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

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Castillo-Blas, Celia 


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.


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.


3402 Inorganic Chemistry, 40 Engineering, 34 Chemical Sciences

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Soft Matter

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