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Lithium metatitanate, Li2TiO3, is a leading candidate for application as a tritium breeding material in a future fusion reactor. Following transmutation of lithium, the tritium must escape the crystal in order to be extracted for use in the fusion plasma. The rate-limiting step to release tritium from the Li2TiO3 pebbles is diffusion through the crystal grains. In this work, the activation barriers for tritium diffusion have been calculated using density functional theory. The results show that tritium can diffuse as an interstitial with a barrier of 0.52 eV. However, when a tritium ion becomes bound to a lithium vacancy defect, the energy required to either detrap the tritium from the vacancy or for the cluster to diffuse increases to >1 eV. Overall, these results suggest that the introduction of lithium vacancies due to Li burn-up may lead to an increase in tritium retention in the pebbles.
Nanodiamonds produced by the detonation method are used as lubricants, polishing compositions, polymer composites, etc. To reveal how nanodiamonds differ in terms of surface properties and interact with natural organic matter, we used tritium-labelled humic substances to quantitively describe their adsorption onto the nanodiamond surface. It was shown that the adsorption of humic substances onto nanodiamonds resulted in fractionation of humic substances that was strongly dependent on the zeta potential of nanodiamonds in water but did not significantly affect the uptake of nanodiamonds by wheat seedlings. The uptake of nanodiamond particles by plants was determined by the functional composition of the particle surface.
A solid phase extraction method for removing polar tritiated contaminants from tritium-containing waste oils has been developed. The composition of the degradation products present in the waste oil was determined. The results indicated that upon exposure to tritium gas, fragment methyl ketones, carboxylic acids, and lactones were the main polar products of the mineral-based oil oxidation. The nonpolar fragmentation products included n-alkanes, monomethylalkanes, and acyclic isoprenoids and were analogous to those formed during [Formula: see text]-irradiation of the oil. Various polar and nonpolar fragmentation products containing an isoprenoid skeleton were found to be formed via an oxidative/radiation scission of long-chain acyclic isoprenoids.
The human neuropeptide neuromedin S (NMS) consists of 33 amino acids. The introduction of tritium atoms into NMS has not been described so far. This represents a gap for using [3H]NMS in radioreceptor binding assays or in tracking and monitoring their metabolic pathway. Two approaches for the incorporation of tritium into NMS were explored in this study: (1) halogenation at the His-18 residue followed by catalyzed iodine-127/tritium exchange and (2) conjugation of tritiated N-succinimidyl-[2,3-3H3]propionate ([3H]NSP) to at least one of the three available primary amines of amino acids Ile-1, Lys-15, and Lys-16 in the peptide sequence. Although iodination of histidine was achieved, subsequent iodine-127/deuterium exchange was unsuccessful. Derivatization at the three possible amino positions in the peptide using nonradioactive NSP resulted in a mixture of unconjugated NSM and 1- to 3-conjugations at different amino acids in the peptide sequence. Each labeling position in the mixture was assigned following detailed LC-MS/MS analysis. After separating the mixture, it was shown in an in vitro fluorometric imaging plate reader (FLIPR) and in a competitive binding assay that the propionyl-modified NMS derivatives were comparable to the unlabeled NMS, regardless of the degree of labeling and the labeling position(s). A molecular simulation with NMS in the binding pocket of the protein neuromedin U receptor 2 (NMUR2) confirmed that the possible labeling positions are located outside the binding region of NMUR2. Tritium labeling was achieved at the N-terminal Ile-1 using [3H]NSP in 7% yield with a radiochemical purity of >95% and a molar activity of 90 Ci/mmol. This approach provides access to tritiated NMS and enables new investigations to characterize NMS or corresponding NMS ligands.
