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1.
Proc Natl Acad Sci U S A ; 121(13): e2305030121, 2024 Mar 26.
Artigo em Inglês | MEDLINE | ID: mdl-38517975

RESUMO

During wildfires and fossil fuel combustion, biomass is converted to black carbon (BC) via incomplete combustion. BC enters the ocean by rivers and atmospheric deposition contributing to the marine dissolved organic carbon (DOC) pool. The fate of BC is considered to reside in the marine DOC pool, where the oldest BC 14C ages have been measured (>20,000 14C y), implying long-term storage. DOC is the largest exchangeable pool of organic carbon in the oceans, yet most DOC (>80%) remains molecularly uncharacterized. Here, we report 14C measurements on size-fractionated dissolved BC (DBC) obtained using benzene polycarboxylic acids as molecular tracers to constrain the sources and cycling of DBC and its contributions to refractory DOC (RDOC) in a site in the North Pacific Ocean. Our results reveal that the cycling of DBC is more dynamic and heterogeneous than previously believed though it does not comprise a single, uniformly "old" 14C age. Instead, both semilabile and refractory DBC components are distributed among size fractions of DOC. We report that DBC cycles within DOC as a component of RDOC, exhibiting turnover in the ocean on millennia timescales. DBC within the low-molecular-weight DOC pool is large, environmentally persistent and constitutes the size fraction that is responsible for long-term DBC storage. We speculate that sea surface processes, including bacterial remineralization (via the coupling of photooxidation of surface DBC and bacterial co-metabolism), sorption onto sinking particles and surface photochemical oxidation, modify DBC composition and turnover, ultimately controlling the fate of DBC and RDOC in the ocean.

2.
Proc Natl Acad Sci U S A ; 120(8): e2210005120, 2023 Feb 21.
Artigo em Inglês | MEDLINE | ID: mdl-36780523

RESUMO

Effects of aerosols such as black carbon (BC) on climate and buildup of the monsoon over the Indian Ocean are insufficiently quantified. Uncertain contributions from various natural and anthropogenic sources impede our understanding. Here, we use observations over 5 y of BC and its isotopes at a remote island observatory in northern Indian Ocean to constrain loadings and sources during little-studied monsoon season. Carbon-14 data show a highly variable yet largely fossil (65 ± 15%) source mixture. Combining carbon-14 with carbon-13 reveals the impact of African savanna burning, which occasionally approach 50% (48 ± 9%) of the total BC loadings. The BC mass-absorption cross-section for this regime is 7.6 ± 2.6 m2/g, with higher values during savanna fire input. Taken together, the combustion sources, longevity, and optical properties of BC aerosols over summertime Indian Ocean are different than the more-studied winter aerosol, with implications for chemical transport and climate model simulations of the Indian monsoon.

3.
Small ; 20(20): e2308908, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38105418

RESUMO

The environmental deterioration caused by dye wastewater discharge has received considerable attention in recent decades. One of the most promising approaches to addressing the aforementioned environmental issue is the development of photocatalysts with high solar energy consumption efficiency for the treatment of dye-contaminated water. In this study, a novel low-cost π-π biomass-derived black carbon modified g-C3N4 coupled FeIn2S4 composite (i.e., FeInS/BC-CN) photocatalyst is successfully designed and fabricated that reveals significantly improved photocatalytic performance for the degradation of Eosin Yellow (EY) dye in aqueous solution. Under dark and subsequent visible light irradiation, the amount optimized composite reveals 99% removal performance for EY dye, almost three-fold compared to that of the pristine FeInS and BC-CN counterparts. Further, it is confirmed by means of the electron spin resonance spectrometry, quenching experiments, and density functional theory (DFT) calculations, that the hydroxyl radicals (•OH) and superoxide radicals (•O2 -) are the dominant oxidation species involved in the degradation process of EY dye. In addition, a systematic photocatalytic degradation route is proposed based on the resultant degradation intermediates detectedduring liquid chromatography tandem mass spectrometry (LC-MS/MS) analysis. This work provides an innovative idea for the development of advanced photocatalysts to mitigate water pollution.

