Este trabalho apresenta o levantamento de parâmetros para implementação adequada e segura de pisos, portas, janelas, bancadas, capelas entre outros, de um laboratório radioquímico. A disposição de cada item segue orientações de guias, normas nacionais da Comissão Nacional de Energia Nuclear (CNEN) e internacional da Agencia Internacional de Energia Atômica (IAEA), com objetivo de garantir a proteção radiológica do trabalhador e do ambiente. A disposição adequada dos itens do laboratório radioquímico, garante a qualidade e segurança na produção de fontes radioativas seladas de 57Co 137Cs e 133Ba com atividades 185, 9.3 e 5.4 MBq respectivamente. Estas fontes são utilizadas na verificação de medidores de atividade, equipamento que todo Centro de Medicina Nuclear deve ter disponível segundo recomendações da norma CNEN-NN-3.05 Requisitos de Radioproteção e Segurança para Serviços de Medicina Nuclear para verificação da atividade de radiofármacos que serão administrados nos pacientes para fins de diagnóstico e terapia. Um medidor de atividade fora adquirido pelo laboratório de produção de fontes, com o qual foram realizados os testes de precisão, exatidão, reprodutibilidade e linearidade, que devem apresentar resultados dentro dos limites estabelecidos na norma CNEN-NN-3.05. / This paper presents a survey of parameters for the proper and safe flooring, doors, windows, fume hoods and others, in a radiochemical laboratory. The layout of each item follows guidelines and national standards of the National Commission of Nuclear Energy (CNEN) and the International Atomic Energy Agency (IAEA), aiming to ensure the radiological protection of workers and environment. The adequate items arrangement in the radiochemical laboratory ensures quality and safety in the production of 57Co 137Cs and 133Ba radioactive sealed sources, with activities 185, 9.3 and 5.4 MBq, respectively. These sources are used to verify meter activity equipment and should be available throughout the Nuclear Medicine Center, following the recommendations of CNEN-NN-3.05 standard \"Requirements for Radiation Protection and Safety Services for Nuclear Medicine\", to verify the activity of radiopharmaceuticals that are administered in patients, for diagnosis and therapy.

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Three lateritic profiles from different localities and of varying depth and degrees of development were analyzed for precious metals, platinum, palladium, iridium and gold by radiochemical neutron-activation analysis. In addition, the distribution of major, minor and other trace constituents (iron, silicon, magnesium, nickel, cobalt, chromium, copper, manganese, zinc, uranium, sodium, chlorine and scandium) was determined. Instrumental activation analysis, radiochemical analysis and conventional chemical procedures were used. The mineralogy of the samples was studied using electron microscopy. Sufficient analytical data were obtained to justify the use of molecular proportions and net changes plots, and a coefficient correlation method, in order to elucidate the geochemical behaviour of the elements during the weathering processes.

Radionuclides from natural U-series in sediments from two river catchments in the UK have been studied. The aim was to gain insight into the behaviour of 238U, 234U, 230Th and 226Ra in real natural systems enriched in uranium. A radiochemical method for radium separation followed by alpha spectrometric measurement has been developed. The method allowed use of 225Ra, in equilibrium with the parent 229Th, as a yield determinant, and has been applied in 226Ra concentrations measurements in the selected areas of study.U-series progeny, 238U, 234U, 230Th and 226Ra, in totally dissolved sediments from the valley of the River Noe and the fraction leached by aqua regia, have been measured. Total sediment contents ranged from 9 ± 2 to 184 ± 8 Bq.kg-1 for uranium, 9 ± 3 to 200 ± 13 Bq.kg-1 for thorium and 18 ± 1 to 179 ± 8 Bq.kg-1 for radium. The activity concentrations in the leached fractions, compared with the total, were 46% for uranium, 54% for thorium and 56% for radium, on average. The radionuclides showed extensive disequilibrium and this suggested a complex leaching/accumulation of uranium as well as an impact of organic matter and secondary minerals.Uranium and radium have been geochemically characterised in sediments from near the South Terras abandoned uranium mine, Cornwall. Background activity concentration levels of uranium in sediments ranged from 13 ± 3 to 290 ± 14 Bq.kg-1, with radium from 42 ± 4 to 424 ± 23 Bq.kg-1. Elevated concentrations of uranium and radium were measured in two samples, S3 with 1820 ± 36 Bq.kg-1 for uranium and 940 ± 53 Bq.kg-1 for radium; and S7 with 4350 ± 53 Bq.kg-1 for uranium and 1765 ± 48 Bq.kg-1 for radium. Sequential chemical extraction for the two samples revealed that both uranium and radium were associated with organic and carbonate fractions, with 25 % of the uranium in the resistant phase of S7. 234U/238U activity ratios of the sequential extraction fractions showed different trends in the sediments, and this was linked to the impact of organic matter and/or exchange between water and sediment. Uranium-bearing minerals in association with potassium, calcium, iron, manganese and arsenic have been identified in these sediments.

