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Source analysis of the tropospheric NO2 based on MAX-DOAS measurements in northeastern China النص الكامل
2022
Liu, Feng | Xing, Chengzhi | Su, Pinjie | Luo, Yifu | Zhao, Ting | Xue, Jiexiao | Zhang, Guohui | Qin, Sida | Song, Youtao | Bu, Naishun
Ground-based Multi-Axis Differential Optical Absorption Spectroscopy (Max-DOAS) measurements of nitrogen dioxide (NO₂) were continuously obtained from January to November 2019 in northeastern China (NEC). Seasonal variations in the mean NO₂ vertical column densities (VCDs) were apparent, with a maximum of 2.9 × 10¹⁶ molecules cm⁻² in the winter due to enhanced NO₂ emissions from coal-fired winter heating, a longer photochemical lifetime and atmospheric transport. Daily maximum and minimum NO₂ VCDs were observed, independent of the season, at around 11:00 and 13:00 local time, respectively, and the most obvious increases and decreases occurred in the winter and autumn, respectively. The mean diurnal NO₂ VCDs at 11:00 increased to at 08:00 by 1.6, 5.8, and 6.7 × 10¹⁵ molecules cm⁻² in the summer, autumn and winter, respectively, due to increased NO₂ emissions, and then decreased by 2.8, 4.2, and 5.1 × 10¹⁵ molecules cm⁻² at 13:00 in the spring, summer, and autumn, respectively. This was due to strong solar radiation and increased planetary boundary layer height. There was no obvious weekend effect, and the NO₂ VCDs only decreased by about 10% on the weekends. We evaluated the contributions of emissions and transport in the different seasons to the NO₂ VCDs using a generalized additive model, where the contributions of local emissions to the total in the spring, summer, autumn, and winter were 89 ± 12%, 92 ± 11%, 86 ± 12%, and 72 ± 16%, respectively. The contribution of regional transport reached 26% in the winter, and this high contribution value was mainly correlated with the northeast wind, which was due to the transport channel of air pollutants along the Changbai Mountains in NEC. The NO₂/SO₂ ratio was used to identify NO₂ from industrial sources and vehicle exhaust. The contribution of industrial NO₂ VCD sources was >66.3 ± 16% in Shenyang due to the large amount of coal combustion from heavy industrial activity, which emitted large amounts of NO₂. Our results suggest that air quality management in Shenyang should consider reductions in local NO₂ emissions from industrial sources along with regional cooperative control.
اظهر المزيد [+] اقل [-]The seasonal variations and potential sources of nitrous acid (HONO) in the rural North China Plain النص الكامل
2022
Song, Yifei | Zhang, Yuanyuan | Xue, Chaoyang | Liu, Pengfei | He, Xiaowei | Li, Xuran | Mu, Yujing
Nitrous acid (HONO), an essential precursor of hydroxyl radicals (OH) in the troposphere, plays an integral role in atmospheric photochemistry. However, potential HONO sources remain unclear, particularly in rural areas, where long-term (including seasonal) measurements are scarce. HONO and related parameters were measured at a rural site in the North China Plain (NCP) during the winter of 2017 and summer and autumn of 2020. The mean HONO level was higher in winter (1.79 ± 1.44 ppbv) than in summer (0.67 ± 0.50 ppbv) and autumn (0.83 ± 0.62 ppbv). Source analysis revealed that the heterogeneous conversion (including photo-enhanced conversion) of NO₂ on the ground surface dominated the daytime HONO production in the three seasons (43.1% in winter, 54.3% in summer, and 62.0% in autumn), and the homogeneous reaction of NO and OH contributed 37.8, 12.2, and 28.4% of the daytime HONO production during winter, summer, and autumn, respectively. In addition, the total contributions of other sources (direct vehicle emissions, particulate nitrate photolysis, NO₂ uptake and its photo-enhanced reaction on the aerosol surface) to daytime HONO production were less than 5% in summer and autumn and 12.0% in winter. Unlike winter and autumn, an additional HONO source was found in summer (0.45 ± 0.21 ppbv h⁻¹, 31.4% to the daytime HONO formation), which might be attributed to the HONO emission from the fertilized field. Among the primary radical sources (photolysis of HONO, O₃, and formaldehyde), HONO photolysis was dominant, with contributions of 82.6, 49.3, and 63.2% in winter, summer, and autumn, respectively. Our findings may aid in understanding HONO formation in different seasons in rural areas and may highlight the impact of HONO on atmospheric oxidation capacity.
