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1. 发明授权

US08692032B2 Methods of using tungsten carbide catalysts in preparation of ethylene glycol 有权
标题翻译：使用碳化钨催化剂制备乙二醇的方法
公开(公告)号：US08692032B2
公开(公告)日：2014-04-08
申请号：US13539041
申请日：2012-06-29
申请人： Tao Zhang , Na Ji , Mingyuan Zheng , Aiqin Wang , Yuying Shu , Xiaodong Wang , Jingguang Chen
发明人： Tao Zhang , Na Ji , Mingyuan Zheng , Aiqin Wang , Yuying Shu , Xiaodong Wang , Jingguang Chen
IPC分类号： C07C27/00 , C07C29/00
CPC分类号： B01J37/0201 , B01J21/18 , B01J23/6527 , B01J23/888 , B01J27/22 , B01J37/08 , C07C29/00 , Y02P20/52 , C07C31/202
摘要： Tungsten carbide catalysts are used in preparation of ethylene glycol by hydrogenating degradation of cellulose. The catalyst includes tungsten carbide as main catalytic active component, added with small amount of one or more transition metals such as nickel, cobalt, iron, ruthenium, rhodium, palladium, osmium, iridium, platinum, and copper as the second metal, supported on one or more porous complex supports such as active carbon, alumina, silica, titanium dioxide, silicon carbide, zirconium oxide, for conversion of cellulose to ethylene glycol. The catalyst realizes high efficiency, high selectivity, and high yield in the conversion of cellulose to ethylene glycol at the temperature of 120-300° C., hydrogen pressure of 1-10 MPa, and hydrothermal conditions. Compared to the existing industrial synthetic method of ethylene glycol using ethylene as feedstock, the invention has the advantages of using renewable raw material resources, environment friendly process, and excellent atom economy.
摘要翻译：通过氢化纤维素的降解，使用碳化钨催化剂制备乙二醇。催化剂包括碳化钨作为主要催化活性组分，添加少量一种或多种过渡金属如镍，钴，铁，钌，铑，钯，锇，铱，铂和铜作为第二金属，负载在用于将纤维素转化为乙二醇的一种或多种多孔复合物载体如活性炭，氧化铝，二氧化硅，二氧化钛，碳化硅，氧化锆。催化剂在120-300℃，氢气压力1-10MPa，水热条件下，纤维素向乙二醇的转化率高，效率高，选择性高，产率高。与现有的以乙烯为原料的乙二醇工业合成方法相比，本发明具有使用可再生原料资源，环保工艺，原子经济优良的优点。

2. 发明申请

US20120283487A1 METHODS OF USING TUNGSTEN CARBIDE CATALYSTS IN PREPARATION OF ETHYLENE GLYCOL 有权
标题翻译：使用碳纳米管催化剂制备乙二醇的方法
公开(公告)号：US20120283487A1
公开(公告)日：2012-11-08
申请号：US13539041
申请日：2012-06-29
申请人： Tao Zhang , Na JI , Mingyuan Zheng , Aiqin WANG , Yuying SHU , Xiaodong WANG , Jingguang CHEN
发明人： Tao Zhang , Na JI , Mingyuan Zheng , Aiqin WANG , Yuying SHU , Xiaodong WANG , Jingguang CHEN
IPC分类号： C07C29/132
CPC分类号： B01J37/0201 , B01J21/18 , B01J23/6527 , B01J23/888 , B01J27/22 , B01J37/08 , C07C29/00 , Y02P20/52 , C07C31/202
摘要： Tungsten carbide catalysts are used in preparation of ethylene glycol by hydrogenating degradation of cellulose. The catalyst includes tungsten carbide as main catalytic active component, added with small amount of one or more transition metals such as nickel, cobalt, iron, ruthenium, rhodium, palladium, osmium, iridium, platinum, and copper as the second metal, supported on one or more porous complex supports such as active carbon, alumina, silica, titanium dioxide, silicon carbide, zirconium oxide, for conversion of cellulose to ethylene glycol. The catalyst realizes high efficiency, high selectivity, and high yield in the conversion of cellulose to ethylene glycol at the temperature of 120-300° C., hydrogen pressure of 1-10 MPa, and hydrothermal conditions. Compared to the existing industrial synthetic method of ethylene glycol using ethylene as feedstock, the invention has the advantages of using renewable raw material resources, environment friendly process, and excellent atom economy.
摘要翻译：通过氢化纤维素的降解，使用碳化钨催化剂制备乙二醇。催化剂包括碳化钨作为主要催化活性组分，添加少量一种或多种过渡金属如镍，钴，铁，钌，铑，钯，锇，铱，铂和铜作为第二金属，负载在用于将纤维素转化为乙二醇的一种或多种多孔复合物载体如活性炭，氧化铝，二氧化硅，二氧化钛，碳化硅，氧化锆。催化剂在120-300℃，氢气压力1-10MPa，水热条件下，纤维素向乙二醇的转化率高，效率高，选择性高，产率高。与现有的以乙烯为原料的乙二醇工业合成方法相比，本发明具有使用可再生原料资源，环保工艺，原子经济优良的优点。

