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1.
Environ Pollut ; 356: 124355, 2024 Jun 11.
Article in English | MEDLINE | ID: mdl-38871170

ABSTRACT

Due to the significance of atmospheric HONO as a reservoir for radicals and the presence of substantial unknown sources of HONO, there is a pressing need for accurate and consistent measurement of its concentration. In this study, we compared the measurements obtained from the monitor for aerosols and gases in ambient air (MARGA) based on wet chemical method with those from the incoherent broadband cavity-enhanced absorption spectroscopy (IBBCEAS) based on optical method to assess the suitability of the MARGA instrument for accurate HONO detection. The diurnal patterns obtained by the two instruments are similar, with peaks at 8 a.m. and lows at 5 p.m. Over the course of the observation period, it was often observed that HONO concentrations recorded by the MARGA instrument consistently exceeded those obtained through the IBBCEAS technique, accounting for approximately 91.33% of the total observation time. Throughout the entire observation period, the R2 value between the two instruments was 0.49, indicating relatively good correlation. However, with a slope of only 0.27, it suggests poor agreement between the two instruments. Furthermore, the R2 and slopes between the two instruments vary with the seasons and day-night. The larger the quartile values of NO2, NH3, and BC, the greater the slopes of both MARGA and IBBCEAS instruments, and the higher the concentrations of NO2, NH3, and BC (indicator of semivolatile oxidizable hydrocarbons), the greater the differences between the two instruments, all indicating that NH3 may promote the reaction of NO2 with semivolatile oxidizable hydrocarbons to produce HONO. The O3 with its strong oxidizing properties may cause underestimation in the MARGA instrument by oxidizing NO2- to NO3- in the absorbing solution. It is challenging to derive a universal correction formula due to the interference of various chemical substances. Hence, MARGA should not be used for HONO research in the future.

2.
Anal Chem ; 96(5): 1834-1842, 2024 Feb 06.
Article in English | MEDLINE | ID: mdl-38266381

ABSTRACT

Light-absorbing organic aerosols, referred to as brown carbon (BrC), play a vital role in the global climate and air quality. Due to the complexity of BrC chromophores, the identified absorbing substances in the ambient atmosphere are very limited. However, without comprehensive knowledge of the complex absorbing compounds in BrC, our understanding of its sources, formation, and evolution mechanisms remains superficial, leading to great uncertainty in climatic and atmospheric models. To address this gap, we developed a constrained non-negative matrix factorization (NMF) model to resolve the individual ultraviolet-visible spectrum for each substance in dissolved organic aerosols, with the power of ultrahigh-performance liquid chromatography-diode array detector-ultrahigh-resolution mass spectrometry (UHPLC-DAD-UHRMS). The resolved spectra were validated by selected standard substances and validation samples. Approximately 40,000 light-absorbing substances were recognized at the MS1 level. It turns out that BrC is composed of a vast number of substances rather than a few prominent chromophores in the urban atmosphere. Previous understanding of the absorbing feature of BrC based on a few identified compounds could be biased. Weak-absorbing substances missed previously play an important role in BrC absorption when they are integrated due to their overwhelming number. This model brings the property exploration of complex dissolved organic mixtures to a molecular level, laying a foundation for identifying potentially significant compositions and obtaining a comprehensive chemical picture.

3.
Sci Total Environ ; 914: 170035, 2024 Mar 01.
Article in English | MEDLINE | ID: mdl-38218482

ABSTRACT

Surface ozone pollution under climate warming has become a serious environmental issue. In the summer of 2022, abnormal warming spread over most of the Northern Hemisphere and resulted in the abnormal increase in O3 concentrations. In this study, we focused on the coastal cities in China and investigated the O3 trends in July during 2015 to 2022. Four regions with different locations and emission levels were selected for comparison. A significant increase of O3 concentration in July 2022 were observed in the southern coastal cities (16.7-22.8 µg m-3) while the opposite characteristics were found in the northern coastal cities (decrease of 0.26-2.18 µg m-3). The results indicated various distribution patterns of the O3 concentrations responded to heat wave across China. The weakening of East Asian summer monsoon, extension of the western Pacific subtropical high, significant warming, stronger solar radiation, lower relative humidity, less rainfall and sinking motion of atmosphere in 2022 were beneficial for O3 generation and accumulation in the southern coastal areas. Meteorological changes in July 2022 could lead to an increase of 15.6 % in O3 concentrations in southern coastal cities compared to that in 2015-2021, based on the analysis of machine learning. Air temperature was the main contributor to high O3 concentrations in the coast of Fujian province, while other coastal cities depended on relative humidity. This study indicated the challenge of O3 pollution control in coastal areas under global warming, especially in extreme heat wave events.

