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Expanding applications of iron oxide nanoparticles by surface functionalization: From magnetic resonance imaging to nano-catalysis

Posted on:2010-10-27Degree:Ph.DType:Dissertation
University:Southern Illinois University at CarbondaleCandidate:Duanmu, ChuansongFull Text:PDF
GTID:1444390002990200Subject:Organic Chemistry
Abstract/Summary:
In this dissertation, research efforts mainly focused on exploring the applications of superparamagnetic iron oxide nanoparticles (SPIONs) in MR imaging and nanocatalysis via surface functionalization. A dopamine-based surface-functionalization strategy was established. The Simanek dendrons (G1 to G3), oligonucleotides and amino acids were loaded onto SPION surfaces via this approach to develop pH-sensitive MRI contrast agents, specific-DNA MR probes and a biomimetic hydrolysis catalyst.;Dendron-SPION conjugates (G1 to G3) have good aqueous solubilities and high transverse relaxivities (>300 s-1·mM-1). They also showed interesting strong pH-sensitive R2 and R2* relaxivities, which were governed by the clustering states of dendron-SPIONs in different pH environments. Values of R2m and R2*m /R2m varied by over an order of magnitude around pH 5. The efficient cell-uptake (∼3 million/cell) and low cytotoxicity of G1 to G3-SPIONs were demonstrated on HeLa cell cultures. The strong R2* effects were observed indicating the SPION clustering in HeLa cells.;Two SPION-oligonuleotide conjugates were synthesized by coupling two half-match oligonucleotides onto domapine-capped SPIONs via SPDP linkers. They served as MR probes to detect a single-strand DNA with the same sequence to miRNA-21 based on the change of R2 values due to the DNA-bridged SPION clustering. The detection limit of the DNA could reach to 16.5 nM.;A biomimetic hydrolysis nanocatalyst (i.e., Fe2O3-Asp-His complex) was developed by loading Asp and His-dopamine derivatives onto SPIONs. Paraoxon and nitrophenyl acetate were hydrolyzed under a mild condition (neutral pH, 37 °C) catalyzed by the Fe2O3-Asp-His complex. The two amino acids Asp and His cooperated with each other on the SPION surfaces to catalyze hydrolysis reactions. This catalyst could be recycled by a magnet and reused for four times without a significant loss of catalytic activity.
Keywords/Search Tags:SPION
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