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1.
Huan Jing Ke Xue ; 45(5): 2581-2595, 2024 May 08.
Artículo en Chino | MEDLINE | ID: mdl-38629523

RESUMEN

Inorganic aerosol is the main component of haze days in winter over Tianjin. In this study, two typical high concentrations of secondary inorganic aerosol (SIA) processes, defined as CASE1 and CASE2, were selected during polluted days in January 2020 over Tianjin, and the effects of meteorological factors, regional transport, and chemical processes were comprehensively investigated combined with observations and numerical models (WRF-NAQPMS). The average SIA concentrations in CASE1 and CASE2 were 76.8 µg·m-3 and 66.0 µg·m-3, respectively, and the nitrate concentration was higher than that of sulfate and ammonium, which were typical nitrate-dominated pollution processes. Meteorological conditions played a role in inorganic aerosol formation. The temperature of approximately -6-0℃ and 2-4℃ and the relative humidity of 50%-60% and 80%-100% would be suitable conditions for the high SIA concentration (>80 µg·m-3) in CASE1, whereas the temperature of approximately 2-4℃ and the relative humidity of 60%-70% would be suitable in CASE2. The average contribution rates of external sources to SIA in the CASE1 and CASE2 processes were 62.3% and 22.1%, which were regional transport-dominant processes and local emission-dominant processes, respectively. The contribution of the local emission of CASE1 to nitrate and sulfate was 16.2 µg·m-3 and 8.2 µg·m-3, respectively, higher than that of external sources (31.7 µg·m-3 and 8.8 µg·m-3). the local contribution of CASE2 to nitrate and sulfate was 29.3 µg·m-3 and 25.1 µg·m-3, respectively, whereas the contribution from external sources was 8.1 µg·m-3 and 9.4 µg·m-3, respectively. The quantitative result indicated that local formation and regional transport resulted in higher nitrate concentration than sulfate in CASE1, in contrast to only local sources in CASE2. The gas phase reaction was the main source of inorganic aerosol formation, contributing 48.9% and 57.8% in CASE1 and CASE2, respectively, whereas the heterogeneous reactions were also important processes, with contribution rates of 48.1% and 42.2% to SIA. The effect of aqueous phase reaction was negligible.

2.
Sci Total Environ ; 928: 172345, 2024 Jun 10.
Artículo en Inglés | MEDLINE | ID: mdl-38621537

RESUMEN

Fine particulate matter (PM2.5) causes millions of premature deaths each year worldwide. Oxidative potential (OP) has been proposed as a better metric for aerosol health effects than PM2.5 mass concentration alone. In this study, we report for the first time online measurements of PM2.5 OP in wintertime Beijing and surroundings based on a dithiothreitol (DTT) assay. These measurements were combined with co-located PM chemical composition measurements to identify the main source categories of aerosol OP. In addition, we highlight the influence of two distinct pollution events on aerosol OP (spring festival celebrations including fireworks and a severe regional dust storm). Source apportionment coupled with multilinear regression revealed that primary PM and oxygenated organic aerosol (OOA) were both important sources of OP, accounting for 41 ± 12 % and 39 ± 10 % of the OPvDTT (OP normalized by the sampled air volume), respectively. The small remainder was attributed to fireworks and dust, mainly resulting from the two distinct pollution events. During the 3.5-day spring festival period, OPvDTT spiked to 4.9 nmol min-1 m-3 with slightly more contribution from OOA (42 ± 11 %) and less from primary PM (31 ± 15 %). During the dust storm, hourly-averaged PM2.5 peaked at a very high value of 548 µg m-3 due to the dominant presence of dust-laden particles (88 % of total PM2.5). In contrast, only mildly elevated OPvDTT values (up to 1.5 nmol min-1 m-3) were observed during this dust event. This observation indicates that variations in OPvDTT cannot be fully explained using PM2.5 alone; one must also consider the chemical composition of PM2.5 when studying aerosol health effects. Our study highlights the need for continued pollution control strategies to reduce primary PM emissions, and more in-depth investigations into the source origins of OOA, to minimize the health risks associated with PM exposure in Beijing.