4.
Environ Sci Technol ; 58(2): 1187-1198, 2024 Jan 16.
Article in English | MEDLINE | ID: mdl-38117945

ABSTRACT

Atmospheric particles have profound implications for the global climate and human health. Among them, ultrafine particles dominate in terms of the number concentration and exhibit enhanced toxic effects as a result of their large total surface area. Therefore, understanding the driving factors behind ultrafine particle behavior is crucial. Machine learning (ML) provides a promising approach for handling complex relationships. In this study, three ML models were constructed on the basis of field observations to simulate the particle number concentration of nucleation mode (PNCN). All three models exhibited robust PNCN reproduction (R2 > 0.80), with the random forest (RF) model excelling on the test data (R2 = 0.89). Multiple methods of feature importance analysis revealed that ultraviolet (UV), H2SO4, low-volatility oxygenated organic molecules (LOOMs), temperature, and O3 were the primary factors influencing PNCN. Bivariate partial dependency plots (PDPs) indicated that during nighttime and overcast conditions, the presence of H2SO4 and LOOMs may play a crucial role in influencing PNCN. Additionally, integrating additional detailed information related to emissions or meteorology would further enhance the model performance. This pilot study shows that ML can be a novel approach for simulating atmospheric pollutants and contributes to a better understanding of the formation and growth mechanisms of nucleation mode particles.


Subject(s)
Air Pollutants , Humans , Air Pollutants/analysis , Particle Size , Pilot Projects , Environmental Monitoring/methods , Particulate Matter/analysis
5.
J Environ Sci (China) ; 138: 561-571, 2024 Apr.
Article in English | MEDLINE | ID: mdl-38135420

ABSTRACT

To gain a comprehensive understanding of sources and health risks of trace elements in an area of China with high population densities and low PM2.5 concentrations, 15 trace elements (Al, K, Ca, Ti, V, Cr, Mn, Fe, Ni, Cu, Zn, As, Sn, Ba, Pb) in PM2.5 were monitored from December 2020 to November 2021 in a representative city, Xiamen. The concentrations of trace elements in Xiamen displayed an obvious seasonal variation and were dominated by K, Fe, Al, Ca and Zn. Based on Positive Matrix Factorization analysis, source appointment revealed that the major sources of trace elements in Xiamen were traffic, dust, biomass and firework combustion, industrial manufacture and shipping emission. According to health risk assessment combined with the source appointment results, it indicated that the average noncarcinogenic risk was below the threshold and cancer risk of four hazardous metals (Cr, Ni, As, Pb) exceeded the threshold (10-6). Traffic-related source had almost half amount of contribution to the health risk induced by PM2.5-bound trace elements. During the dust transport period or Spring Festival period, the health risks exceeded an acceptable threshold even an order of magnitude higher, suggesting that the serious health risks still existed in low PM2.5 environment at certain times. Health risk assessment reminded that the health risk reduction in PM2.5 at southeastern China should prioritize traffic-related hazardous trace elements and highlighted the importance of controlling vehicles emissions in the future.


