Layered precursors for new zeolitic materials: Synthesis and characterization of B-RUB-39 and its condensation product B-RUB-41

Grünewald-Lüke, A.; Gies, Hermann; Müller, Ulrich; Yilmaz, Bilge; Imai, Hiroyuki; Tatsumi, Takashi; Xie, Bin; Xiao, Feng‐Shou; Bao, Xinhe; Zhang, Weiping; Vos, Dirk De

doi:10.1016/j.micromeso.2011.05.036

Cited by 16 publications

(19 citation statements)

References 21 publications

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“…suggest that B atoms seem to incorporate into one type of Si sites in the C 16 33 for which the authors concluded that the small amount of B atoms incorporated were preferentially siting in a single T site based on a relatively sharp (ca. 1 ppm fwhm) dominant 11 B NMR peak and XRD data.…”

Section: A Average Long-range Structures From Diffraction and Elemmentioning

confidence: 99%

“…24,25 Previous investigations have suggested near-random 19 or relatively unselective distributions of heteroatoms in zeolite frameworks. In rare cases, heteroatoms are incorporated into specific framework sites (e.g., B in the borosilicate zeolite MCM-70 32 and layered borosilicate RUB-39, 33 Al 21,34 or Ga 35 in natrolite-type zeolites), leading to resolved 29 Si NMR signals. (The Q n notation describes bonding configurations of T-sites, where n refers to the number of connected T-sites for a given T-site.)…”

Section: Introductionmentioning

confidence: 99%

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Local environments of boron heteroatoms in non-crystalline layered borosilicates

Garaga

Hsieh

Nour

et al. 2015

Phys. Chem. Chem. Phys.

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Boron heteroatom distributions are shown to be significantly different in two closely related layered borosilicates synthesized with subtly different alkylammonium surfactant species. The complicated order and disorder near framework boron sites in both borosilicates were characterized at the molecular level by using a combination of multi-dimensional solid-state nuclear magnetic resonance (NMR) spectroscopy techniques and first-principles calculations. Specifically, two-dimensional (2D) solid-state J-mediated (through-bond) (11)B{(29)Si} NMR analyses provide direct and local information on framework boron sites that are covalently bonded to silicon sites through bridging oxygen atoms. The resolution and identification of correlated signals from distinct (11)B-O-(29)Si site pairs reveal distinct distributions of boron heteroatoms in layered borosilicate frameworks synthesized with the different C16H33N(+)Me3 and C16H33N(+)Me2Et structure-directing surfactant species. The analyses establish that boron atoms are distributed non-selectively among different types of silicon sites in the layered C16H33N(+)Me3-directed borosilicate framework, whereas boron atoms are preferentially incorporated into incompletely condensed Q(3)-type sites in the C16H33N(+)Me2Et-directed borosilicate material. Interestingly, framework boron species appear to induce framework condensation of their next-nearest-neighbor silicon sites in the C16H33N(+)Me3-directed borosilicate. By comparison, the incorporation of boron atoms is found to preserve the topology of the C16H33N(+)Me2Et-directed borosilicate frameworks. The differences in boron site distributions and local boron-induced structural transformations for the two surfactant-directed borosilicates appear to be due to different extents of cross-linking of the siliceous frameworks. The molecular-level insights are supported by density functional theory (DFT) calculations, which show the distinct influences of boron atoms on the C16H33N(+)Me3- and C16H33N(+)Me2Et-directed borosilicate frameworks, consistent with the experimental observations.

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Section: A Average Long-range Structures From Diffraction and Elemmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Local environments of boron heteroatoms in non-crystalline layered borosilicates

Garaga

Hsieh

Nour

et al. 2015

Phys. Chem. Chem. Phys.

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“…1 Additionally, detection and quantification limits allow the determination of a diversity of metals and nonmetals in a myriad of sample types such as cements, ceramics, silicates, geological materials, metallosilicates, refractory compounds, aluminophosphates, silicoaluminophosphates, clays, phyllosilicates, and coals. 4,[6][7][8][9][10][11][12][13][14] The chemical analysis of the inorganic solids mentioned above by ICP OES using conventional acid dissolution methods, in open flasks on hot plate, 15 usually involves costly and time-consuming procedures for sample preparation, 3 requiring a long analysis time and large amounts of reagents. Additionally, such conventional procedures do not assure complete dissolution of some solid inorganic samples, especially geological samples 15,16 (including silicates 8,13,17 and aluminosilicates) 14,16 even when a large amount of concentrated acids is used.…”