اظهر المزيد [+] اقل [-]Characteristics, source apportionment and long-range transport of black carbon at a high-altitude urban centre in the Kashmir valley, North-western Himalaya النص الكامل
2022
Bhat, Mudasir Ahmad | Romshoo, Shakil Ahmad | Beig, Gufran
Six years of data (2012–2017) at an urban site-Srinagar in the Northwest Himalaya were used to investigate temporal variability, meteorological influences, source apportionment and potential source regions of BC. The daily BC concentration varies from 0.56 to 40.16 μg/m³ with an inter-annual variation of 4.20–7.04 μg/m³ and is higher than majority of the Himalayan urban locations. High mean annual BC concentration (6.06 μg/m³) is attributed to the high BC observations during winter (8.60 μg/m³) and autumn (8.31 μg/m³) with a major contribution from Nov (13.88 μg/m³) to Dec (13.4 μg/m³). A considerable inter-month and inter-seasonal BC variability was observed owing to the large changes in synoptic meteorology. Low BC concentrations were observed in spring and summer (3.14 μg/m³ and 3.21 μg/m³), corresponding to high minimum temperatures (6.6 °C and 15.7 °C), wind speed (2.4 and 1.6 m/s), ventilation coefficient (2262 and 2616 m²/s), precipitation (316.7 mm and 173.3 mm) and low relative humidity (68% and 62%). However, during late autumn and winter, frequent temperature inversions, shallow PBL (173–1042 m), stagnant and dry weather conditions cause BC to accumulate in the valley. Through the observation period, two predominant diurnal BC peaks were observed at ⁓9:00 h (7.75 μg/m³) and ⁓21:00 h (6.67 μg/m³). Morning peak concentration in autumn (11.28 μg/m³) is ⁓2–2.5 times greater than spring (4.32 μg/m³) and summer (5.23 μg/m³), owing to the emission source peaks and diurnal boundary layer height. Diurnal BC concentration during autumn and winter is 65% and 60% higher than spring and summer respectively. During autumn and winter, biomass burning contributes approximately 50% of the BC concentration compared to only 10% during the summer. Air masses transport considerable BC from the Middle East and northern portions of South Asia, especially the Indo-Gangetic Plains, to Srinagar, with serious consequences for climate, human health, and the environment.
اظهر المزيد [+] اقل [-]Organophosphate pesticides in South African eutrophic estuaries: Spatial distribution, seasonal variation, and ecological risk assessment النص الكامل
2022
Olisah, Chijioke | Rubidge, Gletwyn | Human, Lucienne R.D. | Adams, Janine B.
The seasonal variation, spatial distribution, and ecological risks of thirteen organophosphate pesticides (OPPs) were studied in the Sundays and Swartkops estuaries in South Africa. Ten pesticides were detected in surface water samples from both estuaries, while all OPPs were detected in sediments. The highest concentration of OPPs (18.8 μg pyrazophos L⁻¹) was detected in surface water samples from Swartkops Estuary, while 48.7 μg phosalone kg⁻¹ dw was the highest in sediments collected from Sundays Estuary. There was no clear seasonal pattern in OPPs occurrence in surface water from both systems. However, their occurrence in sediments was in the following order: winter > autumn > summer > spring, perhaps indicating major pesticide input in the winter seasons. Results from ecological risk assessment showed that pyraclofos and chlorpyrifos (CHL) in surface water from both systems are respectively likely to cause high acute and chronic toxicity to fish (risk quotient – RQ > 1). For sediments of both estuaries, the highest acute and chronic RQs for fish were calculated for isazophos and CHL respectively. The majority of the detected OPPs in sediments posed potential high risks to Daphnia magna from both systems. These results suggest that these aquatic organisms (fish, and Daphnia), if present in the studied estuaries, can develop certain forms of abnormalities due to OPP exposure. To this end, proper measures should be taken to reduce OPP input into the estuarine systems.
