RESUMO
Monolithic aerogels are promising candidates for use in atmospheric environmental purification due to their structural advantages, such as fine building block size together with high specific surface area, abundant pore structure, etc. Additionally, monolithic aerogels possess a unique monolithic macrostructure that sets them apart from aerogel powders and nanoparticles in practical environmental clean-up applications. This review delves into the available synthesis strategies and atmospheric environmental applications of monolithic aerogels, covering types of monolithic aerogels including SiO2, graphene, metal oxides and their combinations, along with their preparation methods. In particular, recent developments for VOC adsorption, CO2 capture, catalytic oxidation of VOCs and catalytic reduction of CO2 are highlighted. Finally, challenges and future opportunities for monolithic aerogels in the atmospheric environmental purification field are proposed. This review provides valuable insights for designing and utilizing monolithic aerogel-based functional materials.
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Poluentes Atmosféricos , Géis , Poluentes Atmosféricos/química , Géis/química , Atmosfera/química , Adsorção , Dióxido de Carbono/química , Recuperação e Remediação Ambiental/métodos , Dióxido de Silício/químicaRESUMO
The acidity of atmospheric aerosols influences fundamental physicochemical processes that affect climate and human health. We recently developed a novel and facile water-probe-based method for directly measuring of the pH for micrometer-size droplets, providing a promising technique to better understand aerosol acidity in the atmosphere. The complex chemical composition of fine particles in the ambient air, however, poses certain challenges to using a water-probe for pH measurement, including interference from interactions between compositions and the influence of similar compositions on water structure. To explore the universality of our method, it was employed to measure the pH of ammonium, nitrate, carbonate, sulfate, and chloride particles. The pH of particles covering a broad range (0-14) were accurately determined, thereby demonstrating that our method can be generally applied, even to alkaline particles. Furthermore, a standard spectral library was developed by integrating the standard spectra of common hydrated ions extracted through the water-probe. The library can be employed to identify particle composition and overcome the spectral overlap problem resulting from similar effects. Using the spectral library, all ions were identified and their concentrations were determined, in turn allowing successful pH measurement of multicomponent (ammonium-sulfate-nitrate-chloride) particles. Insights into the synergistic effect of Cl-, NO3-, and NH4+ depletion obtained with our approach revealed the interplay between pH and volatile partitioning. Given the ubiquity of component partitioning and pH variation in particles, the water probe may provide a new perspective on the underlying mechanisms of aerosol aging and aerosol-cloud interaction.
Assuntos
Aerossóis , Monitoramento Ambiental , Análise Espectral Raman , Água , Concentração de Íons de Hidrogênio , Análise Espectral Raman/métodos , Água/química , Monitoramento Ambiental/métodos , Aerossóis/análise , Poluentes Atmosféricos/análise , Poluentes Atmosféricos/química , Atmosfera/química , Material Particulado/análiseRESUMO
A novel system for measuring net photochemical ozone production rates in the atmosphere based on cavity ring-down spectroscopy (OPR-CRDS) was developed. The system consists of two chambers (a reaction chamber and a reference chamber) and a dual-channel Ox-CRDS detector. To minimize the wall loss of Ox in the chambers, the inner surfaces of both chambers are coated with Teflon film. The performance of the OPR-CRDS system was characterized. It was found that even though the photolysis frequency (J value) decreased by 10%, the decrease in the P(O3) caused by the ultraviolet-blocking film coating was less than 3%. The two chambers had a good consistency in the mean residence time and the measurement of NO2 and Ox under the condition of no sunlight. The detection limit of the OPR-CRDS was determined to be 0.20 ppbv/hr. To further verify the accuracy of the system, the direct measurement values of the OPR-CRDS system were compared with the calculation results based on radical (OH, HO2, and RO2) reactions, and a good correlation was obtained between the measured and calculated values. Finally, the developed instrument was applied to obtain the comprehensive field observations at an urban site in the Yangtze River Delta (China) for 40 days, the time series and change characteristics of the P(O3) were obtained directly, and the good environmental adaptability and stability of the OPR-CRDS system were demonstrated. It is expected that the new instrument will be beneficial to investigations of the relationship between P(O3) and its precursors.
