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1.
J Virol ; : e0040924, 2024 Jun 13.
Artigo em Inglês | MEDLINE | ID: mdl-38869284

RESUMO

Aerosol transmission remains a major challenge for control of respiratory viruses, particularly those causing recurrent epidemics, like influenza A virus (IAV). These viruses are rarely expelled alone, but instead are embedded in a consortium of microorganisms that populate the respiratory tract. The impact of microbial communities and inter-pathogen interactions upon stability of transmitted viruses is well-characterized for enteric pathogens, but is under-studied in the respiratory niche. Here, we assessed whether the presence of five different species of commensal respiratory bacteria could influence the persistence of IAV within phosphate-buffered saline and artificial saliva droplets deposited on surfaces at typical indoor air humidity, and within airborne aerosol particles. In droplets, presence of individual species or a mixed bacterial community resulted in 10- to 100-fold more infectious IAV remaining after 1 h, due to bacterial-mediated flattening of drying droplets and early efflorescence. Even when no efflorescence occurred at high humidity or the bacteria-induced changes in droplet morphology were abolished by aerosolization instead of deposition on a well plate, the bacteria remained protective. Staphylococcus aureus and Streptococcus pneumoniae were the most stabilizing compared to other commensals at equivalent density, indicating the composition of an individual's respiratory microbiota is a previously unconsidered factor influencing expelled virus persistence.IMPORTANCEIt is known that respiratory infections such as coronavirus disease 2019 and influenza are transmitted by release of virus-containing aerosols and larger droplets by an infected host. The survival time of viruses expelled into the environment can vary depending on temperature, room air humidity, UV exposure, air composition, and suspending fluid. However, few studies consider the fact that respiratory viruses are not alone in the respiratory tract-we are constantly colonized by a plethora of bacteria in our noses, mouth, and lower respiratory system. In the gut, enteric viruses are known to be stabilized against inactivation and environmental decay by gut bacteria. Despite the presence of a similarly complex bacterial microbiota in the respiratory tract, few studies have investigated whether viral stabilization could occur in this niche. Here, we address this question by investigating influenza A virus stabilization by a range of commensal bacteria in systems representing respiratory aerosols and droplets.

2.
J Virol ; 97(10): e0127123, 2023 10 31.
Artigo em Inglês | MEDLINE | ID: mdl-37819131

RESUMO

IMPORTANCE: The respiratory tract of humans is constantly exposed to potentially harmful agents, such as small particles or pathogens, and thus requires protective measures. Respiratory mucus that lines the airway epithelia plays a major role in the prevention of viral infections by limiting the mobility of viruses, allowing subsequent mucociliary clearance. Understanding the interplay between respiratory mucus and viruses can help elucidate host and virus characteristics that enable the initiation of infection. Here, we tested a panel of primary influenza A viruses of avian or human origin for their sensitivity to mucus derived from primary human airway cultures and found that differences between virus strains can be mapped to viral neuraminidase activity. We also show that binding of influenza A viruses to decoy receptors on highly glycosylated mucus components constitutes the major inhibitory function of mucus against influenza A viruses.


Assuntos
Vírus da Influenza A , Influenza Humana , Muco , Neuraminidase , Animais , Humanos , Aves , Vírus da Influenza A/metabolismo , Muco/metabolismo , Neuraminidase/metabolismo , Sistema Respiratório/metabolismo
3.
Allergy ; 79(2): 294-301, 2024 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-37654007

RESUMO

While the number and types of indoor air pollutants is rising, much is suspected but little is known about the impact of their potentially synergistic interactions, upon human health. Gases, particulate matter, organic compounds but also allergens and viruses, fall within the 'pollutant' definition. Distinct populations, such as children and allergy and asthma sufferers are highly susceptible, while a low socioeconomic background is a further susceptibility factor; however, no specific guidance is available. We spend most of our time indoors; for children, the school environment is of paramount importance and potentially amenable to intervention. The interactions between some pollutant classes have been studied. However, a lot is missing with respect to understanding interactions between specific pollutants of different classes in terms of concentrations, timing and sequence, to improve targeting and upgrade standards. SynAir-G is a European Commission-funded project aiming to reveal and quantify synergistic interactions between different pollutants affecting health, from mechanisms to real life, focusing on the school setting. It will develop a comprehensive and responsive multipollutant monitoring system, advance environmentally friendly interventions, and disseminate the generated knowledge to relevant stakeholders in accessible and actionable formats. The aim of this article it to put forward the SynAir-G hypothesis, and describe its background and objectives.


