Assessing oxidative stress induction ability and oxidative potential of PM2.5 in cities in eastern and western Japan.

Oxidative stress is an important cause of respiratory diseases associated with exposure to PM2.5. Accordingly, acellular methods for assessing the oxidative potential (OP) of PM2.5 have been evaluated extensively for use as indicators of oxidative stress in living organisms. However, OP-based assessments only reflect the physicochemical properties of particles and do not consider particle-cell interactions. Therefore, to determine the potency of OP under various PM2.5 scenarios, oxidative stress induction ability (OSIA) assessments were performed using a cell-based method, the heme oxygenase-1 (HO-1) assay, and the findings were compared with OP measurements obtained using an acellular method, the dithiothreitol assay. For these assays, PM2.5 filter samples were collected in two cities in Japan. To quantitatively determine the relative contribution of the quantity of metals and subtypes of organic aerosols (OA) in PM2.5 to the OSIA and the OP, online measurements and offline chemical analysis were also performed. The findings showed a positive relationship between the OSIA and OP for water-extracted samples, confirming that the OP is generally well suited for use as an indicator of the OSIA. However, the correspondence between the two assays differed for samples with a high water-soluble (WS)-Pb content, which had a higher OSIA than would be expected from the OP of other samples. The results of reagent-solution experiments showed that the WS-Pb induced the OSIA, but not the OP, in 15-min reactions, suggesting a reason for the inconsistent relationship between the two assays across samples. Multiple linear regression analyses and reagent-solution experiments showed that WS transition metals and biomass burning OA accounted for approximately 30-40% and 50% of the total OSIA or the total OP of water-extracted PM2.5 samples, respectively. This is the first study to evaluate the association between cellular oxidative stress assessed by the HO-1 assay and the different subtypes of OA.

Chemokine expression in human 3-dimensional cultured epidermis exposed to PM2.5 collected by cyclonic separation.

Fine particulate matter (PM2.5) exposure has a risk of inducing several health problems, especially in the respiratory tract. The skin is the largest organ of the human body and is therefore the primary target of PM2.5. In this study, we examined the effects of PM2.5 on the skin using a human 3-dimensional cultured epidermis model. PM2.5 was collected by cyclonic separation in Yokohama, Japan. Global analysis of 34 proteins released from the epidermis revealed that the chemokines, chemokine C-X-C motif ligand 1 (CXCL1) and interleukin 8 (IL-8), were significantly increased in response to PM2.5 exposure. These chemokines stimulated neutrophil chemotaxis in a C-X-C motif chemokine receptor 2-dependent manner. The oxidative stress and signal transducer and activator of transcription 3 pathways may be involved in the increased expression of CXCL1 and IL-8 in the human epidermis model. Interestingly, in the HaCaT human keratinocyte cell line, PM2.5 did not affect chemokine expression but did induce IL-6 expression, suggesting a different effect of PM2.5 between the epidermis model and HaCaT cells. Overall, PM2.5 could induce the epidermis to release chemokines, followed by neutrophil activation, which might cause an unregulated inflammatory reaction in the skin.

Involvement of polycyclic aromatic hydrocarbons and endotoxin in macrophage expression of interleukin-33 induced by exposure to particulate matter.

Air pollutants are important factors that contribute to the development and/or exacerbation of allergic inflammation accompanied by asthma, but experimental evidence still needs to be collected. Interleukin 33 (IL-33) is closely involved in the onset and progression of asthma. In this study, we examined the effects of particulate matter (PM) on IL-33 expression in macrophages. PM2.5 collected in Yokohama, Japan by the cyclone device significantly induced IL-33 expression in human THP-1 macrophages, and the induction was clearly suppressed by pretreatment with the aryl hydrocarbon receptor (AhR) antagonist CH-223191 or the Toll-like receptor 4 (TLR4) antagonist TAK-242. PM2.5-induced IL-33 expression was significantly attenuated in AhR-knockout or TLR4-mutated macrophages, suggesting an important role of polycyclic aromatic hydrocarbons (PAHs) and endotoxin in IL-33 stimulation. PM samples derived from tunnel dust slightly but significantly induced IL-33 expression, while road dust PM did not affect IL-33 expression. The PAH concentration in tunnel dust was higher than that in road dust. Tunnel dust or road dust PM contained less endotoxin than PM2.5 collected in Yokohama. These data suggest that the potency of IL-33 induction could depend on the concentration of PAHs as well as endotoxin in PMs. Caution regarding PAHs and endotoxin levels in air pollutants should be taken to prevent IL-33-induced allergic inflammation.

Simulation of the transition metal-based cumulative oxidative potential in East Asia and its emission sources in Japan.

The aerosol oxidative potential (OP) is considered to better represent the acute health hazards of aerosols than the mass concentration of fine particulate matter (PM2.5). The proposed major contributors to OP are water soluble transition metals and organic compounds, but the relative magnitudes of these compounds to the total OP are not yet fully understood. In this study, as the first step toward the numerical prediction of OP, the cumulative OP (OPtm*) based on the top five key transition metals, namely, Cu, Mn, Fe, V, and Ni, was defined. The solubilities of metals were assumed constant over time and space based on measurements. Then, the feasibility of its prediction was verified by comparing OPtm* values based on simulated metals to that based on observed metals in East Asia. PM2.5 typically consists of primary and secondary species, while OPtm* only represents primary species. This disparity caused differences in the domestic contributions of PM2.5 and OPtm*, especially in large cities in western Japan. The annual mean domestic contributions of PM2.5 were 40%, while those of OPtm* ranged from 50 to 55%. Sector contributions to the OPtm* emissions in Japan were also assessed. The main important sectors were the road brake and iron-steel industry sectors, followed by power plants, road exhaust, and railways.

