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1.
Proc Natl Acad Sci U S A ; 121(31): e2404595121, 2024 Jul 30.
Artigo em Inglês | MEDLINE | ID: mdl-39047040

RESUMO

New particle formation (NPF) substantially affects the global radiation balance and climate. Iodic acid (IA) is a key marine NPF driver that recently has also been detected inland. However, its impact on continental particle nucleation remains unclear. Here, we provide molecular-level evidence that IA greatly facilitates clustering of two typical land-based nucleating precursors: dimethylamine (DMA) and sulfuric acid (SA), thereby enhancing particle nucleation. Incorporating this mechanism into an atmospheric chemical transport model, we show that IA-induced enhancement could realize an increase of over 20% in the SA-DMA nucleation rate in iodine-rich regions of China. With declining anthropogenic pollution driven by carbon neutrality and clean air policies in China, IA could enhance nucleation rates by 1.5 to 50 times by 2060. Our results demonstrate the overlooked key role of IA in continental NPF nucleation and highlight the necessity for considering synergistic SA-IA-DMA nucleation in atmospheric modeling for correct representation of the climatic impacts of aerosols.

2.
Proc Natl Acad Sci U S A ; 119(32): e2201729119, 2022 Aug 09.
Artigo em Inglês | MEDLINE | ID: mdl-35917351

RESUMO

The gas-phase formation of new particles less than 1 nm in size and their subsequent growth significantly alters the availability of cloud condensation nuclei (CCN, >30-50 nm), leading to impacts on cloud reflectance and the global radiative budget. However, this growth cannot be accounted for by condensation of typical species driving the initial nucleation. Here, we present evidence that nucleated iodine oxide clusters provide unique sites for the accelerated growth of organic vapors to overcome the coagulation sink. Heterogeneous reactions form low-volatility organic acids and alkylaminium salts in the particle phase, while further oligomerization of small α-dicarbonyls (e.g., glyoxal) drives the particle growth. This identified heterogeneous mechanism explains the occurrence of particle production events at organic vapor concentrations almost an order of magnitude lower than those required for growth via condensation alone. A notable fraction of iodine associated with these growing particles is recycled back into the gas phase, suggesting an effective transport mechanism for iodine to remote regions, acting as a "catalyst" for nucleation and subsequent new particle production in marine air.

3.
Annu Rev Phys Chem ; 74: 99-121, 2023 Apr 24.
Artigo em Inglês | MEDLINE | ID: mdl-36696587

RESUMO

Atmospheric aerosols exert a significant but highly uncertain effect on the global climate, and roughly half of these particles originate as small clusters formed by collisions between atmospheric trace vapors. These particles typically consist of acids, bases, and water, stabilized by salt bridge formation and a network of strong hydrogen bonds. We review spectroscopic studies of this process, focusing on the clusters likely to be involved in the first steps of particle formation and the intermolecular interactions governing their stability. These studies typically focus on determining structure and stability and have shown that acid-base chemistry in the cluster may violate chemical intuition derived from solution-phase behavior and that hydration of these clusters is likely to be complex to describe. We also suggest fruitful areas for extension of these studies and alternative spectroscopic techniques that have not yet been applied to this problem.

4.
Environ Sci Technol ; 58(12): 5453-5460, 2024 Mar 26.
Artigo em Inglês | MEDLINE | ID: mdl-38477969

RESUMO

Many types of living plants release gaseous trimethylamine (TMA), making it a potentially important contributor to new particle formation (NPF) in remote areas. However, a panoramic view of the importance of forest biogenic TMA at the regional scale is lacking. Here, we pioneered nationwide mobile measurements of TMA across a transect of contiguous farmland in eastern China and a transect of subtropical forests in southern China. In contrast to the farmland route, TMA concentrations measured during the subtropical forest route correlated significantly with isoprene, suggesting potential TMA emissions from leaves. Our high time-resolved concentrations obtained from a weak photo-oxidizing atmosphere reflected freshly emitted TMA, indicating the highest emission intensity from irrigated dryland (set as the baseline of 10), followed by paddy field (7.1), subtropical evergreen forests (5.9), and subtropical broadleaf and mixed forests (4.3). Extrapolating their proportions roughly to China, subtropical forests alone, which constitute half of the total forest area, account for nearly 70% of the TMA emissions from the nation's total farmland. Our estimates, despite the uncertainties, take the first step toward large-scale assessment of forest biogenic amines, highlighting the need for observational and modeling studies to consider this hitherto overlooked source of TMA.


