波谱学杂志 >

2022 , Vol. 39 >Issue 4: 439 - 447

DOI: https://doi.org/10.11938/cjmr20222983

研究论文

SSZ-13分子筛上甲醇转化过程中甲氧基物种的生成与活性研究

  • 覃瑞 ,
  • 王超 ,
  • 王强 ,
  • 胡敏 ,
  • 李金林 ,
  • 徐君 ,
  • 邓风
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  • 1. 中南民族大学, 催化转化与能源材料化学教育部重点实验室, 催化材料科学湖北省重点实验室, 湖北 武汉 430074
    2. 中国科学院精密测量科学与技术创新研究院, 武汉物理与数学研究所, 波谱与原子分子物理国家重点实验室, 武汉磁共振中心, 湖北 武汉 430071
    3. 中国科学院大学, 北京 100049

收稿日期: 2022-03-15

  网络出版日期: 2022-04-28

基金资助

国家自然科学基金资助项目(22072165);国家自然科学基金资助项目(21991092);国家自然科学基金资助项目(U1932218);国家自然科学基金资助项目(21733013);国家自然科学基金资助项目(22061130202);湖北省自然科学基金资助项目(2021CFA021)

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Formation and Reactivity of Surface Methoxy Species in Methanol Conversion over SSZ-13 Zeolite

  • Rui QIN ,
  • Chao WANG ,
  • Qiang WANG ,
  • Min HU ,
  • Jin-lin LI ,
  • Jun XU ,
  • Feng DENG
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  • 1. Key Laboratory of Catalysis and Energy Materials Chemistry of Ministry of Education & Hubei Key Laboratory of Catalysis and Materials Science, South-Central Minzu University, Wuhan 430074, China
    2. National Center for Magnetic Resonance in Wuhan, State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, Wuhan Institute of Physics and Mathematics, Innovation Academy for Precision Measurement Science and Technology, Chinese Academy of Sciences, Wuhan 430071, China
    3. University of Chinese Academy of Sciences, Beijing 100049, China

Received date: 2022-03-15

  Online published: 2022-04-28

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摘要

本文使用固体核磁共振（NMR）技术研究了SSZ-13分子筛上甲醇制烯烃反应过程中表面甲氧基物种的生成以及反应活性.通过二维13C-27Al HMQC NMR方法确证了甲醇在分子筛骨架Brønsted酸位上生成的甲氧基物种，以及在Lewis酸位上生成的另外一种表面甲氧基物种.13C NMR结合气相色谱-质谱（GC-MS）实验结果表明，这两种甲氧基物种在甲醇制烯烃反应中均具有较高的反应活性，既可以导致烃池物种的生成，也可以参与烃池反应生成碳氢化合物.

关键词： SSZ-13分子筛; 固体核磁共振; 甲醇转化; 表面物种; 反应机理

本文引用格式

覃瑞 , 王超 , 王强 , 胡敏 , 李金林 , 徐君 , 邓风 . SSZ-13分子筛上甲醇转化过程中甲氧基物种的生成与活性研究[J]. 波谱学杂志, 2022 , 39(4) : 439 -447 . DOI: 10.11938/cjmr20222983

Abstract

The formation and reactivity of surface methoxy species in methanol reaction over SSZ-13 zeolite were investigated by using solid-state nuclear magnetic resonance (NMR) technique. The surface methoxy species bound to Brønsted acid sites was identified by two-dimensional 13C-27Al heteronuclear multiple quantum coherence (HMQC) NMR experiment. The formation of another surface methoxy species bound to Lewis acid sites was also observed. The combination of 13C NMR and gas chromatography-mass spectrometry (GC-MS) showed that the two kinds of surface methoxy species possess high reactivity, contributing to the formation of hydrocarbon pool species and hydrocarbons via the hydrocarbon pool mechanism.

Key words： SSZ-13 zeolite; solid-state nuclear magnetic resonance; methanol conversion; surface species; reaction mechanism

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