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1.
Sci Total Environ ; 814: 152775, 2022 Jan 04.
Artigo em Inglês | MEDLINE | ID: mdl-34990674

RESUMO

The investigation of water-soluble organic carbon (WSOC), which is important in the biogeochemical cycle of precipitation, can provide a comprehensive view of chromophores within the atmospheric boundary layer. In this work, the optical properties and molecular characteristics of WSOC in precipitation over the Guanzhong Basin (GB) of North China were investigated using ultraviolet-visible (UV-vis) absorption and excitation-emission matrix (EEM) fluorescence spectra, and Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) coupled with electrospray ionization (ESI). Furthermore, sources and wet deposition of WSOC were estimated using in-situ measurements and modeling. The light-absorption by WSOC at 250-300 nm (UV region) and 400-550 nm (visible region) was 64.17% and 15.36% relative to the estimated total light-absorption, respectively. Parallel factor (PARAFAC) analysis revealed three types of fluorophores in WSOC at Xi'an (XN), including two humic-like substances (HULIS) and one protein-like substance (PRLIS), with HULIS accounting for 79% of total fluorescence intensity. FT-ICR MS analysis revealed that CHO and CHON were the most abundant components of WSOC at XN, each containing a variety of lignins, protein/amino sugars, and lipids. Moreover, the positive matrix factorization (PMF) model identified the contributions from three main sources (secondary precursors and aerosols, and coal combustion) of WSOC in precipitation at XN. The annual wet deposition flux of WSOC in precipitation at XN was estimated as about 0.63 g C m-2 yr-1, lower than that at other polluted cities. These findings add to our understanding of chromophoric dissolved organic carbon budgets, which is critical for accurately assessing the global carbon cycle.

2.
Chemosphere ; 288(Pt 1): 132377, 2022 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-34600012

RESUMO

Volatile methyl siloxanes (VMS) have been widely used in personal care products and industrial applications, and are an important component of VOCs (volatile organic compounds) indoors. They have sufficiently long lifetimes to undergo long-range transport and to form secondary aerosols through atmospheric oxidation. To investigate these silicon-containing secondary organic aerosols (Si-SOA), we collected PM2.5 samples during 8th-21st August 2018 (summer) and 3rd-23rd January 2019 (winter) at an urban site of Beijing. As the oxidation of VMS mainly results in hydrophilic polar semi-volatile and non-volatile oxidation products, the differences between total water-soluble Si and total water-soluble inorganic Si were used to estimate water-soluble organic Si, considered to be secondary organic Si (SO-Si). The average concentrations of SO-Si during the summer and winter campaigns were 4.6 ± 3.7 and 13.2 ± 8.6 ng m-3, accounting for approximately 80.1 ± 10.1% and 80.2 ± 8.7% of the total water-soluble Si, and 1.2 ± 1.2% and 5.0 ± 6.9% of total Si in PM2.5, respectively. The estimated Si-SOA concentrations were 12.7 ± 10.2 ng m-3 and 36.6 ± 23.9 ng m-3 on average in summer and winter, which accounted for 0.06 ± 0.07% and 0.16 ± 0.22% of PM2.5 mass, but increased to 0.26% and 0.92% on certain days. We found that net solar radiation is positively correlated with SO-Si levels in the summer but not in winter, suggesting seasonally different formation mechanisms.


Assuntos
Poluentes Atmosféricos , Compostos Orgânicos Voláteis , Aerossóis/análise , Poluentes Atmosféricos/análise , Pequim , Monitoramento Ambiental , Material Particulado/análise , Silício , Compostos Orgânicos Voláteis/análise
3.
Environ Sci Technol ; 56(1): 175-184, 2022 Jan 04.
Artigo em Inglês | MEDLINE | ID: mdl-34898191

