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Transient intermediate in the formation of an amorphous metal-organic framework.

Published version
Peer-reviewed

Repository DOI


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Authors

Castillo-Blas, Celia 

Abstract

Amorphous metal-organic frameworks are rarely formed via direct synthesis. Our limited understanding of their atomic assembly in solution prevents full exploitation of their unique structural complexity. Here, we use in situ synchrotron X-ray absorption spectroscopy with sub-second time resolution to probe the formation of the amorphous Fe-BTC framework. Using a combination of spectral fingerprinting, linear combination analysis, and principal component analysis coupled with kinetic analyses, we reveal a multi-stage formation mechanism that, crucially, proceeds via the generation of a transient intermediate species.

Description

Acknowledgements: AFS acknowledges the EPSRC for a PhD studentship award under the industrial CASE scheme, along with Johnson Matthew PLC (JM11106). MFT acknowledges Corning Incorporated for a PhD studentship. TDB thanks the Royal Society for both a University Research Fellowship (URF\R\211013) and a research grant (RGS\R2\212221). TDB and CCB acknowledge funding from a Leverhulme Trust Research Project Grant (RPG-2020-005). We would thank Diamond Light Source for the provision of beam time at the I20-EDE beamline (Experiment Number SP28536-1). AFS would also like to thank Dr Hamish Yeung (University of Birmingham) for useful discussions regarding nucleation and MOF formation.

Keywords

3402 Inorganic Chemistry, 40 Engineering, 34 Chemical Sciences

Journal Title

Soft Matter

Conference Name

Journal ISSN

1744-683X
1744-6848

Volume Title

Publisher

Royal Society of Chemistry (RSC)
Sponsorship
Royal Society (RGS\R2\212221, URF\R\211013)
Leverhulme Trust (RPG-2020-005)
Engineering and Physical Sciences Research Council (JM11106)