Assuntos
Poluentes Atmosféricos , Poluição do Ar em Ambientes Fechados , Asma , Poluentes Ambientais , Criança , Humanos , Poluição do Ar em Ambientes Fechados/efeitos adversos , Poluentes Atmosféricos/efeitos adversos , Poluentes Atmosféricos/análise , Material Particulado , Asma/epidemiologia , Asma/etiologia , Monitoramento Ambiental
4.
Environ Sci Technol ; 58(4): 1986-1997, 2024 Jan 30.
Artigo em Inglês | MEDLINE | ID: mdl-38237915

RESUMO

Humans are the primary sources of CO2 and NH3 indoors. Their emission rates may be influenced by human physiological and psychological status. This study investigated the impact of physiological and psychological engagements on the human emissions of CO2 and NH3. In a climate chamber, we measured CO2 and NH3 emissions from participants performing physical activities (walking and running at metabolic rates of 2.5 and 5 met, respectively) and psychological stimuli (meditation and cognitive tasks). Participants' physiological responses were recorded, including the skin temperature, electrodermal activity (EDA), and heart rate, and then analyzed for their relationship with CO2 and NH3 emissions. The results showed that physiological engagement considerably elevated per-person CO2 emission rates from 19.6 (seated) to 46.9 (2.5 met) and 115.4 L/h (5 met) and NH3 emission rates from 2.7 to 5.1 and 8.3 mg/h, respectively. CO2 emissions reduced when participants stopped running, whereas NH3 emissions continued to increase owing to their distinct emission mechanisms. Psychological engagement did not significantly alter participants' emissions of CO2 and NH3. Regression analysis revealed that CO2 emissions were predominantly correlated with heart rate, whereas NH3 emissions were mainly associated with skin temperature and EDA. These findings contribute to a deeper understanding of human metabolic emissions of CO2 and NH3.


Assuntos
Amônia , Dióxido de Carbono , Humanos
5.
Environ Sci Technol ; 58(20): 8748-8759, 2024 May 21.
Artigo em Inglês | MEDLINE | ID: mdl-38709019

RESUMO

Sea spray aerosols (SSA) greatly affect the climate system by scattering solar radiation and acting as seeds for cloud droplet formation. The ecosystems in the Arctic Ocean are rapidly changing due to global warming, and the effects these changes have on the generation of SSA, and thereby clouds and fog formation in this region, are unknown. During the ship-based Arctic Century Expedition, we examined the dependency of forced SSA production on the biogeochemical characteristics of seawater using an on-board temperature-controlled aerosol generation chamber with a plunging jet system. Our results indicate that mainly seawater salinity and organic content influence the production and size distribution of SSA. However, we observed a 2-fold higher SSA production from waters with similar salinity collected north of 81°N compared to samples collected south of this latitude. This variability was not explained by phytoplankton and bacterial abundances or Chlorophyll-a concentration but by the presence of glucose in seawater. The synergic action of sea salt (essential component) and glucose or glucose-rich saccharides (enhancer) accounts for >80% of SSA predictability throughout the cruise. Our results suggest that besides wind speed and salinity, SSA production in Arctic waters is also affected by specific organics released by the microbiota.


