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1.
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
2.
J Environ Sci (China) ; 104: 242-252, 2021 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-33985727

RESUMO

Extensive studies on aerosol chemistry have been carried out in megacities in China, however, aerosol characterization in Central China Plain (CCP) is limited. Here we conducted real-time measurements of fine particle composition with a time-of-flight aerosol chemical speciation monitor in Kaifeng, Henan province in October 2019. Our results showed that nitrate and organics constituted the major fraction of non-refractory PM2.5 for the entire study, on average accounting for 34% and 33%, respectively. However, aerosol composition was substantially different among four periods due to different meteorological conditions and chemical processing. For instance, nitrate presented the lowest contribution during the first period due to evaporative loss associated with high temperature (T), and then rapidly increased during polluted periods as a function of relative humidity (RH). Positive matrix factorization analysis showed the dominance of secondary organic aerosol (SOA) in OA, and also the changes in OA composition under different T and RH levels. In addition, this study is unique with two periods of local emission controls. Back trajectory and coefficient of divergence analysis showed that air pollution in CCP was overall homogeneously distributed. As a result, the effectiveness of local emission controls in this region was strongly affected by meteorological conditions and regional transport. We found that one of the periods with emission control even showed the highest concentrations for the entire study. Our results point towards the limited effect of local emission controls in mitigating air pollution in CCP, and highlight the importance of joint emission controls under unfavorable meteorological conditions.


Assuntos
Poluentes Atmosféricos , Material Particulado , Aerossóis/análise , Poluentes Atmosféricos/análise , China , Cidades , Monitoramento Ambiental , Material Particulado/análise
3.
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.

4.
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
5.
Proc Natl Acad Sci U S A ; 118(8)2021 02 23.
Artigo em Inglês | MEDLINE | ID: mdl-33593919

RESUMO

Secondary organic aerosol (SOA) produced by atmospheric oxidation of primary emitted precursors is a major contributor to fine particulate matter (PM2.5) air pollution worldwide. Observations during winter haze pollution episodes in urban China show that most of this SOA originates from fossil-fuel combustion but the chemical mechanisms involved are unclear. Here we report field observations in a Beijing winter haze event that reveal fast aqueous-phase conversion of fossil-fuel primary organic aerosol (POA) to SOA at high relative humidity. Analyses of aerosol mass spectra and elemental ratios indicate that ring-breaking oxidation of POA aromatic species, leading to functionalization as carbonyls and carboxylic acids, may serve as the dominant mechanism for this SOA formation. A POA origin for SOA could explain why SOA has been decreasing over the 2013-2018 period in response to POA emission controls even as emissions of volatile organic compounds (VOCs) have remained flat.

6.
Chemosphere ; 258: 127310, 2020 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-32947673

RESUMO

We characterized the aerosol composition and sources of particulate matter (PM) in Sanmenxia, a polluted city located in the Fen-Wei Plain region of Central China. The PM2.5 concentration decreased by 18% from 72 µg m-3 in 2014 to 59 µg m-3 in 2019. All chemical species presented pronounced seasonal variations, with their highest concentrations in winter due to enhanced emissions and the frequent stagnant meteorological conditions. Nitrate was the major fraction of PM2.5 during all seasons (35-41%) except summer (25%), while sulfate was a dominant species in summer (29%) compared to other seasons (16-18%) from July 2018 to June 2019. The detailed analysis of a wintertime severe haze episode that lasted for approximately half a month demonstrated that secondary aerosols, including secondary organic aerosol, sulfate, nitrate, and ammonium, contributed 89% to non-refractory PM1 (NR-PM1), indicating the remarkable role of secondary aerosol formation in air pollution in Sanmenxia. Positive matrix factorization analysis further showed considerably enhanced low-volatility oxygenated organic aerosol (OA) and hydrocarbon-like OA during severe haze episodes, while significant contributions in semi-volatile oxygenated OA and coal combustion OA during clean periods. Severe pollution events in the city were generally associated with air masses from the southwest, and we also found that aerosol species, especially secondary aerosol species, showed distinct forenoon increases that were caused by the subsidence of air pollutants aloft. Our results highlight that future air quality improvement would benefit substantially from a more efficient control of gaseous precursors, particularly the NOx emissions from industry and vehicle emissions.