4.
Exp Eye Res ; 239: 109755, 2024 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-38128749

RESUMO

The threats of air pollution to human health have been gradually discovered, including its effects on eyes. The purpose of the study is to investigate the potential correlation between ocular surface exposure to black carbon and ocular surface structural damage as well as tear film dysfunction. To achieve this goal, 60 6-8-week-aged male BALB/C mice were randomly divided into 4 groups (n = 15). 0.5 mg/ml (group A), 1 mg/ml (group B), 5 mg/ml (group C) black carbon suspension droplets and PBS solution (group D) were used in the right eyes, 4 µl per time of three times per day. Tear break-up time, corneal fluorescein staining scores, and tear volume were assessed before treatment (day 0) and on days 4, 7, 10, and 14 after treatment. On day 14, the mice were sacrificed, and corneal and conjunctival tissues were collected for histological analysis. As the exposure time increased, there were no significant changes in the measured parameters from PBS-treated group of mice (P > 0.05). However, in the black carbon-treated group, there were significant decreases in tear film break-up time, significant increases in corneal fluorescein staining scores, and significant reductions in tear secretion (all P < 0.05). After 14 days, H&E staining of the corneal epithelium showed that in the PBS-treated group of mice, the corneal epithelial cells were neatly arranged, with no inflammatory cell infiltration, while in the black carbon-treated group, the corneal epithelium was significantly thickened, the basal cell arrangement was disrupted, the number of cell layers increased, and there was evidence of inflammatory cell infiltration. In the ultrastructure of the corneal epithelium, it could be observed that the black carbon-treated group had an increased amount of corneal epithelial cell detachment compared to the PBS-treated group, at the same time, the intercellular connections were looser, and there was a decrease in the number of microvilli and desmosomes in the black carbon-treated group. The results indicate that the ocular surface exposure to black carbon can result in a decrease in tear film stability and tear secretion in mice. Moreover, it can induce alterations in the corneal structure.


Assuntos
Síndromes do Olho Seco , Poluentes Ambientais , Masculino , Humanos , Animais , Camundongos , Idoso , Poluentes Ambientais/metabolismo , Camundongos Endogâmicos BALB C , Córnea/metabolismo , Fluoresceína/metabolismo , Lágrimas/metabolismo , Carbono/toxicidade , Carbono/metabolismo , Síndromes do Olho Seco/metabolismo
5.
Environ Sci Technol ; 58(6): 2750-2761, 2024 Feb 13.
Artigo em Inglês | MEDLINE | ID: mdl-38294931

RESUMO

With the increased occurrences of wildfires worldwide, there has been an increase in scientific interest surrounding the chemistry of fire-derived "black" carbon (BC). Traditionally, wildfire research has assumed that condensed aromatic carbon (ConAC) is exclusively produced via combustion, and thus, ConAC is equated to BC. However, the lack of correlations between ConAC in soils or rivers and wildfire history suggests that ConAC may be produced non-pyrogenically. Here, we show quantitative evidence that this occurs during the oxidation of biomass with environmentally ubiquitous hydroxyl radicals. Pine wood boards exposed to iron nails and natural weather conditions for 12 years yielded a charcoal-like ConAC-rich material. ConAC was also produced during laboratory oxidations of pine, maple, and brown-rotted oak woods, as well as algae, corn root, and tree bark. Back-of-the-envelope calculations suggest that biomass oxidation could be producing massive non-pyrogenic ConAC fluxes to terrestrial and aquatic environments. These estimates (e.g., 163-182 Tg-ConAC/year to soils) are much higher than the estimated pyrogenic "BC" fluxes (e.g., 128 Tg-ConAC/year to soils) implying that environmental ConAC is primarily non-pyrogenic. This novel perspective suggests that wildfire research trajectories should shift to assessing non-pyrogenic ConAC sources and fluxes, developing new methods for quantifying true BC, and establishing a new view of ConAC as an intermediate species in the biogeochemical processing of biomass during soil humification, aquatic photochemistry, microbial degradation, or mineral-organic matter interactions. We also advise against using BC or pyrogenic carbon (pyC) terminologies for ConAC measured in environmental matrices, unless a pyrogenic source can be confidently assigned.