Subject(s)
Air Pollutants , Trace Elements , Particulate Matter/analysis , Air Pollutants/analysis , Trace Elements/analysis , Lead/analysis , Environmental Monitoring , Dust/analysis , China
6.
Environ Sci Technol ; 57(42): 15956-15967, 2023 10 24.
Article in English | MEDLINE | ID: mdl-37842878

ABSTRACT

Organic aerosols (OA) have gained attention as a substantial component of atmospheric aerosols owing to their impact on atmospheric visibility, climate, and human health. Although oxygenated organic molecules (OOMs) are essential contributors to OA formation, the sources, transformations, and fates of the OOMs are not fully understood. Herein, anthropogenic OOMs (AOOMs), anthropogenic volatile organic compounds (AVOCs), and OA were concurrently measured in Xiamen, a coastal city in southeastern China. Our results show that the AOOMs exhibited a high nitrogen content (76%) and a low oxidation degree. Strong photochemical processes of aromatic VOCs were the predominant sources of AOOMs. Also, NOx concentrations and the occurrence of multigeneration OH radical oxidations were the critical factors that might influence the formation of AOOMs. Finally, the newly developed aerosol dynamic model's results show that more than 35% of the OA mass growth rate is attributed to the gas-particle partitioning of AOOMs. Further sensitivity testing demonstrates that the contribution of AOOMs to OA growth is significantly enhanced during high-particulate-concentration periods, especially under low-temperature conditions. This study emphasizes the vital role of photochemically produced AOOMs derived from AVOCs in OA growth in a coastal urban atmosphere.


Subject(s)
Air Pollutants , Volatile Organic Compounds , Humans , Volatile Organic Compounds/analysis , Volatile Organic Compounds/chemistry , Coal , Atmosphere , Aerosols/analysis , China , Air Pollutants/analysis
7.
Sci Total Environ ; 901: 166318, 2023 Nov 25.
Article in English | MEDLINE | ID: mdl-37586504

ABSTRACT

The concentrations of ground-level ozone (O3) in China have undergone a rapid increase in recent years, resulting in adverse impacts on the air quality and climate change. However, limited research has been conducted on the coastal urban agglomerations with increasingly serious O3 pollution. Therefore, in order to better understand in situ photochemistry, comprehensive field observations of O3 and its precursors, coupled with the model simulation, were conducted in autumn of 2019 at six sites in an urban agglomeration along the coastline of southeastern China. Results indicated that O3 pollution in the southern part of the urban agglomeration was more severe than that in the northern part, due to higher levels of O3 precursors and stronger atmospheric oxidation capacity (AOC) in the southern regions. Oxygenated volatile organic compounds (OVOCs), NO2, and CO dominated the total OH reactivity, and the site-average daytime Ox (O3 + NO2) increments correlated well (R2 = 0.94) with the total OH reactivity of CO and VOCs at these sites except for Quanzhou, where industrial emissions (35.1 %) and solvent usages (33.7 %) dominated the VOC sources. However, vehicle exhausts (31.1 %) were the most predominant contributors to the VOC sources at other sites. The results of model simulations showed that net O3 formation rates were larger at the southern sites. Furthermore, O3 production was mainly controlled by VOCs at most sites, but co-limited by VOCs and NOx at Quanzhou. The most significant VOC groups contributing to O3 formation were aromatics and alkenes, with m/p-xylene, toluene, propene, and ethene being the main contributors at these sites. This study offers a more comprehensive understanding of the characteristics and formation of photochemical pollutions on the scale of the urban areas, indicating the critical need to reduce VOC emissions as a means of mitigating their photochemical effects.