Assuntos
Florestas , Metilaminas , Fazendas , China , Solo
5.
Environ Sci Technol ; 58(25): 10956-10968, 2024 Jun 25.
Artigo em Inglês | MEDLINE | ID: mdl-38868859

RESUMO

Marine dimethyl sulfide (DMS) emissions are the dominant source of natural sulfur in the atmosphere. DMS oxidizes to produce low-volatility acids that potentially nucleate to form particles that may grow into climatically important cloud condensation nuclei (CCN). In this work, we utilize the chemistry transport model ADCHEM to demonstrate that DMS emissions are likely to contribute to the majority of CCN during the biological active period (May-August) at three different forest stations in the Nordic countries. DMS increases CCN concentrations by forming nucleation and Aitken mode particles over the ocean and land, which eventually grow into the accumulation mode by condensation of low-volatility organic compounds from continental vegetation. Our findings provide a new understanding of the exchange of marine precursors between the ocean and land, highlighting their influence as one of the dominant sources of CCN particles over the boreal forest.


Assuntos
Atmosfera , Atmosfera/química
6.
Environ Sci Technol ; 2024 Sep 09.
Artigo em Inglês | MEDLINE | ID: mdl-39252395

RESUMO

Iodic acid (IA), the key driver of marine aerosols, is widely detected within the gas and particle phases in the marine boundary layer (MBL) and even the free troposphere (FT). Although atmospheric bases like dimethylamine (DMA) and ammonia (NH3) can enhance IA particles formation, their different efficiencies and spatial distributions make the dominant base-stabilization mechanisms of forming IA particles unclear. Herein, we investigated the IA-DMA-NH3 nucleation system through quantum chemical calculations at the DLPNO-CCSD(T)/aug-cc-pVTZ(-PP)//ωB97X-D/6-311++G(3df,3pd) + aug-cc-pVTZ-PP level of theory and cluster dynamics simulations. We provide molecular-level evidence that DMA and NH3 can jointly stabilize the IA clusters. The formation rates of IA clusters initially decline before rising from the MBL to the FT, owing to variations in mechanism. In the MBL, IA-DMA nucleation predominates, while the contribution of IA-DMA-NH3 synergistic nucleation cannot be overlooked in polar and NH3-polluted regions. In the lower FT, IA-DMA-NH3 nucleation prevails, whereas in the upper FT, IA-NH3 nucleation dominates. The efficiency of IA-DMA-NH3 nucleation is comparable to that of IA-iodous acid nucleation in the MBL and sulfuric acid-NH3 nucleation in the FT. Hence, the IA-DMA-NH3 mechanism holds promise for revealing the missing sources of tropospheric IA particles.

7.
Environ Sci Technol ; 58(3): 1601-1614, 2024 Jan 23.
Artigo em Inglês | MEDLINE | ID: mdl-38185880

RESUMO

Highly oxygenated organic molecules (HOMs) are a major source of new particles that affect the Earth's climate. HOM production from the oxidation of volatile organic compounds (VOCs) occurs during both the day and night and can lead to new particle formation (NPF). However, NPF involving organic vapors has been reported much more often during the daytime than during nighttime. Here, we show that the nitrate radicals (NO3), which arise predominantly at night, inhibit NPF during the oxidation of monoterpenes based on three lines of observational evidence: NPF experiments in the CLOUD (Cosmics Leaving OUtdoor Droplets) chamber at CERN (European Organization for Nuclear Research), radical chemistry experiments using an oxidation flow reactor, and field observations in a wetland that occasionally exhibits nocturnal NPF. Nitrooxy-peroxy radicals formed from NO3 chemistry suppress the production of ultralow-volatility organic compounds (ULVOCs) responsible for biogenic NPF, which are covalently bound peroxy radical (RO2) dimer association products. The ULVOC yield of α-pinene in the presence of NO3 is one-fifth of that resulting from ozone chemistry alone. Even trace amounts of NO3 radicals, at sub-parts per trillion level, suppress the NPF rate by a factor of 4. Ambient observations further confirm that when NO3 chemistry is involved, monoterpene NPF is completely turned off. Our results explain the frequent absence of nocturnal biogenic NPF in monoterpene (α-pinene)-rich environments.


