The determination of three selected sites for the construction and operation of a low level radioactive waste storage and burial facility

Radioactive wastes are by-products of the use of radiation technologies. As with many technologies, the wastes are required to be disposed of in a safe manner so as to minimise risk to human health. This study examines the requirements for a hypothetical repository and develops techniques for decision making to permit the establishment of a shallow ground burial facility to receive an inventory of low-level radioactive wastes. Australia’s overall inventory is used as an example. Essential and desirable siting criteria are developed and applied to Australia's Northern Territory resulting in the selection of three candidate sites for laboratory investigations into soil behaviour. The essential quantifiable factors which govern radionuclide migration and ultimately influence radiation doses following facility closure are reviewed. Simplified batch and column procedures were developed to enable laboratory determination of distribution and retardation coefficient values for use in one-dimensional advection-dispersion transport equations. Batch and column experiments were conducted with Australian soils sampled from the three identified candidate sites using a radionuclide representative of the current national low-level radioactive waste inventory. The experimental results are discussed and site soil performance compared. The experimental results are subsequently used to compare the relative radiation health risks between each of the three sites investigated. A recommendation is made as to the preferred site to construct an engineered near-surface burial facility to receive the Australian low-level radioactive waste inventory.

Vibrational spectroscopic study of the mineral penkvilksite Na2TiSi4O11·2H2O – a mineral used for the uptake of radionuclides

We have used vibrational spectroscopy to study the formula and molecular structure of the mineral penkvilksite Na 2TiSi 4O 11·2H 2O. Penkvilksite is a mineral which may be used in the uptake of radioactive elements. Both Raman and infrared spectroscopies identify a band at 3638 cm−1 attributed to an OH-stretching vibration of hydroxyl units. The inference is that OH units are involved in the structure of penkvilksite. The formula may be well written as Na 2TiSi 4O 10(OH)2·H 2O. The mineral is characterised by a very intense Raman band at 1085 cm−1 and a broad infrared band at 1080 cm−1 assigned to SiO-stretching vibrations. Raman bands at 620, 667 and 711 cm−1 are attributed to SiO and TiO chain bonds. Water-stretching vibrations are observed as Raman bands at 3197, 3265, 3425 and 3565 cm−1. Vibrational spectroscopy enables aspects of the molecular structure of the mineral penkvilksite to be ascertained. Penkvilksite is a mineral which can incorporate actinides and lanthanides from radioactive waste.

Anterior temporal cortex and semantic memory : reconciling findings from neuropsychology and functional imaging

Studies of semantic impairment arising from brain disease suggest that the anterior temporal lobes are critical for semantic abilities in humans; yet activation of these regions is rarely reported in functional imaging studies of healthy controls performing semantic tasks. Here, we combined neuropsychological and PET functional imaging data to show that when healthy subjects identify concepts at a specific level, the regions activated correspond to the site of maximal atrophy in patients with relatively pure semantic impairment. The stimuli were color photographs of common animals or vehicles, and the task was category verification at specific (e.g., robin), intermediate (e.g., bird), or general (e.g., animal) levels. Specific, relative to general, categorization activated the antero-lateral temporal cortices bilaterally, despite matching of these experimental conditions for difficulty. Critically, in patients with atrophy in precisely these areas, the most pronounced deficit was in the retrieval of specific semantic information.

The brain serotonin transporter binding in young adults; methodological considerations and association with Bulimia Nervosa and acquired obesity

