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Eight-year dry deposition of atmospheric mercury to a tropical high mountain background site downwind of the East Asian continent
2019
Phu Nguyen, Ly Sy | Zhang, Leiming | Lin, Da-Wei | Lin, Neng-Huei | Sheu, Guey-Rong
Atmospheric deposition, either dry or wet, has been identified as an important pathway of mercury (Hg) input to terrestrial and aquatic systems. Although East Asia is the major atmospheric Hg emission source region, very few studies have been conducted to quantify atmospheric Hg deposition in its downwind region. In this study, 8-year (2009–2016) atmospheric Hg dry deposition was reported at the Lulin Atmospheric Background Station (LABS), a high mountain forest site in central Taiwan. Dry deposition of speciated Hg was estimated using a bi-directional air-surface flux exchange model for gaseous elemental mercury (GEM) and dry deposition models for gaseous oxidized mercury (GOM) and particulate-bound mercury (PBM), making use of the monitored speciated atmospheric Hg concentrations. Annual total Hg dry deposition ranged from 51.9 to 84.9 μg m−2 yr−1 with a multi-year average of 66.1 μg m−2 yr−1. Among the three forms of atmospheric Hg, GEM was the main contributor to the total dry deposition, contributing about 77.8% to the total, due to the high density of forest canopy as well as the much higher concentration of GEM than GOM and PBM at LABS. Mercury dry deposition is higher in winter and spring than in summer and fall, partly due to the elevated Hg concentrations associated with air masses from East and Southeast Asia where with high atmospheric Hg emissions. The mean annual dry/wet deposition ratio of 2.8 at LABS indicated that Hg deposition to forest landscape was governed by dry rather than wet deposition.
Show more [+] Less [-]Allergenicity of recombinant Humulus japonicus pollen allergen 1 after combined exposure to ozone and nitrogen dioxide
2018
Hong, Qiang | Zhou, Shumin | Zhao, Hui | Peng, Jiaxian | Li, Yang | Shang, Yu | Wu, Minghong | Zhang, Wei | Lu, Senlin | Li, Shuijun | Yu, Shen | Wang, Weiqian | Wang, Qingyue
Ozone (O₃) and nitrogen dioxide (NO₂) are thought to play primary roles in aggravating air pollution-induced health problems. However, the effects of joint O₃/NO₂ on the allergenicity of pollen allergens are unclear. Humulus japonicus pollen allergen 1 (Hum j1) is a profilin protein that causes widespread pollinosis in eastern Asia. In order to study the effects of combined O₃/NO₂ on the allergenicity of Hum j1, tandem six-histidine peptide tag (His6)-fused recombinant Hum j1 (rHum j1) was expressed in a prokaryotic system and purified through His6 affinity chromatography. The purified rHum j1 was used to immunize SD rats. Rat sera with high titers of IgG and IgE antibodies against rHum j1 were used for allergenicity quantification. The rHum j1 was exposed to O₃/NO₂, and changes in allergenicity of the exposed rHum j1 were assayed using the immunized rat antibodies. Tandem LC-MS/LC (liquid chromatography-mass spectrometer/liquid chromatography spectrometer) chromatography and UV and circular dichroism (CD) spectroscopy were used to study the structural changes in rHum j1. Our data demonstrated that a novel disulfide bond between the sulfhydryl groups of two neighboring cysteine molecules was formed after the rHum j1 exposure to joint O₃/NO₂, and therefore IgE-binding affinity was increased and the allergenicity was reinforced. Our results provided clues to elucidate the mechanism behind air pollution-induced increase in pollinosis prevalence.
Show more [+] Less [-]The origin and migration of the dissolved sulfate from precipitation in Seoul, Korea
2018
Kim, Yeongmin | Lee, Insung | Lim, Chungwan | Farquhar, James | Lee, Sang-Mook | Kim, Hyoungbum
This study incorporated stable isotope analyses with chemical analyses to determine the origin and migration of sulfur sources in East Asia, and these findings were compared with our decadal research from 2000 to 2001 and 2002 to 2003. The multiple sulfur isotope composition (32S, 33S and 34S) of the dissolved sulfate in precipitation was first measured from 2011 to 2013 in Seoul, South Korea. The δ34Snss values were −1.1‰ to 7.9‰ (avg. 3.6‰), strongly suggesting that sulfur derived from the combustion of Chinese coal is the predominant source of sulfate in the Seoul region. Low NO3/SO42− ratios in the precipitation samples indicated an insignificant effect of sulfur from vehicle exhaust. The seasonal variation of δ34Snss values appears to be caused by increasing biogenic sulfur activity during the spring and summer seasons. The some Δ33S values (0.13‰–0.16‰) measured in the three samples were sufficiently small; thus, whether these values can be attributed to mass-independent fractionation remains unclear. Measuring the Δ33S anomalies in dissolved sulfate provides valuable insights for identifying the sources of sulfur transferred from the stratosphere to the troposphere and upper troposphere.
