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Core-shell zeolite@aqueous miscible organic-layered double hydroxides.

ABSTRACT: We report a general method for the synthesis of core-shell hybrid materials containing a microporous zeolite core with an aqueous miscible organic-layered double hydroxide (AMO-LDH) shell using a simple in situ coprecipitation method. For example, zeolite-HY@AMO-Mg₂Al-CO₃-LDH contains a 150 nm hierarchical AMO-Mg₂Al-CO₃-LDH surface coating on zeolite-HY. It exhibits a similar BET surface area (698 m² g^-1) as the parent zeolite-HY but this surface area has been re-allocated between microspores and mesopores. We believe that surface aluminium sites act as nucleation sites for the formation of the LDH coating and so robustly links it into the zeolite lattice. We expect that this new hybrid structure with micropores dominating in the core and mesopores populating the shell will provide a desirable new hybrid structure type for adsorption or catalysis.

SUBMITTER: Chen C

PROVIDER: S-EPMC5975924 | biostudies-literature | 2016 Feb

REPOSITORIES: biostudies-literature

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Core-shell zeolite@aqueous miscible organic-layered double hydroxides.

Chen Chunping C Byles Coral F H CFH Buffet Jean-Charles JC Rees Nicholas H NH Wu Yue Y O'Hare Dermot D

Chemical science 20151113 2

We report a general method for the synthesis of core-shell hybrid materials containing a microporous zeolite core with an aqueous miscible organic-layered double hydroxide (AMO-LDH) shell using a simple in situ coprecipitation method. For example, zeolite-HY@AMO-Mg2Al-CO3-LDH contains a 150 nm hierarchical AMO-Mg2Al-CO3-LDH surface coating on zeolite-HY. It exhibits a similar BET surface area (698 m2 g-1) as the parent zeol ...[more]

PMID: 29910903

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Project description:Research on two-dimensional materials is one of the most relevant fields in materials science. Layered double hydroxides (LDHs), a versatile class of anionic clays, exhibit great potential in photocatalysis, energy storage and conversion, and environmental applications. However, its implementation in real-life devices requires the development of efficient and reproducible large-scale synthesis processes. Unfortunately, reliable methods that allow for the production of large quantities of two-dimensional LDHs with well-defined morphologies and high crystallinity are very scarce. In this work, we carry out a scale-up of the urea-based CoAl-LDH synthesis method. We thoroughly study the effects of the mass scale-up (25-fold: up to 375 mM) and the volumetric scale-up (20-fold: up to 2 L). For this, we use a combination of several structural (XRD, TGA, and N2 and CO2 isotherms), microscopic (SEM, TEM, and AFM), magnetic (SQUID), and spectroscopic techniques (ATR-FTIR, UV-vis, XPS, ICP-MS, and XANES-EXAFS). In the case of the volumetric scale-up, a reduction of 45% in the lateral dimensions of the crystals (from 3.7 to 2.0 µm) is observed as the reaction volume increases. This fact is related to modified heating processes affecting the alkalinization rates and, concomitantly, the precipitation, even under recrystallization at high temperatures. In contrast, for the tenfold mass scale-up, similar morphological features were observed and assigned to changes in nucleation and growth. However, at higher concentrations, simonkolleite-like Co-based layered hydroxide impurities are formed, indicating a phase competition during the precipitation related to the thermodynamic stability of the growing phases. Overall, this work demonstrates that it is possible to upscale the synthesis of high-quality hexagonal CoAl-LDH in a reproducible manner. It highlights the most critical synthesis aspects that must be controlled and provides various fingerprints to trace the quality of these materials. These results will contribute to bringing the use of these 2D layered materials closer to reality in different applications of interest.

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Core-shell zeolite@aqueous miscible organic-layered double hydroxides.

Publications

Core-shell zeolite@aqueous miscible organic-layered double hydroxides.

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