Luo Jinsong, Xiao Tianci, Liu Chengyuan, Pan Yang
National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui, 230029, P. R. China.
ChemSusChem. 2025 Jan 14;18(2):e202400884. doi: 10.1002/cssc.202400884. Epub 2024 Sep 23.
This review summarized the recent research progress on the crucial role of formaldehyde during the methanol-to-hydrocarbons (MTH) reaction. As a reaction intermediate, formaldehyde participates in the formation of carbon-carbon, the establish of dual-cycle, and the coking process of MTH reaction. Different techniques for formaldehyde detection in the study of MTH are also introduced.The conversion of methanol-to-hydrocarbons (MTH) over zeolite catalysts has been the subject of intense research since its discovery. Great effort has been devoted to the investigation of four key topics: the initiation of C-C bonds, the establishment of hydrocarbon pool (HCP), the adjustment of product selectivity, and the deactivation process of catalysts. Despite 50 years of study, some mechanisms remain controversial. However, an intermediate species, formaldehyde (HCHO), has recently garnered considerable attention for its influence on the entire MTH process. The discovery of HCHO and its significant role in the MTH process has been facilitated by the application of in situ analytical techniques, such as synchrotron radiation photoionization mass spectrometry (SR-PIMS) and photoelectron photoion coincidence spectroscopy (PEPICO). It is now revealed that HCHO is involved in the initiation, propagation, and termination process of MTH reaction. Such mechanistic understanding of HCHO's involvement has provided valuable insights for optimizing the MTH process.
本综述总结了近期关于甲醛在甲醇制烃(MTH)反应中关键作用的研究进展。作为反应中间体,甲醛参与了碳 - 碳键的形成、双循环的建立以及MTH反应的结焦过程。还介绍了MTH研究中甲醛检测的不同技术。自发现以来,甲醇在沸石催化剂上转化为烃(MTH)一直是深入研究的课题。人们致力于研究四个关键主题:碳 - 碳键的引发、烃池(HCP)的建立、产物选择性的调节以及催化剂的失活过程。尽管经过了50年的研究,一些机理仍存在争议。然而,一种中间物种甲醛(HCHO)最近因其对整个MTH过程的影响而备受关注。原位分析技术的应用,如同步辐射光电离质谱(SR - PIMS)和光电子 - 光电离符合光谱(PEPICO),促进了HCHO的发现及其在MTH过程中的重要作用。现在已经揭示,HCHO参与了MTH反应的引发、传播和终止过程。对HCHO参与过程的这种机理理解为优化MTH过程提供了有价值的见解。