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1.
Environ Sci Technol ; 58(11): 5068-5078, 2024 Mar 19.
Artículo en Inglés | MEDLINE | ID: mdl-38446141

RESUMEN

Sulfate aerosol is one of the major components of secondary fine particulate matter in urban haze that has crucial impacts on the social economy and public health. Among the atmospheric sulfate sources, Mn(II)-catalyzed SO2 oxidation on aerosol surfaces has been regarded as a dominating one. In this work, we measured the reaction kinetics of Mn(II)-catalyzed SO2 oxidation in single droplets using an aerosol optical tweezer. We show that the SO2 oxidation occurs at the Mn(II)-active sites on the aerosol surface, per a piecewise kinetic formulation, one that is characterized by a threshold surface Mn(II) concentration and gaseous SO2 concentration. When the surface Mn(II) concentration is lower than the threshold value, the reaction rate is first order with respect to both Mn(II) and SO2, agreeing with our traditional knowledge. But when surface Mn(II) concentration is above the threshold, the reaction rate becomes independent of Mn(II) concentration, and the reaction order with respect to SO2 becomes greater than unity. The measured reaction rate can serve as a tool to estimate sulfate formation based on field observation, and our established parametrization corrects these calculations. This framework for reaction kinetics and parametrization holds promising potential for generalization to various heterogeneous reaction pathways.


Asunto(s)
Contaminantes Atmosféricos , Material Particulado , Material Particulado/análisis , Óxidos de Azufre , Sulfatos/análisis , Aerosoles , Catálisis
2.
Sci Total Environ ; 918: 170379, 2024 Mar 25.
Artículo en Inglés | MEDLINE | ID: mdl-38280593

RESUMEN

Alkyl-PAHs (APAHs) have been identified worldwide, which could rapidly react with chlorine and OH radicals in the atmosphere. In this study, a comprehensive investigation is conducted for SOA generated by a representative alkyl-naphthalene (1-methyl naphthalene, 1-MN) initiated by Cl, including yield, chemical composition, and volatility of SOA. To better understand 1-MN atmospheric oxidation, reaction mechanisms of 1MN with Cl atoms and OH radicals are proposed and compared under different nitrogen oxides (NOx) conditions. The SOA yields are comparable for Cl-initiated and OH-initiated reactions under high NOx conditions but increased in Cl-initiated reactions under low NOx conditions. The compounds with ten carbons are more abundant in Cl-initiated SOA, while compounds with nine carbons have higher intensity, suggesting that Cl caused ring-retained and alkyl-lost products and OH produces ring-broken and alkyl-retained compounds. The volatility of SOA is remarkably low, and SOA formed from Cl oxidation is slightly higher than that from OH oxidation. These results reveal that 1MN-derived SOA with OH and Cl radicals would have different physical-chemical properties and may play an important role in air quality and health effects.

3.
Sci Total Environ ; 912: 168333, 2024 Feb 20.
Artículo en Inglés | MEDLINE | ID: mdl-37952675

RESUMEN

During the COVID-19 lockdown in the Beijing-Tianjin-Hebei (BTH) region in China, large decrease in nitrogen oxides (NOx) emissions, especially in the transportation sector, could not avoid the occurrence of heavy PM2.5 pollution where nitrate dominated the PM2.5 mass increase. To experimentally reveal the effect of NOx control on the formation of PM2.5 secondary components (nitrate in particular), photochemical simulation experiments of mixed volatile organic compounds (VOCs) under various NOx concentrations with smog chamber were performed. The proportions of gaseous precursors in the control experiment were comparable to ambient conditions typically observed in the BTH region. Under relatively constant VOCs concentrations, when the initial NOx concentration was reduced to 40% of that in the control experiment (labelled as NOx,0), the particle mass concentration was not significantly reduced, but when the initial NOx concentration decreased to 20 % of NOx,0, the mass concentration of particles as well as nitrate and organics showed a sudden decrease. A "critical point" where the mass concentration of secondary aerosol started to decline as the initial NOx concentration decreased, located at 0.2-0.4 NOx,0 (or 0.18-0.44 NO2,0) in smog chamber experiments. The oxidation capacity and solar radiation intensity played key roles in the mass concentration and compositions of the formed particles. In field observations in the BTH region in the autumn and winter seasons, the "critical point" exist at 0.15-0.34 NO2,0, which coincided mostly with the laboratory simulation results. Our results suggest that a reduction of NOx emission by >60% could lead to significant reductions of secondary aerosol formation, which can be an effective way to further alleviate PM2.5 pollution in the BTH region.

