天然气化工
天然氣化工
천연기화공
NATURAL GAS CHEMICAL INDUSTRY
2001年
3期
23-26
,共4页
杨意泉%王琪%杨华%袁友珠%于腊佳%戴深峻
楊意泉%王琪%楊華%袁友珠%于臘佳%戴深峻
양의천%왕기%양화%원우주%우석가%대심준
甲硫醇%钼基催化剂%ESR%XPS
甲硫醇%鉬基催化劑%ESR%XPS
갑류순%목기최화제%ESR%XPS
研究以(NH4)6Mo7O24*4H2O为前驱物料所制得的MoO3/K2CO3/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K2CO3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=2.01,g=2.04)等信号,随着K2CO3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-(161.5eV)、(S-S)2-(162.5eV)和S6+(168.5eV)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。
研究以(NH4)6Mo7O24*4H2O為前驅物料所製得的MoO3/K2CO3/SiO2催化劑對高硫化氫閤成氣一步法閤成甲硫醇的催化活性,攷察K2CO3助劑對鉬基催化劑催化行為的影響。ESR錶徵結果顯示,工作態催化劑觀測到氧包圍的"oxo-Mo(V)"(g=1.93)、硫包圍的"thio-Mo(V)"(g=1.98)和S(g=2.01,g=2.04)等信號,隨著K2CO3添加量的增加,oxo-Mo(V)含量增加,thio-Mo(V)含量減少;XPS錶徵顯示,鉬包含瞭Mo4+、Mo5+和Mo6+的混閤價態,硫包含瞭S2-(161.5eV)、(S-S)2-(162.5eV)和S6+(168.5eV)等3種物種,Mo5+/Mo4+摩比為0.4和S2-/(S-S)2-比接近1有利于甲硫醇的生成。
연구이(NH4)6Mo7O24*4H2O위전구물료소제득적MoO3/K2CO3/SiO2최화제대고류화경합성기일보법합성갑류순적최화활성,고찰K2CO3조제대목기최화제최화행위적영향。ESR표정결과현시,공작태최화제관측도양포위적"oxo-Mo(V)"(g=1.93)、류포위적"thio-Mo(V)"(g=1.98)화S(g=2.01,g=2.04)등신호,수착K2CO3첨가량적증가,oxo-Mo(V)함량증가,thio-Mo(V)함량감소;XPS표정현시,목포함료Mo4+、Mo5+화Mo6+적혼합개태,류포함료S2-(161.5eV)、(S-S)2-(162.5eV)화S6+(168.5eV)등3충물충,Mo5+/Mo4+마비위0.4화S2-/(S-S)2-비접근1유리우갑류순적생성。
The catalytic activity of MoO3/K2CO3/SiO2 prepared with precursor (NH4)6Mo7O24 for the methantiol directly synthesis from syngas blending with high H2S content and the effects of promoter K2CO3 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 K2CO3 content increasing,while thio-Mo(V) was found to decrease.The XPS characterization indicated that Mo4+,Mo5+ and Mo6+ are main species included in the Mo content,and that S2- (161.5eV),(S-S)2-(162.5eV) and S6+(168.5eV) species are included in the S content.