4 results on '"Samantha L. Anderson"'
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2. Taking lanthanides out of isolation: tuning the optical properties of metal-organic frameworks
- Author
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Christopher P. Ireland, Kevin Sivula, Aiman Rahmanudin, Samantha L. Anderson, Andrzej Gładysiak, Maria Fumanal, Stavroula Kampouri, Gloria Capano, Davide Tiana, Kyriakos C. Stylianou, Néstor Guijarro, and Berend Smit
- Subjects
Lanthanide ,Materials science ,Absorption spectroscopy ,Metal organic frameworks ,02 engineering and technology ,Orbital overlap ,010402 general chemistry ,01 natural sciences ,catalysts ,Electronic ,Absorption (electromagnetic radiation) ,complexes ,Ligand ,Ln-MOF ,General Chemistry ,021001 nanoscience & nanotechnology ,0104 chemical sciences ,Chemistry ,Chemical physics ,Chemical Sciences ,Metal-organic framework ,Density functional theory ,0210 nano-technology ,Optical ,Hydrogen ,Visible spectrum - 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., Computational and experimental study into two families of lanthanide-based metal organic frameworks with the same ligand, tuned to have different structural and optical properties.
- Published
- 2020
3. Formation pathways of metal–organic frameworks proceeding through partial dissolution of the metastable phase
- Author
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Christopher P. Ireland, Bess Vlaisavljevich, Andrzej Gładysiak, Wouter van Beek, Kevin J. Gagnon, Pascal Miéville, Peter G. Boyd, Davide Tiana, Pascal Schouwink, Kyriakos C. Stylianou, Samantha L. Anderson, and Berend Smit
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Chemical transformation ,Chemistry ,Rational design ,Physics::Optics ,Nanotechnology ,02 engineering and technology ,General Chemistry ,010402 general chemistry ,021001 nanoscience & nanotechnology ,Condensed Matter Physics ,01 natural sciences ,0104 chemical sciences ,Solvent ,Chemical engineering ,Phase (matter) ,Metastability ,General Materials Science ,Metal-organic framework ,Chemical stability ,0210 nano-technology ,Dissolution - Abstract
Understanding how crystalline materials are assembled is important for the rational design of metal–organic frameworks (MOFs), through streamlining their synthesis and controlling their properties for targeted applications. Herein, we report for the first time the construction of two 3-dimensional Tb(III) based MOFs; a metastable MOF acting as an intermediate phase, that partially dissolves and transforms into a chemically and thermodynamically stable MOF. This chemical transformation occurs solely in a N,N-dimethylformamide/water solvent mixture, and is triggered when additional energy is provided to the reaction. In situ studies reveal the partial dissolution of the metastable phase after which the MOF components are reassembled into the thermodynamically stable phase. The marked difference in thermal and chemical stability between the kinetically and thermodynamically controlled phases is contrasted by their identical chemical building unit composition.
- Published
- 2017
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4. In silico design and screening of hypothetical MOF-74 analogs and their experimental synthesis
- Author
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Lianheng Tong, Berend Smit, Maciej Haranczyk, Ben Slater, Kyriakos C. Stylianou, Samantha L. Anderson, Sanliang Ling, and Matthew Witman
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Computer science ,In silico ,02 engineering and technology ,General Chemistry ,Experimental validation ,010402 general chemistry ,021001 nanoscience & nanotechnology ,Network topology ,01 natural sciences ,Combinatorial chemistry ,Chemical space ,0104 chemical sciences ,Chemical Sciences ,Density functional theory ,0210 nano-technology ,Biological system ,PubChem ,Topology (chemistry) - Abstract
© 2016 The Royal Society of Chemistry. In this work we present the in silico design of metal-organic frameworks (MOFs) exhibiting 1-dimensional rod topologies. We introduce an algorithm for construction of this family of MOF topologies, and illustrate its application for enumerating MOF-74-type analogs. Furthermore, we perform a broad search for new linkers that satisfy the topological requirements of MOF-74 and consider the largest database of known chemical space for organic compounds, the PubChem database. Our in silico crystal assembly, when combined with dispersion-corrected density functional theory (DFT) calculations, is demonstrated to generate a hypothetical library of open-metal site containing MOF-74 analogs in the 1-D rod topology from which we can simulate the adsorption behavior of CO2. We finally conclude that these hypothetical structures have synthesizable potential through computational identification and experimental validation of a novel MOF-74 analog, Mg2(olsalazine).
- Published
- 2016
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