Penetration factor and indoor deposition rate of elementary and particulate iodine in a Japanese house for assessing the effectiveness of sheltering for radiation exposures.

Sheltering is one of the countermeasures for protection against radiation exposures in nuclear accidents. The effectiveness of sheltering is often expressed by the reduction factor, that is the ratio of the indoor to the outdoor cumulative radioactivity concentrations or doses. The indoor concentration is mainly controlled by the air exchange rate, penetration factor, and indoor deposition rate. The penetration factor and indoor deposition rate depend on the surface and the materials and structure of windows and doors as it is these openings in the building envelope that control penetration. We investigated experimentally these parameters of I2and particles. The experiment was performed in two apartment houses, three single-family houses, and chambers. The obtained penetration factor ranged from 0.3 to 1 for particles of 0.3-1µm and 0.15-0.7 for I2depending on the air exchange rate. The indoor deposition rate for a house room ranged from 0.007 to 0.2 h-1for particles of 0.3-1µm and 0.2-1.5 h-1for I2.

Bioaccessibility of Fukushima-Accident-Derived Cs in Soils and the Contribution of Soil Ingestion to Radiation Doses in Children.

Ingestion of contaminated soil is one potential internal exposure pathway in areas contaminated by the Fukushima Daiichi Nuclear Power Plant accident. Doses from this pathway can be overestimated if the availability of radioactive nuclides in soils for the gastrointestinal tract is not considered. The concept of bioaccessibility has been adopted to evaluate this availability based on in vitro tests. This study evaluated the bioaccessibility of radioactive cesium from soils via the physiologically-based extraction test (PBET) and the extractability of those via an extraction test with 1 mol/L of hydrochloric acid (HCl). The bioaccessibility obtained in the PBET was 5.3% ± 1%, and the extractability in the tests with HCl was 16% ± 3%. The bioaccessibility was strongly correlated with the extractability. This result indicates the possibility that the extractability in HCl can be used as a good predictor of the bioaccessibility with PBET. In addition, we assessed the doses to children from the ingestion of soil via hand-to-mouth activity based on our PBET results using a probabilistic approach considering the spatial distribution of radioactive cesium in Date City in Fukushima Prefecture and the interindividual differences in the surveyed amounts of soil ingestion in Japan. The results of this assessment indicate that even if children were to routinely ingest a large amount of soil with relatively high contamination, the radiation doses from this pathway are negligible compared with doses from external exposure owing to deposited radionuclides in Fukushima Prefecture.

Characterization of Pathogenic Escherichia coli in River Water by Simultaneous Detection and Sequencing of 14 Virulence Genes.

The occurrence of pathogenic Escherichia coli in environmental waters increases the risk of waterborne disease. In this study, 14 virulence genes in 669 E. coli isolates (549 isolates from the Yamato River in Japan, and 30 isolates from each of the following hosts: humans, cows, pigs, and chickens) were simultaneously quantified by multiplex PCR and dual index sequencing to determine the prevalence of potentially pathogenic E. coli. Among the 549 environmental isolates, 64 (12%) were classified as extraintestinal pathogenic E. coli (ExPEC) while eight (1.5%) were classified as intestinal pathogenic E. coli (InPEC). Only ExPEC-associated genes were detected in human isolates and pig isolates, and 11 (37%) and five (17%) isolates were classified as ExPEC, respectively. A high proportion (63%) of cow isolates possessed Shiga-toxin genes (stx1 or stx2) and they were classified as Shiga toxin-producing E. coli (STEC) or enterohemorrhagic E. coli (EHEC). Among the chicken isolates, 14 (47%) possessed iutA, which is an ExPEC-associated gene. This method can determine the sequences as well as the presence/absence of virulence genes. By comparing the sequences of virulence genes, we determined that sequences of iutA were different among sources and may be useful for discriminating isolates, although further studies including larger numbers of isolates are needed. Results indicate that humans are a likely source of ExPEC strains in the river.

Fecal source tracking in water by next-generation sequencing technologies using host-specific Escherichia coli genetic markers.

