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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.
Показать больше [+] Меньше [-]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.
Показать больше [+] Меньше [-]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.
Показать больше [+] Меньше [-]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.
Показать больше [+] Меньше [-]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.
Показать больше [+] Меньше [-]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.
Показать больше [+] Меньше [-]Effects of ozone stress on flowering phenology, plant-pollinator interactions and plant reproductive success
2021
Duque, Laura | Poelman, Erik H. | Steffan-Dewenter, Ingolf
Tropospheric ozone is a highly oxidative pollutant with the potential to alter plant metabolism. The direct effects of ozone on plant phenotype may alter interactions with other organisms, such as pollinators, and, consequently, affect plant reproductive success. In a set of greenhouse experiments, we tested whether exposure of plants to a high level of ozone affected their phenological development, their attractiveness to four different pollinators (mason bees, honeybees, hoverflies and bumblebees) and, ultimately, their reproductive success. Exposure of plants to ozone accelerated flowering, particularly on plants that were growing in autumn, when light and temperature cues, that commonly promote flowering, were weaker. Simultaneously, there was a tendency for ozone-exposed plants to disinvest in vegetative growth. Plant exposure to ozone did not substantially affect pollinator preference, but bumblebees had a tendency to visit more flowers on ozone-exposed plants, an effect that was driven by the fact that these plants tended to have more open flowers, meaning a stronger attraction signal. Honeybees spent more time per flower on ozone-exposed plants than on control plants. Acceleration of flower production and the behavioural responses of pollinators to ozone-exposed plants resulted in retained reproductive fitness of plants pollinated by bumblebees, honeybees and mason bees, despite the negative effects of ozone on plant growth. Plants that were pollinated by hoverflies had a reduction in reproductive fitness in response to ozone. In a natural setting, acceleration of flowering by ozone might foster desynchronization between plant and pollinator activities. This can have a strong impact on plants with short flowering periods and on plants that, unlike wild mustard, lack compensatory mechanisms to cope with the absence of pollinator activity in the beginning of flowering.
Показать больше [+] Меньше [-]Simultaneous observation of atmospheric peroxyacetyl nitrate and ozone in the megacity of Shanghai, China: Regional transport and thermal decomposition
2021
Zhang, Gen | Jing, Shengao | Xu, Wanyun | Gao, Yaqin | Yan, Chao | Liang, Linlin | Huang, Cheng | Wang, Hongli
Atmospheric peroxyacetyl nitrate (PAN) and ozone (O₃) are two typical indicators for photochemical pollution that have adverse effects on the ecosystem and human health. Observation networks for these pollutants have been expanding in developed regions of China, such as North China Plain (NCP) and Pearl River Delta (PRD), but are sparse in Yangtze River Delta (YRD), meaning their concentration and influencing factors remain poorly understood. Here, we performed a one-year measurement of atmospheric PAN, O₃, particulate matter with aerodynamic diameter smaller than 2.5 μm (PM₂.₅), nitrogen oxides (NOₓ), carbon monoxide (CO), and meteorological parameters from December 2016 to November 2017 in Shanghai. Overall, high hourly maximum PAN and O₃ were found to be 7.0 and 185 ppbv in summer, 6.2 and 146 ppbv in autumn, 5.8 and 137 ppbv in spring, and 6.0 and 76.7 ppbv in winter, respectively. Continental air masses probably carried atmospheric pollutants to the sampling site, while frequent maritime winds brought in less polluted air masses. Furthermore, positive correlations (R: 0.72–0.85) between PAN and O₃ were found in summer, indicating a predominant role of photochemistry in their formation. Unlike in summer, weak or no correlations between PAN and O₃ were featured during the other seasons, especially in winter, due to their different loss pathways. Unexpectedly, positive correlations between PAN and PM₂.₅ were found in all seasons. During summer, moderate correlation could be attributed to the strong photochemistry acting as a common driver in the formation of secondary aerosols and PAN. During winter, high PM₂.₅ might promote PAN production through HONO production, hence resulting in a good positive correlation. Additionally, the loss of PAN by thermal decomposition (TPAN) only accounted for a small fraction (ca. 1%) of the total (PAN + TPAN) during a typical winter episode, while it significantly reached 14.4 ppbv (71.1% of the total) in summer.
Показать больше [+] Меньше [-]Impact of residual layer transport on air pollution in Beijing, China
2021
Liu, Yusi | Tang, Guiqian | Wang, Meng | Liu, Baoxian | Hu, Bo | Chen, Qi | Wang, Yuesi
The residual layer (RL) stores a large amount of pollutants, but its effect on near-surface pollution is unknown. In this study, a two-year continuous observation was performed in Beijing using a ceilometer. The generalized boundary layer includes the mixing layer and RL. The results showed that there is no significant seasonal difference in the generalized boundary layer height (GBLH). The average GBLHs in spring, summer, autumn and winter are 1155, 1139, 1036 and 1195 m, respectively. The diurnal variation characteristics of spring, summer and autumn are similar, and the RL disappears when the mixing layer height reaches its peak in the afternoon. In winter, the development of the mixing layer is weak, and there is a 33.8% chance that the RL cannot be breached, thus making the mixing layer height at noon much lower than the GBLH. The concentrations of PM₂.₅ in the mixing layer and RL are 89 and 52 μg m⁻³, respectively, and the probability that the PM₂.₅ concentration in the RL was higher than that near the ground was 38.9%. RL transport represents an important beginning of the pollution event during the winter mornings and afternoons in Beijing. This study is helpful to better understand the structure of the RL and its influence on air pollution.
Показать больше [+] Меньше [-]Understanding the spatiotemporal pollution dynamics of highly fragile montane watersheds of Kashmir Himalaya, India
2021
Bhat, Sami Ullah | Khanday, Shabir A. | Islam, Sheikh Tajamul | Sabha, Inam
Pollution of riverine ecosystems through the multidimensional impact of human footprints around the world poses a serious challenge. Research studies that communicate potential repercussions of landscape structure metrics on snowmelt riverine water quality particularly, in climatically fragile Himalayan watersheds are very scarce. Though, worldwide, grasping the influence of land-use practices on water quality (WQ) has received renewed attention yet, the relevance of spatial scale linked to landscape pattern is still elusive due to its heterogenic nature across diverse geomorphic regions. In this work, therefore, we tried to capture the insights on landscape-aquascape interface by juxtapositioning the impacts of landscape structure pattern on snowmelt stream WQ of the whole Jhelum River Basin (JRB) under three varying spatial scales viz., watershed scale, riparian corridor (1000 m wide) and reach buffer (500 m wide). The percentage of landscape pattern composition and configuration metrics in the JRB were computed in GIS utilizing Landsat-8 OLI/TIRS satellite image having 30 m resolution. To better explicate the influence of land-use metrics on riverine WQ with space and time, we used Redundancy analysis (RDA) and multilinear regression (MLR) modeling. MLR selected land-use structure metrics revealed the varied response of WQ parameters to multi-scale factors except for total faecal coliform bacteria (TC) which showed perpetual presence. The reach-scale explained slightly better (76%) variations in WQ than riparian (75%) and watershed (70%) scales. Likewise, across seasonal scale, autumn (75%), winter (83%), and summer (77%) captured the most WQ variation at catchment, riparian, and reach scales respectively. We observed impairing WQ linkages with agriculture, built-up and barren rocky areas across watersheds, besides, pastures in riparian buffer areas, and fragmentation of landscape patches at the reach scale. Due to little appearance of spatial scale differences, a multi scale perspective landscape planning is emphasized to ensure future sustainability of Kashmir Himalayan water resources.
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