The neurotransmitter serotonin (5-HT) modulates many functions important for life, e.g., appetite and body temperature, and controls development of the neural system. Disturbed 5-HT function has been implicated in mood, anxiety and eating disorders. The serotonin transporter (SERT) controls the amount of effective 5-HT by removing it from the extracellular space. Radionuclide imaging methods single photon emission tomography (SPET) and positron emission tomography (PET) enable studies on the brain SERTs. This thesis concentrated on both methodological and clinical aspects of the brain SERT imaging using SPET. The first study compared the repeatability of automated and manual methods for definition of volumes of interest (VOIs) in SERT images. The second study investigated within-subject seasonal variation of SERT binding in healthy young adults in two brain regions, the midbrain and thalamus. The third study investigated the association of the midbrain and thalamic SERT binding with Bulimia Nervosa (BN) in female twins. The fourth study investigated the association of the midbrain and hypothalamic/thalamic SERT binding and body mass index (BMI) in monozygotic (MZ) twin pairs. Two radioligands for SERT imaging were used: [123I]ADAM (studies I-III) and [123I]nor-beta-CIT (study IV). Study subjects included young adult MZ and dizygotic (DZ) twins screened from the FinnTwin16 twin cohort (studies I-IV) and healthy young adult men recruited for study II. The first study validated the use of an automated brain template in the analyses of [123I]ADAM images and proved automated VOI definition more reproducible than manual VOI definition. The second study found no systematic within-subject variation in SERT binding between scans done in summer and winter in either of the investigated brain regions. The third study found similar SERT binding between BN women (including purging and non-purging probands), their unaffected female co-twins and other healthy women in both brain regions; in post hoc analyses, a subgroup of purging BN women had significantly higher SERT binding in the midbrain as compared to all healthy women. In the fourth study, MZ twin pairs were divided into twins with higher BMI and co-twins with lower BMI; twins with higher BMI were found to have higher SERT binding in the hypothalamus/thalamus than their leaner co-twins. Our results allow the following conclusions: 1) No systematic seasonal variation exists in the midbrain and thalamus between SERT binding in summer and winter. 2) In a population-based sample, BN does not associate with altered SERT status, but alterations are possible in purging BN women. 3) The higher SERT binding in MZ twins with higher BMIs as compared to their leaner co-twins suggests non-genetic association between acquired obesity and the brain 5-HT system, which may have implications on feeding behavior and satiety.

Auger-emitter radiochemotherapy in squamous cell cancers : in vitro and in vivo experiments with In-111-BLMC

Head and neck squamous cell cancer (HNSCC) is the sixth most common cancer worldwide. Despite advances in combined modality therapy (surgery, radiotherapy, chemotherapy) the 5-year survival rate in stage III and IV disease remains at 40% - 60%. Short-range Auger-electron emitters, such as In-111 and In-114m, tagged with a drug, molecule, peptide, protein or nanoparticles brought in close proximity to nuclear DNA represent a fascinating alternative for treating cancer. In this thesis, we studied the usefulness of Indium-111-bleomycin complex (In-111-BLMC) in the diagnostics and potential therapy of HNSCC using in vitro HNSCC cell lines, in vivo nude mice, and in vivo HNSCC patients. In in vitro experiments with HNSCC cell lines, the sensitivity to external beam radiation, BLM, In-111-BLMC, and In-111-Cl3 was studied using the 96-well plate clonogenic assay. The influence of BLM and In-111-BLMC on the cell cycle was measured with flow cytometry. In in vivo nude mice xenograft studies, the activity ratios of In-111-BLMC were obtained in gamma camera images. The effect of In-111-BLMC in HNSCC xenografts was studied. In in vivo patient studies, we determined the tumor uptake of In-111-BLMC with gamma camera and the radioactivity from tumor samples using In-111-BLMC with specific activity of 75, 175, or 375 MBq/mg BLM. The S values, i.e. absorbed dose in a target organ per cumulated activity in a source organ, were simulated for In-111 and In-114m. In vitro studies showed the variation of sensitivity for external beam radiation, BLM, and In-111-BLMC between HNSCC cell lines. IC50 values for BLM were 1.6-, 1.8-, and 2.1-fold higher than In-111-BLMC (40 MBq/mg BLM) in three HNSCC cell lines. Specific In-111 activity of 40 MBq/mgBLM was more effective in killing cells than specific In-111 activity of 195MBq/mgBLM (p=0.0023). In-111-Cl3 alone had no killing effect. The percentage of cells in the G2/M phase increased after exposure to BLM and especially to In-111-BLMC in the three cell lines studied, indicating a G2/M block. The tumor-seeking behavior was shown in the in vivo imaging study of xenografted mice. BLM and In-111-BLMC were more effective than NaCl in reducing xenografted tumor size in HNSCC. The uptake ratios received from gamma images in the in vivo patient study varied from 1.2 to 2.8 in malignant tumors. However, the uptake of In-111-BLMC was unaffected by increasing the injected activity. A positive correlation existed between In-111-BLMC uptake, Ki-67/MIB activity, and number of mitoses. Regarding the S values, In-114m delivered a 4-fold absorbed radiation dose into the tumor compared with In-111, and thus, In-114m-BLMC might be more effective than In-111-BLMC at the DNA level. Auger-electron emitters, such as In-111 and In-114m, might have potential in the treatment of HNSCC. Further studies are needed to develop a radiopharmaceutical agent with appropriate physical properties of the radionuclide and a suitable carrier to bring it to the targeted tissue.