8.
Sci Total Environ ; 891: 164477, 2023 Sep 15.
Article in English | MEDLINE | ID: mdl-37257606

ABSTRACT

Two ozone (O3) processes, summer episode dominated by local production and autumn episode dominated by regional transport, were chosen to investigate the role of HONO in different pollution processes. Meteorological conditions, diurnal variation of O3, potential source contribution factor (PSCF) analysis, concentration weighted trajectory (CWT) models, and the distribution of the eight-hour maximum values of O3 on mainland China all prove that summer O3 was mainly locally generated while autumn O3 episode was more susceptible to regional transport. The gaps between observations and simulation results with the default HONO chemistry in Master Chemical Mechanism (MCM) of Observation Based Model (OBM) were higher in summer episode (0.58 ppb) than autumn episode (0.37 ppb). Although we implemented nine additional sources in the model to revise the HONO chemistry, the simulated values were still lower than the observed values. HONO promoted O3 production by accelerating the reaction of HO2 + NO and RO2 + NO, and promoted loss of O3 by the reaction of OH + NO2 and RO2 + NO2. The net production rate of O3 with HONO constraint increased by 28.50 % in summer and 22.43 % in autumn, which also indicated that HONO played more important role in the O3 production in summer. The difference of NOx of daily RIR between the cases with and without HONO constraint was higher in summer O3 episode (0.15 %/%) than that in autumn O3 episode (0.09 %/%), the same as to VOCs with -0.20 %/% in summer O3 episode and - 0.14 %/% in autumn O3 episode, which indicated that the presence or absence of the HONO constraint has a greater impact on the RIR value in the case of dominant local generation. In brief, the O3 sensitivity would be more favorable for VOCs without HONO constrained in the model, which would inevitably mislead policy makers to develop efficient policies to control O3 pollution.

9.
Curr Res Food Sci ; 6: 100438, 2023.
Article in English | MEDLINE | ID: mdl-36660303

ABSTRACT

To explore the effect and its mechanism of alkali-assisted phosphorylation on the functional properties of Camellia Oleifera seeds cake glutelin (CSCG), CSCG was treated with different concentration of sodium trimetaphosphate (STMP, 1.0, 2.0, 3.0, 4.0, and 5%, w/v) in different pH environment (3.0, 5.0, 7.0, 9.0, and 11.0). The results showed that alkali assist improved the phosphorylation degree of CSCG, and the optimum pH value is 9.0. FT-IR and XPS confirmed the successful modification of phosphate groups on CSCG through covalent interaction. Alkali-assisted phosphorylation decreased the particle size and increased electronegativity of CSCG, as well as changed in its surface hydrophobicity, crystallinity, and intrinsic fluorescence. All these changes of protein structure triggered by alkali-assisted phosphorylation led to the improvement of water solubility, water/oil absorption capacity, emulsifying ability, foamability, and in vitro digestibility of CSCG. This work could provide a theoretical basis for industrial production of CSCG with excellent functional properties.

10.
Sci Total Environ ; 859(Pt 1): 160210, 2023 Feb 10.
Article in English | MEDLINE | ID: mdl-36395845

ABSTRACT

Formaldehyde (HCHO) is a vital reactive carbonyl compound, which plays an important role in the photochemical process and atmospheric oxidation capacity. However, the current studies on the quantification of HCHO impacts on atmospheric photochemistry in southeast coastal areas of China with an obvious upward trend of ozone remain scarce and unclear, thus limiting the full understanding of formation mechanism and control strategy of photochemical pollution. Here, systematic field campaigns were conducted at a typical coastal urban site with good air quality to reveal HCHO mechanism and effects on O3 pollution mechanism during spring and autumn, when photochemical pollution events still frequently appeared. Positive Matrix Factorization model results showed that secondary photochemical formation made the largest contributions to HCHO (69 %) in this study. Based on the photochemical model, the HCHO loss rates in autumn were significantly higher than those in spring (P < 0.05), indicating that strong photochemical conditions constrain high HCHO levels in certain situations. HCHO mechanism increased the ROx concentrations by 36 %, and increased net O3 production rates by 31 %, manifesting that the reduction of HCHO and its precursors' emissions would effectively mitigate O3 pollution. Therefore, the pollution characteristics and photochemical effects of HCHO provided significant guidance for future photochemical pollution control in relatively clean areas.


Subject(s)
Air Pollutants , Ozone , Air Pollutants/analysis , Environmental Monitoring , Photochemical Processes , Ozone/analysis , Cities , China
11.
Sci Total Environ ; 826: 154208, 2022 Jun 20.
Article in English | MEDLINE | ID: mdl-35240183

