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  • About
  • The Global ETD Search service is a free service for researchers to find electronic theses and dissertations. This service is provided by the Networked Digital Library of Theses and Dissertations.
    Our metadata is collected from universities around the world. If you manage a university/consortium/country archive and want to be added, details can be found on the NDLTD website.
1

Vliv stromů na kontaminaci půdy 137Cs / The influence of trees on contamination of soil with 137Cs

TRNKOVÁ, Michaela January 2019 (has links)
Nuclear weapons testing in the atmosphere and accidents in nuclear energy facilities in the last 50 years caused significant contamination of the environment. Half-life of certain leaked radionuclides is several decades and therefore they are still present in today's environment. That is the reason why there is still on going monitoring of radiation situation in the Czech Republic in order to determine the behaviour and kinetics of anthropogenic radionuclides in the environment and the severity of radiological impact on humans. The results of this monitoring serve to review the radiation situation, observe long-term trends and last but not least to gain new knowledge that could facilitate the management od radiological emergencies. The aim of this thesis was to measure the content of 137Cs in soils under and around leafy tree crowns in the area affected by radiation fall and to find out whether the tree's crown has an effect on the distribution of 137Cs in the soils below them. To this end, a research question has been set: Do tree crowns affect the distribution of cesium in the soils below them? For better intelligibility, the introduction of the thesis is devoted to information about ionizing radiation, basic terms and quantities in the field of ionizing radiation, sources of radionuclide contamination, especially the Chernobyl nuclear power plant accident, environmental and population contamination, and elements important for the practical part of this work. The theoretical part is followed by research methodology. The soil samples were collected under five leafy trees of the Walnut species that met the set criteria for collection. Under each tree, samples were taken in three directions at an angle of 120° always at the trunk, in the middle of the crown, at the edge of the crown and outside the crown. Thus, 12 samples per tree, a total of 60 samples. Dry and purified soil samples were measured by semiconductor gamma spectrometry which determined 137Cs radionuclide mass activity values as well as naturally occurring radionuclide40K. Graphs were generated from the measured values. Despite the frequent deviations that may be caused by natural phenomena or human activities, it was found out that tree crowns affect the distribution of 137Cs in the soils below them.
2

Pursuit of purity: Measurement of chelation binding affinities for NOTA, DOTA, and desferal with applications to effective specific activity

Graves, S., Valdovinos, H., Cai, W., Barnhart, T., Nickles, R. 19 May 2015 (has links) (PDF)
Introduction The effective specific activity of a radioisotope is an indirect and highly useful way to describe a radioactive sample’s purity. A high effective specific activity combines the concept of an isotopically pure product with suitability via selectivity of a particular chelating body. The primary goals of this work are twofold: 1) To determine which metallic impurities have the largest impact on the effective specific activity for a given chelator, and 2) to form a model based on the binding affinities of each metal for to calculate a ‘theoretical effective specific activ-ity’ from broad band trace metal analysis. If successful, this information can be used to guide the production of high specific activity products through the systematic elimination of high-impact metallic impurities. Material and Methods Phosphor plate thin layer chromatography (TLC) was used to measure the effective specific activ-ity of 64Cu by NOTA and DOTA, and 89Zr by des-feral (DF). Typical measured effective specific activities are 2–5 Ci/μmol for 64Cu and 1–2 Ci/μmol for 89Zr. Samples were created containing increasing cod competitive burdens (X) of CuCl2, ZnCl2, FeCl2, NiCl2, CrCl3, CoCl2, MnCl2, and YCl3. Standard concentrations were measured by microwave plasma atomic emission spectrometry. 50 pmol of NOTA, DOTA, or DF were added following the activity aliquots of 64Cu or 89Zr. Labeling efficien-cies (64Cu-NOTA, 64Cu-DOTA, 89Zr-DF) were measured using TLC’s, and were fit by linear regression to the form f(X) = b/(1 − AX), where A is the chelation affinity (inverse of dissociation constant) and X is the molar ratio of the metallic impurity to the amount of chelator. Results and Conclusion Affinity of Zr for DF was assumed to be unity, while the affinities of Cu for NOTA and DOTA were explicitly measured and were found to be 0.93 ± 0.13 and 5.2 ± 3.2 respectively. It was found that Cu had the highest affinity for NOTA by a factor of 266, and that Zr had the highest affinity for DF by a factor of 40. • In order of decreasing affinity to NOTA: Cu, Zn, Fe, Co, Cr, Y, and Ni • In order of decreasing affinity to DOTA: Cu, Y, Zn, Co, Ni, Cr, and Fe • In order of decreasing affinity to DF: Zr, Y, Cu, Zn, Ni, Fe, Co, Cr These results suggest that aside from the carrier element it is most important to remove zinc from 64Cu products prior to chelation with NOTA and yttrium from 64Cu and 89Zr products prior to chelation with DOTA and DF, respectively. Therefore, it is logical to believe that 89Zr effective specific activities could be greatly improved by secondary separations with the goal of re-moving additional yttrium target material. Chelation affinities of NOTA, DOTA, and DF for several common metals have successfully been investigated. These values will guide our future attempts to provide high effective specific activity 64¬Cu and 89Zr. Furthermore, a preliminary model has been formed to calculate effective specific activity from the quantitative broad band analysis of trace metals. Future work will include chelator affinity measurements for other likely contaminants, such as scandium, titanium, zirconium, molybdenum, niobium, gold, gallium, and germanium. Details will be presented.
3

