Synthesis and real structure of RUB-11: a novel high-density silica zeolite based on magadiite layers

Publikation: Beitrag in FachzeitschriftArtikelForschungPeer-Review

Autoren

  • Isabel Grosskreuz
  • Yaşar Krysiak
  • Hermann Gies
  • Enrico Mugnaioli
  • Bernd Marler

Organisationseinheiten

Externe Organisationen

  • Ruhr-Universität Bochum
  • Akademie Věd České Republiky (AV ČR)
  • Istituto Italiano di Tecnologia (IIT)
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Details

OriginalspracheEnglisch
Seiten (von - bis)4030-4042
Seitenumfang13
FachzeitschriftNew journal of chemistry
Jahrgang48
Ausgabenummer9
Frühes Online-Datum29 Jan. 2024
PublikationsstatusVeröffentlicht - 2024

Abstract

The discovery of new zeolite framework types plays an important role in producing new porous materials for applications such as adsorption, catalysis, separation, etc. RUB-11, a new all-silica zeolite with high density (2.11 g cm−3), was synthesised at 160 °C from reaction mixtures consisting of SiO2/ethylenediamine/H2O in a xenon atmosphere of 30 bar for a long reaction time (140 d). Physico-chemical characterisation using solid-state NMR spectroscopy, SEM, TG-DSC and ATR-FTIR spectroscopy confirmed that RUB-11 is a framework silicate. The atomic structure was solved by 3D electron diffraction using the fast-automated diffraction tomography method. The structure model of monoclinic symmetry with lattice parameters of a0 = 7.3929(5) Å, b0 = 7.3942(3) Å, c0 = 26.1786(13) Å and β = 98.372(7)° (space group: Pc) was refined against electron diffraction data (dynamical refinement) and powder diffraction data. An additional distance-least-squares refinement confirmed the feasibility of forming a stress-free silica framework of RUB-11 topology. The chemical composition of RUB-11 per unit cell is 30 SiO2. The framework silicate RUB-11 is structurally closely related to layer silicate magadiite and can be regarded as an interlayer expanded zeolite (IEZ) based on magadiite-type layers. Both materials contain topologically identical, dense layers, named m̲a̲g̲ layers. In the case of RUB-11, these layers are interconnected via additional silicon atoms leading to a complete framework with a 2-dimensional pore system consisting of intersecting 8-ring channels. The synthesis route leading to RUB-11 is in contrast to typical IEZs, which are obtained in a two-step process. According to the electron diffraction data and the XRD powder patterns, RUB-11 has a disordered structure. A detailed analysis revealed that two different types of disorder concerning the stacking of layer-like building units (consisting of m̲a̲g̲ layers plus interconnecting silicon atoms) contribute to the real structure of RUB-11. It is surprising that the channel-like pores of RUB-11 are completely empty when separated from the reaction mixture.

ASJC Scopus Sachgebiete

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Synthesis and real structure of RUB-11: a novel high-density silica zeolite based on magadiite layers. / Grosskreuz, Isabel; Krysiak, Yaşar; Gies, Hermann et al.
in: New journal of chemistry, Jahrgang 48, Nr. 9, 2024, S. 4030-4042.

