基于金属与酸性位平衡调控的M/Zeolite协同催化苯加氢烷基化研究

采用双功能催化剂将苯加氢烷基化反应协同耦合为一步是合成环己基苯（CHB）的理想途径，较苯与环己烯烷基化和联苯加氢路线，前者合成CHB将会在技术、环保、效率等方面显示出优良的应用前景。但是目前对苯加氢烷基化反应的催化剂结构与双功能活性位的协同机制尚未有系统的研究，限制了催化剂理性设计和工业化应用。本项目基于研究M/Zeolite催化剂中金属位和酸性位的平衡关系及协同作用机制，从双功能催化剂的控制构筑入手，设计合成一系列金属位和酸性位性质可调控的负载型M/Zeolite催化剂用于苯加氢烷基化反应研究。通过化学吸附和原位光谱等表征技术，研究金属与酸性位的匹配关系和CHB选择性与收率的内在关联。结合DFT计算，揭示其在不同功能区的协同反应机制，阐明催化剂结构与性能之间的构效关系，实现对两种活性位点的定向调控，为新一代苯加氢烷基化合成CHB催化剂开发提供理论基础和技术支撑。

The synergistic coupling of benzene hydrogenation and alkylation on bifunctional catalysts is an ideal way to synthesize cyclohexylbenzene (CHB). Compared with the alkylation of benzene with cyclohexene and biphenyl hydrogenation, the hydroalkylation of benzene shows larger application prospects in technology, environmental friendliness, and efficiency. Until now, the structure of catalysts and the synergistic mechanism of bifunctional sites for benzene hydroalkylation have not been systematically studied, which limits the rational design and industrial application of the catalysts. In order to identify the metal/acid balance and further understand the coupling reaction mechanism, a series of supported M/Zeolite catalysts were designed and synthesized for benzene hydroalkylation. Moreover, the ratio of metal/acid sites are carefully evaluated to reveal its critical role in the reaction. This project investigates the intrinsic correlation between the metal acidic balance and the selectivity as well as yield of CHB with chemisorption and in situ spectroscopy technology. With the power of DFT calculation, the study can also reveal the synergistic reaction mechanism in different functional regions, clarify the structure-activity relationship, and precisely control the formation of the two active sites and their synergy effects. The methodology of combining experimental evidence and computational simulation provides the theoretical basis and feasible experimental support for the development of catalyst formulation for hydroalkylation of benzene to CHB.