模板剂碳化的分子筛限域合成金属纳米簇催化剂及其低温加氢脱芳影响机制

多环芳烃的高效脱除是目前石油化工行业亟待解决的重要科学问题。加氢脱芳反应是脱除多环芳烃的有效途径。它是一个分子数减少的强放热可逆反应，高的反应压力和低的反应温度更加有利于芳烃的加氢饱和。然而，目前加氢脱芳催化剂性能差已成为制约芳烃脱除效率的技术瓶颈。本项目旨在研究萘在固定床上的加氢脱芳反应，并从不同角度提出一种非常简洁的制备高活性催化剂的新策略，即利用模板剂碳化后的分子筛来限域合成低温下具有超高加氢脱芳活性的超小金属纳米簇催化剂。在固定床反应器中，对该类催化剂的加氢脱芳性能和反应机理进行系统研究。研究分子筛类型、金属中心类型、残留的碳物种结构等对催化剂金属纳米簇结构的影响，得到不同催化剂对萘加氢脱芳的反应机理，探索不同的催化剂结构与催化剂活性、稳定性和脱芳产物选择性之间的构效关系。希望通过本项目的研究，尽早开发出低温活性、耐硫性和稳定性都远超贵金属的新型加氢脱芳催化剂。

The efficient removal of polycyclic aromatic hydrocarbon (PAH) is an important scientific problem urgently needed to be solved in the petrochemical industry. Hydrodearomatization (HDA) is an effective way to remove PAHs. It is a strong exothermic reversible reaction with reduced molecular number. High pressure and low temperature are more conducive to the reaction. However, the poor performance of HDA catalysts has become a technical bottleneck restricting the efficiency of aromatics removal. The purpose of this project is to study the HDA reaction of naphthalene in a fixed bed, and propose a new strategy for preparation of highly active catalysts from different perspectives. In other words, the template carbonized zeolites were used to synthesize ultra-small metal nanocluster catalysts with ultra-high HDA activity at low temperature. The HDA performance and reaction mechanism of these catalysts will be systematically studied in a fixed bed reactor. The effects of zeolite type, metal active phase and residual carbon species on the structure of metal nanoclusters of catalysts will be studied. We hope to obtain the reaction mechanism of naphthalene HDA with different catalysts, and explore the structure-activity relationship between different catalysts and catalyst activity, stability and selectivity of dearomatization products. Finally, we hope to develop a new HDA catalyst, which has higher activity, sulfur resistance and stability than noble metal catalyst.