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The demand for monitoring anthropogenic U isotopes, 236 U and 233 U, in seawater will continue to increase due to radioecological issues and the need for tools for environmental dynamics research. In response to this growing demand, herein, a novel and simple method was developed for the collection of U isotopes in seawater, both in the laboratory and field, using a fabric-like amidoxime adsorbent. The results from the adsorption studies showed that the optimum conditions for processing seawater in a glass beaker were as follows: seawater pH 4, amidoxime adsorbent 0.20 mmol per 500 g seawater and an adsorption time of 9 hours. Alternatively, when using a closed polyethylene container in experiments on-board a ship and using the same ratio of adsorbent to seawater as in the beaker experiment in the laboratory, the optimum conditions were as follows: seawater pH 8 and an adsorption time of 24 hours. Under the above-mentioned conditions, more than 95% of the U underwent adsorption in both the beaker and the polyethylene container experiments. In the case of analyte desorption, more than 80% of U in seawater was recovered using 2-3 mol dm -3 HCl or HNO 3 as the eluent. Thus, it was concluded that the amidoxime adsorbent can serve as a simple and effective pre-concentration method for the ultra-trace monitoring of U isotopes in seawater.

The long-lived U isotopes, 233 U and 236 U, have been used increasingly in recent years as marine circulation tracers and for identifying sources of uranium contamination in the environment. The sedimentation histories of these two U isotopes in combination with natural 238 U were reconstructed for an anoxic sediment core collected from Beppu Bay, Japan, in the western North Pacific Ocean showing good time resolution (less than 2.6 y/sample). The 233 U/ 236 U atom ratio showed a prominent peak of (3.20 ± 0.30) × 10 -2 around 1957 which can be attributed to the input from atmospheric nuclear weapons tests including thermonuclear tests conducting in the Equatorial Pacific. The integrated 233 U/ 236 U ratio of (1.64 ± 0.08) × 10 -2 for the sediment was found to be in relatively good agreement with the representative ratio published for global fallout (∼1.4 × 10 -2 ). A prominent increase in the authigenic ratio of 233 U/ 238 U a,s in the leached fraction (1.39 ± 0.11 × 10 -11 ) and the bulk digestion (1.36 ± 0.10 × 10 -11 ) was also observed around 1957. This reflects the input supply of 233 U to the seawater which is known to have a relatively constant 238 U content. The authigenic 236 U/ 238 U a,s ratio (0.18 ± 0.02 × 10 -9 ) obtained for 1921 increased from the early 1950's to a maximum of (6.59 ± 0.60) × 10 -9 around 1962. The variation in this ratio represents well the introduction history of U into the surface environment without site-specific U contamination and the time profile is also consistent with the 137 Cs signature. This work thus provides a benchmark for the long-term use of the isotopic U composition as an input parameter for seawater circulation tracers and as a chronological marker for anoxic sediments and sedimentary rocks. Especially the 233 U/ 236 U ratio may serve as a key-marker for the new geological age Anthropocene., Competing Interests: The authors declare no conflict of interest., (© 2023 The Author(s).)

Behavior of radiocesium in Fukushima after its deposition is mainly controlled by mobility of soil components, of which the density is one of the parameters governing the mobility; however, little information is available on the density of soil components associated with radiocesium in environment. Furthermore, the reduction of the volume of radiocesium-contaminated soil in the interim storage is highly demanded. In this study, we developed a gravitational separation method using a sodium polytungstate (SPT) solution combined with size fractionation to understand the relation between 137 Cs activity and the density of surface soil components and evaluate the feasibility of the method for the volume reduction of the contaminated soil. In all soil samples examined, 137 Cs concentration of the small size (<0.063 mm) and high-density (2.4-2.8 g cm -3 ) fraction was the highest among the separated fractions, whereas most of the radiocesium-rich micro-particles were distributed in the small size (<0.063 mm) and low density (<2.4 g cm -3 ) fraction. Although ultrasonication improved the size separation efficiency, a single-step gravitational separation method using an SPT solution with a density of 2.4 g cm -3 without size separation and ultrasonication revealed that the 137 Cs concentration on 50°C-dry weight basis in the dense (>2.4 g cm -3 ) fraction was 25.6-82.7% lower than that of the bulk sample for all soil samples. In particular, for the samples with a bulk 137 Cs concentration of 29.6 Bq g -1 50°C-dry weight, the 137 Cs concentration in the fraction was below the safety treatment requirement (i.e., 8 Bq g -1 ). Therefore, single-step gravitational separation may be used for the volume reduction of contaminated soils., (Copyright © 2022 Elsevier Ltd. All rights reserved.)