Assuntos
Carbono , Incêndios , Biomassa , Carvão Vegetal , Fuligem/análise , Solo
6.
Environ Sci Technol ; 58(28): 12563-12574, 2024 Jul 16.
Artigo em Inglês | MEDLINE | ID: mdl-38950186

RESUMO

Urban air pollution can vary sharply in space and time. However, few monitoring strategies can concurrently resolve spatial and temporal variation at fine scales. Here, we present a new measurement-driven spatiotemporal modeling approach that transcends the individual limitations of two complementary sampling paradigms: mobile monitoring and fixed-site sensor networks. We develop, validate, and apply this model to predict black carbon (BC) using data from an intensive, 100-day field study in West Oakland, CA. Our spatiotemporal model exploits coherent spatial patterns derived from a multipollutant mobile monitoring campaign to fill spatial gaps in time-complete BC data from a low-cost sensor network. Our model performs well in reconstructing patterns at fine spatial and temporal resolution (30 m, 15 min), demonstrating strong out-of-sample correlations for both mobile (Pearson's R ∼ 0.77) and fixed-site measurements (R ∼ 0.95) while revealing features that are not effectively captured by a single monitoring approach in isolation. The model reveals sharp concentration gradients near major emission sources while capturing their temporal variability, offering valuable insights into pollution sources and dynamics.


Assuntos
Poluentes Atmosféricos , Poluição do Ar , Monitoramento Ambiental , Monitoramento Ambiental/métodos , Poluentes Atmosféricos/análise , Carbono , Fuligem , Cidades
7.
Environ Sci Technol ; 58(24): 10685-10695, 2024 Jun 18.
Artigo em Inglês | MEDLINE | ID: mdl-38839422

RESUMO

Air pollution exposure is typically assessed at the front door where people live in large-scale epidemiological studies, overlooking individuals' daily mobility out-of-home. However, there is limited evidence that incorporating mobility data into personal air pollution assessment improves exposure assessment compared to home-based assessments. This study aimed to compare the agreement between mobility-based and home-based assessments with personal exposure measurements. We measured repeatedly particulate matter (PM2.5) and black carbon (BC) using a sample of 41 older adults in the Netherlands. In total, 104 valid 24 h average personal measurements were collected. Home-based exposures were estimated by combining participants' home locations and temporal-adjusted air pollution maps. Mobility-based estimates of air pollution were computed based on smartphone-based tracking data, temporal-adjusted air pollution maps, indoor-outdoor penetration, and travel mode adjustment. Intraclass correlation coefficients (ICC) revealed that mobility-based estimates significantly improved agreement with personal measurements compared to home-based assessments. For PM2.5, agreement increased by 64% (ICC: 0.39-0.64), and for BC, it increased by 21% (ICC: 0.43-0.52). Our findings suggest that adjusting for indoor-outdoor pollutant ratios in mobility-based assessments can provide more valid estimates of air pollution than the commonly used home-based assessments, with no added value observed from travel mode adjustments.


Assuntos
Poluentes Atmosféricos , Poluição do Ar , Exposição Ambiental , Material Particulado , Humanos , Material Particulado/análise , Poluentes Atmosféricos/análise , Países Baixos , Monitoramento Ambiental/métodos , Masculino , Feminino , Idoso
8.
Environ Sci Technol ; 2024 Jul 18.
Artigo em Inglês | MEDLINE | ID: mdl-39026181

RESUMO

China has implemented strict emission control measures, but it is unclear how they affect black carbon (BC) aging and light absorption. Here, we use the Community Atmosphere Model version 6 (CAM6) with the four-mode version of the Modal Aerosol Module coupled with machine learning (MAM4-ML) to simulate BC aging during 2011-2018 and 2050/2100 following a carbon neutrality scenario (SSP1-2.6), respectively. During 2011-2018, the mass ratio of coatings to BC (RBC) widely increased (5.4% yr-1) over the east of China. The increased secondary organic aerosol (SOA) coatings dominate (88%) the increased RBC, while the sulfate coatings decrease. The drivers of BC coating changes come from the different magnitudes of emission reductions in secondary aerosol precursors (i.e., volatile organic compounds (VOCs) and SO2) and BC. During 2011-2018, the increased RBC enhances the BC mass absorption cross section (MAC, 0.7% yr-1). In 2050/2100 for SSP1-2.6, emission control leads to further increased RBC (95/145%) and BC MAC (12/17%). For both 2011-2018 and 2050/2100, the enhanced BC MAC partly offsets the declining direct radiative effect (DRE) of BC due to direct emission reduction. As a result, the full impact of direct emission reductions of BC on BC DRE is only 75% for 2011-2018 and 90/94% for 2050/2100.

