Size-classified aerosol-bound heavy metals and their effects on human health risks in industrial and remote areas in Japan.

Airborne aerosols were collected in six size classes (PM<0.1, PM0.1-0.5, PM0.5-1, PM1-2.5, PM2.5-10 and PM>10) to investigate aerosol health risks in remote and industrial areas in Japan. We focused on heavy metals and their water-dispersed fractions. The average concentration of heavy metals was 18 ± 25-86 ± 48 ngm-3 for PM<0.1, 46 ± 19-154 ± 80 for PM0.5-1 ngm-3, 98 ± 49-422 ± 186 ngm-3 for PM1-2.5, 321 ± 305-1288 ± 727 ngm-3 for PM2.5-10 and 65 ± 52-914 ± 339 ngm-3 or PM>10, and these concentrations were higher in industrial areas. Heavy metals emitted from domestic anthropogenic sources were added to the long-range transport component of the aerosols. The water-dispersed fraction of heavy metals contained 3.3-40.1% of the total heavy metals in each size class. The relative contribution of Zn and other species (As, Cd, Cr, Ni, Pb, Mn, V and Cu) increased in the water-dispersed fraction. Smaller particles contained greater proportions of the water-dispersed heavy metal fraction. Carcinogenic risk (CR) and the hazard index (HI) were estimated for each size class. The CR of carcinogens was at acceptable levels (<1 ×10-6) for five particle size fractions. The HI values for carcinogens and noncarcinogens were also below acceptable levels (<1) for the same five size fractions. The estimated CR and HI values were dominated by contributions from the inhalation process.

Copper in airborne fine particulate matter (PM2.5) from urban sites causes the upregulation of pro-inflammatory cytokine IL-8 in human lung epithelial A549 cells.

Fine atmospheric particles, such as PM2.5, are strongly related to the onset and exacerbation of inflammatory responses leading to the development of respiratory and cardiovascular diseases. PM2.5 is a complex mixture of tiny particles with different properties (i.e., size, morphology, and chemical components). Moreover, the mechanism by which PM2.5 induces inflammatory responses has not been fully elucidated. Therefore, it is necessary to determine the composition of PM2.5 to identify the main factors causing PM2.5-associated inflammation and diseases. In the present study, we investigated PM2.5 from two sites (Fukue, a remote monitoring site, and Kawasaki, an urban monitoring site) with greatly different environments and PM2.5 compositions. The results of ICP-MS and EDX-SEM indicated that PM2.5 from Kawasaki contained more metals and significantly induced the expression of the pro-inflammatory cytokine gene IL-8 compared to the PM2.5 from Fukue. We also verified the increased secretion of IL-8 protein from exposure to PM2.5 from Kawasaki. We further investigated their effects on inflammatory response and cytotoxicity using metal nanoparticles (Cu, Zn, and Ni) and ions and found that the Cu nanoparticles caused a dose-dependent increase in IL-8 expression together with significant cell death. We also found that Cu nanoparticles enhanced the secretion of IL-8 protein. These results suggest that Cu in PM2.5 is involved in lung inflammation.

Benzo[a]pyrene induces NLRP1 expression and promotes prolonged inflammasome signaling.

Benzo[a]pyrene (BaP), a polycyclic aromatic hydrocarbon in the air, triggers pulmonary inflammation. This study focused on BaP-induced inflammation in the alveolar epithelium. A549 cells were stimulated with BaP for four days. BaP treatment markedly increased NLRP1 expression but slightly decreased NLRP3. Furthermore, aryl hydrocarbon receptor (AhR) knockdown displayed no increase in BaP-induced NLRP1 expression. Similar results were also observed by blocking reactive oxygen species (ROS), which is mediated through AhR, suggesting that the AhR-ROS axis operates in BaP-induced NLRP1 expression. p53 involvement in ROS-mediated NLRP1 induction has also been implied. When we confirmed inflammasome activation in cells treated with BaP for four days, while BaP transiently activated NLRP3, it predominantly activated the NLRP1 inflammasome. These findings have led to the conclusion that BaP could be a potential ligand for the NLRP1 inflammasome persistently observed in the lung epithelium. Our study may provide additional evidence for the sustained pulmonary inflammation caused by environmental air pollution.

Origin of surface water in the Southern Ocean: Implications of soluble radionuclide distributions.

