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1.
Environ Sci Technol ; 58(16): 6988-6997, 2024 Apr 23.
Artigo em Inglês | MEDLINE | ID: mdl-38592860

RESUMO

In 2022, many Chinese cities experienced lockdowns and heatwaves. We analyzed ground and satellite data using machine learning to elucidate chemical and meteorological drivers of changes in O3 pollution in 27 major Chinese cities during lockdowns. We found that there was an increase in O3 concentrations in 23 out of 27 cities compared with the corresponding period in 2021. Random forest modeling indicates that emission reductions in transportation and other sectors, as well as the changes in meteorology, increased the level of O3 in most cities. In cities with over 80% transportation reductions and temperature fluctuations within -2 to 2 °C, the increases in O3 concentrations were mainly attributable to reductions in nitrogen oxide (NOx) emissions. In cities that experienced heatwaves and droughts, increases in the O3 concentrations were primarily driven by increases in temperature and volatile organic compound (VOC) emissions, and reductions in NOx concentrations from ground transport were offset by increases in emissions from coal-fired power generation. Despite 3-99% reduction in passenger volume, most cities remained VOC-limited during lockdowns. These findings demonstrate that to alleviate urban O3 pollution, it will be necessary to further reduce industrial emissions along with transportation sources and to take into account the climate penalty and the impact of heatwaves on O3 pollution.

2.
Environ Sci Technol ; 58(18): 7904-7915, 2024 May 07.
Artigo em Inglês | MEDLINE | ID: mdl-38661303

RESUMO

Nitrogen dioxide (NO2) hydrolysis in deliquesced aerosol particles forms nitrous acid and nitrate and thus impacts air quality, climate, and the nitrogen cycle. Traditionally, it is considered to proceed far too slowly in the atmosphere. However, the significance of this process is highly uncertain because kinetic studies have only been made in dilute aqueous solutions but not under high ionic strength conditions of the aerosol particles. Here, we use laboratory experiments, air quality models, and field measurements to examine the effect of the ionic strength on the reaction kinetics of NO2 hydrolysis. We find that high ionic strengths (I) enhance the reaction rate constants (kI) by more than an order of magnitude compared to that at infinite dilution (kI=0), yielding log10(kI/kI=0) = 0.04I or rate enhancement factor = 100.04I. A state-of-the-art air quality model shows that the enhanced NO2 hydrolysis reduces the negative bias in the simulated concentrations of nitrous acid by 28% on average when compared to field observations over the North China Plain. Rapid NO2 hydrolysis also enhances the levels of nitrous acid in other polluted regions such as North India and further promotes atmospheric oxidation capacity. This study highlights the need to evaluate various reaction kinetics of atmospheric aerosols with high ionic strengths.


Assuntos
Aerossóis , Aerossóis/química , Hidrólise , Concentração Osmolar , Dióxido de Nitrogênio/química , Cinética , Atmosfera/química , Poluentes Atmosféricos/química
3.
Environ Int ; 185: 108487, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38367554

RESUMO

Particulate organic nitrates (pONs) have drawn growing interests due to their effects on nitrogen cycling, air pollution, and regional climate. While secondary formation is typically considered as the major source of pONs, direct emissions from various sources remain poorly explored. Ship exhausts have been known as an important source of reactive nitrogen species, yet pONs emissions from ship have been rarely characterized. In this study, we conducted atmospheric measurement of pONs during a ship-based cruise measurement campaign in the East China Sea and also emission measurement of pONs from ship exhausts. During the ship-based cruise, total five typical kinds of pONs were determined and the average total concentrations of five pONs were 479 ± 193 and 250 ± 139 ng m-3 when sampling was influenced by ship emissions or not, respectively, indicating the notable impact of ship exhaust plumes on ambient pONs. Further, five typical pONs were successfully identified and quantified from ship exhausts, with the average total concentration of 1123 ± 406 µg m-3. The much higher pONs levels in ship exhausts than in ambient particulate matters demonstrated ship emission as an important source for pONs. Additionally, their emission factors from ship exhausts were determined as at a range of 0.1-12.6 mg kWh-1. The chemical transport model simulations indicate that direct pONs emissions from ship exert a significant contribution to atmospheric pONs, especially in the clean marine atmosphere. These findings provide compelling evidence for direct emission of pONs from ship and its considerable effects. We call for further studies to better characterize the direct pONs emissions from ship and other potential sources, which should be incorporated into global and regional models.


