Single-step synthesis and interface tuning of core-shell metal-organic framework nanoparticles

Kieran Orr; Sean  Collins; Emily Reynolds; Frank Nightingale; Hanna Bostroem; Simon Cassidy; Daniel Dawson; Sharon Ashbrook; Oxana Magdysyuk; Paul Midgley; Andrew Goodwin; Hamish Yeung

doi:10.1039/D0SC03940C

Single-step synthesis and interface tuning of core-shell metal-organic framework nanoparticles

Kieran Orr, Sean Collins, Emily Reynolds, Frank Nightingale, Hanna Bostroem, Simon Cassidy, Daniel Dawson, Sharon Ashbrook, Oxana Magdysyuk, Paul Midgley, Andrew Goodwin, Hamish Yeung

Chemistry

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Abstract

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 based on the canonical ZIF-8 (Zn) system and its Cd analogue, 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.

Original language	English
Pages (from-to)	4494-4502
Number of pages	9
Journal	Chemical Science
Volume	12
Issue number	12
Early online date	9 Feb 2021
DOIs	https://doi.org/10.1039/D0SC03940C
Publication status	Published - 28 Mar 2021

Bibliographical note

Funding Information:
HHMY thanks the Samuel and Violette Glasstone Bequest for a fellowship, the John Fell Fund (OUP) for funding, and the University of Birmingham for startup funds. This project has received funding from the European Union Horizon 2020 research and innovation program under the Marie-Sklodowska-Curie grant agreement 641887 (DEFNET). SMC acknowledges support from the Henslow Research Fellowship at Girton College, Cambridge. PAM thanks the EPSRC for nancial support under grant number EP/R025517/1. ALG thanks ERC for funding (Grant. 788144). The research leading to this result has been supported by Diamond Light Source (Beamtimes EE20946 (I12), and EE18786 (I11) Block Allocation Grant); we thank Chiu Tang and Claire Murray for their invaluable assistance on I11. We thank Alex Robertson and Shengda Pu for initial investigations by electron microscopy, and Bill David and Chloe Coates for useful discussions.

ASJC Scopus subject areas

General Chemistry

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Cite this

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title = "Single-step synthesis and interface tuning of core-shell metal-organic framework nanoparticles",

abstract = "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 based on the canonical ZIF-8 (Zn) system and its Cd analogue, 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.",

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AU - Reynolds, Emily

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AU - Cassidy, Simon

AU - Dawson, Daniel

AU - Ashbrook, Sharon

AU - Magdysyuk, Oxana

AU - Midgley, Paul

AU - Goodwin, Andrew

AU - Yeung, Hamish

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Single-step synthesis and interface tuning of core-shell metal-organic framework nanoparticles

Abstract

Bibliographical note

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