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Poluentes Atmosféricos , Monitoramento Ambiental , Ozônio , Ozônio/análise , Monitoramento Ambiental/métodos , Monitoramento Ambiental/instrumentação , Poluentes Atmosféricos/análise , Análise Espectral/métodos , China , Atmosfera/química , FotóliseRESUMO
Nitrogen-containing organic compounds (NOCs) may potentially contribute to aqueous secondary organic aerosols, yet the different formation of NOCs in aerosol particles and cloud droplets remains unclear. With the in-situ measurements performed at a mountain site (1690 m a.s.l.) in southern China, we investigated the formation of NOCs in the cloud droplets and the cloud-free particles, based on their mixing state information of NOCs-containing particles by single particle mass spectrometry. The relative abundance of NOCs in the cloud-free particles was significantly higher than those in cloud residual (cloud RES) particles. NOCs were highly correlated with carbonyl compounds (including glyoxalate and methylglyoxal) in the cloud-free particles, however, limited correlation was observed for cloud RES particles. Analysis of their mixing state and temporal variations highlights that NOCs was mainly formed from the carbonyl compounds and ammonium in the cloud-free particles, rather than in the cloud RES particles. The results support that the formation of NOCs from carbonyl compounds is facilitated in concentrated solutions in wet aerosols, rather than cloud droplets. In addition, we have identified the transport of biomass burning particles that facilitate the formation of NOCs, and that the observed NOCs is most likely contributed to the light absorption. These findings have implications for the evaluation of NOCs formation and their contribution to light absorption.
Assuntos
Aerossóis , Poluentes Atmosféricos , Monitoramento Ambiental , Nitrogênio , Compostos Orgânicos , Aerossóis/análise , Poluentes Atmosféricos/análise , Poluentes Atmosféricos/química , Nitrogênio/química , Nitrogênio/análise , Compostos Orgânicos/química , China , Atmosfera/química , Material Particulado/análise , Material Particulado/químicaRESUMO
Formic and acetic acids are the most abundant gaseous organic acids and play the key role in the atmospheric chemistry. In iodine-adduct chemical ionization mass spectrometry (CIMS), the low utilization efficiency of methyl iodide and humidity interference are two major issues of the vacuum ultraviolet (VUV) lamp initiated CIMS for on-line gaseous formic and acetic acids analysis. In this work, we present a new CIMS based on VUV lamp, and the ion-molecular reactor is separated into photoionization and chemical ionization zones by a reducer electrode. Acetone was added to the photoionization zone, and the VUV photoionization acetone provided low-energy electrons for methyl iodide to generate I-, and the addition of acetone reduced the amount of methyl iodide by 2/3. In the chemical ionization zone, a headspace vial containing ultrapure water was added for humidity calibration, and the vial changes the sensitivity as a function of humidity from ambiguity to well linear correlation (R2 > 0.95). With humidity calibration, the CIMS can quantitatively measure formic and acetic acids in the humidity range of 0%-88% RH. In this mode, limits of detection of 10 and 50 pptv are obtained for formic and acetic acids, respectively. And the relative standard deviation (RSD) of quantitation stability for 6 days were less than 10.5%. This CIMS was successfully used to determine the formic and acetic acids in the underground parking and ambient environment of the Shandong University campus (Qingdao, China). In addition, we developed a simple model based formic acid concentration to assess vehicular emissions.
