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1.
Proc Natl Acad Sci U S A ; 119(32): e2201729119, 2022 Aug 09.
Artículo en Inglés | MEDLINE | ID: mdl-35917351

RESUMEN

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.

2.
Environ Sci Technol ; 58(2): 1236-1243, 2024 Jan 16.
Artículo en Inglés | MEDLINE | ID: mdl-38169373

RESUMEN

Aqueous-phase reactions of α-dicarbonyls with amines or ammonium have been identified as important sources of secondary brown carbon (BrC). However, the kinetics of BrC formation and the effects of pH are still not very clear. In this study, the kinetics of BrC formation by aqueous reactions of α-dicarbonyls (glyoxal and methylglyoxal) with ammonium, amino acids, or alkylamines in bulk solution at different pH values are investigated. Our results reveal pH-parameterized BrC production rate constants, kBrCII (m-1 [M]-2 s-1), based on the light absorption between 300 and 500 nm: log10(kBrCII) = (1.0 ± 0.1) × pH - (7.4 ± 1.0) for reactions with glyoxal and log10(kBrCII) = (1.0 ± 0.1) × pH - (6.3 ± 0.9) for reactions with methylglyoxal. The linear slopes closing to 1.0 indicate that BrC formation is governed by the nitrogen nucleophilic addition pathway. Consequently, the absorptivities of the produced BrC increase exponentially with the increase of pH. BrC from reactions with methylglyoxal at higher pH (≥6.5) exhibits optical properties comparable to BrC from biomass burning or coal combustion, categorized as the "weakly" absorbing BrC, while BrC from reactions with methylglyoxal at lower pH (<6.0) or reactions with glyoxal (pH 5.0-7.0) falls into the "very weakly" absorbing BrC. The pH-dependent BrC feature significantly affects the solar absorption ability of the produced BrC and thus the atmospheric photochemical processes, e.g., BrC produced at pH 7.0 absorbs 14-16 times more solar power compared to that at pH 5.0, which in turn could lead to a decrease of 1 order of magnitude in the photolysis rate constants of O3 and NO2.


Asunto(s)
Contaminantes Atmosféricos , Compuestos de Amonio , Piruvaldehído/química , Fotoquímica , Carbono , Aerosoles/análisis , Aminas , Glioxal , Agua/química , Concentración de Iones de Hidrógeno
3.
Environ Sci Technol ; 58(18): 7947-7957, 2024 May 07.
Artículo en Inglés | MEDLINE | ID: mdl-38676647

RESUMEN

Volatility of organic aerosols (OAs) significantly influences new particle formation and the occurrence of particulate air pollution. However, the relationship between the volatility of OA and the level of particulate air pollution (i.e., particulate matter concentration) is not well understood. In this study, we compared the chemical composition (identified by an ultrahigh-resolution Orbitrap mass spectrometer) and volatility (estimated based on a predeveloped parametrization method) of OAs in urban PM2.5 (particulate matter with aerodynamic diameter ≤ 2.5 µm) samples from seven German and Chinese cities, where the PM2.5 concentration ranged from a light (14 µg m-3) to heavy (319 µg m-3) pollution level. A large fraction (71-98%) of compounds in PM2.5 samples were attributable to intermediate-volatility organic compounds (IVOCs) and semivolatile organic compounds (SVOCs). The fraction of low-volatility organic compounds (LVOCs) and extremely low-volatility organic compounds (ELVOCs) decreased from clean (28%) to heavily polluted urban regions (2%), while that of IVOCs increased from 34 to 62%. We found that the average peak area-weighted volatility of organic compounds in different cities showed a logarithmic correlation with the average PM2.5 concentration, indicating that the volatility of urban OAs increases with the increase of air pollution level. Our results provide new insights into the relationship between OA volatility and PM pollution levels and deepen the understanding of urban air pollutant evolution.