A practical high current 11 MeV production of high specific activity 89Zr

Link, J. M., O'Hara, M. J., Shoner, S. C., Armstrong, J. O., Krohn, K. A. 19 May 2015 (has links) (PDF)
Introduction Zr-89 is a useful radionuclide for radiolabeling proteins and other molecules.1,2 There are many reports of cyclotron production of 89Zr by the 89Y (p,n) reaction. Most irradiations use thin metal backed deposits of Y and irradiation currents up to 100 µA or thicker amounts of Y or Y2O3 with ~ 20 µA irradiations.3,4 We are working to develop high specific activity 89Zr using a low energy 11 MeV cyclotron. We have found that target Y metal contains carrier Zr and higher specific activities are achieved with less Y. The goal of this work was to optimize yield while minimizing the amount of Y that was irradiated. Material and Methods All irradiations were done using a Siemens Eclipse 11 MeV proton cyclotron. Y foils were used for the experiments described here. Y2O3 was tried and abandoned due to lower yield and poor heat transfer. Yttrium metal foils from Alfa Aesar, ESPI Metals and Sigma Aldrich, 0.1 to 1 mm in thickness, were tested. Each foil was irradiated for 10 to 15 minutes. The targets to hold the Y foils were made of aluminum and were designed to fit within the “paper burn” unit of the Siemen’s Eclipse target station, allowing the Y target body to be easily inserted and removed from the system. Several Al targets of 2 cm diam. and 7.6 cm long were tested with the face of the targets from 11, 26 or 90o relative to the beam to vary watts cm−2 on the foil. The front of the foils was cooled by He convection and the foil backs by conduction to the Al target body. The target body was cooled by conduction to the water cooled Al sleeve of the target holder. Results and Conclusion The best target was two stacked, 0.25 mm thick, foils to stop beam. 92% of the 89Zr activity was in the front 0.25 mm Y foil. With the greatest slant we could irradiate up to 30 µA of beam on tar-get. However, the 13×30 mm dimensions of the foil was more mass (0.41 g) and lower specific activity than was desired. Redesign of the target gave a target 90o to the beam with 12×12 mm foils (0.15 g/foil) that were undamaged with up to 30 µA irradiation when two foils were used. This design has a reduction in beam at the edges of ~10%. With this design, a single Y foil, 0.25 mm thick sustained over 31 µA of beam and a peak power on target of 270 watts cm−2. The product was radionuclidically pure 89Zr after all 89mZr and small amounts of 13N produced from oxygen at the surface had decayed (TABLE 1). Our conclusion is that the optimum target is a single 0.25 mm thick Y foil to obtain the greatest specific activity at this proton energy. This produces 167 MBq of 89Zr at EOB with a 15 minute and 31 µA irradiation. We are continuing to redesign the clamp design to reduce losses at the edge of the beam.
4