Assuntos
Espectrometria de Massas , Espectrometria de Massas/métodos , Poluentes Atmosféricos/análise , Iodetos/análise , Iodetos/química , Raios Ultravioleta , Formiatos/análise , Formiatos/química , Atmosfera/química , Monitoramento Ambiental/métodos , Processos Fotoquímicos , Ácido Acético/análise , Ácido Acético/química , Hidrocarbonetos Iodados/análise , Hidrocarbonetos Iodados/químicaRESUMO
The formation of oligomeric hydrogen peroxide triggered by Criegee intermediate maybe contributes significantly to the formation and growth of secondary organic aerosol (SOA). However, to date, the reactivity of C2 Criegee intermediates (CH3CHOO) in areas contaminated with acidic gas remains poorly understood. Herein, high-level quantum chemical calculations and Born-Oppenheimer molecular dynamics (BOMD) simulations are used to explore the reaction of CH3CHOO and H2SO4 both in the gas phase and at the air-water interface. In the gas phase, the addition reaction of CH3CHOO with H2SO4 to generate CH3HC(OOH)OSO3H (HPES) is near-barrierless, regardless of the presence of water molecules. BOMD simulations show that the reaction at the air-water interface is even faster than that in the gas phase. Further calculations reveal that the HPES has a tendency to aggregate with sulfuric acids, ammonias, and water molecules to form stable clusters, meanwhile the oligomerization reaction of CH3CHOO with HPES in the gas phase is both thermochemically and kinetically favored. Also, it is noted that the interfacial HPES- ion can attract H2SO4, NH3, (COOH)2 and HNO3 for particle formation from the gas phase to the water surface. Thus, the results of this work not only elucidate the high atmospheric reactivity of C2 Criegee intermediates in polluted regions, but also deepen our understanding of the formation process of atmospheric SOA induced by Criegee intermediates.
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Ácidos Sulfúricos , Ácidos Sulfúricos/química , Aerossóis , Modelos Químicos , Poluentes Atmosféricos/química , Simulação de Dinâmica Molecular , Atmosfera/químicaRESUMO
The chemistry of sulfur cycle contributes significantly to the atmospheric nucleation process, which is the first step of new particle formation (NPF). In the present study, cycloaddition reaction mechanism of sulfur trioxide (SO3) to hydrogen sulfide (H2S) which is a typical air pollutant and toxic gas detrimental to the environment were comprehensively investigate through theoretical calculations and Atmospheric Cluster Dynamic Code simulations. Gas-phase stability and nucleation potential of the product thiosulfuric acid (H2S2O3, TSA) were further analyzed to evaluate its atmospheric impact. Without any catalysts, the H2S + SO3 reaction is infeasible with a barrier of 24.2 kcal/mol. Atmospheric nucleation precursors formic acid (FA), sulfuric acid (SA), and water (H2O) could effectively lower the reaction barriers as catalysts, even to a barrierless reaction with the efficiency of cis-SA > trans-FA > trans-SA > H2O. Subsequently, the gas-phase stability of TSA was investigated. A hydrolysis reaction barrier of up to 61.4 kcal/mol alone with an endothermic isomerization reaction barrier of 5.1 kcal/mol under the catalytic effect of SA demonstrates the sufficient stability of TSA. Furthermore, topological and kinetic analysis were conducted to determine the nucleation potential of TSA. Atmospheric clusters formed by TSA and atmospheric nucleation precursors (SA, ammonia NH3, and dimethylamine DMA) were thermodynamically stable. Moreover, the gradually decreasing evaporation coefficients for TSA-base clusters, particularly for TSA-DMA, suggests that TSA may participate in NPF where the concentration of base molecules are relatively higher. The present new reaction mechanism may contributes to a better understanding of atmospheric sulfur cycle and NPF.
Assuntos
Poluentes Atmosféricos , Sulfeto de Hidrogênio , Modelos Químicos , Sulfeto de Hidrogênio/química , Poluentes Atmosféricos/química , Reação de Cicloadição , Atmosfera/química , Óxidos de Enxofre/química , Cinética , Enxofre/químicaRESUMO
To explore air contamination resulting from special biomass combustion and suspended dust in Lhasa, the present study focused on the size distribution and chemical characteristics of particulate matter (PM) emission resulting from 7 types of non-fossil pollution sources. We investigated the concentration and size distribution of trace elements from 7 pollution sources collected in Lhasa. Combining Lhasa's atmospheric particulate matter data, enrichment factors (EFs) have been calculated to examine the potential impact of those pollution sources on the atmosphere quality of Lhasa. The highest mass concentration of total elements of biomass combustion appeared at PM0.4, and the second highest concentration existed in the size fraction 0.4-1 µm; the higher proportion (12 %) of toxic metals was produced by biomass combustion. The elemental composition of suspended dust and atmospheric particulate matter was close (except for As and Cd); the highest concentration of elements was all noted in PM2.5-10 (PM3-10). Potassium was found to be one of the main biomass markers. The proportion of Cu in suspended dust is significantly lower than that of atmospheric particulate matter (0.53 % and 3.75 %), which indicates that there are other anthropogenic sources. The EFs analysis showed that the Cr, Cu, Zn, and Pb produced by biomass combustion were highly enriched (EFs > 100) in all particle sizes. The EFs of most trace elements increased with decreasing particle size, indicating the greater influence of humanfactors on smaller particles.