Asunto(s)
Aerosoles , Contaminantes Atmosféricos , Contaminación del Aire , Espectrometría de Masas , Material Particulado , Material Particulado/análisis , Contaminantes Atmosféricos/análisis , Monitoreo del Ambiente/métodos , Volatilización , Compuestos Orgánicos/análisis , China , Compuestos Orgánicos Volátiles/análisis
4.
Environ Sci Technol ; 58(8): 3629-3640, 2024 Feb 27.
Artículo en Inglés | MEDLINE | ID: mdl-38354315

RESUMEN

Key stages in people's lives have particular relevance for their health; the life-course approach stresses the importance of these stages. Here, we applied a life-course approach to analyze the health risks associated with PM2.5-bound elements, which were measured at three sites with varying environmental conditions in eastern China. Road traffic was found to be the primary source of PM2.5-bound elements at all three locations, but coal combustion was identified as the most important factor to induce both cancer risk (CR) and noncancer risk (NCR) across all age groups due to the higher toxicity of elements such as As and Pb associated with coal. Nearly half of NCR and over 90% of CR occurred in childhood (1-6 years) and adulthood (>18 years), respectively, and females have slightly higher NCR and lower CR than males. Rural population is found to be subject to the highest health risks. Synthesizing previous relevant studies and nationwide PM2.5 concentration measurements, we reveal ubiquitous and large urban-rural environmental exposure disparities over China.


Asunto(s)
Contaminantes Atmosféricos , Material Particulado , Masculino , Femenino , Humanos , Material Particulado/análisis , Contaminantes Atmosféricos/análisis , Estaciones del Año , Monitoreo del Ambiente , Medición de Riesgo , China/epidemiología , Carbón Mineral/análisis
5.
Environ Sci Technol ; 58(12): 5453-5460, 2024 Mar 26.
Artículo en Inglés | MEDLINE | ID: mdl-38477969

RESUMEN

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.


Asunto(s)
Bosques , Metilaminas , Granjas , China , Suelo
6.
Environ Sci Technol ; 58(24): 10652-10663, 2024 Jun 18.
Artículo en Inglés | MEDLINE | ID: mdl-38829825

RESUMEN

Secondary organic aerosol (SOA) formation from gasoline vehicles spanning a wide range of emission types was investigated using an oxidation flow reactor (OFR) by conducting chassis dynamometer tests. Aided by advanced mass spectrometric techniques, SOA precursors, including volatile organic compounds (VOCs) and intermediate/semivolatile organic compounds (I/SVOCs), were comprehensively characterized. The reconstructed SOA produced from the speciated VOCs and I/SVOCs can explain 69% of the SOA measured downstream of an OFR upon 0.5-3 days' OH exposure. While VOCs can only explain 10% of total SOA production, the contribution from I/SVOCs is 59%, with oxygenated I/SVOCs (O-I/SVOCs) taking up 20% of that contribution. O-I/SVOCs (e.g., benzylic or aliphatic aldehydes and ketones), as an obscured source, account for 16% of total nonmethane organic gas (NMOG) emission. More importantly, with the improvement in emission standards, the NMOG is effectively mitigated by 35% from China 4 to China 6, which is predominantly attributed to the decrease of VOCs. Real-time measurements of different NMOG components as well as SOA production further reveal that the current emission control measures, such as advances in engine and three-way catalytic converter (TWC) techniques, are effective in reducing the "light" SOA precursors (i.e., single-ring aromatics) but not for the I/SVOC emissions. Our results also highlight greater effects of O-I/SVOCs to SOA formation than previously observed and the urgent need for further investigation into their origins, i.e., incomplete combustion, lubricating oil, etc., which requires improvements in real-time molecular-level characterization of I/SVOC molecules and in turn will benefit the future design of control measures.