Concentration data of soluble radionuclides in the southern South Indian Ocean and Southern Ocean transition zone are rare or insufficient for the study of its current system. We examined the lateral surface variations in soluble natural (226Ra and 228Ra) and anthropogenic (134Cs and 137Cs) radionuclide activity concentrations in the surface waters in this area from November 2021 to March 2022. The surface distributions of 226Ra and 137Cs concentrations were classified into Subantarctic Mode Water-, Antarctic Intermediate Water-, and Upper Circumpolar Deep Water (UCDW)-dominated areas along latitudinal band (40°S-65°S, 110°E-120°E). Notably, the highest 226Ra concentrations occurred along the longitudinal band (60°S-65°S, 40°E-120°E). Significantly lower 137Cs concentrations in the Southern Ocean than those in surface waters in other global oceans were observed along with depletion of 228Ra. Additionally, 226Ra and 137Cs concentrations appeared to show small variations between eastern and western areas (2.5-3.0 mBq/L and 0.06-0.03 mBq/L, respectively). Lateral profiles in the Southern Ocean are governed by a large contribution from deep/old waters (e.g., UCDW), with a small effect from southward transport of Subantarctic Mode Water.

Calculating source contributions to urban atmospheric polycyclic aromatic hydrocarbons and nitropolycyclic aromatic hydrocarbons using 1-nitropyrene and pyrene: An application to an Asian dust event.

A method to calculate source contributions to atmospheric polycyclic aromatic hydrocarbons (PAHs) and their nitrated congeners (NPAHs) is proposed, using pyrene (Pyr) and 1-nitropyrene (1-NP), as respective representatives of PAHs and NPAHs. This is based on the known increases in NPAH to PAH ratios as combustion temperatures increase. The fractions of 1-NP and Pyr from high temperature combustion sources in total 1-NP and Pyr are respectively calculated as a (0 < a <1) and b (0 < b < 1). By using atmospheric concentrations of Pyr and 1-NP obtained at monitoring sites, contributions of high and low temperature combustion sources were calculated. Using this method, the contributions of automobiles and coal combustion facilities/industries to atmospheric Pyr and 1-NP concentrations were calculated for atmospheric samples collected in Kanazawa, Japan during a seasonal Asian dust event. The results show that Pyr was almost entirely emitted from industries in China and transported long-range to Japan. By contrast, 1-NP was emitted primarily from automobiles in Kanazawa and its surrounding areas, with a small amount of 1-NP possibly transported from China. The proposed method can provide greater clarity on source identification compared to the typically used PAH isomer pairs.

Mass balance and latest fluxes of radiocesium derived from the fukushima accident in the western North Pacific Ocean and coastal regions of Japan.

This article summarizes and discusses mass balance calculations of the activities of Fukushima-derived 137Cs released to the atmosphere and ocean prior to 2018 as well as the 137Cs inventories on land and in the ocean, biota, and sediment. We propose that the consensus value of the total amount of 137Cs released to the atmosphere was 15-21 PBq; atmospheric deposition of 137Cs on land was 3-6 PBq; atmospheric deposition of 137Cs on the North Pacific was 12-15 PBq; and direct discharge of 137Cs to the ocean was 3-6 PBq. We also evaluated the movement of 137Cs from one domain to another for several years after the accident. We calculated that the amount of 137Cs transported by rivers might be 40 TBq. The annual deposition of 137Cs due to resuspension at Okuma during the period 2014-2018 was 4-10 TBq year-1. The 137Cs discharged to the ocean was 0.73-1.0 TBq year-1 in 2016-2018. The integrated amount of FNPP1-derived 137Cs that entered the Sea of Japan from the Pacific Ocean from 2011 until 2017 was 270 ± 20 TBq, 6.4% of the estimated amount of FNPP1-derived 137Cs in Subtropical Mode Water in the North Pacific. The integrated amount of FNPP1-derived 137Cs that returned to the North Pacific Ocean through the Tsugaru Strait from the Sea of Japan was 110 ± 10 TBq. Decontamination efforts removed 134 TBq of 137Cs from surface soil prior to February 2019, an amount that corresponded to 4% of the137Cs deposited on land in Japan.

Radiocaesium derived from the TEPCO Fukushima accident in the North Pacific Ocean: Surface transport processes until 2017.