There is no doubt that estimating the exposure risk of external and internal low-dose radiation is an imperative issue in radiobiological study. Human mesenchymal stem cells (hMSCs) are multipotent and self-renewing, supporting the regeneration of damaged tissue, including tissue damaged by radiation. However, the responses of hMSCs to internal exposure to radionuclides are still insufficiently understood. In order to evaluate the adverse effects produced by internal exposure to tritiated water (HTO) at a low dose, hMSCs were exposed to 2 × 107 Bq/ml HTO, and the biological effects after the exposure were examined. Apoptosis and DNA double-strand breaks (DSBs) were assayed to analyze the cellular response to the damage induced by HTO. Slight enhancement of apoptosis was found after treatment, except at the dose of 9 mGy. The number of DSBs at 24 h post-irradiation showed that the DNA damage was able to be efficiently repaired by the hMSCs. Moreover, the increasing proportion of the cell population in S phase proved that the persistence of residual γH2AX foci at lower concentrations of HTO was attributable to the secondary production of DSBs in DNA replication. Our work adds to the available data, helping us understand the risk of stem cell transformation due to internal exposure and its correlation with low-dose radiation-induced carcinogenesis.
The safety of deep geological repositories is important in the disposal of high-level radioactive waste (HLW). In this study, advection−dispersion experiments were designed to build a transport model through a calibration/validation process, and the transport behavior of tritiated water (HTO) and various iodine species (iodide: I− and iodate: IO3−) was studied on a dynamic compacted granite column. Breakthrough curves (BTCs) were plotted under various flow rates (1−5 mL/min). BTCs showed that the non-sorption effect by anion exclusion was observed only in I− transport because the retardation factor (R) of I− was lower than that of HTO (R = 1). Moreover, equilibrium and nonequilibrium transport models were used and compared to identify the mobile/immobile zones in the compacted granite column. The anion exclusion effect was influenced by the immobile zones in the column. The non-sorption effect by anion exclusion (R < 1) was only observed for I− at 5.0 ± 0.2 mL/min flow rate, and a relatively higher Coulomb’s repulsive force may be caused by the smaller hydration radius of I−(3.31 Å) than that of IO3−(3.74 Å).
The aim of this study was to carry out a comprehensive examination of potential genotoxic effects of low doses of tritium delivered chronically to mice and to compare these effects to the ones resulting from equivalent doses of gamma-irradiation. Mice were chronically exposed for one or eight months to either tritiated water (HTO) or organically bound tritium (OBT) in drinking water at concentrations of 10 kBq/L, 1 MBq/L or 20 MBq/L. Dose rates of internal β-particle resulting from such tritium treatments were calculated and matching external gamma-exposures were carried out. We measured cytogenetic damage in bone marrow and in peripheral blood lymphocytes (PBLs) and the cumulative tritium doses (0.009 - 181 mGy) were used to evaluate the dose-response of OBT in PBLs, as well as its relative biological effectiveness (RBE). Neither tritium, nor gamma exposures produced genotoxic effects in bone marrow. However, significant increases in chromosome damage rates in PBLs were found as a result of chronic OBT exposures at 1 and 20 M Bq/L, but not at 10 kBq/L. When compared to an external acute gamma-exposure ex vivo, the RBE of OBT for chromosome aberrations induction was evaluated to be significantly higher than 1 at cumulative tritium doses below 10 mGy. Although found non-existent at 10 kBq/L (the WHO limit), the genotoxic potential of low doses of tritium (>10 kBq/L), mainly OBT, may be higher than currently assumed.
Radionuclide tritium is widely used in the nuclear energy production industry and creates a threat to human health through radiation exposure. Herein, the radioactive elimination and radioprotective effect of hydrogen-rich water (HRW), a potential antioxidant with various medical applications, on tritiated water (HTO) exposure, was studied in vitro and in vivo. Results showed that intragastric administration of HRW effectively promoted the elimination of urinary tritium, decreased the level of serum tritium and tissue-bound tritium (OBT), and attenuated the genetic damage of blood cells in mice exposed to HTO (18.5 MBq/kg). Pretreatment with HRW effectively reduces tritium accumulation in HTO-treated human blood B lymphocyte AHH-1 cells. In addition, the anti-oxidative properties of HRW could attenuate the increased intracellular ROS (such as O2•-, •OH and ONOO-), resulting in reversing the exhaustion of cellular endogenous antioxidants (reduced GSH and SOD), decreasing lipid peroxidation (MDA), relieving DNA oxidative damage, and depressing cell apoptosis and cytotoxicity induced by HTO exposure. In conclusion, HRW is expected to be an effective radioactive elimination agent through the competition effect of isotope exchange or a radioprotective agent by scavenging free radicals induced by HTO exposure.