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Aerossóis , Poluentes Atmosféricos , Poeira , Monitoramento Ambiental , Tamanho da Partícula , Material Particulado , Poluentes Atmosféricos/análise , Aerossóis/análise , Material Particulado/análise , Poeira/análise , Oligoelementos/análise , Poluição do Ar/estatística & dados numéricos , Poluição do Ar/análise , China , Atmosfera/químicaRESUMO
Airborne microplastics (MPs) are important pollutants that have been present in the environment for many years and are characterized by their universality, persistence, and potential toxicity. This study investigated the effects of terrestrial and marine transport of MPs in the atmosphere of a coastal city and compared the difference between daytime and nighttime. Laser direct infrared imaging (LDIR) and polarized light microscopy were used to characterize the physical and chemical properties of MPs, including number concentration, chemical types, shape, and size. Backward trajectories were used to distinguish the air masses from marine and terrestrial transport. Twenty chemical types were detected by LDIR, with rubber (16.7%) and phenol-formaldehyde resin (PFR; 14.8%) being major components. Three main morphological types of MPs were identified, and fragments (78.1%) are the dominant type. MPs in the atmosphere were concentrated in the small particle size segment (20-50 µm). The concentration of MPs in the air mass from marine transport was 14.7 items/m3 - lower than that from terrestrial transport (32.0 items/m3). The number concentration of airborne MPs was negatively correlated with relative humidity. MPs from terrestrial transport were mainly rubber (20.2%), while those from marine transport were mainly PFR (18%). MPs in the marine transport air mass were more aged and had a lower number concentration than those in the terrestrial transport air mass. The number concentration of airborne MPs is higher during the day than at night. These findings could contribute to the development of targeted control measures and methods to reduce MP pollution.
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Poluentes Atmosféricos , Monitoramento Ambiental , Microplásticos , China , Microplásticos/análise , Poluentes Atmosféricos/análise , Cidades , Atmosfera/química , Tamanho da PartículaRESUMO
Heterogeneous oxidation by gas-phase oxidants is an important chemical transformation pathway of secondary organic aerosol (SOA) and plays an important role in controlling the abundance, properties, as well as climate and health impacts of aerosols. However, our knowledge on this heterogeneous chemistry remains inadequate. In this study, the heterogeneous oxidation of α-pinene ozonolysis SOA by hydroxyl (OH) radicals was investigated under both low and high relative humidity (RH) conditions, with an emphasis on the evolution of molecular composition of SOA and its RH dependence. It is found that the heterogeneous oxidation of SOA at an OH exposure level equivalent to 12 hr of atmospheric aging leads to particle mass loss of 60% at 25% RH and 95% at 90% RH. The heterogeneous oxidation strongly changes the molecular composition of SOA. The dimer-to-monomer signal ratios increase dramatically with rising OH exposure, in particular under high RH conditions, suggesting that aerosol water stimulates the reaction of monomers with OH radicals more than that of dimers. In addition, the typical SOA tracer compounds such as pinic acid, pinonic acid, hydroxy pinonic acid and dimer esters (e.g., C17H26O8 and C19H28O7) have lifetimes of several hours against heterogeneous OH oxidation under typical atmospheric conditions, which highlights the need for the consideration of their heterogeneous loss in the estimation of monoterpene SOA concentrations using tracer-based methods. Our study sheds lights on the heterogeneous oxidation chemistry of monoterpene SOA and would help to understand their evolution and impacts in the atmosphere.