اظهر المزيد [+] اقل [-]PM2.5 composition and sources in the San Joaquin Valley of California: A long-term study using ToF-ACSM with the capture vaporizer النص الكامل
2022
Sun, Peng | Farley, Ryan N. | Li, Lijuan | Srivastava, Deepchandra | Niedek, Christopher R. | Li, Jianjun | Wang, Ningxin | Cappa, Christopher D. | Pusede, Sally E. | Yu, Zhenhong | Croteau, Philip | Zhang, Qi
The San Joaquin Valley (SJV) of California has suffered persistent particulate matter (PM) pollution despite many years of control efforts. To further understand the chemical drivers of this problem and to support the development of State Implementation Plan for PM, a time-of-flight aerosol chemical speciation monitor (ToF-ACSM) outfitted with a PM₂.₅ lens and a capture vaporizer has been deployed at the Fresno-Garland air monitoring site of the California Air Resource Board (CARB) since Oct. 2018. The instrument measured non-refractory species in PM₂.₅ continuously at 10-min resolution. In this study, the data acquired from Oct. 2018 to May 2019 were analyzed to investigate the chemical characteristics, sources and atmospheric processes of PM₂.₅ in the SJV. Comparisons of the ToF-ACSM measurement with various co-located aerosol instruments show good agreements. The inter-comparisons indicated that PM₂.₅ in Fresno was dominated by submicron particles during the winter whereas refractory species accounted for a major fraction of PM₂.₅ mass during the autumn associated with elevated PM₁₀ loadings. A rolling window positive matrix factorization analysis was applied to the organic aerosol (OA) mass spectra using the Multilinear Engine (ME-2) algorithm. Three distinct OA sources were identified, including vehicle emissions, local and regional biomass burning, and formation of oxygenated species. There were significant seasonal variations in PM₂.₅ composition and sources. During the winter, residential wood burning and oxidation of nitrogen oxides were major contributors to the occurrence of haze episodes with PM₂.₅ dominated by biomass burning OA and nitrate. In autumn, agricultural activities and wildfires were found to be the main cause of PM pollution. PM₂.₅ concentrations decreased significantly after spring and were dominated by oxygenated OA during March to May. Our results highlight the importance of using seasonally dependent control strategies to mitigate PM pollution in the SJV.
اظهر المزيد [+] اقل [-]Long-term exposure to ambient temperature and mortality risk in China: A nationwide study using the difference-in-differences design النص الكامل
2022
Hu, Jianxiong | Zhou, Maigeng | Qin, Mingfang | Tong, Shilu | Hou, Zhulin | Xu, Yanjun | Zhou, Chunliang | Xiao, Yize | Yu, Min | Huang, Biao | Xu, Xiaojun | Lin, Lifeng | Liu, Tao | Xiao, Jianpeng | Gong, Weiwei | Hu, Ruying | Li, Junhua | Jin, Donghui | Zhao, Qinglong | Yin, Peng | Xu, Yiqing | Zeng, Weilin | Li, Xing | He, Guanhao | Huang, Cunrui | Ma, Wenjun
The short-term effects of ambient temperature on mortality have been widely investigated. However, the epidemiological evidence on the long-term effects of temperature on mortality is rare. In present study, we conducted a nationwide quasi-experimental design, which based on a variant of difference-in-differences (DID) approach, to examine the association between long-term exposure to ambient temperature and mortality risk in China, and to analyze the effect modification of population characteristics and socioeconomic status. Data on mortality were collected from 364 communities across China during 2006–2017, and environmental data were obtained for the same period. We estimated a 2.93 % (95 % CI: 2.68 %, 3.18 %) increase in mortality risk per 1 °C decreases in annual temperature, the greater effects were observed on respiratory diseases (5.16 %, 95 % CI: 4.53 %, 5.79 %) than cardiovascular diseases (3.43 %, 95 % CI: 3.06 %, 3.80 %), and on younger people (4.21 %, 95 % CI: 3.73 %, 4.68 %) than the elderly (2.36 %, 95 % CI: 2.06 %, 2.65 %). In seasonal analysis, per 1 °C decreases in average temperature was associated with 1.55 % (95 % CI: 1.23 %, 1.87 %), −0.53 % (95 % CI: −0.89 %, −0.16 %), 2.88 % (95 % CI: 2.45 %, 3.31 %) and 4.21 % (95 % CI: 3.98 %, 4.43 %) mortality change in spring, summer, autumn and winter, respectively. The effects of long-term temperature on total mortality were more pronounced among the communities with low urbanization, low education attainment, and low GDP per capita. In total, the decrease of average temperature in summer decreased mortality risk, while increased mortality risk in other seasons, and the associations were modified by demographic characteristics and socioeconomic status. Our findings suggest that populations with disadvantaged characteristics and socioeconomic status are vulnerable to long-term exposure of temperature, and targeted policies should be formulated to strengthen the response to the health threats of temperature exposure.