Modeling Transition Metals in East Asia and Japan and Its Emission Sources.

Emission inventories of anthropogenic transition metals, which contribute to aerosol oxidative potential (OP), in Asia (Δx = 0.25°, monthly, 2000-2008) and Japan (Δx = 2 km, hourly, mainly 2012) were developed, based on bottom-up inventories of particulate matters and metal profiles in a speciation database for particulate matters. The new inventories are named Transition Metal Inventory (TMI)-Asia v1.0 and TMI-Japan v1.0, respectively. It includes 10 transition metals in PM2.5 and PM10, which contributed to OP based on reagent experiments, namely, Cu, Mn, Co, V, Ni, Pb, Fe, Zn, Cd, and Cr. The contributions of sectors in the transition metals emission in Japan were also investigated. Road brakes and iron-steel industry are primary sources, followed by other metal industry, navigation, incineration, power plants, and railway. In order to validate the emission inventory, eight elements such as Cu, Mn, V, Ni, Pb, Fe, Zn, and Cr in anthropogenic dust and those in mineral dust were simulated over East Asia and Japan with Δx = 30 km and Δx = 5 km domains, respectively, and compared against the nation-wide seasonal observations of PM2.5 elements in Japan and the long-term continuous observations of total suspended particles (TSPs) at Yonago, Japan in 2013. Most of the simulated elements generally agreed with the observations, while Cu and Pb were significantly overestimated. This is the first comprehensive study on the development and evaluation of emission inventory of OP active elements, but further improvement is needed.

Design and demonstration of high-Q photonic heterostructure nanocavities suitable for integration.

We have investigated the localized design of heterostructure photonic crystal nanocavities in order to make them more suitable for integration. While retaining theoretical quality factors of more than ten million, the total length of the heterostructure nanocavity can be reduced to ~5 mum and the shifted air holes comprising the heterostructure can be restricted to the two rows nearest the nanocavity on each side. Though the area for the heterostructure nanocavity investigated thus far was larger than 10 x 10 microm(2) in the photonic crystal slab, heterostructure nanocavities of this new design have sizes of approximately 3 x 5 microm(2), thus allowing dense integration.

High-Q nanocavity with a 2-ns photon lifetime.

We have succeeded in fabricating a photonic crystal nanocavity with a photon lifetime of 2.1 ns, which corresponds to a quality factor of 2.5 x 10(6). This lifetime is the longest recorded thus far in photonic crystal cavities, and was brought about by improvements in the fabrication process. Comparing our experimental quality factor with the results of calculations shows that we have suppressed variations in the radii and positions of the air holes composing a nanocavity such that their standard deviations are less than 1 nm.

Gaseous nitrous acid (HONO) and nitrogen oxides (NOx) emission from gasoline and diesel vehicles under real-world driving test cycles.

Reactive nitrogen species emission from the exhausts of gasoline and diesel vehicles, including nitrogen oxides (NOx) and nitrous acid (HONO), contributes as a significant source of photochemical oxidant precursors in the ambient air. Multiple laboratory and on-road exhaust measurements have been performed to estimate the NOx emission factors from various vehicles and their contribution to atmospheric pollution. Meanwhile, HONO emission from vehicle exhaust has been under-measured despite the fact that HONO can contribute up to 60% of the total hydroxyl budget during daytime and its formation pathway is not fully understood. A profound traffic-induced HONO to NOx ratio of 0.8%, established by Kurtenbach et al. since 2001, has been widely applied in various simulation studies and possibly linked to under-estimation of HONO mixing ratios and OH radical budget in the morning. The HONO/NOx ratios from direct traffic emission have become debatable when it lacks measurements for direct HONO emission from vehicles upon the fast-changing emission reduction technology. Several recent studies have reported updated values for this ratio. This study has reported the measurement of HONO and NOx emission as well as the estimation of exhaust-induced HONO/NOx ratios from gasoline and diesel vehicles using different chassis dynamometer tests under various real-world driving cycles. For the tested gasoline vehicle, which was equipped with three-way catalyst after-treatment device, HONO/NOx ratios ranged from 0 to 0.95 % with very low average HONO concentrations. For the tested diesel vehicle equipped with diesel particulate active reduction device, HONO/NOx ratios varied from 0.16 to 1.00 %. The HONO/NOx ratios in diesel exhaust were inversely proportional to the average speeds of the tested vehicles. IMPLICATIONS: Photolysis of HONO is a dominant source of morning OH radicals. Conventional traffic-induced HONO/NOx ratio of 0.8% has possibly linked to underestimation of the total HONO budget and consequently underestimation of OH radical budget. The recently reported HONO/NOx ratio of ~1.6% was used to stimulate HONO emission, which resulted in increased HONO concentrations during morning peak hours and its impact of 14% OH increment in the morning. However, the results were still lower than the measured concentrations. More studies should be conducted to establish an updated traffic-induced HONO/NOx ratio.