Development of radiosynthesis methods for 18F-labelled radiopharmaceuticals : General considerations and production of a dopamine transporter radioligand

Positron emission tomography (PET) is a molecular imaging technique that utilises radiopharmaceuticals (radiotracers) labelled with a positron-emitting radionuclide, such as fluorine-18 (18F). Development of a new radiotracer requires an appropriate radiosynthesis method: the most common of which with 18F is nucleophilic substitution with [18F]fluoride ion. The success of the labelling reaction is dependent on various factors such as the reactivity of [18F]fluoride, the structure of the target compound in addition to the chosen solvent. The overall radiosynthesis procedure must be optimised in terms of radiochemical yield and quality of the final product. Therefore, both quantitative and qualitative radioanalytical methods are essential in developing radiosynthesis methods. Furthermore, biological properties of the tracer candidate need to be evaluated by various pre-clinical studies in animal models. In this work, the feasibility of various nucleophilic 18F-fluorination strategies were studied and a labelling method for a novel radiotracer, N-3-[18F]fluoropropyl-2beta-carbomethoxy-3beta-4-fluorophenyl)nortropane ([18F]beta-CFT-FP), was optimised. The effect of solvent was studied by labelling a series of model compounds, 4-(R1-methyl)benzyl R2-benzoates. 18F-Fluorination reactions were carried out both in polar aprotic and protic solvents (tertiary alcohols). Assessment of the 18F-fluorinated products was studied by mass spectrometry (MS) in addition to conventional radiochromatographic methods, using radiosynthesis of 4-[18F]fluoro-N-[2-[1-(2-methoxyphenyl)-1-piperazinyl]ethyl-N-2-pyridinyl-benzamide (p-[18F]MPPF) as a model reaction. Labelling of [18F]beta-CFT-FP was studied using two 18F-fluoroalkylation reagents, [18F]fluoropropyl bromide and [18F]fluoropropyl tosylate, as well as by direct 18F-fluorination of sulfonate ester precursor. Subsequently, the suitability of [18F]beta-CFT-FP for imaging dopamine transporter (DAT) was evaluated by determining its biodistribution in rats. The results showed that protic solvents can be useful co-solvents in aliphatic 18F-fluorinations, especially in the labelling of sulfonate esters. Aromatic 18F-fluorination was not promoted in tert-alcohols. Sensitivity of the ion trap MS was sufficient for the qualitative analysis of the 18F-labelled products; p-[18F]MPPF was identified from the isolated product fraction with a mass-to-charge (m/z) ratio of 435 (i.e. protonated molecule [M+H]+). [18F]beta-CFT-FP was produced most efficiently via [18F]fluoropropyl tosylate, leading to sufficient radiochemical yield and specific radioactivity for PET studies. The ex vivo studies in rats showed fast kinetics as well as the specific uptake of [18F]beta-CFT-FP to the DAT rich brain regions. Thus, it was concluded that [18F]beta-CFT-FP has potential as a radiotracer for imaging DAT by PET.