Show more [+] Less [-]Trans-Pacific transport of dust aerosols from East Asia: Insights gained from multiple observations and modeling
2017
Guo, Jianping | Lou, Mengyun | Miao, Yucong | Wang, Yuan | Zeng, Zhaoliang | Liu, Huan | He, Jing | Xu, Hui | Wang, Fu | Min, Min | Zhai, Panmao
East Asia is one of the world's largest sources of dust and anthropogenic pollution. Dust particles originating from East Asia have been recognized to travel across the Pacific to North America and beyond, thereby affecting the radiation incident on the surface as well as clouds aloft in the atmosphere. In this study, integrated analyses are performed focusing on one trans-Pacific dust episode during 12–22 March 2015, based on space-borne, ground-based observations, reanalysis data combined with Hybrid Single Particle Lagrangian Integrated Trajectory Model (HYSPLIT), and the Weather Research and Forecasting Model coupled with Chemistry (WRF-Chem). From the perspective of synoptic patterns, the location and strength of Aleutian low pressure system largely determined the eastward transport of dust plumes towards western North America. Multi-sensor satellite observations reveal that dust aerosols in this episode originated from the Taklimakan and Gobi Deserts. Moreover, the satellite observations suggest that the dust particles can be transformed to polluted particles over the East Asian regions after encountering high concentration of anthropogenic pollutants. In terms of the vertical distribution of polluted dust particles, at the very beginning, they were mainly located in the altitudes ranging from 1 km to 7 km over the source region, then ascended to 2 km–9 km over the Pacific Ocean. The simulations confirm that these elevated dust particles in the lower free troposphere were largely transported along the prevailing westerly jet stream. Overall, observations and modeling demonstrate how a typical springtime dust episode develops and how the dust particles travel over the North Pacific Ocean all the way to North America.
Show more [+] Less [-]Global-scale patterns in anthropogenic Pb contamination reconstructed from natural archives
2016
Marx, Samuel K. | Rashid, Shaqer | Stromsoe, Nicola
During the past two centuries metal loads in the Earth's atmosphere and ecosystems have increased significantly over pre-industrial levels. This has been associated with deleterious effects to ecosystem processes and human health. The magnitude of this toxic metal burden, as well as the spatial and temporal patterns of metal enrichment, is recorded in sedimentary archives across the globe. This paper presents a compilation of selected Pb contamination records from lakes (n = 10), peat mires (n = 10) and ice fields (n = 7) from Europe, North and South America, Asia, Australia and the Northern and Southern Hemisphere polar regions. These records quantify changes in Pb enrichment in remote from source environments. The presence of anthropogenic Pb in the environment has a long history, extending as far back as the early to mid-Holocene in North America, Europe and East Asia. However, results show that Pb contamination in the Earth's environment became globally ubiquitous at the beginning of the Second Industrial Revolution (c.1850–1890 CE), after which the magnitude of Pb contamination increased significantly. This date therefore serves as an effective global marker for the onset of the Anthropocene. Current global average Pb enrichment rates are between 6 and 35 times background, however Pb contamination loads are spatially variable. For example, they are >100 times background in Europe and North America and 5–15 times background in Antarctica. Despite a recent decline in Pb loads in some regions, most notably Europe and North America, anthropogenic Pb remains highly enriched and universally present in global ecosystems, while concentrations are increasing in some regions (Australia, Asia and parts of South America and Antarctica). There is, however, a paucity of Pb enrichment records outside of Europe, which limits assessments of global contamination.
Show more [+] Less [-]Improvement of aerosol optical properties modeling over Eastern Asia with MODIS AOD assimilation in a global non-hydrostatic icosahedral aerosol transport model
2014
Dai, Tie | Schutgens, Nick A.J. | Gotō, Daisuke | Shi, Guangyu | Nakajima, Teruyuki
A new global aerosol assimilation system adopting a more complex icosahedral grid configuration is developed. Sensitivity tests for the assimilation system are performed utilizing satellite retrieved aerosol optical depth (AOD) from the Moderate Resolution Imaging Spectroradiometer (MODIS), and the results over Eastern Asia are analyzed. The assimilated results are validated through independent Aerosol Robotic Network (AERONET) observations. Our results reveal that the ensemble and local patch sizes have little effect on the assimilation performance, whereas the ensemble perturbation method has the largest effect. Assimilation leads to significantly positive effect on the simulated AOD field, improving agreement with all of the 12 AERONET sites over the Eastern Asia based on both the correlation coefficient and the root mean square difference (assimilation efficiency). Meanwhile, better agreement of the Ångström Exponent (AE) field is achieved for 8 of the 12 sites due to the assimilation of AOD only.