ABSTRACT

New particle formation (NPF) has a great impact on regional and global climate, air quality and human health. This study uses a Scanning Mobility Particle Sizer (SMPS) for simultaneous measurement of particle number size distribution (PNSD) in wintertime to investigate NPF in the coastal city of Xiamen. The mean particle number concentration, surface area concentration and volume concentration were 7.25 × 103 cm-3, 152.54 µm2 cm-3, and 4.03 µm3 cm-3, respectively. Particle number concentration was mainly influenced by the nucleation mode and the Aitken mode, whereas the main contributor to particle surface area concentration and volume concentration was accumulation mode particles. The frequency of NPF events occurred was around 41.4% in December 2019. The typical growth rates of new formed particles were 1.41-2.54 nm h-1, and the observed formation rates were 0.49-1.43 cm-3 s-1. A comparative analysis of conditions between event and non-event days was performed. The results emphasized that air temperature, UV radiation and relative humidity were the most decisive meteorological factors, and NPF events usually occurred under clean atmospheric conditions with low PM concentrations. Although condensation sink was high when NPF event occurred, the level of SO2 and O3 concentration was also high.


Subject(s)
Air Pollutants , Particulate Matter , Aerosols/analysis , Air Pollutants/analysis , China , Environmental Monitoring , Humans , Particle Size , Particulate Matter/analysis
12.
Sci Total Environ ; 806(Pt 2): 150654, 2022 Feb 01.
Article in English | MEDLINE | ID: mdl-34597568

ABSTRACT

Carbonaceous aerosols are major components in PM2.5 of both polluted and clean atmosphere. Accurate source apportionment of carbonaceous aerosols may support effective PM2.5 control. Dual-carbon isotope method (14C and 13C) was adopted to identify the contribution of three main air pollution sources biogenic and biomass (fbb), liquid fossil (fliq.fossil) and coal (fcoal). The aerosol samples were collected at three types of sites with distinctly different degree of air pollution: urban, rural and regional background. The seasonal variation of source apportionment of the carbonaceous aerosols in urban Beijing was discussed. Modern biogenic and biomass made an absolute dominance of 92.9 ± 0.5% contribution to the carbonaceous aerosols at the background site Mt. Yulong due to long-range transport from Southeast Asia. The three main sources contributed jointly to the atmospheric carbonaceous aerosols at the rural site Wangdu and the urban site Beijing. The biogenic and biomass source was the major contribution in summer (47.0 ± 0.3%) and autumn (49.3 ± 0.3%) of Beijing, while coal source increased from summer (26.8 ± 13.8%) to autumn (34.7 ± 11.5%). Heating significantly increased the coal source to the dominant contribution (47.0 ± 16.9%) in winter of Beijing. Separate day and night time coal contributions were used to evaluate the two origins of coal combustion: industrial use vs. residential use. The results of source apportionment for carbonaceous aerosols provide scientific support for the prevention and control of air pollution.


Subject(s)
Air Pollutants , Particulate Matter , Aerosols/analysis , Air Pollutants/analysis , Carbon/analysis , Carbon Isotopes , China , Environmental Monitoring , Particulate Matter/analysis , Seasons , Vehicle Emissions/analysis
13.
Environ Pollut ; 286: 117577, 2021 Oct 01.
Article in English | MEDLINE | ID: mdl-34438498

ABSTRACT

Revealing the changes in chemical compositions and sources of PM2.5 is important for understanding aerosol chemistry and emission control strategies. High time-resolved characterization of water-soluble inorganic ions, elements, organic carbon (OC), and elemental carbon (EC) in PM2.5 was conducted in a coastal city of southeast China during the COVID-19 pandemic. The results showed that the average concentration of PM2.5 during the city lockdown (CLD) decreased from 46.2 µg m-3 to 24.4 µg m-3, lower than the same period in 2019 (PM2.5: 37.1 µg m-3). Concentrations of other air pollutants, such as SO2, NO2, PM10, OC, EC, and BC, were also decreased by 27.3%-67.8% during the CLD, whereas O3 increased by 28.1%. Although SO2 decreased from 4.94 µg m-3to 1.59 µg m-3 during the CLD, the concentration of SO42- (6.63 µg m-3) was comparable to that (5.47 µg m-3) during the non-lockdown period, which were attributed to the increase (16.0%) of sulfate oxidation rate (SOR). Ox (O3+NO2) was positively correlated with SO42-, suggesting the impacts of photochemical oxidation. A good correlation (R2 = 0.557) of SO42- and Fe and Mn was found, indicating the transition-metal ion catalyzed oxidation. Based on positive matrix factorization (PMF) analysis, the contribution of secondary formation to PM2.5 increased during the epidemic period, consisting with the increase of secondary organic carbon (SOC), while other primary sources including traffic, dust, and industry significantly decreased by 9%, 8.5%, and 8%, respectively. This study highlighted the comprehensive and nonlinear response of chemical compositions and formation mechanisms of PM2.5 to anthropogenic emissions control under relatively clean conditions.


