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1.
Environ Pollut ; : 118827, 2022 Jan 10.
Artigo em Inglês | MEDLINE | ID: mdl-35026327

RESUMO

We quantify for the first time marine aerosol properties and their differences in the offshore and remote ocean in the mid-latitude South Asian waters, low-latitude South Asian waters, and equatorial waters of the Western Pacific Ocean, based on shipboard cruise observations conducted by the Western Pacific Ocean Scientific Observation Network in winter 2018, and further investigate the effects of long-range transport of continental aerosols on the marine environment. During the overall observation period, the average number concentration of particle matter which aerodynamic diameters<2.5 µm (PM2.5N) was 35.1 ±â€¯87.4 cm-3 and the mass concentration (PM2.5M) was 12.3 ±â€¯9.1 µg/m3. The PM2.5N and PM2.5M during the continental air mass transport period were 7.2 and 1.3 times higher than those during the non-transport period (109.2 ±â€¯169.3 cm-3, 15.9 ±â€¯14.9 µg/m3), respectively. Excluding transport period, the average PM2.5N and PM2.5M are reduced by 120% and 7%. Coarse mode particle number concentration (PM2.5-10N) and mass concentration (PM2.5-10M) are not significantly influenced by continental air masses (only a reduction of 7% and 2%). The variation of marine aerosol concentrations in different latitudes zones is greatly influenced by continental aerosol transport. The offshore PM2.5M/PM10M was 30%, 21%, and 22% in the mid-latitude sea of South Asia, a low-latitude sea of South Asia, and the equatorial sea, respectively. In comparison, in the remote ocean, the distribution ratio of PM2.5M/PM10M tended to be steady (22%-23%), and the background characteristics of marine aerosols were clearly represented. The aerosol concentration decreases with the increase of wind speed during the transport period, and the wind speed reflects the scavenging effect on aerosol. In the non-transport period, the wind speed at the sea surface promotes the generation of marine aerosols, and the impact in wind speed is strongest in the PM2.5-PM5 particle size range.

2.
Sci Total Environ ; 802: 149695, 2022 Jan 01.
Artigo em Inglês | MEDLINE | ID: mdl-34438127

RESUMO

Particle number size distribution (PNSD) is of importance for understanding the mechanisms of particle growth, haze formation and climate impacts. However, the measurements of PNSD aloft in megacities are very limited. Here we report the first simultaneous winter measurements of size-resolved particle number concentrations along with collocated gaseous species and aerosol composition at ground level and 260 m in Beijing. Our study showed that the vertical differences of particle number concentrations between ground level and aloft varied significantly as a function of particle size throughout the study. Further analysis illustrated the impacts of boundary dynamics and meteorological conditions on the vertical differences of PNSD. In particular, the temperature and relative humidity inversions were one of the most important factors by decoupling the boundary layer into different sources and processes. Positive matrix factorization analysis identified six sources of PNSD at both ground level and city aloft. The local source emissions dominantly contributed to Aitken-mode particles, and showed the largest vertical gradients in the city. Comparatively, the regional particles were highly correlated between ground level and city aloft, and the vertical differences were relatively stable throughout the day. Our results point towards a complex vertical evolution of PNSD due to the changes in boundary layer dynamics, meteorological conditions, sources, and processes in megacities.


Assuntos
Poluentes Atmosféricos , Aerossóis/análise , Poluentes Atmosféricos/análise , Pequim , China , Monitoramento Ambiental , Tamanho da Partícula , Material Particulado/análise , Estações do Ano
3.
Environ Pollut ; 292(Pt A): 118218, 2022 Jan 01.
Artigo em Inglês | MEDLINE | ID: mdl-34571069

RESUMO

Exposure of crops to high concentrations of ozone can cause substantial reductions in yield that pose a serious threat to global food security. Here we provide comprehensive estimates of yield losses for key crops across China between 2014 and 2017 attributed to ozone using a number of new approaches. We use an air quality model at 5 km resolution and crop-specific dose-response functions developed for both concentration- and flux-based metrics. We bias correct modelled ozone concentrations and metrics using observations from more than 1000 locations. We find that on a 4-year average basis, production losses of key crops are 34-91 million metric tonnes (Mt/yr), dependent on the approach used, with highest losses in Henan province. At a national level, loss of winter wheat production derived using a China-specific dose-response function increased by 82% from 2014 to 2017, with large interannual variations in the North China Plain and in eastern China. Winter wheat losses estimated using flux-based functions, which require robust simulation of stomatal conductance and underlying vegetation physiology, are significantly lower, at 30 Mt/yr. We show that the definition of the growing season may have a greater impact on estimated losses than small biases in ozone surface concentrations. Although uncertainties remain, our findings demonstrate that increasing ozone concentrations have substantial adverse impacts on crop yields and threaten food security in China. It is important to control ozone concentrations to mitigate these negative impacts.