اظهر المزيد [+] اقل [-]Toxicity and endocrine-disrupting potential of PM2.5: Association with particulate polycyclic aromatic hydrocarbons, phthalate esters, and heavy metals النص الكامل
2022
Zhou, Qinghua | Chen, Jinyuan | Zhang, Junfan | Zhou, Feifei | Zhao, Jingjing | Wei, Xiuzhen | Zheng, Kaiyun | Wu, Jian | Li, Bingjie | Pan, Bingjun
The adverse effects of fine atmospheric particulate matter with aerodynamic diameters of ≤2.5 μm (PM₂.₅) are closely associated with particulate chemicals. In this study, PM₂.₅ samples were collected from highway and industry sites in Hangzhou, China, during the autumn and winter, and their cytotoxicity and pulmonary toxicity and endocrine-disrupting potential (EDP) were evaluated in vitro and in vivo; the particulate polycyclic aromatic hydrocarbons (PAHs), phthalate esters (PAEs), and heavy metals were then characterized. The toxicological results suggested that the PM₂.₅ from highway site induced higher cytotoxicity (cell viability inhibition, intracellular oxidative stress, and cell membrane injury) and pulmonary toxicity (inflammatory response (IR) and oxidative stress (OS)) than the samples from industry site, while the PM₂.₅ from industry site exhibited higher EDP (estrogenic and anti-androgenic activity). The cytotoxicity and pulmonary toxicity of PM₂.₅ in the winter were higher than those in the autumn, while no seasonal difference in the endocrine-disrupting potential was observed (p > 0.05). The Pearson correlation analysis between the biological effects and particulate chemicals revealed that the PM₂.₅-induced inflammatory response and oxidative stress were closely associated with the particulate PAHs and heavy metals (Pearson correlation coefficients: rIR, PAHₛ = 0.822–0.988, rIR, ₕₑₐᵥy ₘₑₜₐₗₛ = 0.895–0.971, rOS, PAHₛ = 0.843–0.986, and rOS, ₕₑₐᵥy ₘₑₜₐₗₛ = 0.887–0.933), while particulate di (2-ethylhexyl)phthalate (DEHP) substantially contributed to the EDP of PM₂.₅ (rEDP, DEHP = 0.981). This study indicated that the toxicity and EDP of PM₂.₅ could vary with the surrounding environment and season, which was closely associated with the variations of particulate chemicals. Further studies are needed to clarify the associations between the harmful effects of PM₂.₅ and other contributing factors.
اظهر المزيد [+] اقل [-]The relationship between greenspace and personal exposure to PM2.5 during walking trips in Delhi, India النص الكامل
2022
Mueller, William | Wilkinson, Paul | Milner, James | Loh, Miranda | Vardoulakis, Sotiris | Petard, Zoë | Cherrie, Mark | Puttaswamy, Naveen | Balakrishnan, Kalpana | Arvind, D.K.
The presence of urban greenspace may lead to reduced personal exposure to air pollution via several mechanisms, for example, increased dispersion of airborne particulates; however, there is a lack of real-time evidence across different urban contexts. Study participants were 79 adolescents with asthma who lived in Delhi, India and were recruited to the Delhi Air Pollution and Health Effects (DAPHNE) study. Participants were monitored continuously for exposure to PM₂.₅ (particulate matter with an aerodynamic diameter of less than 2.5 μm) for 48 h. We isolated normal day-to-day walking journeys (n = 199) from the personal monitoring dataset and assessed the relationship between greenspace and personal PM₂.₅ using different spatial scales of the mean Normalised Difference Vegetation Index (NDVI), mean tree cover (TC), and proportion of surrounding green land use (GLU) and parks or forests (PF). The journeys had a mean duration of 12.7 (range 5, 53) min and mean PM₂.₅ personal exposure of 133.9 (standard deviation = 114.8) μg/m³. The within-trip analysis showed weak inverse associations between greenspace markers and PM₂.₅ concentrations only in the spring/summer/monsoon season, with statistically significant associations for TC at the 25 and 50 m buffers in adjusted models. Between-trip analysis also indicated inverse associations for NDVI and TC, but suggested positive associations for GLU and PF in the spring/summer/monsoon season; no overall patterns of association were evident in the autumn/winter season. Associations between greenspace and personal PM₂.₅ during walking trips in Delhi varied across metrics, spatial scales, and season, but were most consistent for TC. These mixed findings may partly relate to journeys being dominated by walking along roads and small effects on PM₂.₅ of small pockets of greenspace. Larger areas of greenspace may, however, give rise to observable spatial effects on PM₂.₅, which vary by season.