Effect Of Synthetic Pyrethroid Lambda- Cyhalothrin On Helicoverpa Armigera Glutathione S-transferases

Konus, Metin 01 December 2004 (has links) (PDF)
Helicoverpa armigera is a polyphagous pest. Due to excessive use of insecticides, the field populations of H. armigera have become resistant to synthetic pyrethroids by one or combination of three mechanisms / reduced penetration through the cuticle, decreased nerve sensitivity and enhanced metabolism by the detoxification enzymes especially glutathione S-transferases. In this study, gut sections of H. armigera were obtained from Adana and Antalya field populations and susceptible populations from Israel. Each gut section was homogenized separately in 1.0 ml, 40 mM and pH 7.5 phosphate buffers. GST activity was determined using CDNB as substrate. Product formation linearly increased up to 29.5&micro / g proteins in 20mM, pH 7.5 phosphate buffers. Maximum reaction rate was reached at 30&amp / #9702 / C. The Vmax and Km values for GST towards CDNB and GSH were calculated with Lineweaver-Burk and Eadie-Scatchard plots as CDNB Vmax / 6.54&micro / mol/min/mg, 6.35&micro / mol/min/mg , Km / 0.29mM, 0.28mM ,respectively and as GSH Vmax / 6.42&micro / mol/min/mg, 6.65&micro / mol/min/mg, Km / 0.22mM, 0.23mM, respectively. Cytosolic GST activity of each individual from Adana, Antalya and susceptible populations were determined under optimized conditions. The mean of GST activity in Adana population (n=50) and Antalya population (n=50) were found 7.824&micro / mol/min/mg and 9.518&micro / mol/min/mg, respectively. The mean of GST activity in susceptible population (n=50) was determined as 3.272&micro / mol/min/mg. According to these results, GST activities of Adana and Antalya field populations&rsquo / showed statistically significant increase (p&lt / 0.05) than susceptible H. armigera populations with ANOVA method. In addition, Antalya population showed statistically increase (p&lt / 0.05) GST activity than Adana.
5

Obsah cesia - 137 v jednotlivých druzích půd ve vybraných lokalitách ČR / The contents of caesium-137 in different soil types in selected locations in CR

ČADOVÁ, Michaela January 2017 (has links)
Caesium-137 is one of the major artificial radioactive elements, whose sources are atmospheric nuclear tests carried out in the 20th century and nuclear power plant incidents such as Chernobyl. Because of uneven precipitation, there were significant differences in radioactive fallout levels in different areas of the Czech Republic during the passage of the radioactive cloud from Chernobyl. Due to the high solubility of Caesium-137 in water and easy distribution in the environment, there is contamination of the lower soil levels where the plant root systems are located. The aim of this work is to collect soil samples from selected localities, where in 1986 significant contamination was detected as originating from Chernobyl, determination of their Caesium-137 content by gamma semiconductor spectrometry and comparison depending on the type of soil. The research question was set as: Does Caesium-137 content differ in different soil types? As part of this study, samples of uncultivated agricultural land and forest land were collected from layers 0-5, 5-10 and 10-15 cm in Kvilda, Zadov and Churanov. For comparison, results were also collected from a locality where the radioactive fallout was not so significant. This locality is around the village Straz nad Nezarkou, which is found on the protected nature reserves of Trebon. From the results of measuring the soil it was found that even after thirty years since the Chernobyl disaster occurred, Caesium-137 is still found in the upper layers of soils, specifically to depths of 5 cm. The highest specific activity of Caesium-137 was measured in the forest soils in Zadov at depths of 0-5 cm (364 Bq.kg-1) from the total range of all samples, 2,24 Bq.kg-1 to 364 Bq.kg-1. The highest specific activity of potassium K-40 was measured in uncultivated agricultural land in the locality of Kvilda at depths of 0-5 cm (883 Bq.kg-1).
6