Assuntos
Poluentes Atmosféricos , Poluição do Ar , Poluentes Atmosféricos/análise , Navios , Monitoramento Ambiental , Material Particulado/análise , Poluição do Ar/análise , Emissões de Veículos/análise , Poeira , Carvão Mineral , China
4.
Environ Pollut ; 344: 123368, 2024 Mar 01.
Artigo em Inglês | MEDLINE | ID: mdl-38246217

RESUMO

Nitrophenols have received extensive attention due to their strong light-absorbing ability in the near-ultraviolet-visible region, which could be influenced by the atmospheric processes of nitrophenols. However, our knowledge and understanding of the formation and evolution of nitrophenols are still in the nascent stages. In the present study, the mixing states of four mononitrophenol particles (i.e., nitrophenol, methynitrophenol, nitrocatechol, and methoxynitrophenol), and one nitropolycyclic aromatic hydrocarbon particles (i.e., nitronaphthol (NN)) were investigated using a single-particle aerosol mass spectrometer (SPAMS) in November 2019 in Qingdao, China. The results showed, for the first time, that mononitrophenols and NN exhibit different mixing states and diurnal variations. Four mononitrophenols were internally mixed well with each other, and with organic acids, nitrates, potassium, and naphthalene. The diurnal variation in the number fraction of mononitrophenols presented two peaks at 07:00 to 09:00 and 18:00 to 20:00, and a valley at noon. Atmospheric environmental conditions, including NO2, O3, relative humidity, and temperature, can significantly influence the diurnal variation of mononitrophenols. Multiple linear regression and random forest regression models revealed that the main factors controlling the diurnal variation of mononitrophenols were photochemical reactions during the day and aqueous-phase reactions during the night. Unlike mononitrophenols, about 62-83% of NN were internally mixed with [NH4]+ and [H(NO3)2]-, but not with organic acids and potassium. The diurnal variation of NN was also different from that of mononitrophenols, generally increased from 17:00 to 10:00 and then rapidly decreaed from 11:00 to 16:00. These results imply that NN may have sources and atmospheric processes that are different from mononitrophenols. We speculate that this is mostly controlled by photochemical reactions and mixing with [NH4]+, which may influence the diurnal variation of NN in the ambient particles; however, this requires further confirmation. These findings extend our current understanding of the atmospheric formation and evolution of nitrophenols.


Assuntos
Poluentes Atmosféricos , Nitrofenóis , Potássio , Ritmo Circadiano , Antifúngicos , China , Poeira , Aerossóis , Monitoramento Ambiental , Material Particulado , Estações do Ano
5.
J Hazard Mater ; 465: 133175, 2024 Mar 05.
Artigo em Inglês | MEDLINE | ID: mdl-38086305

RESUMO

Fog significantly affects the air quality and human health. To investigate the health effects and mechanisms of atmospheric fine particulate matter (PM2.5) during fog episodes, PM2.5 samples were collected from the coastal suburb of Qingdao during different seasons from 2021 to 2022, with the major chemical composition in PM2.5 analyzed. The oxidative potential (OP) of PM2.5 was determined using the dithiothreitol (DTT) method. A positive matrix factorization model was adopted for PM2.5. Interpretable machine learning (IML) was used to reveal and quantify the key components and sources affecting OP. PM2.5 exhibited higher oxidative toxicity during fog episodes. Water-soluble organic carbon (WSOC), NH4+, K+, and water-soluble Fe positively affected the enhancement of DTTV (volume-based DTT activity) during fog episodes. The IML analysis demonstrated that WSOC and K+ contributed significantly to DTTV, with values of 0.31 ± 0.34 and 0.27 ± 0.22 nmol min-1 m-3, respectively. Regarding the sources, coal combustion and biomass burning contributed significantly to DTTV (0.40 ± 0.38 and 0.39 ± 0.36 nmol min-1 m-3, respectively), indicating the significant influence of combustion-related sources on OP. This study provides new insights into the effects of PM2.5 compositions and sources on OP by applying IML models.