Asunto(s)
Aerosoles , Gasolina , Emisiones de Vehículos , Compuestos Orgánicos Volátiles , Contaminantes Atmosféricos/química , Compuestos Orgánicos/química
7.
Environ Sci Technol ; 57(33): 12351-12361, 2023 08 22.
Artículo en Inglés | MEDLINE | ID: mdl-37542457

RESUMEN

Aqueous-phase reactions of α-dicarbonyls with ammonium or amines have been identified as important sources of secondary brown carbon (BrC). However, the identities of most chromophores in these reactions and the effects of pH remain largely unknown. In this study, the chemical structures, formation pathways, and optical properties of individual BrC chromophores formed through aqueous reactions of α-dicarbonyls (glyoxal and methylglyoxal) with ammonium, amino acids, or methylamine at different pH's were characterized in detail by liquid chromatography-photodiode array-high resolution tandem mass spectrometry. In total, 180 chromophores are identified, accounting for 29-79% of the light absorption of bulk BrC for different reactions. Thereinto, 155 newly identified chromophores, including 76 imidazoles, 57 pyrroles, 10 pyrazines, 9 pyridines, and 3 imidazole-pyrroles, explain additionally 9-69% of the light absorption, and these chromophores mainly involve four formation pathways, including previously unrecognized reactions of ammonia or methylamine with the methylglyoxal dimer for the formation of pyrroles. The pH in these reactions also shows remarkable effects on the formation and transformation of BrC chromophores; e.g., with the increase of pH from 5.0 to 7.0, the light absorption contributions of imidazoles in identified chromophores decrease from 72% to 65%, while the light absorption contributions of pyrazines increase from 5% to 13% for the methylglyoxal + ammonium reaction; meanwhile, more small nitrogen heterocycles transformed into oligomers (e.g., C9 and C12 pyrroles) via reaction with methylglyoxal. These newly identified chromophores and proposed formation pathways are instructive for future field studies of the formation and transformation of aqueous-phase BrC.


Asunto(s)
Aminas , Compuestos de Amonio , Piruvaldehído/química , Carbono , Aerosoles/análisis , Agua/química , Metilaminas , Pirroles
8.
Environ Sci Technol ; 57(38): 14269-14279, 2023 09 26.
Artículo en Inglés | MEDLINE | ID: mdl-37698874

RESUMEN

Methylsiloxanes have gained growing attention as emerging pollutants due to their toxicity to organisms. As man-made chemicals with no natural source, most research to date has focused on volatile methylsiloxanes from personal care or household products and industrial processes. Here, we show that methylsiloxanes can be found in primary aerosol particles emitted by vehicles based on aerosol samples collected in two tunnels in São Paulo, Brazil. The aerosol samples were analyzed with thermal desorption-proton transfer reaction-mass spectrometry (TD-PTR-MS), and methylsiloxanes were identified and quantified in the mass spectra based on the natural abundance of silicon isotopes. Various methylsiloxanes and derivatives were found in aerosol particles from both tunnels. The concentrations of methylsiloxanes and derivatives ranged 37.7-377 ng m-3, and the relative fractions in organic aerosols were 0.78-1.9%. The concentrations of methylsiloxanes exhibited a significant correlation with both unburned lubricating oils and organic aerosol mass. The emission factors of methylsiloxanes averaged 1.16 ± 0.59 mg kg-1 of burned fuel for light-duty vehicles and 1.53 ± 0.37 mg kg-1 for heavy-duty vehicles. Global annual emissions of methylsiloxanes in vehicle-emitted aerosols were estimated to range from 0.0035 to 0.0060 Tg, underscoring the significant yet largely unknown potential for health and climate impacts.


Asunto(s)
Contaminantes Ambientales , Emisiones de Vehículos , Humanos , Brasil , Aerosoles , Clima
9.
Sensors (Basel) ; 23(16)2023 Aug 14.
Artículo en Inglés | MEDLINE | ID: mdl-37631698