Show more [+] Less [-]The sensitivities of ozone and PM2.5 concentrations to the satellite-derived leaf area index over East Asia and its neighboring seas in the WRF-CMAQ modeling system
2022
Park, Jincheol | Jung, Jia | Choi, Yunsoo | Mousavinezhad, Seyedali | Pouyaei, Arman
Vegetation plays an important role as both a sink of air pollutants via dry deposition and a source of biogenic VOC (BVOC) emissions which often provide the precursors of air pollutants. To identify the vegetation-driven offset between the deposition and formation of air pollutants, this study examines the responses of ozone and PM₂.₅ concentrations to changes in the leaf area index (LAI) over East Asia and its neighboring seas, using up-to-date satellite-derived LAI and green vegetation fraction (GVF) products. Two LAI scenarios that examine (1) table-prescribed LAI and GVF from 1992 to 1993 AVHRR and 2001 MODIS products and (2) reprocessed 2019 MODIS LAI and 2019 VIIRS GVF products were used in WRF-CMAQ modeling to simulate ozone and PM₂.₅ concentrations for June 2019. The use of up-to-date LAI and GVF products resulted in monthly mean LAI differences ranging from −56.20% to 96.81% over the study domain. The increase in LAI resulted in the differences in hourly mean ozone and PM₂.₅ concentrations over inland areas ranging from 0.27 ppbV to −7.17 ppbV and 0.89 μg/m³ to −2.65 μg/m³, and the differences of those over the adjacent sea surface ranging from 0.69 ppbV to −2.86 ppbV and 3.41 μg/m³ to −7.47 μg/m³. The decreases in inland ozone and PM₂.₅ concentrations were mainly the results of dry deposition accelerated by increases in LAI, which outweighed the ozone and PM₂.₅ formations via BVOC-driven chemistry. Some inland regions showed further decreases in PM₂.₅ concentrations due to reduced reactions of PM₂.₅ precursors with hydroxyl radicals depleted by BVOCs. The reductions in sea surface ozone and PM₂.₅ concentrations were accompanied by the reductions in those in upwind inland regions, which led to less ozone and PM₂.₅ inflows. The results suggest the importance of the selective use of vegetation parameters for air quality modeling.
Show more [+] Less [-]Geostationary satellite-derived ground-level particulate matter concentrations using real-time machine learning in Northeast Asia
2022
Park, Seohui | Im, Jungho | Kim, Jhoon | Kim, Sang-min
Rapid economic growth, industrialization, and urbanization have caused frequent air pollution events in East Asia over the last few decades. Recently, aerosol data from geostationary satellite sensors have been used to monitor ground-level particulate matter (PM) concentrations hourly. However, many studies have focused on using historical datasets to develop PM estimation models, often decreasing their predictability for unseen data in new days. To mitigate this problem, this study proposes a novel real-time learning (RTL) approach to estimate PM with aerodynamic diameters of <10 μm (PM₁₀) and <2.5 μm (PM₂.₅) using hourly aerosol data from the Geostationary Ocean Color Imager (GOCI) and numerical model outputs for daytime conditions over Northeast Asia. Three schemes with different weighting strategies were evaluated using 10-fold cross-validation (CV). The RTL models, which considered both concentration and time as weighting factors (i.e., Scheme 3) yielded consistent improvement for 10-fold CV performance on both hourly and monthly scales. The real-time calibration results for PM₁₀ and PM₂.₅ were R² = 0.97 and 0.96, and relative root mean square error (rRMSE) = 12.1% and 12.0%, respectively, and the 10-fold CV results for PM₁₀ and PM₂.₅ were R² = 0.73 and 0.69 and rRMSE = 41.8% and 39.6%, respectively. These results were superior to results from the offline models in previous studies, which were based on historical data on an hourly scale. Moreover, we estimated PM concentrations in the ocean without using land-based variables, and clearly demonstrated the PM transport over time. Because the proposed models are based on the RTL approach, the density of in-situ monitoring sites could be a major uncertainty factor. This study identified that a high error occurred in low-density areas, whereas a low error occurred in high-density areas. The proposed approach can be operated to monitor ground-level PM concentrations in real-time with uncertainty analysis to ensure optimal results.