A LOWER INITIAL ABUNDANCE OF SHORT-LIVED Ca-41 IN THE EARLY SOLAR SYSTEM AND ITS IMPLICATIONS FOR SOLAR SYSTEM FORMATION

The short-lived radionuclide Ca-41 plays an important role in constraining the immediate astrophysical environment and the formation timescale of the nascent solar system due to its extremely short half-life (0.1 Myr). Nearly 20 years ago, the initial ratio of Ca-41/Ca-40 in the solar system was determined to be (1.41 +/- 0.14) x 10(-8), primarily based on two Ca-Al-rich Inclusions (CAIs) from the CV chondrite Efremovka. With an advanced analytical technique for isotopic measurements, we reanalyzed the potassium isotopic compositions of the two Efremovka CAIs and inferred the initial ratios of Ca-41/Ca-40 to be (2.6 +/- 0.9) x 10(-9) and (1.4 +/- 0.6) x 10(-9) (2 sigma), a factor of 7-10 lower than the previously inferred value. Considering possible thermal processing that led to lower Al-26/Al-27 ratios in the two CAIs, we propose that the true solar system initial value of Ca-41/Ca-40 should have been similar to 4.2 x 10(-9). Synchronicity could have existed between Al-26 and Ca-41, indicating a uniform distribution of the two radionuclides at the time of CAI formation. The new initial Ca-41 abundance is 4-16 times lower than the calculated value for steady-state galactic nucleosynthesis. Therefore, Ca-41 could have originated as part of molecular cloud materials with a free decay time of 0.2-0.4 Myr. Alternative possibilities, such as a last-minute input from a stellar source and early solar system irradiation, could not be definitively ruled out. This underscores the need for more data from diverse CAIs to determine the true astrophysical origin of Ca-41.

Interpreting the environmental record in the sediments of Blelham Tarn

Two aspects of the environmental record in the sediments of Blelham Tarn have been investigated: (1) the ecological history of the catchment, and lake-catchment relationships, by detailed analysis of the preserved pollen (as an indication of vegetation) and sediment composition with respect to a range of inorganic and organic geochemical variables and (2) a detailed investigation of the manner in which sediment is being formed today, including the way in which microfossils (pollen and diatoms) are being recruited and incorporated into sediments. When the record was examined by biological and geochemical analysis, together with radionuclide dating, of closely spaced samples, it was found that the changes of the last 30 yrs represented only the most recent episode in a long history of modification of the lake by man. To find an approach to this it is necessary to go back for at least 2500 yrs.

Construção e automação de um mapa de vulnerabilidade de solos ao 137Cs.

O comportamento dos radionuclídeos no solo pode variar de acordo com sua interação com os elementos que compões este solo. O fator de transferência (FT) é o parâmetro que descreve a interação que ocorre entre o solo e as plantas para um determinado radionuclídeo, observando que este solo tem propriedades químicas e físicas que favorecem seu crescimento. Através de ferramentas computacionais e baseado em solos extremos, com o FT conhecidos na literatura e nos parâmetros de solo que interferem no comportamento de 137Cs (como K trocável, capacidade de troca catiônica e pH), este trabalho visa aplicar técnicas de geoprocessamento para a criação de um mapa de vulnerabilidade de solos ao 137Cs e sua automação. Este estudo mostra que o uso de técnicas de geoprocessamento visando o mapeamento da vulnerabilidade ao 137Cs pode ser uma ferramenta importante para o planejamento de ações de emergência em áreas rurais, a identificação de áreas risco à contaminação radioativa, na escolha de ações corretivas adequadas, bem como no suporte a criação de políticas públicas.

Hardware reconfigurável para identificação de radionuclídeos utilizando o método de agrupamento subtrativo.

Fontes radioativas possuem radionuclídeos. Um radionuclídeo é um átomo com um núcleo instável, ou seja, um núcleo caracterizado pelo excesso de energia que está disponível para ser emitida. Neste processo, o radionuclídeo sofre o decaimento radioativo e emite raios gama e partículas subatômicas, constituindo-se na radiação ionizante. Então, a radioatividade é a emissão espontânea de energia a partir de átomos instáveis. A identificação correta de radionuclídeos pode ser crucial para o planejamento de medidas de proteção, especialmente em situações de emergência, definindo o tipo de fonte de radiação e seu perigo radiológico. Esta dissertação apresenta a aplicação do método de agrupamento subtrativo, implementada em hardware, para um sistema de identificação de elementos radioativos com uma resposta rápida e eficiente. Quando implementados em software, os algoritmos de agrupamento consumem muito tempo de processamento. Assim, uma implementação dedicada para hardware reconfigurável é uma boa opção em sistemas embarcados, que requerem execução em tempo real, bem como baixo consumo de energia. A arquitetura proposta para o hardware de cálculo do agrupamento subtrativo é escalável, permitindo a inclusão de mais unidades de agrupamento subtrativo para operarem em paralelo. Isso proporciona maior flexibilidade para acelerar o processo de acordo com as restrições de tempo e de área. Os resultados mostram que o centro do agrupamento pode ser identificado com uma boa eficiência. A identificação desses pontos pode classificar os elementos radioativos presentes em uma amostra. Utilizando este hardware foi possível identificar mais do que um centro de agrupamento, o que permite reconhecer mais de um radionuclídeo em fontes radioativas. Estes resultados revelam que o hardware proposto pode ser usado para desenvolver um sistema portátil para identificação radionuclídeos.