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Aerossóis , Poluentes Atmosféricos , Monoterpenos Bicíclicos , Umidade , Radical Hidroxila , Oxirredução , Aerossóis/química , Radical Hidroxila/química , Monoterpenos Bicíclicos/química , Poluentes Atmosféricos/química , Poluentes Atmosféricos/análise , Ozônio/química , Modelos Químicos , Atmosfera/química , Monoterpenos/químicaRESUMO
As an important component of secondary aerosols, sulfate plays a crucial role in regulating atmospheric radiative balance and influencing the secondary formation of ozone (O3). In real atmosphere, atmospheric oxidants NO2 and O3 can promote the oxidation of SO2 to form sulfate (SO42-) through multiphase chemistry that occur at different time scales. Due to the combined impact of meteorology, pollution sources, atmospheric chemistry, etc., time-scale dependence of SO2-SO42- conversion makes the impact of NO2/O3 on it more complex. In this study, based on long-term time series (2013-2020) of air pollution variables from seven stations in Hong Kong, the Multifractal Detrended Cross-Correlation Analysis (MFDCCA) method has been employed to quantify the cross-correlations between SO2 and SO42- in real atmosphere at different time scales, for examining the time-scale dependence of SO2-SO42- conversion efficiency. Furthermore, the Pearson correlation analysis has been used to study the influence of NO2/O3 on SO2-SO42- conversion, and the regional and seasonal differences have been analyzed by considering factors such as meteorology, pollution sources, and regional transport. Changes in the main components of secondary aerosols are closely linked with the co-control of regional PM2.5 and O3. Therefore, the exploration of the impact of co-existing NO2/O3 gases on the secondary formation of sulfates in real atmosphere is significant.
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Poluentes Atmosféricos , Atmosfera , Monitoramento Ambiental , Dióxido de Nitrogênio , Ozônio , Sulfatos , Ozônio/química , Sulfatos/química , Sulfatos/análise , Atmosfera/química , Poluentes Atmosféricos/análise , Dióxido de Nitrogênio/análise , Hong Kong , Aerossóis/análise , Poluição do Ar/estatística & dados numéricos , Dióxido de Enxofre/análise , Dióxido de Enxofre/químicaRESUMO
Benzene, toluene, ethylbenzene, and xylene (BTEX) pollution poses a serious threat to public health and the environment because of its respiratory and neurological effects, carcinogenic properties, and adverse effects on air quality. BTEX exposure is a matter of grave concern in India owing to the growing vehicular and development activities, necessitating the assessment of atmospheric concentrations and their spatial variation. This paper presents a comprehensive assessment of ambient concentrations and spatiotemporal variations of BTEX in India. The study investigates the correlation of BTEX with other criteria pollutants and meteorological parameters, aiming to identify interrelationships and diagnostic indicators for the source characterization of BTEX emissions. Additionally, the paper categorizes various regions in India according to the Air Quality Index (AQI) based on BTEX pollution levels. The results reveal that the northern zone of India exhibits the highest levels of BTEX pollution compared to central, eastern, and western regions. In contrast, the southern zone experiences the least pollution with BTEX. Seasonal analysis indicates that winter and post-monsoon periods, characterized by lower temperatures, are associated with higher BTEX levels due to the accumulation of localized emissions. When comparing the different zones in India, high traffic emissions and localized activities, such as solvent use and solvent evaporation, are found to be the primary sources of BTEX. The findings of the current study aid in source characterization and identification, and better understanding of the region's air quality problems, which helps in the development of focused BTEX pollution reduction and control strategies.