RESUMO

Biogenic volatile organic compound (BVOC) emissions have long been known to play vital roles in modulating the formation of ozone and secondary organic aerosols (SOAs). While early studies have evaluated their impact globally or regionally, the BVOC emissions emitted from urban green spaces (denoted as U-BVOC emissions) have been largely ignored primarily due to the failure of low-resolution land cover in resolving such processes, but also because their important contribution to urban BVOCs was previously unrecognized. In this study, by utilizing a recently released high-resolution land cover dataset, we develop the first set of emission inventories of U-BVOCs in China at spatial resolutions as high as 1 km. This new dataset resolved densely distributed U-BVOCs in urban core areas. The U-BVOC emissions in megacities could account for a large fraction of total BVOC emissions, and the good agreement of the interannual variations between the U-BVOC emissions and ozone concentrations over certain regions stresses their potentially crucial role in influencing ozone variations. The newly constructed U-BVOC emission inventory is expected to provide an improved dataset to enable the research community to re-examine the modulation of BVOCs on the formation of ozone, SOA, and atmospheric chemistry in urban environments.

4.
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
5.
Sci Total Environ ; 805: 150284, 2022 Jan 20.
Artigo em Inglês | MEDLINE | ID: mdl-34537711

RESUMO

Solid-phase extraction (SPE) is a traditional pretreatment procedure widely used for dissolved organic matter (DOM) desalination and enrichment prior to the Fourier transform-ion cyclotron resonance mass spectrometry (FT-ICR MS) analysis, and the extracts are usually acidified to pH = 2 with hydrochloric acid (HCl) before passing through the cartridge. However, little is known about the effects of acidification on the integrity and molecular composition of DOM. Here, the differences in the molecular compositions in acidified and nonacidified DOM samples of soil, seawater and atmospheric aerosol were performed by FT-ICR MS. The results showed that the quantity and intensity of aromatic compounds with high oxygen content (e.g., polyphenols, tannin-like and highly oxygenated organic compounds) were greatly enhanced after acidification, while highly saturated compounds (lipid-like and aliphatic/peptide-like) were absent. The underlying reason is the variation of solubility and hydrolysis of DOM under acidic conditions. Meanwhile, the effect of acidification on the molecular composition of DOM was also dependent on their original environmental media. Based on these results, we suggest that the extracts of soil samples are selectively acidified according to the focus of research, while the extract is acidified for seawater samples and the pH of the extract can be unadjusted for aerosol samples before the SPE procedure. These findings provide a reference for the selection of suitable pretreatment methods for different experimental purposes and for the comprehensive characterization of samples with different properties.


Assuntos
Compostos Orgânicos , Extração em Fase Sólida , Concentração de Íons de Hidrogênio , Espectrometria de Massas , Solo
6.
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.

7.
Environ Sci Technol ; 55(23): 15680-15693, 2021 12 07.
Artigo em Inglês | MEDLINE | ID: mdl-34775752

RESUMO

Molecular analyses help to investigate the key precursors and chemical processes of secondary organic aerosol (SOA) formation. We obtained the sources and molecular compositions of organic aerosol in PM2.5 in winter in Beijing by online and offline mass spectrometer measurements. Photochemical and aqueous processing were both involved in producing SOA during the haze events. Aromatics, isoprene, long-chain alkanes or alkenes, and carbonyls such as glyoxal and methylglyoxal were all important precursors. The enhanced SOA formation during the severe haze event was predominantly contributed by aqueous processing that was promoted by elevated amounts of aerosol water for which multifunctional organic nitrates contributed the most followed by organic compounds having four oxygen atoms in their formulae. The latter included dicarboxylic acids and various oxidation products from isoprene and aromatics as well as products or oligomers from methylglyoxal aqueous uptake. Nitrated phenols, organosulfates, and methanesulfonic acid were also important SOA products but their contributions to the elevated SOA mass during the severe haze event were minor. Our results highlight the importance of reducing nitrogen oxides and nitrate for future SOA control. Additionally, the formation of highly oxygenated long-chain molecules with a low degree of unsaturation in polluted urban environments requires further research.