Show more [+] Less [-]Biochar-induced reduction of N2O emission from East Asian soils under aerobic conditions: Review and data analysis
2021
Lee, Sun-Il | Park, Hyun-Jin | Jeong, Young-Jae | Seo, Bo-Seong | Kwak, Jin-Hyeob | Yang, Hye In | Xu, Xingkai | Tang, Shuirong | Cheng, Weiguo | Im, Sang-sŏn | Choi, Woo-Jung
Global meta-analyses showed that biochar application can reduce N₂O emission. However, no relevant review study is available for East Asian countries which are responsible for 70% of gaseous N losses from croplands globally. This review analyzed data of the biochar-induced N₂O mitigation affected by experimental conditions, including experimental types, biochar types and application rates, soil properties, and chemical forms and application rates of N fertilizer for East Asian countries. The magnitude of biochar-induced N₂O mitigation was evaluated by calculating N₂O reduction index (Rᵢₙdₑₓ, percentage reduction of N₂O by biochar relative to control). The Rᵢₙdₑₓ was further standardized against biochar application rate by calculating Rᵢₙdₑₓ per unit of biochar application rate (ton ha⁻¹) (Unit Rᵢₙdₑₓ). The Rᵢₙdₑₓ averaged across different experimental types (n = 196) was −21.1 ± 2.4%. Incubation and pot experiments showed greater Rᵢₙdₑₓ than column and field experiments due to higher biochar application rate and shorter experiment duration. Feedstock type and pyrolysis temperature also affected Rᵢₙdₑₓ; either bamboo feedstock or pyrolysis at > 400 °C resulted in a greater Rᵢₙdₑₓ. The magnitude of Rᵢₙdₑₓ also increased with increasing biochar rate. Soil properties did not affect Rᵢₙdₑₓ when evaluated across all experimental types, but there was an indication that biochar decreased N₂O emission more at a lower soil moisture level in field experiments. The magnitude of Rᵢₙdₑₓ increased with increasing N fertilizer rate up to 500–600 kg N ha⁻¹, but it decreased thereafter. The Unit Rᵢₙdₑₓ averaged across experimental types was −1.2 ± 0.9%, and it was rarely affected by experimental type and conditions but diminished with increasing biochar rate. Our results highlight that since N₂O mitigation by biochar is affected by biochar application rate, Rᵢₙdₑₓ needs to be carefully evaluated by standardizing against biochar application rate to suggest the best conditions for biochar usage in East Asia.
Show more [+] Less [-]Nitrogen burden from atmospheric deposition in East Asian oceans in 2010 based on high-resolution regional numerical modeling
2021
Itahashi, Syuichi | Hayashi, Kentaro | Takeda, Shigenobu | Umezawa, Yu | Matsuda, Kazuhide | Sakurai, Tatsuya | Uno, Itsushi
East Asian oceans are possibly affected by a high nitrogen (N) burden because of the intense anthropogenic emissions in this region. Based on high-resolution regional chemical transport modeling with horizontal grid scales of 36 and 12 km, we investigated the N burden into East Asian oceans via atmospheric deposition in 2010. We found a high N burden of 2–9 kg N ha⁻¹ yr⁻¹ over the Yellow Sea, East China Sea (ECS), and Sea of Japan. Emissions over East Asia were dominated by ammonia (NH₃) over land and nitrogen oxides (NOₓ) over oceans, and N deposition was dominated by reduced N over most land and open ocean, whereas it was dominated by oxidized N over marginal seas and desert areas. The verified numerical modeling identified that the following processes were quantitatively important over East Asian oceans: the dry deposition of nitric acid (HNO₃), NH₃, and coarse-mode (aerodynamic diameter greater than 2.5 μm) NO₃⁻, and wet deposition of fine-mode (aerodynamic diameter less than 2.5 μm) NO₃⁻ and NH₄⁺. The relative importance of the dry deposition of coarse-mode NO₃⁻ was higher over open ocean. The estimated N deposition to the whole ECS was 390 Gg N yr⁻¹; this is comparable to the discharge from the Yangtze River to the ECS, indicating the significant contribution of atmospheric deposition. Based on the high-resolution modeling over the ECS, a tendency of high deposition in the western ECS and low deposition in the eastern ECS was found, and a variety of deposition processes were estimated. The dry deposition of coarse-mode NO₃⁻ and wet deposition of fine-mode NH₄⁺ were the main factors, and the wet deposition of fine-mode NO₃⁻ over the northeastern ECS and wet deposition of coarse-mode NO₃⁻ over the southeastern ECS were also found to be significant processes determining N deposition over the ECS.
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