Svalové dysbalance u vodních slalomářů měřeno pomocí TMG / Muscle imbalances in white water canoeing measured by TMG

Hapák, Michal January 2020 (has links)
Title: Muscle imbalances in white water canoeing measured by TMG Aims: The aim of this paper was to select the endangered muscle groups, to identify possible imbalances using tensiomyograph (TMG 100) and to define hypotheses about the influence of training load in water slalom on the development of imbalances in the selected specific muscle groups. Methods: This work has a character of a qualitative research. Specifically, 6 case studies were carried out, appended by control measurements after one year, in which emphasis was placed on the detection of characteristic muscle imbalances that could arise as a result of specific training activities in water slalom. To measure these muscle imbalances, we used tensiomyograph (TMG 100). Results: Among the measured participants, we found that during a one-year training cycle, significant changes in the functionality of individual muscle groups have occurred. The most endangered groups, ie the groups with the most significant changes, included BB, DEL, LD and TRM. There have been also notable changes in the functional symmetry of the elbow joint, where 4 out of 5 participants have deteriorated during the year. It was also found, that women might be more prone to imbalances as an effect of the specific activity compared to men. Key words: white water...
7

Fungos micorrízicos arbusculares e nível de potássio no solo na absorção de 137césio e efeitos na resposta antioxidativa do feijoeiro / Arbuscular mycorrhizal fungi and soil potassium supply on the 137césio uptake and its effects on the antioxidative response of common bean

