Natural Radionuclide Contents in Human Whole-Body Ashes

Whole-body ashes from nine cremated adult humans were acquired from local mortuaries in Ft. Collins, Colorado (USA) with the consent of next of kin. Ashes of each individual corpse were ground, homogenized and sealed in a steel can for 30 days before gamma-spectroscopy measurements were made to determine the ²²⁸Ra, ²²⁸Th, ²³⁸U, ²²⁶Ra and ⁴⁰K contents. The median values of radionuclide contents in our study subjects were generally higher than literature values in which only a selected set of organs had been analyzed. Direct estimates of natural or man-made radionuclides in whole-body human ashes should be more accurate than estimates based on analysis of small bone or tissue samples that require extrapolation to the entire body.     

Evaluation by using radionuclide uptake of bone in Paget's disease of bone: special reference to treatment with calcitonin

Bone scintigraphy using 99mTc-MDP was performed on 2 patients with Paget's disease of bone before and after the treatment with a synthetic eel calcitonin analogue [Asu1,7)-eel calcitonin, ECT] at a dose of 40 U per day. All pagetic lesions showed markedly the increased accumulation of the radionuclide. The uptake ratio, defined as the count rate of 99mTc-MDP over each bone lesion to that over the control bone, was calculated. The response to the calcitonin therapy was evaluated with the uptake ratio of the radionuclide. The uptake ratio decreased markedly within the first 3 months of the treatment, in association with a palliation of bone pain, while the serum alkaline phosphatase activities which had been within the normal range or slightly high before the treatment did not show any significant change or did not reflect a clinical feature (e.g. bone pain) with the treatment. Thus, the uptake ratio on the bone scintigram seemed to offer the most sensitive and most reliable information for the evaluation of calcitonin treatment of Paget's disease of bone.     

Determination of the in vitro dissolution rates of 238U, 230Th, and 231Pa in contaminated soils from the St. Louis FUSRAP sites

The dissolution rates for ²³⁸U, ²³⁰Th, and ²³¹Pa from 8 contaminated soils in simulated lung fluid were determined. The soil samples were provided by the US Army Corps of Engineers and were collected from various areas at their St. Louis, Missouri FUSRAP sites. Each soil was subjected to a 100 day in vitro dissolution experiment, during which the amount of each radionuclide that had dissolved was periodically measured. At the conclusion of the experiment, a plot of the relative amount of radionuclide dissolved vs. time was constructed for each radionuclide in each soil. The dissolution rates for each radionuclide were then determined by fitting multiple first-order exponential functions to each plot. The results of these experiments were then used assign in vitro dissolution rate classifications to each radionuclide in each soil according to ICRP 30 guidelines.     

Paper chromatographic and paper elettrophoretic study of the solution chemistry of Tc-99m-methylendiphosphonate and of Tc-99m-dimercaptosuccinate for improving the tumour-affinity of Tc-99m during scintigraphic imaging of cancer

In order to find the conditions under which Tc-99m-methylenediphosphonate (Tc-99m-MDP) and Tc-99m(V)-dimercaptosuccinate (Tc-99m(V)-DMSA) may become tumour-seeking agents, leaving healthy organs free from the radionuclide uptake, the solution chemistry of these radiopharmaceuticals was studied by paper chromatography and paper electrophoresis in distilled water, in physiological saline, in NAHCO3, and ascorbic acid solutions. Both radiopharmaceuticals are anionic in the radiopharmaceutical solution but get easily hydrolysed to form cationic Tc-99m species which concentrates in healthy bone and in some bone metastases. Tc-99m (V)-DMSA being more stable remains long in the blood pool giving undesirable presence of the radionuclide in lung, heart and kidneys, in addition to its reduced uptake in bone metastases and in some primaries. We are trying to eliminate these drawbacks of healthy organ uptake of Tc-99-m(V)-DMSA not only to get a clean scintigraphic image of the tumour with this radiopharmaceutical but to extend its formulation, thus obtained, to prepare radiopharmaceutical with Re-188, which is the higher homologue of Tc-99m, for systemic therapy of cancer. Essentially similar solution chemistry of both radiopharmaceuticals suggests that like Tc-99m-MDP, technetium-99m-dimercaptosuccinate is also a complex of tetravalent Tc-99m and not of pentavalent Tc-99m as so far supposed to be.     

