The concentration and isotopic composition of mercury (Hg) were studied in frozen soils along a southwest-northeast transect over the Himalaya-Tibet. Soil total Hg (HgT) concentrations were significantly higher in the southern slopes (72 ± 54 ng g−1, 2SD, n = 21) than those in the northern slopes (43 ± 26 ng g−1, 2SD, n = 10) of Himalaya-Tibet. No significant relationship was observed between HgT concentrations and soil organic carbon (SOC), indicating that the HgT variation was not governed by SOC. Soil from the southern slopes showed significantly negative mean δ202Hg (−0.53 ± 0.50‰, 2SD, n = 21) relative to those from the northern slopes (−0.12 ± 0.40‰, 2SD, n = 10). The δ202Hg values of the southern slopes are more similar to South Asian anthropogenic Hg emissions. A significant correlation between 1/HgT and δ202Hg was observed in all the soil samples, further suggesting a mixing of Hg from South Asian anthropogenic emissions and natural geochemical background. Large ranges of Δ199Hg (−0.45 and 0.24‰) were observed in frozen soils. Most of soil samples displayed negative Δ199Hg values, implying they mainly received Hg from gaseous Hg(0) deposition. A few samples had slightly positive odd-MIF, indicating precipitation-sourced Hg was more prevalent than gaseous Hg(0) in certain areas. The spatial distribution patterns of HgT concentrations and Hg isotopes indicated that Himalaya-Tibet, even its northern part, may have been influenced by transboundary atmospheric Hg pollution from South Asia.

Atmospheric pollution by polycyclic aromatic hydrocarbons (PAHs) has become a serious problem, especially in Asia, as PAHs can severely affect ecologically important mountainous areas. Using pine needles and mosses as bio-indicators, this study examined PAH pollution in a mountainous study area and evaluated the influence of transboundary PAHs. PAHs in urban areas were also evaluated for comparison. The study sites were alpine areas and urban areas (inland or coastal cities) across central Japan, in the easternmost part of Asia where atmospheric pollutants are transported from mainland Asia. The mean PAH concentrations of pine needles and mosses were 198.9 ± 184.2 ng g⁻¹ dry weight (dw) and 131.8 ± 60.7 ng g⁻¹ dw (mean ± SD), respectively. Pine needles preferentially accumulated PAHs with low molecular weights (LMW PAHs) and exhibited large differences in both PAH concentration and isomer ratios between alpine and urban sites. These differences can be explained by the strong influence of LMW PAHs emitted from domestic sources, which decreased and changed during transport from urban to alpine sites due to dry/wet deposition and photodegradation. In contrast, mosses accumulated a higher ratio of PAHs with high molecular weight (HMW PAHs). A comparison of isomer ratios showed that the PAH source for alpine moss was similar to that for northern coastal cities, which are typically influenced by long-transported PAHs from East Asia. Thus, these results indicate that alpine moss can also be strongly affected by the transboundary PAHs. It is likely that the uptake characteristics of moss, alpine climate, and alpine locations far from urban areas can strengthen the influence of transboundary pollution. Based on these results, the limitations and most effective use of bioindicators of PAH pollution for preserving alpine ecosystems are discussed.