Influência de um extrato aquoso de Coriandrum sativum na marcação in vitro de constituintes sanguíneos com tecnécio-99m e de sua associação com vibração gerada por plataforma oscilante na biodistribuição do radiofármaco Na99mTcO4 e na concentração de biomarcadores em ratos Wistar

Coriandrum sativum, conhecido popularmente como coentro, é um vegetal usado na alimentação humana. Também é utilizado como planta medicinal para tratamento de diabetes, complicações gastrintestinais, e como um antiedêmico, antisséptico e emenagogo. Em investigações acerca dos efeitos do extrato de plantas, é importante a determinação de alguns parâmetros físico-químicos. Diversos modelos experimentais têm sido usados, inclusive com o emprego de radionuclídeos. Em procedimentos da Medicina Nuclear que auxiliam o diagnóstico de doenças, o tecnécio-99m (99mTc) é o radionuclídeo mais utilizado. Hemácias marcadas com 99mTc estão entre as várias estruturas celulares que podem ser marcadas com este radionuclídeo e usadas como radiofármaco. Para a marcação com 99mTc é necessária a presença de um agente redutor, e o mais utilizado é o cloreto estanoso (SnCl2). As terapias com drogas e condições de dieta além de doenças podem alterar a marcação de constituintes sanguíneos, bem como a biodistribuição de diferentes radiofármacos. A exposição às vibrações geradas por plataforma oscilatória produz exercícios de corpo inteiro. O objetivo deste estudo foi caracterizar a preparação de um extrato do Coriandrum sativum, através de parâmetros físico-químicos, verificar os efeitos desse produto natural na radiomarcação de constituintes sanguíneos e em associação à vibração gerada pela plataforma na biodistribuição de Na99mTcO4 e na concentração de alguns biomarcadores. O extrato de coentro teve a o pico de absorbância em 480 nm. O extrato de coentro foi inversamente correlacionado com a concentração na condutividade elétrica. Foi encontrado o maior valor de pH na menor concentração do extrato (0,5 mg/mL). Não houve uma alteração significativa na marcação de constituintes sanguíneos com 99mTc. E a associação do extrato de coentro e vibração gerada por plataforma com frequência de 12 Hz teve efeito no baço, como observado na fixação do radiofármaco nesse órgão e ação em alguns órgãos alternando a concentração de alguns biomarcadores. Em conclusão, parâmetros físico-químicos podem ser úteis para caracterizar o extrato estudado. Provavelmente, as propriedades redox associadas com substâncias desse extrato podem ser os responsáveis pela ausência do efeito na radiomarcação de constituintes sanguíneos. A determinação da captação do Na99mTcO4 em diferentes órgãos permite verificar que o extrato de coentro sozinho não foi capaz de interferir na biodistribuição do radiofármaco. Contudo o tratamento de animais com vibração gerada pela plataforma alterou significativamente a fixação do pertecnetato de sódio no baço e a concentração do colesterol, triglicerídeo, CK e bilirrubina.

Avaliação do impacto radiológico atmosférico de uma unidade de mineração e beneficiamento de urânio