3.
Sci Total Environ ; 926: 171989, 2024 May 20.
Artículo en Inglés | MEDLINE | ID: mdl-38547971

RESUMEN

To understand the characteristics of atmospheric pollution above the urban canopy in warm seasons, the characteristics of sub-micron aerosol (PM1) was studied based on high-altitude observations at the Beijing 325 m meteorological tower. The PM1 at 260 m was 34, 29 and 21 µg m-3 in May 2015, June 2015, and June 2017, respectively, indicating a reduction in PM1 pollution above the urban canopy. Meanwhile, an overall decrease was also observed in the concentrations of all PM1 chemical species (excluding Chl and BC) and organic aerosol (OA) factors. Previous instances of heavy haze in Beijing often coincided with high humidity and stagnant weather conditions. However, the heightened pollution episodes in June 2017 were accompanied by high wind speeds and low relative humidity. Compared to May 2015, the contribution of secondary components to PM1 in June 2017 was more prominent, with the total proportion of SNA (sulfate, nitrate, and ammonium) and more-oxidized oxygenated OA (MO-OOA) to PM1 increased by approximately 10 %. Secondary species of NH4NO3, (NH4)2SO4, and MO-OOA, as well as black carbon, collectively contributed the vast majority of aerosol extinction coefficient (bext), with the four species contributing a total of ≥96 % to bext at 260 m. Hydrocarbon-like OA, cooking OA, and less-oxidized oxygenated OA have undergone significant reductions, so continued emphasis on controlling local sources to reduce these three aerosol species and addressing regional sources to further mitigate overall aerosol species is imperative. In lower pollution situation, the diurnal variation of PM was smoother, and its pollution sources were more regionally uniform, which might be attributed to the reduced diversity and complexity in the physical and chemical processes in air pollution.

4.
Sci Total Environ ; 919: 170633, 2024 Apr 01.
Artículo en Inglés | MEDLINE | ID: mdl-38340865

RESUMEN

Biogenic and anthropogenic organic vapors are crucial precursors of ozone and secondary organic aerosol (SOA) in the atmosphere. Here we conducted real-time measurements of gaseous organic compounds using a Vocus proton-transfer-reaction mass spectrometer (Vocus PTR-MS) at the Shanghuang mountain site (1128 m a.s.l.) in southeastern China during November 2022. Our results revealed a substantial impact of mixed biogenic and anthropogenic compounds at the mountain site, with oxygenated volatile organic compounds (OVOCs) comprising 74 % of the organic vapors. Two distinct periods, characterized by sunny days (P1) and persistent cloud events (P2), were observed. P1 exhibited higher concentrations of biogenic-related emissions compared to P2. For instance, isoprene, monoterpenes, and sesquiterpenes during P1 were 2.4-2.9 times higher than those during P2. OVOCs such as acetaldehyde, MVK + MACR, acetone, and MEK also showed higher concentrations during P1, indicating a dominant source from the photochemical oxidation of biogenic VOCs. Anthropogenic-related VOCs like benzene and toluene had higher concentrations during P2, displaying different diurnal cycles compared to P1. Our analysis identified four biogenic-related factors dominated by isoprene and sesquiterpene oxidation products, and two anthropogenic-related factors. During P1, biogenic sources contributed approximately 80 % to total organic compounds, while during P2, anthropogenic sources, particularly the aromatic-related factor, increased from 16 % to 35 %. Furthermore, a unique factor characterized by C2 amines and C3 amides and periodic plumes indicated the influence of industrial emissions from regional transport. The study highlights the significant variations in sources and compositions of gaseous organic compounds at regional mountain sites due to changes in meteorology and photochemical processing, potentially impacting regional ozone and SOA formation.

5.
Sci Bull (Beijing) ; 69(7): 978-987, 2024 Apr 15.
Artículo en Inglés | MEDLINE | ID: mdl-38242834

RESUMEN

Aerosol ammonium (NH4+), mainly produced from the reactions of ammonia (NH3) with acids in the atmosphere, has significant impacts on air pollution, radiative forcing, and human health. Understanding the source and formation mechanism of NH4+ can provide scientific insights into air quality improvements. However, the sources of NH3 in urban areas are not well understood, and few studies focus on NH3/NH4+ at different heights within the atmospheric boundary layer, which hinders a comprehensive understanding of aerosol NH4+. In this study, we perform both field observation and modeling studies (the Community Multiscale Air Quality, CMAQ) to investigate regional NH3 emission sources and vertically resolved NH4+ formation mechanisms during the winter in Beijing. Both stable nitrogen isotope analyses and CMAQ model suggest that combustion-related NH3 emissions, including fossil fuel sources, NH3 slip, and biomass burning, are important sources of aerosol NH4+ with more than 60% contribution occurring on heavily polluted days. In contrast, volatilization-related NH3 sources (livestock breeding, N-fertilizer application, and human waste) are dominant on clean days. Combustion-related NH3 is mostly local from Beijing, and biomass burning is likely an important NH3 source (∼15%-20%) that was previously overlooked. More effective control strategies such as the two-product (e.g., reducing both SO2 and NH3) control policy should be considered to improve air quality.

