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Source analysis of the tropospheric NO2 based on MAX-DOAS measurements in northeastern China 全文
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.
显示更多 [+] 显示较少 [-]Dispersion of airborne mercury species emitted from the cement plant 全文
2022
Nair, Sreekanth Vijayakumaran | Kotnik, Jože | Gačnik, Jan | Živković, Igor | Koenig, Alkuin Maximilian | Mlakar, Tanja Ljubič | Horvat, Milena
The cement industry is the second largest source of anthropogenic mercury (Hg) emissions in Europe, accounting for 11% of global anthropogenic Hg emissions. The main objective of this study was to examine the influence of Hg emissions from the Salonit Anhovo cement plant on Hg levels measured in the ambient air at Vodarna, 1 km downwind from the flue gas chimney. The findings reveal that the plant raw mill operational status plays an important role in Hg concentrations in the flue gas emitted from the plant. Emitted total gaseous mercury was, on average, higher (49.4 μg/m³) when raw mills were in the direct mode (both raw mills-off) and lower (23.4 μg/m³) in the combined mode (both raw mills-on). The average Hg concentrations in Vodarna were 3.14 ng/m³ for gaseous elemental mercury, 53.7 pg/m³ for gaseous oxidised mercury, and 41.9 pg/m³ for particulate bound mercury for the whole measurement period. Atmospheric Hg speciation in Vodarna, coupled with plant emissions and wind data, has revealed that the total gaseous mercury emitted from the cement plant is clearly related to all Hg species measured in Vodarna. Wind blowing from the northeastern quadrant (mostly NE, ENE) is responsible for the elevated Hg levels in Vodarna, where gaseous oxidised mercury levels are highly linked to the cement plant emissions. However, elevated levels of Hg species in the absence of northeastern winds indicate potential inputs from other unknown local sources as well as inputs from regional and global transport mechanisms.
显示更多 [+] 显示较少 [-]Influence of a weak typhoon on the vertical distribution of air pollution in Hong Kong: A perspective from a Doppler LiDAR network 全文
2021
Huang, Tao | Yang, Yuanjian | O’Connor, Ewan James | Lolli, Simone | Haywood, Jim | Osborne, M. (Martin) | Cheng, Jack Chin-Ho | Guo, Jianping | Yim, Steve Hung-Lam
High particulate matter (PM) and ozone (O₃) concentration in Hong Kong are frequently observed during the summertime typhoon season. Despite the critical effect of a typhoon on air pollution, contributions of vertical wind profile and cloud movement during transboundary air pollution (TAP) on surface PM and O₃ concentration have yet to be fully understood. This work is the first study to apply a network of Doppler light detection and ranging (LiDAR) as well as back trajectory analysis to comprehensively analyze the effect of a weak Typhoon (Danas) occurring during 16–19 July 2019 on different variations in PM and O₃ concentration. During the typhoon Danas, three types of surface air pollution with five episodes were identified: (1) low PM and high O₃ concentration; (2) co-occurring high PM and O₃ concentration and (3) high PM and low O₃ concentration. Employing our 3D Real-Time Atmospheric Monitoring System (3DREAMs) along with surface observations, we found the important role of TAP in the increases in surface PM and O₃ concentration with significant vertical wind shear that transported air pollutants at upper levels, and strong vertical mixing that brought air pollutants to the ground level. Cloud movement related to typhoon periphery, as well as high solar radiation due to sinking motion and remote transport by continental wind, have an impact on local O₃ concentration. For the substantial difference in O₃ concentration between two air quality measurement sites, the similar vertical aerosol distributions and wind profiles suggest the comparable TAP contributions at the two sites and thus infer the critical role of local O₃ photochemical process in the O₃ difference. This work comprehensively reveals the influences of a weak typhoon on variations in PM and O₃ during the five episodes, providing important references for air quality monitoring and forecast in regions under the influence of typhoon.
显示更多 [+] 显示较少 [-]PAHs in an urban-industrial area: The role of lichen transplants in the detection of local and study area scale patterns 全文
2021
Lucadamo, L. | Gallo, L. | Corapi, A.