Subject(s)
Air Pollutants , COVID-19 , Aerosols/analysis , Air Pollutants/analysis , China , Communicable Disease Control , Environmental Monitoring , Humans , Pandemics , Particulate Matter/analysis , SARS-CoV-2 , Seasons , Sulfates , Vehicle Emissions/analysis
14.
Sci Total Environ ; 770: 145402, 2021 May 20.
Article in English | MEDLINE | ID: mdl-33736387

ABSTRACT

Identifying the nature and extent of atmospheric PM2.5-bound toxic organic pollutants is beneficial to evaluate human health risks of air pollution. Seasonal observations of PM2.5-bound polycyclic aromatic hydrocarbons (PAHs) and nitro-PAHs (NPAHs) in the Yangtze River Delta (YRD) were investigated, along with criteria air pollutants and meteorological parameters. With the elevated PM2.5 level, the percentage of 4-ring PAHs and typical NPAH including 3-Nitrobiphenyl (3-NBP) and 2-Nitrofluoranthene (2-NFLT) increased by 19-40%. PM2.5-bound 2-NFLT was positively correlated with O3 and NO2, suggesting the contribution of atmospheric oxidation capacity to enhance the secondary formation of NPAHs in the atmosphere. Positive matrix factorization (PMF) analysis indicated that traffic emissions (44.9-48.7%), coal and biomass combustion (27.6-36.0%) and natural gas and volatilization (15.3-27.5%) were major sources of PAHs, and secondary formation (39.8-53.8%) was a predominant contributor to total NPAH concentrations. Backward trajectory analysis showed that air masses from North China transported to the YRD region increased PAH and NPAH concentrations. Compare to clean days, the BaP equivalent concentrations of total PAHs and NPAHs during haze pollution days were enhanced by 10-25 and 2-6 times, respectively. The Incremental Lifetime Cancer Risks (ILCRs) of PAHs by inhalation exposure also indicated high potential health risks in the YRD region. The results implied that the health risks of PM2.5-bound PAHs and NPAHs could be sharply enhanced with the increase of PM2.5 concentrations.


Subject(s)
Air Pollutants , Air Pollution , Polycyclic Aromatic Hydrocarbons , Air Pollutants/analysis , China , Environmental Monitoring , Humans , Particulate Matter/analysis , Polycyclic Aromatic Hydrocarbons/analysis , Rivers , Seasons
15.
Sci Total Environ ; 741: 140470, 2020 Nov 01.
Article in English | MEDLINE | ID: mdl-32886967

ABSTRACT

Chemical compositions of non-refractory submicron aerosol (NR-PM1) were measured via an Aerodyne Aerosol Chemical Speciation Monitor at the coastal city Xiamen during the 2017 BRICS summit from August 10 to September 10. Mean hourly concentration of NR-PM1 was 13.55 ± 8.83 µg m-3 during the study period, decreasing from 18.83 µg m-3 before-BRICS to 13.02 µg m-3 in BRCIS I and 8.42 µg m-3 in BRICS II. Positive matrix factor analyses resolved four organic aerosols (OA): a hydrocarbon-like OA (HOA, 14.78%), a cooking-related OA (COA, 28.21%), a biomass burning OA (BBOA, 18.00%), and an oxygenated OA (OOA, 39.22%). The contributions of local pollutants like nitrate and HOA reduced, while the proportions of sulfate and OOA increased during the control episodes. The diurnal patterns of NR-PM1 species and OA components in each episode were characterized. The results showed that BC, nitrate, COA, and HOA had peaks in the morning and evening, which became less obvious under the emission control. Moreover, the diurnal variations of all species in Ep 3 with emission control were much flatter due to the effect of transport. Backward trajectories analysis confirmed the long-range transport of air masses from the continent, which resulted in the high proportions of sulfate (43.69%) and OOA (50.28%) in Ep 3. Our study implies the significant effect of emission control on reducing primary pollutants, but the formation of particles during the long-range transport need to be paid more attention when set the air quality control strategies in coastal cities.