6.
Environ Sci Technol ; 58(1): 617-627, 2024 Jan 09.
Artigo em Inglês | MEDLINE | ID: mdl-38112179

RESUMO

In recent years, the magnitude and frequency of regional ozone (O3) episodes have increased in China. We combined ground-based measurements, observation-based model (OBM), and the Weather Research and Forecasting and Community Multiscale Air Quality (WRF-CMAQ) model to analyze a typical persistent O3 episode that occurred across 88 cities in northeastern China during June 19-30, 2021. The meteorological conditions, particularly the wind convergence centers, played crucial roles in the evolution of O3 pollution. Daily analysis of the O3 formation sensitivity showed that O3 formation was in the volatile organic compound (VOC)-limited or transitional regime at the onset of the pollution episode in 92% of the cities. Conversely, it tended to be or eventually became a NOx-limited regime as the episode progressed in the most polluted cities. Based on the emission-reduction scenario simulations, mitigation of the regional O3 pollution was found to be most effective through a phased control strategy, namely, reduction of a high ratio of VOCs to NOx at the onset of the pollution and lower ratio during evolution of the O3 episode. This study presents a new possibility for regional O3 pollution abatement in China based on a reasonable combination of OBM and the WRF-CMAQ model.


Assuntos
Poluentes Atmosféricos , Poluição do Ar , Ozônio , Compostos Orgânicos Voláteis , Ozônio/análise , Poluentes Atmosféricos/análise , Monitoramento Ambiental , China , Compostos Orgânicos Voláteis/análise
7.
J Environ Sci (China) ; 138: 543-560, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38135419

RESUMO

Observation-based method for O3 formation sensitivity research is an important tool to analyze the causes of ground-level O3 pollution, which has broad application potentials in determining the O3 pollution formation mechanism and developing prevention and control strategies. This paper outlined the development history of research on O3 formation sensitivity based on observational methods, described the principle and applicability of the methodology, summarized the relative application results in China and provided recommendations on the prevention and control of O3 pollution in China based on relevant study results, and finally pointed out the shortcomings and future development prospects in this field in China. The overview study showed that the O3 formation sensitivity in some urban areas in China in recent years presented a gradual shifting tendency from the VOC-limited regime to the transition regime or the NOx-limited regime due to the implementation of the O3 precursors emission reduction policies; O3 pollution control strategies and precursor control countermeasures should be formulated based on local conditions and the dynamic control capability of O3 pollution control measures should be improved. There are still some current deficiencies in the study field in China. Therefore, it is recommended that a stereoscopic monitoring network for atmospheric photochemical components should be further constructed and improved; the atmospheric chemical mechanisms should be vigorously developed, and standardized methods for determining the O3 formation sensitivity should be established in China in the near future.


Assuntos
Poluentes Atmosféricos , Ozônio , Compostos Orgânicos Voláteis , Ozônio/análise , Poluentes Atmosféricos/análise , Compostos Orgânicos Voláteis/análise , Monitoramento Ambiental , China , Estudos Observacionais como Assunto
8.
Environ Sci Technol ; 57(42): 15979-15989, 2023 10 24.
Artigo em Inglês | MEDLINE | ID: mdl-37821356