High levels of fecal bacteria are a concern for the aquatic environment, and identifying sources of those bacteria is important for mitigating fecal pollution and preventing waterborne disease. Escherichia coli has been used as an indicator of fecal pollution, however less success has been achieved using this organism for library-independent microbial source tracking. In this study, using next-generation sequencing technology we sequenced the whole genomes of 22 E. coli isolates from known sources (9 from humans, 2 from cows, 6 from pigs, and 5 from chickens) and identified candidate host-specific genomic regions. Specificity testing on the candidate regions was performed using 30 E. coli isolates from each source. Finally, we identified 4 human-, 2 cow-, 3 pig-, and 4 chicken-specific genetic markers useful for source tracking. We also found that a combination of multiplex PCR and dual index sequencing is effective for detecting multiple genetic markers in multiple isolates at one time. This technique was applied to investigating identified genetic markers in 549 E. coli isolates obtained from the Yamato River, Japan. Results indicate that humans constitute a major source of water contamination in the river. However, further work must include isolates obtained from geographically diverse animal hosts to make this method more reliable.

Acrylamide and Glycidamide Hemoglobin Adduct Levels and Breast Cancer Risk in Japanese Women: A Nested Case-Control Study in the JPHC.

BACKGROUND: Acrylamide (AA) is classified as "probably carcinogenic to humans (class 2A)" by the International Agency for Research on Cancer. AA causes cancer owing to its mutagenic and genotoxic metabolite, glycidamide (GA), and its effects on sex hormones. Both AA and GA can interact with hemoglobin to hemoglobin adducts (HbAA and HbGA, respectively), which are considered appropriate biomarkers of internal exposure of AA. However, few epidemiologic studies reported an association of HbAA and HbGA with breast cancer. METHODS: We conducted a nested case-control study within the Japan Public Health Center-based Prospective Study cohort (125 cases and 250 controls). Cases and controls were categorized into tertiles (lowest, middle, and highest) using the distribution of HbAA or HbGA levels in the control group and estimated ORs and 95% confidence intervals (CI) using conditional logistic regression, adjusting for potential confounders. RESULTS: No association was observed between HbAA (ORHighestvs.Lowest, 1.34; 95% CI, 0.69-2.59), HbGA (ORHighest vs. Lowest, 1.46; 95% CI, 0.79-2.69), their sum HbAA+HbGA (ORHighest vs. Lowest, 1.36; 95% CI, 0.72-2.58) and breast cancer; however, some evidence of positive association was observed between their ratio, HbGA/HbAA, and breast cancer (ORHighest vs. Lowest, 2.19; 95% CI, 1.11-4.31). CONCLUSIONS: There was no association between biomarkers of AA and breast cancer. IMPACT: It is unlikely that AA increases breast cancer risk; however, the association of AA with breast cancer may need to be evaluated, with a focus not only on the absolute amount of HbAA or HbGA but also on HbGA/HbAA and the activity of metabolic genes.

Identifying the contribution of charge effects to airborne transmission of aerosols in confined spaces.

Aerosols in indoor air have various adverse effects on human health. Considering the use of forced ventilation and fan mixing (individually and in combination), the variation in charge number and their effects on aerosol transmission in confined spaces were explored in this study with the distinction of particle sources. In the case of sources originating from the external space, natural penetration acquires a greater number of negative charges. Forced ventilation of a confined space acts on the fate of particles in the neighboring confined space, while the internal fan has a negligible effect on both the number concentration and charge number of particles in the exterior. The combination of forced ventilation and fan mixing increases charge numbers, altering the lifetime of particles in the external regional environment by deposition or adsorption, particularly for neutralized particles. In the case of sources originating from the interior area, application of an internal fan weakens the ventilation effect from forced ventilation, resulting in internal particle loss by depositing on internal surfaces due to electrostatic charge, increasing the potential risk of resuspension. Additionally, source origin is associated with particle fate, and the charge generated under the action of external forces contributes to the transmission pathways and the fate of the particles in the air. This study investigates the transmission pathways and the fate of aerosols from the perspective of charge number, hopefully contributing to an in-depth understanding of the transmission mechanisms of toxic substances in confined spaces with aerosols as carriers.

