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1.
Alzheimers Dement ; 18(11): 2188-2198, 2022 11.
Artigo em Inglês | MEDLINE | ID: mdl-35103387

RESUMO

INTRODUCTION: Particulate air pollutants may induce neurotoxicity by increasing homocysteine levels, which can be lowered by high B vitamin intakes. Therefore, we examined whether intakes of three B vitamins (folate, B12 , and B6 ) modified the association between PM2.5 exposure and incidence of all-cause dementia. METHODS: This study included 7183 women aged 65 to 80 years at baseline. B vitamin intakes from diet and supplements were estimated by food frequency questionnaires at baseline. The 3-year average PM2.5 exposure was estimated using a spatiotemporal model. RESULTS: During a mean follow-up of 9 years, 342 participants developed all-cause dementia. We found that residing in locations with PM2.5 exposure above the regulatory standard (12 µg/m3 ) was associated with a higher risk of dementia only among participants with lower intakes of these B vitamins. DISCUSSION: This is the first study suggesting that the putative neurotoxicity of PM2.5 exposure may be attenuated by high B vitamin intakes.


Assuntos
Demência , Complexo Vitamínico B , Feminino , Humanos , Incidência , Material Particulado/efeitos adversos , Ácido Fólico , Demência/epidemiologia , Saúde da Mulher , Vitamina B 12
2.
Brain ; 143(1): 289-302, 2020 01 01.
Artigo em Inglês | MEDLINE | ID: mdl-31746986

RESUMO

Evidence suggests exposure to particulate matter with aerodynamic diameter <2.5 µm (PM2.5) may increase the risk for Alzheimer's disease and related dementias. Whether PM2.5 alters brain structure and accelerates the preclinical neuropsychological processes remains unknown. Early decline of episodic memory is detectable in preclinical Alzheimer's disease. Therefore, we conducted a longitudinal study to examine whether PM2.5 affects the episodic memory decline, and also explored the potential mediating role of increased neuroanatomic risk of Alzheimer's disease associated with exposure. Participants included older females (n = 998; aged 73-87) enrolled in both the Women's Health Initiative Study of Cognitive Aging and the Women's Health Initiative Memory Study of Magnetic Resonance Imaging, with annual (1999-2010) episodic memory assessment by the California Verbal Learning Test, including measures of immediate free recall/new learning (List A Trials 1-3; List B) and delayed free recall (short- and long-delay), and up to two brain scans (MRI-1: 2005-06; MRI-2: 2009-10). Subjects were assigned Alzheimer's disease pattern similarity scores (a brain-MRI measured neuroanatomical risk for Alzheimer's disease), developed by supervised machine learning and validated with data from the Alzheimer's Disease Neuroimaging Initiative. Based on residential histories and environmental data on air monitoring and simulated atmospheric chemistry, we used a spatiotemporal model to estimate 3-year average PM2.5 exposure preceding MRI-1. In multilevel structural equation models, PM2.5 was associated with greater declines in immediate recall and new learning, but no association was found with decline in delayed-recall or composite scores. For each interquartile increment (2.81 µg/m3) of PM2.5, the annual decline rate was significantly accelerated by 19.3% [95% confidence interval (CI) = 1.9% to 36.2%] for Trials 1-3 and 14.8% (4.4% to 24.9%) for List B performance, adjusting for multiple potential confounders. Long-term PM2.5 exposure was associated with increased Alzheimer's disease pattern similarity scores, which accounted for 22.6% (95% CI: 1% to 68.9%) and 10.7% (95% CI: 1.0% to 30.3%) of the total adverse PM2.5 effects on Trials 1-3 and List B, respectively. The observed associations remained after excluding incident cases of dementia and stroke during the follow-up, or further adjusting for small-vessel ischaemic disease volumes. Our findings illustrate the continuum of PM2.5 neurotoxicity that contributes to early decline of immediate free recall/new learning at the preclinical stage, which is mediated by progressive atrophy of grey matter indicative of increased Alzheimer's disease risk, independent of cerebrovascular damage.