Este trabalho teve como objetivo avaliar o impacto radiológico atmosférico da Unidade de Concentrado de Urânio URA, Caetité, BA, através da modelagem da dispersão de radionuclídeos e a estimativa da dose efetiva anual (em mSv.ano-1). Para tal, utilizou-se o programa MILDOS-AREA que foi desenvolvido pelo Argonne National Laboratory (ANL) em conjunto com a U.S. Nuclear Regulatory Commission (USNRC), para avaliar impacto radiológico ambiental atmosférico nas instalações de mineração e beneficiamento de urânio. O incremento de dose efetiva anual para três grupos críticos hipotéticos e oito grupos populacionais reais foi estimado com base na medida de fluxos de radônio e na estimativa das concentrações de radionuclídeos em particulados no ar dos principais termos fontes da URA (cava da mina, depósito de estéril e britador). Paralelamente, as medidas de concentração de radônio e taxa de kerma no ar, reportadas nos relatórios dos programas de monitoração ambiental pré-operacional (PMAPO) e operacional (PMAO) da URA, foram avaliadas. Os valores de dose efetiva anual estimados para os grupos críticos hipotéticos variaram de 1,78E-02 a 2,10E-02 mSv.ano-1, enquanto que para os grupos populacionais, variaram de 7,49E-05 a 1,56E-02 mSv.ano-1. A maior contribuição para o incremento da dose foi devida a inalação do radônio, sendo responsável por quase a totalidade da dose efetiva anual estimada. A média da concentração de atividade de radônio no entorno da URA foi 137,21 Bq m-3 e não sendo observada diferenças significativas entre as concentrações de radônio reportadas nos programas de monitoramento ambiental pré-operacional (valores de background) e operacional. Os valores médios de taxa de kerma no ar no entorno da URA foram de 0,136 μGy h-1. No entanto, em todos os pontos de monitoramento, os valores reportados no programa operacional foram inferiores aos valores reportados no programa pré-operacional (background), o que sugere problemas de medidas ou de coleta de dados durante a realização deste programa. O operador da URA utilizou para avaliação de impacto radiológico atmosférico, resultados apresentados em seus relatórios finais de análise de segurança (RFAS), um modelo próprio de simulação de dispersão, denominado Impacto Ambiental Radiológico (IAR7). Uma comparação entre o MILDOS-AREA e o IAR7, utilizando os mesmos parâmetros de entrada reportados no RFAS sugere que o IAR7 subestimou as concentrações de radônio no ar para os grupos críticos hipotéticos. Os resultados de simulação com o MILDOS-AREA mostram que as doses efetivas estimadas para os grupos críticos hipotéticos são inferiores a 0,3 mSv.ano-1 que é a restrição de dose estabelecida pela Comissão Nacional de Energia Nuclear. Recomenda-se que o código MILDOS-AREA seja utilizado no Brasil, para fins de licenciamento e controle, tendo em vista que o mesmo é um código validado e já utilizado em outros países para avaliar impacto radiológico ambiental atmosférico em instalações de mineração e beneficiamento de urânio

PICES Press, Vol. 21, No. 2, Summer 2013

•The 2013 Inter-sessional Science Board Meeting: A Note from the Science Board Chairman (pp. 1-4) •ICES/PICES Workshop on Global Assessment of the Implications of Climate Change on the Spatial Distribution of Fish and Fisheries (pp. 5-8) •PICES participates in a Convention on Biological Diversity Regional Workshop (pp. 9-11) •Social and Economic Indicators for Status and Change within North Pacific Ecosystems (pp. 12-13) •The Fourth International Jellyfish Bloom Symposium (pp. 14-15) •Workshop on Radionuclide Science and Environmental Quality in the North Pacific (pp. 16-17) •PICES-MAFF Project on Marine Ecosystem Health and Human Well-Being: Indonesia Workshop (pp. 18-19) •Socioeconomic Indicators for United States Fisheries and Fishing Communities (pp. 20-23) •Harmful Algal Blooms in a Changing World (pp. 24-25, 27) •Enhancing Scientific Cooperation between PICES and NPAFC (pp. 26-27) •Workshop on Marine Biodiversity Conservation and Marine Protected Areas in the Northwest Pacific (pp. 28-29) •The State of the Western North Pacific in the Second Half of 2012 (pp. 30-31) •Stuck in Neutral in the Northeast Pacific Ocean (pp. 32-33) •The Bering Sea: Current Status and Recent Trends (pp. 34-36) •For your Bookshelf (p. 37) •Howard Freeland takes home Canadian awards (p. 38)

The production of radionuclides for nuclear medicine from a compact, low-energy accelerator system.

The field of nuclear medicine is reliant on radionuclides for medical imaging procedures and radioimmunotherapy (RIT). The recent shut-downs of key radionuclide producers have highlighted the fragility of the current radionuclide supply network, however. To ensure that nuclear medicine can continue to grow, adding new diagnostic and therapy options to healthcare, novel and reliable production methods are required. Siemens are developing a low-energy, high-current - up to 10MeV and 1mA respectively - accelerator. The capability of this low-cost, compact system for radionuclide production, for use in nuclear medicine procedures, has been considered.