Cette travail été réalisée dans le cadre de la Projet LignoStarch ANR CP2D pour connaître les différents phénomènes induite par rayonnement ionisants dans les mélanges de l'amidon et lignine au niveau moléculaire. L'amidon peut être utilisé seul ou en combinaison avec d'autres composés pour élaborer des articles biodégradables à partir de ressources renouvelables. La lignine et ses dérivés sont bons candidats pour limiter la sensibilité d'eau des matériaux à base d'amidon, mais ils ne sont pas compatibles avec des polysaccharides. Le traitement sous faisceau d'électrons est proposé comme une méthode efficace pour induire les liaisons covalentes entre les deux constituants (amidon et lignine). En comparaison avec les mélanges de départ, les propriétés des mélanges irradiés montrent qu'il est possible d'ajuster les propriétés mécaniques du matériau final. Afin d'améliorer la compréhension et la maîtrise de ces effets de l'irradiation, une étude de mélanges modèles de maltodextrines et de divers alcools ou acides aromatiques a été réalisée. Les résultats montrent une compétition entre les phénomènes de dégradation par scission et le greffage. Les analyses par CES, RMN, et MALDI-TOF permettent de mettre en évidence et de quantifier les greffages consécutifs à l'irradiation. L'exploitation par la méthode statistique proposée par Saito des données relatives à l'évolution des masses molaires et des fractions de gel dans des mélanges à base de pullulane permet d'accéder à des grandeurs quantifiant l'efficacité des deux réactions en compétition. Ainsi, les rendements radiochimiques de coupure de chaine G(S) et de pontage G(X) ont pu être calculés pour différentes quantités d'alcool cinnamique introduites dans les mélanges. Les évolutions observées rendent bien compte de la formation de gel qui n'est observée qu'en présence d'une quantité minimale d'alcool aromatique, lorsque la condition G(s) < 4 G(x) est satisfaite. Mots Clés : Amidon, Lignine, Maltodextrine, Maltotriose, Pullulane, Composés Modèles de la Lignine (Additif Aromatiques), Scission, Réticulation, Greffage, Faisceau d'Electrons, Rendements Radiochimiques de Scission G(s) et Réticulation G(x), Méthode Saito, Méthode Charlesby-Pinner. / This work was part of the LignoStarch ANR CP2D Project aimed at understanding the radiation-induced processes and mechanisms in thermoplastic starch – lignin mixture at the molecular level. Starch has the advantage of being biodegradable and agriculture based renewable resource that can be converted into a thermoplastic material with or without any additive. Lignin and its derivatives are good candidates for reducing the water sensitivity of starch based materials; however being hydrophobic in nature they are not compatible with the polysaccharides. Electron Beam radiation has been proposed as an efficient method for modifying the starch lignin blends and creating covalent linkages between the two constituents for improved blend stability. Previous studies as part of the Project have shown that the mechanical properties of the irradiated blends can be positively modified by choosing an appropriate blend composition. For a better understanding of how the properties of the blend can be tailored, an understanding of the radiation-induced processes was carried out using model blends comprising maltodextrin and different aromatic compounds having structural features of lignin monomers. The blends were analyzed using SEC, NMR, and MALDI-TOF for placing in evidence the phenomenon of radiation-induced grafting to compete with chain scission in presence of the aromatic additives. The quantification of the radiochemical yields of scission G(s) and crosslinking G(x) were carried out using the blends of pullulan polysaccharide as a function of varying amounts of aromatic additive in the blend. The methods of calculation exploited here are based on the study of radiation-induced molecular mass changes before the formation of gel as proposed by Saito and the quantification of sol-gel content for formulations resulting in gel as proposed by the Charlesby-Pinner method. The condition of gel formation G(s) < 4 G(x) is found to be valid for a certain minimum quantity of aromatic additive for high applied doses.Keywords: Starch, Lignin, Maltodextrin, Pullulan, Lignin-like Monomers (Aromatic Additives), Scission, Crosslinking, Grafting, Electron Beam, Radiochemical yields of Scission G(s) and Crosslinking G(x), Saito Method, Charlesby-Pinner Method.