3. 发明申请

US20100256424A1 METHOD OF PREPARING ETHYLENE GLYCOL CELLULOSE 有权
标题翻译：制备乙二醇纤维素的方法
公开(公告)号：US20100256424A1
公开(公告)日：2010-10-07
申请号：US12734601
申请日：2008-10-31
申请人： Tao Zhang , Mingyuan Zheng , Na Ji , Aigin Wang , Yuying Shu , Hui Wang , Xiaodong Wang , Jingguang Chen
发明人： Tao Zhang , Mingyuan Zheng , Na Ji , Aigin Wang , Yuying Shu , Hui Wang , Xiaodong Wang , Jingguang Chen
IPC分类号： C07C29/00
CPC分类号： C07C29/00 , B01J21/063 , B01J21/18 , B01J23/652 , B01J23/6527 , B01J23/85 , B01J23/888 , B01J27/19 , B01J27/22 , B01J27/25 , Y02P20/52 , C07C31/202
摘要： A method for preparing ethylene glycol from cellulose uses the cellulose as the feed for the reaction. The cellulose conversion is performed over catalysts which are composed of the metallic state, carbides, nitrides, or phosiphides of molybdenum or tungsten, and metallic cobalt, nickel, ruthenium, rhodium, palladium, iridium, and platinum of the group 8, 9, or 10 transition metals. The catalytic conversion of cellulose is conducted at 120 to 300° C. and hydrogen pressure 1 to 12 MPa under the hydrothermal conditions to achieve the high efficiency, high selectivity, and high yield of ethylene glycol. Compared to the existing method of preparing ethylene glycol from ethylene, the method, using the renewable raw material for the reaction, is friendly to the environment, and has high atom economy.
摘要翻译：从纤维素制备乙二醇的方法使用纤维素作为反应的进料。纤维素转化在由金属状态，碳化物，氮化物或钼或钨的高温以及金属钴，镍，钌，铑，钯，铱和铂组成的催化剂上进行，第8,9或9族 10个过渡金属。在水热条件下，纤维素的催化转化率为120〜300℃，氢压为1〜12MPa，达到乙二醇的高效率，高选择性和高产率。与从乙烯制备乙二醇的现有方法相比，使用可再生原料进行反应的方法对环境友好，原子经济性好。

4. 发明授权

US07960594B2 Method of preparing ethylene glycol from cellulose 有权
标题翻译：从纤维素制备乙二醇的方法
公开(公告)号：US07960594B2
公开(公告)日：2011-06-14
申请号：US12734601
申请日：2008-10-31
申请人： Tao Zhang , Mingyuan Zheng , Na Ji , Aigin Wang , Yuying Shu , Hui Wang , Xiaodong Wang , Jingguang Chen
发明人： Tao Zhang , Mingyuan Zheng , Na Ji , Aigin Wang , Yuying Shu , Hui Wang , Xiaodong Wang , Jingguang Chen
IPC分类号： C07C29/00
CPC分类号： C07C29/00 , B01J21/063 , B01J21/18 , B01J23/652 , B01J23/6527 , B01J23/85 , B01J23/888 , B01J27/19 , B01J27/22 , B01J27/25 , Y02P20/52 , C07C31/202
摘要： A method for preparing ethylene glycol from cellulose uses the cellulose as the feed for the reaction. The cellulose conversion is performed over catalysts which are composed of the metallic state, carbides, nitrides, or phosiphides of molybdenum or tungsten, and metallic cobalt, nickel, ruthenium, rhodium, palladium, iridium, and platinum of the group 8, 9, or 10 transition metals. The catalytic conversion of cellulose is conducted at 120 to 300° C. and hydrogen pressure 1 to 12 MPa under the hydrothermal conditions to achieve the high efficiency, high selectivity, and high yield of ethylene glycol. Compared to the existing method of preparing ethylene glycol from ethylene, the method, using the renewable raw material for the reaction, is friendly to the environment, and has high atom economy.
摘要翻译：从纤维素制备乙二醇的方法使用纤维素作为反应的进料。纤维素转化在由金属状态，碳化物，氮化物或钼或钨的高温以及金属钴，镍，钌，铑，钯，铱和铂组成的催化剂上进行，第8,9或9族 10个过渡金属。在水热条件下，纤维素的催化转化率为120〜300℃，氢压为1〜12MPa，达到乙二醇的高效率，高选择性和高产率。与从乙烯制备乙二醇的现有方法相比，使用可再生原料进行反应的方法对环境友好，原子经济性好。

