Development of novel ammoxidation catalysts with tailored anion structures based on transition metal nitrides and oxynitrides

丙烯腈（ACN）是化学工业中用于制造丙烯酸纤维、聚合物和涂料的重要中间体，目前通过昂贵且日益稀缺的丙烯的氨氧化来生产。该项目旨在开发新的催化剂，使其能够使用更便宜和丰富的丙烷，这具有很高的工业利益，经济潜力和可持续性，因为可以更有效地利用自然资源（天然气和石油）。尽管在过去十年中进行了大量研究，但丙烷基ACN工艺仍处于起步阶段。目前，最好的催化剂是基于公知的MoVNbTe混合氧化物（“Mitsubishi”系统），其提供仅60%的最大ACN产率。提高催化剂性能的尝试主要基于改性催化剂阳离子组成，但成功有限。因此，预期使用“Mitsubishi”催化剂的基于丙烷的ACN路线不能再显著改进。因此，应开发定制催化剂的新路线，其不仅像往常一样改变MoVNbTe氧化物中的阳离子组成，而且利用不同阴离子结构的独特性质，例如，例如，在一个实施例中，由混合的过渡金属氮化物和氮氧化物制成。将遵循一种复杂，合理的方法，将催化剂合成，在工作条件下探索催化剂功能，以及催化测试和动力学研究，利用两个合作实验室在研究计划的每个步骤中的互补技能。为了探索新型催化剂的结构特征在芳烃底物氨氧化反应中的应用潜力和作用，还将使用甲苯作为反应物。

Acrylonitrile (ACN) is an important intermediate in chemical industry for the manufacture of acrylic fibres, polymers and coatings being currently produced by ammoxidation of costly and increasingly scarce propylene. This project aims at developing novel catalysts allowing the use of cheaper and abundant propane, which is of high industrial interest, economic potential and sustainability, since natural resources (gas and oil) can be more efficiently used. Despite much research in the last decade, propane-based ACN processes are still in their infancy. Currently, the best catalysts are based on well-known MoVNbTe mixed oxides (“Mitsubishi” systems) which provide maximum ACN yields of only 60 %. Attempts to enhance the catalytic performance were mainly based on modifying the catalysts cation composition, yet with limited success. Therefore, it is anticipated that the propane-based route to ACN using “Mitsubishi” catalysts cannot be considerably improved anymore. Hence, novel routes to tailored catalysts shall be developed, which do not just vary the cation composition in MoVNbTe oxides as usual, but exploit the unique properties of different anion structures, e. g., from mixed transition metal nitrides and oxynitrides. A complex, rational approach will be followed that integrates catalyst synthesis, catalyst function explored under working conditions as well as catalytic tests and kinetic studies, taking advantage of the complementary skills of the two collaborating laboratories in each step of the research program. For exploring the application potential and the role of structural features of the new catalysts with respect to ammoxidation of aromatic substrates, toluene shall also be used as reactant.