Hikaru Amano

A natural attenuation of arsenic in drainage from an abandoned arsenic mine dump

Abstract At the abandoned As mine in Nishinomaki, Japan, discharged water from the mining and waste dump area is acidic and rich in As. However, the As concentration in the drainage has been decreased to below the maximum contaminant level (0.01 mg/l for drinking water, Japan) without any artificial treatments before mixing with a tributary to populated areas. This implies that the As concentration in water from the waste dump area has been naturally attenuated. To elucidate the reaction mechanisms of the natural attenuation, analysis of water quality and characterization of the precipitates from the stream floor were performed by measuring pH, ORP and electric conductivity on-site, as well as X-ray diffraction, ICP-mass spectrometry and ion-chromatography. Selective extractions and mineral alteration experiments were also conducted to estimate the distribution of As in constituent phases of the precipitates and to understand the stability of As-bearing phases, respectively. The water contamination resulted from oxidation of sulfide minerals in the waste rocks, i.e., the oxidation of pyrite and realgar and subsequent release of Fe, SO4, As(V) and proton. The released Fe(II) transformed to Fe(III) by bacterial oxidation; schwertmannite then formed immediately. While the As concentrations in the stream were lowered nearly to background level downstream, those in the ochreous precipitates were up to several tens of mg/g. The As(V) was effectively removed by the formed schwertmannite and had been naturally attenuated. Although schwertmannite is metastable with respect to goethite, the experiments show that the transformation of schwertmannite to goethite may be retarded by the presence of absorbed As(V) in the structure. Therefore, the attenuation of As in the drainage and the retention of As by schwertmannite are expected to be maintained for the long term.

Radiation measurements in the Chiba Metropolitan Area and radiological aspects of fallout from the Fukushima Dai-ichi Nuclear Power Plants accident

Large amounts of radioactive substances were released into the environment from the Fukushima Dai-ichi Nuclear Power Plants in eastern Japan as a consequence of the great earthquake (M 9.0) and tsunami of 11 March 2011. Radioactive substances discharged into the atmosphere first reached the Chiba Metropolitan Area on 15 March. We collected daily samples of air, fallout deposition, and tap water starting directly after the incident and measured their radioactivity. During the first two months maximum daily concentrations of airborne radionuclides observed at the Japan Chemical Analysis Center in the Chiba Metropolitan Area were as follows: 4.7 × 10(1) Bq m(-3) of (131)I, 7.5 Bq m(-3) of (137)Cs, and 6.1 Bq m(-3) of (134)Cs. The ratio of gaseous iodine to total iodine ranged from 5.2 × 10(-1) to 7.1 × 10(-1). Observed deposition rate maxima were as follows: 1.7 × 10(4) Bq m(-2) d(-1) of (131)I, 2.9 × 10(3) Bq m(-2) d(-1) of (137)Cs, and 2.9 × 10(3) Bq m(-2) d(-1) of (134)Cs. The deposition velocities (ratio of deposition rate to concentration) of cesium radionuclides and (131)I were detectably different. Radioactivity in tap water caused by the accident was detected several days after detection of radioactivity in fallout in the area. Radiation doses were estimated from external radiation and internal radiation by inhalation and ingestion of tap water for people living outdoor in the Chiba Metropolitan Area following the Fukushima accident.

Characteristics of humic substances in the Kuji River waters as determined by high-performance size exclusion chromatography with fluorescence detection

Direct measurement by high-performance size exclusion chromatography with fluorescence detection was applied to the characterization of humic substances in river waters from the Kuji River system, which runs through forest hills and an agricultural plain in Japan. The monitoring wavelength of excitation 320 nm and emission 430 nm corresponds to the fluorescence maxima for aquatic fulvic acid. Chromatograms of the river waters showed four peaks; each peak position was in good agreement among these samples. Peak height ratios for the samples from the upstream Kuji River and its tributaries were different from those of the midstream and downstream sections of the Kuji River, which may reflect differences in the characteristics of humic substances and other organic materials supplied from soil to river.

Characteristics of Chernobyl-derived radionuclides in particulate form in surface waters in the exclusion zone around the Chernobyl Nuclear Power Plant

Abstract The distribution of Chernobyl-derived radionuclides in river and lake water bodies at 6–40 km from the Chernobyl Nuclear Power Plant was studied. Current levels of radionuclides (Cesium-137, Strontium-90, Plutonium, Americium and Curium isotopes) in water bodies and their relation to the ground contamination are presented. The investigation of the radionuclide composition of aqueous and ground contamination revealed that radionuclides on suspended solids (particulate form) originate mainly from the erosion of the contaminated surface soil layer in the zone. Apparent distribution ratios between particulate and dissolved forms are compared to known distribution coefficients.

Measurement of 90Sr in environmental samples by cation-exchange and liquid scintillation counting

Abstract A new method for the measurement of 90Sr in environmental samples by cation-exchange and liquid scintillation counting is described. Strontium carbonate is purified by precipitation and ion-exchange, weighed for the determination of chemical yield, dissolved in hydrochloric acid and mixed with the liquid scintillator, Aquasol-2. Two channels of a low-background liquid scintillation counter are used to determine 90Sr, 90Y and 89Sr, free from the effects of environmental tritium. The values of 90Sr obtained by this method are in good agreement with those from ordinary 90Y milking and the gas proportional counting method. The concentration of 90Sr in the air at Tokai-mura in Japan has been measured by the new method.