A massive amount of soils and inflammable materials of plants etc. contaminated by radiocesium are generated from decontamination work in the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident affected area. In present study, the removal experiments of 137 Cs in a soil collected from the FDNPP accident affected area were carried out in a lab-scale electrical heating horizontal furnace through thermal treatment with CaCl 2 addition over a temperature of 900 - 1300 °C. The results indicated that the average radioactive concentration of 137 Cs in the soil was 52.8 Bq/g. The removal ratio of 137 Cs in the soil treated at 1300 °C was 96.3 % when 20 % CaCl 2 was added. The addition of CaCl 2 and CaO mixture exhibited a synergistic effect on the removal of 137 Cs, relative to the addition of CaCl 2 alone. Accordingly, the addition of CaCl 2 or its mixture with CaO during thermal treatment is suggested to remove 137 Cs in the soil collected from the FDNPP accident affected area. Additionally, segregation of the soil sample to fine and coarse fraction and then treated individually are also recommended., (Copyright © 2020 Elsevier B.V. All rights reserved.)

The structural form and elemental distribution of material originating from different Fukushima Daiichi Nuclear Power Plant reactors (Units 1 and 3) is hereby examined to elucidate their contrasting release dynamics and the current in-reactor conditions to influence future decommissioning challenges. Complimentary computed X-ray absorption tomography and X-ray fluorescence data show that the two suites of Si-based material sourced from the different reactor Units have contrasting internal structure and compositional distribution. The known event and condition chronology correlate with the observed internal and external structures of the particulates examined, which suggest that Unit 1 ejecta material sustained a greater degree of melting than that likely derived from reactor Unit 3. In particular, we attribute the near-spherical shape of Unit 1 ejecta and their internal voids to there being sufficient time for surface tension to round these objects before the hot (and so relatively low viscosity) silicate melt cooled to form glass. In contrast, a more complex internal form associated with the sub-mm particulates invoked to originate from Unit 3 suggest a lower peak temperature, over a longer duration. Using volcanic analogues, we consider the structural form of this material and how it relates to its environmental particulate stability and the bulk removal of residual materials from the damaged reactors. We conclude that the brittle and angular Unit 3 particulate are more susceptible to further fragmentation and particulate generation hazard than the round, higher-strength, more homogenous Unit 1 material.

Environmental contaminations of 129 I were continuously monitored in various sample preparation rooms for accelerator mass spectrometry at the University of Tsukuba. Monitoring of 129 I was performed in the rooms used for the treatment of samples in the past, in order to compare with the results obtained in the sample preparation rooms. Ambient levels of atmospheric 129 I in each room were estimated from the measured concentrations in the alkali trap solutions. This article reports the results of one year of monitoring the temporal changes of stable iodine ( 127 I) and 129 I contamination rates in the alkali trap solutions. It was found that 129 I contamination rates were lower than approximately 10 4 atoms cm -2 day -1 in the rooms where ether no samples or only samples with environmental background levels of 129 I were handled. Values from 10 4 to 10 5 atoms cm -2 day -1 were recorded in another room where environmental samples, such as the samples derived from nuclear power plant accidents, were treated. Higher levels of 129 I, ranging from 10 6 to 10 7 atoms cm -2 day -1 , were recorded in rooms used for treating neutron-activated iodine. The experimental results show that the 129 I level depended on the 129 I sample-preparation histories for the respective rooms. It is possible to estimate the 129 I contamination risk from the atmosphere to the samples by knowing the 129 I level in the preparation room.

