利用多元醇氟化法制备了氟化铝、氟化镁及镁铝复合型氟化物等催化剂,并对所制催化剂在1,1,1,3,3-五氟丙烷(HFC-245fa)气相脱氟化氢制备1,3,3,3-四氟丙烯(HFO-1234ze)反应中的催化性能进行了研究。结果表明,单一氟化镁催化剂活性较低,HFC...利用多元醇氟化法制备了氟化铝、氟化镁及镁铝复合型氟化物等催化剂,并对所制催化剂在1,1,1,3,3-五氟丙烷(HFC-245fa)气相脱氟化氢制备1,3,3,3-四氟丙烯(HFO-1234ze)反应中的催化性能进行了研究。结果表明,单一氟化镁催化剂活性较低,HFC-245fa转化率仅为7.8%;以摩尔分数为9%Al/MgF_2作为催化HFC-245fa脱氟化氢反应催化剂,在反应温度为280℃,接触时间为25 s,催化剂用量为5 m L时,HFC-245fa的转化率、HFO-1234ze的选择性分别达到53%和100%,与单一组分氟化铝催化性能相当,且运行200 h后保持96%的初始活性。展开更多
Solid materials PMo 12 and PMo 12 /CaF 2 were prepared, and the surface structure, chemisorption to methane and the behavior of LSSR for the materials have been investigated by using IR, XRD, BET and laser stimulated ...Solid materials PMo 12 and PMo 12 /CaF 2 were prepared, and the surface structure, chemisorption to methane and the behavior of LSSR for the materials have been investigated by using IR, XRD, BET and laser stimulated surface reaction techniques. With different amounts of PMo 12 , the distribution of PMo 12 can be controlled from less than one layer to multi layer on the surface of CaF 2. There exist Lewis base sites O 2- in MoO and Mo—O—Mo bonds as well as Lewis acid site —Mo 6+ — on the solid surfaces. Methane can be adsorbed on the surface MoO and Mo—O—Mo bonds with the molecular adsorption state, and the adsorption amount on MoO bond is greater. With 960 cm -1 laser to excite the surface MoO bond, the partial oxidation of methane occurred obviously at normal pressure and 200 ℃. Methanol is the direct product of methane oxidation, while HCHO, CH 3OCH 3 and hydrocarbons are the products of methanol reacted continuously on the solid surface. As CaF 2 doesn’t adsorb 960 cm -1 laser, PMo 12 /CaF 2 can utilize the laser energy more efficiently than that of PMo 12 . According to the characterization and reaction results, a mechanism of LSSR for methane partial oxidation to methanol is given.展开更多
文摘利用多元醇氟化法制备了氟化铝、氟化镁及镁铝复合型氟化物等催化剂,并对所制催化剂在1,1,1,3,3-五氟丙烷(HFC-245fa)气相脱氟化氢制备1,3,3,3-四氟丙烯(HFO-1234ze)反应中的催化性能进行了研究。结果表明,单一氟化镁催化剂活性较低,HFC-245fa转化率仅为7.8%;以摩尔分数为9%Al/MgF_2作为催化HFC-245fa脱氟化氢反应催化剂,在反应温度为280℃,接触时间为25 s,催化剂用量为5 m L时,HFC-245fa的转化率、HFO-1234ze的选择性分别达到53%和100%,与单一组分氟化铝催化性能相当,且运行200 h后保持96%的初始活性。
文摘Solid materials PMo 12 and PMo 12 /CaF 2 were prepared, and the surface structure, chemisorption to methane and the behavior of LSSR for the materials have been investigated by using IR, XRD, BET and laser stimulated surface reaction techniques. With different amounts of PMo 12 , the distribution of PMo 12 can be controlled from less than one layer to multi layer on the surface of CaF 2. There exist Lewis base sites O 2- in MoO and Mo—O—Mo bonds as well as Lewis acid site —Mo 6+ — on the solid surfaces. Methane can be adsorbed on the surface MoO and Mo—O—Mo bonds with the molecular adsorption state, and the adsorption amount on MoO bond is greater. With 960 cm -1 laser to excite the surface MoO bond, the partial oxidation of methane occurred obviously at normal pressure and 200 ℃. Methanol is the direct product of methane oxidation, while HCHO, CH 3OCH 3 and hydrocarbons are the products of methanol reacted continuously on the solid surface. As CaF 2 doesn’t adsorb 960 cm -1 laser, PMo 12 /CaF 2 can utilize the laser energy more efficiently than that of PMo 12 . According to the characterization and reaction results, a mechanism of LSSR for methane partial oxidation to methanol is given.
基金supported by Key Technologies R&D Program of He'nan Scientific and Technological Committee(082102210050)Foundation of He'nan Educational Committee(2008B150018,2011A150023)+1 种基金Foundation for Young and Middle-aged Key Teachers of Shangqiu Normal CollegeTraining Programm Foundation for the Major Project of Shangqiu Normal College(2011ZDPY02)