Electron charge redistribution following electrophilic attack on heterocycles: nitrogen as a charge transducer

It is shown that an electrophilic attack on the ring nitrogen in pyrrole or tryptamine produces an electron charge redistribution that is qualitatively different from the redistribution caused by an attack on the oxygen in furan. The electrophilic attacks are represented theoretically as interactions with a positive point charge and calculated by an ab-initio LCAO-SCF method with gaussian basis sets. Results show that an attacked nitrogen responds to the perturbation by moving electronic charge to the adjacent carbons whereas oxygen retains most of the charge polarized by the interaction. The nitrogen also acts as a charge transducer in other systems that are structurally very different. As a consequence of the charge redistribution, the comparative susceptibility of various sites in the heterocyclic molecules to an electrophilic attack may also depend on the response of the molecule to a prior attack on the heteroatom. The results indicate the need for dynamical reactivity considerations which reflect the variability in the molecular response to an incipient attack and the possibility that enhanced reactivity can be induced at certain sites by this response.     

(212)Pb@C(60) and its water-soluble derivatives: synthesis, stability, and suitability for radioimmunotherapy

Fullerenes could potentially play a valuable role in radioimmunotherapy by more stably encapsulating radionuclides, especially where conventional chelation chemistry is inadequate due to the physical and/or chemical properties of the radionuclide. One of the therapeutically useful radionuclides that requires improved containment in vivo is 212Pb (tau1/2 = 10.6 h), the beta-emitting parent to alpha-emitting 212Bi (tau1/2 = 60.6 min). Myelotoxicity resulting from the accumulation of 212Pb in the bone marrow has limited the use of this radionuclide despite its favorable decay characteristics. In this work, 212Pb@C60 and its malonic ester derivatives were prepared for the first time by allowing the 212Pb to recoil into C60 following alpha-decay from its parent, 0.15-s 216Po, generated in situ from the decay of 224Ra (tau1/2 = 15 days). Repeated washing of the organic phase containing the 212Pb@C60 malonic esters with challenge solutions containing cold Pb2+ ions demonstrated that some of the 212Pb could not be exchanged and was apparently inside of the fullerenes. Malonic esters of endohedral alpha-emitting 213Bi (tau1/2 = 45 min) fullerenes were prepared by an analogous procedure. Following acidification of the esters, a preliminary biodistribution study in mice was performed with the untargeted water-soluble radiofullerenes. It was found that 212Pb did not accumulate in bone after being administered as an endohedral fullerene, in contrast to results with polyhydroxylated radiofullerenes and conventional polyaminocarboxylate chelators for 212Pb. The results indicate that 212Pb is held more tightly in the fullerene than in other methods and suggest that fullerenes may have an important role in the targeted delivery of 212Pb.     

Bioassay of 210Po in human urine and internal contamination of man

The deliberate poisoning of A. Litvinenko in London in late 2006 with ²¹⁰Po, attracted attention to the difficulties in identifying internal contamination with alpha emitting radionuclides and to the limited knowledge available on the cycling of many naturally occurring radioisotopes in the body and their baseline concentration values in humans. To cope with the emergency caused by the spread of high ²¹⁰Po activity, which contaminated several people and places in London, we were called upon to analyze urine samples in potentially contaminated people. A reference group of adult humans was also selected for determination of baseline ²¹⁰Po values to be used for comparative purposes. Concentrations of ²¹⁰Po in urine samples from three Portuguese citizens that have been at contaminated places, in London, ranged from 2.3 to 4.1 mBq·L⁻¹ while in the reference group ²¹⁰Po concentrations ranged from 0.5 to 4.8 mBq·L⁻¹. Analytical quality of results was ensured through participation in an international inter laboratory comparison exercise on ²¹⁰Po determination in aqueous samples. Results indicated that people potentially exposed to ²¹⁰Po in London were not internally contaminated with the radionuclide used as a poisoning agent, and the levels of this radionuclide measured in the urine were similar to the naturally occurring levels in the reference group. Polonium levels in urine and in man are discussed in the light of ²¹⁰Po levels in the human diet.     