RESUMO

Aerosol nitrate (NO3-) constitutes a significant component of fine particles in China. Prioritizing the control of volatile organic compounds (VOCs) is a crucial step toward achieving clean air, yet its impact on NO3- pollution remains inadequately understood. Here, we examined the role of VOCs in NO3- formation by combining comprehensive field measurements conducted during the China International Import Expo (CIIE) in Shanghai (from 10 October to 22 November 2018) and multiphase chemical modeling. Despite a decline in primary pollutants during the CIIE, NO3- levels increased compared to pre-CIIE and post-CIIE─NO3- concentrations decreased in the daytime (by -10 and -26%) while increasing in the nighttime (by 8 and 30%). Analysis of the observations and backward trajectory indicates that the diurnal variation in NO3- was mainly attributed to local chemistry rather than meteorological conditions. Decreasing VOCs lowered the daytime NO3- production by reducing the hydroxyl radical level, whereas the greater VOCs reduction at night than that in the daytime increased the nitrate radical level, thereby promoting the nocturnal NO3- production. These results reveal the double-edged role of VOCs in NO3- formation, underscoring the need for transferring large VOC-emitting enterprises from the daytime to the nighttime, which should be considered in formulating corresponding policies.


Assuntos
Poluentes Atmosféricos , Ozônio , Compostos Orgânicos Voláteis , Nitratos/análise , Compostos Orgânicos Voláteis/análise , Poluentes Atmosféricos/análise , China , Poluição Ambiental/análise , Monitoramento Ambiental , Ozônio/análise
9.
Water Res ; 244: 120402, 2023 Oct 01.
Artigo em Inglês | MEDLINE | ID: mdl-37572460

RESUMO

Chemical speciation of mercury (Hg) in clouds largely determines the photochemistry of Hg in the atmosphere and consequently influences Hg deposition on the surface through precipitation. Cloud water chemistry has notably changed over the last decade in response to global changes, however, the effects on Hg speciation remain poorly understood. During summer 2021, we collected sixty cloud water samples at Mt. Tai in eastern China and compared the cloud chemistry and Hg speciation with our previous findings during summer 2015. The results showed that although there were no statistically significant differences in the concentrations of total Hg (THg), dissolved Hg (DHg), and particulate Hg (PHg), there was a distinct shift in DHg species from the predominated Hg-DOM (78.6% in 2015 campaign) to the more homogeneously distributed Hg(OH)2 (28.4% in 2021 campaign), HgBr2 (26.5%), Hg-DOM (17.3%) and HgBrOH (17.0%). Changes in cloud water chemistry, particularly the significant increase in pH values to 6.49 ± 0.27 and unexpectedly high levels of bromide ions (Br-, 0.19 ± 0.22 mg L-1), were found to drive the changing of Hg speciation by enhancing Hg(II) hydrolysis and binding by Br-. Elevated Br- originating primarily from the continent likely caused noticeable differences in the dominating DHg species between cloud water sourced from marine and continental regions. The changes in chemical speciation of DHg were estimated to result in a 2.6-fold decrease in Hg(II) photoreduction rate between 2015 and 2021 campaigns (0.178 ± 0.054 h-1 vs. 0.067 ± 0.027 h-1), implying a shortened lifetime of atmospheric Hg and increased ecological risks associated with Hg wet deposition.


Assuntos
Mercúrio , Poluentes Químicos da Água , Mercúrio/análise , Água , Monitoramento Ambiental/métodos , China , Poluentes Químicos da Água/análise
10.
Sci Total Environ ; 898: 165303, 2023 Nov 10.
Artigo em Inglês | MEDLINE | ID: mdl-37419351

RESUMO

Nitrate (NO3-) is a major component of atmospheric fine particles. Recent studies in eastern China have shown the increasing trend of NO3- in contrast to the ongoing control of nitrogen oxide (NOx). Here, we elucidate the effects of reduced sulfur dioxide (SO2) on the enhancement of NO3- formation based on field measurements at the summit of Mt. Tai (1534 m a.s.l.) and present detailed modelling analyses. From 2007 to 2018, the measured springtime concentrations of various primary pollutants and fine sulfate (SO42-) decreased sharply (-16.4 % to -89.7 %), whereas fine NO3- concentration increased by 22.8 %. The elevated NO3- levels cannot be explained by the changes in meteorological conditions or other related parameters but were primarily attributed to the considerable reduction in SO42- concentrations (-73.4 %). Results from a multi-phase chemical box model indicated that the reduced SO42- levels decreased the aerosol acidity and prompted the partitioning of HNO3 into the aerosol phase. WRF-Chem model analyses suggest that such a negative effect is a regional phenomenon throughout the planetary boundary layer over eastern China in spring. This study provides new insights into the worsening situation of NO3- aerosol pollution and has important implications for controlling haze pollution in China.