Assuntos
Poluentes Atmosféricos , Monoterpenos Bicíclicos , Ozônio , Compostos Orgânicos Voláteis , Monoterpenos/química , Nitratos/química , Aerossóis/análise , Compostos Orgânicos Voláteis/química
8.
Environ Sci Technol ; 58(17): 7314-7324, 2024 Apr 30.
Artigo em Inglês | MEDLINE | ID: mdl-38626432

RESUMO

New particle formation via the ion-mediated sulfuric acid and ammonia molecular clustering mechanism remains the most widely observed and experimentally verified pathway. Recent laboratory and molecular level observations indicate iodine-driven nucleation as a potentially important source of new particles, especially in coastal areas. In this study, we assess the role of iodine species in particle formation using the best available molecular thermochemistry data and coupled to a detailed 1-d column model which is run along air mass trajectories over the Southern Ocean and the coast of Antarctica. In the air masses traversing the open ocean, ion-mediated SA-NH3 clustering appears insufficient to explain the observed particle size distribution, wherein the simulated Aitken mode is lacking. Including the iodine-assisted particle formation improves the modeled Aitken mode representation with an increase in the number of freshly formed particles. This implies that more particles survive and grow to Aitken mode sizes via condensation of gaseous precursors and heterogeneous reactions. Under certain meteorological conditions, iodine-assisted particle formation can increase cloud condensation nuclei concentrations by 20%-100%.


Assuntos
Aerossóis , Iodo , Regiões Antárticas , Iodo/química , Tamanho da Partícula , Poluentes Atmosféricos , Material Particulado
9.
Environ Sci Technol ; 2024 Sep 26.
Artigo em Inglês | MEDLINE | ID: mdl-39327447

RESUMO

Aerosol particles originating from the Qinghai-Tibet Plateau (QTP) readily reach the free troposphere, potentially affecting global radiation and climate. Although new particle formation (NPF) is frequently observed at such high altitudes, its precursors and their underlying chemistry remain poorly understood. This study presents direct observational evidence of anthropogenic influences on biogenic NPF on the southeastern QTP, near the Himalayas. The mean particle nucleation rate (J1.7) is 2.6 cm-3 s-1, exceeding the kinetic limit of sulfuric acid (SA) nucleation (mean SA: 2.4 × 105 cm-3). NPF is predominantly driven by highly oxygenated organic molecules (HOMs), possibly facilitated by low SA levels. We identified 1538 ultralow-volatility HOMs driving particle nucleation and 764 extremely low-volatility HOMs powering initial particle growth, with mean total concentrations of 1.5 × 106 and 3.7 × 106 cm-3, respectively. These HOMs are formed by atmospheric oxidation of biogenic precursors, unexpectedly including sesquiterpenes and diterpenes alongside the commonly recognized monoterpenes. Counterintuitively, over half of HOMs are organic nitrates, mainly produced by interacting with anthropogenic NOx via RO2+NO terminations or NO3-initiated oxidations. These findings advance our understanding of NPF mechanisms in this climate-sensitive region and underscore the importance of heavy terpene and NOx-influenced chemistry in assessing anthropogenic-biogenic interactions with climate feedbacks.

10.
Environ Res ; 251(Pt 1): 118542, 2024 Jun 15.
Artigo em Inglês | MEDLINE | ID: mdl-38403149

RESUMO

Secondary aerosols constitute a significant fraction of atmospheric aerosols, yet our understanding of their formation mechanism and fate is very limited. In this work, the secondary organic aerosol (SOA) formation and aging of ambient air of Delhi are studied using a potential aerosol mass (PAM) reactor, an oxidation flow reactor (OFR), coupled with aerosol chemical speciation monitor (ACSM), proton transfer reaction time of flight mass spectrometer (PTR-ToF-MS), and scanning mobility particle sizer with counter (SMPS + C). The setup mimics atmospheric aging of up to several days with the generation of OH radicals. Variations in primary volatile organic compounds (VOCs) and oxygenated volatile organic compounds (OVOCs) as a function of photochemical age were investigated. Primary VOCs such as benzene, toluene, xylene, trimethyl benzene, etc. decrease and OVOCs like formic acid, formaldehyde, acetone, ethanol, etc. increase substantially upon oxidation in OFR. The highest organic aerosol (OA) enhancement was observed for the 4.2 equivalent photochemical days of aging i.e., 1.84 times the ambient concentration, and net OA loss was observed at very high OH exposure, typically after 8.4 days of photochemical aging due to heterogeneous oxidation followed by fragmentation/evaporation. In ambient air, OA enhancement is highest during nighttime due to the high concentrations of precursor VOCs in the atmosphere. SMPS + C results demonstrated substantial new particle formation upon aging and decrement in preexisting aerosol mass. This is the first experimental study conducting an in-situ evaluation of potential SOA mass generated from the ambient aerosols in India.