We report temporal variations of 137Cs activity concentrations in surface waters of six regions of the western and central North Pacific Ocean during 2011-2017 using a combination of 1264 previously published data and 42 new data. In the western and central North Pacific Ocean at latitudes of 30-42°N and longitudes of 140°E to 160°W, eastward transport of radiocaesium was clearly apparent. 137Cs activity concentrations in surface water decreased rapidly to ∼2-3 Bq m-3 in 2015/2016, still a bit higher than 137Cs activity concentrations before the FNPP1 accident (1.5-2 Bq m-3). 134Cs/137Cs activity ratios decay-corrected to 11 March 2011 were ∼0.5-0.8. To the south of 30°N and between 130°E and 160°W in the western and central Pacific Ocean, 137Cs activity concentrations were around 1-7 Bq m-3 in 2011/2012 but then stabilized at a few Bq m-3 up to 2017.134Cs activity concentrations were detected at levels of 0.1-0.9 Bq m-3, and 134Cs/137Cs activity ratios decay-corrected to 11 March 2011 were ∼0.3-0.5. Temporal variations of model-simulated 137Cs activity concentrations in surface water in the region of interest showed good agreement with observations, except in the southwestern North Pacific Ocean.

Source-Receptor Relationship Analysis of the Atmospheric Deposition of PAHs Subject to Long-Range Transport in Northeast Asia.

The source-receptor relationship analysis of PAH deposition in Northeast Asia was investigated using an Eulerian regional-scale aerosol chemical transport model. Dry deposition (DD) of PAH was controlled by wind flow patterns, whereas wet deposition (WD) depended on precipitation in addition to wind flow patterns. The contribution of WD was approximately 50-90% of the total deposition, except during winter in Northern China (NCHN) and Eastern Russia (ERUS) because of the low amount of precipitation. The amount of PAH deposition showed clear seasonal variation and was high in winter and low in summer in downwind (South Korea, Japan) and oceanic-receptor regions. In the downwind region, the contributions from NCHN (WD 28-52%; DD 54-55%) and Central China (CCHN) (WD 43-65%; DD 33-38%) were large in winter, whereas self-contributions (WD 20-51%; DD 79-81%) were relatively high in summer. In the oceanic-receptor region, the deposition amount decreased with distance from the Asian continent. The amount of DD was strongly influenced by emissions from neighboring domains. The contributions of WD from NCHN (16-20%) and CCHN (28-35%) were large. The large contributions from China in summer to the downwind region were linked to vertical transport of PAHs over the Asian continent associated with convection.

Recirculation of FNPP1-derived radiocaesium observed in 2015/2016 in coastal regions of Japan.

We conducted enhanced surface water sampling at more than 80 stations in coastal regions on both the Japan Sea and Pacific Ocean sides of Japan in winter 2015/2016 to examine the recirculation behaviour of FNPP1-derived radiocaesium in the surface layer 5 years after the 2011 FNPP1 accident. We found that a small part of the FNPP1-derived radiocaesium had already recirculated in the surface layer and reached the Japanese coast.

Transboundary transport of anthropogenic sulfur in PM2.5 at a coastal site in the Sea of Japan as studied by sulfur isotopic ratio measurement.

Sulfur isotopic ratios (δ(34)S) in size separated aerosol particles (PM2.5 and coarse particles) were measured at Niigata-Maki facing the Sea of Japan. Non-sea salt δ(34)S (δ(34)Snss) in PM2.5 showed seasonal variations with relatively high values in winter (1.0-3.9‰ in spring, 2.8-4.5‰ in summer, 1.3-4.5‰ in autumn, 3.7-5.7‰ in winter). Taking into consideration air mass transport routes, δ(34)Snss in the air masses which originated in the Asian continent and were transported over the Sea of Japan to the monitoring sites were higher than those values for air masses which were transported over the Japanese islands after leaving the Asian continent for each season. Considering that the δ(34)Snss in sulfuric acid derived from domestic emissions in Japan are lower than those of δ(34)Snss in coal, the lower δ(34)Snss for the air mass transported over the Japanese islands suggest that sulfuric acid in PM2.5 modified the δ(34)Snss due to aerosol mixing with sulfuric acid in Japan. Material balance calculations suggested that the relative contribution of transboundary transport in winter was also higher than for other seasons (40-75% in spring, 51-63% in summer, 45-73% in autumn, and 53-81% in winter). In particular, the contribution to the air masses which were transported directly from the Asian continent was relatively large (75% in spring, 59% in autumn, 78% in winter) in comparison with that for the air masses which were transported over Japan.

Source contribution analysis of surface particulate polycyclic aromatic hydrocarbon concentrations in northeastern Asia by source-receptor relationships.