5. 发明授权

US08324433B2 Method for producing ethylene glycol from polyhydroxy compound 有权
标题翻译：从多羟基化合物制备乙二醇的方法
公开(公告)号：US08324433B2
公开(公告)日：2012-12-04
申请号：US12916625
申请日：2010-10-31
申请人： Tao Zhang , Mingyuan Zheng , Aiqin Wang , Na Ji , Jifeng Pang , Zhijun Tai , Likun Zhou , Jingguang Chen , Xiaodong Wang
发明人： Tao Zhang , Mingyuan Zheng , Aiqin Wang , Na Ji , Jifeng Pang , Zhijun Tai , Likun Zhou , Jingguang Chen , Xiaodong Wang
IPC分类号： C07C29/132 , C07C29/60
CPC分类号： B01J23/6525 , B01J21/04 , B01J21/06 , B01J21/063 , B01J21/08 , B01J21/18 , B01J23/652 , B01J23/6527 , B01J23/85 , B01J23/882 , B01J23/883 , B01J23/888 , B01J27/19 , B01J27/22 , B01J27/24 , B01J37/0205 , B01J37/18 , C07C29/00 , C07C29/132 , Y02P20/52 , C07C31/202 , C07C31/26
摘要： A method for producing ethylene glycol, including (a) adding a polyhydroxy compound and water to a sealed high-pressure reactor, (b) removing air and introducing hydrogen, and (c) allowing the polyhydroxy compound to react in the presence of a catalyst while stiffing. The catalyst includes a first active ingredient and a second active ingredient. The first active ingredient includes a transition metal of Group 8, 9, or 10 selected from iron, cobalt, nickel, ruthenium, rhodium, palladium, iridium, and platinum, and/or a mixture thereof. The second active ingredient includes a metallic state of molybdenum and/or tungsten, or a carbide, nitride, or phosphide thereof. The method is carried out at a hydrogen pressure of 1-12 MPa, at a temperature of 120-300° C. for not less than 5 min in a one-step catalytic reaction. The efficiency, selectivity, and the yield of ethylene glycol are high. The preparation process is simple and the materials used are renewable.
摘要翻译：一种生产乙二醇的方法，包括（a）在密封的高压反应器中加入多羟基化合物和水，（b）除去空气和引入氢，和（c）使多羟基化合物在催化剂存在下反应同时僵硬。催化剂包括第一活性成分和第二活性成分。第一活性成分包括选自铁，钴，镍，钌，铑，钯，铱和铂的第8,9或10族的过渡金属和/或它们的混合物。第二活性成分包括钼和/或钨的金属状态，或其碳化物，氮化物或磷化物。该方法在1-12MPa的氢气压力下，在120-300℃的温度下在一步催化反应中不少于5分钟进行。乙二醇的效率，选择性和产率高。制备过程简单，使用的材料是可再生的。

6. 发明申请

US20120178974A1 MESOPOROUS CARBON SUPPORTED TUNGSTEN CARBIDE CATALYSTS, PREPARATION AND APPLICATIONS THEREOF 有权
标题翻译：多孔碳载体碳纳米管催化剂，其制备及应用
公开(公告)号：US20120178974A1
公开(公告)日：2012-07-12
申请号：US13395460
申请日：2010-10-22
申请人： Tao Zhang , Yanhua Zhang , Aiqin Wang , Mingyuan Zheng
发明人： Tao Zhang , Yanhua Zhang , Aiqin Wang , Mingyuan Zheng
IPC分类号： C07C29/00 , B01J37/06 , B01J37/02 , B01J27/22
CPC分类号： B01J27/22 , B01J21/18 , B01J35/1028 , B01J35/1047 , B01J35/1061 , B01J37/0018 , B01J37/0201 , B01J37/084 , C07C29/00 , Y02P20/52 , C07C31/202
摘要： A supported tungsten carbide catalyst comprises tungsten carbide as its active component and a mesoporous carbon as its support, wherein tungsten carbide is highly dispersed on the surface and in the channels of the mesoporous carbon, and the content of tungsten element is in the range from 30% to 42% by mass based on the mesoporous carbon. This catalyst can be prepared by impregnation process. This catalyst can be used for the direct catalytic conversion of cellulose to ethylene glycol under the hydrothermal conditions and at a temperature of 245° C. and the hydrogen pressure of 6 MPa with high reactivity, selectivity and stability.
摘要翻译：载体碳化钨催化剂包括碳化钨作为其活性组分和介孔碳作为其载体，其中碳化钨高分散在中孔碳的表面和通道中，钨元素的含量在30 相对于介孔碳为质量％〜42质量％。该催化剂可以通过浸渍法制备。该催化剂可用于在水热条件下，在245℃的温度和6MPa的氢气压力下，将纤维素直接催化转化为乙二醇，具有高反应性，选择性和稳定性。