Spatial variation of the levels of polycyclic aromatic hydrocarbons (PAHs) was evaluated within an urban-industrial district where the main anthropogenic pressures are a 15 MW biomass power plant (BPP) and road traffic. The use of a high-density lichen transplant network and wind quantitative relationships made it possible to perform a hierarchical analysis of contamination. Combined uni-bi and multivariate statistical analyses of the resulting databases revealed a dual pattern. In its surroundings (local scale), the BPP affected the bioaccumulation of fluoranthene, pyrene and total PAHs, although a confounding effect of traffic (mostly petrol/gasoline engines) was evident. Spatial variation of the rate of diesel vehicles showed a significant association with that of acenaphthylene, acenaphthene, fluorene, anthracene and naphthalene. The series of high-speed wind values suggests that wind promotes diffusion rather than dispersion of the monitored PAHs. At the whole study area scale, the BPP was a source of acenaphthylene and acenaphthene, while diesel vehicles were a source of acenaphthylene. PAHs contamination strongly promotes oxidative stress (a threefold increase vs pre-exposure levels) in lichen transplants, suggesting a marked polluting effect of anthropogenic sources especially at the expense of the mycobiont. The proposed monitoring approach could improve the apportionment of the different contributions of point and linear anthropogenic sources of PAHs, mitigating the reciprocal biases affecting their spatial patterns.
显示更多 [+] 显示较少 [-]Influence of dike-induced morphologic and sedimentologic changes on the benthic ecosystem in the sheltered tidal flats, Saemangeum area, west coast of Korea 全文
2020
Kim, Dohyeong | Jo, Joohee | Kim, Bora | Ryu, Jongseong | Choi, Kyungsik
The effects of dike construction on the geomorphology and sedimentary processes of tidal flats were investigated using high-precision topographic profiling, short cores, and unmanned aviation vehicle (UAV)-assisted photogrammetry to understand their adverse consequences on the benthic ecosystem. Tidal flats at the south of Shinsi Island near one of the two sluice gates of the Saemangeum dike, display prominent morphologic features known as shelly sand ridges or cheniers (sensu Otvos, 2000) that have migrated landward about 5 m in a year. The tidal flats were dominated by erosion from winter to spring and by deposition during the remainder of the year except for the periods of heavy precipitation when tidal drainage channels became larger and deeper by headward erosion. With overall coarser-grained surface sediments, the presence of actively migrating wave-built cheniers are in stark contrast to muddy tidal flats with a monotonous morphology before the completion of the Saemangeum dike in 2006. Southeasterly waves reflected from the dike during winter to spring when north to northwesterly winds prevail account for the wave-induced onshore sediment transport and rapid morphologic changes in the tidal flats despite their location protected from offshore waves. The diversity and biomass of major macrofauna species tend to increase during rapid erosion and decrease during rapid deposition, highlighting the anthropogenic effect of dike-induced physical disturbance on the benthic ecosystem in the otherwise sheltered tidal flats.
显示更多 [+] 显示较少 [-]Sub micron aerosol variability and its ageing process at a high altitude site in India: Impact of meteorological conditions 全文
2020
Mukherjee, Subrata | Singla, Vyoma | Meena, Guman Singh | Aslam, Mohammad Yusuf | Safai, Pramod Digambar | Buchunde, Pallavi | Vasudevan, Anil Kumar | Jena, Chinmay Kumar | Ghude, Sachin Dinkar | Dani, Kundan | Pandithurai, Govindan
The effect of relative humidity and temperature on the submicron aerosol variability and its ageing process was studied over a high altitude site, Mahabaleshwar in south-west India. The mass composition of non-refractory particulate matter of 1 μm (NR-PM₁) size was obtained using Time of Flight Aerosol Chemical Speciation Monitor (ToF-ACSM) along with the measurements on a few trace gases during winter (December 2017–February 2018) and summer season (20th March - 5th May 2018). Sulfate exhibited strong dependence on the relative humidity (RH) as its mass fraction increased with the increase in RH. The Sulfate oxidation ratio (SOR) calculated during summer season also showed an increasing trend with RH indicating the influence of aqueous phase oxidation on sulfate fraction. On the other hand, OOA showed remarkable enhancement in its mass fraction with the increase in temperature along with the corresponding increase in f₄₄ and tropospheric ozone. OOA, ozone and f₄₄ ratio increased 14–34%, 8–26% and 25–43% respectively with the increase in temperature from 18 to 30 °C. This is indicative of the dominance of photochemical ageing processes during high temperature conditions. The extent of photochemical ageing was found to be higher during summer season (mean temperature ∼25.4 ± 2.6 °C) as compared to winter season (mean temperature ∼20.5 ± 2.6 °C). The nitrate diurnal was majorly governed by gas to particle partitioning process during winter season, whereas the summertime nitrate diurnal was influenced primarily by its formation rate. The non parametric wind regression analysis revealed that the mass concentration during winter was majorly contributed by distant sources from north east direction while during summer the local sources were more dominant.