For accurately determining nutrients in seawater by continuous flow analysis (CFA), the characteristic of the calibration curve was examined in detail. Under absorbance below 0.8, the calibration curve and the bracketing methods showed more accurate results that the bias fell below 0.5%. The analytical results of dissolved silica in seawater from the nutrient maximum layer of the Pacific Ocean obtained by the proposed methods showed good agreement with those obtained by an ion exclusion chromatography postcolumn absorption spectrophotometry (IEC-postcolumn) and an ion exclusion chromatography isotope dilution ICP mass spectrometry (IEC-ID-ICP-MS). From the results, the analysis of nutrients in seawater could be accurately carried out by CFA with an expanded uncertainty of below 1% using both the calibration curve and the bracketing methods with an appropriate absorbance range.

Both the three-dimensional internal structure and elemental distribution of near-field radioactive fallout particulate material released during the March 2011 accident at the Fukushima Daiichi Nuclear Power Plant is analysed using combined high-resolution laboratory and synchrotron radiation x-ray techniques. Results from this study allow for the proposition of the likely formation mechanism of the particles, as well as the potential risks associated with their existence in the environment, and the likely implications for future planned reactor decommissioning. A suite of particles is analyzed from a locality 2 km from the north-western perimeter of the site - north of the primary contaminant plume in an area formerly attributed to being contaminated by fallout from reactor Unit 1. The particles are shown to exhibit significant structural similarities; being amorphous with a textured exterior, and containing inclusions of contrasting compositions, as well as an extensive internal void volume - bimodal in its size distribution. A heterogeneous distribution of the various elemental constituents is observed inside a representative particle, which also exhibited a Fukushima-derived radiocesium (134Cs, 135Cs and 137Cs) signature with negligible natural Cs. We consider the structure and composition of the particle to suggest it formed from materials associated with the reactor Unit 1 building explosion, with debris fragments embedded into the particles surface. Such a high void ratio, comparable to geological pumice, suggests such material formed during a rapid depressurisation and is potentially susceptible to fragmentation through attrition.

The Fukushima Daiichi Nuclear Power Plant (FDNPP) accident released abundant radioactive particles into the surrounding environment. Herein, we analyzed the activity of 90 Sr in these particles to estimate the contribution of this radionuclide to the overall radiation exposure and shed light on the processes that occurred during the accident. Seven radioactive particles were isolated from the dust and soil samples collected from areas surrounding the FDNPP, and the minimum/maximum 137 Cs activities were determined as 224/4,100 Bq. Based on the size, specific activity, and 134 Cs/ 137 Cs activity ratios, we concluded that six of the seven radioactive particles were released from the Unit 1 reactor, while one particle was released from the Unit 3 reactor by a hydrogen explosion. Strontium-90 was detected in all radioactive particles, and the minimal/maximal 90 Sr activities were determined as 0.046/1.4 Bq. 137 Cs/ 90 Sr activity ratios above 1000 were observed for all seven particles, that is, compared to 137 Cs, 90 Sr had negligible contribution to the overall radiation exposure. The 137 Cs/ 90 Sr activity ratios of the radioactive particles were similar to those of terrestrial environmental samples and were higher for particles released from the Unit 1 reactor than for samples collected from the Unit 1 reactor building, which indicates possibility of additional 90 Sr-rich contamination after release of the particles.