6.
Sci Total Environ ; 917: 170485, 2024 Mar 20.
Artículo en Inglés | MEDLINE | ID: mdl-38296080

RESUMEN

Understanding aerosol vertical distribution is of great importance to climate change and atmospheric chemistry, but there is a dearth of systematical analysis for aerosol vertical distribution amid rapid emission decline after 2013 in China. Here, the GEOS-Chem model and multiple-sourced observations were applied to quantify the changes of aerosol vertical distributions in response to clean air actions. In 2013-2020, the MODIS aerosol optical depth (AOD) presented extensive decreasing trends by -7.9 %/yr to -4.2 %/yr in summer and -6.1 %/yr to -5.8 %/yr in winter in polluted regions. Vertically, the aerosol extinction coefficient (AEC) from CALIPSO decreased by -8.0 %/yr to -5.5 %/yr below ~1 km, but the trends weakened significantly with increasing altitude. Compared with available measurements, the model can reasonably reproduce 2013-2020 trends and seasonality in AOD and vertical AEC. Model simulations confirm that emission reduction was the dominant driver of the 2013-2020 decline in AOD, while the effect of meteorology varied seasonally, with contributions ranging from -2 % to 13 % in summer and -67 % to -2 % in winter. Vertical distributions of emission-driven AEC trends strongly depended on emission reductions, local planetary boundary layer height, and relative humidity. For aerosol components, sulfate accounted for ~50 % of the AOD decline during summer, followed by ammonium and organic aerosol, while in winter the contribution of organic aerosol doubled (24 %-35 %), and nitrate exhibited a weak increasing trend. Chemical production and meteorological conditions (e.g., relative humidity) primarily drove the nitrate contribution, but emission reduction and hygroscopicity were decisive for other components. This work provides an integrated observational and modeling effort to better understand rapid changes in aerosol vertical distribution over China.

7.
J Hazard Mater ; 465: 133094, 2024 Mar 05.
Artículo en Inglés | MEDLINE | ID: mdl-38029589

RESUMEN

Prevalence of subclinical hypothyroidism substantially increased during the last decade in China, which has been commonly/clinically diagnosed as elevation in thyrotropin (thyroid-stimulating hormone [TSH]). Tobacco smoke containing toxic substances has been linked to thyroid dysfunction; however, data on perturbation of TSH following air pollution exposure in human has not been assessed at nationwide population level. We investigated the longitudinal impact of daily ambient air pollution estimated at residential level on serum TSH in 1.38 million women from China's 29 mainland provinces between 2014 and 2019. We observed that particulate matter with aerodynamic diameter ≤ 10 and ≤ 2.5 µm (PM10, PM2.5) and nitrogen dioxide (NO2) at cumulative lag 0-7 days of exposure were associated with percent elevations in TSH (0.88% [95% CI: 0.71, 1.05] per [interquartile range, IQR: 54.8 µg/m3] of PM10; 0.89% [95% CI, 0.71, 1.07] per IQR [40.3 µg/m3] of PM2.5; 2.01% [95% CI: 1.81, 2.22] per IQR [27.4 µg/m3] of NO2). Greater associations were observed in participants living in areas with ≥adequate iodine intake and those with low BMI levels and high inflammation status. Our results suggest that increased concentrations of recent ambient air pollutants at exposure ranges commonly encountered in Asia were associated with increases in TSH, supporting disturbing role of short-term air pollution exposure on the regulation of thyroid hormone homeostasis.