Assuntos
Poluentes Atmosféricos , Poluição do Ar , Ozônio , Poluentes Atmosféricos/análise , China , Produtos Agrícolas , Ozônio/análise
4.
Environ Pollut ; 292(Pt B): 118407, 2022 Jan 01.
Artigo em Inglês | MEDLINE | ID: mdl-34715272

RESUMO

Benefiting from the pollution controls implemented by the Chinese government, the concentrations of PM2.5, SO2, NO2 and CO showed a significant decrease in Beijing during 2013-2017. In this study, an observation-based method was employed to estimate the relative contributions of regional transport (MaxRTC) and local emissions (MinLEC) to air pollutant levels during 2013-2017 in Beijing. The results showed that the MaxRTC to SO2 and PM2.5 increased significantly over the five years, while those to CO and NO2 changed little. Furthermore, the difference in the emissions control efficiency (ΔECE) between Beijing (receptor region) and Shijiazhuang (source region), which refers to the concentration changes corresponding to unit emission changes of a certain air pollutant between the two regions, was introduced to verify the estimated variation in MaxRTC and MinLEC over 2013-2017. The negative value of ΔECE found for PM2.5 and SO2 supports the conclusion of an increasing effect of regional transport. This implies that local emissions control alone is not adequate for mitigating Beijing's air pollution, especially with the demand for continuously improving air quality. Joint prevention and control with regard to air quality on a regional scale is more important and urgent in the next Five-Year Plan.


Assuntos
Poluentes Atmosféricos , Poluição do Ar , Poluentes Atmosféricos/análise , Poluição do Ar/análise , Pequim , China , Monitoramento Ambiental , Material Particulado/análise
5.
Sci Total Environ ; 806(Pt 4): 150951, 2022 Feb 01.
Artigo em Inglês | MEDLINE | ID: mdl-34656590

RESUMO

It is very important for air pollution prevention and control to accurately quantify atmospheric environment capacity (AEC) in the planetary boundary layer (PBL). This study developed a high temporal-resolution dynamic multi-box algorithm to estimate PM2.5 AEC with a PBL ceilometer and Doppler wind profile lidar in Beijing City. Compared with the traditional A-value method, two primary improvements are introducing the time coefficient and vertical multi-box assumption into the original box model. The algorithm can accurately calculate the PM2.5 AEC under different circulation patterns and predict the short-time dynamic change of AEC. The results show that the time coefficient effectively reduced the estimation errors when the initial PM2.5 concentration, horizontal wind speed and PBL heights change greatly with time, such situation is consistent with most circulation patterns. And the improvement of multi-box model is much more remarkable when the PM2.5 concentration and horizontal wind change greatly in the vertical direction, such as A, NE and W type circulations. The ideal AEC under polluted circulation patterns won't increase infinitely with wind speed and PBL height, generally less than 30 t/h. The horizontal advection has a much greater effect on expanding the capacity of PM2.5 than the vertical diffusion under clean circulation patterns, and the maximum value of ideal AEC can reach 50 t/h. The positive residual AEC under clean circulations indicates surplus capacity for PM2.5 because of vigorous turbulences, while weak diffusion and ventilation conditions under polluted circulations lead to negative residual AEC and insufficient capacity of atmosphere.


Assuntos
Poluentes Atmosféricos , Poluição do Ar , Poluentes Atmosféricos/análise , Poluição do Ar/análise , Algoritmos , China , Monitoramento Ambiental , Material Particulado/análise , Estações do Ano
6.
J Environ Sci (China) ; 115: 465-473, 2022 May.
Artigo em Inglês | MEDLINE | ID: mdl-34969474