In order to achieve the highly efficient 99m Tc production from 100 MoO 3 by the 100 Mo(n, 2n) 99 Mo reaction, we have developed a new protocol to synthesize nano-sized Mo particles, of which the size was controlled by the inner space of the liposomes. Calcium and molybdate ions were encapsulated into ∼100 nm size liposomes. The liposome suspensions were then mixed and heated to promote the membrane fusion. As a result, the insoluble CaMoO 4 nanoparticles precipitated inside the liposomes. The median particle diameter of 168 nm and average diameter of 169 ± 56 nm (n = 109) were obtained from an SEM image, and the particles have a powellite-structure. The formation process of the particles was then examined. The formation of nano-sized CaMoO 4 was observed by the high resolution TEM image and TEM image of negative-stained liposome. At the room temperature, the fusion of liposome did not occur significantly. These results suggest that nanocrystals of the CaMoO 4 were likely formed in the liposomes because of the liposome fusion and aggregated during the drying processes of reaction solution., (Copyright © 2018 Elsevier Inc. All rights reserved.)

The anthropogenic long-lived radionuclide 129 I is receiving increased attraction as a new oceanic tracer in addition to usage as a fingerprint of radionuclide contamination of the marine environment. To demonstrate the robustness of 129 I as an oceanic tracer in the Northwest Pacific area, specifically in the Japan Sea, the input history of 129 I to surface seawater was reconstructed using a hermatypic coral core sample from Iki Island in the Tsushima strait. Iodine isotopes in each annual band were measured using AMS and ICP-MS after appropriate pre-treatments of small amounts of coral powder. The 129 I/ 127 I ratios in the 1940s were almost at background levels (<1 × 10 -11 ) and increased abruptly in the early 1950s. Thereafter, the ratios continuously increased with some fluctuations; the maximum ratio, 7.13 ± 0.72 × 10 -11 , being found in the late 1990s. After that period, the ratios remained nearly constant until the present time (2011). The 129 I originated mainly from the nuclear weapons testings of the 1950s and the early 1960s, and from airborne releasing by nuclear reprocessing facilities. The dataset obtained here was used to construct a simple model to estimate the diffusion coefficient of 129 I in the Japan Sea. The 129 I/ 236 U ratios over the observation period were also reconstructed to help constraining sources of 129 I to the marine environment. Based on the results, the 129 I/ 236 U ratio obtained here could be an endmember of the water mass in the Kuroshio Current area of the Northwest Pacific Ocean., (Copyright © 2018 Elsevier Ltd. All rights reserved.)

Evaluation of radiation exposure from diet is necessary under the assumption of a virtual accident as a part of emergency preparedness. Here, we developed a model with complete consideration of the regional food trade using deposition data simulated by a transport model, and estimated the dietary intake of radionuclides and the effectiveness of regulation (e.g., restrictions on the distribution of foods) after the Fukushima accident and in virtual accident scenarios. We also evaluated the dilution factors (i.e., ratios of contaminated foods to consumed foods) and cost-effectiveness of regulation as basic information for setting regulatory values. The doses estimated under actual emission conditions were generally consistent with those observed in food-duplicate and market-basket surveys within a factor of three. Regulation of restricted food distribution resulted in reductions in the doses of 54⁻65% in the nearest large city to the nuclear power plant. The dilution factors under actual emission conditions were 4.4% for radioiodine and 2.7% for radiocesium, which are ~20 times lower than those used in the Japanese provisional regulation values after the Fukushima accident. Strict regulation worsened the cost-effectiveness for both radionuclides. This study highlights the significance and utility of the developed model for a risk analysis of emergency preparedness and regulation.