Assuntos
Aerossóis , Glucose , Salinidade , Água do Mar , Regiões Árticas , Água do Mar/química , Glucose/metabolismo , Fitoplâncton
6.
Environ Sci Technol ; 57(1): 486-497, 2023 01 10.
Artigo em Inglês | MEDLINE | ID: mdl-36537693

RESUMO

Respiratory viruses, including influenza virus and SARS-CoV-2, are transmitted by the airborne route. Air filtration and ventilation mechanically reduce the concentration of airborne viruses and are necessary tools for disease mitigation. However, they ignore the potential impact of the chemical environment surrounding aerosolized viruses, which determines the aerosol pH. Atmospheric aerosol gravitates toward acidic pH, and enveloped viruses are prone to inactivation at strong acidity levels. Yet, the acidity of expiratory aerosol particles and its effect on airborne virus persistence have not been examined. Here, we combine pH-dependent inactivation rates of influenza A virus (IAV) and SARS-CoV-2 with microphysical properties of respiratory fluids using a biophysical aerosol model. We find that particles exhaled into indoor air (with relative humidity ≥ 50%) become mildly acidic (pH ∼ 4), rapidly inactivating IAV within minutes, whereas SARS-CoV-2 requires days. If indoor air is enriched with nonhazardous levels of nitric acid, aerosol pH drops by up to 2 units, decreasing 99%-inactivation times for both viruses in small aerosol particles to below 30 s. Conversely, unintentional removal of volatile acids from indoor air may elevate pH and prolong airborne virus persistence. The overlooked role of aerosol acidity has profound implications for virus transmission and mitigation strategies.


Assuntos
Poluição do Ar em Ambientes Fechados , COVID-19 , Aerossóis e Gotículas Respiratórios , Humanos , Concentração de Íons de Hidrogênio , SARS-CoV-2 , Inativação de Vírus , Transmissão de Doença Infecciosa
7.
Proc Natl Acad Sci U S A ; 117(52): 33028-33033, 2020 12 29.
Artigo em Inglês | MEDLINE | ID: mdl-33318218

RESUMO

Oxidized organic aerosol (OOA) is a major component of ambient particulate matter, substantially impacting climate, human health, and ecosystems. OOA is readily produced in the presence of sunlight, and requires days of photooxidation to reach the levels observed in the atmosphere. High concentrations of OOA are thus expected in the summer; however, our current mechanistic understanding fails to explain elevated OOA during wintertime periods of low photochemical activity that coincide with periods of intense biomass burning. As a result, atmospheric models underpredict OOA concentrations by a factor of 3 to 5. Here we show that fresh emissions from biomass burning exposed to NO2 and O3 (precursors to the NO3 radical) rapidly form OOA in the laboratory over a few hours and without any sunlight. The extent of oxidation is sensitive to relative humidity. The resulting OOA chemical composition is consistent with the observed OOA in field studies in major urban areas. Additionally, this dark chemical processing leads to significant enhancements in secondary nitrate aerosol, of which 50 to 60% is estimated to be organic. Simulations that include this understanding of dark chemical processing show that over 70% of organic aerosol from biomass burning is substantially influenced by dark oxidation. This rapid and extensive dark oxidation elevates the importance of nocturnal chemistry and biomass burning as a global source of OOA.


Assuntos
Poluentes Atmosféricos/química , Poluição do Ar/estatística & dados numéricos , Biomassa , Material Particulado/química , Aerossóis/química , Cidades , Modelos Teóricos , Dióxido de Nitrogênio/análise , Dióxido de Nitrogênio/química , Oxirredução , Oxigênio/química
8.
Environ Sci Technol ; 56(15): 10608-10618, 2022 08 02.
Artigo em Inglês | MEDLINE | ID: mdl-35786903

RESUMO

Particulate sulfate is one of the most important components in the atmosphere. The observation of rapid sulfate aerosol production during haze events provoked scientific interest in the multiphase oxidation of SO2 in aqueous aerosol particles. Diverse oxidation pathways can be enhanced or suppressed under different aerosol acidity levels and high ionic strength conditions of atmospheric aerosol. The importance of ionic strength to sulfate multiphase chemistry has been verified under laboratory conditions, though studies in the actual atmosphere are still limited. By utilizing online observations and developing an improved solute strength-dependent chemical thermodynamics and kinetics model (EF-T&K model, EF is the enhancement factor that represents the effect of ionic strength on an aerosol aqueous-phase reaction), we provided quantitative evidence that the H2O2 pathway was enhanced nearly 100 times and dominated sulfate formation for entire years (66%) in Tianjin (a northern city in China). TMI (oxygen catalyzed by transition-metal ions) (14%) and NO2 (14%) pathways got the second-highest contributions. Machine learning supported the result that aerosol sulfate production was more affected by the H2O2 pathway. The collaborative effects of atmospheric oxidants and SO2 on sulfate aerosol production were further investigated using the improved EF-T&K model. Our findings highlight the effectiveness of adopting target oxidant control as a new direction for sustainable mitigation of sulfate, given the already low SO2 concentrations in China.