RESUMO

Cross-boundary transport of air pollution is a difficult issue in pollution control for the North China Plain. In this study, an industrial district (Shahe City) with a large glass manufacturing sector was investigated to clarify the relative contribution of fine particulate matter (PM2.5) to the city's high levels of pollution. The Nest Air Quality Prediction Model System (NAQPMS), paired with Weather Research and Forecasting (WRF), was adopted and applied with a spatial resolution of 5 km. During the study period, the mean mass concentrations of PM2.5, SO2, and NO2 were observed to be 132.0, 76.1, and 55.5 µg/m3, respectively. The model reproduced the variations in pollutant concentrations in Shahe at an acceptable level. The simulation of online source-tagging revealed that pollutants emitted within a 50-km radius of downtown Shahe contributed 63.4% of the city's total PM2.5 concentration. This contribution increased to 73.9±21.2% when unfavorable meteorological conditions (high relative humidity, weak wind, and low planetary boundary layer height) were present; such conditions are more frequently associated with severe pollution (PM2.5 ≥ 250 µg/m3). The contribution from Shahe was 52.3±21.6%. The source apportionment results showed that industry (47%), transportation (10%), power (17%), and residential (26%) sectors were the most important sources of PM2.5 in Shahe. The glass factories (where chimney stack heights were normally < 70 m) in Shahe contributed 32.1% of the total PM2.5 concentration in Shahe. With an increase in PM2.5 concentration, the emissions from glass factories accumulated vertically and narrowed horizontally. At times when pollution levels were severe, the horizontally influenced area mainly covered Shahe. Furthermore, sensitivity tests indicated that reducing emissions by 20%, 40%, and 60% could lead to a decrease in the mass concentration of PM2.5 of of 12.0%, 23.8%, and 35.5%, respectively.


Assuntos
Poluentes Atmosféricos , Poluição do Ar , Poluentes Atmosféricos/análise , Poluição do Ar/análise , China , Cidades , Monitoramento Ambiental , Material Particulado/análise , Estações do Ano
7.
Sci Total Environ ; : 151953, 2021 Nov 26.
Artigo em Inglês | MEDLINE | ID: mdl-34843782

RESUMO

We revealed that the absorption aerosol lying below or above the morning residual layer (MRL) promotes (stove effect, heating the MRL layer) or strongly inhibits (dome effect, heating the temperature inversion layer) the development of planetary boundary layer (PBL) after sunrise, while scattering aerosol exhibits similar suppression (surface or aloft umbrella effect) on the PBL regardless of its vertical location. However, the role of different type of aerosols (i.e., strong absorption aerosol and purely scattering aerosol) present from MRL to upper atmosphere remains lacking and therefore, needs to be further explored. Utilizing a large-eddy simulation model constrained by the in-situ observations in urban Beijing, we observed that the dome inhibition of absorption aerosols on PBL development becomes weaker as elevating the aerosol layer, and the effect (virtual dome effect) remains no change beyond a certain height, which is defined as the dome effective height z. This height z is highly related to the surface sensible heat flux. By comparison, the altitude of light-scattering aerosols relative to the MRL was less important. The scattering aerosols exhibit similar inhibition from MRL to upper atmosphere (aloft umbrella effect), but to a weaker extent than the virtual dome effect. The virtual dome effect and aloft umbrella effect play a leading role during some extremely polluted scenarios with deep aerosol layer, such as sandstorms and volcanic eruptions. Aerosol dome, virtual dome, and aloft umbrella effects, together with aerosol stove and surface umbrella effects, further advance the understanding on aerosol-PBL interactions, which is, more broadly, applied to interpret the impact of aerosol on PBL over other ecosystems as well as exoplanet atmospheres.