Assuntos
Aerossóis/análise , Poluentes Atmosféricos/análise , Poluição do Ar/estatística & dados numéricos , Poluição do Ar/análise , China , Cidades , Carvão Mineral/análise , Monitoramento Ambiental/métodos , Poluentes Ambientais/análise , Poluição Ambiental/análise , Hidrocarbonetos/química , Nitratos/análise , Óxidos de Nitrogênio/análise , Material Particulado/análise , Estações do Ano , Emissões de Veículos/análise
7.
Chemosphere ; 255: 126850, 2020 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-32402868

RESUMO

Water-soluble organic aerosol (WSOA) constitutes a large fraction of OA and plays an important role in formation of secondary OA (SOA). Here we characterized the sources and molecular composition of WSOA in summer in Beijing using high-resolution aerosol mass spectrometer and orbitrap mass spectrometer equipped with electrospray ionization. Our results showed that WSOA was the major fraction of OA on average accounting for 69% in summer, which is much higher than that (47%) in winter. However, the oxidation degree of WSOA was comparable between summer and winter (O/C = 0.62 vs. 0.63). Positive matrix factorization analysis showed that SOA contributed dominantly to WSOA (72%) indicating that WSOA was mainly from secondary formation. The two water-soluble SOA factors that are associated with regional processing (OOA-1) and photochemical production (OOA-2), respectively, showed very different behaviors throughout the study. OOA-2 showed much enhanced contribution during polluted periods with low relative humidity (RH), while OOA-1 played a more important role during high RH periods. Molecular composition analysis of WSOA revealed a high diversity of CHO (compounds only containing carbon, hydrogen and oxygen) and CHOS (sulfur-containing organics) in WSOA in summer. Particularly, the relative intensity fraction of CHOS- compounds was increased by 42% from clean to polluted days which was associated with large increases (20%) in organosulfates (OSs) with lower O∗/C (0.1-0.4), and OOA-1. These results suggest the formation of more unsaturated OSs in OOA-1 during polluted days in summer. Comparatively, the biogenic-derived OSs remained relatively stable (24-31%) for the entire study highlighting the ubiquitous importance of biogenic SOA in summer.


Assuntos
Aerossóis/análise , Poluentes Atmosféricos/análise , Monitoramento Ambiental , Pequim , Umidade , Espectrometria de Massas , Oxirredução , Estações do Ano , Água/análise
8.
Environ Pollut ; 263(Pt B): 114455, 2020 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-32278981

RESUMO

Black carbon (BC) exerts a large impact on climate radiative forcing and public health, and such impacts depend strongly on chemical composition and mixing state. Here a single particle aerosol mass spectrometry (SPA-MS) along with an aerosol chemical speciation monitor was employed to characterize the composition and mixing state of BC-containing particles in summer and winter in Beijing. Approximately 2 million BC-containing particles were chemically analyzed, and the particles were classified into nine and eight different types in summer and winter, respectively, according to mass spectral signatures and composition. The BC-containing particles in summer were dominated by the type of nitrate-related BC (BC-N, 56.7%), while in winter the BC mixed with organic carbon (OC) and sulfate (BCOC-S), and OC and nitrate (BCOC-N) were two dominant types accounting for 44.9% and 16.6%, respectively. The number fractions of BC-N in summer, and BCOC-N and BC-SN in winter increased largely during periods with severe air pollution, suggesting the enhanced secondary formation on BC-containing particles. We also found that the primary emissions of the biomass burning and coal combustion can affect BC mixing state substaintially as indicated by the considerable fraction of BC mixed with levoglucosan and polycyclic aromatic hydrocarbons in winter. Bivariate polar plots and back trajectory analysis indicated that the sulfate-associated BC-containing particles were mostly from regional transport while the nitrate-related type was more from local production. The optical parameter of absorbing Ångström exponents (AAE) of BC was 1.2 and 1.5 in summer and winter, respectively, and the AAE dependence of BC mixing state was also different in the two seasons. While higher fractions of BC-N were observed during lower AAE periods in summer, the variations of dominant OC-related BC-containing particles in winter were fairly stable as a function of AAE.


