Fumikazu Ikemori

Sulfate Aerosol as a Potential Transport Medium of Radiocesium from the Fukushima Nuclear Accident

To date, areas contaminated by radionuclides discharged from the Fukushima Dai-ichi nuclear power plant accident have been mapped in detail. However, size of the radionuclides and their mixing state with other aerosol components, which are critical in their removal from the atmosphere, have not yet been revealed. We measured activity size distributions of (134)Cs and (137)Cs in aerosols collected 47 days after the accident at Tsukuba, Japan, and found that the activity median aerodynamic diameters of (134)Cs and (137)Cs in the first sample (April 28-May 12) were 0.54 and 0.53 μm, respectively, and those in the second sample (May 12-26) were both 0.63 μm. The activity size distributions of these radiocesium were within the accumulation mode size range and almost overlapped with the mass size distribution of non-sea-salt sulfate aerosol. From the analysis of other aerosol components, we found that sulfate was the potential transport medium for these radionuclides, and resuspended soil particles that attached radionuclides were not the major airborne radioactive substances at the time of measurement. This explains the relatively similar activity sizes of radiocesium measured at various sites during the Chernobyl accident. Our results can serve as basic data for modeling the transport/deposition of radionuclides.

Local and seasonal variations in concentrations of chlorinated polycyclic aromatic hydrocarbons associated with particles in a Japanese megacity.

Concentrations of particle-bound polycyclic aromatic hydrocarbons (PAHs) and chlorinated PAHs (ClPAHs) were measured in different seasons at five sampling stations in Nagoya, a Japanese megacity. The annual mean total ClPAH and total PAH concentrations were 43.3-92.6pg/m(3) and 5200-8570pg/m(3), respectively. The concentrations of total ClPAHs were significantly variable than those of total PAHs, and both total concentrations through the seasons did not significantly correlate at any of the stations. Principal component analysis was used to characterize the ClPAH sources, resulted that ClPAHs were found to be associated with the sources of high-molecular-weight PAHs in the warmer seasons and of low-molecular-weight PAHs in the colder seasons. These findings suggest that principal sources of particle-bound ClPAHs are present in the local area, and change in the seasons. Toxic equivalent (TEQ) concentrations were estimated to assess the risks associated with exposure to ClPAHs in air. The TEQ concentrations in the samples were 0.05-0.32pg-TEQ/m(3). The TEQ concentrations in summer were approximately half the TEQ concentrations in the other seasons at all of the stations.

Optimisation of pre-treatment and ionisation for GC/MS analysis for the determination of chlorinated PAHs in atmospheric particulate samples

Chlorinated polycyclic aromatic hydrocarbons (ClPAHs) have been discovered to represent ubiquitous environmental pollutants in the last decade. In the present study, sample pre-treatment and ionisation conditions associated with the gas chromatography/mass spectrometry (GC/MS) analysis of ClPAHs were evaluated. The optimal pre-treatment of ambient air particulate samples was achieved using fractionation over silica gel with 10% dichloromethane in n-hexane as the eluent. The optimised condition of GC/MS with electron impact ionisation permitted analysis of all target ClPAHs. Not all target ClPAHs were detected using GC/MS with negative chemical ionisation, although this technique exhibited greater sensitivity for several of the compounds compared to electron impact ionisation. The analytical method was applied to the survey of ClPAHs in atmospheric particulate matter obtained close to an industrial site and in a standard sample of tunnel dust. Fourteen and eighteen species of ClPAHs were detected in the industrial air samples and tunnel dust, respectively, confirming the capability of the method. The compositions of ClPAHs were significantly different between air samples and tunnel dust. It suggests that alternative emission sources rather than vehicle exhaust could play a significant role in the air.

Associations Between Fine Particulate Matter Components and Daily Mortality in Nagoya, Japan

BACKGROUNDnSeasonal variation and regional heterogeneity have been observed in the estimated effect of fine particulate matter (PM2.5) mass on mortality. Differences in the chemical compositions of PM2.5 may cause this variation. We investigated the association of the daily concentration of PM2.5 components with mortality in Nagoya, Japan.nnnMETHODSnWe combined daily mortality counts for all residents aged 65 years and older with concentration data for PM2.5 mass and components in Nagoya from April 2003 to December 2007. A time-stratified case-crossover design was used to examine the association of daily mortality with PM2.5 mass and each component (chloride, nitrate, sulfate, sodium, potassium, calcium, magnesium, ammonium, elemental carbon [EC], and organic carbon [OC]).nnnRESULTSnWe found a stronger association between mortality and PM2.5 mass in transitional seasons. In analysis for each PM2.5 component, sulfate, nitrate, chloride, ammonium, potassium, EC, and OC were significantly associated with mortality in a single-pollutant model. In a multi-pollutant model, an interquartile range increase in the concentration of sulfate was marginally associated with an increase in all-cause mortality of 2.1% (95% confidence interval, -0.1 to 4.4).nnnCONCLUSIONSnThese findings suggest that some specific PM components have a more hazardous effect than others and contribute to seasonal variation in the health effects of PM2.5.