7. 发明申请

US20120172633A1 METHODS FOR PREPARING ETHYLENE GLYCOL FROM POLYHYDROXY COMPOUNDS 有权
标题翻译：从聚羟基化合物制备乙烯甘油的方法
公开(公告)号：US20120172633A1
公开(公告)日：2012-07-05
申请号：US13395470
申请日：2010-11-04
申请人： Tao Zhang , Zhijun Tai , Aiqin Wang , Mingyuan Zheng
发明人： Tao Zhang , Zhijun Tai , Aiqin Wang , Mingyuan Zheng
IPC分类号： C07C29/132
CPC分类号： B01J23/888 , B01J23/30 , B01J23/42 , B01J23/462 , B01J23/468 , B01J23/6527 , B01J23/755 , B01J35/0006 , C07C29/132 , Y02P20/52 , C07C31/202
摘要： This invention provides methods for producing ethylene glycol from polyhydroxy compounds such as cellulose, starch, hemicellulose, glucose, sucrose, fructose, fructan, xylose and soluble xylooligosaccharides. The methods uses polyhydroxy compounds as the reactant, a composite catalyst having active components comprising one or more transition metals of Groups 8, 9, or 10, including iron, cobalt, nickel, ruthenium, rhodium, palladium, iridium, and platinum, as well as tungsten oxide, tungsten sulfide, tungsten hydroxide, tungsten chloride, tungsten bronze oxide, tungsten acid, tungstate, metatungstate acid, metatungstate, paratungstate acid, paratungstate, peroxotungstic acid, pertungstate, heteropoly acid containing tungsten. Reacting at a temperature of 120-300° C. and a hydrogen pressure of 1-13 MPa under hydrothermal conditions to accomplish one-step catalytic conversion. It realizes efficient, highly selective, high yield preparation of ethylene glycol and propylene glycol from polyhydroxy compounds. The advantage of processes disclosed in this invention include renewable raw material and high atom economy. At the same time, compared with other technologies that converts biomass raw materials into polyols, methods disclosed herein enjoy advantages including simple reaction process, high yield of targeted products, as well as easy preparation and low cost for the catalysts.
摘要翻译：本发明提供从多羟基化合物如纤维素，淀粉，半纤维素，葡萄糖，蔗糖，果糖，果聚糖，木糖和可溶性低聚木糖中生产乙二醇的方法。该方法使用多羟基化合物作为反应物，具有包含一种或多种第8,9或10族过渡金属（包括铁，钴，镍，钌，铑，钯，铱和铂）的活性组分的复合催化剂以及作为氧化钨，硫化钨，氢氧化钨，氯化钨，青铜氧化钨，钨酸，钨酸盐，偏钨酸，偏钨酸盐，仲钨酸，仲钨酸盐，过钨酸，过钨酸盐，含钨杂多酸。在水热条件下，在120-300℃的温度和1-13MPa的氢压下进行反应，完成一步催化转化。它实现了从多羟基化合物的乙二醇和丙二醇的高效，高选择性，高产率的制备。本发明公开的方法的优点包括可再生原料和高原子经济性。同时，与将生物质原料转化为多元醇的其他技术相比，本文公开的方法具有包括简单的反应过程，高产率的目标产物以及易于制备和低成本的优点。

