Electronic origins of photocatalytic activity in d0 metal organic frameworks View Full Text


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Article Info

DATE

2016-03-29

AUTHORS

Maxim A. Nasalevich, Christopher H. Hendon, Jara G. Santaclara, Katrine Svane, Bart van der Linden, Sergey L. Veber, Matvey V. Fedin, Arjan J. Houtepen, Monique A. van der Veen, Freek Kapteijn, Aron Walsh, Jorge Gascon

ABSTRACT

Metal-organic frameworks (MOFs) containing d0 metals such as NH2-MIL-125(Ti), NH2-UiO-66(Zr) and NH2-UiO-66(Hf) are among the most studied MOFs for photocatalytic applications. Despite structural similarities, we demonstrate that the electronic properties of these MOFs are markedly different. As revealed by quantum chemistry, EPR measurements and transient absorption spectroscopy, the highest occupied and lowest unoccupied orbitals of NH2-MIL-125(Ti) promote a long lived ligand-to-metal charge transfer upon photoexcitation, making this material suitable for photocatalytic applications. In contrast, in case of UiO materials, the d-orbitals of Zr and Hf, are too low in binding energy and thus cannot overlap with the π* orbital of the ligand, making both frontier orbitals localized at the organic linker. This electronic reconfiguration results in short exciton lifetimes and diminishes photocatalytic performance. These results highlight the importance of orbital contributions at the band edges and delineate future directions in the development of photo-active hybrid solids. More... »

PAGES

23676

References to SciGraph publications

Identifiers

URI

http://scigraph.springernature.com/pub.10.1038/srep23676

DOI

http://dx.doi.org/10.1038/srep23676

DIMENSIONS

https://app.dimensions.ai/details/publication/pub.1013701502

PUBMED

https://www.ncbi.nlm.nih.gov/pubmed/27020767


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