16.
Sci Total Environ ; 719: 137493, 2020 Jun 01.
Article in English | MEDLINE | ID: mdl-32120104

ABSTRACT

Peroxyacetyl nitrate (PAN) can effectively indicate photochemical pollution, and also plays a vital role in regional oxidant balance. One-year continuous monitoring of PAN in a coastal city of southeastern China was investigated. The mean concentration of PAN in winter (0.64 ppb) was close to that in autumn (0.73 ppb), indicating that photochemical pollution was still non-negligible in the cold season. The peak occurrence time between O3 and PAN had a delay of 1-2 h in four seasons, due to the rapid decomposition rate of PAN in midday. Emission sources of the precursors are located to the south of the monitoring site, so high concentrations of PAN and O3 are frequently observed under southerly wind conditions. The air mass with low concentration of PAN (0.22-0.34 ppb) and O3 (18.17-23.67 ppb) originated from the ocean with less anthropogenic air pollutants. Continental air mass with high PAN concentration might be related to the contribution of heterogeneous reactions of PM2.5 to the promotion of PAN formation. In the polluted case, PAN concentration was often higher than 1.0 ppb and reached the peak of 4.2 ppb, suggesting the influence of photochemical reactions and local accumulation. High concentrations of HONO and sufficient ultraviolet radiation might be the main factors for rapid photochemical production of PAN. Besides, the lifetime of PAN in winter under the condition of high PM2.5 concentration (≥35 µg·m-3) was up to 3.246 days. This study provided insights into photochemical mechanism and pollution process in a coastal city of southeastern China.

17.
Sci Total Environ ; 707: 136194, 2020 Mar 10.
Article in English | MEDLINE | ID: mdl-31972916

ABSTRACT

The quasi-stationary front is a significant weather system which influences East Asia in spring. The air quality deteriorated along with the moist circumstance when the quasi stationary front dominated the area. Surface meteorological parameters, air pollutants and PM2.5 chemical species were observed during the air pollution episode. Liquid water content and aerosol acidity were calculated by thermodynamic model in order to investigate heterogeneous/aqueous reactions for secondary aerosol formation. The episode was divided into four stages based on quasi-stationary front influences. Hourly PM2.5 concentrations were up to 150.2 µg·m-3 while O3 concentrations reached the minimum value of 1.27 µg·m-3, indicating that the precursor gas NOx participated in the different reactions during the episode. Nitrate proportion of water-soluble inorganic ions was 42.2%. High concentrations of secondary inorganic aerosol ions and the high sulfur oxidation ratio (SOR) and nitrogen oxidation ratio (NOR) indicated the increasing conversions from SO2 and NOx to their corresponding particulate phases. Ratios of [NO3-]/[SO42-] and [NH4+]/[SO42-] in the four stages declared that nitrate formation preferred heterogeneous conversions. A series of liquid water content (LWC) fitting equations between relative humidity and inorganic ions were conducted to verify heterogeneous aqueous reactions of NO2 and secondary nitrate formation. The results of this study highlighted the significance of LWC and chemical reactions associated with acidity during the specific synoptic situation in South China.