Assuntos
Doença de Alzheimer/epidemiologia , Encéfalo/diagnóstico por imagem , Exposição Ambiental/estatística & dados numéricos , Memória Episódica , Material Particulado , Sintomas Prodrômicos , Idoso , Idoso de 80 Anos ou mais , Doença de Alzheimer/diagnóstico por imagem , Doença de Alzheimer/fisiopatologia , Doença de Alzheimer/psicologia , Disfunção Cognitiva/diagnóstico por imagem , Disfunção Cognitiva/epidemiologia , Disfunção Cognitiva/fisiopatologia , Disfunção Cognitiva/psicologia , Estudos de Coortes , Feminino , Humanos , Estudos Longitudinais , Imageamento por Ressonância Magnética , Estudos Prospectivos , Fatores de Risco , Estados Unidos/epidemiologia
3.
Environ Sci Technol ; 54(21): 13807-13816, 2020 11 03.
Artigo em Inglês | MEDLINE | ID: mdl-33064461

RESUMO

Atmospheric pollution represents a complex mixture of air chemicals that continually interact and transform, making it difficult to accurately evaluate associated toxicity responses representative of real-world exposure. This study leveraged data from a previously published article and reevaluated lung cell transcriptional response induced by outdoor atmospheric pollution mixtures using field-based exposure conditions in the industrialized Houston Ship Channel. The tested hypothesis was that individual and co-occurring chemicals in the atmosphere relate to altered expression of critical genes involved in inflammation and cancer-related processes in lung cells. Human lung cells were exposed at an air-liquid interface to ambient air mixtures for 4 h, with experiments replicated across 5 days. Real-time monitoring of primary and secondary gas-phase pollutants, as well as other atmospheric conditions, was simultaneously conducted. Transcriptional analysis of exposed cells identified critical genes showing differential expression associated with both individual and chemical mixtures. The individual pollutant identified with the largest amount of associated transcriptional response was benzene. Tumor necrosis factor (TNF) and interferon regulatory factor 1 (IRFN1) were identified as key upstream transcription factor regulators of the cellular response to benzene. This study is among the first to measure lung cell transcriptional responses in relation to real-world, gas-phase air mixtures.


Assuntos
Poluentes Atmosféricos , Poluição do Ar , Neoplasias , Poluentes Atmosféricos/análise , Poluição do Ar/análise , Humanos , Inflamação/induzido quimicamente , Inflamação/genética , Pulmão , Texas
4.
Am J Geriatr Psychiatry ; 27(10): 1083-1096, 2019 10.
Artigo em Inglês | MEDLINE | ID: mdl-31311712

RESUMO

OBJECTIVES: Although several environmental factors contribute to the etiology of late-life depressive symptoms, the role of ambient air pollution has been understudied. Experimental data support the neurotoxicity of airborne particulate matter with aerodynamic diameter of ≤2.5 µm (PM2.5), but it remains unclear whether long-term exposure is associated with late-life depressive symptoms. Our secondary aim was to explore whether the observed associations between exposure and depressive symptoms are explained by dementia risk. DESIGN, SETTING, AND PARTICIPANTS: Prospective community-dwelling cohort study from the Women's Health Initiative Study of Cognitive Aging (1999-2010). Our analyses included 1,989 older women (baseline age 73.3 ± 3.75) with no prior depression or cognitive impairment. MEASUREMENTS: Participants completed annual assessments of depressive symptoms (15-item Geriatric Depression Scale). Average ambient PM2.5 exposure at the residential location was estimated by spatiotemporal modeling for the 3-years preceding each neuropsychological assessment. Participants underwent separate annual examinations for incident dementia defined by DSM-IV. Latent-class mixture models examined the association between PM2.5 and identified trajectories of symptoms. RESULTS: Six trajectories of depressive symptoms were identified. Across all women, PM2.5 exposure was positively associated with depressive symptoms. The effect was especially strong in two clusters with sustained depressive symptoms (n = 625 sustained-mild [31%]; n = 125 sustained-moderate; [6%]). Among those with sustained-moderate symptoms, the estimated adverse effect of PM2.5 exposure was greater than that of hypertension. Among women without dementia, associations were modestly attenuated. CONCLUSION: Long-term exposure to ambient fine particles was associated with increased depressive symptoms among older women without prior depression or cognitive impairment.