Kinetics of 1H --> 31P NMR cross-polarization in bone apatite and its mineral standards

Kinetics of NMR cross-polarization (CP) from protons to phosphorus-31 nuclei was studied in the following samples: mineral of whole human bone, apatite prepared from bone, natural brushite, synthetic hydroxyapatite (hydrated and calcined), and synthetic carbonatoapatite of type B with 9 wt% of CO(3) (2-). In order to avoid an effect of magic angle spinning on CP and relaxation, the experiments were carried out on static samples. Parameters of the CP kinetics were discussed for trabecular and cortical bone tissue from adult subjects in comparison to the synthetic mineral standards. It was found that carbonatoapatite shows similar CP behavior to the bone mineral. Both materials undergo two-component CP kinetics. The fast-relaxing classical component is from the surface of apatite crystals and the slow-relaxing nonclassical component comes from the crystal interior. The components have been unambiguously assigned using inverse CP from phosphorus-31 to protons. The study provides information on a structured water layer, which covers crystal surface of carbonato- and bone apatite. The layer encompasses ca 40% of apatite phosphorus and its thickness is more than ca 2 nm.     

Analyses of radionuclides in soil,water, and agriculture products near the Urgeiriça uranium mine in Portugal

Analyses of soils, irrigation waters, agriculture products (lettuce), green pasture, and cheese were performed in samples collected in the area of the old Urgeiriça uranium mine and milling facilities, Centre-North of Portugal, in order to assess the transfer of uranium series radionuclides in the environment and to man. Soils close to milling tailings display an enhancement of radioactivity. In the drainage basin of the stream Ribeira da Pantanha, receiving drainage from the tailings piles and discharges from the acid mine water treatment plant, there was enhancement of uranium series radionuclide concentrations in water and suspended matter. Agriculture products from kitchen gardens irrigated with water from the Ribeira da Pantanha show an increase of radioactivity, mainly due to uranium isotopes. Agriculture products from other kitchen gardens in this area, irrigated with groundwater, as well pasture and cheese produced locally from sheep milk did not show enhanced radionuclide concentrations. In the Urgeiriça area, some soils display radionuclide concentrations higher than soils in reference areas and, in agriculture products grown there, ²²⁶Ra was the radionuclide more concentrated by vegetables. Through ingestion of these products ²²⁶Ra may be the main contributor to the increment of radiation dose received by local population.     

Evaluation of matrix-assisted laser desorption ionization mass spectrometry for studying the sec-butyllithium and n-butyllithium initiated ring-opening polymerization of hexamethylcyclotrisiloxane (D3)

Matrix assisted laser desorption ionization (MALDI) was used to study the organolithium initiated ring-opening polymerization of hexamethylcyclotrisiloxane (D3) in a mixed solvent system. The mass spectral peak intensities were monitored to determine the effects of polymerization time, initiator concentration, and reaction temperature on the formation of the mono, di, and trisiloxanolate initiator species and the extent of chain redistribution. The three initiator species were formed by reacting n-butyllithium and sec-butyllithium with D3 in nonpolar solvent. The mass spectral results showed that sec-butyllithium and n-butyllithium form different populations of initiator species under the same conditions and that the measured mass spectral peak intensities do not accurately represent the population of siloxanolate initiator species prior to propagation. The changes in peak intensities were attributed to chain redistribution.     

Major-to-ultratrace elements in bone-marrow fluid as determined by ICP-AES and ICP-MS.

The major-to-ultratrace elements in human bone-marrow fluid were determined by ICP-AES (inductively coupled plasma atomic emission spectrometry), and ICP-MS (inductively coupled plasma mass spectrometry). The bone-marrow fluid sample was centrifuged prior to acid digestion to exclude the bone piece from bone marrow, and then digested with nitric acid. As a result, 20 elements could be determined over the concentration range from 1610 microg g(-1) for Na to 0.00043 microg g(-1) for W. It was found that Fe, Zn and Sb were enriched by ca. 264-, 7- and 15-fold, respectively, in bone-marrow fluid, compared to those in human blood serum. Alkali metals (K, Rb, Cs), except for Na, were also significantly enriched in bone-marrow fluid. Furthermore, the concentrations of various elements, such as Fe, P, Al, Zn, Cu, Se, Zr, Sn, Ag and W, were significantly higher than those in open seawater.     

