CH4部分氧化制氢Ni-Cu/ZrSiO催化剂的研究

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。

STUDY ON Ni-Cu/ZrSiO CATALYST FOR PARTIAL OXIDATION OF CH4 TO PRODUCE HYDROGEN

The surface complex support ZrO2-SiO2 (ZrSiO) was prepared by surface reaction modification, and Ni-Cu/ZrSiO bimetallic catalyst was prepared by isovolumic impregnation. Adsorption and reaction of CH4 with H2O and O2 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 Znn+ and Lewis basic site Zr-O－. With the cooperation of metal site M, Lewis acid site Znn+ and Lewis basic site Zr-O－, CH4 was activated and dissociated into CO and H2, H2O was dissociated into H2 and O on the catalyst. Under condition of reaction temperature 450 ℃, n(CH4)∶ n(O2)∶ n(H2O)=1∶0.5∶2.5 and methane space velocity (SVCH4)＝1200h－1, the main reaction products on Ni-Cu/ZrSiO catalyst are H2 and CO2, with a selectivity over 95%.