11.
Sci Total Environ ; 892: 164702, 2023 Sep 20.
Artigo em Inglês | MEDLINE | ID: mdl-37302609

RESUMO

To evaluate the optical properties and molecular composition of water-soluble organic carbon (WSOC) in the atmosphere of coastal cities, particle samples were collected in Tianjin, Qingdao and Shanghai, three coastal cities in eastern China. Subsequent analysis by ultraviolet visible and fluorescence spectrometer and electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry were performed. The results showed that the concentration levels and light absorption ability of WSOC decreased from the north to south cities, ranking as Tianjin > Qingdao > Shanghai. Three major fluorescent components including less­oxygenated humic-like substances (52-60 %), highly­oxygenated humic-like substances (15-31 %) and protein-like substances (17-31 %) were identified in WSOC based on the fluorescence spectroscopy and parallel factor analysis, which might be closely related to anthropogenic emissions and continental sources as well as secondary formation processes. Five subgroups of molecular components were further identified in WSOC, including the predominant CHON compounds (35-43 %), sulfur-containing compounds (i.e., CHONS and CHOS compounds, 24-43 %), CHO compounds (20-26 %) and halogen-containing compounds (1-7 %). Compared to marine air masses influenced samples, WSOC affected by continental air masses exhibited higher light absorption coefficients and generally had a higher degree of aromaticity and unsaturation, as well as contained more molecular formulas of WSOC, especially enriched with sulfur-containing compounds. In contrast, relatively more abundant halogen-containing compounds were identified in the marine air masses influenced samples. Overall, this study provided new insights into the light-absorbing and chemical properties of WSOC in coastal cities, especially under the influences of continental and marine air masses.


Assuntos
Poluentes Atmosféricos , Carbono , Carbono/análise , China , Material Particulado/análise , Poluentes Atmosféricos/análise , Cidades , Água/química , Substâncias Húmicas/análise , Aerossóis/análise , Compostos de Enxofre , Halogênios/análise , Enxofre/análise , Monitoramento Ambiental/métodos
12.
Atmos Environ (1994) ; 308: 119864, 2023 Sep 01.
Artigo em Inglês | MEDLINE | ID: mdl-37250918

RESUMO

The COVID-19 pandemic promoted strict restrictions to human activities in China, which led to an unexpected increase in ozone (O3) regarding to nitrogen oxides (NOx) and volatile organic compounds (VOCs) co-abatement in urban China. However, providing a quantitative assessment of the photochemistry that leads to O3 increase is still challenging. Here, we evaluated changes in O3 arising from photochemical production with precursors (NOX and VOCS) in industrial regions in Shanghai during the COVID-19 lockdowns by using machine learning models and box models. The changes of air pollutants (O3, NOX, VOCs) during the COVID-19 lockdowns were analyzed by deweathering and detrending machine learning models with regard to meteorological and emission effects. After accounting for effects of meteorological variability, we find increase in O3 concentration (49.5%). Except for meteorological effects, model results of detrending the business-as-usual changes indicate much smaller reduction (-0.6%), highlighting the O3 increase attributable to complex photochemistry mechanism and the upward trends of O3 due to clear air policy in Shanghai. We then used box models to assess the photochemistry mechanism and identify key factors that control O3 production during lockdowns. It was found that empirical evidence for a link between efficient radical propagation and the optimized O3 production efficiency of NOX under the VOC-limited conditions. Simulations with box models also indicate that priority should be given to controlling industrial emissions and vehicle exhaust while the VOCs and NOX should be managed at a proper ratio in order to control O3 in winter. While lockdown is not a condition that could ever be continued indefinitely, findings of this study offer theoretical support for formulating refined O3 management in industrial regions in Shanghai, especially in winter.

