节点文献
CO在负载型Ru、Co和Ru-Co金属簇催化剂上的脱附及表面加H2反应
DESORPTION AND HYDROGENATION OF CO ON SUPPORTED Ru,Co AND Ru-Co CLUSTER CATALYSTS
【摘要】 担载于Al_2O_3和ZrO_2上的三种金属羰基络合物在He气中进行程序升温分解(TPDE)时,其羰基发生表面歧化反应生成CO_2能力的次序为NaRuCo_3(CO)_(12)>>Ru_3(CO)_(12)>>C_3H_7CCo_3(CO)_9。吸附于担载Ru_3和Co_3上的CO在He气中进行程序升温脱附(TPD)时发生表面歧化反应生成CO_2。在H_2气中,吸附于担载Ru_3上的CO力H_2生成CH_4,吸附于担载Co_3上的CO却生成Co_2,在担载RuCo_3上的CO几乎完全力H_2生成CH_4。以ZrO_2为载体的Ru_3、Co_3和RuCo_3催化剂上的CO吸附和反应能力均大于以Al_2O_3为载体者。吸附于以ZrO_2为载体的RuCo_3催化剂上的CO在TPD和IR谱上并不显示CO物种的存在,分析了C_(ads)和O_(ads)物种存在的原因。根据实验结果还讨论了金属、载体对催化性能的影响和表面反应机理。
【Abstract】 TPDE-GC results show that the ability for disproportionation of carbonylgroups in three metal carbonyls supported on Al2O3 and ZrO2 follows the follwing order :NaRuCo3(CO)12》Ru3(CO)12》C3H7CCo3(CO)9.During the TPD of CO adsorbed on Ru3and Co3 catalysts prepared from supported complexes in He stream,the desorbed productwas CO2.It is obvious that the CO2 was formed from the surface disproportionation of COadsorbed on both catalysts,During the TPSR of CO in H2 stream,the CO adsorbed on sup-ported Ru3 catalysts was mainly hydrogenated to CH4.However,the reaction product of COadsorbed on supported Co3 catalysts was composed essentially of CO2.It is noticed that theadsorbed species of CO on RuCo3/ZrO2 was not observed in TPD-GC profile and IR spectra.Nevertheless,during the TPSR of CO in H2 stream,Iarge amount of CH4 in reaction productwas observed. It seems that the CO on RuCo3/ZrO2 catalyst prepared from NaRuCo3(CO)12complex is easily dissociated to Cadsand Oads due to the common action of Na ̄+ and ZrO2.TP-SR-GC results show that the abilities for adsorption and reaction of CO on Ru3, Co3 andRuCo3 supported on ZrO2 are higher than those with as the support Al2O3.The selectivity tomethane in the conversion of CO on supported RuCo3 is higher than that on supported Ru.
【Key words】 supported carbonyl metal cluster; decarbonylation; dispersed Ru3; Co3 and RuCo3 catalysts; desorption and surface reaction of CO; surface hydrogena- tion of CO;
- 【文献出处】 燃料化学学报 ,JOURNAL OF FUEL CHEMISTRY AND TECHNOLOGY , 编辑部邮箱 ,1994年01期
- 【分类号】TQ
- 【被引频次】8
- 【下载频次】116