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Poluentes Atmosféricos , Derivados de Benzeno , Benzeno , Monitoramento Ambiental , Tolueno , Xilenos , Índia , Poluentes Atmosféricos/análise , Xilenos/análise , Derivados de Benzeno/análise , Tolueno/análise , Benzeno/análise , Poluição do Ar/estatística & dados numéricos , Poluição do Ar/análise , Estações do Ano , Atmosfera/químicaRESUMO
This study has employed the master chemical mechanism (MCM) to investigate the influence of the ozone oxidation pathways in the atmospheric formation of H2SO4 from short-chain olefins in industrialized areas. In-situ H2SO4 formation data were obtained using a high-resolution chemical ionization time-of-flight mass spectrometer, and the simulated H2SO4 concentrations calculated using updated parameters for the MCM model exhibited good agreement with observations. In the simulation analysis of different reaction pathways involved in H2SO4 formation, hydroxyl radicals were found to dominate H2SO4 production during the daytime, while olefin ozone oxidation contributed up to 65% of total H2SO4 production during the night-time. A sensitivity analysis of the H2SO4 production parameters has revealed a high sensitivity to changes in sulfur dioxide, and a relatively high sensitivity to olefins with fast ozonolysis reaction rates and bimolecular reaction rates of resulting stabilized Criegee Intermediates. A high relative humidity promotes daytime H2SO4 formation, but has an inhibiting effect during the night-time due to the different dominant reaction pathways.
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Poluentes Atmosféricos , Alcenos , Oxirredução , Ozônio , Ácidos Sulfúricos , Ozônio/química , Alcenos/química , Ácidos Sulfúricos/química , Poluentes Atmosféricos/química , Atmosfera/química , Modelos Químicos , Dióxido de Enxofre/química , Monitoramento AmbientalRESUMO
Nitrogen oxides (NOx) are crucial in tropospheric photochemical ozone (O3) production and oxidation capacity. Currently, the widely used NOx measurement technique is chemiluminescence (CL) (CL-NOx), which tends to overestimate NO2 due to atmospheric oxidation products of NOx (i.e., NOz). We developed and characterized a NOx measurement system using the cavity attenuated phase shift (CAPS) technique (CAPS-NOx), which is free from interferences with nitrogen-containing species. The NOx measured by the CAPS-NOx and CL-NOx analyzers were compared. Results show that both analyzers showed consistent measurement results for NO, but the NO2 measured by the CAPS-NOx analyzer (NO2_CAPS) was mostly lower than that measured by the CL-NOx analyzer (NO2_CL), which led to the deviations in O3 formation sensitivity regime and Ox (= O3 + NO2) sources (i.e., regional background and photochemically produced Ox) determined by the ozone production efficiencies (OPE) calculated from NO2_CL and NO2_CAPS. Overall, OPE_CL exceeded OPE_CAPS by 18.9%, which shifted 3 out of 13 observation days from the VOCs-limited to the transition regime when judging using OPE_CL, as compared to calculations using OPE_CAPS. During the observation period, days dominated by regional background Ox accounted for 46% and 62% when determined using NO2_CL and NO2_CAPS, respectively. These findings suggest that the use of the CL-NOx analyzer tends to underestimate both the VOCs-limited regime and the regional background Ox dominated days. The newly built CAPS-NOx analyzer here can promote the accurate measurement of NO2, which is meaningful for diagnosing O3 formation regimes and Ox sources.
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Poluentes Atmosféricos , Monitoramento Ambiental , Óxidos de Nitrogênio , Ozônio , Óxidos de Nitrogênio/análise , Poluentes Atmosféricos/análise , Monitoramento Ambiental/métodos , Monitoramento Ambiental/instrumentação , Ozônio/análise , Atmosfera/químicaRESUMO
Suspended atmospheric microplastics (SAMPs) display varying occurrence characteristics on different underlying surfaces in urban areas. This study investigated the occurrence characteristics, source apportionment, and transportation patterns of SAMPs in two typical underlying surfaces: the downtown area (Site T) and the industrial area (Site C) of a coastal city in China. In the spring of 2023, a total of 32 types comprising 1325 SAMPs were detected. The average MP abundances were found to be 3.74 ± 2.86 n/m3 in Site T and 2.67 ± 1.68 n/m3 in Site C. In Site T, SAMPs attributed to living source constituted 78.05%, while industry was the main source in Site C with a proportion reaching 42.89%, consistent with the functional zoning of the underlying surface. Furthermore, HYSPLIT analysis revealed that there was no significant difference between these two sites in long-distance horizontal transport affected by external airflow regardless of altitude; conversely, PCA indicated a notable correlation between vertical velocity and both abundance and species diversity. According to the hourly average wind speeds, the maximum transmission distance was computed as 350 km for updraft and the minimum transmission distances was as low as 32 m for downdraft. Subsequently, the coincidence between the source proportion of SAMPs on random day and meteorological parameters confirmed the synergistic impact on SAMPs transport influenced by functional zoning, geographic environment, and vertical velocity.