Pre-detonation technical nuclear forensics techniques for research reactor spent fuel were developed in a collaborative project with Savannah River National Lab ratory. An inverse analysis method was employed to reconstruct reactor parameters from a spent fuel sample using results from a radiochemical analysis. In the inverse analysis, a reactor physics code is used as a forward model. Verification and validation of different reactor physics codes was performed for usage in the inverse analysis. The verification and validation process consisted of two parts. The first is a variance analysis of Monte Carlo reactor physics burnup simulation results. The codes used in this work are MONTEBURNS and MCNPX/CINDER. Both utilize Monte Carlo transport calculations for reaction rate and flux results. Neither code has a variance analysis that will propagate through depletion steps, so a method to quantify and understand the variance propagation through these depletion calculations was developed. The second verification and validation process consisted of comparing reactor physics code output isotopic compositions to radiochemical analysis results. A sample from an Oak Ridge Research Reactor spent fuel assembly was acquired through a drilling process. This sample was then dissolved in nitric acid and diluted in three different quantities, creating three separate samples. A radiochemical analysis was completed and the results were compared to simulation outputs at different levels ofdetail. After establishing a forward model, an inverse analysis was developed to re-construct the burnup, initial uranium isotopic compositions, and cooling time of a research reactor spent fuel sample. A convergence acceleration technique was used that consisted of an analytical calculation to predict burnup, initial 235U, and 236U enrichments. The analytic calculation results may also be used stand alone or in a database search algorithm. In this work, a reactor physics code is used as a for- ward model with the analytic results as initial conditions in a numerical optimization algorithm. In the numerical analysis, the burnup and initial uranium isotopic com- positions are reconstructed until the iterative spent fuel characteristics converge with the measured data. Upon convergence of the sample’s burnup and initial uranium isotopic composition, the cooling time can be reconstructed. To reconstruct cooling time, the standard decay equation is inverted and solved for time. Two methods were developed. One method uses the converged burnup and initial uranium isotopic compositions along in a reactor depletion simulation. The second method uses an isotopic signature that does not decay out of its mass bin and has a simple production chain. An example would be 137Cs which decays into the stable 137Ba. Similar results are achieved with both methods, but extended shutdown time or time away from power results in over prediction of the cooling time. The over prediction of cooling time and comparison of different burnup reconstruction isotope results are indicator signatures of extended shutdown or time away from power. Due to dynamic operation in time and function, detailed power history reconstruction for research reactors is very challenging. Frequent variations in power, repeated variable shutdown time length, and experimentation history affect the spectrum an individual assembly is burned with such that full reactor parameter reconstruction is difficult. The results from this technical nuclear forensic analysis may be used with law enforcement, intelligence data, macroscopic and microscopic sample characteristics in a process called attribution to suggest or exclude possible sources of origin for a sample.

