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M.Sc. (Chemistry) / Secondary cancer tumour formation, often called metastasis, remains one of the great scientific challenges in public health. Patients with skeletal metastases have a low survival rate, with great discomforts experienced by the sufferers. Pain, decreased mobility, pathologic bone fractures are some of the effects that these patients have to live with. Significant inroads have been made in using radio pharmaceuticals as a pain palliation treatment for bone metastases. They comprise of a bone seeking phosphonate ligand and a radionuclide. The structural variation of the phosphonate affects to a great extend the effectiveness of the radiopharmaceutical with the greatest shortfall being myelosuppression at high doses. In this study an attempt is made at synthesizing novel bisphosphonates, APDDAM and APDDPE. After several synthetic steps from the protected β-alanine tert butyl ester, the free acid precursor was achieved (as shown in the NMR and elemental analysis) in good yields. Unfortunately the final reaction step to form the bisphosphonate ligand was unsuccessful, with the free acid precursor dissociating in the acidic conditions to form salts. A polymer ligand poly-HEDP was synthesized from its free acid form in relatively low yields. The ligand was used in potentiometric studies with the metal ions Ca(II), Mg(II), Cu(II), Zn(II), Sn(II) and Sn(IV) to evaluate its potential as radiopharmaceutical candidate. The ESTA model formation constants obtained were used in the ECCLES blood plasma model to evaluate the competitive stability of the complexes against biological metal ions and ligands. The Sn(IV)-poly-HEDP complex was shown to be unstable, with a 100 % dissociation. On the other hand the Sn(II)-poly-HEDP showed much improved stability with 100 % of the metal ion remaining bound to the ligand.

This document only includes an excerpt of the corresponding thesis or dissertation. To request a digital scan of the full text, please contact the Ruth Lilly Medical Library's Interlibrary Loan Department (rlmlill@iu.edu).

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This research involved the study of sediment cores from Loch Etive, Loch Long, Loch Goil and Loch Fyne with the aims of investigating the geochemistry of natural, and manmade radionuclides and heavy metals within the sea loch environment. The main aims of the research were to determine accumulation rates and the extent of mixing within these sediments and to assess the fluxes, sources and temporal variations in input of pollutant heavy metals to these environments. In recent years it has been suggested that Pb is mobile in sea loch sediments which questions the validity of applying ²¹⁰Pb dating in this environment. This has important implications with respect to interpreting sediment cores to assess temporal trends of pollutant inputs and investigating the rates of physical and biogeochemical processes that are taking place in the coastal environment. Hence, one of the aims of this research was to determine whether Pb was mobile in these sediments. The ²⁰⁶Pb/²⁰⁷Pb isotope ratio can potentially be used to determine the extent of pollutant Pb input from leaded petrol to the environment and a further objective of the work was to investigate the isotopic signature of pollutant Pb in the sediment. Concentration of ²¹⁰Pb, ²²⁶Ra, ²²⁸Ra, ²²⁸Th, ²³⁸U, ¹³⁷Cs, ¹³⁴Cs and ²⁴¹Am in the sediments were analysed using gamm a spectroscopy and the heavy metals, Pb, Zn and Cu were determined using X-ray Fluorescence. Stable Pb isotope ratios were determined using Inductively coupled plasma Mass spectrometry. The results obtained indicated that Pb is not subject to diagenetic mobility in these sediments and that ²¹⁰Pb profiles can be used to determine sedimentation rates for most of the sediment cores. lt was not possible to determine accumulation rates for the two cores from Loch Fyne by ²¹⁰Pb dating, and in this case the sedimentation rate was assessed by correlating the maximum concentration of ¹³⁷Cs in the sediments with the maximum ¹³⁷Cs discharge from Sellafield, BNFL's reprocessing plant located on the Cumbrian coast. The flux of ²¹⁰Pb to the lochs varied significantly suggesting that there has been sediment focusing of fine and/or organic rich material to the deeper sites, resulting in an enhanced flux of ²¹⁰Pb to these sediments. Sellafield waste radionuclides also provided useful chronologies by relating sediment maximum concentrations to maxima in the discharges. ¹³⁷Cs was observed to be subject to diffusive movement, invalidating the use of its total depth of penetration as a chronological indicator. The temporal trends of pollutant metal input agreed well with known historical trends and the Pb isotope profiles indicated that the onset of deposition from pollutant Pb from petrol occurred in the late 1920's. The maximum input of Pb from petrol peaked in the early 1980's and since then there has been a decrease in this input. The two sea lochs which were closest to the industrial centre of Glasgow exhibited a large anthropogenic pollutant input, confirming that these sediments have been highly perturbed by human activities, either directly as a result of sludge dumping or due to changes in land use (eg. road construction, deforestation, etc.) in the catchment. All the sea lochs reflected a change in the supply of material to the sediments over the last eighty years, indicating that increased anthropogenic activity has had an effect on these environments.