8.
Environ Pollut ; 294: 118578, 2021 Nov 26.
Artigo em Inglês | MEDLINE | ID: mdl-34843855

RESUMO

Lipids are important biogenic markers to indicate the sources and chemical process of aerosol particles in the atmosphere. To better understand the influences of biogenic and anthropogenic sources on forest aerosols, total suspended particles (TSP) were collected at Mt. Changbai, Shennongjia, and Xishuangbanna that are located at different climatic zones in northeastern, central and southwestern China. n-Alkanes, fatty acids and n-alcohols were detected in the forest aerosols based on gas chromatography-mass spectrometry. The total concentrations of aliphatic compounds ranged from 15.3 ng m-3 to 566 ng m-3, and fatty acids were the most abundant (44-95%) followed by n-alkanes and n-alcohols. Low molecular weight- (LFAs) and unsaturated fatty acids (UnFAs) showed diurnal variation with higher concentrations during the nighttime in summer, indicating the potential impact from microbial activities on forest aerosols. The differences of oleic acid (C18:1) and linoleic acid (C18:2) concentrations between daytime and nighttime increased at lower latitude, indicating more intense photochemical degradation occurred at lower latitude regions. High levels of n-alkanes during daytime in summer with higher values of carbon preference indexes, combining the strong odd carbon number predominance with a maximum at C27 or C29, implied the high contributions of biogenic sources, e.g., higher plant waxes. In contrast, higher concentrations of low molecular weight n-alkanes were detected in winter forest aerosols. Levoglucosan showed a positive correlation (R2 > 0.57) with high- and low molecular weight aliphatic compounds in Mt. Changbai, but such a correlation was not observed in Shennongjia and Xishuangbanna. These results suggest the significant influence of biomass burning in Mt. Changbai, and fossil fuel combustion might be another important anthropogenic source of forest aerosols. This study adds useful information to the current understanding of forest organic aerosols at different geographical locations in China.

9.
Sci Rep ; 11(1): 22824, 2021 Nov 24.
Artigo em Inglês | MEDLINE | ID: mdl-34819530

RESUMO

Vegetable gardens are increasingly common in urban areas and can provide numerous societal benefits; however, contamination with potential toxic elements (PTEs) due to urbanization and industrialization is cause for concern. The present study aimed to assess the source of contamination and pollution levels in urban garden soils, as well as the health risks for adults and children consuming vegetables grown in such environments. Various types of vegetable samples and their corresponding soils from 26 community gardens were collected throughout Chengdu City in southwestern China. The results showed that leafy vegetables, particularly lettuce leaves and Chinese cabbage, had relatively higher levels of Cd (0.04 mg/kg FW) and Pb (0.05 mg/kg FW), while higher levels of As (0.07 mg/kg FW), Cr (0.07 mg/kg FW), and Hg (0.003 mg/kg FW) were found in amaranths, tomatoes, and Houttuynia cordatas, respectively. The pollution indices revealed that the vegetable purplish soils were relatively more polluted by Cd and As, and the concentrations of these metals in vegetables were correlated with their concentrations in the soils. Principal component analysis grouped the PTEs in two dimensions that cumulatively explained 62.3% of their variation, and hierarchical clustering identified two distinct clusters indicating that Cr originated from a unique source. The health risk assessment revealed that exposure to As and Cd induced the greatest non-carcinogenic risk, whereas Cr was most likely to cause cancer risks. Furthermore, contaminated vegetable consumption was riskier for children than adults. The critical factors contributing to PTE contamination in vegetable gardens were determined to be vegetable species, total soil element content, soil pH, and soil organic matter content. Overall, Cr and As pollution present the greatest concern, and community health care services must enact more effective regulatory and preventative measures for urban gardens in terms of PTEs.

10.
Sci Total Environ ; 807(Pt 2): 150306, 2021 Oct 09.
Artigo em Inglês | MEDLINE | ID: mdl-34634352

RESUMO

Aim at the effects of the coastal characteristic on ozone pollution in the Yangtze River Delta (YRD), a campaign was launched at the Ningbo, China in the summer of 2020, which mainly covered the monitoring of the vertical profiles of ozone (O3) concentration, three-dimensional wind field, temperature and humidity profiles and parameters of boundary layer dynamic-thermodynamic structure. At the coastal research station, a sea-land breeze (SLB) circulation accompanied by a concurrent coastal low-level jets (CLLJ) structure was observed and identified during 11-12 May 2020. The sea breeze first formed at 10:00 LT on 11 May, turned to land breeze at night, and returned to sea breeze again at 10:00 LT the next morning, prevailing at altitudes of 0-0.5 km and 0-0.3 km respectively. Land breeze at night carries O3 from the inland to the sea forming high ozone levels over the sea, and the shift of the sea breeze during daytime further blew pollution back to the land. Additionally, the conversion of SLB contributed to the occurrence of CLLJ at the altitudes of ~0.3-0.7 km by 02:00 and 06:00 LT, of which the center of wind speed reached ~13 m s-1. The CLLJ-induced turbulent activity decoupled the residual layer (RL) and stable boundary layer, leading to a reduction of RL-O3 levels and an increase of ~50 µg m-3 in surface-O3 concentration. The YRD's unique coastal characteristics make O3 pollution causes in coastal areas more complicated.