9.
Environ Sci Technol ; 58(27): 11998-12007, 2024 Jul 09.
Artigo em Inglês | MEDLINE | ID: mdl-38935345

RESUMO

Landscape wildfires generate a substantial amount of dissolved black carbon (DBC) annually, yet the molecular nitrogen (N) structures in DBC are poorly understood. Here, we systematically compared the chemodiversity of N-containing molecules among three different DBC samples from rice straw biochar pyrolyzed at 300, 400, and 500 °C, one leached dissolved organic carbon (LDOC) sample from composted rice straw, and one fire-affected soil dissolved organic matter (SDOMFire) sample using Fourier-transform ion cyclotron resonance mass spectrometry (FT-ICR MS). N-Containing molecules contributed 20.0%, 36.1%, and 43.7% of total compounds in Combined DBC (pooling together the three DBC), LDOC, and SDOMFire, respectively, and molecules with fewer N atoms had higher proportions (i.e., N1 > N2 > N3). The N-containing molecules in Combined DBC were dominated by polycyclic aromatic (62.2%) and aromatic (14.4%) components, while those in LDOC were dominated by lignin-like (50.4%) and aromatic (30.1%) components. The composition and structures of N-containing molecules in SDOMFire were more similar to those in DBC than in LDOC. As the temperature rose, the proportion of the nitrogenous polycyclic aromatic component in DBC significantly increased with concurrent enhanced oxidation and unsaturation of N. As indicated by density functional theory (DFT)-based thermodynamic calculations, the proportion of aliphatic amide N decreased from 23.2% to 7.9%, whereas that of nitroaromatic N increased from 10.0% to 39.5% as the temperature increased from 300 to 500 °C; alternatively, the proportion of aromatic N in the 5/6 membered ring remained relatively stable (∼31%) and that of aromatic amide N peaked at 400 °C (32.7%). Our work first provides a comprehensive and thorough description of molecular N structures of DBC, which helps to better understand and predict their fate and biogeochemical behavior.


Assuntos
Espectrometria de Massas , Nitrogênio , Termodinâmica , Nitrogênio/química , Estrutura Molecular , Carbono/química , Solo/química
10.
Environ Sci Technol ; 58(16): 7165-7175, 2024 Apr 23.
Artigo em Inglês | MEDLINE | ID: mdl-38597176

RESUMO

Increasing wildfire frequency, a consequence of global climate change, releases incomplete combustion byproducts such as aquatic pyrogenic dissolved organic matter (DOM) and black carbon (DBC) into waters, posing a threat to water security. In August 2022, a series of severe wildfires occurred in Chongqing, China. Samples from seven locations along the Yangtze and Jialing Rivers revealed DBC, quantified by the benzene poly(carboxylic acid) (BPCA) method, comprising 9.5-19.2% of dissolved organic carbon (DOC). High concentrations of BPCA-DBC with significant polycondensation were detected near wildfire areas, likely due to atmospheric deposition driven by wind. Furthermore, Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR-MS) revealed that wildfires were associated with an increase in condensed aromatics, proteins, and unsaturated hydrocarbons, along with a decrease in lignins. The condensed aromatics primarily consisted of dissolved black nitrogen (DBN), contributing to abundant high-nitrogen-containing compounds in locations highly affected by wildfires. Meanwhile, wildfires potentially induced the input of recalcitrant sulfur-containing protein-like compounds, characterized by high oxidation, aliphatic nature, saturation, and low aromaticity. Overall, this study revealed the appearance of recalcitrant DBC and dissolved organic sulfur in river waters following wildfire events, offering novel insights into the potential impacts of wildfires on water quality and environmental biogeochemistry.

11.
Environ Sci Technol ; 58(2): 1142-1151, 2024 Jan 16.
Artigo em Inglês | MEDLINE | ID: mdl-38159290

RESUMO

Landscape fires annually generate large quantities of black carbon. The water-soluble fraction of black carbon (i.e., dissolved black carbon/DBC) is an important constituent of the dissolved organic carbon (DOC) pool, playing a crucial role in the global budget of refractory carbon and climate change. A key challenge in constraining the flux and fate of riverine DBC is to develop targeted and accurate quantification methods. Herein, we report that benzenepentacarboxylic acid (B5CA) intrinsically present in DBC can be used as an exclusive and holistic marker (representing both condensed aromatics and less-/nonaromatic fractions) for DBC quantification. B5CA was universally detected in water extractions of biochar and fire-affected soils with relatively large abundance but not produced by nonthermogenic processes. It has good mobility in the environment as it is not readily precipitated by cations or adsorbed by common geosorbents. B5CA also represents the recalcitrant components of DBC with excellent stability against photodegradation and biodegradation. Applying B5CA as the DBC marker in surface waters of the Changjiang River (i.e., the third largest river in the world), we calculate the DBC concentration in the downstream Changjiang River to be 4.8 ± 5.5% of the DOC flux. Our work provides a simple and reliable approach for the accurate quantification and source tracking of DBC in the soil and aquatic carbon pools.


