Hybrid organic/inorganic nanomaterials: Development of malonamide-functionalized nanoparticles designed for lanthanide ion detection
Datum
2010-03
Autor:innen
Zeitschriftentitel
ISSN der Zeitschrift
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Verlag
University of Oregon
Zusammenfassung
Hybrid nanoscale complexes incorporate the attributes of organic and inorganic components to yield novel multifunctional materials. Because the individual components themselves and the combinations used can be widely varied to tune the properties of the resulting complex, the potential for new properties and practical applications is nearly limitless. However, widespread use of these materials relies on appropriate design, synthesis and characterization strategies to ensure proper function and compositional integrity. This dissertation describes the chemistry of these hybrids, made possible by combining organic ligands, inorganic nanoparticles, and metal ions, and the interesting optical and spectroscopic properties associated with the hybrid nanomaterials.
Organic ligands containing Bunte salt and acyclic malonamide functionalities were attached to gold nanoparticles to produce colorimetric sensors for lanthanide ion detection. Bunte salt functionality stabilizes the gold core and malonamide functionality offers selective and sensitive lanthanide ion binding. The binding interaction controls a nanoparticle cross-linking event that changes the color of the nanoparticle solution, resulting in visual, colorimetric lanthanide ion detection. Next, the concentration of malonamide ligand was diluted and replaced with a diluent ligand yielding nanoparticles stabilized with a mixed ligand composition. The mixed ligand environment makes the optical response of the colorimetric sensor reversible. Furthermore, the use of Bunte salt ligands during nanoparticle synthesis has allowed the investigation of the role of reducing agent on nanoparticle stability.
In addition to exploring interactions pertaining to gold nanoparticle complexes, a new approach to sensitize europium ion luminescence was developed by fabricating a zinc oxide/europium complex. A molecular linker permits simultaneous zinc oxide nanoparticle functionalization and trivalent europium binding in order to tether the europium ion close to the nanoparticle surface. The zinc oxide nanoparticle can then act as an inorganic antenna, transferring energy to the europium ion and enhancing its luminescence.
Finally, a strategy was developed to synthesize bifunctional bicyclic malonamides. Synthesis of these ligands allows the enhanced f-block ion binding affinity of bicyclic malonamides to be incorporated into functional materials to compare their performance to our previously prepared acyclic malonamide hybrid complexes.
This dissertation includes my previously published and co-authored materials.
Beschreibung
xviii, 174 p. : ill. (some col.) A print copy of this thesis is available through the UO Libraries. Search the library catalog for the location and call number.
Schlagwörter
Lanthanide, Ion detection, Malonamide, Inorganic chemistry