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1.
Environ Sci Pollut Res Int ; 29(11): 16233-16249, 2022 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-34642887

RESUMO

Particulate matter is usually regarded as the dominant pollutant in Tehran megacity in Iran. However, the number of ozone exceedance days significantly increased in recent years. This study analyzes simultaneous measurements of O3 and NOx (NO+NO2) concentrations to improve our understanding of ozone evolution during the summers of 2017 to 2019. The k-means clustering technique was used to select five representative air quality monitoring sites in Tehran to capture O3 and NOx concentrations' variability. The findings show that all of the investigated sites failed to meet the ozone non-attainment criterion. The ozone weekend effect is seen in the study of weekday/weekend differences in 2017 and 2018, but not in 2019, which can be due to the shift in the ozone production regime. The summer mean variation analysis can also be used to deduce this regime change. In 2017, the O3 and NO2 summer mean variations suggest a holdback in the NO2 upward trend and a reversal in the O3 downward trend that had been in place since 2012. Air mass back trajectory clustering reveals that east and north-east air mass clusters have the most significant impact on Tehran's O3 pollution and the highest regional contribution to OX. The study of OX against NOx shows that the regional contribution to OX increased from 2017 to 2018 and then decreased in 2019; however, the local contribution is the opposite. The diurnal analysis of the regional and local contributions to OX indicated that OX in Tehran might be primarily affected by pollutants from a short distance. The findings reveal critical changes in the behavior of O3 in recent years, indicating that decision-makers in Tehran should reconsider air pollution control measures.


Assuntos
Poluentes Atmosféricos , Poluição do Ar , Ozônio , Poluentes Atmosféricos/análise , Poluição do Ar/análise , Análise por Conglomerados , Monitoramento Ambiental , Irã (Geográfico) , Ozônio/análise
2.
Anal Chem ; 92(1): 1316-1325, 2020 01 07.
Artigo em Inglês | MEDLINE | ID: mdl-31825206

RESUMO

Metal emissions are of major environmental and practical concern because of their highly toxic effects on human health and ecosystems. Current technologies available in the market for their detection are typically limited by a time resolution of 1 h or longer (e.g., via semicontinuous X-ray fluorescence measurements) or are nonquantitative (e.g., laser ablation mass spectrometry). In this work, we report the development of a novel technique for the real-time detection and monitoring of metal particles in situ using an extractive electrospray ionization (EESI) source coupled to a high-resolution time-of-flight mass spectrometer (TOF-MS). The experiments were conducted in negative ionization mode using disodium ethylenediamine tetraacetic acid (EDTA) dihydrate to chelate with metals and form stable metal complexes. Results for water-soluble metal compounds were obtained. The following representative metal ions were examined: Pb, Cd, Zn, Ce (III), Ba, Ni, Fe(II), Fe(III), Cu(II), Cr, Mo, Co(II), Mg, Nd, Li, Ti, Ca, Cs, Ag, Tm, Er(III), La(III), Yb(III), Eu(III), Pr(III), Gd(III), Lu(III), Dy(III), Tb(III), Ho, and Ru(III). The results showed a very good linear mass response (R2 = 0.9983), low ng/m3 limits of detection (LoD), and a fast response time (1 s). The stability and repeatability of the developed EESI-TOF-MS were tested under complex dynamic and periodic experimental conditions, and negligible matrix effects were measured for internally and externally mixed metal particles. Benchmark testing against inductively coupled plasma-mass spectrometry (ICP-MS) was also performed, highlighting the online measurement capabilities of aerosol metals with a LoD lower than those of ICP-MS. Proof-of-concept ambient measurements were performed in New Delhi, India, and very promising results were obtained, allowing further exploitation elsewhere.


Assuntos
Metais Pesados/análise , Aerossóis/análise , Ácido Edético/química , Espectrometria de Massas por Ionização por Electrospray , Fatores de Tempo
3.
Environ Sci Technol ; 53(4): 2209-2219, 2019 02 19.
Artigo em Inglês | MEDLINE | ID: mdl-30648378

RESUMO

We have systematically examined the gas and particle phase emissions from seven wood combustion devices. Among total carbon mass emitted (excluding CO2), CO emissions were dominant, together with nonmethane volatile organic compounds (NMVOCs) (10-40%). Automated devices emitted 1-3 orders of magnitude lower CH4 (0.002-0.60 g kg-1 of wood) and NMVOCs (0.01-1 g kg-1 of wood) compared to batch-operated devices (CH4: 0.25-2.80 g kg-1 of wood; NMVOCs: 2.5-19 g kg-1 of wood). 60-90% of the total NMVOCs were emitted in the starting phase of batch-operated devices, except for the first load cycles. Partial-load conditions or deviations from the normal recommended operating conditions, such as use of wet wood/wheat pellets, oxygen rich or deficit conditions, significantly enhanced the emissions. NMVOCs were largely dominated by small carboxylic acids and alcohols, and furans. Despite the large variability in NMVOCs emission strengths, the relative contribution of different classes showed large similarities among different devices and combustion phases. We show that specific improper operating conditions may even for advanced technology not result in the emission reduction of secondary organic aerosol (SOA) forming compounds and thus not reduce the impact of wood combustion on climate and health.


