dc.contributor.author	Anderson, Samantha L.
dc.contributor.author	Tiana, Davide
dc.contributor.author	Ireland, Christopher P.
dc.contributor.author	Capano, Gloria
dc.contributor.author	Fumanal, Maria
dc.contributor.author	Gladysiak, Andrzej
dc.contributor.author	Kampouri, Stavroula
dc.contributor.author	Rahmanudin, Aiman
dc.contributor.author	Guijarro, Néstor
dc.contributor.author	Sivula, Kevin
dc.contributor.author	Stylianou, Kyriakos C.
dc.contributor.author	Smit, Berend
dc.contributor.funder	Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung	en
dc.contributor.funder	Horizon 2020	en
dc.contributor.funder	Swiss National Supercomputing Centre	en
dc.date.accessioned	2021-09-17T12:06:41Z
dc.date.available	2021-09-17T12:06:41Z
dc.date.issued	2020-03-20
dc.date.updated	2021-09-16T08:42:14Z
dc.description.abstract	Metal organic frameworks (MOFs) are increasingly used in applications that rely on the optical and electronic properties of these materials. These applications require a fundamental understanding on how the structure of these materials, and in particular the electronic interactions of the metal node and organic linker, determines these properties. Herein, we report a combined experimental and computational study on two families of lanthanide-based MOFs: Ln-SION-1 and Ln-SION-2. Both comprise the same metal and ligand but with differing structural topologies. In the Ln-SION-2 series the optical absorption is dominated by the ligand and using different lanthanides has no impact on the absorption spectrum. The Ln-SION-1 series shows a completely different behavior in which the ligand and the metal node do interact electronically. By changing the lanthanide in Ln-SION-1, we were able to tune the optical absorption from the UV region to absorption that includes a large part of the visible region. For the early lanthanides we observe intraligand (electronic) transitions in the UV region, while for the late lanthanides a new band appears in the visible. DFT calculations showed that the new band in the visible originates in the spatial orbital overlap between the ligand and metal node. Our quantum calculations indicated that Ln-SION-1 with late lanthanides might be (photo)conductive. Experimentally, we confirm that these materials are weakly conductive and that with an appropriate co-catalysts they can generate hydrogen from a water solution using visible light. Our experimental and theoretical analysis provides fundamental insights for the rational design of Ln-MOFs with the desired optical and electronic properties.	en
dc.description.sponsorship	Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung (Ambizione Energy Grant n.PZENP2_166888; National Center of Competence in Research (NCCR), Materials' Revolution: Computational Design and Discovery of Novel Materials (MARVEL) DD4.5; Grant n.IZKSZ2_162130; Project Funding 200021_172759 ); Swiss National Supercomputing Centre (Project no. s611)	en
dc.description.status	Peer reviewed	en
dc.description.version	Published Version	en
dc.format.mimetype	application/pdf	en
dc.identifier.citation	Anderson, S. L., Tiana. D., Ireland, C. P., Capano, G., Fumanal, M., Gladysiak, A., Kampouri, S., Rahmanudin, A., Guijarro, N., Sivula, K., Stylianou, K. C. and Smit, B. (2020) 'Taking lanthanides out of isolation: tuning the optical properties of metal-organic frameworks', Chemical Science, 11(16), pp. 4164-4170. doi: 10.1039/d0sc00740d	en
dc.identifier.doi	10.1039/d0sc00740d	en
dc.identifier.eissn	2041-6539
dc.identifier.endpage	4170	en
dc.identifier.issn	2041-6520
dc.identifier.issued	16	en
dc.identifier.journaltitle	Chemical Science	en
dc.identifier.startpage	4164	en
dc.identifier.uri	https://hdl.handle.net/10468/11948
dc.identifier.volume	11	en
dc.language.iso	en	en
dc.publisher	Royal Society of Chemistry	en
dc.relation.project	info:eu-repo/grantAgreement/EC/H2020::MSCA-IF-EF-ST/705861/EU/Accelerated Synthesis of Nanoporous Photocatalysts for Indoor Air Purification/ASPAir	en
dc.rights	© 2020, the Authors. Open Access. This material is licensed under a Creative Commons Attribution-NonCommercial 3.0 Unported (CC BY-NC 3.0) licence.	en
dc.rights.uri	https://creativecommons.org/licenses/by-nc/3.0/	en
dc.subject	Ln-MOF	en
dc.subject	Hydrogen	en
dc.subject	Metal organic frameworks	en
dc.subject	Optical	en
dc.subject	Electronic	en
dc.subject	Lanthanide	en
dc.title	Taking lanthanides out of isolation: tuning the optical properties of metal-organic frameworks	en
dc.type	Article (peer-reviewed)	en

Taking lanthanides out of isolation: tuning the optical properties of metal-organic frameworks

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