甲醇制烯烃（MTO）作为一种替代传统石油裂解制烯烃的可持续发展路线，是当今多相催化领域的研究热点。MTO反应机理，尤其是第一个C-C键的形成过程，是亟待解决的难点。本项目将围绕MTO反应第一个C-C键活性物种形成及其在整个MTO反应机理网络中的作用开展研究。以不同孔道结构的SAPO-34、H-ZSM-5和H-ZSM-22分子筛为研究对象，利用一维13C和17O MAS NMR以及二维1H-13C和1H-17O HETCOR(固体异核化学位移相关谱)技术确定不同分子筛上的初始C-C键含氧物种。利用原位紫外-红外-质谱和原位固体核磁与紫外联用技术确定C-C键活性物种到烃池物种的转化过程。利用周期性密度泛函理论（DFT）对重要反应步骤涉及的过渡态和转化能垒附以理论计算研究。在以上实验和理论研究的基础上，明确MTO反应初始C-C键活性物种以及烃池物种的形成过程，掌握MTO完整反应机理网络。

As an alternative process for obtaining olefins, the methanol-to-olefin (MTO) conversion has attracted extensive attentions in recent years. As an important issue for MTO mechanism, the formation process of the first carbon-carbon (C-C) bond and the complete reaction mechanism are still not clear until now. In this case, the present work will focus on the exact route for the formation of the first C-C bond and the whole reaction mechanism of MTO conversion. Zeolites with different pore structures, e.g., SAPO-34, H-ZSM-5 and H-ZSM-22 will be used as the model catalysts, and the first C-C bond-containing intermediates formed during the MTO conversion will be investigated by one-dimensional (1D) 17O MAS NMR and two-dimensional (2D) NMR experiments (e.g. 1H-17O HETCOR, HETCOR: HETeronuclear CORrelation), and 13C MAS NMR as well as 1H-13C HETCOR NMR spectroscopy. The formation process of the active “hydrocarbon pool” species from the first C-C bond-containing intermediates will be in situ monitored by FTIR-UV/Vis-MS and 13C MAS NMR spectroscopy. The important transition states of the intermediates and the barriers will be investigated by DFT calculations. The successful execution of this project will make it possible to clarify the formation of the first C-C bond, to understand the complete reaction mechanism of the MTO conversion, and to develop reaction routes to desired reaction products with high selectivity.