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Development of Technique for Chemical Conversion of Natural Gas

天然气化学转化技术的发展

基本信息

批准号：
01470079
负责人：
MORIKAWA Akira
金额：
$ 4.74万
依托单位：
Tokyo Institute of Technology
依托单位国家：
日本
项目类别：
Grant-in-Aid for General Scientific Research (B)
财政年份：
1989
资助国家：
日本
起止时间：
1989 至 1990
项目状态：
已结题

项目摘要

It has been found that LiNO_3-doped NiO was a catalyst effective for oxidative coupling of methane to produce ethane and ethylene. This catalyst was identified as a compound, LiNiO_2. When methane was brought into contact with LiNiO_2, methane was converted to ethylene and ethane and LiNiO_2 was changed into a mixture of Li_2O and NiO. LiNiO_2 was restored when oxygen gas was added to the system. From the Kinetic and spectroscopic studies of this catalytic system, it has been concluded that oxidative coupling of methane on LiNiO_2 proceeds through the reaction of methane with the catalyst and reoxidation of the reduced catalyst.LiClーdoped NiO was a catalyst effective for selective formation of ethylene during oxidative coupling of methane. LiCl suppressed deep oxidation of methane and enhanced the successive oxidative dehydrogenation of ethane to ethylene.Two effective catalysts for formation of oxygenated compounds in oxidation of alkanes with molecular oxygen have been found. One was B_2O_3-Al_2O_3, which gave acetaldehyde from ethane. The main products on this catalyst were acetaldehyde and ethylene. A mechanism including the common intermediate for the formations of the two products were proposed. Another was B_2O_3-P_2O_5, on which propane was converted to propionaldehyde, acetone, acetaldehyde, and propylene.Oxidative coupling of methane into ethylene and ethane over LiNiO_2 was enhanced when oxygen was removed electrochemically from the catalyst through a stabilized zirconia oxygen-anion conductor. On the other hand, the same enhancement was observed over LiCl-doped NiO when oxygen was pumped to the catalyst. The mechanisms of the new catalytic systems controlled electrochemically were proposed.

LiNO_3掺杂的NiO是甲烷氧化偶联制乙烷和乙烯的有效催化剂。该催化剂被鉴定为化合物LiNiO_2。当甲烷与LiNiO_2接触时，甲烷转化为乙烯和乙烷，LiNiO_2转化为Li_2O和NiO的混合物。当通入氧气后，LiNiO_2的还原性得到恢复。动力学和光谱研究表明，LiNiO_2上的甲烷氧化偶联反应是通过甲烷与催化剂的反应和还原态催化剂的再氧化进行的，LiCl掺杂NiO是甲烷氧化偶联反应中选择性生成乙烯的有效催化剂。LiCl抑制了甲烷的深度氧化，促进了乙烷氧化脱氢制乙烯，发现了两种有效的分子氧氧化烷烃生成含氧化合物的催化剂，一种是B_2O_3-Al_2O_3，它能使乙烷生成乙醛;该催化剂的主要产物为乙醛和乙烯。提出了一种包括两种产物形成的共同中间体的机理。另一种是B_2O_3-P_2O_5催化剂，丙烷在该催化剂上可转化为丙醛、丙酮、乙醛和丙烯，当通过稳定的氧化锆氧-阴离子导体电化学除氧时，甲烷在LiNiO_2上氧化偶联为乙烯和乙烷的反应得到增强。另一方面，当向催化剂中泵入氧气时，在掺杂LiCl的NiO上观察到了相同的增强作用。提出了电化学控制新催化体系的机理。