4.
Sci Total Environ ; 905: 166852, 2023 Dec 20.
Artículo en Inglés | MEDLINE | ID: mdl-37717750

RESUMEN

Peroxyacetyl nitrate (PAN) is a typical secondary photochemical product in the atmospheric environment with significant adverse effects on human health and plant growth. In this study, PAN and other pollutants, as well as meteorological conditions were observed intensively from August to September in 2022 at a typical urban sampling site in Beijing, China. The mean and maximum PAN concentrations during the observation period were 1.00 ± 0.97 ppb and 4.84 ppb, respectively. Severe photochemical pollution occurred during the observation period, with the mean PAN concentration about 3.1 times higher than that during the clean period. There was a good positive correlation between O3 and PAN, and their correlation was higher during the O3 exposure period than that during the clean period. The simulated results by box-model coupled with the Master Chemical Mechanism (MCM v3.3.1) showed that the O3-related reactions were the largest sources of OH radicals during O3 exposure period, which was conducive to the co-contamination of PAN and O3. Acetaldehyde (CH3CHO) and methylglyoxal (MGLY) were the largest OVOCs precursors of peroxyacetyl radicals (PA), with the contributions to the total PA generated by OVOCs about 67 % - 83 % and 17 % - 30 %, respectively. The reduction of emissions from liquefied petroleum gas (LPG) and solvent usage has the highest reduction effect on PAN and O3, followed by the control of gasoline vehicle exhaust emissions. This study deepens the understanding of the PAN photochemistry in urban areas with high O3 background conditions and the impact of anthropogenic activities on the photochemical pollution. Meanwhile, the findings of this study highlight the necessity of strengthening anthropogenic emissions control to effectively reduce the co-contamination of PAN and O3 in Beijing in the future.

5.
Sci Total Environ ; 903: 166605, 2023 Dec 10.
Artículo en Inglés | MEDLINE | ID: mdl-37640078

RESUMEN

Nitrous acid (HONO) is an established precursor of hydroxyl (OH) radical and has significant impacts on the formation of PM2.5 and O3. Despite extensive research on HONO observation in recent years, knowledge regarding its sources and sinks in urban areas remains inadequate. In this study, we monitored the atmospheric concentrations of HONO and related pollutants, including gaseous nitric acid and particulate nitrate, simultaneously at a supersite in downtown Chengdu, a megacity in southwestern China during spring, when was chosen due to its tolerance for both PM2.5 and O3 pollution. Furthermore, we employed the random forest model to fill the missing data of HONO, which exhibited good predictive performance (R2 = 0.96, RMSE = 0.36 ppbv). During this campaign, the average mixing ratio of HONO was measured to be 1.0 ± 0.7 ppbv. Notably, during periods of high O3 and PM2.5 concentrations, the mixing ratio of HONO was >50 % higher compared to the clean period. We developed a comprehensive parameterization scheme for the HONO budget, and it performed well in simulating diurnal variations of HONO. Based on the HONO budget analysis, we identified different mechanisms that dominate HONO formation at different times of the day. Vehicle emissions and NO2 heterogeneous conversions were found to be the primary sources of HONO during nighttime (21.0 %, 30.2 %, respectively, from 18:00 to 7:00 the next day). In the morning (7:00-12:00), NO2 heterogeneous conversions and the reaction of NO with OH became the main sources (35.0 %, 32.2 %, respectively). However, in the afternoon (12:00-18:00), the heterogeneous photolysis of HNO3 on PM2.5 was identified as the most substantial source of HONO (contributing 52.5 %). This study highlights the significant variations in primary HONO sources throughout the day.