Donha, Riviane Maria Albuquerque 28 February 2014 (has links)
Associações entre fungos micorrízicos arbusculares e plantas hospedeiras podem transferir césio (137Cs) para o vegetal. A mobilidade do césio (Cs+) nos solos e sua similaridade química com o potássio (K+) constituem a principal ameaça à contaminação da vegetação pelo radionuclídeo. Foi realizado experimento com plantas de feijão (Phaseolus vulgaris L.) variedade Iapar Tangará, com o objetivo de avaliar o coeficiente de transferência direta do 137Cs do solo para a planta, a absorção, o transporte e o acúmulo do radionuclídeo 137Cs nas folhas, caule e raízes das plantas, a produção de massa seca do feijoeiro, o diâmetro do caule das plantas, a peroxidação lipídica, avaliar as enzimas do sistema antioxidativo (catalase, ascorbato peroxidase, glutationa redutase e superóxido dismutase), o teor de clorofila em unidade SPAD, em função dos efeitos da: (I) inoculação ou não com fungos micorrízicos arbusculares (FMA) e (II) do nível de potássio em quatro tipos de solos: Nitossolo, Chernossolo, Argissolo e Gleissolo. O delineamento experimental foi o de blocos completos ao acaso, utilizando esquema fatorial de quatro tipos de solo x dois níveis de potássio x presença e ausência de micorrizas com três repetições, totalizando 48 unidades experimentais. Foi calculada a atividade específica do 137Cs no solo e na planta e, por fim, a determinação do coeficiente de transferência direta do 137Cs do solo para o vegetal. Nas plantas cultivadas em Argissolo, Chernossolo e Gleissolo, foi observada maior atividade específica de 137Cs nas raízes do feijão em relação às folhas e ao caule, na condição de baixo nível de potássio e ausência de inoculação de FMA. O coeficiente de transferência solo-planta do 137Cs e a atividade na planta foram maiores no Argissolo e Nitossolo, com baixo teor de potássio e sem a presença de FMA. Constatou-se interação entre os tipos de solo, teor de K e presença de FMA quanto à peroxidação de lipídeos, sendo que houve maior dano nas folhas das plantas cultivadas no Chernossolo, principalmente no tratamento sem aplicação de FMA e com baixo teor de K. Não foi observada interação entre os solos e a inoculação com FMA para a quantificação de peróxido de hidrogênio (H2O2) nas folhas, todavia, constatou-se efeito para os teores de K no solo. Quanto ao sistema enzimático antioxidativo, a atividade da catalase, glutationa redutase, ascorbato peroxidase e superóxido dismutase houve interação entre os tipos de solo, níveis de K e presença ou ausência de FMA. Maior atividade da superóxido dismutase (SOD) foi demonstrada nas plantas cultivadas no Argissolo, sem a presença de FMA, também independente dos teores de K. O aumento nos teores de K nos solos não impediu a transferência direta de 137Cs do solo para as plantas, porém, reduziu a absorção do nuclídeo pelo feijoeiro. O tipo de solo influenciou na disponibilidade de 137Cs às plantas de feijão e por sua vez, nas atividades das enzimas do sistema de defesa da planta. A inoculação com os FMA não foi efetiva para evitar a transferência e a absorção de 137Cs pelas plantas / Associations between arbuscular mycorrhizal fungi (AMF) and host plants might transfer cesium (137Cs) for the plant. The mobility of cesium (Cs+) in soils and their chemical similarity to potassium (K+) are the main threat to contamination of vegetation by radionuclide. Experiment with common bean (Phaseolus vulgaris L.) variety Iapar Tangara was conducted with the objective of evaluating the coefficient of direct transfer of 137Cs from soil to the plant, absorption, transport and accumulation of the radionuclide 137Cs in the leaves, stem and plant roots, the dry mass of bean stem diameter of plants, lipid peroxidation, evaluate the antioxidant system enzymes (catalase, ascorbate peroxidase, glutathione reductase and superoxide dismutase), the content of chlorophyll SPAD unit, due to the effects of: (I) or without inoculation with mycorrhizal fungi (AMF) and (II) the level of potassium in four types of soil: Nitosol Chernosol, Alfisol and Ultisol. The experimental design was a randomized complete block, factorial design using four soil types x two levels of potassium x presence and absence of mycorrhizae with three replications, totaling 48 experimental units. The specific activity of 137Cs in soil and plant and finally, the coefficient of 137Cs direct transfer from soil to plant was calculated. In plants grown in Alfisol and Ultisol Chernosol, higher specific activity of 137Cs in bean roots compared to the leaves and the stem was observed under the condition of low potassium and absence of AMF inoculation. The coefficient of soil-plant transfer of 137Cs activity and yield were higher in the Ultisol and Alfisol with low potassium and without the presence of AMF. Found an interaction between soil types, K content and the presence of AMF as to lipid peroxidation, and there was more damage on the leaves of plants grown at Chernosol, primarily in the treatment without application of AMF and low in K. No interaction between soil and AMF inoculation for quantification of hydrogen peroxide (H2O2) in the leaves was observed, however, it was found to effect the K in the soil. As for the antioxidant enzyme system, the activity of catalase, glutathione reductase, ascorbate peroxidase and superoxide dismutase was no interaction between soil types, levels of K and the presence or absence of AMF. Increased activity of superoxide dismutase (SOD) has been demonstrated in plants grown in Ultisol without the presence of AMF, independent of the levels of K. The increase of K in the soil did not prevent the direct transfer of 137Cs from soil to plants, however, reduced the uptake of the nuclide by bean. Soil type influenced the availability of 137Cs to bean plants and in turn, the enzyme activities of the plant defense system. Inoculation with AMF was not effective to prevent the transfer and uptake of 137Cs by plants
8

Fungos micorrízicos arbusculares e nível de potássio no solo na absorção de 137césio e efeitos na resposta antioxidativa do feijoeiro / Arbuscular mycorrhizal fungi and soil potassium supply on the 137césio uptake and its effects on the antioxidative response of common bean