Acrylamide-Hemoglobin Adduct Levels in a Japanese Population and Comparison with Acrylamide Exposure Assessed by the Duplicated Method or a Food Frequency Questionnaire.

The levels of hemoglobin adducts of acrylamide (AA-Hb), a biomarker of acrylamide exposure, have not been reported for Japanese subjects. Herein, we determined the AA-Hb levels in a Japanese population and compared them with the estimated dietary intake from the duplicate diet method (DM) and a food frequency questionnaire (FFQ). One-day DM samples, FFQ, and blood samples were collected from 89 participants and analyzed for acrylamide. AA-Hb was analyzed using liquid chromatography tandem mass spectrometry and the N-alkyl Edman method. Participants were divided into tertiles of estimated acrylamide intake and geometric means (GMs) of AA-Hb adjusted for sex and smoking status. A stratified analysis according to smoking status was also performed. The average AA-Hb levels for all participants, never, past, and current smokers were 46, 38, 65, and 86 pmol/g Hb, respectively. GMs of AA-Hb levels in all participants were significantly associated with tertiles of estimated acrylamide intake from DM (p for trend = 0.02) and FFQ (p for trend = 0.04), although no association with smokers was observed. AA-Hb levels reflected smoking status, which were similar to values reported in Western populations, and they were associated with estimated dietary intake of acrylamide when adjusted for sex and smoking status.

[Biodistribution of ultrafine particles of titanium dioxide by intratracheal administration to mice].

TiO2 ultrafine particles are used as photo-catalysis. When ultrafine particles are exposed to hosts, they are invaded in alveolar, transferred to organs through blood vessels and may express biological effects. We administered TiO2 ultra-fine particles (5 nm, 100 nm) intratracheally to mice, and collected whole blood and removed organs (liver, lung, kidney, spleen and brain) after 1, 4 and 24 hours. The quantity of Ti in the blood and these organs was analyzed by PIXE (Particle Induced X-Ray Emission) or ICP/MS (Inductively Coupled Plasma-Mass Spectrometry). Compared to control mice, the quantity of Ti in the exposed mice was not different. Consequently, we observed the solution of dissolved TiO2 ultrafine particles by Scanning Electron Microscope, and observed the particles which aggregated. That diameter was about 1 microm. We concluded that the particles had aggregated before administration to mice, so they didn't invade the blood vessels or organs from the pulmonary alveolus in the lung.

Modeling and identifying the sources of radiocesium contamination in separate sewerage systems.

The Fukushima Dai-ichi nuclear power plant accident released radiocesium in large amounts. The released radionuclides contaminated much of the surrounding environment, including sewers in urban areas of Fukushima prefecture. In this study we attempted to identify and quantify the sources of radiocesium contamination in separate sewerage systems and developed a compartment model based on the Radionuclide Migration in Urban Environments and Drainage Systems (MUD) model. Measurements of the time-dependent radiocesium concentration in sewer sludge combined with meteorological, demographic, and radiocesium dietary intake data indicated that rainfall-derived inflow and infiltration (RDII) and human excretion were the chief contributors of radiocesium contamination in a separate sewerage system. The quantities of contamination derived from RDII and human excretion were calculated and used in the modified MUD model to simulate radiocesium contamination in sewers in three urban areas in Fukushima prefecture: Fukushima, Koriyama, and Nihonmatsu Cities. The Nash efficiency coefficient (0.88-0.92) and determination coefficient (0.89-0.93) calculated in an evaluation of our compartment model indicated that the model produced satisfactory results. We also used the model to estimate the total volume of sludge with radiocesium concentrations in excess of the clearance level, based on the number of months elapsed after the accident. Estimations by our model suggested that wastewater treatment plants (WWTPs) in Fukushima, Koriyama, and Nihonmatsu generated about 1,750,000m3 of radioactive sludge in total, a level in good agreement with the real data.

Exposure assessment of carbon nanotubes at pilot factory focusing on quantitative determination of catalytic metals.