Asunto(s)
Contaminantes Atmosféricos , Contaminación del Aire , Humanos , Femenino , Dióxido de Nitrógeno/toxicidad , Exposición a Riesgos Ambientales/análisis , Contaminación del Aire/análisis , Contaminantes Atmosféricos/análisis , Material Particulado/toxicidad , China/epidemiología , Tirotropina
8.
J Environ Sci (China) ; 138: 516-530, 2024 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-38135417

RESUMEN

On-line chemical characterization of atmospheric particulate matter (PM) with soft ionization technique and ultrahigh-resolution Mass Spectrometry (UHRMS) provides molecular information of organic constituents in real time. Here we describe the development and application of an automatic measurement system that incorporates PM2.5 sampling, thermal desorption, atmospheric pressure photoionization, and UHRMS analysis. Molecular formulas of detected organic compounds were deducted from the accurate (±10 ppm) molecular weights obtained at a mass resolution of 100,000, allowing the identification of small organic compounds in PM2.5. Detection efficiencies of 28 standard compounds were determined and we found a high sensitivity and selectivity towards organic amines with limits of detection below 10 pg. As a proof of principle, PM2.5 samples collected off-line in winter in the urban area of Beijing were analyzed using the Ionization Module and HRMS of the system. The automatic system was then applied to conduct on-line measurements during the summer time at a time resolution of 2 hr. The detected organic compounds comprised mainly CHON and CHN compounds below 350 m/z. Pronounced seasonal variations in elemental composition were observed with shorter carbon backbones and higher O/C ratios in summer than that in winter. This result is consistent with stronger photochemical reactions and thus a higher oxidation state of organics in summer. Diurnal variation in signal intensity of each formula provides crucial information to reveal its source and formation pathway. In summary, the automatic measurement system serves as an important tool for the on-line characterization and identification of organic species in PM2.5.


Asunto(s)
Contaminantes Atmosféricos , Material Particulado , Material Particulado/análisis , Contaminantes Atmosféricos/análisis , Espectrometría de Masas , Presión Atmosférica , Aerosoles/análisis , Aminas , Monitoreo del Ambiente/métodos
9.
J Environ Sci (China) ; 138: 585-596, 2024 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-38135422

RESUMEN

We developed a single-particle optical particle counter with polarization detection (SOPC) for the real-time measurement of the optical size and depolarization ratio (defined as the ratio of the vertical component to the parallel component of backward scattering) of atmospheric particles, the polarization ratio (DR) value can reflect the irregularity of the particles. The SOPC can detect aerosol particles with size larger than 500 nm and the maximum particle count rate reaches ∼1.8 × 105 particles per liter. The SOPC uses a modulated polarization laser to measure the optical size of particles according to forward scattering signal and the DR value of the particles by backward S and P signal components. The sampling rate of the SOPC was 106 #/(sec·channel), and all the raw data were processed online. The calibration curve was obtained by polystyrene latex spheres with sizes of 0.5-10 µm, and the average relative deviation of measurement was 3.96% for sub 3 µm particles. T-matrix method calculations showed that the DR value of backscatter light at 120° could describe the variations in the aspect ratio of particles in the above size range. We performed insitu observations for the evaluation of the SOPC, the mass concentration constructed by the SOPC showed good agreement with the PM2.5 measurements in a nearby state-controlled monitoring site. This instrument could provide useful data for source appointment and regulations against air pollution.


Asunto(s)
Contaminación del Aire , Monitoreo del Ambiente , Monitoreo del Ambiente/métodos , Tamaño de la Partícula , Luz , Microesferas
10.
Environ Sci Technol ; 57(42): 15945-15955, 2023 10 24.
Artículo en Inglés | MEDLINE | ID: mdl-37823561

RESUMEN

Air quality in China has continuously improved during the Three-Year Action Plan (2018-2020); however, the changes in aerosol composition, properties, and sources in Beijing summer remain poorly understood. Here, we conducted real-time measurements of aerosol composition in five summers from 2018 to 2022 along with WRF-Community Multiscale Air Quality simulations to characterize the changes in aerosol chemistry and the roles of meteorology and emission reductions. Largely different from winter, secondary inorganic aerosol and photochemical-related secondary organic aerosol (SOA) showed significant decreases by 55-67% in summer, and the most decreases occurred in 2021. Comparatively, the decreases in the primary aerosol species and gaseous precursors were comparably small. While decreased atmospheric oxidation capacity as indicated by ozone changes played an important role in changing SOA composition, the large decrease in aerosol liquid water and small increase in particle acidity were critical for nitrate changes by decreasing gas-particle partitioning substantially (∼28%). Analysis of meteorological influences demonstrated clear and similar transitions in aerosol composition and formation mechanisms at a relative humidity of 50-60% in five summers. Model simulations revealed that emission controls played the decisive role in reducing sulfate, primary OA, and anthropogenic SOA during the Three-Year Action Plan, while meteorology affected more nitrate and biogenic SOA.