A Bayesian approach to assess data from radionuclide activity analyses in environmental samples

A Bayesian statistical approach is introduced to assess experimental data from the analyses of radionuclide activity concentration in environmental samples (low activities). A theoretical model has been developed that allows the use of known prior information about the value of the measurand (activity), together with the experimental value determined through the measurement. The model has been applied to data of the Inter-laboratory Proficiency Test organised periodically among Spanish environmental radioactivity laboratories that are producing the radiochemical results for the Spanish radioactive monitoring network. A global improvement of laboratories performance is produced when this prior information is taken into account. The prior information used in this methodology is an interval within which the activity is known to be contained, but it could be extended to any other experimental quantity with a different type of prior information available.     

Développement et validation d'un modèle mécanique de la tête humaine

This paper presents the development and the validation of a 3D finite-element human head model intended to better understand the head injury mechanisms in case of head impact. A very realistic skull geometry has been obtained by digitalisation of a dry adult skull. Based on the established knowledge of bone mechanical properties, an elastic brittle law was attributed to the skull simulated by composite shell elements. The dynamical model response was compared with two experimental impact tests from the bibliography concerning epidural pressure and a third impact involving skull fracture. The results of the model validation appear promising and the model could be a powerful tool to predict the aggressiveness level of a head impact.     

The dose-effect of icariin on the proliferation and osteogenic differentiation of human bone mesenchymal stem cells

Icariin had been reported as a potential agent for osteogenesis, but the dose-effect relationship needed further research to realize the clinical application of icariin. We isolated and purified human bone mesenchymal stem cells (hBMSCs) and stimulated them with different concentrations of icariin. The cytotoxicity of icariin was evaluated by the methylthiazolytetrazolium (MTT) assay method. The proliferation and osteogenic differentiation of such hBMSCs were investigated for different concentrations of icariin. We found that icariin had a dose-dependent effect on the proliferation and osteogenic differentiation of hBMSCs in a suitable concentration range from 10(-9) M to 10(-6) M, but at concentrations above 10(-5) M, the cytotoxicity limited its use. The extremely low cost of icariin and its high abundance make it appealing for bone regeneration.     

Two Approaches for Sequential Extraction of Radionuclides in Soils: Batch and Column Methods

Abstract

A three-step sequential extraction protocol designed by Community Bureau of Reference (BCR) is applied to two types of soil (sandy and sandy-loam) which had been previously contaminated with a radionuclide aerosol containing ¹³⁴Cs, ⁸⁵Sr and ^110mAg. This scheme is applied using both batch and column methods. The radionuclide distribution obtained with this scheme depends both on the method and on soil type. Compared with the batch method, column extraction is an inadvisable method. Kinetic aspects seem to be important, especially in the first and third fractions. The radionuclide distribution shows that radiostrontium has high mobility, radiocaesium is highly retained by clay minerals whereas Fe/Mn oxides and organic matter have an important role in radiosilver retention.     

Fall out and radionuclide analysis on the Pratas Island in South China Sea

The radionuclide concentration in environmental samples and radiation level on Pratas Island are measured prior to the commercial operation of Da-Ya Bay Nuclear Power Plant nearby. Except for some minute amount of⁶⁰Co and¹⁵⁷Cs, radiation background is mainly from naturally occurring radionuclides. Automatic radiation surveillance and a routine sampling program on Pratas Island are essential to provide early warning for Taiwan in case of nuclear emergency.     