8.
Environ Sci Technol ; 2021 Oct 26.
Artigo em Inglês | MEDLINE | ID: mdl-34699200

RESUMO

Aqueous extracts of biogenic secondary organic aerosols (BSOAs) have been found to exhibit fluorescence that may interfere with the laser/light-induced fluorescence (LIF) detection of primary biological aerosol particles (PBAPs). In this study, we quantified the interference of BSOAs to PBAPs by directly measuring airborne BSOA particles, rather than aqueous extracts. BSOAs were generated by the reaction of d-limonene (LIM) or α-pinene (PIN) and ozone (O3) with or without ammonia in a chamber under controlled conditions. With an excitation wavelength of 355 nm, BSOAs exhibited peak emissions at 464-475 nm, while fungal spores exhibited peak emissions at 460-483 nm; the fluorescence intensity of BSOAs with diameters of 0.7 µm was in the same order of magnitude as that of fungal spores with diameters of 3 µm. The number fraction of 0.7 µm BSOAs that exhibited fluorescence above the threshold was in the range of 1.9-15.9%, depending on the species of precursors, relative humidity (RH), and ammonia. Similarly, the number fraction of 3 µm fungal spores that exhibited fluorescence above the threshold was 4.9-36.2%, depending on the species of fungal spores. Normalized fluorescence by particle volumes suggests that BSOAs exhibited fluorescence in the same order of magnitude as pollen and 10-100 times higher than that of fungal spores. A comparison with ambient particles suggests that BSOAs caused significant interference to ambient fine particles (15 of 16 ambient fine particle measurements likely detected BSOAs) and the interference was smaller for ambient coarse particles (4 of 16 ambient coarse particle measurements likely detected BSOAs) when using LIF instruments.

9.
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
10.
Environ Sci Technol ; 2021 Aug 25.
Artigo em Inglês | MEDLINE | ID: mdl-34428888

RESUMO

Until now, there has been a lack of knowledge regarding the vertical profiles of nitrate formation in the urban boundary layer (BL) based on triple oxygen isotopes. Here, we conducted vertical measurements of the oxygen anomaly of nitrate (Δ17O-NO3-) on a 325 m meteorological tower in urban Beijing during the winter and summer. The simultaneous vertical measurements suggested different formation mechanisms of nitrate aerosols at ground level and 120 and 260 m in the winter due to the less efficient vertical mixing under stable atmospheric conditions. Particularly, different chemical processes of nitrate aerosols at the three heights were found between clean days and polluted days in the winter. On clean days, nocturnal chemistry (NO3 + HC and N2O5 uptake) contributed to nitrate production equally with OH/H2O + NO2 at ground level, while it dominated aloft (contributing 80% of nitrate production at 260 m), due to the higher aerosol liquid water content and O3 concentration there. On polluted days, nocturnal reactions dominated the formation of nitrate at the three heights. Particularly, the contribution of the OH/H2O + NO2 pathway to nitrate production increased from the ground level to 120 m might be attributed to the hydrolysis of NO2 to HONO and then further photolysis to OH radicals in the day. In contrast, the proportion of N2O5 + H2O decreased at 260 m, likely due to the low relative humidity aloft that inhibited the N2O5 hydrolysis reactions in the residual layer. Our results highlighted that the differences between meteorology and gaseous precursors could largely affect particulate nitrate formation at different heights within the polluted urban BL.

11.
Sci Total Environ ; 797: 149115, 2021 Nov 25.
Artigo em Inglês | MEDLINE | ID: mdl-34346364

RESUMO

Terrestrial lipid biomarkers are one of the key tracers in the studies of atmospheric aerosols. Here, we investigated such organic compounds in marine aerosols collected at Chichijima Island, the western North Pacific for two 4-year periods: 1990-1993 and 2006-2009. A homologous series of lipid biomarkers including C18-C37n-alkanes, C9-C34 fatty acids, and C14-C35 fatty alcohols were determined by gas chromatography/mass spectrometry (GC/MS). The atmospheric levels of these tracers increased from 1990-1993 to 2006-2009. Their seasonal trends were clearly characterized by winter-spring maxima and summer-fall minima. The relative abundance of the high-molecular-weight (HMW) n-alkanes (C25-C37) and n-alcohols (C20-C35) in total HMW lipids peaked in winter and winter/fall, respectively, whereas those of HMW fatty acids (C20-C34) peaked in summer. Air-mass backward trajectory analyses suggest that the Asian continent, Southeast Asia including tropical regions, and the Central Pacific are the main source regions. The seasonal shift and distribution of the carbon preference index and average chain length for the HMW lipids were controlled by the changes in climatic factors and source regions. The higher abundance of terrestrial lipids during 2006-2009 than 1990-1993 indicates a higher emission from terrestrial plantation in the 2000s than in the early 1990s in upwind regions of East Asia. Furthermore, HMW lipid compounds exhibited much stronger positive correlations with levoglucosan, a biomass-burning tracer, during 2006-2009 than 1990-1993, suggesting that biomass-burning emissions contributed more significantly in this century.