6.
Chem Res Chin Univ ; 39(3): 326-341, 2023.
Artículo en Inglés | MEDLINE | ID: mdl-37303472

RESUMEN

Secondary air pollutants, originating from gaseous pollutants and primary particulate matter emitted by natural sources and human activities, undergo complex atmospheric chemical reactions and multiphase processes. Secondary gaseous pollutants represented by ozone and secondary particulate matter, including sulfates, nitrates, ammonium salts, and secondary organic aerosols, are formed in the atmosphere, affecting air quality and human health. This paper summarizes the formation pathways and mechanisms of important atmospheric secondary pollutants. Meanwhile, different secondary pollutants' toxicological effects and corresponding health risks are evaluated. Studies have shown that secondary pollutants are generally more toxic than primary ones. However, due to their diverse source and complex generation mechanism, the study of the toxicological effects of secondary pollutants is still in its early stages. Therefore, this paper first introduces the formation mechanism of secondary gaseous pollutants and focuses mainly on ozone's toxicological effects. In terms of particulate matter, secondary inorganic and organic particulate matters are summarized separately, then the contribution and toxicological effects of secondary components formed from primary carbonaceous aerosols are discussed. Finally, secondary pollutants generated in the indoor environment are briefly introduced. Overall, a comprehensive review of secondary air pollutants may shed light on the future toxicological and health effects research of secondary air pollutants.

7.
Adv Atmos Sci ; : 1-23, 2023 Apr 28.
Artículo en Inglés | MEDLINE | ID: mdl-37359906

RESUMEN

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

8.
J Environ Sci (China) ; 123: 183-202, 2023 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-36521983

RESUMEN

Atmospheric nanoparticles are crucial components contributing to fine particulate matter (PM2.5), and therefore have significant effects on visibility, climate, and human health. Due to the unique role of atmospheric nanoparticles during the evolution process from gas-phase molecules to larger particles, a number of sophisticated experimental techniques have been developed and employed for online monitoring and characterization of the physical and chemical properties of atmospheric nanoparticles, helping us to better understand the formation and growth of new particles. In this paper, we firstly review these state-of-the-art techniques for investigating the formation and growth of atmospheric nanoparticles (e.g., the gas-phase precursor species, molecular clusters, physicochemical properties, and chemical composition). Secondly, we present findings from recent field studies on the formation and growth of atmospheric nanoparticles, utilizing several advanced techniques. Furthermore, perspectives are proposed for technique development and improvements in measuring atmospheric nanoparticles.


Asunto(s)
Contaminantes Atmosféricos , Nanopartículas , Humanos , Material Particulado/análisis , Nanopartículas/química , Contaminantes Atmosféricos/análisis , Monitoreo del Ambiente/métodos , Aerosoles/análisis , Tamaño de la Partícula
9.
Environ Pollut ; 316(Pt 1): 120710, 2023 Jan 01.
Artículo en Inglés | MEDLINE | ID: mdl-36414162

RESUMEN

The atmospheric chemistry of nitrous acid (HONO) has received extensive attention because of its significant contribution to hydroxyl (OH) radicals. Heterogeneous reaction of NO2 is an important HONO source, and its reaction mechanism is affected by many factors, such as concentration of gaseous NO2, surface adsorbed water, relative humidity and temperature. Although laboratory studies have confirmed the effect of temperature on heterogeneous reaction of NO2, there are few field observations reporting about it. We have conducted a field observation in the early spring 2021 when the temperature ranges widely (-0.1-24.7 °C). Concentrations of HONO and related pollutants at the urban area of Beijing are obtained. The hourly averaged HONO concentration reaches 4.87 ppb with a mean value of 1.48 ± 1.09 ppb. Combined with box model and RACM2 mechanism, we found an optimal temperature (∼10 °C) existing for heterogeneous reaction of NO2 during this measurement. When considering the promotion effect of optimal temperature, the contribution of heterogeneous reaction of NO2 to HONO can increase by 10%. This result will provide essential information for developing an accurate model of HONO chemistry in the atmosphere especially for certain periods or regions with temperature changing largely. Moreover, heterogeneous reaction of NO2 is the vital source of HONO, contributing 63-76% to simulated HONO during this measurement. Note that HONO photolysis is the most important formation pathway of OH radicals, and ambient HONO concentration is the obbligato constraint for evaluating atmospheric oxidation by model simulations.


