【摘要】 研究以 (NH4 ) 6Mo7O2 4 ·4H2 O为前驱物料所制得的MoO3 /K2 CO3 /SiO2 催化剂对高硫化氢合成气一步法合成甲硫醇的催化活性 ,考察K2 CO3 助剂对钼基催化剂催化行为的影响。ESR表征结果显示 ,工作态催化剂观测到氧包围的“oxo -Mo(V)”(g =1.93)、硫包围的“thio -Mo(V)”(g =1.98)和S(g =2 .0 1,g =2 .0 4)等信号 ,随着K2 CO3 添加量的增加 ,oxo -Mo(V)含量增加 ,thio -Mo(V)含量减少 ;XPS表征显示 ,钼包含了Mo4 + 、Mo5+ 和Mo6+ 的混合价态 ,硫包含了S2 -(16 1.5eV)、(S -S) 2 -(16 2 .5eV)和S6+ (16 8.5eV)等 3种物种 ,Mo5+ /Mo4 + 摩比为 0 .4和S2 -/ (S -S) 2 -比接近 1有利于甲硫醇的生成更多还原

【Abstract】 The catalytic activity of MoO 3/K 2CO 3/SiO 2 prepared with precursor (NH 4) 6Mo 7O 24 for the methantiol directly synthesis from syngas blending with high H 2S content and the effects of promoter K 2CO 3 on the catalytic behavior of molybdenum based catalyst were studied.The results of ESR characterization show that the signals of O surrounded “oxo Mo(V)”( g =1.93),S surrounded“thio Mo(V)”( g =1.98),and S( g = 2.01 and 2.04)in functioning catalyst can be detected.The content of oxo Mo(V) was found to increase with the added K 2CO 3 content increasing,while thio Mo(V) was found to decrease.The XPS characterization indicated that Mo 4+ ,Mo 5+ and Mo 6+ are main species included in the Mo content,and that S 2- (161.5eV),(S-S) 2- (162.5eV) and S 6+ (168.5eV) species are included in the S content.更多还原