Assuntos
Poluentes Atmosféricos , Aerossóis/análise , Poluentes Atmosféricos/análise , Biomarcadores , Biomassa , Monitoramento Ambiental , Lipídeos/análise , Material Particulado/análise , Estações do Ano
12.
Atmos Chem Phys ; 21(7): 5549-5573, 2021 Apr 12.
Artigo em Inglês | MEDLINE | ID: mdl-34462630

RESUMO

Epidemiological studies have consistently linked exposure to PM2.5 with adverse health effects. The oxidative potential (OP) of aerosol particles has been widely suggested as a measure of their potential toxicity. Several acellular chemical assays are now readily employed to measure OP; however, uncertainty remains regarding the atmospheric conditions and specific chemical components of PM2.5 that drive OP. A limited number of studies have simultaneously utilised multiple OP assays with a wide range of concurrent measurements and investigated the seasonality of PM2.5 OP. In this work, filter samples were collected in winter 2016 and summer 2017 during the atmospheric pollution and human health in a Chinese megacity campaign (APHH-Beijing), and PM2.5 OP was analysed using four acellular methods: ascorbic acid (AA), dithiothreitol (DTT), 2,7-dichlorofluorescin/hydrogen peroxidase (DCFH) and electron paramagnetic resonance spectroscopy (EPR). Each assay reflects different oxidising properties of PM2.5, including particle-bound reactive oxygen species (DCFH), superoxide radical production (EPR) and catalytic redox chemistry (DTT/AA), and a combination of these four assays provided a detailed overall picture of the oxidising properties of PM2.5 at a central site in Beijing. Positive correlations of OP (normalised per volume of air) of all four assays with overall PM2.5 mass were observed, with stronger correlations in winter compared to summer. In contrast, when OP assay values were normalised for particle mass, days with higher PM2.5 mass concentrations (µgm-3) were found to have lower mass-normalised OP values as measured by AA and DTT. This finding supports that total PM2.5 mass concentrations alone may not always be the best indicator for particle toxicity. Univariate analysis of OP values and an extensive range of additional measurements, 107 in total, including PM2.5 composition, gas-phase composition and meteorological data, provided detailed insight into the chemical components and atmospheric processes that determine PM2.5 OP variability. Multivariate statistical analyses highlighted associations of OP assay responses with varying chemical components in PM2.5 for both mass- and volume-normalised data. AA and DTT assays were well predicted by a small set of measurements in multiple linear regression (MLR) models and indicated fossil fuel combustion, vehicle emissions and biogenic secondary organic aerosol (SOA) as influential particle sources in the assay response. Mass MLR models of OP associated with compositional source profiles predicted OP almost as well as volume MLR models, illustrating the influence of mass composition on both particle-level OP and total volume OP. Univariate and multivariate analysis showed that different assays cover different chemical spaces, and through comparison of mass- and volume-normalised data we demonstrate that mass-normalised OP provides a more nuanced picture of compositional drivers and sources of OP compared to volume-normalised analysis. This study constitutes one of the most extensive and comprehensive composition datasets currently available and provides a unique opportunity to explore chemical variations in PM2.5 and how they affect both PM2.5 OP and the concentrations of particle-bound reactive oxygen species.