Assuntos
Poluentes Atmosféricos , Material Particulado , Aerossóis/análise , Poluentes Atmosféricos/análise , China , Peróxido de Hidrogênio , Oxidantes , Material Particulado/análise , Sulfatos/análise , Sulfatos/química , Óxidos de Enxofre/análise , Óxidos de Enxofre/química , Água
9.
Environ Sci Technol ; 56(12): 7657-7667, 2022 06 21.
Artigo em Inglês | MEDLINE | ID: mdl-35544773

RESUMO

Fairbanks, Alaska, is a subarctic city with fine particle (PM2.5) concentrations that exceed air quality regulations in winter due to weak dispersion caused by strong atmospheric inversions, local emissions, and the unique chemistry occurring under the cold and dark conditions. Here, we report on observations from the winters of 2020 and 2021, motivated by our pilot study that showed exceptionally high concentrations of fine particle hydroxymethanesulfonate (HMS) or related sulfur(IV) species (e.g., sulfite and bisulfite). We deployed online particle-into-liquid sampler-ion chromatography (PILS-IC) in conjunction with a suite of instruments to determine HMS precursors (HCHO, SO2) and aerosol composition in general, with the goal to characterize the sources and sinks of HMS in wintertime Fairbanks. PM2.5 HMS comprised a significant fraction of PM2.5 sulfur (26-41%) and overall PM2.5 mass concentration of 2.8-6.8% during pollution episodes, substantially higher than what has been observed in other regions, likely due to the exceptionally low temperatures. HMS peaked in January, with lower concentrations in December and February, resulting from changes in precursors and meteorological conditions. Strong correlations with inorganic sulfate and organic mass during pollution events suggest that HMS is linked to processes responsible for poor air quality episodes. These findings demonstrate unique aspects of air pollution formation in cold and humid atmospheres.


Assuntos
Poluentes Atmosféricos , Poluição do Ar , Aerossóis/química , Poluentes Atmosféricos/análise , Poluição do Ar/análise , Alaska , Monitoramento Ambiental/métodos , Material Particulado/análise , Projetos Piloto , Estações do Ano , Enxofre
10.
Environ Sci Technol ; 56(11): 7163-7173, 2022 06 07.
Artigo em Inglês | MEDLINE | ID: mdl-35483018

RESUMO

The interaction between water vapor and atmospheric aerosol leads to enhancement in aerosol water content, which facilitates haze development, but its concentrations, sources, and impacts remain largely unknown in polluted urban environments. Here, we show that the Indian capital, Delhi, which tops the list of polluted capital cities, also experiences the highest aerosol water yet reported worldwide. This high aerosol water promotes secondary formation of aerosols and worsens air pollution. We report that severe pollution events are commonly associated with high aerosol water which enhances light scattering and reduces visibility by 70%. Strong light scattering also suppresses the boundary layer height on winter mornings in Delhi, inhibiting dispersal of pollutants and further exacerbating morning pollution peaks. We provide evidence that ammonium chloride is the largest contributor to aerosol water in Delhi, making up 40% on average, and we highlight that regulation of chlorine-containing precursors should be considered in mitigation strategies.


Assuntos
Poluentes Atmosféricos , Poluição do Ar , Aerossóis/análise , Poluentes Atmosféricos/análise , Poluição do Ar/análise , Cloreto de Amônio , China , Monitoramento Ambiental , Índia , Material Particulado/análise , Estações do Ano
11.
Environ Sci Technol ; 55(22): 15072-15081, 2021 11 16.
Artigo em Inglês | MEDLINE | ID: mdl-34709803

