制备了负载于大孔容、高比表面的γ-Al2O3载体上的Ni基催化剂.采用固定床流动反应装置,考察了催化剂焙烧温度、反应条件(反应温度、压力、空速以及反应原料气组成)对甲烷三重整反应(TRM)制合成气的催化性能的影响.结果表明,650℃焙烧的催化剂具有较好的稳定性.在常压、850℃、10080h^-1、n(CH4)/n(CO2)/n(H2O)/n(O2)=1/0.48/0.54/0.1的条件下,CH4转化率达到95.4%,CO2转化率达到84.6%,在此条件下连续运行9h未见活性下降.TRM反应适宜于在高温、低压下进行,原料组成的变化不会影响CH4转化率,但会影响CO2转化率和产物合成气的n(H2)/n(Co)比.
Ni was dispersed on γ-Al2O3 with large pore volume and high specific surface area by using wet impregnation method. The catalytic performances of Ni/Al2O3 in tri-reforming of methane to syngas (TRM) under different reaction conditions such as temperature, pressure and space velocity, and the feedstock composition were studied in a fix-bed reactor. The effect of calcination temperature on stability of catalysts was also investigated. The results showed that catalyst calcined at 650 ℃ exhibited higher stability than catalysts calcined at other temperatures. 95.4% of CH4 conversion and 84.6% of CO2 conversion were achieved at 850℃ under atmospheric pressure and with feed composition of n( CH4 )/n ( CO2 )/n ( H2 O)/n ( 02 ) = 1/0.48/0.54/0.1 and space velocity of 10 080 h^-1. High temperature and low pressure are favorable to TRM reaction. Feed compositions affect only on CO2 conversion and n(H2)/n(CO) ratio of syngas, whereas not on CH4 conversion.