Asunto(s)
Contaminantes Atmosféricos , Beijing , Contaminantes Atmosféricos/análisis , Material Particulado/análisis , Nitratos , Monitoreo del Ambiente , Aerosoles/análisis
11.
J Environ Sci (China) ; 132: 31-42, 2023 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-37336608

RESUMEN

Black carbon (BC) aerosols in the atmosphere play a significant role in climate systems due to their strong ability to absorb solar radiation. The lifetime of BC depends on atmospheric transport, aging and consequently on wet scavenging processes (in-cloud and below-cloud scavenging). In this study, sequential rainwater samples in eight rainfall events collected in 2 mm interval were measured by a tandem system including a single particle soot photometer (SP2) and a nebulizer. The results showed that the volume-weighted average (VWA) mass concentrations of refractory black carbon (rBC) in each rainfall event varied, ranging from 10.8 to 78.9 µg/L. The highest rBC concentrations in the rainwater samples typically occurred in the first fraction from individual rainfall events. The geometric mean median mass-equivalent diameter (MMD) decreased under precipitation, indicating that rBC with larger sizes was relatively aged and preferentially removed by wet scavenging. A positive correlation (R2 = 0.73) between the VWA mass concentrations of rBC in rainwater and that in ambient air suggested the important contribution of scavenging process. Additionally, the contributions of in-cloud and below-cloud scavenging were distinguished and accounted for 74% and 26% to wet scavenging, respectively. The scavenging ratio of rBC particles was estimated to be 0.06 on average. This study provides helpful information for better understanding the mechanism of rBC wet scavenging and reducing the uncertainty of numerical simulations of the climate effects of rBC.


Asunto(s)
Contaminantes Atmosféricos , Contaminantes Atmosféricos/análisis , Beijing , Hollín/análisis , Aerosoles/análisis , Carbono , Monitoreo del Ambiente/métodos
12.
Adv Atmos Sci ; : 1-23, 2023 Apr 28.
Artículo en Inglés | MEDLINE | ID: mdl-37359906

RESUMEN

Atmospheric chemistry research has been growing rapidly in China in the last 25 years since the concept of the "air pollution complex" was first proposed by Professor Xiaoyan TANG in 1997. For papers published in 2021 on air pollution (only papers included in the Web of Science Core Collection database were considered), more than 24 000 papers were authored or co-authored by scientists working in China. In this paper, we review a limited number of representative and significant studies on atmospheric chemistry in China in the last few years, including studies on (1) sources and emission inventories, (2) atmospheric chemical processes, (3) interactions of air pollution with meteorology, weather and climate, (4) interactions between the biosphere and atmosphere, and (5) data assimilation. The intention was not to provide a complete review of all progress made in the last few years, but rather to serve as a starting point for learning more about atmospheric chemistry research in China. The advances reviewed in this paper have enabled a theoretical framework for the air pollution complex to be established, provided robust scientific support to highly successful air pollution control policies in China, and created great opportunities in education, training, and career development for many graduate students and young scientists. This paper further highlights that developing and low-income countries that are heavily affected by air pollution can benefit from these research advances, whilst at the same time acknowledging that many challenges and opportunities still remain in atmospheric chemistry research in China, to hopefully be addressed over the next few decades.

13.
Proc Natl Acad Sci U S A ; 120(26): e2218274120, 2023 Jun 27.
Artículo en Inglés | MEDLINE | ID: mdl-37339212

RESUMEN

Heat waves and air pollution extremes exert compounding effects on human health and food security and may worsen under future climate change. On the basis of reconstructed daily O3 levels in China and meteorological reanalysis, we found that the interannual variability of the frequency of summertime co-occurrence of heat wave and O3 pollution in China is regulated mainly by a combination of springtime warming in the western Pacific Ocean, western Indian Ocean, and Ross Sea. These sea surface temperature anomalies impose influences on precipitation, radiation, etc., to modulate the co-occurrence, which were also confirmed with coupled chemistry-climate numerical experiments. We thus built a multivariable regression model to predict co-occurrence a season in advance, and correlation coefficient could reach 0.81 (P < 0.01) for the North China Plain. Our results provide useful information for the government to take actions in advance to mitigate damage from these synergistic costressors.