11.
Environ Pollut ; 291: 118114, 2021 Dec 15.
Artigo em Inglês | MEDLINE | ID: mdl-34536649

RESUMO

Low molecular weight organic compounds are ubiquitous in the atmosphere. However, knowledge on their concentrations and molecular distribution in fresh snow remains limited. Here, twelve fresh snow samples collected at eight sites in China were investigated for dicarboxylic acids and related compounds (DCRCs) including oxocarboxylic acids and α-dicarbonyls. Dissolved organic carbon (DOC) concentrations in the snow samples ranged from 0.99 to 14.6 mg C L-1. Concentrations of total dicarboxylic acids were from 225 to 1970 µg L-1 (av. 650 µg L-1), while oxoacids (28.3-173, av. 68.1 µg L-1) and dicarbonyls (12.6-69.2, av. 31.3 µg L-1) were less abundant, accounting for 4.6-8.5% (6.2%), 0.45-1.4% (0.73%), and 0.12-0.88% (0.46%) of DOC, respectively. Molecular patterns of dicarboxylic acids are characterized by a predominance of oxalic acid (C2) (95.0-1030, av. 310 µg L-1), followed by phthalic (Ph) (9.69-244, av. 69.9 µg L-1) or succinic (C4) (23.8-163, av. 63.7 µg L-1) acid. Higher concentrations of Ph in snow from Beijing and Tianjin than other urban and rural regions suggest significant emissions from vehicular exhausts and other fossil fuel combustion sources in megacities. C2 constituted 40-54% of total diacids, corresponding to 1.5-2.6% of snow DOC. The total measured DCRCs represent 5.5-10% of snow DOC, which suggests that there are large amounts of unknown organics requiring further investigations. The spatial distributions of diacids exhibited higher loadings in megacities than rural and island sites. Molecular distributions of diacids indicated that the photochemical modification was restrained under the weak solar radiation during the snow events, while anthropogenic primary sources had a more significant influence in megacities than rural areas and islands.


Assuntos
Poluentes Atmosféricos , Aerossóis/análise , Poluentes Atmosféricos/análise , China , Ácidos Dicarboxílicos/análise , Monitoramento Ambiental , Estações do Ano , Neve
12.
Environ Pollut ; 288: 117783, 2021 Nov 01.
Artigo em Inglês | MEDLINE | ID: mdl-34329065

RESUMO

The Central Plains Economic Region (CPER) located along the transport path to the Beijing-Tianjin-Hebei area has experienced severe PM2.5 pollution in recent years. However, few modeling studies have been performed on the sources of PM2.5, especially the impacts of emission reduction strategies. In this study, the Nested Air Quality Prediction Model System (NAQPMS) with an online tracer-tagging module was adopted to investigate source sectors of PM2.5 and a series of sensitivity tests were conducted to investigate the impacts of different sector-based mitigation strategies on PM2.5 pollution. The response surfaces of pollutants to sector-based emission changes were built. The results showed that resident-related sector (resident and agriculture), fugitive dust, traffic and industry emissions were the main sources of PM2.5 in Zhengzhou, contributing 49%, 19%, 15% and 13%, respectively. Response surfaces of pollutants to sector-based emission changes in Henan revealed that the combined reduction of resident-related sector and industry emissions efficiently decreased PM2.5 in Zhengzhou. However, reduced emissions in only the Henan region barely satisfied the national air quality standard of 75 µg/m3, whereas a 50%-60% reduction in resident-related sector and industry emissions over the whole region could reach this goal. On severely polluted days, even a 60% reduction in these two sectors over the whole region was insufficient to satisfy the standard of 75 µg/m3. Moreover, a reduction in traffic emissions resulted in an increase in the O3 concentration. The results of the response surface method showed that PM2.5 in Zhengzhou decreased by 19% in response to the COVID-19 lockdown, which approached the observed reduction of 21%, indicating that the response surface method could be employed to study the impacts of the COVID-19 lockdown on air pollution. This study provides a scientific reference for the formulation of pollution mitigation strategies in the CPER.