Assuntos
Aerossóis , Poluentes Atmosféricos , Oxirredução , Compostos Orgânicos Voláteis , Aerossóis/análise , Aerossóis/química , Índia , Compostos Orgânicos Voláteis/análise , Poluentes Atmosféricos/análise , Poluentes Atmosféricos/química , Monitoramento Ambiental
11.
Environ Sci Technol ; 57(35): 13092-13103, 2023 09 05.
Artigo em Inglês | MEDLINE | ID: mdl-37607019

RESUMO

Interactions between water and organic molecules in sub-4 nm clusters play a significant role in the formation and growth of secondary organic aerosol (SOA) particles. However, a complete understanding of the relevant water microphysics has not yet been achieved due to challenges in the experimental characterization of soft nuclei. Here, we use molecular dynamics simulations to study the phase-mixing states, surface tension, water activity, and water accommodation coefficient of organic-water clusters representative of freshly nucleated SOA particles. Our results reveal large deviations from the behavior expected based on continuum theories. In particular, the phase-mixing state has a strong dependence on cluster size; surface tension displays a minimum at a specific organic-water mass ratio (morg/mw ∼ 4.5 in this study) corresponding to a minimum inhibition of droplet nucleation associated with the Kelvin effect; and the water accommodation coefficient increases by a factor of 2 with nanocluster hygroscopic growth, in agreement with recent experimental studies. Overall, our results yield parametric relations for water microphysical properties in sub-4 nm clusters and provide insight into the role of water in the initial stages of SOA nucleation and growth.


Assuntos
Água , Tensão Superficial , Molhabilidade
12.
Proc Natl Acad Sci U S A ; 117(7): 3427-3432, 2020 02 18.
Artigo em Inglês | MEDLINE | ID: mdl-32015109

RESUMO

High levels of ultrafine particles (UFPs; diameter of less than 50 nm) are frequently produced from new particle formation under urban conditions, with profound implications on human health, weather, and climate. However, the fundamental mechanisms of new particle formation remain elusive, and few experimental studies have realistically replicated the relevant atmospheric conditions. Previous experimental studies simulated oxidation of one compound or a mixture of a few compounds, and extrapolation of the laboratory results to chemically complex air was uncertain. Here, we show striking formation of UFPs in urban air from combining ambient and chamber measurements. By capturing the ambient conditions (i.e., temperature, relative humidity, sunlight, and the types and abundances of chemical species), we elucidate the roles of existing particles, photochemistry, and synergy of multipollutants in new particle formation. Aerosol nucleation in urban air is limited by existing particles but negligibly by nitrogen oxides. Photooxidation of vehicular exhaust yields abundant precursors, and organics, rather than sulfuric acid or base species, dominate formation of UFPs under urban conditions. Recognition of this source of UFPs is essential to assessing their impacts and developing mitigation policies. Our results imply that reduction of primary particles or removal of existing particles without simultaneously limiting organics from automobile emissions is ineffective and can even exacerbate this problem.


Assuntos
Material Particulado/química , Emissões de Veículos/análise , Poluentes Atmosféricos/química , Oxirredução , Tamanho da Partícula , Temperatura
13.
Proc Natl Acad Sci U S A ; 117(41): 25344-25351, 2020 10 13.
Artigo em Inglês | MEDLINE | ID: mdl-32989149