14.
Environ Pollut ; 327: 121569, 2023 Jun 15.
Artículo en Inglés | MEDLINE | ID: mdl-37028792

RESUMEN

To understand the source, formation, and seasonality of biogenic secondary organic aerosol (BSOA), a nine-stage cascade impactor was utilized to collect size-segregated particulate samples from April 2017 to January 2018 in Beijing, China. BSOA tracers derived from isoprene, monoterpene, and sesquiterpene were measured with gas chromatography-mass spectrometry. Isoprene and monoterpene SOA tracers exhibited significant seasonal variations, with a summer maximum and a winter minimum. Dominance of 2-methyltetrols (isoprene SOA tracers) with a good correlation with levoglucosan (a biomass burning tracer), which was combined with the detection of methyltartaric acids (possible indicators for aged isoprene) in summer, implies possible biomass burning and long-range transport. In contrast, sesquiterpene SOA tracer (ß-caryophyllinic acid) was dominant in winter and was probably associated with the local burning of biomass. Bimodal size distributions were observed for most isoprene SOA tracers, consistent with previous laboratory experiments and field studies showing that they can be formed not only in the aerosol phase but also in the gas phase. Monoterpene SOA tracers cis-pinonic acid and pinic acid showed a coarse-mode peak (5.8-9.0 µm) in four seasons due to their volatile nature. Sesquiterpene SOA tracer ß-caryophyllinic acid showed a unimodal pattern with a major fine-mode peak (1.1-2.1 µm), which is linked to local biomass burning. The tracer-yield method was used to quantify the contributions of isoprene, monoterpene, and sesquiterpene to secondary organic carbon (SOC) and SOA. The highest isoprene SOC and SOA concentrations occurred in summer (2.00 µgC m-3 and 4.93 µg m-3, respectively), contributing to 1.61% of OC and 5.22% of PM2.5, respectively. These results suggest that BSOA tracers are promising tracers for understanding the source, formation, and seasonality of BSOA.


Asunto(s)
Contaminantes Atmosféricos , Sesquiterpenos , Contaminantes Atmosféricos/análisis , Beijing , Monoterpenos/análisis , Sesquiterpenos/análisis , Aerosoles/análisis , Estaciones del Año , Material Particulado/análisis , Monitoreo del Ambiente/métodos
15.
Environ Pollut ; 325: 121440, 2023 May 15.
Artículo en Inglés | MEDLINE | ID: mdl-36921656

RESUMEN

The interaction of aerosols and the planetary boundary layer (PBL) plays an important role in deteriorating urban air quality. Aerosols from different sources may have different effects on regulating PBL structures owing to their distinctive dominant compositions and vertical distributions. To characterize the complex feedback of aerosols on PBL over the Beijing megacity, multiple approaches, including in situ observations in the autumn and winter of 2016-2019, backward trajectory clusters, and large-eddy simulations, were adopted. The results revealed notable distinctions in aerosol properties, vertical distributions and thermal stratifications among three types of air masses from the West Siberian Plain (Type-1), Central Siberian Plateau (Type-2) and Mongolian Plateau (Type-3). Low loadings of 0.28 ± 0.26 and 0.15 ± 0.08 of aerosol optical depth (AOD) appeared in the Type-1 and Type-2, accompanied by cool and less stable stratification, with a large part (80%) of aerosols concentrated below 1500 m. For Type-3, the AOD and single scattering albedo (SSA) were as high as 0.75 ± 0.54 and 0.91 ± 0.05, demonstrating severe pollution levels of abundant scattering aerosols. Eighty percent of the aerosols were constrained within a lower height of 1150 m owing to the warmer and more stable environment. Large-eddy simulations revealed that aerosols consistently suppressed the daytime convective boundary layer regardless of their origins, with the PBL height (PBLH) decreasing from 1120 m (Type-1), 1160 m (Type-2) and 820 m (Type-3) in the ideal clean scenarios to 980 m, 1100 m and 600 m, respectively, under polluted conditions. Therefore, the promotion of absorbing aerosols below the residual layer on PBL could be greatly hindered by the suppression effects generated by both absorbing aerosols in the upper temperature inversion layer and scattering aerosols. Moreover, the results indicated the possible complexities of aerosol-PBL interactions under future emission-reduction scenarios and in other urban regions.


