甲醇制烯烃“烃池”物种的甲基化、裂化/消去速率匹配研究

当前甲醇制烯烃技术经济性不够理想，对反应机理——“烃池”机理认识不够清楚是高效催化剂及工艺研发的最大阻碍。申请人利用在甲醇转化领域多年的研究积累，从“烃池”机理先甲基化后裂化/消去的基本原理出发缜密分析，认为甲醇制丙烯工艺面临的催化剂失活快、产品收率低等诸多问题均是由裂化/消去速率大于甲基化速率导致的，并基于该观点首次提出研究“甲基化与裂化/消去速率匹配性”问题。通过专门设计、搭建瞬态响应反应装置研究甲醇制烃反应中“烃池”物种甲基化和裂化/消去过程，结合原位红外/紫外光谱、D/13C同位素追踪实验、模型反应及理论计算等手段深入研究影响甲基化、裂化/消去速率的本征因素，揭示“烃池”机理运行本质，在此基础上聚焦调节两个步骤速率匹配的有效手段，最终显著延长甲醇制丙烯催化剂单程寿命，优化产物分布。

The current methanol to olefins/propene (MTO/P) technology is not economical enough, and insufficient understanding of "hydrocarbon pool (HP)" mechanism hinders the development of high efficient catalyst and process. With accumulation of years of research in methanol conversion, the applicant think that fast deactivation, low product yield and many other problems existed in MTP reaction are caused by.the low cracking/elimination (C/E) rate that doesn't match well with the rate of methylation. In this project, the methylation step and the C/E step will be decoupled by a specially designed transient response (TR) device, and the intrinsic factors affecting the methylation and C/E rate will be studied by combining the TR technique with in situ infrared/ultraviolet spectrum, D/13C isotope tracing experiment, model reaction and theoretical calculation, and the nature of HP mechanism will be revealed. On this basis, the relative rate of the two steps will be effectively adjusted, and significantly prolonged lifetime of catalyst and optimized product distribution will be realized.