固体核磁共振技术在甲醇制烯烃反应中的应用
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高树树 1,2,徐舒涛 1,*( ),魏迎旭 1,刘中民 1
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Applications of Solid-State Nuclear Magnetic Resonance Spectroscopy in Methanol-to-Olefins Reaction
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Shu-shu GAO 1,2,Shu-tao XU 1,*( ),Ying-xu WEI 1,Zhong-min LIU 1
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图4. (a) 275 ℃下,13C-甲醇在H-SSZ-13催化剂上转化的原位13C MAS NMR谱图,其中154、245 ppm为五甲基环戊烯基正离子(PMCP+)特征峰,0~40 ppm为烷烃类物种;(b) ①以甲醇为原料,通过直接反应机理生成初始乙烯;②初始乙烯产生MCP类物种;③ MCP类物种与甲醇共反应生成PMBs物种;④通过间接机制包括芳烃循环、烯烃循环和环戊二烯循环生成烯烃[47]
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Fig.4. (a) In situ 13C MAS NMR spectra of 13CH3OH reaction over H-SSZ-13 catalyst at 275 ℃, the characteristic signals at 154 and 245 ppm illustrate the formation of pentamethylcyclopentenyl cation (PMCP+), 0~40 ppm are assigned to the paraffin; (b) ① The initial ethene is generated from methanol by direct mechanism; ② MCP species are produced from initial ethene; ③ PMBs species are produced from the co-reaction of MCP species and methanol; ④ The olefins are formed via indirect mechanism including of aromatics-based, alkenes-based, and cyclopentadienes based cycles[47]
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