8. 发明授权

US08889585B2 Mesoporous carbon supported tungsten carbide catalysts, preparation and applications thereof 有权
标题翻译：介孔碳载体碳化钨催化剂，的制备及应用
公开(公告)号：US08889585B2
公开(公告)日：2014-11-18
申请号：US13395460
申请日：2010-10-22
申请人： Tao Zhang , Yanhua Zhang , Aiqin Wang , Mingyuan Zheng
发明人： Tao Zhang , Yanhua Zhang , Aiqin Wang , Mingyuan Zheng
IPC分类号： B01J21/18 , B01J23/00 , C07C27/00 , C07C29/00 , C07C31/18 , B01J27/22 , B01J35/10 , B01J37/00 , B01J37/02 , B01J37/08
CPC分类号： B01J27/22 , B01J21/18 , B01J35/1028 , B01J35/1047 , B01J35/1061 , B01J37/0018 , B01J37/0201 , B01J37/084 , C07C29/00 , Y02P20/52 , C07C31/202
摘要： A supported tungsten carbide catalyst comprises tungsten carbide as its active component and a mesoporous carbon as its support, wherein tungsten carbide is highly dispersed on the surface and in the channels of the mesoporous carbon, and the content of tungsten element is in the range from 30% to 42% by mass based on the mesoporous carbon. This catalyst can be prepared by impregnation process. This catalyst can be used for the direct catalytic conversion of cellulose to ethylene glycol under the hydrothermal conditions and at a temperature of 245° C. and the hydrogen pressure of 6 MPa with high reactivity, selectivity and stability.
摘要翻译：载体碳化钨催化剂包括碳化钨作为其活性组分和介孔碳作为其载体，其中碳化钨高分散在中孔碳的表面和通道中，钨元素的含量在30 相对于介孔碳为质量％〜42质量％。该催化剂可以通过浸渍法制备。该催化剂可用于在水热条件下，在245℃的温度和6MPa的氢气压力下，将纤维素直接催化转化为乙二醇，具有高反应性，选择性和稳定性。

9. 发明授权

US08323937B2 Continuous catalytic generation of polyols from cellulose 有权
标题翻译：从纤维素连续催化产生多元醇
公开(公告)号：US08323937B2
公开(公告)日：2012-12-04
申请号：US13192739
申请日：2011-07-28
申请人： Tao Zhang , Aiqin Wang , Mingyuan Zheng , Changzhi Li , Jifeng Pang , Tom N. Kalnes , John Q. Chen , Joseph A. Kocal
发明人： Tao Zhang , Aiqin Wang , Mingyuan Zheng , Changzhi Li , Jifeng Pang , Tom N. Kalnes , John Q. Chen , Joseph A. Kocal
IPC分类号： C12P7/18 , C07C31/20
CPC分类号： C12P7/18 , C07C29/132 , Y02P20/582 , C07C31/20
摘要： A catalytic process for generating at least one polyol from a feedstock comprising cellulose is performed in a continuous manner using a catalyst comprising nickel tungsten carbide. The process involves, contacting, continuously, hydrogen, water, and a feedstock comprising cellulose, with the catalyst to generate an effluent stream comprising at least one polyol and recovering the polyol from the effluent stream.
摘要翻译：使用包含镍碳化钨的催化剂以连续方式进行从包含纤维素的原料生成至少一种多元醇的催化方法。该方法包括连续地将包含纤维素的氢，水和原料与催化剂接触以产生包含至少一种多元醇的流出物流并从流出物流中回收多元醇。

10. 发明授权

US08410319B2 Continuous catalytic generation of polyols from cellulose with recycle 有权
标题翻译：从纤维素连续催化生成多元醇，再循环
公开(公告)号：US08410319B2
公开(公告)日：2013-04-02
申请号：US13192835
申请日：2011-07-28
申请人： Tom N. Kalnes , John Q. Chen , Joseph A. Kocal , Tao Zhang , Aiqin Wang , Mingyuan Zheng , Changzhi Li , Jifeng Pang
发明人： Tom N. Kalnes , John Q. Chen , Joseph A. Kocal , Tao Zhang , Aiqin Wang , Mingyuan Zheng , Changzhi Li , Jifeng Pang
IPC分类号： C07C29/74
CPC分类号： C07C29/132 , C07C31/20
摘要： A catalytic process for generating at least one polyol from a feedstock comprising cellulose is performed in a continuous manner. The process involves, contacting, continuously, hydrogen, water, and a feedstock comprising cellulose, with a catalyst to generate an effluent stream comprising at least one polyol, water, hydrogen, and at least one co-product. The water, hydrogen, and at least one co-product are separated from the effluent stream and recycled to the reaction zone. The polyol is recovered from the effluent stream.
摘要翻译：以包含纤维素的原料生成至少一种多元醇的催化方法是以连续方式进行的。该方法包括使含有纤维素的氢，水和原料与催化剂连续地接触，以产生包含至少一种多元醇，水，氢和至少一种共同产物的流出物流。将水，氢和至少一种副产物与流出物流分离并再循环至反应区。从流出物流中回收多元醇。

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