RESUMEN

The accurate voltage measurement of distribution networks is of great significance in power dispatching and fault diagnosis. Voltage sensors based on the spatial electric field effect do not require grounding, which provides the possibility for the distributed measurement of transmission line voltages. However, the divider ratio of suspension grounding voltage sensors is affected by the height between the sensor and the ground, as well as the distance between the sensor and the telegraph pole. In this paper, a self-calibration method based on internal capacitance transformation is proposed to realize the on-line calibration of suspension grounding voltage sensors. The calibration is accomplished by switching different parameters in the conditioning circuit, and the calibration process does not require power failure or known input excitation. In addition, the impact of electric fields in the other two phases of three-phase transmission lines on measurement through simulation research is quantified in this paper. In order to reduce the impact of interference electric fields, an equipotential shielding structure is designed. The circuit topology and probe prototype have been developed and testing has been conducted in laboratory conditions; the experimental results show that the maximum relative error of voltage amplitude is 1.65%, and the phase relative error is 0.94%. The measurement accuracy is not limited by the height to ground or the distance to the telegraph pole. In addition, in the application of an equipotential shielding probe, the maximum deviation of measured voltage is 0.7% with and without interference electric fields.

10.
Sensors (Basel) ; 23(8)2023 Apr 10.
Artículo en Inglés | MEDLINE | ID: mdl-37112192

RESUMEN

Noncontact voltage measurement has the advantages of simple handling, high construction safety, and not being affected by line insulation. However, in practical measurement of noncontact voltage, sensor gain is affected by wire diameter, wire insulation material, and relative position deviation. At the same time, it is also subject to interference from interphase or peripheral coupling electric fields. This paper proposes a noncontact voltage measurement self-calibration method based on dynamic capacitance, which realizes self-calibration of sensor gain through unknown line voltage to be measured. Firstly, the basic principle of the self-calibration method for noncontact voltage measurement based on dynamic capacitance is introduced. Subsequently, the sensor model and parameters were optimized through error analysis and simulation research. Based on this, a sensor prototype and remote dynamic capacitance control unit that can shield against interference are developed. Finally, the accuracy test, anti-interference ability test, and line adaptability test of the sensor prototype were conducted. The accuracy test showed that the maximum relative error of voltage amplitude was 0.89%, and the phase relative error was 1.57%. The anti-interference ability test showed that the error offset was 0.25% when there were interference sources. The line adaptability test shows that the maximum relative error in testing different types of lines is 1.01%.

11.
Sensors (Basel) ; 23(5)2023 Feb 21.
Artículo en Inglés | MEDLINE | ID: mdl-36904593

RESUMEN

Three-phase four-wire power cables are a primary kind of power transmission method in low-voltage distribution networks. This paper addresses the problem that calibration currents are not easily electrified during the transporting of three-phase four-wire power cable measurements, and proposes a method for obtaining the magnetic field strength distribution in the tangential direction around the cable, finally enabling online self-calibration. The simulation and experimental results show that this method can self-calibrate the sensor arrays and reconstruct the phase current waveforms in three-phase four-wire power cables without calibration currents, and this method is not affected by disturbances such as wire diameter, current amplitudes, and high-frequency harmonics. This study reduces the time and equipment costs required to calibrate the sensing module compared to related studies using calibration currents. This research offers the possibility of fusing sensing modules directly with running primary equipment, and the development of hand-held measurement devices.

12.
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.

13.
Proc Natl Acad Sci U S A ; 116(18): 8657-8666, 2019 04 30.
Artículo en Inglés | MEDLINE | ID: mdl-30988177

RESUMEN

Regional severe haze represents an enormous environmental problem in China, influencing air quality, human health, ecosystem, weather, and climate. These extremes are characterized by exceedingly high concentrations of fine particulate matter (smaller than 2.5 µm, or PM2.5) and occur with extensive temporal (on a daily, weekly, to monthly timescale) and spatial (over a million square kilometers) coverage. Although significant advances have been made in field measurements, model simulations, and laboratory experiments for fine PM over recent years, the causes for severe haze formation have not yet to be systematically/comprehensively evaluated. This review provides a synthetic synopsis of recent advances in understanding the fundamental mechanisms of severe haze formation in northern China, focusing on emission sources, chemical formation and transformation, and meteorological and climatic conditions. In particular, we highlight the synergetic effects from the interactions between anthropogenic emissions and atmospheric processes. Current challenges and future research directions to improve the understanding of severe haze pollution as well as plausible regulatory implications on a scientific basis are also discussed.


