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Formation and Fate of Formaldehyde in Methanol-to-Hydrocarbon Reaction: In Situ Synchrotron Radiation Photoionization Mass Spectrometry Study
Authors:Wu Wen  Shengsheng Yu  Chaoqun Zhou  Prof. Hao Ma  Prof. Zhongyue Zhou  Chuangchuang Cao  Dr. Jiuzhong Yang  Minggao Xu  Prof. Fei Qi  Prof. Guobin Zhang  Prof. Yang Pan
Affiliation:1. National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui, 230029 P. R. China;2. Key Laboratory for Power Machinery and Engineering of Ministry of Education, Shanghai Jiao Tong University, Shanghai, 200240 P. R. China
Abstract:HCHO has been confirmed as an active intermediate in the methanol-to-hydrocarbon (MTH) reaction, and is critical for interpreting the mechanisms of coke formation. Here, HCHO was detected and quantified during the MTH process over HSAPO-34 and HZSM-5 by in situ synchrotron radiation photoionization mass spectrometry. Compared with conventional methods, excellent time-resolved profiles were obtained to study the formation and fate of HCHO, and other products during the induction, steady-state reaction, and deactivation periods. Similar formation trends of HCHO and methane, and their close correlation in yields suggest that they are derived from disproportionation of methanol at acidic sites. In the presence of Y2O3, the amount of HCHO changes, affecting the hydrogen-transfer processes of olefins into aromatics and aromatics into cokes. The yield of HCHO affects the aromatic-based cycle and the formation of ethylene, indicating that ethylene is mainly formed from the aromatic-based cycle.
Keywords:Formaldehyd  Massenspektrometrie  Reaktionsmechanismen  Oberflächenchemie  Zeolithe
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