Utilizing the energy released from the nuclear fusion of deuterium with tritium (D‑T) may be an important method of supplying energy in the future. The ionizing radiation emitted from nuclear fusion is a potential health risk to humans, including scientists who are currently performing nuclear fusion experiments and the employees of fusion nuclear plants, in the future. However, there have been few reports on the biological effects of fusion radiation. In the present study, using the High Intensity D‑T Fusion Neutron Generator, the DNA damage and its regulation in normal human fibroblasts exposed to fusion radiation were investigated. Heme oxygenase 1 (HO‑1), which is reported to induce anti‑inflammatory activity, was upregulated in the irradiated cells. Pretreatment with the HO‑1 inhibitor, protoporphyrin IX zinc (II), exacerbated double strand break formation following exposure to fusion radiation. The expression of cyclooxygenase‑2 (COX‑2) contributed to the upregulation of HO‑1, as demonstrated by the result that its inhibitor, NS‑398, inhibited the induction of HO‑1 in irradiated cells. It was further clarified that the ataxia telangiectasia mutated DNA damage response was activated and it stimulated the phosphorylation of p38 mitogen‑activated protein kinase, which was responsible for the upregulation of COX‑2 and HO‑1. These results provide novel information on fusion radiation‑induced biological effects and potential targets for decreasing the associated health risks.
Targeting toxic amyloid beta (Aβ) oligomers is currently a very attractive drug development strategy for treatment of Alzheimer´s disease. Using mirror-image phage display against Aβ1-42, we have previously identified the fully D-enantiomeric peptide D3, which is able to eliminate Aβ oligomers and has proven therapeutic potential in transgenic Alzheimer´s disease animal models. However, there is little information on the pharmacokinetic behaviour of D-enantiomeric peptides in general. Therefore, we conducted experiments with the tritium labelled D-peptide D3 (3H-D3) in mice with different administration routes to study its distribution in liver, kidney, brain, plasma and gastrointestinal tract, as well as its bioavailability by i.p. and p.o. administration. In addition, we investigated the metabolic stability in liver microsomes, mouse plasma, brain, liver and kidney homogenates, and estimated the plasma protein binding. Based on its high stability and long biological half-life, our pharmacokinetic results support the therapeutic potential of D-peptides in general, with D3 being a new promising drug candidate for Alzheimer´s disease treatment.
Radiation doses from organically bound tritium (OBT) in foods have been a major concern near nuclear facilities. The current dose coefficient for OBT is calculated using a standard model from the International Commission on Radiological Protection, in which some biokinetic values are not based on human metabolic data. Here, the biokinetics of ingested OBT, and radiation doses from them, were estimated by administering labelled compounds and foods to volunteers, using a deuterium (D) tracer as a substitute for tritium. After the administration of D-labelled glucose, alanine, palmitic acid, or soybean, the D/H ratios in urine were measured for up to 119 days, and the biokinetic parameter values were determined for OBT metabolism. The slow degradation rates of OBT could not be obtained, in many volunteers administered glucose and alanine. The estimated committed effective dose for 1 Bq of tritium in palmitic acid varied from 3.2 × 10-11 to 3.5 × 10-10 Sv Bq-1 among volunteers and, for those administered soybean, it varied from 1.9 × 10-11 to 1.8 × 10-10 Sv Bq-1. These results suggest that OBT, present in some ingested ingredients, gives higher doses than the current dose coefficient value of 4.2 × 10-11 Sv Bq-1.