Assuntos
Poluentes Atmosféricos/análise , Aerossóis/análise , Pequim , Carbono/análise , Monitoramento Ambiental , Material Particulado/análise , Estações do Ano
9.
Sci Total Environ ; 710: 136336, 2020 Mar 25.
Artigo em Inglês | MEDLINE | ID: mdl-31926416

RESUMO

Land surface temperature (LST) is defined as an important indicator in the formation and evolution of climate. In some cases, changes in landscape patterns affect LST, even more than the contribution of greenhouse gases. Although much work has been done with respect to the correlations between urban development and thermal environment dynamics, the related questions regarding relationships between LST and landscape patterns in arid regions are not thoroughly considered. Understanding these questions is important in climate change and land planning. The objective of this study was to explore the spatiotemporal variations of LST by distribution index (DI) and Mann-Kendall mutation analysis method and to quantify the relationships between landscape patterns, climatic factors, topographic factors, and the land surface thermal environment (LSTE) by the ordinary linear regressions (OLS) model. The landscape patterns dataset, which was validated by a field trip, was extracted from the Land satellite (Landsat) TM/OLI images by the Random Forest methodology in ArcGIS software. The MODIS/LST product was validated by the "Monthly dataset of China's surface climate" and a field trip. Annual LST increased by 0.54 °C (23.15 °C in 2000 and 23.79 °C in 2015). In different landscape patterns, the percentage of areas with a high level of LST showed a significant difference. In barren land, the highest area proportion for the high LST level was larger than in other landscape patterns. Meanwhile, the area of low LST was mainly concentrated in water bodies. Considerable changes have occurred in landscape patterns, in which the most noteworthy was cultivated land encroaching on grass land (3708.44 km2). The composition of landscape patterns was more important than distribution in determining the region's LST. These findings provide valuable information for land planners dealing with climate change and ecosystem conservation in arid regions.

10.
Environ Pollut ; 255(Pt 2): 113345, 2019 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-31610508

RESUMO

Despite substantial mitigation of particulate matter (PM) pollution during the past decade in Beijing, the response of aerosol chemistry to clean air action and meteorology remains less understood. Here we characterized the changes in aerosol composition as responses to emission reductions by using two-year long-term measurements in 2011/2012 and 2017/2018, and WRF-Chem model. Our results showed substantial decreases for all aerosol species except nitrate from 2011/2012 to 2017/2018. Chloride exhibited the largest decrease by 65-89% followed by organics (37-70%), mainly due to reductions in coal combustion emissions in winter and agriculture burning in June. Primary and secondary organic aerosol (SOA) showed comparable decreases by 61-70% in fall and winter, and 34-63% in spring and summer, suggesting that reductions in primary emissions might also suppress SOA formation. The changes in nitrate were negligible and even showed increases due to less reductions in NOx emissions and increased formation potential from N2O5 heterogeneous reactions. As a result, nitrate exceeded sulfate and became the major secondary inorganic aerosol species in PM with the contribution increasing from 14-21% to 22-32%. Further analysis indicated that the reductions in aerosol species from 2011/2012 to 2017/2018 were mainly caused by the decreases of severely polluted events (PM1 > 100 µg m-3). WRF-Chem simulations suggested that the decreases in OA and sulfate in fall and winter were mainly resulted from emission reductions (27-36% and 25-43%) and favorable meteorology (4-10% and 19-30%), while they were dominantly contributed by emission changes in spring and summer. Comparatively, the changes in nitrate were mainly associated with meteorological variations while the contributions of emissions changes were relatively small. Our results highlight different chemical responses of aerosol species to emission changes and meteorology, suggesting that future mitigation of air pollution in China needs species-targeted control policy.