Riviane Maria Albuquerque Donha 28 February 2014 (has links)
Associações entre fungos micorrízicos arbusculares e plantas hospedeiras podem transferir césio (137Cs) para o vegetal. A mobilidade do césio (Cs+) nos solos e sua similaridade química com o potássio (K+) constituem a principal ameaça à contaminação da vegetação pelo radionuclídeo. Foi realizado experimento com plantas de feijão (Phaseolus vulgaris L.) variedade Iapar Tangará, com o objetivo de avaliar o coeficiente de transferência direta do 137Cs do solo para a planta, a absorção, o transporte e o acúmulo do radionuclídeo 137Cs nas folhas, caule e raízes das plantas, a produção de massa seca do feijoeiro, o diâmetro do caule das plantas, a peroxidação lipídica, avaliar as enzimas do sistema antioxidativo (catalase, ascorbato peroxidase, glutationa redutase e superóxido dismutase), o teor de clorofila em unidade SPAD, em função dos efeitos da: (I) inoculação ou não com fungos micorrízicos arbusculares (FMA) e (II) do nível de potássio em quatro tipos de solos: Nitossolo, Chernossolo, Argissolo e Gleissolo. O delineamento experimental foi o de blocos completos ao acaso, utilizando esquema fatorial de quatro tipos de solo x dois níveis de potássio x presença e ausência de micorrizas com três repetições, totalizando 48 unidades experimentais. Foi calculada a atividade específica do 137Cs no solo e na planta e, por fim, a determinação do coeficiente de transferência direta do 137Cs do solo para o vegetal. Nas plantas cultivadas em Argissolo, Chernossolo e Gleissolo, foi observada maior atividade específica de 137Cs nas raízes do feijão em relação às folhas e ao caule, na condição de baixo nível de potássio e ausência de inoculação de FMA. O coeficiente de transferência solo-planta do 137Cs e a atividade na planta foram maiores no Argissolo e Nitossolo, com baixo teor de potássio e sem a presença de FMA. Constatou-se interação entre os tipos de solo, teor de K e presença de FMA quanto à peroxidação de lipídeos, sendo que houve maior dano nas folhas das plantas cultivadas no Chernossolo, principalmente no tratamento sem aplicação de FMA e com baixo teor de K. Não foi observada interação entre os solos e a inoculação com FMA para a quantificação de peróxido de hidrogênio (H2O2) nas folhas, todavia, constatou-se efeito para os teores de K no solo. Quanto ao sistema enzimático antioxidativo, a atividade da catalase, glutationa redutase, ascorbato peroxidase e superóxido dismutase houve interação entre os tipos de solo, níveis de K e presença ou ausência de FMA. Maior atividade da superóxido dismutase (SOD) foi demonstrada nas plantas cultivadas no Argissolo, sem a presença de FMA, também independente dos teores de K. O aumento nos teores de K nos solos não impediu a transferência direta de 137Cs do solo para as plantas, porém, reduziu a absorção do nuclídeo pelo feijoeiro. O tipo de solo influenciou na disponibilidade de 137Cs às plantas de feijão e por sua vez, nas atividades das enzimas do sistema de defesa da planta. A inoculação com os FMA não foi efetiva para evitar a transferência e a absorção de 137Cs pelas plantas / Associations between arbuscular mycorrhizal fungi (AMF) and host plants might transfer cesium (137Cs) for the plant. The mobility of cesium (Cs+) in soils and their chemical similarity to potassium (K+) are the main threat to contamination of vegetation by radionuclide. Experiment with common bean (Phaseolus vulgaris L.) variety Iapar Tangara was conducted with the objective of evaluating the coefficient of direct transfer of 137Cs from soil to the plant, absorption, transport and accumulation of the radionuclide 137Cs in the leaves, stem and plant roots, the dry mass of bean stem diameter of plants, lipid peroxidation, evaluate the antioxidant system enzymes (catalase, ascorbate peroxidase, glutathione reductase and superoxide dismutase), the content of chlorophyll SPAD unit, due to the effects of: (I) or without inoculation with mycorrhizal fungi (AMF) and (II) the level of potassium in four types of soil: Nitosol Chernosol, Alfisol and Ultisol. The experimental design was a randomized complete block, factorial design using four soil types x two levels of potassium x presence and absence of mycorrhizae with three replications, totaling 48 experimental units. The specific activity of 137Cs in soil and plant and finally, the coefficient of 137Cs direct transfer from soil to plant was calculated. In plants grown in Alfisol and Ultisol Chernosol, higher specific activity of 137Cs in bean roots compared to the leaves and the stem was observed under the condition of low potassium and absence of AMF inoculation. The coefficient of soil-plant transfer of 137Cs activity and yield were higher in the Ultisol and Alfisol with low potassium and without the presence of AMF. Found an interaction between soil types, K content and the presence of AMF as to lipid peroxidation, and there was more damage on the leaves of plants grown at Chernosol, primarily in the treatment without application of AMF and low in K. No interaction between soil and AMF inoculation for quantification of hydrogen peroxide (H2O2) in the leaves was observed, however, it was found to effect the K in the soil. As for the antioxidant enzyme system, the activity of catalase, glutathione reductase, ascorbate peroxidase and superoxide dismutase was no interaction between soil types, levels of K and the presence or absence of AMF. Increased activity of superoxide dismutase (SOD) has been demonstrated in plants grown in Ultisol without the presence of AMF, independent of the levels of K. The increase of K in the soil did not prevent the direct transfer of 137Cs from soil to plants, however, reduced the uptake of the nuclide by bean. Soil type influenced the availability of 137Cs to bean plants and in turn, the enzyme activities of the plant defense system. Inoculation with AMF was not effective to prevent the transfer and uptake of 137Cs by plants
9