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Poluentes Atmosféricos , Monitoramento Ambiental , Microplásticos , China , Microplásticos/análise , Poluentes Atmosféricos/análise , Atmosfera/química , Vento , CidadesRESUMO
In this study, spatiotemporal analysis of forest fires in Turkiye was undertaken, with a specific focus on the large-scale atmospheric systems responsible for causing these fires. For this purpose, long-term variations in forest fires were classified based on the occurrence types (i.e. natural/lightning, negligence/inattention, arson, accident, unknown). The role of large-scale atmospheric circulations causing natural originated forest fires was investigated using NCEP/NCAR Reanalysis sea level pressure, and surface wind products for the selected episodes. According to the main results, Mediterranean (MeR), Aegean (AR), and Marmara (MR) regions of Turkiye are highly susceptible to forest fires. Statistically significant number of forest fires in the MeR and MR regions are associated with global warming trend of the Eastern Mediterranean Basin. In monthly distribution, forest fires frequently occur in the MeR part of Turkiye during September, August, and June months, respectively, and heat waves are responsible for forest fires in 2021. As a consequence of the extending summer Asiatic monsoon to the inner parts of Turkiye and the location of Azores surface high over Balkan Peninsula result in atmospheric blocking and associated calm weather conditions in the MeR (e.g. Mugla and Antalya provinces). When this blocking continues for a long time, southerly winds on the back slopes of the Taurus Mountains create a foehn effect, calm weather conditions and lack of moisture in the soil of Antalya and Mugla settlements trigger the formation of forest fires.
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Monitoramento Ambiental , Florestas , Análise Espaço-Temporal , Incêndios Florestais , Turquia , Atmosfera/química , Incêndios , Tempo (Meteorologia)RESUMO
ß-caryophyllonic acid (BCA), as an important precursor of aqueous secondary organic aerosols (aqSOA), has adverse effects on the atmospheric environment and human health. However, the key atmospheric chemical reaction process in which BCA participates in the formation of aqueous secondary organic aerosols is still unclear. In this study, the reaction mechanism and kinetics of BCA with ·OH and O3 were investigated by quantum chemical calculations. The initiation reactions between BCA and ·OH include addition and H-abstraction reaction pathways, subsequent intermediates will also react with O2, ultimately undergo a cracking reaction to generate small molecular substances. The reaction of BCA with O3 can generate primary ozone oxides and the Criegee Intermediates oIM3, subsequent main reaction products include keto-BCA, as well as other small molecule aqSOA precursors. The entire reaction process increases the O/C ratio of aqSOA in the aqueous phase and generates products of small molecules such as 4-formylpropionic acid, which plays an important role in the formation of aqSOA. At 298K, the transformation rate constants of BCA initiated by ·OH and O3 are 1.47 × 1010 M-1 s-1 and 3.16 × 105 M-1 s-1, respectively, the atmospheric lifetimes of BCA reacting with ·OH range from 0.86 h-5.40 h, while the lifetimes of BCA reacting with O3 range from 0.44 h-10.04 years. This suggests that BCA primarily reacts with ·OH. However, under higher O3 concentrations, its ozonolysis becomes significant, promoting the formation of aqSOA. According to the risk assessment, the toxicity of most transformation products (TPs) gradually decreased, but the residual developmental toxicity could not be ignored. In this paper, the atmospheric liquid phase oxidation mechanisms of sesquiterpene unsaturated derived acid were studied from the microscopic level, which has guiding significance for the formation and transformation of aqSOA in atmosphere.