Assuntos
Carbono , Ácidos Carboxílicos , Solo , Rios , Fuligem , Água
12.
Environ Sci Technol ; 58(28): 12575-12584, 2024 Jul 16.
Artigo em Inglês | MEDLINE | ID: mdl-38952258

RESUMO

There is a notable lack of continuous monitoring of air pollutants in the Global South, especially for measuring chemical composition, due to the high cost of regulatory monitors. Using our previously developed low-cost method to quantify black carbon (BC) in fine particulate matter (PM2.5) by analyzing reflected red light from ambient particle deposits on glass fiber filters, we estimated hourly ambient BC concentrations with filter tapes from beta attenuation monitors (BAMs). BC measurements obtained through this method were validated against a reference aethalometer between August 2 and 23, 2023 in Addis Ababa, Ethiopia, demonstrating a very strong agreement (R2 = 0.95 and slope = 0.97). We present hourly BC for three cities in sub-Saharan Africa (SSA) and one in North America: Abidjan (Côte d'Ivoire), Accra (Ghana), Addis Ababa (Ethiopia), and Pittsburgh (USA). The average BC concentrations for the measurement period at the Abidjan, Accra, Addis Ababa Central summer, Addis Ababa Central winter, Addis Ababa Jacros winter, and Pittsburgh sites were 3.85 µg/m3, 5.33 µg/m3, 5.63 µg/m3, 3.89 µg/m3, 9.14 µg/m3, and 0.52 µg/m3, respectively. BC made up 14-20% of PM2.5 mass in the SSA cities compared to only 5.6% in Pittsburgh. The hourly BC data at all sites (SSA and North America) show a pronounced diurnal pattern with prominent peaks during the morning and evening rush hours on workdays. A comparison between our measurements and the Goddard Earth Observing System Composition Forecast (GEOS-CF) estimates shows that the model performs well in predicting PM2.5 for most sites but struggles to predict BC at an hourly resolution. Adding more ground measurements could help evaluate and improve the performance of chemical transport models. Our method can potentially use existing BAM networks, such as BAMs at U.S. Embassies around the globe, to measure hourly BC concentrations. The PM2.5 composition data, thus acquired, can be crucial in identifying emission sources and help in effective policymaking in SSA.


Assuntos
Poluentes Atmosféricos , Cidades , Monitoramento Ambiental , Material Particulado , Monitoramento Ambiental/métodos , Poluentes Atmosféricos/análise , Material Particulado/análise , África , Carbono/análise , Fuligem/análise
13.
Environ Sci Technol ; 58(1): 760-770, 2024 Jan 09.
Artigo em Inglês | MEDLINE | ID: mdl-38149879

RESUMO

The photochemically generated oxidative organic radicals (POORs) in dissolved black carbon (DBC) was investigated and compared with that in dissolved organic matter (DOM). POORs generated in DBC solutions exhibited higher one-electron reduction potential values (1.38-1.56 V) than those in DOM solutions (1.22-1.38 V). We found that the photogeneration of POORs from DBC is enhanced with dissolved oxygen (DO) increasing, while the inhibition of POORs is observed in reference to DOM solution. The behavior of the one-electron reducing species (DBC•-/DOM•-) was employed to explain this phenomenon. The experimental results revealed that the DO concentration had a greater effect on DBC•- than on DOM•-. Low DO levels led to a substantial increase in the steady-state concentration of DBC•-, which quenched the POORs via back-electron reactions. Moreover, the contribution of POORs to the degradation of 19 emerging organic contaminants (EOCs) in sunlight-exposed DBC and DOM solutions was estimated. The findings indicate that POORs play an important role in the photodegradation of EOCs previously known to react with triplets, especially in DBC solutions. Compared to DOM solutions, POOR exhibits a lower but considerable contribution to EOC attenuation. This study enhances the understanding of pollutant fate in aquatic environments by highlighting the role of DBC in photochemical pollutant degradation and providing insights into pollutant transformation mechanisms involving POORs.