Asunto(s)
Ácido Nitroso , Ozono , Radical Hidroxilo , Dióxido de Nitrógeno , Beijing
10.
J Environ Sci (China) ; 124: 557-569, 2023 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-36182163

RESUMEN

Atmospheric oxidizing capacity (AOC) is the fundamental driving factors of chemistry process (e.g., the formation of ozone (O3) and secondary organic aerosols (SOA)) in the troposphere. However, accurate quantification of AOC still remains uncertainty. In this study, a comprehensive field campaign was conducted during autumn 2019 in downtown of Beijing, where O3 and PM2.5 episodes had been experienced successively. The observation-based model (OBM) is used to quantify the AOC at O3 and PM2.5 episodes. The strong intensity of AOC is found at O3 and PM2.5 episodes, and hydroxyl radical (OH) is the dominating daytime oxidant for both episodes. The photolysis of O3 is main source of OH at O3 episode; the photolysis of nitrous acid (HONO) and formaldehyde (HCHO) plays important role in OH formation at PM2.5 episode. The radicals loss routines vary according to precursor pollutants, resulting in different types of air pollution. O3 budgets and sensitivity analysis indicates that O3 production is transition regime (both VOC and NOx-limited) at O3 episode. The heterogeneous reaction of hydroperoxy radicals (HO2) on aerosol surfaces has significant influence on OH and O3 production rates. The HO2 uptake coefficient (γHO2) is the determining factor and required accurate measurement in real atmospheric environment. Our findings could provide the important bases for coordinated control of PM2.5 and O3 pollution.


Asunto(s)
Contaminantes Atmosféricos , Ozono , Compuestos Orgánicos Volátiles , Aerosoles/análisis , Contaminantes Atmosféricos/análisis , Beijing , China , Monitoreo del Ambiente , Formaldehído , Radical Hidroxilo/análisis , Ácido Nitroso , Oxidantes , Oxidación-Reducción , Ozono/análisis , Material Particulado/análisis , Compuestos Orgánicos Volátiles/análisis
11.
J Am Chem Soc ; 144(37): 16953-16964, 2022 09 21.
Artículo en Inglés | MEDLINE | ID: mdl-36070362

RESUMEN

Organosulfates (OSs) are well-known and ubiquitous constituents of atmospheric aerosol particles and have been used as secondary organic aerosol markers in many field studies. Hence, it is imperative to understand the formation of OS species in the atmosphere. Recently, hydroxy acids (HAs) and hydroxy acid sulfates have been extensively detected in the atmospheric environment. However, the reaction mechanism of HAs to form OSs is much less understood. In this work, we have mainly investigated the reaction of typical α-HAs, including glycolic acid (GA) and lactic acid (LA), and SO3 at the liquid aerosol surface using quantum chemistry calculations and Born-Oppenheimer molecular dynamics simulations. The OH group orientation of α-HAs at the air-water interface is found to exert a significant impact on the formation of OSs. The OH group pointing to the gas phase is obviously beneficial to the formation of OSs. Two key factors are discovered important to the reaction of α-HAs adsorbed on the liquid surface with SO3: (a) the exposure position of the active site to the gas phase and (b) the reactivity of the exposed site to the attracted SO3 molecule. Moreover, we found that the air-water interface exerts a significant influence on the physicochemical behaviors of GA and LA, especially on their OH group orientation, and thus leads to their different properties for the SO3 colliding reaction. The presented reaction mechanism provides a new feasible pathway for the production of OSs at the liquid aerosol surface, which may have important impacts on the formation of organic aerosols.