Asunto(s)
Contaminantes Atmosféricos/análisis , Contaminación del Aire/análisis , China , Ecosistema , Monitoreo del Ambiente , Humanos , Material Particulado/análisis
14.
Sensors (Basel) ; 22(21)2022 Nov 07.
Artículo en Inglés | MEDLINE | ID: mdl-36366268

RESUMEN

Traditional contact voltage measurement requires a direct electrical connection to the system, which is not easy to install and maintain. The voltage measurement based on the electric field coupling plate capacitance structure does not need to be in contact with the measured object or the ground, which can avoid the above problems. However, most of the existing flat-plate structure voltage measurement sensors are not only expensive to manufacture, but also bulky, and when the relative position between the wire under test and the sensor changes, it will bring great measurement errors, making it difficult to meet actual needs. Aiming to address the above problems, this paper proposes a multi-electrode array structure non-contact voltage sensor and signal processing algorithm. The sensor is manufactured by the PCB process, which effectively reduces the manufacturing cost and process difficulty. The experimental and simulation results show that, when the relative position of the wire and the sensor is offset by 10 mm in the 45° direction, the relative error of the traditional single-electrode voltage sensor is 17.62%, while the relative error of the multi-electrode voltage sensor designed in this paper is only 0.38%. In addition, the ratio error of the sensor under the condition of power frequency of 50 Hz is less than ±1% and the phase difference is less than 4°. The experimental results show that the sensor has good accuracy and linearity.


Asunto(s)
Algoritmos , Procesamiento de Señales Asistido por Computador , Electrodos , Capacidad Eléctrica
15.
J Environ Sci (China) ; 114: 365-375, 2022 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-35459499

RESUMEN

The health effects of trace metal elements in atmospheric fine particulate matter (PM2.5) are widely recognized, however, the emission factor profiles and chemical fractionation of metal elements in different sources were poorly understand. In this study, sixteen metal elements, including Cd, Pb, V, Zn, Ba, Sb, As, Fe, Sr, Cr, Rb, Co, Mn, Cu, Ni and Sn from biomass burning, bituminite and anthracite combustion, as well as dust, were quantified. The results show different emission sources were associated with distinct emission profiles, holding important implications for source apportionment of ambient particulate metals. Specifically, Fe was the dominant metal species (28-1922 mg/kg) for all samples, and was followed by different metals for different samples. For dust, Mn (39.9 mg/kgdust) had the second-highest emission factor, while for biomass burning, it was Cr and Ba (7.5 and 7.4 mg/kgbiomass, respectively). For bituminous coal combustion, the emission factor of Zn and Ba was 6.2 and 6.0 mg/kgbituminous, respectively, while for anthracite combustion the corresponding emission factor was 5.6 and 4.3 mg/kganthracite, respectively. Moreover, chemical fractionation (i.e., the exchangeable, reducible fraction, oxidizable, and residual fraction) and the bioavailability index (BI) values of the metal elements from different sources were further investigated to reveal the link between different emission sources and the potential health risk. The findings from this study hold important implications for source apportionment and source-specific particulate metal-associated health effects.


Asunto(s)
Contaminantes Atmosféricos , Metales Pesados , Oligoelementos , Contaminantes Atmosféricos/análisis , Fraccionamiento Químico , Carbón Mineral , Polvo , Monitoreo del Ambiente/métodos , Metales/análisis , Metales Pesados/análisis , Material Particulado/análisis , Oligoelementos/análisis
16.
Rapid Commun Mass Spectrom ; 35(14): e9113, 2021 Jul 31.
Artículo en Inglés | MEDLINE | ID: mdl-33908097