Influence of contemporary carbon originating from the 2003 Siberian forest fire on organic carbon in PM2.5 in Nagoya, Japan.

In May 2003, high concentrations of organic carbon (OC) in PM2.5 were measured in Nagoya, a representative metropolitan area in Japan. To investigate the influence of possible forest fires on PM2.5 in Japan via long-range aerosol transport, the radiocarbon ((14)C) concentrations of PM2.5 samples from April 2003 to March 2004 were measured. (14)C concentrations in total carbon (TC) from May to early June showed higher values than those in other periods. The OC/elemental carbon (EC) ratios from May to early June were also significantly higher than the ones in other periods. In addition, OC concentrations from May to early June were typically high. These results indicate that the abundant OC fraction from May to early June in Nagoya consisted predominantly of contemporary carbon. Furthermore, simulations of diffusion and transport of organic matter (OM) in East Asia showed that abundant OM originating from East Siberia spread over East Asia and Japan in May and early June. Backward air mass trajectories from this time frame indicate that the air mass in Nagoya likely first passed through East Siberia where fire events were prevalent. However, the backward trajectories showed that the air mass after early June did not originate mainly from Siberia, and correspondingly, the (14)C and OC concentrations showed lower values than those from May to early June. Therefore, the authors conclude that contemporary carbon originating from the forest fire in East Siberia was transported to Nagoya, where it significantly contributed to the high observed concentrations of both OC and (14)C.

Weak size dependence of resuspended radiocesium adsorbed on soil particles collected after the Fukushima nuclear accident.

Most studies of the properties of airborne radionuclides emitted from the Fukushima Daiichi Nuclear Power Plant have focused on the relatively early stages of the accident, and little is known about the characteristics of radiocesium in the long-term. In this study, we analyzed activity size distributions of airborne radiocesium collected over 5 months in Tsukuba, Japan. Radiocesium in the accumulation mode size range (0.1-2xa0μm in aerodynamic diameter) was overwhelming in the early aerosol samples and decreased with time, while that associated with coarse aerosols remained airborne. We examined the radiocesium adsorbed onto airborne soil particles, and found that the size dependence of 137Cs surface density adsorbed on soil particles was weak. That is, radiocesium was distributed homogeneously throughout the aerodynamic diameter range of 2.1-11xa0μm. This characteristic may be related to the reported structure of radiocesium-bearing soil particles collected from the ground, which consisted of an aggregate of specific clay minerals and other non-cesium adsorbing particles. The resuspension factors for the first two aerosol samples collected during late April and May 2011 were close to those in European cities in the months following the Chernobyl accident, despite different soil and weather conditions.

Source apportionment of chlorinated polycyclic aromatic hydrocarbons associated with ambient particles in a Japanese megacity

Chlorinated polycyclic aromatic hydrocarbons (ClPAHs) are novel species of environmental contaminants whose possible sources remain unclear. The occurrence of ClPAHs within total suspended particles (TSP) is compared with weekly air samples at two sites of differing characteristics (industrial and residential) in the megacity of Nagoya, Japan. Samples were collected over 12 months during 2011–2012. All 24 species of targeted ClPAHs were detected at both industrial and residential sites, where mean concentrations of total ClPAHs in TSP were 20.7 and 14.1u2009pg/m3, respectively. High concentrations at the industrial site were frequently observed during winter, suggesting potent seasonal ClPAH sources there. Positive matrix factorization modeling of particulate ClPAH source identification and apportioning were conducted for datasets including ClPAHs, PAHs, elements and ions, plus elemental carbons in TSP. Eight factors were identified as possible ClPAH sources, with estimates that the dominant one was a specific source of ClPAH emission (31%), followed by traffic (23%), photodegradable and semi-volatile species (18%), long-range transport (11%), and industry and oil combustion (10%). Source contributions of ClPAHs differed substantially from those of PAHs. This suggests specific and/or potent ClPAH sources in the local area, and that the production mechanisms between ClPAHs and PAHs are substantially different.

Distributions and multiple sources of chlorinated polycyclic aromatic hydrocarbons in the air over Japan

Chlorinated polycyclic aromatic hydrocarbons (ClPAHs) have been detected in the air at discrete sites in Japan, but there is no information on their distributions throughout Japan. This study was a widespread survey of atmospheric concentrations of ClPAHs throughout Japan. The majority of 24 species of ClPAHs were detected in either the gas or particle phase at all sampling sites. The concentrations were weakly related to human population densities. The relationships between total concentrations of ClPAHs and PAHs suggested that atmospheric ClPAHs at ~70% of the sites were derived from common sources of PAHs. A ternary diagram based on diagnostic ratios of 1-chloropyrene, 7-chlorobenz[a]anthracene, and 6-chlorobenzo[a]pyrene normalized to 3-chlorofluoranthene suggested that waste combustion was the likely source of ClPAHs in summer and that vehicular emissions and coal burning were the likely sources of ClPAHs in winter. A heat map analysis estimated from the concentrations of individual compounds at each site suggested that there were three categories of sources at the sites: i) common sources of ClPAHs and PAHs that had moderate impacts, ii) common sources of ClPAHs and PAHs that had high impacts, and iii) specific sources of ClPAHs.