Following the Fukushima Dai-ichi Nuclear Power Station accident, regional road dust, heavily contaminated with radiocesium, now represents a potential source of radiocesium pollution in river water. To promote effective countermeasures for reducing the risk from radiocesium pollution, it is important to understand its sources. This study evaluated the utility of metals, including Al, Fe, and Zn as road dust tracers, and applied them to analyze sources of 137 Cs in rivers around Fukushima during wet weather. Concentrations of Zn in road dust were higher than agricultural and forest soils, whereas concentrations of Fe and Al were the opposite. Concentrations of Zn were weakly but significantly correlated with benzothiazole, a molecular marker of tires, indicating Zn represents an effective tracer of road dust. Al, Fe, and Zn were frequently detected in suspended solids in river water during wet weather. Distribution coefficients of these metals and 137 Cs exceeded 10 4 , suggesting sorptive behavior in water. Although concentrations of Al, Fe, Zn, and 137 Cs were higher in fine fractions of road dust and soils than in coarse fractions, use of ratios of 137 Cs to Al, Fe, or Zn showed smaller differences among size fractions. The results demonstrate that combinations of these metals and 137 Cs are useful for analyzing sources of radiocesium in water. These ratios in river water during wet weather were found to be comparable with or lower than during dry weather and were closer to soils than road dust, suggesting a limited contribution from road dust to radiocesium pollution in river water., (Copyright © 2017 Elsevier Ltd. All rights reserved.)

The vaporization mechanisms of water-insoluble Cs in raw ash and Cs-doped ash during thermal treatment with CaCl 2 addition was systematically examined in a lab-scale electrical heating furnace over a temperature range of 500-1500 °C. The results indicate that the water-insoluble Cs in the ash was associated with aluminosilicate as pollucite. Addition of 10% CaCl 2 caused the maximum vaporization ratio of Cs in the raw ash to reach approximately 80% at temperatures higher than 1200 °C, whereas approximately 95% of Cs was vaporized at temperatures higher than 1300 °C when 30% CaCl 2 was added. The formation of an intermediate compound, CsCaCl 3 , through the chemical reaction of Cs with CaCl 2 was responsible for Cs vaporization by means of the subsequent decomposition of this intermediate upon the increase in temperature. The indirect chlorination of Cs by the gaseous chlorine released from the decomposition of CaCl 2 was insignificant. A high CaCl 2 content in the resulting annealed products with 30% CaCl 2 addition delayed the decomposition of CsCaCl 3 and thus lowered the Cs vaporization ratio compared to that with 10% CaCl 2 addition at 900-1250 °C. Thermal treatment with CaCl 2 addition is a proposed method to remove Cs from Cs-contaminated incineration ash.

The migration and dispersion of radioactive Cs (mainly (134)Cs and (137)Cs) are of critical concern in the area surrounding the Fukushima Daiichi Nuclear Power Plant (FDNPP). Considerable uncertainty remains in understanding the properties and dynamics of radioactive Cs transport by surface water, particularly during rainfall-induced flood events to the ocean. Physical and chemical properties of unique estuary sediments, collected from the Kuma River, 4.0km south of the FDNPP, were quantified in this study. These were deposited after storm events and now occur as dried platy sediments on beach sand. The platy sediments exhibit median particle sizes ranging from 28 to 32μm. There is increasing radioactivity towards the bottom of the layers deposited; approximately 28 and 38Bqg(-1) in the upper and lower layers, respectively. The difference in the radioactivity is attributed to a larger number of particles associated with radioactive Cs in the lower part of the section, suggesting that radioactive Cs in the suspended soils transported by surface water has decreased over time. Sequential chemical extractions showed that ~90% of (137)Cs was strongly bound to the residual fraction in the estuary samples, whereas 60~80% of (137)Cs was bound to clays in the six paddy soils. This high concentration in the residual fraction facilitates ease of transport of clay and silt size particles through the river system. Estuary sediments consist of particles <100μm. Radioactive Cs desorption experiments using the estuary samples in artificial seawater revealed that 3.4±0.6% of (137)Cs was desorbed within 8h. More than 96% of (137)Cs remained strongly bound to clays. Hence, particle size is a key factor that determines the travel time and distance during the dispersion of (137)Cs in the ocean., (Copyright © 2016 Elsevier B.V. All rights reserved.)