Assuntos
Aerossóis , Poluentes Atmosféricos , Atmosfera , Radical Hidroxila , Ozônio , Ozônio/química , Radical Hidroxila/química , Atmosfera/química , Aerossóis/química , Poluentes Atmosféricos/química , CinéticaRESUMO
A field survey was conducted in the central Tibetan Plateau (Nam Co) in China for high-time resolution measurements of gaseous elemental mercury (GEM), gaseous oxidized mercury (GOM), and particle-bound mercury (PBM). Average concentrations (± 1 SD) of GEM, PBM, and GOM from November 2014 to March 2015 were 1.11 ± 0.20 ng m-3, 50.8 ± 26.5 pg m-3, and 3.6 ± 3.2 pg m-3, respectively. During the monitoring period, both GEM and GOM exhibited relative stability in their monthly variations, whereas PBM concentrations were significantly higher in winter compared to those in later autumn and early spring. In terms of diurnal variations, the maximum concentration of GEM was typically observed after sunrise, while PBM reached its peak before sunrise, and the highest concentration of GOM was recorded in the afternoon. Vertical convection conditions, photochemical production, and gas-particle partitioning were responsible for the diurnal cycle of atmospheric mercury. Based on modeling results, it was determined that the air mass transported from South Asia significantly impacted atmospheric mercury levels at Nam Co Station. The regions of western and central Nepal, central and eastern Pakistan, and northern India were identified as potential sources of atmospheric mercury at Nam Co.
Assuntos
Poluentes Atmosféricos , Atmosfera , Monitoramento Ambiental , Mercúrio , Mercúrio/análise , Poluentes Atmosféricos/análise , Tibet , Atmosfera/química , ChinaRESUMO
Big impacts on the early Earth would have created highly reducing atmospheres that generated molecules needed for the origin of life, such as nitriles. However, such impactors could have been followed by collisions that were sufficiently big to vaporize the ocean and destroy any pre-existing life. Thus, a post-impact-reducing atmosphere that gives rise to life needs to be followed by a lack of subsequent sterilizing impacts for life to persist. We assume that prebiotic chemistry required a post-impact-reducing atmosphere. Then, using statistics for the impact history on Earth and the minimum impact mass needed to generate post-impact highly reducing atmospheres, we show that the median timing of impact-driven biopoiesis is favored early in the Hadean, â¼4.35 Ga. However, uncertainties are large because impact bombardment is stochastic, and so biopoiesis could have occurred between 4.45 and 3.9 Ga within 95% uncertainty. In an optimistic scenario for biopoiesis from post-impact-reducing atmospheres, we find that the origin of life is favorable in â¼90% of stochastic impact realizations. In our most pessimistic case, biopoiesis is still fairly likely (â¼20% chance). This potentially bodes well for life on rocky exoplanets that have experienced an early episode of impact bombardment given how planets form.
Assuntos
Atmosfera , Origem da Vida , Atmosfera/química , Planeta Terra , Fatores de Tempo , Exobiologia/métodosRESUMO
The interaction between planets and stellar winds can lead to atmospheric loss and is, thus, important for the evolution of planetary atmospheres1. The planets in our Solar System typically interact with the solar wind, whose velocity is at a large angle to the embedded stellar magnetic field. For planets without an intrinsic magnetic field, this interaction creates an induced magnetosphere and a bow shock in front of the planet2. However, when the angle between the solar wind velocity and the solar wind magnetic field (cone angle) is small, the interaction is very different3. Here we show that when the cone angle is small at Mars, the induced magnetosphere degenerates. There is no shock on the dayside, only weak flank shocks. A cross-flow plume appears and the ambipolar field drives planetary ions upstream. Hybrid simulations with a 4° cone angle show agreement with observations by the Mars Atmosphere and Volatile Evolution mission4 and Mars Express5. Degenerate, induced magnetospheres are complex and not yet explored objects. It remains to be studied what the secondary effects are on processes like atmospheric loss through ion escape.