There are over 100 modified bases that occur in RNA with the majority found in transfer RNA. It has been widely believed that the queuine modification is limited to four transfer RNA species in vivo. However, given the vast amount of the human genome (60-70%) that is transcribed into non-coding RNA (Mattick [10]), probing the presence of modified bases in these RNAs is of fundamental importance. The mechanism of incorporation of queuine, via transglycosylation, makes this uniquely poised to probe base modification in RNA. Results of incubations of Escherichia coli cell cultures with [(3)H] preQ(1) (a queuine precursor in eubacteria) clearly demonstrate preQ(1) incorporation into a number of RNA species of various sizes larger than transfer RNA. Specifically, significant levels of preQ(1) incorporation into ribosomal RNA are observed. The modification of other large RNAs was also observed. These results confirm that non-coding RNAs contain modified bases and lead to the supposition that these modifications are necessary to control non-coding RNA structure and function as has been shown for transfer RNA.
There has been tritium groundwater leakage to the land side of Fukushima Dai-ichi nuclear power plants since 2013. Groundwater was continuously collected from the end of 2013 to 2019, with an average tritium concentration of approximately 20 Bq/L. Based on tritium data published by Tokyo Electric Power Company Holdings (TEPCO) (17,000 points), the postulated source of the leakage was (1) leaks from a contaminated water tank that occurred from 2013 to 2014, or (2) a leak of tritium that had spread widely over an impermeable layer under the site. Based on our results, sea side and land side tritium leakage monitoring systems should be strengthened.
Getters are among the key functional components in the tritium-producing burnable absorber rods (TPBARs) of light water reactors (LWRs) and are used to capture the released tritium gas. They are nickel-plated zircaloy-4 tubes that, upon exposure to irradiation or tritium in the light water reactors, undergo alteration in structure, chemical composition, and chemistry. Understanding the radial tritium distribution is key to gaining insight into the evolution of new chemistry upon irradiation to predict getter performance. The holy grail is to develop a method akin to selectively peeling off the layers of an onion in an effort to get a radial map of elements and particularly tritium across the getter. Toward this goal, the overall aim of this work is to establish a correlative technique that can be used to determine radial tritium distribution across getters. To this end, this work specifically focuses on the validation of a correlative method for controlled radial dissolution of nickel-plated getters. Here, pristine getters as well as getters loaded with different mass ratios of hydrogen and deuterium are used as the nonradioactive surrogates of tritium, the idea being that the methodology can be readily extended to tritiated getter components. Here, the surface nickel layers as well as the bulk zirconium layers are sequentially dissolved in a controlled, uniform way using voltage-assisted electrochemical dissolution techniques. The dissolution is complemented by periodic elemental analysis of the electrolyte solution during and post dissolution. This is complemented by microscopic analyses on the exposed surfaces to provide a correlative technique for a complete picture of the radial distribution of various elements across the getter.
The increased potential for tritium releases from either nuclear reactors or from new facilities raises questions about the appropriateness of the current ICRP and WHO recommendations for tritium exposures to human populations. To study the potential toxicity of tritium as a function of dose, including at a regulatory level, mice were chronically exposed to tritium in drinking water at one of three concentrations, 10 kBq.l-1, 1 MBq.l-1 or 20 MBq.l-1. Tritium was administered as either HTO or as tritiated non-essential amino acids (TAA). After one month's exposure, a dose-dependent decrease in red blood cells (RBC) and iron deprivation was seen in all TAA exposed groups, but not in the HTO exposed groups. After eight months of exposure this RBC decrease was compensated by an increase in mean globular volume - suggesting the occurrence of an iron deficit-associated anemia. The analysis of hematopoiesis, of red blood cell retention in the spleen and of iron metabolism in the liver, the kidneys and the intestine suggested that the iron deficit was due to a decrease in iron absorption from the intestine. In contrast, mice exposed to external gamma irradiation at equivalent dose rates did not show any change in red blood cell numbers, white blood cell numbers or in the plasma iron concentration. These results showed that health effects only appeared following chronic exposure to concentrations of tritium above regulatory levels and the effects seen were dependent upon the speciation of tritium.