Nanomaterial-based adsorbents: the prospect of developing new generation radionuclide generators to meet future research and clinical demands

Nanostructured materials by virtue of huge surface to volume ratios, altered physical properties, tailored surface chemistry, favorable adsorption characteristics, and enhanced surface reactivity resulting from the nanoscale dimensions, have attracted considerable attention as a new class of adsorbent material in column chromatographic separation. This emerging class of adsorbent represents an innovative paradigm and is expected to play an important role in the development of radionuclide generators for nuclear medicine. The optimal combination of suitable nanomaterial and appropriate parent/daughter radionuclide pair forms the basis of such generators. Development of such generators is currently under intensive investigations and the utility of such systems is expected to pave the way for broad panoply of diagnostic and therapeutic applications in nuclear medicine. While nanomaterial-based radionuclide generator is still in its infancy, the use of such novel class of adsorbents is expected to have potential impact on shaping the radionuclide generator technology of future generation. This review provides a comprehensive summary on the utility of nanomaterials as effective adsorbents in the development column chromatographic radionuclide generators for medical applications. This overview outlines a critical assessment of role of the nanosorbents, recent developments, the contemporary status, and key challenges and apertures to the near future.     

Charge redistribution and photoacidity: neutral versus cationic photoacids

A series of pyrene photoacids is used to investigate excited-state proton transfer with time-dependent pump-probe spectroscopy. The deprotonation dynamics of a cationic photoacid, 8-aminopyrene-1,3,6-trisulfonic acid trisodium salt (APTS), shows single exponential dynamics( approximately 30 ps) in water. This is in contrast to what is observed for the neutral photoacids 8-hydroxypyrene-1,3,6-trisulfonic acid trisodium salt (HPTS) and 8-hydroxy-N,N,N',N',N",N"-hexamethylpyrene-1,3,6-trisulfonamide, which display biexponential dynamics. For the cationic photoacid, the vast majority of the intramolecular charge redistribution does not occur in the protonated state. Instead, the charge redistribution, which is responsible for the photoacidity and the observed spectroscopic changes, occurs primarily following the excited-state proton transfer. The lack of charge redistribution prior to proton transfer causes APTS to display single exponential kinetics. In contrast, the dynamics for the neutral photoacids are multiexponential because major charge redistribution precedes proton transfer followed by additional charge redistribution that accompanies proton transfer. Previous studies of HPTS in water are discussed in terms of the results presented here.     

Integration exosomes with MOF-modified multifunctional scaffold for accelerating vascularized bone regeneration

Designing a multifunctional scaffold with osteogenic and angiogenic properties holds promise for ideal bone regeneration. Innovative scaffold was here constructed by immobilizing exosomes derived from human bone mesenchymal stem cells (hBMSCs) onto porous polymer meshes which developed by PLGA and Cu-based MOF (PLGA/CuBDC@Exo). The synthesized exosome-laden scaffold capable of providing a dual cooperative controllable release of bioactive copper ions and exosomes that promote osteogenesis and angiogenesis, thereby achieving cell-free bone regeneration. In vitro assay revealed the composite stent not only substantially upregulated the expression of osteogenic-related proteins (ALP, Runx2, Ocn) and VEGF in hBMSCs, but promoted the migration and tube formation of the human umbilical vein endothelial cells (HUVECs). In vivo evaluation further confirmed this scaffold dramatically stimulated bone regeneration and angiogenesis in critical-sized defects in rats. Altogether, this composite scaffold carrying therapeutic exosomes had an osteogenic-angiogenic coupling effect and offered a new idea for cell-free bone tissue engineering.     

Application of the nuclide identification system SHAMAN in monitoring the Comprehensive Test Ban Treaty

SHAMAN is an expert system for qualitative and quantitative radionuclide identification in gamma spectrometry. SHAMAN requires as input the calibrations, peak search, and fitting results from reliable spectral analysis software, such as SAMPO. SHAMAN uses a comprehensive reference library with 2600 radionuclides and 80 000 gamma-lines, as well as a rule base consisting of sixty inference rules. Identification results are presented both via an interactive graphical interface and in the form of configurable text reports. An organization has been established for monitoring the recent Comprehensive Test Ban Treaty. For radionuclide monitoring, 80 stations will be set up around the world. Air-filter gammaspectra will be collected from these stations on a daily basis and they will need to be reliably analyzed with minimum turnaround time. SHAMAN is currently being evaluated within the prototype monitoring system as an automated radionuclide identifier, in parallel with existing radionuclide identification software. In air-filter monitoring, very low concentrations of radionuclides are measured from bulky sources in close geometry and with long counting time. In this case true coincidence summing and self-absorption become important factors. SHAMAN is able to take into account these complicated phenomena, and the results it produces have been found to be very reliable and accurate.