Asunto(s)
Contaminantes Atmosféricos , Beijing , Contaminantes Atmosféricos/análisis , Retroalimentación , Monitoreo del Ambiente/métodos , China , Aerosoles/análisis
16.
Environ Pollut ; 319: 121016, 2023 Feb 15.
Artículo en Inglés | MEDLINE | ID: mdl-36610651

RESUMEN

The land-sea breeze circulation significantly impacts the atmospheric transport of organic aerosols in coastal regions. However, the links between organic aerosols and land-sea breezes remain poorly understood. In this study, organic marker compounds for biomass burning, primary biological aerosols, biogenic and anthropogenic secondary organic aerosols (SOA) in fine particles from a coastal city in East China were analysed using gas chromatography-mass spectrometry. Land-sea breeze circulations were identified to explore their potential influence on organic molecular compositions. Organic marker compounds showed obvious diurnal/seasonal patterns. Surprisingly, due to the combined influence of weakened East Asian monsoons and land-sea breezes, all detected organic markers decreased except α/ß-pinene SOA markers during land-sea breeze periods in early autumn; whereas, all the organic markers increased except α/ß-pinene SOA markers, pollen and plant debris markers during land-sea breeze periods in early spring. Furthermore, the reaction pathway and aging of biogenic SOA were also related to land-sea breezes. During the land-sea breeze periods, the ratios of 2-methylglyceric acid (2-MGA) to 2-methyltetrols increased in early autumn, indicating that more isoprene-derived SOA generated from the high-NOx (nitrogen oxides) pathway when the land-sea breezes occurred; while the ratios decreased in early spring, this may be related to the chemical transformation of 2-MGA to 2-MGA sulfates. Changes in the ratio of monoterpene SOA markers demonstrate that monoterpene SOA was relatively aged during sea breeze periods, while it was fresher when the land breeze occurred. Although boundary layer height, emissions, gas/particle partitioning, etc. are important reasons for the diurnal variations of organic aerosols, night/day ratios of molecular markers increased obviously when land-sea breezes occurred in both early autumn and early spring. Our results provide new insights into the shift in the chemical composition of organic aerosols over coastal areas that are influenced by land-sea breezes.


Asunto(s)
Contaminantes Atmosféricos , Compuestos Orgánicos , Monoterpenos Bicíclicos/análisis , Compuestos Orgánicos/análisis , Aerosoles/análisis , China , Contaminantes Atmosféricos/análisis
17.
J Environ Sci (China) ; 123: 292-305, 2023 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-36521991

RESUMEN

Observations and numerical models are mainly used to investigate the spatiotemporal distribution and vertical structure characteristics of aerosols to understand aerosol pollution and its effects. However, the limitations of observations and the uncertainties of numerical models bias aerosol calculations and predictions. Data assimilation combines observations and numerical models to improve the accuracy of the initial, analytical fields of models and promote the development of atmospheric aerosol pollution research. Numerous studies have been conducted to integrate multi-source data, such as aerosol optical depth and aerosol extinction coefficient profile, into various chemical transport models using various data assimilation algorithms and have achieved good assimilation results. The definition of data assimilation and the main algorithms will be briefly presented, and the progress of aerosol assimilation according to two types of aerosol data, namely, aerosol optical depth and extinction coefficient, will be presented. The application of vertical aerosol data assimilation, as well as the future trends and challenges of aerosol data assimilation, will be further analysed.


Asunto(s)
Contaminantes Atmosféricos , Contaminantes Atmosféricos/análisis , Monitoreo del Ambiente/métodos , Aerosoles/análisis , Modelos Químicos , Tecnología
18.
J Environ Sci (China) ; 125: 499-512, 2023 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-36375933

