Functionalised metal-organic frameworks: A novel approach to stabilising single metal atoms

P. Szilágyi; D. M. Rogers; I. Zaiser; E Callini; Stuart Turner; A Borgschulte; A. Züttel; H. Geerlings; M Hirscher; B. Dam

doi:10.1039/c7ta03134c

Functionalised metal-organic frameworks: A novel approach to stabilising single metal atoms

P. Szilágyi^*, D. M. Rogers, I. Zaiser, E Callini, Stuart Turner, A Borgschulte, A. Züttel, H. Geerlings, M Hirscher, B. Dam

^*Corresponding author for this work

ChemE/Materials for Energy Conversion and Storage

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Abstract

We have investigated the potential of metal-organic frameworks for immobilising single atoms of transition metals using a model system of Pd supported on NH₂-MIL-101(Cr). Our transmission electron microscopy and in situ Raman spectroscopy results give evidence for the first time that functionalised metal-organic frameworks may support, isolate and stabilise single atoms of palladium. Using thermal desorption spectroscopy we were able to evaluate the proportion of single Pd atoms. Furthermore, in a combined theoretical-experimental approach, we show that the H-H bonds in a H₂ molecule elongate by over 15% through the formation of a complex with single atoms of Pd. Such deformation would affect any hydrogenation reaction and thus the single atoms supported on metal-organic frameworks may become promising single atom catalysts in future.

Original language	English
Pages (from-to)	15559-15566
Number of pages	8
Journal	Journal of Materials Chemistry A
Volume	5
Issue number	30
DOIs	https://doi.org/10.1039/c7ta03134c
Publication status	Published - 2017

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abstract = "We have investigated the potential of metal-organic frameworks for immobilising single atoms of transition metals using a model system of Pd supported on NH2-MIL-101(Cr). Our transmission electron microscopy and in situ Raman spectroscopy results give evidence for the first time that functionalised metal-organic frameworks may support, isolate and stabilise single atoms of palladium. Using thermal desorption spectroscopy we were able to evaluate the proportion of single Pd atoms. Furthermore, in a combined theoretical-experimental approach, we show that the H-H bonds in a H2 molecule elongate by over 15% through the formation of a complex with single atoms of Pd. Such deformation would affect any hydrogenation reaction and thus the single atoms supported on metal-organic frameworks may become promising single atom catalysts in future.",

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AU - Szilágyi, P.

AU - Rogers, D. M.

AU - Zaiser, I.

AU - Callini, E

AU - Turner, Stuart

AU - Borgschulte, A

AU - Züttel, A.

AU - Geerlings, H.

AU - Hirscher, M

AU - Dam, B.

PY - 2017

Y1 - 2017

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AB - We have investigated the potential of metal-organic frameworks for immobilising single atoms of transition metals using a model system of Pd supported on NH2-MIL-101(Cr). Our transmission electron microscopy and in situ Raman spectroscopy results give evidence for the first time that functionalised metal-organic frameworks may support, isolate and stabilise single atoms of palladium. Using thermal desorption spectroscopy we were able to evaluate the proportion of single Pd atoms. Furthermore, in a combined theoretical-experimental approach, we show that the H-H bonds in a H2 molecule elongate by over 15% through the formation of a complex with single atoms of Pd. Such deformation would affect any hydrogenation reaction and thus the single atoms supported on metal-organic frameworks may become promising single atom catalysts in future.

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Functionalised metal-organic frameworks: A novel approach to stabilising single metal atoms

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