اظهر المزيد [+] اقل [-]Dual-carbon isotope constraints on source apportionment of black carbon in the megacity Guangzhou of the Pearl River Delta region, China for 2018 autumn season النص الكامل
2022
Jiang, Fan | Liu, Junwen | Cheng, Zhineng | Ding, Ping | Xu, Yuanqian | Zong, Zheng | Zhu, Sanyuan | Zhou, Shengzhen | Yan, Caiqing | Zhang, Zhisheng | Zheng, Junyu | Tian, Chongguo | Li, Jun | Zhang, Gan
Black carbon (BC) aerosol negatively affects air quality and contributes to climate warming globally. However, little is known about the relative contributions of different source control measures to BC reduction owing to the lack of powerful source-diagnostic tools. We combine the fingerprints of dual-carbon isotope using an optimized Bayesian Markov chain Monte Carlo (MCMC) scheme and for the first time to study the key sources of BC in megacity Guangzhou of the Pearl River Delta (PRD) region, China in 2018 autumn season. The MCMC model-derived source apportionment of BC shows that the dominant contributor is petroleum combustion (39%), followed by coal combustion (34%) and biomass burning (27%). It should be noted that the BC source pattern is highly sensitive to the variations of air masses transported with an enhanced contribution of fossil source from the eastern area, suggesting the important impact of regional atmospheric transportation on the BC source profile in the PRD region. Also, we further found that fossil fuel combustion BC contributed 84% to the total BC reduction during 2013–2018. The response of PM₂.₅ concentration to the ¹⁴C-derived BC source apportionment is successfully fitted (r = 0.90) and the results predicted that it would take ∼6 years to reach the WHO PM₂.₅ guideline value (10 μg m⁻³) for the PRD region if the emission control measures keep same as they are at present. Taken together, our findings suggest that dual-carbon isotope is a powerful tool in constraining the source apportionment of BC for the evaluations of air pollution control and carbon emission measures.
اظهر المزيد [+] اقل [-]New global aerosol fine-mode fraction data over land derived from MODIS satellite retrievals النص الكامل
2021
Yan, Xing | Zang, Zhou | Liang, Zhen | Luo, Nana | Ren, Rongmin | Cribb, Maureen | Li, Zhanqing
The space-borne measured fine-mode aerosol optical depth (fAOD) is a gross index of column-integrated anthropogenic particulate pollutants, especially over the populated land. The fAOD is the product of the AOD and the fine-mode fraction (FMF). While there exist numerous global AOD products derived from many different satellite sensors, there have been much fewer, if any, global FMF products with a quality good enough to understand their spatiotemporal variations. This is key to understanding the global distribution and spatiotemporal variations of air pollutants, as well as their impacts on global environmental and climate changes. Modifying our newly developed retrieval algorithm to the latest global-scale Moderate Resolution Imaging Spectroradiometer (MODIS) aerosol product (Collection 6.1), a global 10-year FMF product is generated and analyzed here. We first validate the product through comparisons with the FMF derived from Aerosol Robotic Network (AERONET) measurements. Among our 169,313 samples, the satellite-derived FMFs agreed with the AERONET spectral deconvolution algorithm (SDA)-retrieved FMFs with a root-mean-square error (RMSE) of 0.22. Analyzed using this new product are the global patterns and interannual and seasonal variations of the FMF over land. In general, the FMF is large (>0.80) over Mexico, Myanmar, Laos, southern China, and Africa and less than 0.5 in the Sahelian and Sudanian zones of northern Africa. Seasonally, higher FMF values occur in summer and autumn. The linear trend in the satellite-derived and AERONET FMFs for different countries was explored. The upward trend in the FMFs was particularly strong over Australia since 2008. This study provides a new global view of changes in FMFs using a new satellite product that could help improve our understanding of air pollution around the world.
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