显示更多 [+] 显示较少 [-]Ground-based and OMI-TROPOMI NO2 measurements at El Arenosillo observatory: Unexpected upward trends 全文
2020
Adame, J.A. | Gutierrez-Alvarez, I. | Bolivar, J.P. | Yela, M.
Eleven years, January 2008 to June 2019, of hourly nitrogen dioxide (NO₂) levels recorded at El Arenosillo observatory (Southwestern Europe) were analyzed. Annual averages ranged between 4 μg m⁻³ and 6 μg m⁻³ with peaks exceeding 40 μg m⁻³. A slight monthly variation was observed with maximum and minimum values in the cold (∼6 μg m⁻³) and warm (∼4 μg m⁻³) seasons respectively. A diurnal pattern was found with a weak amplitude (∼3 μg m⁻³). The monthly trends were investigated using surface observations and OMI (Ozone Monitoring instrument) satellite measurements. An unexpected upward trend was obtained in the last five years. The periods with elevated NO₂ concentrations in the last years were analyzed, showing an increase in its frequency and concentrations, linked with the upward trend observed. The weather conditions in these NO₂ peaks were studied using local surface meteorology, mean sea level pressure and wind fields from the data reanalysis of ERA5. The transport of NO₂ was explored using TROPOMI (Tropospheric Monitoring Instrument) measurements. The events occurred under conditions governed by high-pressure systems, which induced weak synoptic airflows or the development of mesoscale processes. Four scenarios of NO₂ transport were identified, associated with weak synoptic flows from inland or Southern Portugal and with mesoscale processes. The gulf of Cadiz plays an important role as a reservoir where the NO₂ coming from the south of Portugal, the Western Mediterranean Basin and urban-industrial areas can be accumulated and later transported inland. A strong correlation was found between the increase of NO₂ observed in the last years and positive anomalies of the temperature and geopotential height at 850 and 500 hPa levels. These findings could indicate that the causes of the changes in the NO₂ would be attributed to alterations in the weather patterns associated with a warmer climate.
显示更多 [+] 显示较少 [-]Assessment of forest fire impacts on carbonaceous aerosols using complementary molecular marker receptor models at two urban locations in California's San Joaquin Valley 全文
2019
Bae, Min-Suk | Skiles, Matthew J. | Lai, Alexandra M. | Olson, Michael R. | de Foy, Benjamin | Schauer, James J.
Two hundred sixty-three fine particulate matter (PM₂.₅) samples were collected over fourteen months in Fresno and Bakersfield, California. Samples were analyzed for organic carbon (OC), elemental carbon (EC), water soluble organic carbon (WSOC), and 160 organic molecular markers. Chemical Mass Balance (CMB) and Positive Matrix Factorization (PMF) source apportionment models were applied to the results in order to understand monthly and seasonal source contributions to PM₂.₅ OC. Similar source categories were found from the results of the CMB and PMF models to PM₂.₅ OC across the sites. Six source categories with reasonably stable profiles, including biomass burning, mobile, food cooking, two different secondary organic aerosols (SOAs) (i.e., winter and summer), and forest fires were investigated. Both the CMB and the PMF models showed a strong seasonality in contributions of some sources, as well as dependence on wind transport for both sites. The overall relative source contributions to OC were 24% CMB wood smoke, 19% CMB mobile sources, 5% PMF food cooking, 2% CMB vegetative detritus, 17% PMF SOA summer, 22% PMF SOA winter, and 12% PMF forest fire. Back-trajectories using the Weather Research and Forecasting model combined with the FLEXible PARTicle dispersion model (WRF-FLEXPART) were used to further characterize wind transport. Clustering of the trajectories revealed dominant wind patterns associated with varying concentrations of the different source categories. The Comprehensive Air Quality Model with eXtensions (CAMx) was used to simulate aerosol transport from forest fires and thus confirm the impacts of individual fires, such as the Rough Fire, at the measurement sites.
