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氧渗透膜反应器的烷烃氧化脱氢
引用本文:阎瑞强,;刘卫,;宋春林.氧渗透膜反应器的烷烃氧化脱氢[J].化学物理学报(中文版),2014,27(6):690-696.
作者姓名:阎瑞强  ;刘卫  ;宋春林
作者单位:[1]台州学院材料工程系,台州318000; [2]西南大学材料与能源学部,重庆400715; [3]中国科学技术大学材料科学与工程系,中国科学院能量转换材料重点实验室,合肥230026
基金项目:This work was supported by the Fundamental Research Funds for the Central Universities (No.SWU113045 and No.XDJK2013C089).
摘    要:研究了乙烷和丙烷在催化膜反应器中的氧化脱氢反应.所用的膜材料为La2Ni0.9V0.1O4+δ和Ba0.5Sr0.5Co0.8Fe0.2O3-δ.为了平衡氧气通量和额外的均匀气相反应,实验选择在中温段进行(550或者650℃).实验结果表明膜的氧渗透通量和膜表面上主要激活烷烃的活性位在获得高的烷烃转化率过程中起决定性作用.乙烷和丙烷的氧化脱氢实验数据均符合Mars-van Krevelen机理,其中烷烃和膜表面的晶格氧反应产生相应的烯烃.同时证明了气相和膜表面的氧浓度是决定烯烃选择性的关键.

关 键 词:氧化脱氢  膜反应器  选择性  转化率
收稿时间:2014-07-01

Oxidative Dehydrogenation of Alkanes using Oxygen-Permeable Membrane Reactor
Rui-qiang Yan,Wei Liu,Chun-lin Song.Oxidative Dehydrogenation of Alkanes using Oxygen-Permeable Membrane Reactor[J].化学物理学报(中文版),2014,27(6):690-696.
Authors:Rui-qiang Yan  Wei Liu  Chun-lin Song
Institution:1.Department of Materials Engineering, Taizhou University, Taizhou 318000, China2.Faculty of Materials and Energy, Southwest University, Chongqing 400715, China3.CAS Key Lab Mat Energy Convers, Department of Materials Science and Engineering, University of Science and Technology of China, Hefei 230026, China
Abstract:The oxidative dehydrogenation (ODH) reactions of ethane and propane were investigated in a catalytic membrane reactor, incorporating oxygen-permeable membranes based upon La2Ni0.9V0.1O4+δor Ba0.5Sr0.5Co0.8Fe0.2O3-δ. As a compromise between the occurrence of a measureable oxygen flux and excessive homogenous gas phase reactions, the measurements were conducted at an intermediate temperature, either at 550 or 650 oC. The results show the dominating role of the oxygen flux across the membrane and available sites at the membrane surface in primary activation of the alkane and, hence, in achieving high alkane conversions. The experimental data of ODH of propane and ethane on both membrane materials can be reconciled on the basis of Mars-van Krevelen mechanism, in which the alkane reacts with lattice oxygen on the membrane surface to produce the corresponding olefin. It is further demonstrated that the oxygen concentration in the gas phase and on the membrane surface is crucial for determining the olefin selectivity.
Keywords:Oxidative dehydrogenation  Membrane reactor  Oxygen-permeable membrane
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