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Single-Step Synthesis and Interface Tuning of Core–shell Metal–organic Framework Nanoparticles

preprint
submitted on 18.07.2020 and posted on 21.07.2020 by Kieran Orr, Sean M. Collins, Emily Reynolds, Frank Nightingale, Hanna Boström, Simon J. Cassidy, Daniel M. Dawson, Sharon Ashbrook, Oxana Magdysyuk, Paul A. Midgley, Andrew Goodwin, Hamish Yeung
Control over the spatial distribution of components in metal–organic frameworks has potential to unlock improved performance and new behaviour in separations, sensing and catalysis. We report an unprecedented single-step synthesis of multi-component metal–organic framework (MOF) nanoparticles, which form with a core–shell structure whose internal interface can be systematically tuned. We use scanning transmission electron microscopy, X-ray energy dispersive spectroscopy and a new composition gradient model to fit high-resolution X-ray diffraction data to show how core–shell composition and interface characteristics are intricately controlled by synthesis temperature and reaction composition. Particle formation is investigated by in situ X-ray diffraction, which reveals that the spatial distribution of components evolves with time and is determined by the interplay of phase stability, crystallisation kinetics and diffusion. This work opens up new possibilities for the control and characterisation of functionality, component distribution and interfaces in MOF-based materials.

Funding

DEFect NETwork materials science and engineering

European Commission

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EP/R025517/1

The Complexity Revolution: Exploiting Unconventional Order in Next-Generation Materials Design

European Research Council

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History

Email Address of Submitting Author

h.yeung@bham.ac.uk

Institution

University of Birmingham

Country

UK

ORCID For Submitting Author

0000-0003-1629-6275

Declaration of Conflict of Interest

No conflict of interest

Version Notes

V1-submission

Exports