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Source analysis of the tropospheric NO2 based on MAX-DOAS measurements in northeastern China
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.
Show more [+] Less [-]Derivation of copper water quality criteria in the Bohai Sea of China considering the effects of multiple environmental factors on copper toxicity
2022
Li, Yang | Mu, Di | Wu, Hong-Qing | Tan, Dan-Dan | Liu, Xian-Hua | Sun, Jun | Ji, Zhi-Yong
Copper has become one of the most important heavy metal pollutants in the environment because of its wide application and high toxicity, but research on water quality criteria (WQCs) on copper is limited, especially the derivation of seawater WQC. In addition, the toxicity of copper in the seawater system is affected by various environmental factors. Therefore, establishing a WQC that meets the characteristics of the regional environment is a top priority. The correlations between four factors of temperature, salinity, pH, dissolved organic carbon (DOC) and the toxic effect values of copper were analyzed in this study, and the temperature was determined as the most influential factor among the four factors in the Bohai Sea. A specific correlation between temperature and the toxic effects of copper was identified, and WQCs were derived based on the identified correlation and the variations of the Bohai Sea's temperature in different seasons by species sensitivity distribution (SSD) method. Under the condition of the winter, spring, autumn, and summer with an average water temperature of 0.09, 15.96, 17.83, and 24.87 °C, the obtained short-term water quality criteria (SWQCs) were 44.29, 4.70, 4.31, and 3.33 μg/L; the long-term water quality criteria (LWQCs) were 18.14, 1.93, 1.77 and 1.36 μg/L. The findings indicated the importance of introducing specific environmental conditions during the derivation process. This work could provide valuable information for pollution prevention and aquatic life protection in the Bohai Sea and provide a valuable reference for the derivation of criteria in other regions alike.
Show more [+] Less [-]Spatiotemporal distribution and environmental control factors of halocarbons in the Yangtze River Estuary and its adjacent marine area during autumn and spring
2022
Zou, Yawen | He, Zhen | Liu, Chunying | Yang, Gui-Peng
The oceanic production and release of volatile halocarbons (VHCs) to the atmosphere play a vital role in regulating the global climate. In this study, seasonal and spatial variations in VHCs, including trichlorofluoromethane (CFC-11), methyl iodide (CH₃I), dibromomethane (CH₂Br₂), and bromoform (CHBr₃), and environmental parameters affecting their concentrations were characterized in the atmosphere and seawater of the Yangtze River Estuary and its adjacent marine area during two cruises from October 17 to October 26, 2019 and from May 12 to May 25, 2020. Significant seasonal variations were observed in the atmosphere and seawater because of seasonal differences in the prevalent monsoon, water mass (Yangtze River Diluted Water), and biogenic production. VHCs concentrations were positively correlated with Chl-a concentrations in the surface water during autumn. The average sea-to-air fluxes of CH₃I, CH₂Br₂, and CHBr₃ in autumn were 19.7, 4.0, and 7.6 nmol m⁻² d⁻¹, respectively, while those in spring were 6.3, 6.4, and −3.6 nmol m⁻² d⁻¹. In the ship-based incubation experiments, ocean acidification and dust deposition had no significant effects on VHCs concentrations. The concentrations of CH₂Br₂ and CHBr₃ were significantly positively correlated with phytoplankton biomass under lower pH condition (M3: pH 7.9). This result indicated that CH₂Br₂ and CHBr₃ concentrations were mainly related to the biological release.