Asunto(s)
Sulfatos , Agua , Aerosoles/química , Hidroxiácidos , Ácido Láctico , Sulfatos/química
12.
Sci Total Environ ; 841: 156771, 2022 Oct 01.
Artículo en Inglés | MEDLINE | ID: mdl-35724777

RESUMEN

Atmospheric trace metals are a key component of particulate matter and significantly influence the atmospheric process and human health. The dissolved fraction of trace metals represents their bioavailability and exhibits high chemical activity. However, the optimum measurement method for detecting the soluble fraction of trace metals is still undetermined. The impact of variations in pollution on the soluble fraction is largely unrevealed. Therefore, in this work, a one-month field observation was conducted in Central China and different extraction solvents were used to determine the proper measurement method for the soluble fraction of trace metals and investigate the variation pattern under different pollution conditions. The findings show that solvents with acidity near that of aerosol water can better reflect the actual soluble fraction of trace metals in fine particulate matter. The soluble fraction of trace metals tends to increase with pollution level increased, demonstrating unexpectedly high health risks and chemical activity under heavy haze conditions. Our results indicate that remediation and trace metal pollution control are urgently needed.


Asunto(s)
Contaminantes Atmosféricos , Metales Pesados , Oligoelementos , Contaminantes Atmosféricos/análisis , China , Monitoreo del Ambiente/métodos , Humanos , Metales Pesados/análisis , Material Particulado/análisis , Solventes , Oligoelementos/análisis
13.
Environ Sci Technol ; 56(12): 7637-7646, 2022 06 21.
Artículo en Inglés | MEDLINE | ID: mdl-35638231

RESUMEN

Severe winter haze events in Beijing and North China Plain are characterized by rapid production of sulfate aerosols with unresolved mechanisms. Oxidation of SO2 by O2 in the absence of metal catalysts (uncatalyzed autoxidation) represents the most ubiquitous SO2 conversion pathway in the atmosphere. However, this reaction has long been regarded as too slow to be atmospherically meaningful. This traditional view was based on the kinetic studies conducted in bulk dilute solutions that mimic cloudwater but deviate from urban aerosols. Here, we directly measure the sulfate formation rate via uncatalyzed SO2 autoxidation in single (NH4)2SO4 microdroplets, by using an aerosol optical tweezer coupled with a cavity-enhanced Raman spectroscopy technique. We find that the aqueous reaction of uncatalyzed SO2 autoxidation is accelerated by two orders of magnitude at the high ionic strength (∼36 molal) conditions in the supersaturated aerosol water. Furthermore, at acidic conditions (pH 3.5-4.5), uncatalyzed autoxidation predominately occurs on droplet surface, with a reaction rate unconstrained by SO2 solubility. With these rate enhancements, we estimate that the uncatalyzed SO2 autoxidation in aerosols can produce sulfate at a rate up to 0.20 µg m-3 hr-1, under the winter air pollution condition in Beijing.


Asunto(s)
Contaminantes Atmosféricos , Dióxido de Azufre , Aerosoles/química , Contaminantes Atmosféricos/análisis , China , Monitoreo del Ambiente , Cinética , Material Particulado/análisis , Sulfatos/química , Dióxido de Azufre/análisis , Óxidos de Azufre , Agua
14.
Environ Sci Technol ; 56(12): 7771-7778, 2022 06 21.
Artículo en Inglés | MEDLINE | ID: mdl-35609338

RESUMEN

There is a large gap between the simulated and observed sulfate concentrations during winter haze events in North China. Although multiphase sulfate formation mechanisms have been proposed, they have not been evaluated using chemical transport models. In this study, the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) was used to apportion sulfate formation. It was found that Mn-catalyzed oxidation on aerosol surfaces was the dominant sulfate formation pathway, accounting for 92.3 ± 3.5% of the sulfate formation during haze events. Gas-phase oxidation contributed 3.1 ± 0.5% to the sulfate formation due to the low OH levels. The H2O2 oxidation in aerosol water accounted for 4.2 ± 3.6% of the sulfate formation, caused by the rapid consumption of H2O2. The contributions of O3, NO2 oxidation, and transition metal ion-catalyzed reactions in aerosol water could be negligible owing to the low aerosol water content, low pH, and high ionic strength. The contributions from in-cloud reactions were negligible due to the barrier provided by stable stratification during winter haze events.