During a randomized Phase 1 clinical trial the drug candidate, PF-04895162 (ICA-105665), caused transaminase elevations (≥grade 1) in six of eight healthy subjects treated at 300 mg twice daily for 2-weeks (NCT01691274). This was unexpected since studies in rats (<6 months) and cynomolgus monkeys (<9 months) treated up to 100 mg/kg/day did not identify the liver as a target organ. Mechanistic studies showed PF-04895162 had low cytotoxic potential in human hepatocytes, but inhibited liver mitochondrial function and bile salt export protein (BSEP) transport. Clinical relevance of these postulated mechanisms of liver injury was explored in three treated subjects that consented to analysis of residual pharmacokinetic plasma samples. Compared to a nonresponder, two subjects with transaminase elevations displayed higher levels of miRNA122 and total/conjugated bile acid species, whereas one demonstrated impaired postprandial clearance of systemic bile acids. Elevated taurine and glycine conjugated to unconjugated bile acid ratios were observed in two subjects, one before the onset of elevated transaminases. Based on the affinity of conjugated bile acid species for transport by BSEP, the profile of plasma conjugated/unconjugated bile acid species was consistent with inhibition of BSEP. These data collectively suggest that the human liver injury by PF-04895162 was due to alterations in bile acid handling driven by dual BSEP/mitochondrial inhibition, two important risk factors associated with drug-induced liver injury in humans. Alterations in systemic bile acid composition were more important than total bile acids in the manifestation of clinical liver injury and may be a very early biomarker of BSEP inhibition.
Health effects of tritium, a β-emitter and a by-product of the nuclear industry, is a subject of significant controversy. This mouse in vivo study was undertaken to monitor biological effects of low level tritium exposure. Mice were exposed to tritiated drinking water (HTO) at 10 KBq/L, 1 MBq/L and 20 MBq/L concentrations for one month. The treatment did not result in a significant increase of apoptosis in splenocytes. To examine if this low level tritium exposure alters radiosensitivity, the extracted splenocytes were challenged in vitro with 2 Gy γ-radiation, and apoptotic responses at 1 and 24 h were measured. No alterations in the radiosensitivity were detected in cells from mice exposed to tritium compared to sham-treated mice. In contrast, low dose γ-irradiation at 20 or 100 mGy, resulted in a significant increase in resistance to apoptotic cell death after 2 Gy irradiation; an indication of the radioadaptive response. Overall, our data suggest that low concentrations of tritium given to mice as HTO in drinking water do not exert cytotoxic effect in splenocytes, nor do they change cellular sensitivity to additional high dose γ-radiation. The latter may be considered as the lack of a radioadaptive response, typically observed after low dose γ-irradiation.
Tritium is released into the ocean from nuclear facilities located at coastal areas. In addition, tritiated water is decided to be released into the ocean from the Fukushima Dai-ichi Nuclear Power Plant. Although released tritium concentration would be strictly controlled, impact of tritium on the marine products is major concern for the public. In this study, deuterium transfers from seawater into seaweed (ulva) and abalone were measured. In addition, organically bound deuterium (OBD) transfer from ulva into abalone was measured. OBD concentrations in ulva were saturated in 2 weeks and those in abalone were saturated in 6 months. Ulva and abalone were exposed to seawater containing 0.2% (mol-D/mol-H) deuterium. Maximum OBD concentrations in ulva were ~0.1% (mol-D/mol-H) and those in abalone muscle were ~0.035% (mol-D/mol-H). Numerical deuterium transfer model was constructed. Obtained numerical model well represented the OBD-enriched ulva feeding experiment.
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