18.
Environ Sci Technol ; 53(24): 14222-14232, 2019 12 17.
Article in English | MEDLINE | ID: mdl-31722173

ABSTRACT

To elucidate the influence of long-range transported biomass burning organic aerosols (BBOA) on the Tibetan Plateau, the molecular compositions and light absorption of HUmic-Like Substances (HULIS), major fractions of brown carbon, were characterized during the premonsoon season. Under the significant influence of biomass burning, HULIS concentrations increased to as high as 26 times of the background levels, accounting for 54% of water-soluble organic carbon (WSOC) and 50% of organic carbon (OC). The light absorption of HULIS also enhanced up to 42 times of the background levels, contributing 61% of the WSOC absorption and 50% of OC absorption. Meanwhile, elevated nitrogen-containing compounds (NOCs) among HULIS were observed. The NOCs from fresh and aged BBOA were unambiguously identified on the molecular level, through comparing with the molecular compositions of NOCs from lab-controlled and field burning experiments. N-Heterocyclic bases represent major fractions in the reduced nitrogen compounds from fresh BBOA, and nitroaromatic compounds are important groups among the oxidized nitrogen compounds from aged BBOA. The nitrogen-containing compounds, including nitroaromatics and N-heterocyclic compounds, were also important chromophores, which contributed to the enhanced light absorption of extracted HULIS during biomass burning-influenced periods.


Subject(s)
Air Pollutants , Nitrogen , Aerosols , Biomass , Carbon , Environmental Monitoring , Particulate Matter , Tibet
19.
Sci Total Environ ; 692: 1135-1145, 2019 Nov 20.
Article in English | MEDLINE | ID: mdl-31539945

ABSTRACT

To investigate the impact of the Western Pacific subtropical high (WPSH) on the air pollution episode of Xiamen, a coastal city in Southeastern China, this study focused on formation processes and influencing mechanisms of an air pollution episode from 17th to 23rd September 2017. The results showed that the WPSH fluctuated in this period and intensified this air pollution with local emissions. The episode was divided into four stages according to WPSH center locations to diagnose the air pollution. Visibility declined below 10 km twice while fine particulate matte (PM2.5) concentration was up to 89.05 µg/m3 during this episode. As a consequence of high temperature (28.33 ±â€¯1.25 °C) resulted from WPSH, atmospheric oxidation at high level (140.81 ±â€¯56.49 µg/m3) was the driving force of secondary aerosols generations. Oxidation determined photo-chemical reactions with the pathways of gas-phase and heterogeneous formation. Sulfate was formed from gas-phase oxidation by SO2 in daytime while heterogeneous reaction occurred at night. Nitrate generation was dominated by not only excess ammonium but also intense oxidation. Reconstruction light extinction results coupling with trajectories revealed that (NH4)2SO4, NH4NO3 and OM were the priority factors to the reduction of atmospheric visibility. These findings provided new insights of air pollution episode diagnosis and indicative function of WPSH impacts on local air quality in Southeast China.

20.
Sci Total Environ ; 657: 1491-1500, 2019 Mar 20.
Article in English | MEDLINE | ID: mdl-30677915

ABSTRACT

Volatile organic compounds (VOCs) are important trace gases in the atmosphere, affecting air quality (e.g. ozone and secondary organic aerosol formation) and human health. To understand the emission, transport and chemistry of VOCs in the southeast of China (Fujian Province), a campaign was conducted in summer and winter of 2016 at three contrasting sites in close proximity. One measurement site (Mt. Wuyi) is a mountainous forest site (1139 m a.s.l.) located in a natural reserve, while the other two sites (Fuzhou, Xiamen) are coastal urban sites with high population and vehicle density. Comparison of VOCs at these three sites provides a valuable perspective on regional air pollution and transport. Many of the measured alkanes, alkenes and aromatics exhibited clear seasonal and diurnal patterns, driven by variations of hydroxyl (OH) radicals, which is the predominant oxidant of VOCs in the atmosphere. By examining tracer-tracer correlations for VOCs, variability-lifetime analysis and 36 h backward trajectories, strong emissions from vehicular exhaust, liquefied petroleum gas (LPG) and solvent usage were identified as key sources in Fuzhou and Xiamen, whereas at Mt. Wuyi the main emission sources were local emissions (e.g. biomass burning) in summer and long-range transport in winter. The results indicate that natural sites could be impacted strongly by surrounding urbanization. Isoprene and propylene in summer and propylene in winter contributed the most to ozone formation at the three sites. The data in this study provides a useful benchmark for future research on air quality monitoring and emission sources in the region.

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