After the 2011 nuclear accident in Fukushima, radiocesium was released from the Fukushima Dai-ichi Nuclear Power Plant and contaminated waters in urban areas near Tokyo. By intensive field monitoring during 3 years, this study investigated the temporal trends and the occurrence of radiocesium during dry and wet weather, and analyzed the variations in radiocesium during rainfall events and factors controlling them. Concentrations of particulate radiocesium decreased rapidly from May 2012 to March 2013 and reached an equilibrium in 2014. Concentrations of particulate (137)Cs during wet weather were almost double those during dry weather in the same period. In contrast to the small variations in (137)Cs concentrations in the particulate phase on a suspended solids (SS) weight basis during events, those in the dissolved phase on a liquid-volume basis fluctuated greatly, resulting in variations in the partition coefficient (apparent Kd). The apparent Kd of (137)Cs during wet weather ranged from 30,000 to 150,000 L kg(-1) and showed a significant negative correlation with SS concentrations during wet weather. Specific surface area in solids contributed to the variations in apparent Kd., (Copyright © 2016 Elsevier Ltd. All rights reserved.)

To evaluate the deposition density and extent of subsurface infiltration of (129)I and (137)Cs in the restricted area that was highly contaminated by the accident of Fukushima Dai-ichi Nuclear Power Plant, cumulative inventories of (129)I and (137)Cs, concentrations of (129)I and (137)Cs, and (129)I/(137)Cs ratio in 30-cm-long soil columns were compared with pre-accident levels from the same area. The cores were collected before and after the accident from locations of S-1 (4 km west of FDNPP) and S-2 (8 km west of FDNPP). Deposition densities of (129)I and (137)Cs in the soil following the accident were 0.90-2.33 Bq m(-2) and 0.80-4.04 MBq m(-2), respectively, which were 14-39 and 320-510 times larger than the pre-accident levels of (129)I (59.3-63.3 mBq m(-2)) and (137)Cs (2.51-7.88 kBq m(-2)), respectively. Approximately 90% of accident-derived (129)I and (137)Cs deposited in the 30-cm soil cores was concentrated in the surface layer from 0 to 44-95 kg m(-2) of mass depth (0-4.3-6.2 cm depth) and from 0 to 16-25 kg m(-2) of mass depth (0-1.0-3.1 cm depth), respectively. The relaxation mass depths (h0) of 10.8-11.2 kg m(-2) for (129)I estimated in the previous study were larger than those of 8.1-10.6 kg m(-2) for (137)Cs at both sites, owing to the larger infiltration depth of radioiodine mainly by the gravitational water penetration in the surface soil in our study sites. Approximately 7-9% of the accident-derived (129)I was present in the lower layer from 44 to 100 kg m(-2) (4.3-8.6 cm depth) at S-1, and from 95 to 160 kg m(-2) (6.2-10.2 cm depth) at S-2. Approximately 1% of (137)Cs seems to infiltrate deeper than (129)I in the lower layer at each site in contrast to the surface layer., (Copyright © 2015 Elsevier Ltd. All rights reserved.)

In 2011, a large radioactive discharge occurred at the Fukushima Daiichi nuclear power plant. This plant is located within a climatically temperate region where outdoor swimming pools are popular. Although it is relatively easy to decontaminate pools by refilling them with fresh water, it is difficult to maintain safe conditions given highly contaminated diurnal dust falls from the surrounding contaminated ground. Our objectives in this paper were to conduct daily radioactivity measurements, to determine the quantity of radioactive contaminants from the surrounding environment that invade outdoor pools, and to investigate the efficacy of traditional pool cleaners in removing radioactive contaminants. The depositions in the paper filterable particulates ranged from 0 to 62,5 Bq/m(2)/day, with the highest levels found in the southern Tohoku District containing Fukushima Prefecture and in the Kanto District containing Tokyo Metro. They were approximately correlated with the ground contamination. Traditional pool cleaners eliminated 99% of contaminants at the bottom of the pool, reducing the concentration to 41 Bq/m(2) after cleaning. Authors recommended the deposition or the blown radionuclides into outdoor swimming pools must be considered into pool regulations when the environments exactly polluted with radionuclides., (Copyright © 2014 Elsevier Ltd. All rights reserved.)

