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• W88786888 abstract "The separation and concentration of metal ions under dynamic flow conditions is of interest from both pure and applied research perspectives. By fabricating functional thin films on electrode surfaces, metal ion recognition interfaces may be tailored to uptake specific ions from solution and chemical events at interfaces may be followed in-situ. Investigations designed to produce tailored surfaces for the selective uptake of metal ions in solution were conducted. As signal amplification is an important aspect in sensing metal ions, the use of dendrimers as functional materials was explored as their many terminal groups can act as receptors or attachment sites for further receptors. Specifically, the immobilisation of poly(amidoamine) (PAMAM) and poly(propylene imine) (PPI) dendrimers onto carboxylic acid-terminated self-assembled monolayers (SAMs) on gold were imdertaken. Research was directed at finding an appropriate methodology for covalently linking the terminal amine (NH2) functional groups of the dendrimers onto the acid functional groups in the SAMs. Two strategies, involving fluorinated molecules, to produce chemical species that were reactive towards the amine groups were followed. The fluorine atom provided spectroscopic tag for monitoring the surface reactions. PM-FTIR and XPS were employed to study the self-assembled films. Initially an acid fluoride SAM analogue of 11-mercaptoundecanoic acid (MUA) monolayer was utilized, but it was found that the monolayer was not stable. This procedure was deemed unsuitable. Attention was then diverted to performing an in-situ coupling reaction using pentafluorophenol and a carbodiimide reagent to generate the pentafluorophenyl ester. The ester intermediate was characterised by the appearance of a fluorine signal in the XPS spectrum of the film. The same reaction was also performed on -OH and -CH3 terminated SAMs which were devoid of -COOH functionality, and no fluorine signal was apparent. By comparing the components in carbon spectral envelope, it was deduced that only 30 % of-COOH groups were activated by this method due to the steric hindrance foimd in single component monolayers. The ester intermediate was then exposed to a dilute solution of PAMAM dendrimer (generation 4) and the deposition was indicated by the appearance of a nitrogen signal and concomitant disappearance of the fluorine signal. As well as single component SAMs, mixed SAMs prepared from -OH and -COOH terminated thiols or -CH3 and -COOH terminated thiols were also explored as anchors for immobilisation of the dendrimers. From XPS data, it was seen that the ester intermediate could be generated on the surface of these mixed films as a result of the presence of the - COOH groups. It was found that dendrimers could be immobilised onto these mixed monolayers. Non-specific adsorption of the dendrimers also occurs as evidenced by the appearance of amide I and n bands in the surface infrared spectra of dendrimers adsorbed on octadecyl disulfide SAMs. The interactions between the receptor and metal analyte is important for the development of metal ion sensing surfaces. EXAFS was employed as a technique to probe complexes formed by dendrimers with metal ions. The binding modes of Cu(n) in PAMAM and PPI dendrimers were elucidated using EXAFS with supporting evidence from NMR spectroscopy. NMR data also provides evidence for the binding of metal ions to the internal receptor sites in the dendrimer. TEM experiments established the existence of Cu(n)-PAMAM clusters. The structure of Hg-PPI complexes was also determined using EXAFS. These are the first structures to be elucidated for copper-PAMAM dendrimer and mercury dendrimer complexes. Preliminary studies were conducted to test the ability of the self-assembled dendrimer films for the uptake of metal ions from solution. The response of the immobilised dendritic films to Hg(n) and Cu(II) ions under dynamic flow conditions was investigated using the quartz crystal microbalance (QCM) technique. It was foimd that the dendrimer functionalised QCM system was not sensitive enough to register a significant response. Modifying the bare gold electrode on the QCM with roughened electrodeposited gold, induced a greater frequency response for Hg(n) ion uptake." @default.
• W88786888 created "2016-06-24" @default.
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• W88786888 date "2003-01-01" @default.
• W88786888 modified "2023-09-26" @default.
• W88786888 title "Dendritic receptors on self-assembled surfaces for metal ion uptake" @default.
• W88786888 hasPublicationYear "2003" @default.
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