Direct observation of tin sites and their reversible interconversion in zeolites by solid-state NMR spectroscopy

Metal-substituted zeolites are an important type of solid Lewis acid with a wide range of applications. Despite the importance of this type of catalyst, identifying active sites can be challenging because different types of metal sites experience similar environments in zeolites. Here we show direct...

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Veröffentlicht in:Communications chemistry Jg. 1; H. 1
Hauptverfasser: Qi, Guodong, Wang, Qiang, Xu, Jun, Wu, Qinming, Wang, Chao, Zhao, Xingling, Meng, Xiangju, Xiao, Fengshou, Deng, Feng
Format: Journal Article
Sprache:Englisch
Veröffentlicht: London Nature Publishing Group UK 19.04.2018
Nature Publishing Group
Schlagworte:
639/638/11/878
639/638/440
639/638/77/887
Catalysts
Chemistry
Chemistry and Materials Science
Chemistry/Food Science
Hydroxyl groups
Identification methods
Lewis acid
NMR spectroscopy
Protons
Solid state
Spectrum analysis
Substitutes
Tin
Zeolites
ISSN:2399-3669, 2399-3669
Online-Zugang:Volltext
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Abstract Metal-substituted zeolites are an important type of solid Lewis acid with a wide range of applications. Despite the importance of this type of catalyst, identifying active sites can be challenging because different types of metal sites experience similar environments in zeolites. Here we show direct observation of different tin sites in Sn-β zeolite. Two types of open tin sites are unambiguously identified via correlating the hydroxyl groups to Sn atoms with one- and two-dimensional proton-detected 1 H/ 119 Sn correlation solid-state NMR spectroscopy, which only amounts to ca. 17% of the total tin content. A reversible transformation between the open and closed tin site is observed. The results provide valuable insights into the nature of tin sites in Sn-β zeolite and open an avenue for the use of proton-detected solid-state NMR methods for characterization of metal sites in zeolite catalysts. Identifying active sites in metal-substituted zeolite catalysts can be challenging as different metal sites can have similar molecular environments. Here the authors use solid-state NMR to identify two different open tin sites in Sn-β zeolite, and to detect a reversible conversion between open and closed sites.
AbstractList Metal-substituted zeolites are an important type of solid Lewis acid with a wide range of applications. Despite the importance of this type of catalyst, identifying active sites can be challenging because different types of metal sites experience similar environments in zeolites. Here we show direct observation of different tin sites in Sn-β zeolite. Two types of open tin sites are unambiguously identified via correlating the hydroxyl groups to Sn atoms with one- and two-dimensional proton-detected 1H/119Sn correlation solid-state NMR spectroscopy, which only amounts to ca. 17% of the total tin content. A reversible transformation between the open and closed tin site is observed. The results provide valuable insights into the nature of tin sites in Sn-β zeolite and open an avenue for the use of proton-detected solid-state NMR methods for characterization of metal sites in zeolite catalysts.Identifying active sites in metal-substituted zeolite catalysts can be challenging as different metal sites can have similar molecular environments. Here the authors use solid-state NMR to identify two different open tin sites in Sn-β zeolite, and to detect a reversible conversion between open and closed sites.
Metal-substituted zeolites are an important type of solid Lewis acid with a wide range of applications. Despite the importance of this type of catalyst, identifying active sites can be challenging because different types of metal sites experience similar environments in zeolites. Here we show direct observation of different tin sites in Sn-β zeolite. Two types of open tin sites are unambiguously identified via correlating the hydroxyl groups to Sn atoms with one- and two-dimensional proton-detected 1 H/ 119 Sn correlation solid-state NMR spectroscopy, which only amounts to ca. 17% of the total tin content. A reversible transformation between the open and closed tin site is observed. The results provide valuable insights into the nature of tin sites in Sn-β zeolite and open an avenue for the use of proton-detected solid-state NMR methods for characterization of metal sites in zeolite catalysts.