14.
Sci Total Environ ; 874: 162424, 2023 May 20.
Artigo em Inglês | MEDLINE | ID: mdl-36868278

RESUMO

Surface ozone pollution has become the biggest issue in China's air pollution since particulate matters have been improved in the atmosphere. Compared with normal winter/summer, extremely cold/hot weather sustained several days and nights by unfavorable meteorology is more impactful in this regard. However, ozone changes in extreme temperatures and their driving processes remain rarely understood. Here, we combine comprehensive observational data analysis and 0-D box models to quantify the contributions of different chemical processes and precursors to ozone change in these unique environments. Analyses of radical cycling indicate that temperature accelerates OH-HO2-RO2, optimizing ozone production efficiency in higher temperatures. The HO2 + NO → OH + NO2 reaction was the most influenced by temperature change, followed by OH + VOCs → HO2/RO2. Although most reactions in ozone formation increased with temperature, the increase in ozone production rates was greater than the rate of ozone loss, leading to a fast net ozone accumulation in heat waves. Our results also show that the ozone sensitivity regime is VOC-limited in extreme temperatures, highlighting the significance of volatile organic compound (VOC) control (particularly the control of alkenes and aromatics). In the context of global warming and climate change, this study helps us deeply understand ozone formation in extreme environments and design abatement policies for ozone pollution in such conditions.

15.
Sci Total Environ ; 858(Pt 3): 159951, 2023 Feb 01.
Artigo em Inglês | MEDLINE | ID: mdl-36336034

RESUMO

Volatile organic compounds (VOCs) management has been recently given a high priority in China to mitigate ozone (O3) air pollution. However, there is a relatively poor understanding of VOCs due to their complexity and fewer observations. To better understand the pollution characteristics of VOCs and their impact on O3 pollution, two-year continuous measurements were conducted at four representative sites in Ji'nan, eastern China. These four sites cover urban, background, and industrial areas (within a petroleum refinery). Ambient VOCs showed higher concentrations at industrial site than at urban and background sites, owing to intensive emissions from petrochemical industry. The VOCs compositions present spatial heterogeneity with alkenes dominated in total reactivity at urban and background sites, while alkenes and aromatics together dominated at industrial site. The VOCs emission profile from petrochemical industry was calculated based on observational data, which revealed a huge impact on light alkanes (C2-C5), light alkenes (ethene), and aromatics (toluene and m/p-xylene). The positive matrix factorization (PMF) model analysis further refined the impact of different petrochemical industrial processes. Alkanes and alkenes dominated the emissions during refining process, while aromatics dominated during solvent usage process. Analysis by an observation-based model indicated stronger in-situ O3 production and higher sensitivity to nitrogen oxides at industrial site compared to urban and background sites. The reduction of VOCs emissions from petrochemical industry would significantly reduce the O3 concentrations. The analyses underline the significant impact of petrochemical industry on VOCs and O3 pollution, and provide important reference for the formulation of refined and effective control strategies.


Assuntos
Cidades , Monitoramento Ambiental , Compostos Orgânicos Voláteis , China
16.
J Environ Manage ; 324: 116327, 2022 Dec 15.
Artigo em Inglês | MEDLINE | ID: mdl-36183531