Pursuit of purity: Measurement of chelation binding affinities for NOTA, DOTA, and desferal with applications to effective specific activity

Graves, S., Valdovinos, H., Cai, W., Barnhart, T., Nickles, R. January 2015 (has links)
Introduction The effective specific activity of a radioisotope is an indirect and highly useful way to describe a radioactive sample’s purity. A high effective specific activity combines the concept of an isotopically pure product with suitability via selectivity of a particular chelating body. The primary goals of this work are twofold: 1) To determine which metallic impurities have the largest impact on the effective specific activity for a given chelator, and 2) to form a model based on the binding affinities of each metal for to calculate a ‘theoretical effective specific activ-ity’ from broad band trace metal analysis. If successful, this information can be used to guide the production of high specific activity products through the systematic elimination of high-impact metallic impurities. Material and Methods Phosphor plate thin layer chromatography (TLC) was used to measure the effective specific activ-ity of 64Cu by NOTA and DOTA, and 89Zr by des-feral (DF). Typical measured effective specific activities are 2–5 Ci/μmol for 64Cu and 1–2 Ci/μmol for 89Zr. Samples were created containing increasing cod competitive burdens (X) of CuCl2, ZnCl2, FeCl2, NiCl2, CrCl3, CoCl2, MnCl2, and YCl3. Standard concentrations were measured by microwave plasma atomic emission spectrometry. 50 pmol of NOTA, DOTA, or DF were added following the activity aliquots of 64Cu or 89Zr. Labeling efficien-cies (64Cu-NOTA, 64Cu-DOTA, 89Zr-DF) were measured using TLC’s, and were fit by linear regression to the form f(X) = b/(1 − AX), where A is the chelation affinity (inverse of dissociation constant) and X is the molar ratio of the metallic impurity to the amount of chelator. Results and Conclusion Affinity of Zr for DF was assumed to be unity, while the affinities of Cu for NOTA and DOTA were explicitly measured and were found to be 0.93 ± 0.13 and 5.2 ± 3.2 respectively. It was found that Cu had the highest affinity for NOTA by a factor of 266, and that Zr had the highest affinity for DF by a factor of 40. • In order of decreasing affinity to NOTA: Cu, Zn, Fe, Co, Cr, Y, and Ni • In order of decreasing affinity to DOTA: Cu, Y, Zn, Co, Ni, Cr, and Fe • In order of decreasing affinity to DF: Zr, Y, Cu, Zn, Ni, Fe, Co, Cr These results suggest that aside from the carrier element it is most important to remove zinc from 64Cu products prior to chelation with NOTA and yttrium from 64Cu and 89Zr products prior to chelation with DOTA and DF, respectively. Therefore, it is logical to believe that 89Zr effective specific activities could be greatly improved by secondary separations with the goal of re-moving additional yttrium target material. Chelation affinities of NOTA, DOTA, and DF for several common metals have successfully been investigated. These values will guide our future attempts to provide high effective specific activity 64¬Cu and 89Zr. Furthermore, a preliminary model has been formed to calculate effective specific activity from the quantitative broad band analysis of trace metals. Future work will include chelator affinity measurements for other likely contaminants, such as scandium, titanium, zirconium, molybdenum, niobium, gold, gallium, and germanium. Details will be presented.
10