Show more [+] Less [-]Accumulation characteristic of nitrogen in reservoirs during the ice-covered period under superimposed influence of ice and sediments: A case study of Biliuhe reservoir
2022
Hu, Suduan | Wang, Tianxiang | Xu, Shiguo | Ma, Lingxiao | Wang, Tianzi | Sun, Ya
Reservoirs located in middle and high latitudes freeze for months in winter, where the accumulation characteristics of pollutants are changed by superimposed influence of salt exclusion from ice on the surface and pollution release from sediments at the bottom. Taking total nitrogen (TN) of Biliuhe reservoir in Northeast China as an example, we developed a model to simulate TN accumulation characteristics influenced by ice and sediments during the freezing period (NACISF), and quantified contributions of TN from ice and sediments. Model parameters of ice and sediments were determined by laboratory freeze-up simulation experiment and sediment release flux simulation experiment, and water quality data were obtained from field investigations. Results showed that the annual average amount of TN input during the ice-covered period from 2015 to 2020 was 220.77 t, the output was 400.11 t, and the accumulated amount was 589.52 t. TN excluded from ice and released from sediments contributed 8.12% and 7.17% of the total TN inputs in winter, respectively. Analysis showed that the TN excluded from ice was positively correlated with ice thickness and initial TN concentration. The maximum ice thickness of Biliuhe reservoir had a 13 year cyclic feature, and the proportion of TN excluded from ice to the total TN inputs in different periods ranged from 10.68% to 17.30% (mean 13.18%). Meanwhile, TN accumulated seasonally as summer > autumn > winter > spring. The TN exclusion effect in 2050 would be weakened when considering the combined effects of climate change and human activities, with a reduction of about 40.85% compared to the current. It is concluded that the NACISF model took into account the influences of both ice and sediments, which provided a detailed understanding of the accumulation characteristics of TN during freezing period, and had important reference significance for water quality management in winter.
Show more [+] Less [-]The seasonal variations and potential sources of nitrous acid (HONO) in the rural North China Plain
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.
Show more [+] Less [-]PM2.5 composition and sources in the San Joaquin Valley of California: A long-term study using ToF-ACSM with the capture vaporizer
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.
Show more [+] Less [-]The relationship between greenspace and personal exposure to PM2.5 during walking trips in Delhi, India
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.
Show more [+] Less [-]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
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.
Show more [+] Less [-]Impact of deep basin terrain on PM2.5 distribution and its seasonality over the Sichuan Basin, Southwest China
2022
Shu, Zhuozhi | Zhao, Tianliang | Liu, Yubao | Zhang, Lei | Ma, Xiaodan | Kuang, Xiang | Li, Yang | Huo, Zhaoyang | Ding, QiuJi | Sun, Xiaoyun | Shen, Lijuan
The terrain effect on atmospheric environment is poorly understood in particular for the polluted region with underlying complex topography. Therefore, this study targeted the Sichuan Basin (SCB), a deep basin with severe PM₂.₅ pollution enclosed by the eastern Tibetan Plateau (TP), Yunnan-Guizhou Plateaus (YGP) and mountains over Southwest China, and we investigated the terrain effect on seasonal PM₂.₅ distribution and the meteorological mechanism based on the WRF-Chem simulation with stuffing the basin topography. It is characterized that the three-dimensional distribution of topography-induced PM₂.₅ concentrations over the SCB with the seasonal shift of regional PM₂.₅ averages from approximately 30 μg m⁻³ in summer to 90 μg m⁻³ in winter at surface layer and from summertime 10 μg m⁻³ to wintertime 30 μg m⁻³ in the lower free troposphere. Such basin-forced PM₂.₅ changes presented the vertically monotonical declines concentrated within the lower troposphere below 3.6 km in spring, 2.3 km in summer, 2.6 km in autumn and 4.8 km in winter. Impacts of deep basin aggravated PM₂.₅ accumulation within the SCB and transport toward the surrounding plateaus contributing approximately 50–90% to PM₂.₅ levels over the regions of eastern TP and northern YGP. In the SCB, atmospheric thermal structure in the lower troposphere could build a vertical convergence layer between the boundary layer and free troposphere, acting as a lid inhibiting air diffusion, which was regulated by the terrain effects on interactions of westerlies and Asian monsoons, especially the wintertime strong warm lid deteriorating air pollution in the SCB. Furthermore, warm and humid air conditions within the basin prompted sulfur oxidation ratio by +0.02 and nitrogen oxidation ratio by +0.22 effectively producing the secondary PM₂.₅ in atmospheric environment.
Show more [+] Less [-]Organophosphate pesticides in South African eutrophic estuaries: Spatial distribution, seasonal variation, and ecological risk assessment
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.
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