RESUMO

Ozone (O3) pollution has emerged as a major air quality issue in China. Here we emphasize the great challenges in controlling O3 pollution by analyzing the recent experience of the Pearl River Delta (PRD) in southern China in reducing the autumn O3 peaks. Despite significant reductions in the concentration of O3 precursors, i.e., nitrogen oxides (NOx) and volatile organic compounds (VOCs), regional O3 pollution in the PRD was largely worse in autumn 2019 than in autumn 2018. We found that the supra-regional and regional background concentrations of O3 increased significantly in the PRD in autumn 2019 due to increased concentrations of O3 in the vast surrounding areas. We also observed slight increases in the concentrations of PRD-regionally and Guangzhou-locally produced O3. A chemical box-model analysis confirmed a slight increase in the in-situ production of O3 and revealed that increased biogenic VOCs (BVOCs) and decreased NOx levels negated the effect of significant decrease in the anthropogenic VOCs. Taken together, these aspects exacerbated O3 pollution in the PRD region in autumn 2019 relative to autumn 2018. The findings from this study highlight the strong interactions of O3 pollution over multiple regions and the need for collaborative inter-regional efforts to control O3 pollution. The experience of PRD also underlines the key role of BVOCs and the importance of science-based strategies to decrease VOCs and NOx.


Assuntos
Poluentes Atmosféricos , Poluição do Ar , Ozônio , Compostos Orgânicos Voláteis , Ozônio/análise , Compostos Orgânicos Voláteis/análise , Poluentes Atmosféricos/análise , Monitoramento Ambiental , Poluição do Ar/análise , Políticas , China
17.
Environ Sci Technol ; 56(20): 14326-14337, 2022 10 18.
Artigo em Inglês | MEDLINE | ID: mdl-36178303

RESUMO

As important regions of transition between land and sea, the three bay areas of Bohai Bay (BHB), Hangzhou Bay (HZB), and Pearl River Estuary (PRE) in China often suffer from severe photochemical pollution despite scarce anthropogenic emissions. To understand the causes of high ozone (O3) concentrations, the high O3 episode days associated with special synoptic systems in the three bays were identified via observations and simulated by the weather research and forecasting coupled with community multiscale air quality (WRF-CMAQ) model. It was revealed that the interaction between synoptic winds and mesoscale breezes resulted in slow wind speeds over the HZB and PRE, where air pollutants transported from upwind cities gained a long residence time and subsequently participated in intensive photochemical reactions. The net O3 production rates within the bay areas were even comparable to those in surrounding cities. This finding was also applicable to BHB but with lower net O3 production rates, while high levels of background O3 and the regional transport from farther upwind BHB partially elevated the O3 concentrations. Hence, these three bay areas served as O3 "pools" which caused the accumulation of air pollutants via atmospheric dynamics and subsequent intense photochemical reactions under certain meteorological conditions. The results may be applicable to other similar ecotones around the world.


Assuntos
Poluentes Atmosféricos , Poluição do Ar , Ozônio , Poluentes Atmosféricos/análise , Poluição do Ar/análise , China , Monitoramento Ambiental/métodos , Ozônio/análise
18.
Sci Total Environ ; 839: 156149, 2022 Sep 15.
Artigo em Inglês | MEDLINE | ID: mdl-35643128

RESUMO

Coal is well known as the primary energy consumption in China, and the coal chemical industry (CCI) can serve as an important source of volatile organic compounds (VOCs) emissions. However, the characteristics of VOCs emitted from CCI along with their environmental consequences are still poorly understood. To pin down this, an intensive field campaign was carried out at a typical CCI city in northwestern China (Yulin) from February 26 to March 7, 2021. Results showed that VOC compositions in Yulin were distinct from those in the megacities of China as well as in the typical oilfields over the world. The concentration of naphthalene (1.6 ± 1.1 ppbv), an important byproduct of CCI, was significantly higher than that in other cities (<0.2 ppbv). Positive matrix factorization (PMF) model analysis revealed that the direct contribution of the CCI source for VOC emissions is 8.8 ± 1.8%. More importantly, these VOCs emitted from the CCI can account for 17.9 ± 6.8% of ozone (O3) formation potential and 16.9 ± 7.4% of OH reactivity of VOCs, suggesting the significant impacts of the CCI on the air quality and atmospheric oxidizing capacity. During the observation, a rapid increase in O3 concentration after a snowfall was encountered. The changing rate of O3 concentration in the daytime was significantly higher than in its peripheral cities. The increased O3 formation was partially attributed to the CCI, and this enhancement can be further magnified by snow cover due to the increment of surface albedo. These findings deepen the understanding of the characteristics and air quality impact of VOCs related to the CCI and provide valuable insights for the development of air quality control measures in the region influenced by intensive coal chemical production.