RESUMEN

Understanding the aerosol vertical characterization is of great importance to both climate and atmospheric environment. This study investigated the variations of aerosol profiles over eight regions of interest in China after clean air policy (2013-2019) and discussed the drivers of the vertical aerosol structure, using observations from active satellite measurements (CALIPSO). From the annual variation, the amplitude of extinction coefficient profiles showed a decreasing trend with fluctuations, and the maximum was 0.21 km-1 in Beijing-Tianjin-Hebei (JJJ). For regions suffered from air pollution, the variation was greatest below 0.45 km, while it was between 1-1.5 km for Sichuan Basin. The correlation coefficient between the relative humidity (RH) and the extinction coefficient indicated that the increase of RH inhibited the decrease of the extinction coefficient in the Yangtze River Delta. In most regions, the main aerosol subtypes were polluted dust and polluted continental, but they were coarser in JJJ and North West. The frequency of concurrency of dust and polluted dust aerosols decreased in JJJ, but polluted continental aerosols occurred more frequently. Further, the aerosol extinction coefficient profiles under different pollution conditions showed that it changed most during heavy pollution periods in JJJ, especially in 2017, with a significant aerosol loading between ∼700 and 1200 m. The atmospheric reanalysis data revealed that the weak convergence at low level and the divergence at high level supported the upward transport of aerosols in 2017. Overall, the differences in divergence allocation, RH, and wind filed were the main meteorological drivers.


Asunto(s)
Contaminantes Atmosféricos , Contaminación del Aire , Contaminantes Atmosféricos/análisis , Material Particulado/análisis , Monitoreo del Ambiente , Estaciones del Año , Aerosoles/análisis , Contaminación del Aire/análisis , Polvo/análisis , China , Políticas
19.
Sci Total Environ ; 854: 158874, 2023 Jan 01.
Artículo en Inglés | MEDLINE | ID: mdl-36126710

RESUMEN

Aerosol volatility has a substantial impact on gas-particle partitioning, aging process and hence brown carbon (BrC) absorption. Here we analyzed single-particle volatility in winter in Beijing using a thermodenuder coupled with a single particle aerosol mass spectrometer along with a suite of collocated measurements. Our results showed that elemental carbon, metals, organic nitrogen (ON) were the dominant low-volatility components. The ON-containing particles accounting for 50 % of the total low-volatility particles comprised mainly ON-organic carbon (ON-OC) particles which were associated with biomass burning and significantly enhanced during polluted periods with high relative humidity and nitrogen oxides (NOx) levels. By analyzing the relationship between single-particle volatility and BrC, we found that semi-volatile particles related to fossil fuel combustion contributed dominantly to the light absorption of BrC (~50 %). Comparatively, the low-volatility and semi-volatile particles related to biomass burning contributed 21-35 % and 10-15 %, respectively to the BrC light absorption. Our results demonstrated that single particles from different sources with different volatility showed different impacts on BrC absorption. Although low-volatility organic aerosol accounted only for ~16 % of the total ambient organics, they can contribute as much as ~30-40 % to BrC light absorption in winter in Beijing.

20.
Materials (Basel) ; 15(23)2022 Nov 22.
Artículo en Inglés | MEDLINE | ID: mdl-36499778

RESUMEN

Earthen sites are easily eroded by the natural environment, resulting in a large number of micro cracks on the surface. In order to explore the internal relationship between environmental factors and the cracking law of soil sites, this paper carries out dry shrinkage tests of different soil layers at the Zhouqiao site, reconstructs the study on cracking law of earthen soil under dry shrinkage-conditioned microstructure of site soil at different depths based on electron microscope pictures and finite element method, and explores the influence of different moisture content on the cracking of soil samples at the site. The results show that under conditions of dry shrinkage, the thickness of the soil layer has the greatest influence on the cracking of site soil samples. Due to the internal water loss and shrinkage of the soil sample, the thinner the soil layer, the more often the soil layer cracks first. The crack rate of the soil sample with a thickness of 1 cm is nearly three times higher than that of the soil sample with a thickness of 5 cm. Through numerical simulation analysis, it is found that the evolution process of soil fractures at the Zhouqiao site is mainly divided into the formation stages of initial stress field, single main fracture, secondary fracture and fracture network. The formation time of the secondary fracture is longer than that of the initial stress field and single main fracture, and the cracking of the upper soil sample is more serious than that of the lower soil sample. Under conditions of dry shrinkage, the particle arrangement of the soil sample is relatively loose, and there are many cracks inside, which provides evaporation and infiltration channels for water, forming unrecoverable weak pores, and finally, the cracks start to sprout at the weak points. The research results provide some reference for the disease mechanism and safety analysis of earthen sites.

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