Strong acid rain was recently observed over Northeastern China, particularly in summer in Liaoning Province where alkaline dust largely neutralized acids in the past. This seems to be related to the regional transboundary pollution and poses new challenges in acid rain control scheme in China. In order to delve into the regional transport impact, and quantify its potential contributions to such an “eruption” of acid rain over Liaoning, this paper employs an online source tagging model in coupling with the Nested Air Quality Prediction Modeling System (NAQPMS). Validation of predictions shows the model capability in reproducing key meteorological and chemical features. Acid concentration over Liaoning is more pronounced in August (average of 0.087 mg/m³) with strong pollutant import from regional sources against significant depletion of basic species. Seasonal mean contributions from regional sources are assessed at both lower and upper boundary layers to elucidate the main pathways of the impact of regional sources on acid concentration over Liaoning. At the upper layer (1.2 km), regional sources contribute to acid concentration over Liaoning by 67%, mainly from Shandong (16%), Hebei (13%), Tianjin (11%) and Korean Peninsula (9%). Identified main city-receptors in Liaoning are Dandong, Dalian, Chaohu, Yingkou, Liaoyang, Jinfu, Shengyang, Panjin, Tieling, Benxi, Anshan and Fushun. At lower layer (120 m) where Liaoning local contribution is dominant (58%), regional sources account for 39% in acid concentration. However, inter-municipal acid exchanges are prominent at this layer and many cities in Liaoning are revealed as important sources of local acid production. Seasonal acid contribution average within 1.2 km-120 m attains 55%, suggesting dominance of vertical pollutant transport from regional sources towards lower boundary layer in Liaoning. As direct environmental implication, this study provides policy makers with a perspective of regulating the regional transboundary environmental impact assessment in China with application to acid rain control.

Countries in Northeast Asia have been regulating PM₂.₅ sources and studying their local and transboundary origins since PM₂.₅ causes severe impacts on public health and economic losses. However, the separation of local and transboundary impacts is not fully realized because it is impossible to change air pollutant emissions from multiple countries experimentally. Exceptionally, the early stage of the COVID-19 outbreak (January–March 2020) provided a cross-country experiment to separate each impact of PM₂.₅ sources identified in Seoul, a downwind area of China. We evaluated the contributions of PM₂.₅ sources compared to 2019 using dispersion normalized positive matrix factorization (DN-PMF) during three meteorological episodes. Episodes 1 and 2 revealed transboundary impacts and were related to reduced anthropogenic emissions and accumulated primary pollutants in Northeast China. Anthropogenic emissions, except for the residential sector, decreased, but primary air pollutants accumulated by residential coal combustion enhanced secondary aerosol formation. Thus, the contributions of sulfate and secondary nitrate increased in Seoul during episode 1 but then decreased maximally with other primary sources (biomass burning, district heating and incineration, industrial sources, and oil combustion) during episode 2 under meteorological conditions favorable to long-range transport. Local impact was demonstrated by atmospheric stagnation during episode 3. Meteorological condition unfavorable to local dispersion elevated the contributions of mobile and coal combustion and further contributed to PM₂.₅ high concentration events (HCE). Our study separates the local and transboundary impacts and highlights that cooperations in Northeast Asia on secondary aerosol formation and management of local sources are necessary.

The comparison of two methods in calculating transboundary concentrations of NO₂ and PM₁₀ using CMAQ chemical transport model is presented. The total mean annual concentrations for the pollutants were computed from the hourly outputs of the CMAQ model. The first method for calculating the transboundary concentrations is based on switching off the emissions from the studied country, while the remaining emissions are the same as in the full model run. The second method is based on running the model with the emissions from the studied country only. The resulting concentrations are then subtracted from the full model run concentrations. The result of this subtraction represents the transboundary air pollution together with pollution originating from the interaction of national and foreign sources. The pollution which cannot be attributed unambiguously to national or foreign sources is caused by the non-linear processes included in the model. It is evaluated as the difference between the two methods. It is shown that the non-linearity effect is more expressed for PM₁₀ than for NO₂ annual mean concentrations. It is estimated that the non-linearity effect for PM₁₀ can reach values up to 2.7 μg/m3 in absolute value, or up to 16% of the total annual mean concentrations and up to 25% of the total estimated transboundary concentrations in the studied area. It is also demonstrated that this non-linearity effect is more important for both pollutants during some episodes than in the annual mean. The method of removing the bias from the calculated transboundary concentrations is presented, together with the proposed method of evaluation of the uncertainties of the transboundary concentration calculations. The estimated transboundary contribution is evaluated at the locations of Slovak air-quality monitoring stations. The impact of several emission reduction levels on the estimation of the transboundary contribution is also presented. The simulations are performed for the reference year of 2015 for Slovakia, but the proposed methods can by applied universally.