Abstract
Self-assembly of chromophores nanoconfined in porous materials such as zeolite L has led to technologically relevant host-guest systems exploited in solar energy harvesting, photonics, nanodiagnostics and information technology. The response of these hybrid materials to compression, which would be crucial to enhance their application range, has never been explored to date. By a joint high-pressure in situ synchrotron X-ray powder diffraction and ab initio molecular dynamics approach, herein we unravel the high-pressure behaviour of hybrid composites of zeolite L with fluorenone dye. High-pressure experiments were performed up to 6 GPa using non-penetrating pressure transmitting media to study the effect of dye loading on the structural properties of the materials under compression. Computational modelling provided molecular-level insight on the response to compression of the confined dye assemblies, evidencing a pressure-induced strengthening of the interaction between the fluorenone carbonyl group and zeolite L potassium cations. Our results reveal an impressive stability of the fluorenone-zeolite L composites at GPa pressures. The remarkable resilience of the supramolecular organization of dye molecules hyperconfined in zeolite L channels may open the way to the realization of optical devices able to maintain their functionality under extreme conditions.
Highlights
The main motivation of our study was to elucidate the behaviour of luminescent hybrid materials, obtained via the inclusion of the fluorenone dye in zeolite L microcrystals, under compression
If we consider that the technological applications of these composites rely on the presence of confined regular arrays of photoactive species, it is important to understand how this supramolecular organization of dye molecules responds to non-ambient conditions, an applied pressure
This study highlights the stability upon compression of the zeolite L/fluorenone adducts
Summary
Zeolites are crystalline natural or synthetic porous materials consisting of corner-sharing tetrahedral units, characterized by a regular arrangement of cages and channels of molecular size [1,2].The nanometric-scale geometry of zeolite pore systems allows the intensive use of zeolites in several fields such as in molecular separation processes and in heterogeneous catalysis [3,4].Crystals 2018, 8, 79; doi:10.3390/cryst8020079 www.mdpi.com/journal/crystalsCrystals 2018, 8, x FOR PEER REVIEWThe nanometric-scale geometry of zeolite pore systems allows the intensive use of zeolites in severalBesides being instrumental in traditional applications, the ordered arrangements of zeolitic cages fields such as in molecular separation processes and in heterogeneous catalysis [3,4].has long been recognized as a route to create advanced materials based on confined, organizedBesides being instrumental in traditional applications, the ordered arrangements of zeolitic nanostructures, such as luminescent metal clusters [5,6,7,8], quantum dots/wires [9] or lanthanides [10].cages has long been recognized as a route to create advanced materials based on confined, organizedTurning to more complex guests, the incorporation of fluorescent molecules in zeolite cages generally nanostructures, such as luminescent metal clusters [5,6,7,8], quantum dots/wires [9] or lanthanides [10].enhances emission [11,12,13] because it allowsmolecules to obtainin high. The nanometric-scale geometry of zeolite pore systems allows the intensive use of zeolites in several fields such as in molecular separation processes and in heterogeneous catalysis [3,4]. Besides being instrumental in traditional applications, the ordered arrangements of zeolitic cages fields such as in molecular separation processes and in heterogeneous catalysis [3,4]. Has long been recognized as a route to create advanced materials based on confined, organized. Besides being instrumental in traditional applications, the ordered arrangements of zeolitic nanostructures, such as luminescent metal clusters [5,6,7,8], quantum dots/wires [9] or lanthanides [10]. Cages has long been recognized as a route to create advanced materials based on confined, organized.
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