Single-step synthesis and interface tuning of core-shell metal-organic framework nanoparticles
Research output: Contribution to journal › Article › peer-review
Colleges, School and Institutes
- University of Cambridge
- University of Leeds
- University of Oxford
- Max Planck Institute for Solid-State Research
- University of St Andrews
- Diamond Light Source
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.
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.
|Number of pages||9|
|Early online date||9 Feb 2021|
|Publication status||Published - 28 Mar 2021|