固体核磁共振研究OX-ZEO催化合成气一步高效制芳烃反应机理

OX-ZEO（Oxide-Zeolite）催化合成气制芳烃具有反应流程简单、催化稳定性好和产物选择性高等优点，极具工业应用前景。作为合成气一步制芳烃新路线，反应仍存在诸多机理性问题有待进一步研究。固体NMR是表征多相催化剂微观结构和催化反应机理的有力工具。本项目拟应用和发展前沿固体NMR方法研究OX-ZEO催化合成气制芳烃反应中的几个关键机理问题：1）OX-ZEO上CO的活化位点及其生成、调控机制；2）CO和H2在OX-ZEO表面的活化机理；3）反应活性中间体物种及其芳构化机理；4）中间体、产物等客体分子在OX-ZEO上的扩散动力学性质。项目研究成果将丰富合成气催化转化的物理化学基础，为高效催化剂设计开发、反应工艺的优化提供理论指导，同时推动固体NMR技术在多相催化研究中的应用和发展。

The Syngas-to-Aromatics reactions catalyzed by OX-ZEO (Oxide-Zeolite) catalysts exhibit advantages such as simplified reaction procedures, superb catalytic stability and high product selectivity, showing great potential in further industrialization. As a completely new avenue for the one-step Syngas-to-Aromatics reaction, multiple mechanistic insights remain to be explored. Solid-state NMR has shown to be a powerful tool in analyzing the local structures of heterogeneous catalysts as well as investigating the reaction mechanism of heterogeneous catalysis. In this project, state-of-the-art solid-state NMR techniques will be adopted and developed to study several fundamental issues within the Syngas-to-Aromatics reactions: 1) reactive centers for the activation of CO molecules over the OX-ZEO and their formation mechanism and regulation methods; 2) detailed mechanism of the CO and H2 activation over OX-ZEO; 3) the critical reactive intermediates and their aromatization mechanism; 4) the diffusion kinetics of the guest molecules (intermediates, products) within the OX-ZEO catalysts. We believe these researches will broaden our understanding of the syngas conversion chemistry, provide guidelines for rational design of efficient catalysts and optimization of the process conditions，furthermore, promote the application and development of solid-state NMR techniques in the characterization of heterogeneous catalysis.