子前体浸渍并煅烧该混合物在高温下。本发明的催化剂提供显着高的二甲醚产率，因为它们不会导致烃副产物的生产，并且它们的高催化活性保持较长时间。

4. 发明申请

US20070117709A1 Catalyst for dimethyl ether synthesis and its preparation methods 失效
标题翻译：二甲醚合成催化剂及其制备方法
公开(公告)号：US20070117709A1
公开(公告)日：2007-05-24
申请号：US10572707
申请日：2004-08-30
申请人： Ki-Won Jun , Hyun-Seog Roh , Jae-Woo Kim , Jeon-Keun Oh , Jin Bang
发明人： Ki-Won Jun , Hyun-Seog Roh , Jae-Woo Kim , Jeon-Keun Oh , Jin Bang
IPC分类号： B01J29/04 , B01J29/06
CPC分类号： B01J37/0009 , B01J29/06 , B01J29/18 , B01J29/40 , B01J29/7007 , B01J37/0018 , B01J2229/42 , C07C41/09 , C07C43/043
摘要： This invention relates to a catalyst for synthesis of dimethyl ether and its preparation methods. More specifically, this invention relates to a catalyst with improved formulation for a highly efficient synthesis of dimethyl ether via dehydration of methanol. These catalysts are composed of hydrophobic zeolites, cations selected from alkali metal, alkaline earth metal, or ammonium along with alumina, silica, or silica-alumina. The methods of manufacturing the catalyst of this invention include (a)combining hydrophobic zeolites and precursors of alkali or alkaline earth metal cations with pastes of inorganic binders (at least one selected from the group consisting of bohemites, silica sol, and clay) and calcining the mixture at high temperature; (b)combining particles, which are obtained by calcining the hydrophobic zeolites impregnated with precursors of alkali or alkaline earth metal cations, with pastes of inorganic binders (at least one selected from bohemites, silica sol, and clay) and calcining the mixture at high temperature; (c)combining hydrophobic zeolites with pastes of inorganic binders (at least one selected from the group consisting of bohemites, silica sol, and clay), calcining the mixture at high temperature, impregnating the calcined product with precursors of ammonium cations and calcining the mixture at high temperature. The catalysts of this invention provide significantly high yields of dimethyl ether because they do not result in the production of hydrocarbon side products and their high catalytic activities are maintained for a prolonged period of time.
摘要翻译：本发明涉及二甲醚合成催化剂及其制备方法。更具体地说，本发明涉及具有改进配方的催化剂，用于通过甲醇脱水高效合成二甲醚。这些催化剂由疏水性沸石，选自碱金属，碱土金属或铵以及氧化铝，二氧化硅或二氧化硅 - 氧化铝的阳离子组成。制备本发明的催化剂的方法包括（a）将疏水性沸石和碱金属或碱土金属阳离子的前体与无机粘合剂（至少一种选自由bohemites，硅溶胶和粘土组成的组）和煅烧混合物在高温下; （b）将通过煅烧浸渍有碱金属或碱土金属阳离子前体的疏水性沸石获得的颗粒与无机粘合剂（选自硼酸盐，硅溶胶和粘土中的至少一种）的浆料混合并在高温下煅烧该混合物温度; （c）将疏水性沸石与无机粘合剂（选自由bohemites，硅溶胶和粘土组成的组中选出的至少一种）的混合物组合，在高温下煅烧混合物，将煅烧产物与铵阳离子前体浸渍并煅烧该混合物在高温下。本发明的催化剂提供显着高的二甲醚产率，因为它们不会导致烃副产物的生产，并且它们的高催化活性保持较长时间。