OBJECTIVES: The application of multiwall carbon nanotubes (MWCNTs) currently extends to various fields. However, it has been reported that exposure to CNT causes hazardous effects on animals and cells. The purpose of this study was to quantify the exposure to MWCNT in MWCNT/polymer composites for exposure assessment. We focused on catalytic metals included in the MWCNT and the diameter of dust released during the working processes. Although the Co in MWCNTs is not a common catalyst, it was used as a tracer in this study. METHODS: A field survey was conducted in a MWCNT/polymer composite pilot factory. Airborne MWCNTs were monitored using black carbon monitors (BCMs) and optical particle sizers (OPSs) and collected on a filter. The MWCNT powder, all polymer resins used during the working processes, and the filter were analyzed in our lab using inductively coupled plasma mass spectrometry (ICP-MS) and electron microscopic observation. RESULTS: The mean concentration of airborne MWCNT contained in the collected dust was 0.92 µg/m3 a few meters away from the extruder during the working processes (using elemental analysis). The maximum concentration measured using BCMs was shown to be seven times higher than the base concentration during the pelletizing process of polycarbonate (PC) and MWCNT composites. However, free, isolated, and unbound agglomerated MWCNTs were not detected using scanning electron microscopic (SEM) observation. CONCLUSIONS: The result obtained by elemental analysis indicated it was possible to quantify MWCNT in composites. The mean concentration at this factory was lower than the recommended exposure limit. However, additional studies during the pelletizing process are required in the future.

Effect of surfactants on the aggregation and sedimentation of zinc oxide nanomaterial in natural water matrices.

The wide application of surfactants and engineered nanomaterials (ENMs) in industrial and consumer products lead to the high possibility of their co-presence in natural water environment, making it important to study the effect of surfactants on the environmental behavior and fate of ENMs. In this work, we selected an anionic sodium dodecyl sulfate (SDS) and a nonionic nonylphenol ethoxylate (NPEO, Tergitol NP-9) to study their effects on the aggregation and sedimentation of a 20nm ZnO ENM in different water matrices. The adsorption of SDS and NP-9 by ZnO ENM were fitted with Langmuir model, and the maximum adsorption capacities were 43.73±4.62mg/g and 13.79±1.09 respectively. As the surfactant concentration increased from 0 to 0.030% (m:v), SDS reduced the zeta potential of ZnO ENM from 17.56±2.13 to -27.96±2.59mV, whereas NP-9 did not affect the zeta potential. After a 24-h batch reactor experiment, SDS and NP-9 reduced 93.02% and 80.26% of the aggregate size of ZnO ENM (50mgL-1) in maximum at surfactant concentrations≥0.015%. The ZnO ENM was not stable in natural aqueous matrices, mainly because of the relatively high ionic strength. However, surfactants were found to reduce the aggregation and sedimentation of ZnO ENM in six natural water matrices in different degrees. With the presence of 0.030% SDS in tap water, maximum reduction rates of aggregate size and sedimentation were recorded as 69.54% and 26.69%, respectively. The results of this study indicate that the presence of surfactants may alter the behaviors and fate of ENMs in natural water environment.

Effect of surfactants on the aggregation and stability of TiO2 nanomaterial in environmental aqueous matrices.

The high likelihood of the coexistence of surfactants and engineered nano-materials (ENMs) in aqueous environments redoubles the need to study the effects of surfactants on the behavior and transport of nano-materials. In this study, we chose anionic sodium dodecyl sulfate (SDS) and nonionic nonylphenol ethoxylate (NPEO, Tergitol NP-9) to study the effect of surfactants on the behaviors of a typical TiO2 ENM in water environment. An adsorption isotherm and zeta potential study showed that both surfactants could be adsorbed onto the surface of nano-TiO2 but that only SDS can significantly decrease the zeta potential of TiO2. For a better simulation of the dynamic natural water environment, we conducted a 24-h batch experiment to study the aggregation behaviors of nano-TiO2 in the presence of SDS or NP-9 surfactants and recorded the sedimentation of the aggregates in solutions containing the surfactants over a 24h-period. SDS and NP-9 both reduced the growth of the TiO2 aggregates and retarded the aggregate sedimentation at surfactant concentrations ≥0.015% (w:v). The aggregation of TiO2 was far more remarkable in six environmental water matrices from different natural origins than in Milli-Q water, mainly because of the relatively high ionic strength of the former. The introduction of surfactants, however, still retarded the aggregation and sedimentation of TiO2 in the six environmental water matrices. SDS exerted a stronger reductive effect than NP-9. This study reveals that the presence of surfactants may increase the bioavailability and environmental risk of nanomaterial contaminants by retarding the aggregation and promoting the transport of nanomaterials in natural aqueous environments.