RESUMEN

RATIONALE: Organic aerosols (OA) account for a large fraction of atmospheric fine particulate matter and thus are affecting climate and public health. Elucidation of the chemical composition of OA is the key for addressing the role of ambient fine particles at the atmosphere-biosphere interface and mass spectrometry is the main method to achieve this goal. METHODS: High-resolution mass spectrometry (HRMS) is on its way to becoming one of the most prominent analytical techniques, also for the analysis of atmospheric aerosols. The combination of high mass resolution and accurate mass determination allows the elemental compositions of numerous compounds to be easily elucidated. Here a new parameter for the improved classification of OA is introduced - the maximum carbonyl ratio (MCR) - which is directly derived from the molecular composition and is particularly suitable for the identification and characterization of secondary organic aerosols (SOA). RESULTS: The concept is exemplified by the analysis of ambient OA samples from two measurement sites (Hyytiälä, Finland; Beijing, China) and of laboratory-generated SOA based on ultrahigh-performance liquid chromatography (UHPLC) coupled to Orbitrap MS. To interpret the results, MCR-Van Krevelen (VK) diagrams are generated for the different OA samples and the individual compounds are categorized into specific areas in the diagrams. The results show that the MCR index is a valuable parameter for representing atmospheric SOA components in composition and structure-dependent visualization tools such as VK diagrams. CONCLUSIONS: The MCR index is suggested as a tool for a better characterization of the sources and the processing of atmospheric OA components based on HRMS data. Since the MCR contains information on the concentration of highly electrophilic organic compounds in particulate matter (PM) as well as on the concentration of organic (hydro)peroxides, the MCR could be a promising metric for identifying health-related particulate matter parameters by HRMS.

17.
Environ Sci Technol ; 55(11): 7276-7286, 2021 06 01.
Artículo en Inglés | MEDLINE | ID: mdl-34009957

RESUMEN

Vehicle emissions are an important source of urban particular matter. To investigate the secondary organic aerosol (SOA) formation potential of real-world vehicle emissions, we exposed on-road air in Beijing to hydroxyl radicals generated in an oxidation flow reactor (OFR) under high-NOx conditions on-board a mobile laboratory and characterized SOA and their precursors with a suite of state-of-the-art instrumentation. The OFR produced 10-170 µg m-3 of SOA with a maximum SOA formation potential of 39-50 µg m-3 ppmv-1 CO that occurred following an integrated OH exposure of (1.3-2.0) × 1011 molecules cm-3 s. The results indicate relatively shorter photochemical ages for maximum SOA production than previous OFR results obtained under low-NOx conditions. Such timescales represent the balance of functionalization and fragmentation, possibly resulting in different spatial distributions of SOA in different seasons as the oxidant level changes. The detected precursors may explain as much as 13% of the observed SOA with the remaining plausibly contributed by the oxidation of undetected intermediate-volatility organic compounds. Extrapolation of the results suggests an annual SOA production rate of 0.78 Tg yr-1 from mobile gasoline sources in China, highlighting the importance of effective regulation of gaseous vehicular precursors to improve air quality in the future.


Asunto(s)
Contaminantes Atmosféricos , Emisiones de Vehículos , Aerosoles/análisis , Contaminantes Atmosféricos/análisis , Beijing , China , Emisiones de Vehículos/análisis
18.
Environ Sci Technol ; 55(23): 15694-15704, 2021 12 07.
Artículo en Inglés | MEDLINE | ID: mdl-34784716

