改良铜钴催化剂体系上由合成气制混合醇的研究

Syngas Conversion to Mixed Alcohols over Modified Cu-Co Catalysts

在铜钴基催化剂体系上，由合成气制备混合醇的反应在６．０ＭＰａ的条件下进行．双活性组分体系中铜和钴是以强相互作用状态而共存的，分子探针实验表明，铜和钴的并存对于确保醇的碳链增长是重要的，助剂ＭｏＯ_ｘ的加入显著提高了Ｌａ_２Ｚｒ_２Ｏ_７担载的铜钴基催化剂Ｃｏ／ＣｕＬＺ的活性和选择性，其作用主要表现为通过氢的可逆溢流效应而改善了体系的氢化性能，和增大了ＣＯ的插入反应能力。在改良催化剂体系上，获得了５３％的醇选择性和１４７ｇ／Ｋｇｃａｔ／ｈ的混合醇产率，内含３３％的高级醇。

The conversion of syngas to mixed alcohols has been studied with Co-Cu based catalysts supported on La-Zr oxides,modified by the MoOx promoter. The presence of MoOx improves both activity and selectivity of a Co/ CuLZ catalyst greatly. For example, a productivity of 147 g alcohols/ Kg cat/h with 33 wt% of higher alcohols and a total selectivity of 53% to alcohols were obtained. TPR experiments indicated clearly that a strong interaction between Cu and Co or between Co, Cu and Mo is necessary for the improvements of activity and selectivity. Probe molecule experiments(C2H4 added into the syngas ) showed that both monometallic Co and Cu systems possess only slight CO insertion ability into the metal-alkyl group, whereas a synergetic effect between Co and Cu improves their CO insertion ability.Addition of MoOx confirms that a good synergy between Co, Cu and Mo is significant. Another effect of the MoOx promoter is to increase their hydrogenation activity.