13.
Environ Pollut ; 285: 117338, 2021 Sep 15.
Artigo em Inglês | MEDLINE | ID: mdl-34051562

RESUMO

Packaging is necessary for preserving and delivering products and has significant impacts on human health and the environment. Particle matter (PM) may be released from packages and transferred to the air during a typical peeling process, but little is known about this package-to-air migration route of particles. Here, we investigated the emission profiles of total and biological particles, and the horizontal and vertical dispersion abilities and community structure of viable microbes released from packaging to the air by peeling. The results revealed that a lot of inhalable particles and viable microbes were released from package to the air in different migration directions, and this migration can be regulated by several factors including package material, effective peeling area, peeling speed and angles, as well as the characteristics of the migrant itself. Dispersal of package-borne viable microbes provides direct evidence that viable microbes, including pathogens, can survive the aerosolization caused by peeling and be transferred to air over different distances while remaining alive. Based on the experimental data and visual proof in movies, we speculate that nonbiological particles are package fibers fractured and released to air by the external peeling force exerted on the package and that microbe dispersal is attributed to surface-borne microbe suspension by vibration caused by the peeling force. This investigation provides new information that aerosolized particles can deliver package-borne substances and viable microbes from packaging to the ambient environment, motivating further studies to characterize the health effects of such aerosolized particles and the geographic migration of microbes via packaging.


Assuntos
Poluentes Atmosféricos , Aerossóis/análise , Poluentes Atmosféricos/análise , Monitoramento Ambiental , Humanos , Tamanho da Partícula , Material Particulado/análise , Embalagem de Produtos
14.
Environ Pollut ; 285: 117185, 2021 Sep 15.
Artigo em Inglês | MEDLINE | ID: mdl-33957507

RESUMO

Low-molecular-weight dicarboxylic acids, which are important components of secondary organic aerosols, have been extensively studied in recent years. Many studies have focused on ground-level observations and literature reports on the vertical distribution of the organic aerosols within the urban boundary layer are limited. In this study, the vertical profiles of dicarboxylic acids and related organic compounds (DCRCs) in PM2.5 were investigated at altitudinal levels (ground level and 488 m above the ground level) at the Canton Tower in Guangzhou, southern China, to elucidate their primary sources and secondary formation processes. The concentrations of DCRCs at ground level were generally higher than those at 488 m. Oxalic acid (C2) was the most abundant species, followed by succinic acid (C4) and malonic acid (C3) at both heights. The higher ratio of DCRCs-bound carbon to organic carbon (i.e., DCRCs-C/OC) at 488 m (4.8 ± 1.2%) relative to that at ground level (2.7 ± 0.5%) indicated a higher degree of aerosol aging at 488 m. The abundance of C2 was increased and the conversion of C4 to C3 was enhanced due to the photochemical oxidation of its homologues during long-range transport periods. The increase in C2 was associated with in-cloud processes during pollution periods. Principal component analysis showed that DCRCs were mainly derived from atmospheric secondary processing and biomass burning was also an important source of long-chain carboxylic acids during autumn in Guangzhou. Our results illustrate that secondary processing and biomass burning play prominent roles in controlling the abundance of DCRCs. Furthermore, DCRCs are affected by air masses from regional areas, oxidation of their precursors via vertical transport and in-cloud processes.


Assuntos
Poluentes Atmosféricos , Aerossóis/análise , Poluentes Atmosféricos/análise , China , Ácidos Dicarboxílicos/análise , Monitoramento Ambiental , Cetoácidos , Material Particulado/análise , Estações do Ano
15.
Sci Total Environ ; 789: 147966, 2021 Oct 01.
Artigo em Inglês | MEDLINE | ID: mdl-34058574

RESUMO

Accurate source markers, source profiles and species-based emission factors (EFs) are currently the key limitations for source apportionment and emission inventory researches. Fine particles (PM2.5) were collected from stack gases of eight types of stationary sources with a dilution sampling system. The mass percentages and EFs of 89 kinds of chemical species in PM2.5 including water-soluble ions, elements, carbonaceous species and molecular organic species were obtained. Results showed that water-soluble ions (8%-54%) and elements (5%-45%) were the dominant chemical species. Palmitic acid (0.19%-0.62%) and stearic acid (0.21%-0.59%) were the most abundant organic species. PM2.5 source profiles of the eight sources were different from each other with the coefficient of divergence values all higher than 0.4. The addition of organic species could help to further distinguish them. The indicatory chemical components and specific species ratios were obtained by both a statistical equation and randomForest. These indicatory chemical components (e.g. F- for glass factory) and species ratios (e.g. K+/Mg2+ & OC/Mg for pharmaceutical factory) improved the current knowledges of their indicatory performance in source identification of ambient PM2.5. The EFs of PM2.5 from the eight stationary sources ranged from 0.019 to 51.6 kg t-1 of fuel used. The EFs of PM2.5 from the pharmaceutical factory were about 70-2600 times higher than other seven types of sources due to the lack of dust-removing devices. Certain EFs measured in this study were about 10-36,000 times lower than corresponding EFs estimated in previous studies which didn't perform field measurements, indicating the necessity for improving emission inventories continuously. This study contributes to identifying emission sources of PM2.5 especially for subtypes of stationary sources and to establishing species-based emission inventories.