Metal-substituted zeolites are an important type of solid Lewis acid with a wide range of applications. Despite the importance of this type of catalyst, identifying active sites can be challenging because different types of metal sites experience similar environments in zeolites. Here we show direct observation of different tin sites in Sn-β zeolite. Two types of open tin sites are unambiguously identified via correlating the hydroxyl groups to Sn atoms with one- and two-dimensional proton-detected 1 H/ 119 Sn correlation solid-state NMR spectroscopy, which only amounts to ca. 17% of the total tin content. A reversible transformation between the open and closed tin site is observed. The results provide valuable insights into the nature of tin sites in Sn-β zeolite and open an avenue for the use of proton-detected solid-state NMR methods for characterization of metal sites in zeolite catalysts. Identifying active sites in metal-substituted zeolite catalysts can be challenging as different metal sites can have similar molecular environments. Here the authors use solid-state NMR to identify two different open tin sites in Sn-β zeolite, and to detect a reversible conversion between open and closed sites.
ArticleNumber 22
Author Wu, Qinming
Zhao, Xingling
Wang, Chao
Xu, Jun
Qi, Guodong
Deng, Feng
Xiao, Fengshou
Wang, Qiang
Meng, Xiangju
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  givenname: Guodong
  surname: Qi
  fullname: Qi, Guodong
  organization: National Centre for Magnetic Resonance in Wuhan, State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, Key Laboratory of Magnetic Resonance in Biological Systems, Wuhan Institute of Physics and Mathematics, Chinese Academy of Sciences
– sequence: 2
  givenname: Qiang
  surname: Wang
  fullname: Wang, Qiang
  organization: National Centre for Magnetic Resonance in Wuhan, State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, Key Laboratory of Magnetic Resonance in Biological Systems, Wuhan Institute of Physics and Mathematics, Chinese Academy of Sciences
– sequence: 3
  givenname: Jun
  surname: Xu
  fullname: Xu, Jun
  email: xujun@wipm.ac.cn
  organization: National Centre for Magnetic Resonance in Wuhan, State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, Key Laboratory of Magnetic Resonance in Biological Systems, Wuhan Institute of Physics and Mathematics, Chinese Academy of Sciences
– sequence: 4
  givenname: Qinming
  surname: Wu
  fullname: Wu, Qinming
  organization: Department of Chemistry, Zhejiang University
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  givenname: Chao
  surname: Wang
  fullname: Wang, Chao
  organization: National Centre for Magnetic Resonance in Wuhan, State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, Key Laboratory of Magnetic Resonance in Biological Systems, Wuhan Institute of Physics and Mathematics, Chinese Academy of Sciences
– sequence: 6
  givenname: Xingling
  surname: Zhao
  fullname: Zhao, Xingling
  organization: National Centre for Magnetic Resonance in Wuhan, State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, Key Laboratory of Magnetic Resonance in Biological Systems, Wuhan Institute of Physics and Mathematics, Chinese Academy of Sciences
– sequence: 7
  givenname: Xiangju
  surname: Meng
  fullname: Meng, Xiangju
  organization: Department of Chemistry, Zhejiang University
– sequence: 8
  givenname: Fengshou
  surname: Xiao
  fullname: Xiao, Fengshou
  organization: Department of Chemistry, Zhejiang University
– sequence: 9
  givenname: Feng
  surname: Deng
  fullname: Deng, Feng
  email: dengf@wipm.ac.cn
  organization: National Centre for Magnetic Resonance in Wuhan, State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, Key Laboratory of Magnetic Resonance in Biological Systems, Wuhan Institute of Physics and Mathematics, Chinese Academy of Sciences
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SSID ssj0002013778
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Snippet Metal-substituted zeolites are an important type of solid Lewis acid with a wide range of applications. Despite the importance of this type of catalyst,...
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crossref
springer
SourceType Aggregation Database
Enrichment Source
Index Database
Publisher
SubjectTerms 639/638/11/878
639/638/440
639/638/77/887
Catalysts
Chemistry
Chemistry and Materials Science
Chemistry/Food Science
Hydroxyl groups
Identification methods
Lewis acid
NMR spectroscopy
Protons
Solid state
Spectrum analysis
Substitutes
Tin
Zeolites
Title Direct observation of tin sites and their reversible interconversion in zeolites by solid-state NMR spectroscopy
URI https://link.springer.com/article/10.1038/s42004-018-0023-1
https://www.proquest.com/docview/2389680595
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