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submitted on 18.07.2020 and posted on 21.07.2020by 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.