Asunto(s)
Contaminantes Atmosféricos , Material Particulado , Aerosoles/análisis , Contaminantes Atmosféricos/análisis , China , Monitoreo del Ambiente , Peróxido de Hidrógeno , Material Particulado/análisis , Estaciones del Año , Sulfatos/química , Óxidos de Azufre , Agua
15.
J Environ Sci (China) ; 114: 343-353, 2022 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-35459497

RESUMEN

As an important precursor of hydroxyl radical (OH), nitrous acid (HONO) plays a significant role in atmospheric chemistry. Here, an observation of HONO and relevant air pollutants in an urban site of Beijing from 14 to 28 April, 2017 was performed. Two distinct peaks of HONO concentrations occurred during the observation. In contrast, the concentration of particulate matter in the first period (period Ⅰ) was significantly higher than that in the second period (period Ⅱ). Comparing to HONO sources in the two periods, we found that the direct vehicle emission was an essential source of the ambient HONO during both periods at night, especially in period Ⅱ. The heterogeneous reaction of NO2 was the dominant source in period Ⅰ, while the homogeneous reaction of NO with OH was more critical source at night in period Ⅱ. In the daytime, the heterogeneous reaction of NO2 was a significant source and was confirmed by the good correlation coefficients (R2) between the unknown sources (Punknown) with NO2, PM2.5, NO2 × PM2.5 in period Ⅰ. Moreover, when solar radiation and OH radicals were considered to explore unknown sources in the daytime, the enhanced correlation of Punknown with photolysis rate of NO2 and OH ( [Formula: see text]  × OH) were 0.93 in period Ⅰ, 0.95 in period Ⅱ. These excellent correlation coefficients suggested that the unknown sources released HONO highly related to the solar radiation and the variation of OH radicals.


Asunto(s)
Dióxido de Nitrógeno , Ácido Nitroso , Beijing , Ácido Nitroso/análisis , Material Particulado , Emisiones de Vehículos
16.
J Environ Sci (China) ; 114: 334-342, 2022 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-35459496

RESUMEN

The particulate matter (PM) pollution has been significantly improved by carrying out various valid emission control strategies since 2013 in China. Meanwhile the variation trend of nitrous acid (HONO) is worthy to investigate due to its vital role in the atmospheric oxidation process. In this study, field observation in the winter is conducted to investigate the concentration of HONO in an urban area of Beijing. In the winter of 2019, the mean HONO concentration is 1.38 ppbV during the whole winter. Photo-enhanced NO2 heterogeneous reactions on the ground and aerosol surfaces were found as the possible daytime sources of HONO. Compared to O3, photolysis of HONO dominates the primary OH sources during the winter time. To understand the HONO pollution patterns by years variation, multi-year data is summarized and finds that primary pollutants including CO and NO decreased, but secondary pollutants i.e., HONO (mostly generated via secondary process) increased. Our study highlights the requirement to mitigate secondary pollution by control HONO concentration.


Asunto(s)
Contaminantes Ambientales , Ácido Nitroso , Aerosoles , Beijing , Ácido Nitroso/análisis , Estaciones del Año
17.
J Environ Sci (China) ; 114: 37-52, 2022 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-35459500

RESUMEN

As a representative species of intermediate volatile organic compounds (IVOCs), long-chain alkanes are considered to be important precursors of secondary organic aerosols (SOA) in the atmosphere. This work reviews the previous studies on long-chain alkanes in the atmosphere: (1) the detection methods and filed observations of long-chain alkanes in both gas and particle phases are summarized briefly; (2) the laboratory studies of long chain alkanes are reviewed, the kinetic data, reaction mechanism, SOA yields, and physicochemical properties of SOA are included in detail; (3) the research progress related to model simulations of long-chain alkanes are also discussed. In addition, based on available research results, several perspective contents are proposed that can be used as a guideline for future research plans.