Assuntos
Poluentes Atmosféricos , Ozônio , Compostos Orgânicos Voláteis , Poluentes Atmosféricos/análise , Indústria Química , China , Cidades , Carvão Mineral/análise , Monitoramento Ambiental/métodos , Ozônio/análise , Emissões de Veículos/análise , Compostos Orgânicos Voláteis/análise
19.
Sci Total Environ ; 839: 156281, 2022 Sep 15.
Artigo em Inglês | MEDLINE | ID: mdl-35644408

RESUMO

Amines in fine particles constitute a significant fraction of secondary organic aerosols and have adverse effects on air quality and human health. To understand the chemical composition, variation characteristics, and potential sources of fine particulate amines in the coastal area in northern China, field sampling and chemical analysis were conducted in coastal Qingdao in the winter of 2018 and 2019. A total of 15 major amines were identified and quantified by using an ultra-high-performance liquid chromatography coupled with mass spectrometry. The average concentration of total amines in PM2.5 samples was approximately 130 ng m-3. Dimethylamine was the most abundant species with average fractions of 44.8% and 65.0% in the quantified amines during the two field campaigns, followed by triethylamine (22.9% and 8.7%) and methylamine (8.3% and 4.4%). The amines in PM2.5 usually exhibited elevated concentrations in the presence of high levels of SO2 and NOx or in the condition of high relative humidity. A receptor model of positive matrix factorization was employed and seven major sources were identified, including coal combustion, industrial production, vehicle exhaust, biomass burning, agricultural activities, secondary formation, and marine emission. Surprisingly, most of 15 amines in fine particles primarily originated from the primary emissions of anthropogenic activities particularly related to coal combustion and industrial productions, which should be given close concern to address the amine pollution.


Assuntos
Poluentes Atmosféricos , Material Particulado , Aerossóis/análise , Poluentes Atmosféricos/análise , Aminas , China , Carvão Mineral/análise , Monitoramento Ambiental , Cromatografia Gasosa-Espectrometria de Massas , Humanos , Material Particulado/análise , Estações do Ano , Emissões de Veículos/análise
20.
Environ Res ; 212(Pt A): 113182, 2022 09.
Artigo em Inglês | MEDLINE | ID: mdl-35367431

RESUMO

Particulate organic nitrates, among the major components of secondary organic aerosols and fine particles, play important roles in regional nitrogen cycle, ozone budget, and cloud condensation nuclei formation. However, the pollution characteristics of particulate organic nitrates at mountain areas and the effects of anthropogenic pollutant transport remain poorly understood. In this study, field sampling and measurements were conducted at a high-elevation mountain site over North China Plain in winter and spring. Total five kinds of particulate organic nitrates in fine particles were determined by ultra-high performance liquid chromatography-electrospray mass spectrometry. The average total concentrations of particulate organic nitrates were 330 ± 121 ng m-3 and 247 ± 63 ng m-3 in winter and spring. The monoterpene-derived organic nitrates were the dominant components in both seasons with their contribution higher than 70%, accounting for 1.2 ± 0.8% and 2.0 ± 1.0% in organic aerosols in winter and spring, respectively. The significantly higher levels of particulate organic nitrates in winter than spring was ascribed to the strong effects of mountain-valley breezes and coal combustion plumes. The increasing concentrations of NOx and particulate matters brought by the valley breeze at daytime facilitated the formation of MHN215, OAKN359, and OAHN361, while the rising SO2 abundance and the sulfate aerosols transported by elevated emission sources affected the formation of MDCN247 at nighttime.


Assuntos
Poluentes Atmosféricos , Aerossóis/análise , Poluentes Atmosféricos/análise , China , Carvão Mineral/análise , Poeira/análise , Monitoramento Ambiental , Nitratos/análise , Material Particulado/análise , Estações do Ano
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