A tremendous amount of radioactivity was discharged because of the damage to cooling systems of nuclear reactors in the Fukushima No. 1 nuclear power plant in March 2011. Fukushima and its adjacent prefectures were contaminated with fission products from the accident. Here, we show a geographical distribution of radioactive iodine, tellurium, and cesium in the surface soils of central-east Japan as determined by gamma-ray spectrometry. Especially in Fukushima prefecture, contaminated area spreads around Iitate and Naka-Dori for all the radionuclides we measured. Distributions of the radionuclides were affected by the physical state of each nuclide as well as geographical features. Considering meteorological conditions, it is concluded that the radioactive material transported on March 15 was the major contributor to contamination in Fukushima prefecture, whereas the radioactive material transported on March 21 was the major source in Ibaraki, Tochigi, Saitama, and Chiba prefectures and in Tokyo.

alpha-gamma and alpha-electron coincidence spectroscopy for a short-lived heavy actinide nucleus (257)No (T(1/2) = 24.5 s) has been performed using a gas-jet transport system and an on-line isotope separator. Spin-parities of excited states in (253)Fm fed by the alpha decay of (257)No have been identified on the basis of the measured internal conversion coefficients. The nu3/2(+)[622] configuration has been assigned to the ground state of (257)No as well as to the 124.1 keV level in (253)Fm. It was found that the ground-state configuration of (257)No is different from that of lighter N = 155 isotones.

Fluoride complexation of element 104, rutherfordium (Rf), produced in the 248Cm(18O,5n)261Rf reaction has been studied by anion-exchange chromatography on an atom-at-a-time scale. The anion-exchange chromatographic behavior of Rf was investigated in 1.9-13.9 M hydrofluoric acid together with those of the group-4 elements Zr and Hf produced in the 18O-induced reactions on Ge and Gd targets, respectively. It was found that the adsorption behavior of Rf on anion-exchange resin is quite different from those of Zr and Hf, suggesting the influence of relativistic effects on the fluoride complexation of Rf.

Standard reference ranges for all laboratory test values are mandatory. This study was designed to establish a reference range for blood vitamin B1 levels, since the normal range has not been determined in the Japanese population. We founded the Japan Committee for Vitamin Laboratory Standards, which was incorporated with the Vitamin Society of Japan and the Japanese Society of Nutrition and Food Science. We standardized whole blood vitamin B1 levels using three HPLC techniques (post-column reverse-phase HPLC, pre-column reverse-phase HPLC, and precolumn GP-HPLC). The reference range was obtained in 54 volunteers administered a 1,800 kcal diet with 2 mg of vitamin B1 (1.74 mg measured) daily to avoid marginal vitamin B1 deficiency in the population. The range for each assay was 26-47, 28-51, and 28-56 ng/ml, respectively. Our data suggest that 26-28 ng/ml is the lower limit of normal for whole blood vitamin B1, but further studies in a larger population are needed in order to obtain more definitive results.

Thirty-four foods were analyzed in order to determine the content of water-soluble dietary fiber (SDF) and insoluble dietary fiber (IDF). Using the results with the standard table for 227 foods, the intake ratio of IDF/SDF of an average Japanese was calculated for the period 1946-1990. The ratio was 3.22 in 1990 as calculated on the food intakes shown in the national nutrition survey, and the secular change was not detected since 1946 when the ratio was 3.30. The ratio was also shown to be well preserved between types of households including the age of the head. Using dietary records of 60 healthy city workers (average 42.8 years) for 4 weeks, however, the weekly average ratio for an individual was found to vary in the range of 2.25-5.13 although the total average for 60 individuals was 3.33. Thus, the well preserved IDF/SDF intake ratio for an average Japanese showed, on the contrary, a wide variation of food selection between each person.