RESUMO

Air pollutant accumulations during wintertime persistent cold air pool (PCAP) events in mountain valleys are of great concern for public health worldwide. Uncertainties associated with the simulated meteorology under stable conditions over complex terrain hinder realistic simulations of air quality using chemical transport models. We use the Community Multiscale Air Quality (CMAQ) model to simulate the gaseous and particulate species for 1 month in January 2011 during the Persistent Cold Air Pool Study (PCAPS) in the Salt Lake Valley (SLV), Utah (USA). Results indicate that the temporal variability associated with the elevated NOx and PM2.5 concentrations during PCAP events was captured by the model (r = 0.20 for NOx and r = 0.49 for PM2.5). However, concentrations were not at the correct magnitude (NMB = -35/12% for PM2.5 during PCAPs/non-PCAPs), where PM2.5 was underestimated during PCAP events and overestimated during non-PCAP periods. The underestimated PCAP strength is represented by valley heat deficit, which contributed to the underestimated PM2.5 concentrations compared with observations due to the model simulating more vertical mixing and less stable stratification than what was observed. Based on the observations, the dominant PM2.5 species were ammonium and nitrate. We provide a discussion that aims to investigate the emissions and chemistry model uncertainties using the nitrogen ratio method and the thermodynamic ammonium nitrate regime method.


Assuntos
Poluentes Atmosféricos , Poluição do Ar , Poluentes Atmosféricos/análise , Poluição do Ar/análise , Monitoramento Ambiental , Lagos , Material Particulado/análise , Utah
12.
Environ Sci Technol ; 55(11): 7307-7315, 2021 06 01.
Artigo em Inglês | MEDLINE | ID: mdl-34000801

RESUMO

Acidity profoundly affects almost every aspect that shapes the composition of ambient particles and their environmental impact. Thermodynamic analysis of gas-particle composition datasets offers robust estimates of acidity, but they are not available for long periods of time. Fog composition datasets, however, are available for many decades; we develop a thermodynamic analysis to estimate the ammonia in equilibrium with fog water and to infer the pre-fog aerosol pH starting from fog chemical composition and pH. The acidity values from the new method agree with the results of thermodynamic analysis of the available gas-particle composition data. Applying the new method to historical (25 years) fog water composition at the rural station of San Pietro Capofiume (SPC) in the Po Valley (Italy) suggests that the aerosol has been mildly acidic, with its pH decreasing by 0.5-1.5 pH units over the last decades. The observed pH of the fog water also increased 1 unit over the same period. Analysis of the simulated aerosol pH reveals that the aerosol acidity trend is driven by a decrease in aerosol precursor concentrations, and changes in temperature and relative humidity. Currently, NOx controls would be most effective for PM2.5 reduction in the Po valley both during summer and winter. In the future, however, seasonal transitions to the NH3-sensitive region may occur, meaning that the NH3 reduction policy may become increasingly necessary.


Assuntos
Poluentes Atmosféricos , Material Particulado , Aerossóis/análise , Poluentes Atmosféricos/análise , Itália , Material Particulado/análise , Estações do Ano , Água
13.
Environ Sci Technol ; 54(16): 9834-9843, 2020 08 18.
Artigo em Inglês | MEDLINE | ID: mdl-32677824

RESUMO

Ammonium is one of the dominant inorganic water-soluble ions in fine particulate matter (PM2.5). In this study, source apportionment and thermodynamic equilibrium models were used to analyze the relationship between pH and the partitioning of ammonium (ε(NH4+)) using hourly ambient samples collected from Tianjin, China. We found a "Reversed-S curve" between pH and ε(NH4+) from the ambient hourly aerosol dataset when the theoretical ε(NO3-)* (an index identified in this work) was within specific ranges. A Boltzmann function was then used to fit the Reversed-S curve. For the summer data set, when ε(NO3-)* was between 0.7 and 0.8, the fitted R2 was 0.88. Through thermodynamic analysis, we found that the values of k[H+]2 (k = 3.08 × 104 L2 mol-2) and ε(NO3-)* can influence the pH-ε(NH4+) curve. Under certain situations, the values of k[H+]2 and ε(NO3-)* are similar to each other, and ε(NH4+) is sensitive to pH, suggesting that ε(NO3-)* plays an important role in affecting the ε(NH4+). During summer, winter, and spring seasons, when the relative humidity was greater than 0.36 and ε(NO3-)* was between 0.8 and 0.95, there was an obvious Reversed-S curve, with R2 = 0.60. The theoretical k[H+]2 and ε(NO3-)* developed in this work can be used to analyze the gas-particle partitioning of ammonia-ammonium and nitrate-nitric acid in the ambient atmosphere. Also, it is the first time that we created the joint source-NH3/HNO3 maps to integrate sources, aerosol pH and liquid water content, and ions (altogether in one map), which can provide useful information for designing effective strategies to control particulate matter pollution.