Asunto(s)
Contaminantes Atmosféricos , Compuestos Orgánicos Volátiles , Aerosoles/química , Contaminantes Atmosféricos/análisis , Alcanos , Atmósfera/química , Cinética , Compuestos Orgánicos Volátiles/química
18.
J Environ Sci (China) ; 114: 434-443, 2022 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-35459506

RESUMEN

New particle formation (NPF) is the primary source of nanoparticles and contributes a large number of concentrations of cloud condensation nuclei. In recent years, field campaigns and laboratory experiments have been conducted to promote cognition of the mechanism for NPF and its following growth processes. The chemical composition measurement of nanoparticles could help deepen understanding of the initial step of particulate matter formation. In this work, we developed a nanoparticle chemical ionization mass spectrometer to measure nanoparticles' chemical compositions during their initial growth stage. Meanwhile, a non-radioactive ion source was designed for aerosol charging and chemical ionization. Time of flight mass spectrometer coupled with integrated aerosol size selection and collection module would guarantee the picogram level detection limit and high-resolution ability to measure the matrix of ambient samples. The performance of this equipment was overall evaluated, including the transmission efficiency and collection efficiency of custom-built nano differential mobility analyzer, chemical ionization efficiency, and mass resolution of the mass spectrometer. The high sensitivity measurement of ammonium sulfate and methylammonium sulfate aerosols with diameters ranging from 10 to 25 nm could guarantee the application of this instrument in the ambient measurement.


Asunto(s)
Contaminantes Atmosféricos , Nanopartículas , Aerosoles/análisis , Contaminantes Atmosféricos/análisis , Tamaño de la Partícula , Material Particulado/análisis
19.
J Environ Sci (China) ; 114: 85-97, 2022 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-35459517

RESUMEN

The field observation of 54 non-methane hydrocarbon compounds (NMHCs) was conducted from September 1 to October 20 in 2020 during autumn in Haidian District, Beijing. The mean concentration of total NMHCs was 29.81 ± 11.39 ppbv during this period, and alkanes were the major components. There were typical festival effects of NMHCs with lower concentration during the National Day. Alkenes and aromatics were the dominant groups in ozone formation potential (OFP) and OH radical loss rate (LOH). The positive matrix factorization (PMF) running results revealed that vehicular exhaust became the biggest source in urban areas, followed by liquefied petroleum gas (LPG) usage, solvent usage, and fuel evaporation. The box model coupled with master chemical mechanism (MCM) was applied to study the impacts of different NMHCs sources on ozone (O3) formation in an O3 episode. The simulation results indicated that reducing NMHCs concentration could effectively suppress O3 formation. Moreover, reducing traffic-related emissions of NMHCs was an effective way to control O3 pollution at an urban site in Beijing.


Asunto(s)
Contaminantes Atmosféricos , Ozono , Compuestos Orgánicos Volátiles , Contaminantes Atmosféricos/análisis , Beijing , China , Monitoreo del Ambiente/métodos , Hidrocarburos/análisis , Metano , Ozono/análisis , Emisiones de Vehículos/análisis , Compuestos Orgánicos Volátiles/análisis
20.
Environ Sci Technol ; 56(8): 4859-4870, 2022 Apr 19.
Artículo en Inglés | MEDLINE | ID: mdl-35319183

RESUMEN

Long-chain alkanes are a type of intermediate volatility organic compound (IVOC) in the atmosphere and a potential source of secondary organic aerosols (SOAs). C12-C14 n-alkylcyclohexanes are important compositions of IVOCs, with considerable concentrations and emission rates. The reaction rate constants and SOA formation of the reactions of C12-C14 n-alkylcyclohexanes with Cl atoms were investigated in the present study. The reaction rate constants of the long-chain alkanes obtained via the relative-rate method at 298 ± 0.2 K (in units of ×10-10 cm3 molecule-1 s-1) were as follows: khexylcyclohexane = 5.11 ± 0.28, kheptylcyclohexane = 5.56 ± 0.30, and koctylcyclohexane = 5.74 ± 0.31. The gas-phase products of the reactions were identified as mainly small molecules of aldehydes, ketones, and acids. The particle-phase products were mostly monomers and oligomers, but there were still trimers even under high-NOx conditions. Moreover, under high-NOx conditions (urban atmosphere), the SOA yields of hexylcyclohexane are higher than that under low-NOx conditions (remote atmosphere), indicating that more attention should be given to the SOA formation of Cl-initiated n-alkylcyclohexane oxidations in polluted regions. This research can further clarify the oxidation processes and SOA formation of n-alkylcyclohexanes in the atmosphere.

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