Topotactic transformation of naturally occurring layer silicates into porous framework silicates
Final Report Abstract
The joint research project of Ruhr-University Bochum and Waseda University Tokyo aimed to investigate the topotactic transformation of naturally occurring layer silicates into porous framework silicates. The project has been sectioned into a series of five steps, each building on the findings of the previous step. The first step includes the structural characterization of naturally occurring hydrous layer silicates (HLS) magadiite and kenyaite. The structures of the sodium layer silicates were successfully solved after characterising the silicates by a combination of powder X-Ray and electron diffraction techniques, spectroscopic methods and model building. The aim of the second step was to investigate the condensation of natural magadiite to form a structurally ordered silica zeolite of high density (RWZ-1) by exchanging the sodium for hydrogen , refluxing in N-methylformamide (NMF) and finally heating the material. During the third step, two crystalline silicic acids (CSAs), Hydrated H-Apophyllite and H-Carletonite, have been obtained from natural layer silicates (apophyllite and carletonite) by acid leaching. The CSAs which were characterised in detail were sufficiently ordered to analyze their structures. The crystal structure of silhydrite, the only natural silicic acid, remains – while showing similarities to magadiite – unsolved due to the severe structural disorder. Leaching experiments on the mineral gillespite acting as a precursor material were conducted to obtain another silicic acid, but led to a highly disordered H-gillespite material. The fourth step entails attempts to apply the condensation technique of the 3rd step to other silicates, such as H-carletonite and kenyaite. In a fifth step, emphasis is laid on the synthesis of an Interlayer Expanded Zeolite (IEZ) in a single-step-synthesis (RUB-5 and RUB-11), in contrast to the multi-step synthesis of the well established interlayer expansion and subsequent pillaring and condensation. In a profitable side step, SiO2 polymorphs keatite, RUB-11 and silica-sodalite have been investigated in order to determine the thermal expansion with special attention to a material with possibly zero volumetric thermal expansion.
Publications
-
Topotactic conversion of layered silicate magadiite into a novel crystalline silica through interlayer condensation using stepwise heat treatment. Contribution for Pacifichem Conference, Hawaii, USA. (Collection of Abstracts)
M. Koike, Y. Asakura, H. Wada, A. Shimojima, I. Grosskreuz, B. Marler & K. Kuroda
-
The crystal structure of synthetic kenyaite, Na2Si20O40(OH)2·8H2O. Journal of Solid State Chemistry, 300, 122215.
Marler, Bernd; Grosskreuz, Isabel & Gies, Hermann
-
Magadiitetype layers as building blocks for layered and microporous silicates, Contribution for 20th International Zeolite Conference, Valencia, Spain, July
I. Grosskreuz, M. Koike, Y. Krysiak, A. Shimojima, K. Kuroda & B. Marler
-
Magadiitetype layers as building blocks for layered and microporous silicates, Contribution for 8th International Workshop on Layered & Nanostructured Materials, Toledo, Spain 10-13th July. (Collection of Abstracts)
I. Grosskreuz, M. Koike, B. Marler, Y. Krysiak, A. Shimojima & K. Kuroda
-
The crystal structure of mineral magadiite, Na2Si14O28(OH)2∙8H2O. American Mineralogist, 107(11), 2101-2110.
Marler, Bernd; Krysiak, Yaşar; Grosskreuz, Isabel; Gies, Hermann & Kolb, Ute
-
Analysis of disordered magadiite-related layered and microporous silicates. Contribution for 26th Congress of the IUCr
I. Grosskreuz, M. Koike, B. Marler, Y. Krysiak, A. Shimojima & K. Kuroda
-
Bridging the Gap between Zeolites and Dense Silica Polymorphs: Formation of All‐Silica Zeolite with High Framework Density from Natural Layered Silicate Magadiite. Chemistry – A European Journal, 29(61).
Koike, Masakazu; Grosskreuz, Isabel; Asakura, Yusuke; Miyawaki, Ritsuro; Gies, Hermann; Wada, Hiroaki; Shimojima, Atsushi; Marler, Bernd & Kuroda, Kazuyuki
-
Real structure of mineral kenyaite, Na2Si20O40(OH)2 • 8 H2O. Contribution for MinWien2023, a joint meeting of the Mineralogical Societies of Austria, Germany, and Slovakia
I. Grosskreuz & B. Marler
-
Rietveld structure analysis of keatite, a rare, metastable SiO2 polymorph. Zeitschrift für Kristallographie - New Crystal Structures, 238(4), 655-657.
Grosskreuz, Isabel & Marler, Bernd
-
The structure of RUB-1, (C8H16N)6[B6Si48O108], a boron containing levyne-type zeolite, occluding N-methyl-quinuclidinium in the cage-like pores. Zeitschrift für Kristallographie - New Crystal Structures, 238(5), 923-925.
Gruenewald-Lueke, Antje; Grosskreuz, Isabel; Gies, Hermann & Marler, Bernd
-
Thermal expansion of SiO2 polymorphs keatite, RUB-11 and silica-sodalite. Contribution for MinWien2023, a joint meeting of the Mineralogical Societies of Austria, Germany, and Slovakia, Wien, Austria
B. Marler & I. Grosskreuz
-
Synthesis and Crystal Structures of Two Crystalline Silicic Acids: Hydrated H-Apophyllite, H16Si16O40 • 8–10 H2O and H-Carletonite, H32Si64O144. Crystals, 14(4), 326.
Marler, Bernd & Grosskreuz, Isabel
-
Synthesis and real structure of RUB-11, a novel high-density silica zeolite based on magadiite layers. New Journal of Chemistry, 48(9), 4030-4042.
Grosskreuz, Isabel; Krysiak, Yaşar; Gies, Hermann; Mugnaioli, Enrico & Marler, Bernd