Assuntos
Poluentes Atmosféricos , Compostos de Amônio , Aerossóis/análise , Poluentes Atmosféricos/análise , China , Monitoramento Ambiental , Tamanho da Partícula , Material Particulado/análise , Estações do Ano
14.
Environ Sci Technol ; 54(12): 7088-7096, 2020 06 16.
Artigo em Inglês | MEDLINE | ID: mdl-32391689

RESUMO

Transition metal ions, such as water-soluble iron (WS-Fe), are toxic components of fine particles (PM2.5). In Atlanta, from 1998 to 2013, a previous study found that WS-Fe was the PM2.5 species most associated with adverse cardiovascular outcomes. We examined this data set to investigate the sources of WS-Fe and the effects of air quality regulations on ambient levels of WS-Fe. We find that insoluble forms of iron in mineral and road dust combined with sulfate from coal-fired electrical generating units were converted into soluble forms by sulfate-driven acid dissolution. Sulfate produced both the highly acidic aerosol (summer pH 1.5-2) and liquid water required for the aqueous phase acid dissolution, but variability in WS-Fe was mainly driven by particle liquid water. These processes were more pronounced in summer when particles were most acidic, whereas in winter the relative importance of WS-Fe from combustion emissions increased. Although WS-Fe constituted a minute fraction of PM2.5 mass (0.15%), the WS-Fe-PM2.5 mass correlation was high (r = 0.67) and may be explained by these formation routes, which, in part, could account for observed associations between PM2.5 mass and adverse health seen in past studies. Similar processes are expected in many regions, implying that these unexpected benefits from coal-burning reduction may be widespread.


Assuntos
Poluentes Atmosféricos , Poeira , Poluentes Atmosféricos/análise , Carvão Mineral/análise , Poeira/análise , Monitoramento Ambiental , Ferro , Tamanho da Partícula , Material Particulado/análise , Centrais Elétricas , Solo , Enxofre
16.
Environ Sci Technol ; 53(12): 6747-6756, 2019 06 18.
Artigo em Inglês | MEDLINE | ID: mdl-31091086

RESUMO

Oxidative potential (OP), which is the ability of certain components in atmospheric particles to generate reactive oxidative species (ROS) and deplete antioxidants in vivo, is a prevailing toxicological mechanism underlying the adverse health effects associated with exposure to ambient aerosols. While previous studies have identified the high OP of fresh biomass burning organic aerosols (BBOA), it remains unclear how it evolves throughout atmospheric transport. Using the dithiothreitol (DTT) assay as a measure of OP, a combination of field observations and laboratory experiments is used to determine how atmospheric aging transforms the intrinsic OP (OPmassDTT) of BBOA. For ambient BBOA collected during the fire seasons in Greece, OPmassDTT was observed to increase by a factor of 2.1 ± 0.9 for samples of atmospheric ages up to 68 h. Laboratory experiments indicate that aqueous photochemical aging (aging by UVB and UVA photolysis; as well as OH oxidation), as well as aging by ozone and atmospheric dilution can transform the OPmassDTT of the water-soluble fraction of wood smoke within 2 days of atmospheric transport. The results from this work suggest that the air quality impacts of biomass burning emissions can extend beyond regions near fire sites and should be accounted for.