Assuntos
Poluentes Atmosféricos , Poluição do Ar , COVID-19 , Poluentes Atmosféricos/análise , Poluição do Ar/análise , Poluição do Ar/prevenção & controle , China , Controle de Doenças Transmissíveis , Monitoramento Ambiental , Humanos , Material Particulado/análise , SARS-CoV-2
13.
Phys Fluids (1994) ; 33(4): 046605, 2021 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-33953530

RESUMO

A recent study reported that an aerosolized virus (COVID-19) can survive in the air for a few hours. It is highly possible that people get infected with the disease by breathing and contact with items contaminated by the aerosolized virus. However, the aerosolized virus transmission and trajectories in various meteorological environments remain unclear. This paper has investigated the movement of aerosolized viruses from a high concentration source across a dense urban area. The case study looks at the highly air polluted areas of London: University College Hospital (UCH) and King's Cross and St Pancras International Station (KCSPI). We explored the spread and decay of COVID-19 released from the hospital and railway stations with the prescribed meteorological conditions. The study has three key findings: the primary result is that the concentration of viruses decreases rapidly by a factor of 2-3 near the sources although the virus may travel from meters up to hundreds of meters from the source location for certain meteorological conditions. The secondary finding shows viruses released into the atmosphere from entry and exit points at KCSPI remain trapped within a small radial distance of < 50 m. This strengthens the case for the use of face coverings to reduce the infection rate. The final finding shows that there are different levels of risk at various door locations for UCH; depending on which door is used there can be a higher concentration of COVID-19. Although our results are based on London, since the fundamental knowledge processes are the same, our study can be further extended to other locations (especially the highly air polluted areas) in the world.

14.
Sci Total Environ ; 788: 147747, 2021 Sep 20.
Artigo em Inglês | MEDLINE | ID: mdl-34034193

RESUMO

This study used a chemical transport model to investigate the response of secondary inorganic aerosols (SIA) to chemical processes and its precursor emissions over northern and southern city-clusters of China in January 2014. Unexpectedly, SIA concentrations with low levels of precursor emissions were much higher over the southern regions than those over the northern region with high levels of precursor emissions, based on ground observations and high-precision simulations. The sensitivity analysis of chemical processes suggests that the gas-phase chemistry was a critical factor determining the SIA pattern, especially the higher efficiency of nitrogen conversion to nitrate in southern cities controlled by favorable meteorological elements than that in northern city. However, the heterogeneous process led to the decrease of SIA in southern regions by 3% to 36% and the increasing of SIA in NCP by 26.9%, mainly attributing to the impact on nitrate. The reason was that sulfate enhancement by the heterogeneous reactions can compete ammonia (NH3) and the excessive nitric acid converted into nitrogen oxide (NOx), leading to nitrate decrease in southern regions under NH3-deficient regimes. Moreover, through sensitivity experiments of precursor emission reduction by 20%, NH3 control was found to be the most effective for reducing SIA concentrations comparing to sulfur dioxide (SO2) and NOx reduction and a more remarkable decrease of SIA was in southern regions by 10% to 15% than that in northern region by 6.7%. The effect of the synergy control of precursors emission varied in different city-clusters, inferring that the control strategy aimed at improving air quality should be implemented based on specific characteristics of precursors emission in different regions of China.

15.
Indoor Air ; 31(5): 1364-1376, 2021 09.
Artigo em Inglês | MEDLINE | ID: mdl-33876836

RESUMO

Most of human exposure to atmospheric pollutants occurs indoors, and the components of outdoor aerosols may have been changed in the way before reaching indoor spaces. Here we conducted real-time online measurements of mass concentrations and chemical composition of black carbon and the non-refractory species in PM2.5 in an occupied office for approximately one month. The open-close windows and controlled dampness experiments were also performed. Our results show that indoor aerosol species primarily originate from outdoors with indoor/outdoor ratio of these species typically less than unity except for certain organic aerosol (OA) factors. All aerosol species went through filtration upon transport indoors. Ammonium nitrate and fossil fuel OA underwent evaporation or particle-to-gas partitioning, while less oxidized secondary OA (SOA) underwent secondary formation and cooking OA might have indoor sources. With higher particulate matter (PM) mass concentration outdoors than in the office, elevated natural ventilation increased PM exposure indoors and this increased exposure was prolonged when outdoor PM was scavenged. We found that increasing humidity in the office led to higher indoor PM mass concentration particularly more oxidized SOA. Overall, our results highlight that indoor exposure of occupants is substantially different from outdoor in terms of mass concentrations and chemical species.