Assuntos
Poluentes Atmosféricos , Material Particulado , Aerossóis , Biomassa , Madeira
5.
Environ Sci Technol ; 51(18): 10624-10632, 2017 Sep 19.
Artigo em Inglês | MEDLINE | ID: mdl-28816442

RESUMO

An aerosol chemical speciation monitor (ACSM) was deployed to study the primary nonrefractory submicron particulate matter emissions from the burning of commercially available solid fuels (peat, coal, and wood) typically used in European domestic fuel stoves. Organic mass spectra (MS) from burning wood, peat, and coal were characterized and intercompared for factor analysis against ambient data. The reference profiles characterized in this study were used to estimate the contribution of solid fuel sources, along with oil combustion, to ambient pollution in Galway, Ireland using the multilinear engine (ME-2). During periods influenced by marine air masses, local source contribution had dominant impact and nonsea-spray primary organic emissions comprised 88% of total organic aerosol mass, with peat burning found to be the greatest contributor (39%), followed by oil (21%), coal (17%), and wood (11%). In contrast, the resolved oxygenated organic aerosol (OOA) dominated the aerosol composition in continental air masses, with contributions of 50%, compared to 12% in marine air masses. The source apportionment results suggest that the use of domestic solid fuels (peat, wood, and coal) for home heating is the major source of evening and night-time particulate pollution events despite their small use.


Assuntos
Poluentes Atmosféricos/análise , Aerossóis , Carvão Mineral , Monitoramento Ambiental , Incineração , Irlanda , Material Particulado , Solo , Madeira
6.
Sci Data ; 4: 170003, 2017 03 14.
Artigo em Inglês | MEDLINE | ID: mdl-28291234

RESUMO

Cloud condensation nuclei (CCN) number concentrations alongside with submicrometer particle number size distributions and particle chemical composition have been measured at atmospheric observatories of the Aerosols, Clouds, and Trace gases Research InfraStructure (ACTRIS) as well as other international sites over multiple years. Here, harmonized data records from 11 observatories are summarized, spanning 98,677 instrument hours for CCN data, 157,880 for particle number size distributions, and 70,817 for chemical composition data. The observatories represent nine different environments, e.g., Arctic, Atlantic, Pacific and Mediterranean maritime, boreal forest, or high alpine atmospheric conditions. This is a unique collection of aerosol particle properties most relevant for studying aerosol-cloud interactions which constitute the largest uncertainty in anthropogenic radiative forcing of the climate. The dataset is appropriate for comprehensive aerosol characterization (e.g., closure studies of CCN), model-measurement intercomparison and satellite retrieval method evaluation, among others. Data have been acquired and processed following international recommendations for quality assurance and have undergone multiple stages of quality assessment.

7.
Nat Commun ; 5: 5146, 2014 Oct 14.
Artigo em Inglês | MEDLINE | ID: mdl-25312205

RESUMO

The key issue for the implementation of a metamaterial is to demonstrate the existence of collective modes corresponding to coherent oscillations of the meta-atoms. Atoms of natural materials interact with electromagnetic fields as quantum two-level systems. Artificial quantum two-level systems can be made, for example, using superconducting nonlinear resonators cooled down to their ground state. Here we perform an experiment in which 20 of these quantum meta-atoms, so-called flux qubits, are embedded into a microwave resonator. We observe the dispersive shift of the resonator frequency imposed by the qubit metamaterial and the collective resonant coupling of eight qubits. The realized prototype represents a mesoscopic limit of naturally occurring spin ensembles and as such we demonstrate the AC-Zeeman shift of a resonant qubit ensemble. The studied system constitutes the implementation of a basic quantum metamaterial in the sense that many artificial atoms are coupled collectively to the quantized mode of a photon field.

8.
Nature ; 503(7475): 242-6, 2013 Nov 14.
Artigo em Inglês | MEDLINE | ID: mdl-24226888

RESUMO

Single magnetic atoms, and assemblies of such atoms, on non-magnetic surfaces have recently attracted attention owing to their potential use in high-density magnetic data storage and as a platform for quantum computing. A fundamental problem resulting from their quantum mechanical nature is that the localized magnetic moments of these atoms are easily destabilized by interactions with electrons, nuclear spins and lattice vibrations of the substrate. Even when large magnetic fields are applied to stabilize the magnetic moment, the observed lifetimes remain rather short (less than a microsecond). Several routes for stabilizing the magnetic moment against fluctuations have been suggested, such as using thin insulating layers between the magnetic atom and the substrate to suppress the interactions with the substrate's conduction electrons, or coupling several magnetic moments together to reduce their quantum mechanical fluctuations. Here we show that the magnetic moments of single holmium atoms on a highly conductive metallic substrate can reach lifetimes of the order of minutes. The necessary decoupling from the thermal bath of electrons, nuclear spins and lattice vibrations is achieved by a remarkable combination of several symmetries intrinsic to the system: time reversal symmetry, the internal symmetries of the total angular momentum and the point symmetry of the local environment of the magnetic atom.

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