RESUMO

The large concentrations of ultrafine particles consistently observed at high altitudes over the tropics represent one of the world's largest aerosol reservoirs, which may be providing a globally important source of cloud condensation nuclei. However, the sources and chemical processes contributing to the formation of these particles remain unclear. Here we investigate new particle formation (NPF) mechanisms in the Amazon free troposphere by integrating insights from laboratory measurements, chemical transport modeling, and field measurements. To account for organic NPF, we develop a comprehensive model representation of the temperature-dependent formation chemistry and thermodynamics of extremely low volatility organic compounds as well as their roles in NPF processes. We find that pure-organic NPF driven by natural biogenic emissions dominates in the uppermost troposphere above 13 km and accounts for 65 to 83% of the column total NPF rate under relatively pristine conditions, while ternary NPF involving organics and sulfuric acid dominates between 8 and 13 km. The large organic NPF rates at high altitudes mainly result from decreased volatility of organics and increased NPF efficiency at low temperatures, somewhat counterbalanced by a reduced chemical formation rate of extremely low volatility organic compounds. These findings imply a key role of naturally occurring organic NPF in high-altitude preindustrial environments and will help better quantify anthropogenic aerosol forcing from preindustrial times to the present day.

14.
J Environ Manage ; 347: 119079, 2023 Dec 01.
Artigo em Inglês | MEDLINE | ID: mdl-37748297

RESUMO

New particle formation (NPF) contributes more than half of the global aerosol. Diethanolamine (DEA) and methyldiethanolamine (MDEA) are the most common amines used to remove CO2 and H2S, which are lost to the atmosphere from CO2 chemical absorbers, livestock and consumer products and are involved in sulfuric acid (SA)-driven NPF. Ion-induced nucleation (IIN) is an important nucleation pathway for NPF. We investigated the role of IIN on DEA and MDEA enhancing SA-driven NPF using density functional method (DFT), molecular dynamics (MD) simulation and atmospheric cluster dynamics code (ACDC). The effects of SO42-, H3O+, NH4+, HSO4-, NO3-, ammonia, methylamine, dimethylamine, trimethylamine and water (W) on the nucleation of SA-DEA were further investigated. The enhancement ability of DEA is greater than that of dimethylamine (DMA) and MDEA. Participation in SA-based NPF is a removal pathway for DEA and MDEA. DEA-SA clusters are generated that not only aggregate DEA and SA molecules, but also increase further growth of atmospheric ions. The very low Gibbs formation free energy highlights the importance of ion-induced nucleation for SA-based NPF. The order of the ability of common atmospheric ions to increase the (SA)(DEA) cluster nucleation is SO42- > H3O+ > NH4+ > HSO4- > NO3-. The addition of 20 water molecules increases the (SA)(DEA)9 cluster from 1.882 nm to 2.053 nm, promoting SA-based NPF. The atmospheric ions accelerate the aggregation rate of the (SA)5(DEA)5 cluster within 15 ns?


Assuntos
Aminas , Dióxido de Carbono , Aminas/química , Ácidos Sulfúricos/química , Dimetilaminas/química , Água
15.
J Environ Sci (China) ; 123: 54-64, 2023 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-36522013

RESUMO

Sulfuric anhydrides, generated from the cycloaddition reaction of SO3 with carboxylic acids, have been revealed to be potential participants in the nucleation process of new particle formation (NPF). Hence the reaction mechanisms of typical aromatic acids (benzoic acid (BA), phenylacetic acid (PAA), phthalic acid (PA), isophthalic acid (mPA), and terephthalic acid (PTA)) with SO3 to generate the corresponding aromatic sulfuric anhydrides were investigated by density functional theory calculations at the level of M06-2X/6-311++G(3df,3pd). As a result, these reactions were found to be feasible in the gas phase with barriers of 0.34, 0.30, 0.18, 0.08 and 0.12 kcal/mol to generate corresponding aromatic sulfuric anhydrides, respectively. The thermodynamic stabilities of clusters containing aromatic sulfuric anhydrides and atmospheric nucleation precursors (sulfuric acid, ammonia and dimethylamine) were further analyzed to identify the potential role of aromatic sulfuric anhydrides in NPF. As the thermodynamic stability of a cluster depends on both the number and strength of hydrogen bonds, the greater stability of the interactions between atmospheric nucleation precursors and aromatic sulfuric anhydrides than with aromatic acids make aromatic sulfuric anhydrides potential participators in the nucleation process of NPF. Moreover, compared with BA, the addition of a -CH2- functional group in PAA has little influence on the reaction barrier with SO3 but an inhibitive effect on the thermodynamic stability of clusters. The position of the two -COOH functional groups in PA, mPA and PTA does not have a consistent impact on the reaction barrier with SO3 or the thermodynamic stability.


