Details
| Original language | English |
|---|---|
| Pages (from-to) | 4030-4042 |
| Number of pages | 13 |
| Journal | New journal of chemistry |
| Volume | 48 |
| Issue number | 9 |
| Early online date | 29 Jan 2024 |
| Publication status | Published - 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 subject areas
- Chemical Engineering(all)
- Catalysis
- Chemistry(all)
- General Chemistry
- Materials Science(all)
- Materials Chemistry
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In: New journal of chemistry, Vol. 48, No. 9, 2024, p. 4030-4042.
Research output: Contribution to journal › Article › Research › peer review
}
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.
AB - 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.
UR - http://www.scopus.com/inward/record.url?scp=85185167124&partnerID=8YFLogxK
U2 - 10.1039/d3nj03424k
DO - 10.1039/d3nj03424k
M3 - Article
AN - SCOPUS:85185167124
VL - 48
SP - 4030
EP - 4042
JO - New journal of chemistry
JF - New journal of chemistry
SN - 1144-0546
IS - 9
ER -