Assuntos
Poluentes Ambientais , Energia Solar , Fotólise , Oxigênio , Fuligem , Matéria Orgânica Dissolvida , Carbono , Estresse Oxidativo
14.
Environ Sci Technol ; 58(23): 10162-10174, 2024 Jun 11.
Artigo em Inglês | MEDLINE | ID: mdl-38810212

RESUMO

Residential biomass burning is an important source of black carbon (BC) exposure among rural communities in low- and middle-income countries. We collected 7165 personal BC samples and individual/household level information from 3103 pregnant women enrolled in the Household Air Pollution Intervention Network trial. Women in the intervention arm received free liquefied petroleum gas stoves and fuel throughout pregnancy; women in the control arm continued the use of biomass stoves. Median (IQR) postintervention BC exposures were 9.6 µg/m3 (5.2-14.0) for controls and 2.8 µg/m3 (1.6-4.8) for the intervention group. Using mixed models, we characterized predictors of BC exposure and assessed how exposure contrasts differed between arms by select predictors. Primary stove type was the strongest predictor (R2 = 0.42); the models including kerosene use, kitchen location, education, occupation, or stove use hours also provided additional explanatory power from the base model adjusted only for the study site. Our full, trial-wide, model explained 48% of the variation in BC exposures. We found evidence that the BC exposure contrast between arms differed by study site, adherence to the assigned study stove, and whether the participant cooked. Our findings highlight factors that may be addressed before and during studies to implement more impactful cookstove intervention trials.


Assuntos
Culinária , Humanos , Feminino , Gravidez , Adulto , Poluição do Ar em Ambientes Fechados , Fuligem , Carbono , Poluentes Atmosféricos , Exposição Ambiental
15.
Environ Res ; 248: 118380, 2024 May 01.
Artigo em Inglês | MEDLINE | ID: mdl-38307182

RESUMO

Evidence suggests that myocardial interstitial fibrosis, resulting from cardiac remodeling, may possibly be influenced by mechanisms activated through the inhalation of airborne pollutants. However, limited studies have explored the relationship between lifetime exposure to carbon-based particles and cardiac fibrosis, specially using post-mortem samples. This study examined whether long-term exposure to air pollution (estimated by black carbon accumulated in the lungs) is associated with myocardial fibrosis in urban dwellers of megacity of Sao Paulo. Data collection included epidemiological and autopsy-based approaches. Information was obtained by interviewing the next of kin and through the pathologist's report. The individual index of exposure to carbon-based particles, which we designed as the fraction of black carbon (FBC), was estimated through quantification of particles on the macroscopic lung surface. Myocardium samples were collected for histopathological analysis to evaluate the fraction of cardiac fibrosis. The association between cardiac fibrosis and FBC, age, sex, smoking status and hypertension was assessed by means of multiple linear regression models. Our study demonstrated that the association of FBC with cardiac fibrosis is influenced by smoking status and hypertension. Among hypertensive individuals, the cardiac fibrosis fraction tended to increase with the increase of the FBC in both groups of smokers and non-smokers. In non-hypertensive individuals, the association between cardiac fibrosis fraction and FBC was observed primarily in smokers. Long-term exposure to tobacco smoke and environmental particles may contribute to the cardiac remodeling response in individuals with pre-existing hypertension. This highlights the importance of considering hypertension as an additional risk factor for the health effects of air pollution on the cardiovascular system. Moreover, the study endorses the role of autopsy to investigate the effects of urban environment and personal habits in determining human disease.


Assuntos
Poluentes Atmosféricos , Poluição do Ar , Hipertensão , Humanos , Poluentes Atmosféricos/análise , Brasil , Remodelação Ventricular , Pulmão , Fibrose , Carbono/análise
16.
Part Fibre Toxicol ; 21(1): 7, 2024 Feb 17.
Artigo em Inglês | MEDLINE | ID: mdl-38368385