Assuntos
Atmosfera , Ácidos Sulfúricos , Humanos , Atmosfera/química , Ácidos Sulfúricos/química , Dióxido de Enxofre , Termodinâmica , Ligação de Hidrogênio , Anidridos
16.
J Environ Sci (China) ; 131: 11-25, 2023 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-37225372

RESUMO

To understand the contribution of new particle formation (NPF) events to ambient fine particle pollution, measurements of particle size distributions, trace gases and meteorological conditions, were conducted at a suburban site (NJU) from October to December 2016 and at an industrial site (NUIST) from September to November 2015 in Nanjing. According to the temporal evolution of the particle size distributions, three types NPF events were observed: typical NPF (Type A), moderate NPF events (Type B) and strong NPF (Type C) events. The favorable conditions for Type A events included low relative humidity, low concentration of pre-existing particles, and high solar radiation. The favorable conditions of Type B events were similar to Type A, except for a higher concentration of pre-existing particles. Type C events were more likely to happen with the higher relative humidity, lower solar radiation and continuous growth of pre-existing particle concentration. The formation rate of 3 nm (J3) was the lowest for Type A events and highest for Type C events. In contrast, the growth rates of 10 nm and 40 nm particles were the highest for Type A, and lowest for Type C. Results show that NPF events with only higher J3 would lead to the accumulation of nucleation mode particles. Sulfuric acid was important for the formation of particles but had little effect on the growth of particle size.


Assuntos
Meio Ambiente , Poluição Ambiental , China , Gases , Umidade
17.
J Environ Sci (China) ; 123: 327-340, 2023 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-36521996

RESUMO

A compilation of new advances made in the research field of laboratory reaction kinetics in China's Key Development Project for Air Pollution Formation Mechanism and Control Technologies was presented. These advances are grouped into six broad, interrelated categories, including volatile organic compound (VOC) oxidation, secondary organic aerosol (SOA) formation, new particle formation (NPF) and gas-particle partitioning, ozone chemistry, model parameters, and secondary inorganic aerosol (SIA) formation, highlighting the laboratory work done by Chinese researchers. For smog chamber applications, the current knowledge gained from laboratory studies is reviewed, with emphasis on summarizing the oxidation mechanisms of long-chain alkanes, aromatics, alkenes, aldehydes/ketones in the atmosphere, SOA formation from anthropogenic emission sources, and oxidation of aromatics, isoprene, and limonene, as well as SIA formation. For flow tube applications, atmospheric oxidation mechanisms of toluene and methacrolein, SOA formation from limonene oxidation by ozone, gas-particle partitioning of peroxides, and sulfuric acid-water (H2SO4-H2O) binary nucleation, methanesulfonic acid-water (MSA-H2O) binary nucleation, and sulfuric acid-ammonia-water (H2SO4-NH3-H2O) ternary nucleation are discussed.


Assuntos
Poluentes Atmosféricos , Poluição do Ar , Ozônio , Cinética , Limoneno , Aerossóis/análise , Ozônio/química , Poluição do Ar/prevenção & controle , Água , China , Poluentes Atmosféricos/análise
18.
Ecotoxicol Environ Saf ; 243: 114023, 2022 Sep 15.
Artigo em Inglês | MEDLINE | ID: mdl-36030686

RESUMO

Ultrafine particles (UFPs) usually explosive growth during new particle formation (NPF) events. However, the risk of exposure to UFPs on NPF days has been ignored due to the prevalence of mass-based air quality standards. In this study, the daily deposited doses, i.e., the daily deposited particle number dose (DPNd), mass dose (DPMd), and surface area dose (DPSd), of ambient particles in the human respiratory tract in Beijing were evaluated based on the particle number size distribution (3 nm-10 µm) from June 2018 to May 2019 utilizing a Multiple-Path Particle Dosimetry Model (MPPD) after the hygroscopic growth of particles in the respiratory tract had been accounted for. Our observations showed a high frequency (72.6%) of NPF on excellent air quality days, with daily mean PM2.5 concentrations less than 35 µg m-3. The daily DPNd on excellent air quality days was comparable with that on polluted days, although the DPMd on excellent air quality days was as low as 15.6% of that on polluted days. The DPNd on NPF days was ~1.3 times that on non-NPF days. The DPNd in respiratory tract regions decreased in the order: tracheobronchial (TB) > pulmonary (PUL) > extrathoracic (ET) on NPF days, while it was PUL > TB > ET on non-NPF days. The number of deposited nucleation mode particles, which were deposited mainly in the TB region (45%), was 2 times higher on NPF days than that on non-NPF days. Our results demonstrated that the deposition potential due to UFPs in terms of particle number concentrations is high in Beijing regardless of the aerosol mass concentration. More toxicological studies related to UFPs on NPF days, especially those targeting tracheobronchial and pulmonary impairment, are required in the future.


