CH_4部分氧化制氢Ni-CuZrSiO催化剂的研究  

STUDY ON Ni-Cu/ZrSiO CATALYST FOR PARTIAL OXIDATION OF CH_4 TO PRODUCE HYDROGEN

作　　者：王爱菊[1] 钟顺和[1] 

机构地区：[1]天津大学化工学院,天津300072

出　　处：《燃料化学学报》2003年第6期531-537,共7页Journal of Fuel Chemistry and Technology

基　　金：国家自然科学基金(20076035) ~~

摘　　要：采用表面反应改性法制备了ZrO2 SiO2(ZrSiO)表面复合物,用等体积浸渍法制备了ZrSiO负载的Ni Cu双金属催化剂,并用IR、TPD、TPSR和微反技术考察了CH4、H2O和O2在催化剂表面上的化学吸附及反应性能。结果表明,在Ni Cu ZrSiO催化剂上存在着Ni Cu金属位,Lewis酸位Znn+和碱位Zr O-三类活性中心;CH4和H2O在金属位和Lewis酸位Znn+和碱位Zr O-的协同作用下可形成解离吸附态;CH4、H2O和O2在Ni Cu ZrSiO催化剂表面上的主要反应产物为H2和CO2,选择性均在95%以上。The surface complex support ZrO_2-SiO_2 (ZrSiO) was prepared by surface reaction modification, and Ni-Cu/ZrSiO bimetallic catalyst was prepared by isovolumic impregnation. Adsorption and reaction of CH_4 with H_2O and O_2 on the catalyst were characterized by IR, TPD, TPSR and microreactor techniques. The results showed that there exist three kinds of active sites on the catalyst: metal site M, Lewis acid site Zn^(n+) and Lewis basic site Zr-O^-. With the cooperation of metal site M, Lewis acid site Zn^(n+) and Lewis basic site Zr-O^-, CH_4 was activated and dissociated into CO and H_2, H_2O was dissociated into H_2 and O on the catalyst. Under condition of reaction temperature 450?℃, n(CH_4)∶ n(O_2)∶ n(H_20)=1∶0.5∶2.5 and methane space velocity (SVCH_4)=1?200?h^(-1), the main reaction products on Ni-Cu/ZrSiO catalyst are H_2 and CO_2, with a selectivity over 95%.

关 键 词：甲烷 氢气 制备 选择氧化 复合氧化物载体 镍 铜 双金属催化剂 CH4 

分 类 号：TQ116.2[化学工程—无机化工] O643.3[理学—物理化学]