RESUMO

BACKGROUND: Airborne environmental and engineered nanoparticles (NPs) are inhaled and deposited in the respiratory system. The inhaled dose of such NPs and their deposition location in the lung determines their impact on health. When calculating NP deposition using particle inhalation models, a common approach is to use the bulk material density, ρb, rather than the effective density, ρeff. This neglects though the porous agglomerate structure of NPs and may result in a significant error of their lung-deposited dose and location. RESULTS: Here, the deposition of various environmental NPs (aircraft and diesel black carbon, wood smoke) and engineered NPs (silica, zirconia) in the respiratory system of humans and mice is calculated using the Multiple-Path Particle Dosimetry model accounting for their realistic structure and effective density. This is done by measuring the NP ρeff which was found to be up to one order of magnitude smaller than ρb. Accounting for the realistic ρeff of NPs reduces their deposited mass in the pulmonary region of the respiratory system up to a factor of two in both human and mouse models. Neglecting the ρeff of NPs does not alter significantly the distribution of the deposited mass fractions in the human or mouse respiratory tract that are obtained by normalizing the mass deposited at the head, tracheobronchial and pulmonary regions by the total deposited mass. Finally, the total deposited mass fraction derived this way is in excellent agreement with those measured in human studies for diesel black carbon. CONCLUSIONS: The doses of inhaled NPs are overestimated by inhalation particle deposition models when the ρb is used instead of the real-world effective density which can vary significantly due to the porous agglomerate structure of NPs. So the use of realistic ρeff, which can be measured as described here, is essential to determine the lung deposition and dosimetry of inhaled NPs and their impact on public health.


Assuntos
Exposição por Inalação , Nanopartículas , Humanos , Camundongos , Animais , Tamanho da Partícula , Exposição por Inalação/análise , Pulmão , Fuligem , Nanopartículas/química , Carbono
17.
J Aerosol Sci ; 178: 1-20, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38751612

RESUMO

The U. S. Environmental Protection Agency in collaboration with the U. S. Air Force Arnold Engineering Development Complex conducted the VAriable Response In Aircraft nvPM Testing (VARIAnT) 3 and 4 test campaigns to compare nonvolatile particulate matter (nvPM) emissions measurements from a variety of diffusion flame combustion aerosol sources (DFCASs), including a Cummins diesel engine, a diesel powered generator, two gas turbine start carts, a J85-GE-5 turbojet engine burning multiple fuels, and a Mini-CAST soot generator. The VARIAnT research program was devised to understand reported variability in the ARP6320A sampling system nvPM measurements. The VARIAnT research program has conducted four test campaigns to date with the VARIAnT 3 and 4 campaigns devoted to: (1) assessing the response of three different black carbon mass analyzers to particles of different size, morphology, and chemical composition; (2) characterizing the particles generated by 6 different combustion sources according to morphology, effective density, and chemical composition; and (3) assessing any significant difference between black carbon as determined by the 3 mass analyzers and the total PM determined via other techniques. Results from VARIAnT 3 and 4 campaigns revealed agreement of about 20% between the Micro-Soot Sensor, the Cavity Attenuated Phase Shift (CAPS PMSSA) monitor and the thermal-optical reference method for elemental carbon (EC) mass, independent of the calibration source used. For the LII-300, the measured mass concentrations in VARIAnT 3 fall within 18% and in VARIAnT 4 fall within 27% of the reference EC mass concentration when calibrated on a combustor rig in VARIAnT 3 and on an LGT-60 start cart in VARIAnT 4, respectively. It was also found that the three mass instrument types (MSS, CAPS PMSSA, and LII-300) can exhibit different BC to reference EC ratios depending on the emission source that appear to correlate to particle geometric mean mobility diameter, morphology, or some other parameter associated with particle geometric mean diameter (GMD) with the LII-300 showing a slightly stronger apparent trend with GMD. Systematic differences in LII-300 measured mass concentrations have been reduced by calibrating with a turbine combustion as a particle source (combustor or turbine engine). With respect to the particle size measurements, the sizing instruments (TSI SMPS, TSI EEPS, and Cambustion DMS 500) were found to be in general agreement in terms of size distributions and concentrations with some exceptions. Gravimetric measurements of the total aerosol mass produced by the various DFCAs differed from the reference EC, BC and integrated particle size distribution measured aerosol masses. The measurements of particle size distributions and single particle analysis performed using the miniSPLAT indicated the presence of larger particles (≳150 nm) having more compact morphologies, higher effective density, and a composition dominated by OC and containing ash. This increased large particle fraction is also associated with higher values of single scattering albedo measured by the CAPS PMSSA instrument and higher OC measurements. These measurements indicate gas turbine engine emissions can be a more heterogeneous mix of particle types beyond the original E-31 assumption that engine exit exhaust particles are mainly composed of black carbon.