RESUMEN

A prominent source of hydroxyl radicals (•OH), nitrous acid (HONO) plays a key role in tropospheric chemistry. Apart from direct emission, HONO (or its conjugate base nitrite, NO2-) can be formed secondarily in the atmosphere. Yet, how secondary HONO forms requires elucidation, especially for heterogeneous processes involving numerous organic compounds in atmospheric aerosols. We investigated nitrite production from aqueous photolysis of nitrate for a range of conditions (pH, organic compound, nitrate concentration, and cation). Upon adding small oxygenates such as ethanol, n-butanol, or formate as •OH scavengers, the average intrinsic quantum yield of nitrite [Φ(NO2-)] was 0.75 ± 0.15%. With near-UV-light-absorbing vanillic acid (VA), however, the effective Φ(NO2-) was strongly pH-dependent, reaching 8.0 ± 2.1% at a pH of 8 and 1.5 ± 0.39% at a more atmospherically relevant pH of 5. Our results suggest that brown carbon (BrC) may greatly enhance the nitrite production from the aqueous nitrate photolysis through photosensitizing reactions, where the triplet excited state of BrC may generate solvated electrons, which reduce nitrate to NO2 for further conversion to nitrite. This photosensitization process by BrC chromophores during nitrate photolysis under mildly acidic conditions may partly explain the missing HONO in urban environments.


Asunto(s)
Nitratos , Nitritos , Ácido Nitroso , Fotólisis , Ácido Vanílico
19.
Environ Sci Technol ; 55(9): 5701-5710, 2021 05 04.
Artículo en Inglés | MEDLINE | ID: mdl-33826309

RESUMEN

Smog chamber experiments were conducted to characterize the light absorption of brown carbon (BrC) from primary and photochemically aged coal combustion emissions. Light absorption was measured by the UV-visible spectrophotometric analysis of water and methanol extracts of filter samples. The single-scattering albedo at 450 nm was 0.73 ± 0.10 for primary emissions and 0.75 ± 0.13 for aged emissions. The light absorption coefficient at 365 nm of methanol extracts was higher than that of water extracts by a factor of 10 for primary emissions and a factor of 7 for aged emissions. This suggests that the majority of BrC is water-insoluble even after aging. The mass absorption efficiency of this BrC (MAE365) for primary OA (POA) was dependent on combustion conditions, with an average of 0.84 ± 0.54 m2 g-1, which was significantly higher than that for aged OA (0.24 ± 0.18 m2 g-1). Secondary OA (SOA) dominated aged OA and the decreased MAE365 after aging indicates that SOA is less light absorbing than POA and/or that BrC is bleached (oxidized) with aging. The estimated MAE365 of SOA (0.14 ± 0.08 m2 g-1) was much lower than that of POA. A comparison of MAE365 of residential coal combustion with other anthropogenic sources suggests that residential coal combustion emissions are among the strongest absorbing BrC organics.


Asunto(s)
Contaminantes Atmosféricos , Carbono , Aerosoles/análisis , Contaminantes Atmosféricos/análisis , Carbono/análisis , Carbón Mineral , Material Particulado/análisis , Agua
20.
Sensors (Basel) ; 21(24)2021 Dec 16.
Artículo en Inglés | MEDLINE | ID: mdl-34960493

RESUMEN

The tracking and positioning of transmission lines is a key element for UAVs (Unmanned Aerial Vehicles) to achieve autonomous inspection of transmission lines. Current methods are vulnerable to weather and environmental factors, have high costs, and have difficulties in data processing. Therefore, this paper proposes a transmission line tracking and localization method based on the electric field sensor array, which calculates the current UAV's heading angle deflection angle, the distance between the transmission line and the UAV, and the elevation angle, providing a new idea to solve the problem of UAV inspection of transmission lines. At the same time, the electric field distribution of different arrangements of three-phase transmission lines was analyzed using COMSOL to determine the flight area of the UAV. By comparing the electric field distribution of the UAV flight area and single-phase transmission lines, it was verified that the current method is also applicable in the three-phase transmission line scenario, and it was further verified that the sensor array used can sense the change of the UAV position in the flight area, indicating that the electric field sensor array can realize the transmission line tracking and localization of transmission lines. The experimental results showed that, in the three-phase transmission line scenario, when the sensor array moves along the transmission straight wire, the maximum absolute error of the heading angle deflection angle calculated according to this method was 8.2°, the maximum absolute error of the distance between the array and the transmission line was 19.3 cm, and the maximum absolute error of the elevation angle was 11.37°; the error was within a reasonable range and can be used for the UAV to realize autonomous inspection.

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