Assuntos
Poluentes Atmosféricos , Material Particulado , Poluentes Atmosféricos/análise , Poeira/análise , Monitoramento Ambiental , Material Particulado/análise , Centrais Elétricas
17.
Sci Total Environ ; 768: 144198, 2021 May 10.
Artigo em Inglês | MEDLINE | ID: mdl-33736297

RESUMO

In-situ field observations of vertical aerosol profiles for one month in complex terrain (Lushan Mountain, China) were carried out using a cable car, which resolved detailed vertical distributions of mountain aerosols with low-cost operation. Cable-car observations were conducted during the early morning and late afternoon, when mountain and valley winds dominated, respectively. The diurnal aerosol variations at the top and foot of Lushan Mountain were analyzed based on environmental and meteorological stations. The observations indicated that the mountain-valley breezes notably impacted the mountain-area aerosol distribution under weak weather conditions. More uniform aerosol profiles for the afternoon than the morning, with their decreasing rates of PM2.5 (particles with diameters less than 2.5 µm) were 1.64 and 2.28 µg m-3/100 m, respectively. The PM2.5/PM10 ratio at the mountain top increased from 0.69 to 0.81, and that at the mountain base decreased from 0.75 to 0.70 from morning to afternoon. The PM2.5 concentration decreased in and around Lushan Mountain from daytime to nighttime, with the impacted diameter of the 300-m topography line being smaller than ~5 km, while the concentration increased in Jiujiang City. The relative decreasing rate of PM2.5 was higher at the mountain top site (~20%) than at the base site (~2%) from daytime to nighttime. Moreover, uniform aerosol profiles could have been caused by regional transport through a relatively strong low-level synoptic flow (~5 m s-1) and the mountain's dynamic lifting effect.

18.
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.

19.
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
20.
Environ Sci Technol ; 55(8): 5525-5536, 2021 04 20.
Artigo em Inglês | MEDLINE | ID: mdl-33754698

RESUMO

Levoglucosan has been widely used to quantitatively assess biomass burning's contribution to ambient aerosols, but previous such assessments have not accounted for levoglucosan's degradation in the atmosphere. We develop the first global simulation of atmospheric levoglucosan, explicitly accounting for its chemical degradation, to evaluate the impacts on levoglucosan's use in quantitative aerosol source apportionment. Levoglucosan is emitted into the atmosphere from the burning of plant matter in open fires (1.7 Tg yr-1) and as biofuels (2.1 Tg yr-1). Sinks of atmospheric levoglucosan include aqueous-phase oxidation (2.9 Tg yr-1), heterogeneous oxidation (0.16 Tg yr-1), gas-phase oxidation (1.4 × 10-4 Tg yr-1), and dry and wet deposition (0.27 and 0.43 Tg yr -1). The global atmospheric burden of levoglucosan is 19 Gg with a lifetime of 1.8 days. Observations show a sharp decline in levoglucosan's concentrations and its relative abundance to organic carbon aerosol (OC) and particulate K+ from near-source to remote sites. We show that such features can only be reproduced when levoglucosan's chemical degradation is included in the model. Using model results, we develop statistical parametrizations to account for the atmospheric degradation in levoglucosan measurements, improving their use for quantitative aerosol source apportionment.


Assuntos
Poluentes Atmosféricos , Monitoramento Ambiental , Aerossóis/análise , Poluentes Atmosféricos/análise , Atmosfera , Biomassa , Glucose/análogos & derivados , Glucose/análise , Material Particulado/análise , Estações do Ano
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