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Luminescence in metal-organic frameworks: mechanisms and applications as phosphors and sensors
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Lustig, William P.. Luminescence in metal-organic frameworks: mechanisms and applications as phosphors and sensors. Retrieved from https://doi.org/doi:10.7282/t3-mazg-4579

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TitleLuminescence in metal-organic frameworks: mechanisms and applications as phosphors and sensors
NameLustig, William P. (author); Li, Jing (chair); O'Carroll, Deirdre (internal member); Warmuth, Ralf (internal member); Hu, Zhichao (outside member); Rutgers University; School of Graduate Studies
Date Created2019
Other Date2019-10 (degree)
SubjectChemistry and Chemical Biology, Metal-organic framework, Organometallic compounds, Electroluminescence
Extent1 online resource (xv, 89 pages) : illustrations
DescriptionLuminescent metal‐organic frameworks (LMOFs) are a class of supramolecular material composed of metal ions connected by organic ligands to form crystalline frameworks that emit light when excited. In these organic‐inorganic frameworks, single metal ions or metal ion clusters serve as ‘nodes’, with rigid multidentate ligand molecules linking these nodes into an ordered three‐dimensional lattice. Luminescence can arise from the metal nodes, organic ligands, or interactions between these components. Because the properties of an LMOF depend on both the characteristics of the building blocks used to construct it and how these building blocks interact with each other, altering these building blocks can impart an incredible degree of tunability to an LMOF’s properties. However, the complex interactions that are possible between framework components render the rational design of LMOFs with specific luminescent properties challenging.

This work used a combination of spectroscopic, crystallographic, and theoretical methods to understand the chemical and optoelectronic processes that take place within LMOFs. This understanding was then used to develop broadly‐applicable strategies for the rational design of LMOFs for commercial applications, which were in turn used to design and synthesize several new LMOFs with record‐breaking performance as optical sensors and phosphor materials. LMOF‐241 was designed for the detection of common food‐contaminating mycotoxins using a photoinduced electron transfer mechanism. It was used to optically detect mycotoxins with unprecedented speed and sensitivity, with detection limits on the ppb‐scale. A chromophoric‐ligand strategy was previously used to design LMOF‐231 for use as a blue‐excitable, yellow‐emitting phosphor material in white LED bulbs, and it demonstrated the highest quantum yield for any yellow‐emitting LMOF reported (76%). This exceptional quantum yield was improved to 88% in LMOF‐231‐F0.2, which was designed using a bandgap–modulation strategy. Finally, the effect of post‐synthetic structural rigidification on LMOF quantum yield was studied using the isostructural LMOFs‐263 and 301. This work demonstrated that rigidification via structural packing is an effective strategy for increasing luminescence efficiency, with LMOF‐263 demonstrating a nearly five‐fold increase in quantum yield.
NotePh.D.
NoteIncludes bibliographical references
Genretheses, ETD doctoral
Persistent URLhttps://doi.org/doi:10.7282/t3-mazg-4579
LanguageEnglish
CollectionSchool of Graduate Studies Electronic Theses and Dissertations
Organization NameRutgers, The State University of New Jersey
RightsThe author owns the copyright to this work.
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