We analyzed the source-receptor relationships for particulate polycyclic aromatic hydrocarbon (PAH) concentrations in northeastern Asia using an aerosol chemical transport model. The model successfully simulated the observed concentrations. In Beijing (China) benzo[a]pyren (BaP) concentrations are due to emissions from its own domain. In Noto, Oki and Tsushima (Japan), transboundary transport from northern China (>40 °N, 40-60%) and central China (30-40 °N, 10-40%) largely influences BaP concentrations from winter to spring, whereas the relative contribution from central China is dominant (90%) in Hedo. In the summer, the contribution from Japanese domestic sources increases (40-80%) at the 4 sites. Contributions from Japan and Russia are additional source of BaP over the northwestern Pacific Ocean in summer. The contribution rates for the concentrations from each domain are different among PAH species depending on their particulate phase oxidation rates. Reaction with O3 on particulate surfaces may be an important component of the PAH oxidation processes.

Emission and atmospheric transport of particulate PAHs in Northeast Asia.

The emission, concentration levels, and transboundary transport of particulate polycyclic aromatic hydrocarbons (PAHs) in Northeast Asia were investigated using particulate PAH measurements, the newly developed emission inventory (Regional Emission inventory in ASia for Persistent Organic Pollutants version, REAS-POP), and the chemical transport model (Regional Air Quality Model ver2 for POPs version, RAQM2-POP). The simulated concentrations of the nine particulate PAHs agreed well with the measured concentrations, and the results firmly established the efficacy of REAS/RAQM2-POP. It was found that the PAH concentrations in Beijing (China, source region), which were emitted predominantly from domestic coal, domestic biofuel, and other transformations of coal (including coke production), were approximately 2 orders of magnitude greater than those monitored at Noto (Japan, leeward region). In Noto, the PAH concentrations showed seasonal variations; the PAH concentrations were high from winter to spring due to contributions from domestic coal, domestic biofuel, and other transformations of coal, and low in summer. In summer, these contribution were decrease, instead, other sources, such as the on-road mobile source, were relatively increased compared with those in winter. These seasonal variations were due to seasonal variations in emissions from China, as well as transboundary transport across the Asian continent associated with meteorological conditions.

Analysis of 50-y record of surface (137)Cs concentrations in the global ocean using the HAM-global database.

We investigated spatial and temporal variations in (137)Cs concentrations in the surface waters of the global ocean for the period from 1957 to 2005 using the "HAM database - a global version". Based on the 0.5-y average value of (137)Cs concentrations in the surface water in each sea area, we classified the temporal variations into four types. (1) In the North Pacific Ocean where there was high fallout from atmospheric nuclear weapons tests, the rates of decrease in the (137)Cs concentrations changed over the five decades: the rate of decrease from the 1950s to the 1970s was much faster than that after the 1970s, and the (137)Cs concentrations were almost constant after the 1990s. Latitudinal differences in (137)Cs concentrations in the North Pacific Ocean became small with time. (2) In the equatorial Pacific and Indian Oceans, the (137)Cs concentrations varied within a constant range in the 1970s and 1980s, suggesting the advection of (137)Cs from areas of high global fallout in the mid-latitudes of the North Pacific Ocean. (3) In the eastern South Pacific and Atlantic Oceans (south of 40 degrees S), the concentrations decreased exponentially over the five decades. (4) In the Arctic and North Atlantic Oceans, including marginal seas, (137)Cs concentrations were strongly controlled by discharge from nuclear reprocessing plants after the late 1970s. The apparent half-residence times of (137)Cs in the surface waters of the global ocean from 1970 to 2005 ranged from 4.5 to 36.8 years. The apparent half-residence times were longer in the equatorial region and shorter in the higher latitudes. There was no notable difference between the latitudinal distributions of the apparent half-residence times in the Pacific and Indian Oceans. These results suggest that (137)Cs in the North Pacific Ocean is transported to the equatorial, South Pacific, and Indian Oceans by the oceanic circulation.

Return period of enhanced gamma ray dose rates: regional differences observed in Japan.

We estimated the return period of an increased gamma ray dose rate (Delta gamma) derived from (222)Rn progeny deposited with precipitation. The approximate probability distribution for Delta gamma followed a Hazen plot, which is an empirical plotting equation, indicating that the distribution of Delta gamma was approximated by a nearly double-exponential. The distribution of Delta gamma was well represented by the Gumbel distribution, and the return period for Delta gamma was estimated theoretically. There was a notable regional difference in the return period between the coast of the Japan Sea and the inland or Pacific coast areas: the return period for a given Delta gamma at monitoring sites on the Sea of Japan coast was 1.5 to 2.5 times shorter than that in the inland or Pacific coast areas. This variation with locality suggests that the rate of wet-deposition of (222)Rn progeny is larger at sites on the Sea of Japan coast than inland or on the Pacific coast areas. The expected return period for the maximum Delta gamma at each site was about 10 years. This estimation of the return period of Delta gamma is a novel approach to the study of environmental science in fields such as radioactivity.