Assuntos
Aerossóis/análise , Poluentes Atmosféricos/análise , Poluição do Ar em Ambientes Fechados/estatística & dados numéricos , Monitoramento Ambiental , Culinária , Humanos , Umidade , Tamanho da Partícula , Material Particulado , Ventilação
16.
Sci Total Environ ; 770: 144821, 2021 May 20.
Artigo em Inglês | MEDLINE | ID: mdl-33736402

RESUMO

The light absorption black carbon (BC) and brown carbon (BrC) are two important sources of uncertainties in radiative forcing estimate. Here we investigated the light absorption enhancement (Eabs) of BC due to coated materials at an urban (Beijing) and a rural site (Gucheng) in North China Plain (NCP) in winter 2019 by using a photoacoustic extinctiometer coupled with a thermodenuder. Our results showed that the average (±1σ) Eabs was 1.32 (±0.15) at the rural site, which was slightly higher than that at the urban site (1.24 ± 0.15). The dependence of Eabs on coating materials was found to be relatively limited at both sites. However, Eabs presented considerable increases as a function of relative humidity below 70%. Further analysis showed that Eabs during non-heating period in Beijing was mainly caused by secondary components, while it was dominantly contributed by enhanced primary emissions in heating season at both sites. In particular, aerosol particles mixed with coal combustion emissions had a large impact on Eabs (>1.40), while the fresh traffic emissions and freshly oxidized secondary OA (SOA) had limited Eabs (1.00-1.23). Although highly aged or aqueous-phase processed SOA coated on BC showed the largest Eabs, their contributions to the bulk absorption enhancement were generally small. We also quantified the absorption of BrC and source contributions. The results showed the BrC absorption at the rural site was nearly twice that of urban site, yet absorption Ångström exponents were similar. Multiple linear regression analysis highlighted the major sources of BrC being coal combustion emissions and photochemical SOA at both sites with additional biomass burning at the rural site. Overall, our results demonstrated the relatively limited winter light absorption enhancement of BC in different chemical environments in NCP, which needs be considered in regional climate models to improve BC radiative forcing estimates.

17.
J Environ Sci (China) ; 103: 20-32, 2021 May.
Artigo em Inglês | MEDLINE | ID: mdl-33743902

RESUMO

The region along the Taihang Mountains in the North China Plain (NCP) is characterized by serious fine particle pollution. To clarify the formation mechanism and controlling factors, an observational study was conducted to investigate the physical and chemical properties of the fine particulate matter in Jiaozuo city, China. Mass concentrations of the water-soluble ions (WSIs) in PM2.5 and gaseous pollutant precursors were measured on an hourly basis from December 1, 2017, to February 27, 2018. The positive matrix factorization (PMF) method and the FLEXible PARTicle (FLEXPART) model were employed to identify the sources of PM2.5. The results showed that the average mass concentration of PM2.5 was 111 µg/m3 during the observation period. Among the major WSIs, sulfate, nitrate, and ammonium (SNA) constituted 62% of the total PM2.5 mass, and NO3- ranked the highest with an average contribution of 24.6%. NH4+ was abundant in most cases in Jiaozuo. According to chemical balance analysis, SO42-, NO3-, and Cl- might be present in the form of (NH4)2SO4, NH4NO3, NH4Cl, and KCl. The liquid-phase oxidation of SO2 and NO2 was severe during the haze period. The relative humidity and pH were the key factors influencing SO42- formation. We found that NO3- mainly stemmed from homogeneous gas-phase reactions in the daytime and originated from the hydrolysis of N2O5 in the nighttime, which was inconsistent with previous studies. The PMF model identified five sources of PM2.5: secondary origin (37.8%), vehicular emissions (34.7%), biomass burning (11.5%), coal combustion (9.4%), and crustal dust (6.6%).


Assuntos
Poluentes Atmosféricos , Aerossóis/análise , Poluentes Atmosféricos/análise , China , Cidades , Monitoramento Ambiental , Material Particulado/análise , Estações do Ano , Emissões de Veículos/análise
18.
Environ Sci Technol ; 55(8): 4542-4552, 2021 04 20.
Artigo em Inglês | MEDLINE | ID: mdl-33769806