Assuntos
Aerossóis/análise , Poluentes Atmosféricos/análise , Poluição do Ar/estatística & dados numéricos , Monitoramento Ambiental , Material Particulado/análise , Poluição do Ar/análise , Pequim , China , Óxidos de Nitrogênio/análise , Estações do Ano , Sulfatos/análise
11.
Environ Sci Technol ; 53(14): 7984-7995, 2019 Jul 16.
Artigo em Inglês | MEDLINE | ID: mdl-31257870

RESUMO

Atmospheric aerosols over polar regions have attracted considerable attention for their pivotal effects on climate change. In this study, temporospatial variations in single-particle-based depolarization ratios (δ: s-polarized component divided by the total backward scattering intensity) were studied over the Northwest Pacific and the Arctic Ocean using an optical particle counter with a depolarization module. The δ value of aerosols was 0.06 ± 0.01 for the entire observation period, 61 ± 10% lower than the observations for coastal Japan (0.12 ± 0.02) ( Pan et al. Atmos. Chem. Phys. 2016 , 16 , 9863 - 9873 ) and inland China (0.19 ± 0.02) ( Tian et al. Atmos. Chem. Phys. 2018 , 18 , 18203 - 18217 ) in summer. The volume concentration showed two dominant size modes at 0.9 and 2 µm. The supermicrometer particles were mostly related to sea-salt aerosols with a δ value of 0.09 over marine polar areas, ∼22% larger than in the low-latitude region because of differences in chemical composition and dry air conditions. The δ values for fine particles (<1 µm) were 0.05 ± 0.1, 50% lower than inland anthropogenic pollutants, mainly because of the complex mixtures of submicrometer sea salts. High particle concentrations in the Arctic Ocean could mostly be attributed to the strong marine emission of sea salt associated with deep oceanic cyclones, whereas long-range transport pollutants from the continent were among the primary causes of high particle concentrations in the Northwest Pacific region.


Assuntos
Poluentes Atmosféricos , Aerossóis , Regiões Árticas , China , Monitoramento Ambiental , Japão , Oceanos e Mares , Oceano Pacífico , Tamanho da Partícula
12.
Sci Total Environ ; 681: 226-234, 2019 Sep 01.
Artigo em Inglês | MEDLINE | ID: mdl-31103660

RESUMO

To understand the temporal characteristics and vertical distributions of ammonia (NH3) and ammonium (NH4) in urban Beijing, we conducted ground-based and tower-based measurements of gaseous NH3 and submicron aerosol composition. The average mixing ratio of NH3 was 16.5 ±â€¯7.4 ppb, ranging from 3.8 to 36.9 ppb. Gas-to-particle partitioning of NHx (=NH3 + NH4) played a significant role on NH3 concentration as the molar ratio of NH3 to NHx decreased as a function of NH4 concentration. The NH3 concentrations increased as a function of PM1 at lower levels (<125 µg m-3), but remained relatively constant at higher PM and NH4 levels, indicating an enhanced gas-to-particle conversion of NH3 during highly polluted conditions. The potential sources of NHx were found to include fossil fuel combustion and biomass burning. Regional transport could also play an important role on NH3 concentration during the formation stage of haze episodes due to particle-to-gas conversion. Four distinctive types of vertical profiles (87% of the time) of both NH3 and fine particle light extinction coefficient (bext) were observed and they were associated with well-mixed atmosphere, fast accumulation of local emissions, regional transport aloft, and the formation of low urban boundary layer, respectively. However, the vertical profiles of NH3 typically (96% of the time) showed a more homogeneous characteristic than those of bext below 260 m, except periods with both strong temperature inversion and large aerosol gradient, the formation of urban boundary layer shall cause a significant transition in the vertical distribution of NH3 below 260 m. During highly polluted situations (PM1 > 125 µg m-3), the strong effect of gas-to-particle partitioning of NHx sometimes (7% of the time) caused opposite trends in vertical profiles of NH3 and bext.

