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

Research output: Contribution to journalArticlepeer-review

Authors

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

Colleges, School and Institutes

External organisations

  • University of Cambridge
  • University of Leeds
  • University of Oxford
  • ISIS
  • Max Planck Institute for Solid-State Research
  • University of St Andrews
  • Diamond Light Source

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.

Bibliographic 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.

Details

Original languageEnglish
Pages (from-to)4494-4502
Number of pages9
JournalChemical Science
Volume12
Issue number12
Early online date9 Feb 2021
Publication statusPublished - 28 Mar 2021

ASJC Scopus subject areas