Characterization and source profiling of volatile organic compounds in indoor air of private residences in Selangor State, Malaysia.

Volatile Organic Compounds (VOCs) in indoor air were investigated at 39 private residences in Selangor State, Malaysia to characterize the indoor air quality and to identify pollution sources. Twenty-two VOCs including isomers (14 aldehydes, 5 aromatic hydrocarbons, acetone, trichloroethylene and tetrachloroethylene) were collected by 2 passive samplers for 24h and quantitated using high performance liquid chromatography and gas chromatography mass spectrometry. Source profiling based on benzene/toluene ratio as well as statistical analysis (cluster analysis, bivariate correlation analysis and principal component analysis) was performed to identify pollution sources of the detected VOCs. The VOCs concentrations were compared with regulatory limits of air quality guidelines in WHO/EU, the US, Canada and Japan to clarify the potential health risks to the residents. The 39 residences were classified into 2 groups and 2 ungrouped residences based on the dendrogram in the cluster analysis. Group 1 (n=30) had mainly toluene (6.87±2.19µg/m3), formaldehyde (16.0±10.1µg/m3), acetaldehyde (5.35±4.57µg/m3) and acetone (11.1±5.95µg/m3) at background levels. Group 2 (n=7) had significantly high values of formaldehyde (99.3±10.7µg/m3) and acetone (35.8±12.6µg/m3), and a tendency to have higher values of acetaldehyde (23.7±13.5µg/m3), butyraldehyde (3.35±0.41µg/m3) and isovaleraldehyde (2.30±0.39µg/m3). The 2 ungrouped residences showed particularly high concentrations of BTX (benzene, toluene and xylene: 235µg/m3 in total) or acetone (133µg/m3). The geometric mean value of formaldehyde (19.2µg/m3) exceeded an 8-hour regulatory limit in Canada (9µg/m3), while those in other compounds did not exceed any regulatory limits, although a few residences exceeded at least one regulatory limit of benzene or acetaldehyde. Thus, the VOCs in the private residences were effectively characterized from the limited number of monitoring, and the potential health risks of the VOCs exposure, particularly formaldehyde, should be considered in the study area.

Occurrence, fate and environmental risk of linear alkylbenzene sulfonate in the Langat and Selangor River basins, Malaysia.

Five homologs (C10-C14) of linear alkylbenzene sulfonate (LAS) were quantitated in surface water collected in the Langat and Selangor River basins using liquid chromatography-tandem mass spectrometry (LC-MS/MS). A geographic information system (GIS) was used to spatially analyze the occurrence of LAS in both river basins, and the LAS contamination associated with the population was elucidated by spatial analysis at a sub-basin level. The LAS concentrations in the dissolved phase (<0.45 µm) and 4 fractions separated by particle size (<0.1 µm, 0.1-1 µm, 1-11 µm and >11 µm) were analyzed to elucidate the environmental fate of LAS in the study area. The environmental risks of the observed LAS concentration were assessed based on predicted no effect concentration (PNEC) normalized by a quantitative structure-activity relationship model. The LAS contamination mainly occurred from a few populated sub-basins, and it was correlated with the population density and ammonia nitrogen. The dissolved phase was less than 20% in high contamination sites (>1000 µg/L), whereas it was more than 60% in less contaminated sites (<100 µg/L). The environmental fate of LAS in the study area was primarily subject to the adsorption to suspended solids rather than biodegradation because the LAS homologs, particularly in longer alkyl chain lengths, were considerably absorbed to the large size fraction (>11 µm) that settled in a few hours. The observed LAS concentrations exceeded the normalized PNEC at 3 sites, and environmental risk areas and susceptible areas to the LAS contamination were spatially identified based on their catchment areas.