Publikation: Beitrag in FachzeitschriftArtikelForschungPeer-Review

Grosskreuz I, Krysiak Y, Gies H, Mugnaioli E, Marler B. Synthesis and real structure of RUB-11: a novel high-density silica zeolite based on magadiite layers. New journal of chemistry. 2024;48(9):4030-4042. Epub 2024 Jan 29. doi: 10.1039/d3nj03424k
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abstract = "The discovery of new zeolite framework types plays an important role in producing new porous materials for applications such as adsorption, catalysis, separation, etc. RUB-11, a new all-silica zeolite with high density (2.11 g cm−3), was synthesised at 160 °C from reaction mixtures consisting of SiO2/ethylenediamine/H2O in a xenon atmosphere of 30 bar for a long reaction time (140 d). Physico-chemical characterisation using solid-state NMR spectroscopy, SEM, TG-DSC and ATR-FTIR spectroscopy confirmed that RUB-11 is a framework silicate. The atomic structure was solved by 3D electron diffraction using the fast-automated diffraction tomography method. The structure model of monoclinic symmetry with lattice parameters of a0 = 7.3929(5) {\AA}, b0 = 7.3942(3) {\AA}, c0 = 26.1786(13) {\AA} and β = 98.372(7)° (space group: Pc) was refined against electron diffraction data (dynamical refinement) and powder diffraction data. An additional distance-least-squares refinement confirmed the feasibility of forming a stress-free silica framework of RUB-11 topology. The chemical composition of RUB-11 per unit cell is 30 SiO2. The framework silicate RUB-11 is structurally closely related to layer silicate magadiite and can be regarded as an interlayer expanded zeolite (IEZ) based on magadiite-type layers. Both materials contain topologically identical, dense layers, named m̲a̲g̲ layers. In the case of RUB-11, these layers are interconnected via additional silicon atoms leading to a complete framework with a 2-dimensional pore system consisting of intersecting 8-ring channels. The synthesis route leading to RUB-11 is in contrast to typical IEZs, which are obtained in a two-step process. According to the electron diffraction data and the XRD powder patterns, RUB-11 has a disordered structure. A detailed analysis revealed that two different types of disorder concerning the stacking of layer-like building units (consisting of m̲a̲g̲ layers plus interconnecting silicon atoms) contribute to the real structure of RUB-11. It is surprising that the channel-like pores of RUB-11 are completely empty when separated from the reaction mixture.",
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TY - JOUR

T1 - Synthesis and real structure of RUB-11

T2 - a novel high-density silica zeolite based on magadiite layers

AU - Grosskreuz, Isabel

AU - Krysiak, Yaşar

AU - Gies, Hermann

AU - Mugnaioli, Enrico

AU - Marler, Bernd

N1 - Funding Information: This work was financially supported by the Deutsche Forschungsgemeinschaft (Projekt MA 6641/3-1) and the authors thank Dr Ute Kolb, Mainz, Germany, for instructive discussions.

PY - 2024

Y1 - 2024

N2 - The discovery of new zeolite framework types plays an important role in producing new porous materials for applications such as adsorption, catalysis, separation, etc. RUB-11, a new all-silica zeolite with high density (2.11 g cm−3), was synthesised at 160 °C from reaction mixtures consisting of SiO2/ethylenediamine/H2O in a xenon atmosphere of 30 bar for a long reaction time (140 d). Physico-chemical characterisation using solid-state NMR spectroscopy, SEM, TG-DSC and ATR-FTIR spectroscopy confirmed that RUB-11 is a framework silicate. The atomic structure was solved by 3D electron diffraction using the fast-automated diffraction tomography method. The structure model of monoclinic symmetry with lattice parameters of a0 = 7.3929(5) Å, b0 = 7.3942(3) Å, c0 = 26.1786(13) Å and β = 98.372(7)° (space group: Pc) was refined against electron diffraction data (dynamical refinement) and powder diffraction data. An additional distance-least-squares refinement confirmed the feasibility of forming a stress-free silica framework of RUB-11 topology. The chemical composition of RUB-11 per unit cell is 30 SiO2. The framework silicate RUB-11 is structurally closely related to layer silicate magadiite and can be regarded as an interlayer expanded zeolite (IEZ) based on magadiite-type layers. Both materials contain topologically identical, dense layers, named m̲a̲g̲ layers. In the case of RUB-11, these layers are interconnected via additional silicon atoms leading to a complete framework with a 2-dimensional pore system consisting of intersecting 8-ring channels. The synthesis route leading to RUB-11 is in contrast to typical IEZs, which are obtained in a two-step process. According to the electron diffraction data and the XRD powder patterns, RUB-11 has a disordered structure. A detailed analysis revealed that two different types of disorder concerning the stacking of layer-like building units (consisting of m̲a̲g̲ layers plus interconnecting silicon atoms) contribute to the real structure of RUB-11. It is surprising that the channel-like pores of RUB-11 are completely empty when separated from the reaction mixture.

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