Assuntos
Poluentes Atmosféricos , Poluentes Atmosféricos/análise , Poluentes Atmosféricos/toxicidade , Pequim , Monitoramento Ambiental , Humanos , Pulmão/química , Tamanho da Partícula , Material Particulado/análise
19.
J Environ Manage ; 304: 114232, 2022 Feb 15.
Artigo em Inglês | MEDLINE | ID: mdl-34933267

RESUMO

Real-time measurements of particles in the 15-736 nm range have been obtained by a Scanning Mobility Particle Sizer to characterize the evolution of particle size distribution and new particle formation (NPF) events in an urban background area. The annual, weekly and diurnal variations of the modal (nucleation (Nnuc), Aitken (NAit) and accumulation (Nacc)) particle concentrations were characterised. The NAit and Nacc registered their maximums in cold months during rush hours, in the morning (0600-0900 UTC) and in the afternoon (1700-2000 UTC), while the maximums for Nnuc were reached in warm months during midday hours. NAit, Nacc and Ntotal showed a significant negative correlation with wind speed and a different relationship with the planetary boundary layer (PBL) height by periods. In the warm period, a positive significant correlation between PBL and Nnuc was registered, indicating that the higher dispersion promoted by a high PBL causes favourable conditions for the occurrence of NPF events (a low polluted atmosphere). NPF processes are one of the main sources of ultrafine particles (<100 nm) in the warm period. After a visual-based classification, 45 NPF events of type Ia (strong and with a good confidence level) were identified and analysed, occurring primarily between 1100 and 1500 UTC, mainly in spring and summer. In addition, a two-step method was developed for identifying NPF events: cluster analysis followed by discriminant analysis. The application of discriminant analysis to one of the clusters, grouping 93 days, enabled us to identify 55 of the 56 NPF events days included in the cluster. This method is a valuable tool for identifying NPF events quickly and effectively.


Assuntos
Poluentes Atmosféricos , Aerossóis/análise , Poluentes Atmosféricos/análise , Monitoramento Ambiental , Tamanho da Partícula , Material Particulado/análise , Espanha
20.
J Environ Sci (China) ; 111: 75-83, 2022 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-34949375

RESUMO

New particle formation (NPF) events are an increasingly interesting topic in air quality and climate science. In this study, the particle number size distributions, and the frequency of NPF events over Hefei were investigated from November 2018 to February 2019. The proportions of the nucleation mode, Aitken mode, and accumulation mode were 24.59%, 53.10%, and 22.30%, respectively, which indicates the presence of abundant ultrafine particles in Hefei. Forty-six NPF events occurred during the observation days, accounting for 41.82% of the entire observation period. Moreover, the favorable meteorological conditions, potential precursor gases, and PM2.5 range of the NPF events were analyzed. Compared to non-NPF days, the NPF events preferentially occurred on days with lower relative humidity, higher wind speeds, and higher temperatures. When the PM2.5 was 15-20, 70-80, and 105-115 µg/m3, the frequency of the NPF events was higher. Nucleation mode particles were positively related to atmospheric oxidation indicated by ozone when PM2.5 ranged from 15 to 20 µg/m3, and related to gaseous precursors like SO2 and NO2 when PM2.5 was located at 70-80 and 105-115 µg/m3. On pollution days, NPF events did not directly contribute to the increase in the PM2.5 in the daytime, however, NPF events would occur during the night and the growth of particulate matter contributes to the nighttime PM2.5 contents. This could lead to pollution that lasted into the next day. These findings are significant to the improvement of our understanding of the effects of aerosols on air quality.


Assuntos
Poluentes Atmosféricos , Poluição do Ar , Ozônio , Poluentes Atmosféricos/análise , Poluição do Ar/análise , China , Monitoramento Ambiental , Tamanho da Partícula , Material Particulado/análise , Rios , Estações do Ano
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