Assuntos
Poluentes Atmosféricos , Material Particulado , Aerossóis , Biomassa , Grécia , Estresse Oxidativo
17.
Environ Sci Technol ; 53(6): 3048-3057, 2019 03 19.
Artigo em Inglês | MEDLINE | ID: mdl-30793889

RESUMO

Nitrate is one of the most abundant inorganic water-soluble ions in fine particulate matter (PM2.5). However, the formation mechanism of nitrate in the ambient atmosphere, especially the impacts of its semivolatility and the various existing forms of nitrogen, remain under-investigated. In this study, hourly ambient observations of speciated PM2.5 components (NO3-, SO42-, etc.) were collected in Tianjin, China. Source contributions were analyzed by PMF/ME2 (Positive Matrix Factorization using the Multilinear Engine 2) program, and pH were estimated by ISORROPIA-II, to investigate the relationship between pH and nitrate. Five sources (factors) were resolved: secondary sulfate (SS), secondary nitrate (SN), dust, vehicle and coal combustion. SN and pH showed a triangle-shaped relationship. When SS was high, the fraction of nitrate partitioning into the aerosol phase exhibits a characteristic "S-curve" relationship with pH for different seasons. An index ( ITL) is developed and combined with pH to explore the sensitive regions of "S-curve". Controlling the emissions of anions (SO42-, Cl-), cations (Ca2+, Mg2+, etc.) and gases (NO x, NH3, SO2, etc.) will change pH, potentially reducing or increasing SN. The findings of this work provide an effective approach for exploring the formation mechanisms of nitrate under different influencing factors (sources, pH, and IRL).


Assuntos
Poluentes Atmosféricos , China , Monitoramento Ambiental , Gases , Material Particulado
18.
Environ Sci Technol ; 53(15): 8903-8913, 2019 Aug 06.
Artigo em Inglês | MEDLINE | ID: mdl-31294542

RESUMO

In this work, we utilize a rich set of simulated and ground-based observational data in Tianjin, China to examine and compare the differences in aerosol acidity and composition predicted by three popular thermodynamic equilibrium models: ISORROPIA II, the Extended Aerosol Inorganics Model vision IV (E-AIM IV), and the Aerosol Inorganic-Organic Mixtures Functional groups Activity Coefficients model (AIOMFAC). The species used to estimate aerosol acidity for both simulated and ambient data were NH4+, Na+, SO42-, NO3-, and Cl-. For simulated data, there is good agreement between ISORROPIA II and E-AIM IV predicted acidity in the forward and metastable mode, resulting from the hydrogen ion activity coefficient (γ(H+)) and the molality (m(H+)) showing opposite trends. While almost all other inorganic species concentrations are found to be similar among the three models, such is not the case for the bisulfate ion (HSO4-), which is linked to m(H+). We find that differences in predicted bisulfate between the three models primarily result from differences in the treatment of the HSO4- ↔ H+ + SO42- reaction for highly acidic conditions. This difference in bisulfate is responsible for much of the difference in estimated pH for the ambient data (average pH of 3.5 for ISORROPIA II and 3.0 for E-AIM IV).


Assuntos
Poluentes Atmosféricos , Material Particulado , Aerossóis , China , Monitoramento Ambiental , Concentração de Íons de Hidrogênio , Termodinâmica
20.
Proc Natl Acad Sci U S A ; 113(21): 5791-6, 2016 May 24.
Artigo em Inglês | MEDLINE | ID: mdl-27185952

RESUMO

Understanding how dynamical and aerosol inputs affect the temporal variability of hydrometeor formation in climate models will help to explain sources of model diversity in cloud forcing, to provide robust comparisons with data, and, ultimately, to reduce the uncertainty in estimates of the aerosol indirect effect. This variability attribution can be done at various spatial and temporal resolutions with metrics derived from online adjoint sensitivities of droplet and crystal number to relevant inputs. Such metrics are defined and calculated from simulations using the NASA Goddard Earth Observing System Model, Version 5 (GEOS-5) and the National Center for Atmospheric Research Community Atmosphere Model Version 5.1 (CAM5.1). Input updraft velocity fluctuations can explain as much as 48% of temporal variability in output ice crystal number and 61% in droplet number in GEOS-5 and up to 89% of temporal variability in output ice crystal number in CAM5.1. In both models, this vertical velocity attribution depends strongly on altitude. Despite its importance for hydrometeor formation, simulated vertical velocity distributions are rarely evaluated against observations due to the sparsity of relevant data. Coordinated effort by the atmospheric community to develop more consistent, observationally based updraft treatments will help to close this knowledge gap.

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