Aggregation is a critical cause of poor transfer into the brain tissue of intravenously administered cationic PAMAM dendrimer nanoparticles.

Dendrimers have been expected as excellent nanodevices for brain medication. An amine-terminated polyamidoamine dendrimer (PD), an unmodified plain type of PD, has the obvious disadvantage of cytotoxicity, but still serves as an attractive molecule because it easily adheres to the cell surface, facilitating easy cellular uptake. Single-photon emission computed tomographic imaging of a mouse following intravenous injection of a radiolabeled PD failed to reveal any signal in the intracranial region. Furthermore, examination of the permeability of PD particles across the blood-brain barrier (BBB) in vitro using a commercially available kit revealed poor permeability of the nanoparticles, which was suppressed by an inhibitor of caveolae-mediated endocytosis, but not by an inhibitor of macropinocytosis. Physicochemical analysis of the PD revealed that cationic PDs are likely to aggregate promptly upon mixing with body fluids and that this prompt aggregation is probably driven by non-Derjaguin-Landau- Verwey-Overbeek attractive forces originating from the surrounding divalent ions. Atomic force microscopy observation of a freshly cleaved mica plate soaked in dendrimer suspension (culture media) confirmed prompt aggregation. Our study revealed poor transfer of intravenously administered cationic PDs into the intracranial nervous tissue, and the results of our analysis suggested that this was largely attributable to the reduced BBB permeability arising from the propensity of the particles to promptly aggregate upon mixing with body fluids.

Biodistribution of gold nanoparticles in mice and investigation of their possible translocation by nerve uptake around the alveolus.

The effect of nanoparticles in the environment on our health is a cause of concern. The greatest concern with respect to the biological effect of nanoparticles is that they remain in the body and invade tissues, overcoming the protective mechanisms of the body. It is generally believed that nanoparticles invading a living body move into the blood and are carried by the bloodstream to all organs. However, some studies have shown that the inhaled nanoparticles directly translocate to the central nervous system by nerve uptake. Here quantification of the amount of migration of nanoparticles to organs in short time spans (1, 3, and 6 hr) was attempted by animal experiments. Furthermore, the possibility of migration of nanoparticles through the nerves that project around the alveolus, including the nodose ganglion and dorsal root ganglion (DRG), was investigated. Gold (Au) nanoparticles (15 nm) were administered to mice by intratracheal instillation and tail vein injection. After tail vein injection, most nanoparticles were distributed in the liver. After intratracheal instillation, approximately 80% of detected nanoparticles remained in the lungs at 1 hr and were believed to be translocated to digestive organs, including the stomach and intestine, at 3 and 6 hr. With respect to quantification in ganglia, the levels in most samples were lower than the limit of quantification of inductively coupled plasma mass spectrometry (ICP-MS). However, Au nanoparticles were detected in DRG in only some samples of intratracheal instillation. Therefore, this suggests the possibility of translocation of nanoparticles to DRG via nerves.

Future projection of radiocesium flux to the ocean from the largest river impacted by Fukushima Daiichi Nuclear Power Plant.

Following the initial fall out from Fukushima Dai-ichi Nuclear Power Plant (FDNPP), a significant amount of radiocesium has been discharged from Abukuma River into the Pacific Ocean. This study attempted to numerically simulate the flux of radiocesium into Abukuma River by developing the multiple compartment model which incorporate the transport process of the radionuclide from the ground surface of the catchment area into the river, a process called wash off. The results from the model show that the sub-basins with a high percentage of forest area release the radionuclides at lower rate compared to the other sub-basins. In addition the results show that the model could predict the seasonal pattern of the observed data. Despite the overestimation observed between the modeled data and the observed data, the values of R(2) obtained from (137)Cs and (134)Cs of 0.98 and 0.97 respectively demonstrate the accuracy of the model. Prediction of the discharge from the basin area for 100 years after the accident shows that, the flux of radiocesium into the Pacific Ocean is still relatively high with an order of magnitude of 10(9) bq.month(-1) while the total accumulation of the discharge is 111 TBq for (137)Cs and 44 TBq for (134)Cs.