RESUMO

Vertical measurements are essential for the characterization of aerosol and boundary layer interactions; yet, our knowledge of vertical profiles of primary and secondary aerosol species in megacities is limited. Here, we conducted comprehensive vertical measurements of aerosol particle composition on a 325 m meteorological tower with two aerosol chemical speciation monitors in winter in urban Beijing. The simultaneous measurements at ground level, 140, and 240 m illustrated similar aerosol bulk composition at these three heights. However, the vertical ratios varied significantly among different aerosol species. Particularly, the vertical ratios of the aqueous phase and photochemical-related secondary organic aerosol (SOA) (aqOOA/OOA) decreased significantly, accompanied by the increases in ratios of secondary to primary OA, highlighting different chemical properties of OA between ground level and aloft, and the large impacts of vertical changes in meteorology and gaseous precursors on SOA formation. The vertical changes in NO3/SO4 ratios, however, were mostly insignificant, likely due to the low relative humidity and aerosol water content that inhibited nocturnal heterogeneous reactions in the residual layer. Considerable increases in the ratios of 240 m to ground level in the early morning were also observed for most aerosol species, demonstrating impact of residual layer on the air pollution of 2nd day.


Assuntos
Poluentes Atmosféricos , Aerossóis/análise , Poluentes Atmosféricos/análise , Pequim , Monitoramento Ambiental , Meteorologia
19.
Faraday Discuss ; 226: 173-190, 2021 03 01.
Artigo em Inglês | MEDLINE | ID: mdl-33411881

RESUMO

Haze episodes, characterised by extremely high aerosol concentrations and a reduction in visibility to less than 10 km, are a frequent occurrence in wintertime Beijing, despite policy interventions leading to an overall improvement in average annual air quality. The main drivers in the onset of haze episodes in wintertime Beijing are changing synoptic conditions, however, aerosol-radiation interactions and their feedback on boundary layer meteorology are thought to play an essential role in the intensity and longevity of haze episodes. In this study we use a coupled LES aerosol-radiation model (UCLALES-SALSA), which we have recently configured for the urban environment of Beijing. The model's high resolution and control over meteorological and aerosol conditions as well as atmospheric processes means we can directly elucidate and quantify the importance of specific aspects of the aerosol-radiation-meteorology feedback in the cumulative stage of Beijing haze. The main results presented here show (a) synoptic scale meteorology has a larger impact on boundary layer suppression than high aerosol concentrations and (b) unlike previous results obtained using regional models or observationally driven analyses, there is no threshold value at which the aerosol-radiation-meteorology feedback has a significant effect on PBL height. Rather, our work shows that for the aerosol composition in this case study, the role of the feedback effect in reducing PBL height increases under shallow boundary layer conditions and with increasing pollution loading in an almost linear fashion. This lack of a threshold found for our case study has important policy implications since interventions based on such a value will not result in large reductions associated with turning off the feedback process. Furthermore, this work directly shows that although the right synoptic changes are a prerequisite for pollution episodes in Beijing, local and regional emissions drive increases in aerosol load that are sufficient to initiate the aerosol feedback loop. This further drives suppression of the boundary layer top and promotes stagnation of air and increased stability, which can be self-sustaining. This results in higher surface aerosol concentrations for extended periods of time, with severe consequences for human health [Lv et al., Atmos. Environ., 2016, 124, 98-108; Wang et al., Atmos. Chem. Phys., 2019, 19(10), 6949-6967].

20.
Environ Sci Technol ; 55(8): 4344-4356, 2021 04 20.
Artigo em Inglês | MEDLINE | ID: mdl-33502199

RESUMO

Snow serves as a vital scavenging mechanism to gas-phase and particle-phase organic nitrogen substances in the atmosphere, providing a significant link between land-atmosphere flux of nitrogen in the surface-earth system. Here, we used optical instruments (UV-vis and excitation-emission matrix fluorescence) and a Fourier transform ion cyclotron resonance mass spectrometer (FT-ICR MS) to elucidate the molecular composition and potential precursors of snow samples collected simultaneously at four megacities in North China. The elemental O/N ratio (≥3), together with the preference in the negative ionization mode, indicates that the one and two nitrogen atom-containing organics (CHON1 and CHON2) in snow were largely in the oxidized form (as organic nitrates, -ONO2). This study assumed that scavenging of particle-phase and gas-phase organic nitrates might be significant sources of CHON in precipitation. A gas-phase oxidation process and a particle-phase hydrolysis process, at a molecular level, were used to trace the potential precursors of CHON. Results show that more than half of the snow CHON molecules may be related to the oxidized and hydrolyzed processes of atmospheric organics. Potential formation processes of atmospheric organics on a molecular level provide a new concept to better understand the sources and scavenging mechanisms of organic nitrogen species in the atmosphere.


Assuntos
Nitrogênio , Neve , Atmosfera , China , Análise de Fourier , Nitrogênio/análise
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