18.
Sensors (Basel) ; 24(3)2024 Feb 01.
Artigo em Inglês | MEDLINE | ID: mdl-38339682

RESUMO

Black carbon (BC) or soot contains ultrafine combustion particles that are associated with a wide range of health impacts, leading to respiratory and cardiovascular diseases. Both long-term and short-term health impacts of BC have been documented, with even low-level exposures to BC resulting in negative health outcomes for vulnerable groups. Two aethalometers-AethLabs MA350 and Aerosol Magee Scientific AE33-were co-located at a Utah Division of Air Quality site in Bountiful, Utah for just under a year. The aethalometer comparison showed a close relationship between instruments for IR BC, Blue BC, and fossil fuel source-specific BC estimates. The biomass source-specific BC estimates were markedly different between instruments at the minute and hour scale but became more similar and perhaps less-affected by high-leverage outliers at the daily time scale. The greater inter-device difference for biomass BC may have been confounded by very low biomass-specific BC concentrations during the study period. These findings at a mountainous, high-elevation, Greater Salt Lake City Area site support previous study results and broaden the body of evidence validating the performance of the MA350.


Assuntos
Poluentes Atmosféricos , Poluentes Atmosféricos/análise , Fuligem/análise , Carbono/análise , Monitoramento Ambiental/métodos , Material Particulado/análise , Aerossóis
19.
J Environ Manage ; 360: 121074, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38754188

RESUMO

Hazardous Cr(VI) continues to pose critical concerns for environmental and public health, demanding the development of effective remediation methods. In this study, thiol-functionalized black carbon (S-BC) was proposed for Cr(VI) removal by mixing thioglycolic acid (TGA) with black carbon (BC) derived from rice straw residue at 80 °C for 8 h. Using a 1:40 (g mL-1) BC-to-TGA ratio, the resulting S-BC40 sample demonstrated significantly enhanced Cr(VI) sorption capacities of 201.23, 145.78, and 106.60 mg g-1 at pH 3.5, 5.5, and 7.5, surpassing its BC counterpart by 2.0, 2.3, and 2.2 times. Additionally, S-BC40 converted all sorbed Cr into Cr(III) species at pH ≥ 5.5, resulting in an equal distribution of Cr(OH)3 and organic Cr(III) complexes. However, approximately 13% of Cr sorbed on BC remained as Cr(VI) at pH 3.5 and 7.5. Both C-centered and S-centered thiyl radicals might contribute to Cr(VI) reduction; however, sufficient C-S groups replenished via thiol-functionalization was the key for the complete Cr(VI) reduction on S-BC samples as pH ≥ 5.5. Thanks to the exceptional Cr(VI) sorption capacity, affordability, and accessibility, thiol-functionalization stands out as a promising modification method for BC. It presents a distinct opportunity to concurrently achieve the objectives of efficient Cr(VI) remediation and waste recycling.


Assuntos
Carbono , Cromo , Compostos de Sulfidrila , Adsorção , Cromo/química , Compostos de Sulfidrila/química , Carbono/química , Poluentes Químicos da Água/química
20.
Environ Monit Assess ; 196(2): 188, 2024 Jan 23.
Artigo em Inglês | MEDLINE | ID: mdl-38261167

RESUMO

Air pollution is of major health and environmental concern globally and in South Africa. Studies on the sources of PM2.5 air pollution in low- and middle-income countries such as South Africa are limited. This study aimed to identify local and distant sources of PM2.5 pollution in Bloemfontein. PM2.5 samples were collected from June 16, 2020 to August 18, 2021. Trace element concentrations were determined by EDXRF spectroscopy. By use of the US EPA PMF 5.0 program, local sources were determined to be combustion/wood burning (49%), industry (22%), soil dust (10%), base metal/pyrometallurgical and traffic (9.6%) and water treatment/industry (9.4%). The HYSPLIT program was applied to determine distant PM2.5 source areas and the following clusters were identified: Mpumalanga province (52%), Northern Cape province (35%), Indian Ocean (8%) and Atlantic Ocean (6%). The majority of the air was found to come from the Mpumalanga province in the north-east, while the majority of local sources are ascribed to combustion/wood burning. Results from this study can be used to develop an Air Quality Management Plan for Bloemfontein.


Assuntos
Poluição do Ar , Monitoramento Ambiental , África do Sul , Oceano Atlântico , Poeira
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