A practical high current 11 MeV production of high specific activity 89Zr

Link, J. M., O'Hara, M. J., Shoner, S. C., Armstrong, J. O., Krohn, K. A. January 2015 (has links)
Introduction Zr-89 is a useful radionuclide for radiolabeling proteins and other molecules.1,2 There are many reports of cyclotron production of 89Zr by the 89Y (p,n) reaction. Most irradiations use thin metal backed deposits of Y and irradiation currents up to 100 µA or thicker amounts of Y or Y2O3 with ~ 20 µA irradiations.3,4 We are working to develop high specific activity 89Zr using a low energy 11 MeV cyclotron. We have found that target Y metal contains carrier Zr and higher specific activities are achieved with less Y. The goal of this work was to optimize yield while minimizing the amount of Y that was irradiated. Material and Methods All irradiations were done using a Siemens Eclipse 11 MeV proton cyclotron. Y foils were used for the experiments described here. Y2O3 was tried and abandoned due to lower yield and poor heat transfer. Yttrium metal foils from Alfa Aesar, ESPI Metals and Sigma Aldrich, 0.1 to 1 mm in thickness, were tested. Each foil was irradiated for 10 to 15 minutes. The targets to hold the Y foils were made of aluminum and were designed to fit within the “paper burn” unit of the Siemen’s Eclipse target station, allowing the Y target body to be easily inserted and removed from the system. Several Al targets of 2 cm diam. and 7.6 cm long were tested with the face of the targets from 11, 26 or 90o relative to the beam to vary watts cm−2 on the foil. The front of the foils was cooled by He convection and the foil backs by conduction to the Al target body. The target body was cooled by conduction to the water cooled Al sleeve of the target holder. Results and Conclusion The best target was two stacked, 0.25 mm thick, foils to stop beam. 92% of the 89Zr activity was in the front 0.25 mm Y foil. With the greatest slant we could irradiate up to 30 µA of beam on tar-get. However, the 13×30 mm dimensions of the foil was more mass (0.41 g) and lower specific activity than was desired. Redesign of the target gave a target 90o to the beam with 12×12 mm foils (0.15 g/foil) that were undamaged with up to 30 µA irradiation when two foils were used. This design has a reduction in beam at the edges of ~10%. With this design, a single Y foil, 0.25 mm thick sustained over 31 µA of beam and a peak power on target of 270 watts cm−2. The product was radionuclidically pure 89Zr after all 89mZr and small amounts of 13N produced from oxygen at the surface had decayed (TABLE 1). Our conclusion is that the optimum target is a single 0.25 mm thick Y foil to obtain the greatest specific activity at this proton energy. This produces 167 MBq of 89Zr at EOB with a 15 minute and 31 µA irradiation. We are continuing to redesign the clamp design to reduce losses at the edge of the beam.

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