13.
Environ Sci Technol ; 51(24): 14072-14082, 2017 Dec 19.
Artigo em Inglês | MEDLINE | ID: mdl-29131606

RESUMO

Refractory black carbon (rBC) aerosol is an important climate forcer, and its impacts are greatly influenced by the species associated with rBC cores. However, relevant knowledge is particularly lacking at the Tibetan Plateau (TP). Here we report, for the first time, highly time-resolved measurement results of rBC and its coating species in central TP (4730 m a.s.l), using an Aerodyne soot particle aerosol mass spectrometer (SP-AMS), which selectively measured rBC-containing particles. We found that the rBC was overall thickly coated with an average mass ratio of coating to rBC (RBC) of ∼7.7, and the coating species were predominantly secondarily formed by photochemical reactions. Interestingly, the thickly coated rBC was less oxygenated than the thinly coated rBC, mainly due to influence of the transported biomass burning organic aerosol (BBOA). This BBOA was relatively fresh but formed very thick coating on rBC. We further estimated the "lensing effect" of coating semiquantitatively by comparing the measurement data from a multiangle absorption photometer and SP-AMS, and found it could lead to up to 40% light absorption enhancement at RBC > 10. Our findings highlight that BBOA can significantly affect the "lensing effect", in addition to its relatively well-known role as light-absorbing "brown carbon."


Assuntos
Aerossóis , Poluentes Atmosféricos , Fuligem , Biomassa , Carbono , Tibet
14.
Environ Sci Pollut Res Int ; 24(26): 21386-21397, 2017 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-28744677

RESUMO

Brown carbon (BrC) has recently received much attention because of its light absorption features. The chemical compositions, optical properties, and sources of fine aerosol at a high-elevation mountain observatory (4730 m a.s.l.) in the central Tibetan Plateau were measured between 31 May and 1 July 2015. A low flow-rate sampler was used to collect 24-h average fine particulate matter (PM2.5) filter samples. Water-soluble ions, organic carbon (OC), elemental carbon, water-soluble organic carbon (WSOC), and light absorption by water-soluble BrC were determined for 26 filter samples. The mean (± 1σ) OC and WSOC concentrations were 0.76 ± 0.43 and 0.39 ± 0.15 µgC/m3, respectively, and the mean WSOC/OC mass ratio was 0.59 ± 0.22. The OC and WSOC concentrations were relatively higher (0.59-1.80 and 0.33-0.83 µgC/m3, respectively) during the pre-monsoon period (2-13 June) and were relatively lower (0.27-0.77 and 0.12-0.50 µgC/m3, respectively) during the monsoon period (14 June to 1 July), probably because of wet scavenging of aerosols during long-range transport and the presence of cleaner marine air masses during the monsoon period. The absorption spectra of PM2.5 water extracts smoothly increase from visible range to ultraviolet range. The absorption Ångström exponent, which describes the wavelength dependence of water-soluble BrC, was 2.74-10.61 (mean 6.19 ± 1.70), and its value was similar in the pre-monsoon period (6.57 ± 0.56) to that in the monsoon period (5.91 ± 2.14). The water-soluble BrC mass absorption efficiency, 0.38 ± 0.16 m2/(g C), was much lower than those observed in most urban areas but similar to those in other remote sites. Absorption coefficient at 365 nm, typically used as a proxy for water-soluble BrC, correlated well with the WSOC concentration (R 2  = 0.57), K+ concentration (R 2  = 0.75), and organic aerosol biomass burning markers characterized by an Aerodyne aerosol mass spectrometer (C2H4O2+ + C3H5O2+, R 2  = 0.60). It can be inferred that biomass burning was an important source of water-soluble BrC in the study area combined with air mass back trajectory analysis using the NOAA HYSPLIT as well as MODIS data of fire dots and aerosol optical depths. The water-soluble BrC to BC light absorption (at 365 nm) coefficient ratios were 9-27%.


Assuntos
Poluentes Atmosféricos/análise , Carbono/análise , Monitoramento Ambiental/métodos , Luz , Material Particulado/análise , Água/química , Aerossóis , Movimentos do Ar , Altitude , Solubilidade , Tibet
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