Examination onto the mechanism of the heterogeneously catalyzed partial oxidation of acrolein to acrylic acid on heteropolyacids - structure, function and dynamics of the catalyst

用瞬时动力学方法(如TP反应、SSITKA)和动力学模拟研究了Mo/V/W复合氧化物上丙烯醛部分氧化制丙烯酸的非均相催化反应。通过这种方法，可以大大扩展对反应动力学和机理的理解，例如在[Jekewitz2012]中。然而，在甲基丙烯醛的部分氧化中，杂多酸被用于工艺过程(例如，H_2CS_2[Mo11PVOx])。遗憾的是，对于这种多相催化反应，在动力学和催化机理的理解方面还存在着知识空白。在已有的Mo/V/W复合氧化物上丙烯醛部分氧化催化机理的基础上，对杂多酸催化丙烯醛部分氧化的机理进行了探讨。因此，为了获得更详细的杂多酸的动力学、结构和功能的原位信息，应采用瞬变动力学方法和结构化学研究。如果人们成功地理解了混合氧化物和杂多酸反应机理的差异，这可能会导致工业应用过程的改进(从甲基丙烯醛到甲基丙烯酸对杂多酸)。

The heterogeneously catalyzed partial oxidation of acrolein to acrylic acid on Mo/V/W-mixed oxides was examined in the working group of Prof. Vogel via transient kinetic methods (e.g., TPReaction, SSITKA) as well as kinetic simulations. The understanding about the reaction kinetics and the mechanism could be extended by this approach considerably, e.g., in [Jekewitz2012]. In the partial oxidation of methacrolein, however, heteropolyacids are applied in technical processes (e.g., H2Cs2 [Mo11PVOx]). Unfortunately, for this heterogeneous catalyzed reaction knowledge gaps are still existing, about the understanding of the kinetics and the catalytic mechanism. Based on the well-known catalytic mechanism of the partial oxidation of acrolein on Mo/V/W-mixed oxides the mechanism of the partial oxidation of acrolein on heteropolyacids should be cleared up. Therefore, transient kinetic methods and structural chemical investigations should be applied in order to gain more detailed in situ information about the dynamics, structure and function of the heteropolyacids. If one succeeds in understanding the differences between the mechanisms on mixed oxides and heteropolyacids, this could lead to the improvement of the industrially applied process (methacrolein to methacrylic acid on heteropolyacids).