The transfer capability of long-lived Chernobyl radionuclides from surface soil to river water in dissolved forms

Hydrologic runoff is one of the main processes in which radionuclides deposited in the surface environment migrate widely in both particulate and dissolved forms. This paper focuses on the transfer capability of long lived Chernobyl radionuclides from surface soil to river water in dissolved forms. First, concentration and speciation of radioactive Cs, Sr and transuranic isotopes, such as Pu and Am, were examined in undisturbed surface soil along the river in the exclusion zone (30 km zone) near the Chernobyl Nuclear Power Plant (NPP) in order to validate the radioactive contamination characteristics. Almost all radioactivities exist in the very top surface in the undisturbed soil layer. Sr-90 in the soil was estimated to be highest in the water soluble and exchangeable fractions, which were easily accessible to river water as a dissolved fraction. Pu isotopes and Am-241 are major radionuclides in free humic and free fulvic acid fractions. Secondly, surface soil near the Sahan River was extracted with distilled water, as an analogue of rain water, to estimate the dissolved fraction in runoff components from surface soil to river water. After a filtration procedure, extracted water was treated with ultra filtration techniques separating the molecular weight fractions of beyond and below 10,000 Da. Each fraction was measured for the radioactivity and the characteristics of organic materials including humic substances. Most Pu and Am exist in the molecular weight fractions beyond 10,000 Da, in spite of the fact that most of the dissolved organic fractions exist below 10,000 Da. This means that transuranic elements such as Pu and Am are associated with mobile high molecular weight materials like fulvic acids in water leachates.

Formation of organically bound tritium in plants during the 1994 chronic HT release experiment at Chalk River

Trace amounts of elemental tritium (HT) were released continuously to the surface atmosphere at a site at Chalk River Laboratories, Canada over the 12-day period 1994 July 27 to August 8. The test area consisted of four agricultural plots, each 5 m square. One plot was left in its natural state, and the other three were cultivated. Cherry tomatoes, radishes and edible Chinese mustard (Komatsuna in Japanese) were grown in the three cultivated fields. After the HT gas reached the surface of the field, some portion of it was converted into the water form (HTO) mainly by microorganisms in the soil. Then, plant absorbs HTO from both soil and air. Photo synthesized organic material in plant contains tritium,also. The main purpose of this research is to analyze the variation with time of tissue free-water tritium (TFWT) and organically bound tritium (OBT) in several plant species during the HT release. The specific activity of HTO in plants increased rapidly after the HT exposure. The HTO concentration in plant leaves almost attained its maximum value in about 10 days, even though there were several precipitation events, which decreased the soil HTO concentration. The specific activity of OBT in plants increased gradually after the start of the exposure. The OBT concentration in plants did not attain steady state over the whole exposure period of 12 days. The OBT/HTO ratio in plants increased gradually during the release. The ratio in Komatsuna leaves changed from 0.06 to 0.24 between 2 and 11 days. The production rates of OBT in plants are fitted to numerical equations.

In vitro determination of HT oxidation activity and tritium concentration in soil and vegetation during the chronic HT release experiment at Chalk River

The oxidation activity of molecular tritium (HT) in soils and vegetation collected in experimental plots during the 1994 chronic HT release experiment at Chalk River was determined in vitro laboratory experiments after the release. HT oxidation activity was highest in surface soils in the natural plot, about 3-4 times that in soils in the cultivated plots. HT oxidation activity in weeds and Komatsuna leaves was about 2 and 0.4% of that in the cultivated soil, respectively. The number of HT-oxidizing bacteria isolated from soils was highest in the surface soil (0-5 cm) in the natural plot. The viable cell numbers in surface soils in the cultivated and natural plots were almost the same. The total occurrence rates of HT-oxidizing bacteria in the surface soils were 22% in the natural plot, and 7.5% in the cultivated plot. The occurrence rates of HT-oxidizing airborne bacteria during the release on two culture media were 4.2 and 1.9%. 16 refs., 3 figs., 3 tabs.

Uptake of tritium by plants from atmosphere and soil

Uptake of tritiated water (HTO) by plants was examined under field conditions when tritium was available to leaves from only the atmosphere and when tritium was available from both the soil (root uptake) and the atmosphere. Maple, oak, and elm trees, planted in clean soil, were transported to a tritium-contaminated forest, where the atmospheric tritium concentration was elevated, to examine HTO uptake by tree leaves when the source was only in the atmosphere. The results partially agreed with a diffusion model of tritium uptake by plants. Discrepancies found between predicted and measured leaf HTO/air HTO ratios should be attributed to the existence of some isolated water, which is isolated from the transpiration stream in the leaves, that was not available for rapid turnover. The uptake of tritium by trees, when the source was both in the soil and atmosphere, was also examined using deciduous trees (maple and elm) resident to the tritium-contaminated forest. The results were in agreement with a prediction model.

Estimation of 14CO2 flux at soil-atmosphere interface and distribution of 14C in forest ecosystem

To realize the dynamical behavior of 14C among exchangeable carbon reservoirs in terrestrial environment, a method for in situ determination of 14CO2 flux at soil-atmosphere interface and a high flow rate CO2 sampler were developed. This method allowed us to collect integrated quantity of CO2 for determining 14C activity over an extended time period under environmental conditions with minimal site disturbance. The 14CO2 flux from ground surface was estimated to be 1.59 x 10(-5) Bq m (-2) S (-1) in a forest floor with the method. The specific activities of 14C in environmental materials such as some biological and air samples were also determined in the vicinity of the place, where the flux measurement was made, to discuss the behavior of 14C in the forest ecosystem. The results indicated that fresh pine needles had a similar 14C specific activity to the atmospheric CO2 at the same height due to its fairly rapid equilibrium, 14C specific activity in the atmospheric CO2 has a concentration gradient near the ground surface and, at least in this site, CO2 with high 14C specific activity was generated by decomposition of soil organic matter which may be accumulated in soil as a result of former nuclear weapons tests.