显示更多 [+] 显示较少 [-]Understanding long-term variations of meteorological influences on ground ozone concentrations in Beijing During 2006–2016 全文
2019
Chen, Ziyue | Zhuang, Yan | Xie, Xiaoming | Chen, Danlu | Cheng, Nianliang | Yang, Lin | Li, Ruiyuan
Recently, ground ozone has become one major airborne pollutant and the frequency of ozone-induced pollution episodes has increased rapidly across China. However, due to the lack of long-term observation data, relevant research on the characteristics and influencing factors of urban ozone concentrations remains limited. Based on ground ozone observation data during 2006–2016, we quantified the causality influence of individual meteorological factors on ozone concentrations in Beijing using a convergent cross mapping (CCM) method. The result indicated that the influence of each meteorological factor on ozone concentrations varied significantly across seasons and years. At the inter-annual scale, all-year meteorological influences on ozone concentrations were much more stable than seasonal meteorological influences. At the seasonal scale, meteorological influences on ozone concentrations were stronger in spring and autumn. Amongst multiple individual factors, temperature was the key meteorological influencing factor for ozone concentrations in all seasons except winter, when wind, humidity and SSD exerted major influences on ozone concentrations. In addition to temperature, air pressure was another meteorological factor that exerted strong influences on ozone concentrations. At both the inter-annual and seasonal scale, the influence of temperature and humidity on ozone concentrations was generally stable whilst that of other factors experienced large variations. Different from PM2.5, meteorological influences on ozone concentrations were relatively weak in summer, when ozone concentrations were the highest in Beijing. Given the generally stable meteorological influences on ozone concentrations and human-induced emissions of VOCs and NOx across seasons, warming induced notable increase in summertime biogenic emissions of VOCs and NOx can be a major driver for the increasing ozone pollution episodes. This research provides useful references for understanding long-term meteorological influences on ozone concentrations in mega cities in China.
显示更多 [+] 显示较少 [-]Characteristics and formation mechanisms of winter haze in Changzhou, a highly polluted industrial city in the Yangtze River Delta, China 全文
2019
Ye, Siqi | Ma, Tao | Duan, Fengkui | Li, Hui | He, Kebin | Xia, Jing | Yang, Shuo | Zhu, Lidan | Ma, Yongliang | Huang, Tao | Kimoto, Takashi
Changzhou, an industrial city in the Yangtze River Delta, has been experiencing serious haze pollution, particularly in winter. However, studies pertaining to the haze in Changzhou are very limited, which makes it difficult to understand the characteristics and formation of winter haze in this area, and develop effective control measures. In this study, we carried out continuous online observation of particulate matter, chemical components, and meteorology in Changzhou in February 2017. Our results showed that haze pollution occurred frequently in Changzhou winter and exhibited two patterns: dry haze with low relative humidity (RH) and wet haze with high RH. Water-soluble inorganic ions (SO₄²⁻, NO₃⁻, and NH₄⁺) accounted for ∼52.2% of the PM₂.₅ mass, of which sulfate was dominant in wet haze periods while nitrate was dominant in other periods. With the deterioration of haze pollution, the proportion of nitrate in PM₂.₅ increased, while sulfate proportion increased under wet haze and decreased under dry haze. Dry haze and wet haze appeared under slow north wind and south wind, respectively, and strong north wind or sea breeze scavenged pollution. We found that formation of nitrate occurred rapidly in daytime with high concentrations of odd oxygen (Oₓ = O₃ + NO₂), whereas formation of sulfate occurred rapidly during nighttime with high RH, indicating that photochemistry and heterogeneous reaction were the major formation mechanisms for nitrate and sulfate, respectively. Through the cluster analysis of 36-h backward trajectories, five sources of air masses from three directions were identified. High PM₂.₅ concentrations (84.1 μg m⁻³ on average) usually occurred under the influence of two clusters (46%) from the northwest, indicating that regional transport from northern China aggravated the winter haze pollution in Changzhou. Emission reduction, particularly the mobile sources, and regional joint prevention and control can help to mitigate the winter haze in Changzhou.
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