5. 发明授权

US06740783B1 Process for preparing dimethyl ether from crude methanol 失效
标题翻译：从粗甲醇制备二甲醚的方法
公开(公告)号：US06740783B1
公开(公告)日：2004-05-25
申请号：US10413535
申请日：2003-04-15
申请人： Ki-Won Jun , Hyun-Seog Roh , Kew Ho Lee
发明人： Ki-Won Jun , Hyun-Seog Roh , Kew Ho Lee
IPC分类号： C07C4109
CPC分类号： C07C41/09 , C07C43/043
摘要： The present invention relates to a process for preparing dimethyl ether from crude methanol. More particularly, this invention relates to an improved process for preparing dimethyl ether useful as a fresh fuel as well as a raw material in chemical industry with no generation of hydrocarbon as a by-product and no deactivation of a catalyst, performed in such a manner that the dehydration is carried out using as raw material crude methanol that contains water in the presence of the zeolite catalyst represented by the following formula (I), wherein hydrogen cations (H+) of hydrophobic zeolite in said zeolite catalyst are partially replaced with certain metal ions or ammonium ions: HxM(1−x)/nZ (I) wherein H represents a hydrogen cation; M represents one or more cations selected from the group consisting of metal ions of IA Group, IIA Group, IB Group and IIB Group in Periodic Table and ammonium ions; n represents oxidation number of substituted cation (M); x represents mole % ranging from 10 to 90 based on the amount of hydrogen cations; and Z represehts a hydrophobic zeolite having the SiO2/Al2 O3 ratio of 20-200.
摘要翻译：本发明涉及从粗甲醇制备二甲醚的方法。更具体地说，本发明涉及一种制备用作新鲜燃料的二甲醚以及化学工业中的原料的改进方法，其中不产生作为副产物的烃和催化剂的失活，以这种方式进行在由下式（I）表示的沸石催化剂存在下，使用含有水的原料粗甲醇进行脱水，其中所述沸石催化剂中的疏水性沸石的氢阳离子（H +）被部分置换具有某些金属离子或铵离子：其中H表示氢阳离子; M表示选自IA族，IIA族，IB族和IIB族在周期表中的金属离子和铵离子中的一种或多种阳离子; n表示取代阳离子（M）的氧化数; x表示基于氢阳离子的量的10至90的摩尔％; Z代表SiO 2 / Al 2 O 3比为20-200的疏水性沸石。

6. 发明申请

US20060135823A1 Process for preparing dimethylether from methanol 审中-公开
标题翻译：从甲醇制备二甲醚的方法
公开(公告)号：US20060135823A1
公开(公告)日：2006-06-22
申请号：US10545595
申请日：2003-04-10
申请人： Ki-Won Jun , Hyun-Seog Roh , Kew-Ho Lee , Jae-Woo Kim
发明人： Ki-Won Jun , Hyun-Seog Roh , Kew-Ho Lee , Jae-Woo Kim
IPC分类号： C07C41/09
CPC分类号： C07C41/09 , C07C43/043
摘要： The present invention relates to a process for preparing dimethyl ether from methanol. More particularly, this invention relates to an improved process for preparing dimethyl ether with high yield useful as a clean fuel as well as a raw material in chemical industry performed via a catalytic system, wherein dehydration of methanol is first carried out by using a hydrophilic solid acid catalyst and then subsequent dehydration of methanol is carried out continuously by using a hydrophobic zeolite solid acid catalyst in the concurrent presence of unreacted methanol, dimethyl ether produced and water.
摘要翻译：本发明涉及由甲醇制备二甲醚的方法。更具体地说，本发明涉及一种用于制备用作清洁燃料的高产率的二甲醚的改进方法以及通过催化体系进行化学工业的原料，其中甲醇的脱水首先通过使用亲水固体然后在未反应的甲醇，生产的二甲醚和水的同时存在下使用疏水性沸石固体酸催化剂连续进行甲醇的脱水。

7. 发明申请

US20090023958A1 Process for preparing dimethyl ether from crude methanol in an adiabatic reactor 审中-公开
标题翻译：在绝热反应器中由粗甲醇制备二甲醚的方法
公开(公告)号：US20090023958A1
公开(公告)日：2009-01-22
申请号：US11665112
申请日：2005-08-19
申请人： Ki-won Jun , Hyun-seog Roh , Jae-woo Kim , Jeonkeun Oh , Jinhwan Bang
发明人： Ki-won Jun , Hyun-seog Roh , Jae-woo Kim , Jeonkeun Oh , Jinhwan Bang
IPC分类号： C07C41/09
CPC分类号： C07C41/09 , C07C41/01 , C07C43/043
摘要： The present invention relates a process for preparing dimethyl ether from crude methanol in an adiabatic reactor(s)/and more particularly to a process for preparing dimethyl ether wherein crude methanol containing water is dehydrated by using (1) a catalytic system in which the reactant contacts a catalyst 1 of hydrophobic zeolite partially substituted by a specific metal cation and subsequently a catalyst 2 selected from γ-alumina or silica-alumina; and (2) an adiabatic reactor(s). In the present invention, the dehydration is accomplished effectively by avoiding the formation or byproducts and the deactivation of catalyst. Therefore, dimethyl ether useful as clean fuel and a raw material in chemical industry can be produced from crude methanol with an enhanced yield in an adiabatic reactor(s).
摘要翻译：本发明涉及一种在绝热反应器中由粗甲醇制备二甲醚的方法，更具体地涉及一种制备二甲醚的方法，其中含有粗甲醇的水通过使用（1）催化体系脱水，其中反应物接触部分被特定金属阳离子取代并且随后选自γ-氧化铝或二氧化硅 - 氧化铝的催化剂2的疏水性沸石的催化剂1; 和（2）绝热反应器。在本发明中，通过避免形成或副产物和催化剂的失活来有效地实现脱水。因此，用作清洁燃料的二甲醚和化学工业中的原料可以在绝热反应器中以粗甲醇生产，产率提高。

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