An internal monostandard method is proposed for the nondestructive determination of major elements in large samples by prompt γ ray neutron activation analysis. It successfully overcomes the problems characteristic of large samples, such as the absorption and scattering of incident neutrons and the absorption of emitted γ rays. In order to make this proposed method understood theoretically, an equation is presented and its validity for the analysis of large samples discussed. In principle, the proposed method gives relative contents in large solid samples, whereas it allows absolute determination for samples in solution form. As a demonstration for the analysis of a large solid sample, we analyzed an earthen vessel, and the major elements in the sample (Na, Mg, Al, Si, K, Ca, Ti, Mn, and Fe) were determined within the uncertainty of 10%, except for Mn. This method was also tested for samples in solution form, and it was found that the absolute content of a target element could be obtained by constructing a calibration curve using several known standard solutions of different concentrations. Residual radioactivity after irradiation was also examined and found to be so little that the sample could be taken outside the radiation-controlled area within a few days after the irradiation.

Background: Water-soluble fullerenes have recently been shown to exhibit considerable in vitro biological activity including cytotoxicity, site-selective DNA cleavage and inhibition of HIV protease. To assess the potential of these compounds as drugs, studies on the in vivo behavior of fullerenes are needed. We therefore set out to synthesize a radiolabeled, water-soluble fullerene, in order to obtain data on the oral absorption, distribution and excretion of this class of compounds., Results: We synthesized a 14C-labeled water-soluble [60]fullerene using dipolar trimethylenemethane, which undergoes cycloaddition to [60]fullerene. When administered orally to rats, this compound was not efficiently absorbed and was excreted primarily in the feces. When injected intravenously, however, it was distributed rapidly to various tissues, and most of the material was retained in the body after one week. The compound was also able to penetrate the blood-brain barrier. Acute toxicity of the water-miscible fullerene was found to be quite low., Conclusions: Although the water-soluble fullerenes (and possibly their simple metabolites) are not acutely toxic, they are retained in the body for long periods, raising concerns about chronic toxic effects. The fact that fullerenes distribute rapidly to many tissues suggests that they may eventually be useful to deliver highly polar drugs through membranes to a target tissue, however, and they may even have applications in the delivery of drugs to the brain. Recent advances in fullerene synthetic chemistry may also make it possible to control fullerene absorption/excretion profiles in the future.

The immunosuppressive effect of 5'-deoxy-5-fluorouridine (5'-DFUR, Ro 21-9738) was examined for both humoral and cell-mediated immunity in mice in comparison with that of 5-fluorouracil and Ftorafur (FT-207). By both oral and intraperitoneal administration, 5'-DFUR was found to be much less suppressive than 5-fluorouracil and FT-207 in all immune responses tested; hemolysin plaque-forming cells, serum hemolysin titer, delayed-type hypersensitivity and allogeneic tumor rejection. Furthermore, 5'-DFUR did not induce any reduction in either the spleen weight, thymus weight, total spleen cell number, or peripheral leucocyte number.

We found that both thymosin from calf thymus and its constituent peptide alpha 1 prepared by chemical synthesis restore cell-mediated immunity following its suppression in mice by injection of 5-FU. Conditions suitable for assessing the thymosin activity by means of footpad reaction were established in such immunosuppressed mice. In this new animal model, thymosin alpha 1-peptide showed activity at a low dose of 5-50 micrograms/kg, which was 100-1,000 times less than that required for thymosin F-5 preparations. Further studies utilizing the adoptive transfer technique showed that alpha 1-peptide corrects the 5-FU-induced suppression of mature T cells, transferring the DTH response as well as that of macrophage function responsible for the expression of footpad reaction. Furthermore, regeneration of lymph node and bone marrow cells as well as CFU-c (progenitor cells of macrophages and granulocytes) was enhanced by thymosin alpha 1 in the 5-FU-treated mice. All these results indicate that thymosin alpha 1 accelerates the replenishment and maturation of haematopoietic cells, including not only T cells but also macrophages, when they have been severely damaged by the 5-FU treatment.