Este trabalho consiste da preparação, caracterização e estudo do comportamento térmico dos nitrilotriacetatos de terras raras hidratados. A reação entre o cloreto de terra rara e o sal Na2HNTA, em meio aquoso, produziu compostos de fórmula geral mínima TRNTA.xH2O, onde x=2,5 para La e Ce; x=3 para Pr ao Gd (exceto o Pm) e x=4 para TR=Tb ao Lu, incluso Y. A estequiometria desses compostos foi proposta com base nos teores da terra rara, obtidos a partir das curvas TG/DTG, e nos teores de carbono, nitrogênio e hidrogênio por obtidos por análise elementar. Os difratogramas de raios X permitiram identificar três séries isomorfas, que são concordantes com a similaridade no grau de hidratação das espécies, com os espectros de absorção na região do infravermelho e com as curvas TG/DTG e DSC. Os espectros de absorção na região do infravermelho indicaram a formação dos sais, devido ao deslocamento das banda do grupo carboxilato (vCOO- de 1724 cm-1 no ácido livre, para 1670-1560 cm-1 nos sais. Os espectros de emissão do sal de EuNTA.3H2O no estado sólido, evidenciaram que o íon Eu3+ encontra-se numa microssimetria C. O comportamento térmico dos sais foi estudado por TG/DTG em atmosfera dinâmica de ar, N2 e da mistura gasosa (ar + CO2), e razão de aquecimento de 10&#176;C min-1. A decomposição térmica dos sais conduz à formação de intermediários do tipo oxicarbono e/ou dioxicarbonato e em todos os casos o produto final foi o respectivo óxido. Os eventos térmicos foram evidenciados pelas curvas DTA/DSC, por picos no sentido endotérmicos e/ou exotérmicos, e estão em concordância com as variações de massa indicadas nas curvas TG/DTG. As etapas de desidratação e da decomposição foram consideradas separadamente. Através do sistema TG/DTA-CG-MS os possíveis voláteis libertados da decomposição térmica dos sais de Na2HNTA e EuNTA.3H2O foram identificados. / This work consists of the preparation, characterization and thermal behaviour study of the hydrated rare earth nitrilotriacetates. The reaction between rare earth chloride and Na2HNTA salt, aqueous medium, produced the compounds of minimum general formula TRNTA.xH2O, where TR=La-Lu and Y, x=2,5 for La and Ce; x=3 for Pr-Gd and x=4 for Tb-Lu, Y. The stoichiometry of these compounds was proposed based in the percentages of rare earth, obtained from TG/DTG curves, and in the percentages of carbon, nitrogen and hydrogen obtained by elemental analysis. The X rays diffraction patterns allowed to identify three isomorphic series, that are concordant with the similarity in the hydration degree of the species, with infrared spectra and with TG/DTG and DSC curves. Infrared spectra indicated the formation of the salts, due to the band displacement of the carboxylate group (vCOO- of 1724 cm-1 in the free acid, to 1670-1560 cm-1 in the salts. The emission spectra of EuNTA.3H2O salt in the solid state, evidenced that the Eu3+ ion finds in a microssimetry C. The thermal behavior of salts was studied by TG/DTG in air dynamic atmospheres, N2 and of the gaseous mixture (air + CO2) and heating rate of 10&#176;C min-1. The salts thermal decomposition lead to the formation of in intermediary oxicarbonate and/or dioxicarbonate and in all cases the final product was the respective oxide. The thermal events were evidenced by DTA/DSC curves for endothermic and/or exothermic peaks, and they are in concordance with the mass variations indicated in TG/DTG curves. The dehydration and thermal decomposition steps were considered separately. Through TG/DTA-CG/MS system the volatile liberated possible of the thermal decomposition of the Na2HNTA and EuNTA.3H2O were identified.