Thesis (MSc)--Stellenbosch University, 2000. / ENGLISH ABSTRACT: The radionuclide 75Se (T1/2= 119.8 days) decays to the stable isotope 75As by 100 % electron capture. Applications of this radioisotope include its use as a radiotracer in agricultural investigations and as a potential irradiation source in high-activity brachytherapy. The application of this isotope as a radiotracer in clinical studies has been limited due to a lack of availability of carrier-free 75Se. In this study the excitation functions for the production of carrier-free 75Se, other selenium radioisotopes and radiocontaminants produced via natBr(p,x) nuclear reactions were measured by the use of the stacked foil technique. Three separate stacks were assembled from aluminium and copper monitor foils and potassium bromide tablets. The latter were prepared by pressing KBr salt into tablets with a thickness of 200 mg/cm2 and a diameter of 20 mm, which are sandwiched between thin Al foils. The monitor foils, with a diameter of 19 mm, were punched from foil sheets. The stacks were irradiated at proton beam energies of 100.9 MeV, 66.8 MeV and 40.4 MeV respectively at the National Accelerator Centre cyclotron facility. After bombardment the KBr tablets were sealed in plastic bags to prevent the loss of any krypton isotopes produced. The gamma-ray spectra of the induced radioactivity in each of the target foils were recorded by means of a Ge-detector coupled with a SILENA 16-k multichannel analyser. The measured excitation functions for the above-mentioned isotopes are presented. Where applicable the cross-section values are compared with previously published values, while the others are presented as new data. Theoretical calculations by means of the computer code ALICE (IPPE) were also done for comparison. / AFRIKAANSE OPSOMMING: Die radionuklied 75Se (T1/2= 119.8 dae) verval deur 100 % elektronvangs na die stabiele isotoop 75As. Toepassings vir hierdie radioisotoop sluit in sy gebruik as 'n radiospoormiddel in landbou-ondersoeke en as 'n potensiële stralingsbron in hoë aktiwiteit bragiterapie. Die aanwending van hierdie isotoop as 'n radiospoorder in kliniese studies word egter beperk deur die gebrek aan beskikbaarheid van draer-vry 75Se. In hierdie studie is die opwekkingskrommes vir die produksie van draer-vry 75Se, ander selenium radioistope en radiokontaminante bepaal deur die natBr(p,x) kernreaksies te meet met behulp van die foelie-stapel metode. Drie verskillende stapels, bestaande uit aluminium- en koper-monitor foelies en kalium-bromied tablette, is saamgestel. Laasgenoemde is voorberei deur KBr sout saam te pers tot tablette met 'n dikte van 200 mg/cm2 en 'n deursnit van 20 mm en wat omsluit is met dun Al-foelies. Die monitor-foelies, met 'n deursnit van 19 mm, is gepons uit foelieplate. Die stapels is bestraal met protonbundels met energieë van onderskeidelik 100.9 MeV, 66.8 MeV en 40.4 MeV by die Nasionale Versneller Sentrum, Faure, se siklotron-fasiliteit. Na bombardering is die KBr tablette verseël in plastieksakkies om verliese van enige vervaardigde kripton isotope te verhoed. Die gamma-straal spektra van die geinduseeerde radioaktiwiteit in elke teiken is opgeneem met behulp van 'n Ge-detektor wat gekoppel was aan 'n SILENA 16-k multikanaal-analiseerder. Bogenoemde isotope se gemete opwekkingskrommes word aangebied. Waar van toepassing word die kansvlakwaardes vergelyk met vorige gepubliseerde waardes terwyl ander aangebied word as die eerste data bekend. 'n Vergelyking met die teoreties berekende kansvlakwaardes van die rekenaar kode ALICE (IPPE) word ook gedoen.

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