结构化学2024,Vol.43Issue(4) :7-14.DOI:10.1016/j.cjsc.2024.100247

Solid-state NMR study of the stability of MOR framework aluminum

Xinzhi Ding Chong Liu Jing Niu Nan Chen Shutao Xu Yingxu Wei Zhongmin Liu
结构化学2024,Vol.43Issue(4) :7-14.DOI:10.1016/j.cjsc.2024.100247

Solid-state NMR study of the stability of MOR framework aluminum

Xinzhi Ding 1Chong Liu 2Jing Niu 2Nan Chen 3Shutao Xu 2Yingxu Wei 2Zhongmin Liu4
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作者信息

  • 1. National Engineering Research Center of Lower-Carbon Catalysis Technology,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,China;University of Chinese Academy of Sciences,Beijing 100049,China
  • 2. National Engineering Research Center of Lower-Carbon Catalysis Technology,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,China
  • 3. National Engineering Research Center of Lower-Carbon Catalysis Technology,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian,116023,China;School of Chemistry,Dalian University of Technology,Dalian,116024,China
  • 4. National Engineering Research Center of Lower-Carbon Catalysis Technology,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian,116023,China;State Key Laboratory of Catalysis,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian,116023,China
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Abstract

MOR zeolite has been effectively utilized for dimethyl ether(DME)carbonylation reaction due to its unique pore structure and acidity.During industrial production,the transformation of ammonium type MOR zeolite(NH4-MOR)into proton type MOR zeolite(H-MOR)causes inevitable dealumination.Therefore,understanding the influencing factors and dynamic evolution mechanism of zeolite dealumination is crucial.In this work,the sta-bility of framework aluminum was studied by X-ray diffraction(XRD),Fourier transform infrared(FT-IR)spec-troscopy,29Si,27Al,1H magic angle spinning nuclear magnetic resonance(MAS NMR),and DME carbonylation performance evaluation.These results indicate that extra-framework cation Na+and NH4+could better preserve the aluminum structure of the MOR zeolite framework compared to H+,primarily due to the different'attraction'of the framework to water.Furthermore,the impact of water on the zeolite framework aluminum at high tem-perature was studied by manipulating the humidity of the calcination atmosphere,revealing the formation of extra-framework six-coordinated aluminum(Al(Ⅵ)-EF)and the mechanism of water influence on the zeolite framework aluminum.

Key words

H-MOR/Solid-state NMR/H2O/Framework aluminum stability/Dealumination

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出版年

2024
结构化学
中国化学会 中国科学院福建物质结构研究所

结构化学

影响因子:0.44
ISSN:0254-5861
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