Section: Introductionmentioning

confidence: 99%

A Straightforward Method for Determination of Al and Na in Aluminosilicates Using ICP OES

Ramos¹,

Almeida²,

Júnior³

et al. 2017

J. Braz. Chem. Soc.

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The improvements on aluminosilicates dissolution through microwave-assisted acid decomposition procedures for Na and Al quantification by inductively coupled plasma optical emission spectrometry (ICP OES) are reported here. Complete dissolution of the samples is achieved employing 4 mL of HNO 3 and 3-4 mL of HF thus reducing the total amount of these reactants in comparison with procedures found in the literature. Additionally, the type of crucibles used in the calcination for sample preparation step is also evaluated. Na and Al concentrations are in agreement with the expected values on the samples. Estimated silicon amount is achieved by difference of sodium and aluminum, and then Si/Al molar ratios were calculated for samples calcined in both porcelain (Si/Al is in the range 22-42) and platinum (Si/Al is in the range 27-40) crucibles, showing no difference between these procedures.

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“…[9,[15][16][17] In our studies of interlayer-expanded zeolites, heteroatoms such as Al or Ti were inserted into the layered precursor, after which the silylation reaction was performed to obtain the pore-expanded materials, which exhibit superior catalytic performances in olefin-selective oxidation or alkane isomerization reactions. [9,[15][16][17] In our studies of interlayer-expanded zeolites, heteroatoms such as Al or Ti were inserted into the layered precursor, after which the silylation reaction was performed to obtain the pore-expanded materials, which exhibit superior catalytic performances in olefin-selective oxidation or alkane isomerization reactions.…”

Section: Introductionmentioning

confidence: 99%

“…Al atom would create acidity and an acidic catalyst, whereas insertion of tetravalent Ti would result in the oxidation catalyst. [9,[15][16][17] In our studies of interlayer-expanded zeolites, heteroatoms such as Al or Ti were inserted into the layered precursor, after which the silylation reaction was performed to obtain the pore-expanded materials, which exhibit superior catalytic performances in olefin-selective oxidation or alkane isomerization reactions. [18][19][20] However, to the best of our knowledge, few studies have been reported in which T-atoms, other than Si, are introduced onto the linker site.…”

Section: Introductionmentioning

confidence: 99%

Framework Stability and Brønsted Acidity of Isomorphously Substituted Interlayer‐Expanded Zeolite COE‐4: A Density Functional Theory Study

Zhou

Tian

et al. 2014

ChemPhysChem

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COE-4 zeolites possess a unique two-dimensional ten-ring pore structure with the Si(OH)2 hydroxyl groups attached to the linker position between the ferrierite-type layers, which has been demonstrated through the interlayer-expansion approach in our previous work (H. Gies et al. Chem. Mater. 2012, 24, 1536). Herein, density functional theory is used to study the framework stability and Brønsted acidity of the zeolite T-COE-4, in which the tetravalent Si is isomorphously substituted by a trivalent Fe, B, Ga, or Al heteroatom at the linker position. The influences of substitution energy and equilibrium geometry parameters on the stability of T-COE-4 are investigated in detail. The relative acid strength of the linker position is revealed by the proton affinity, charge analysis, and NH3 adsorption. It is found that the range of the ⟨T-O-Si⟩ angles is widened to maintain the stability of isomorphously substituted T-COE-4 zeolites. The smaller the ⟨O1-T-O2⟩ bond angle is, the more difficult is to form the regular tetrahedral unit. Thus, the substitution energies at the linker positions increase in the following sequence: Al-COE-4 < Ga-COE-4 < Fe-COE-4 < B-COE-4. The adsorption of NH3 as a probe molecule indicates that the acidity can affect the hydrogen-bonding interaction between (N-H⋅⋅⋅O2) and (N⋅⋅⋅H-O2). The relative Brønsted-acid strength of the interlayer-expanded T-COE-4 zeolite decreases in the order of Al-COE-4 > Ga-COE-4 > Fe-COE-4 > B-COE-4. These findings may be helpful for the structural design and functional modification of interlayer-expanded zeolites.

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Layered precursors for new zeolitic materials: Synthesis and characterization of B-RUB-39 and its condensation product B-RUB-41

Cited by 16 publications

References 21 publications

Local environments of boron heteroatoms in non-crystalline layered borosilicates

Local environments of boron heteroatoms in non-crystalline layered borosilicates

A Straightforward Method for Determination of Al and Na in Aluminosilicates Using ICP OES

Framework Stability and Brønsted Acidity of Isomorphously Substituted Interlayer‐Expanded Zeolite COE‐4: A Density Functional Theory Study

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