Assuntos
Poluição do Ar/estatística & dados numéricos , Depressão/epidemiologia , Exposição Ambiental/estatística & dados numéricos , Material Particulado/análise , Idoso , Poluentes Atmosféricos/análise , Exposição Ambiental/análise , Feminino , Humanos , Vida Independente , Estudos Prospectivos , Escalas de Graduação Psiquiátrica , Ensaios Clínicos Controlados Aleatórios como Assunto
5.
Environ Sci Technol ; 53(15): 8682-8694, 2019 Aug 06.
Artigo em Inglês | MEDLINE | ID: mdl-31335134

RESUMO

Acid-driven multiphase chemistry of isoprene epoxydiols (IEPOX), key isoprene oxidation products, with inorganic sulfate aerosol yields substantial amounts of secondary organic aerosol (SOA) through the formation of organosulfur compounds. The extent and implications of inorganic-to-organic sulfate conversion, however, are unknown. In this article, we demonstrate that extensive consumption of inorganic sulfate occurs, which increases with the IEPOX-to-inorganic sulfate concentration ratio (IEPOX/Sulfinorg), as determined by laboratory measurements. Characterization of the total sulfur aerosol observed at Look Rock, Tennessee, from 2007 to 2016 shows that organosulfur mass fractions will likely continue to increase with ongoing declines in anthropogenic Sulfinorg, consistent with our laboratory findings. We further demonstrate that organosulfur compounds greatly modify critical aerosol properties, such as acidity, morphology, viscosity, and phase state. These new mechanistic insights demonstrate that changes in SO2 emissions, especially in isoprene-dominated environments, will significantly alter biogenic SOA physicochemical properties. Consequently, IEPOX/Sulfinorg will play an important role in understanding the historical climate and determining future impacts of biogenic SOA on the global climate and air quality.


Assuntos
Atmosfera , Pentanos , Aerossóis , Butadienos , Hemiterpenos , Sulfatos , Tennessee
6.
Atmos Environ (1994) ; 213: 456-462, 2019.
Artigo em Inglês | MEDLINE | ID: mdl-31320832

RESUMO

Fine particulate matter (PM2.5) is known to have an adverse impact on public health and is an important climate forcer. Secondary organic aerosol (SOA) contributes up to 80% of PM2.5 worldwide and multiphase reactions are an important pathway to form SOA. Aerosol-phase state is thought to influence the reactive uptake of gas-phase precursors to aerosol particles by altering diffusion rates within particles. Current air quality models do not include the impact of diffusion-limiting organic coatings on SOA formation. This work examines how α-pinene-derived organic coatings change the predicted formation of SOA from the acid-catalyzed multiphase reactions of isoprene epoxydiols (IEPOX). A box model, with inputs provided from field measurements taken at the Look Rock (LRK) site in Great Smokey Mountains National Park during the 2013 Southern Oxidant and Aerosol Study (SOAS), was modified to incorporate the latest laboratory-based kinetic data accounting for organic coating influences. Including an organic coating influence reduced the modeled reactive uptake when relative humidity was in the 55-80% range, with predicted IEPOX-derived SOA being reduced by up to 33%. Only sensitivity cases with a large increase in Henry's Law values of an order of magnitude or more or in particle reaction rates resulted in the large statistically significant differences form base model performance. These results suggest an organic coating layer could have an impact on IEPOX-derived SOA formation and warrant consideration in regional and global scale models.

7.
Environ Sci Technol ; 51(14): 8166-8175, 2017 Jul 18.
Artigo em Inglês | MEDLINE | ID: mdl-28636383

RESUMO

Secondary organic aerosol (SOA) derived from the photochemical oxidation of isoprene contributes a substantial mass fraction to atmospheric fine particulate matter (PM2.5). The formation of isoprene SOA is influenced largely by anthropogenic emissions through multiphase chemistry of its multigenerational oxidation products. Considering the abundance of isoprene SOA in the troposphere, understanding mechanisms of adverse health effects through inhalation exposure is critical to mitigating its potential impact on public health. In this study, we assessed the effects of isoprene SOA on gene expression in human airway epithelial cells (BEAS-2B) through an air-liquid interface exposure. Gene expression profiling of 84 oxidative stress and 249 inflammation-associated human genes was performed. Our results show that the expression levels of 29 genes were significantly altered upon isoprene SOA exposure under noncytotoxic conditions (p < 0.05), with the majority (22/29) of genes passing a false discovery rate threshold of 0.3. The most significantly affected genes belong to the nuclear factor (erythroid-derived 2)-like 2 (Nrf2) transcription factor network. The Nrf2 function is confirmed through a reporter cell line. Together with detailed characterization of SOA constituents, this study reveals the impact of isoprene SOA exposure on lung responses and highlights the importance of further understanding its potential health outcomes.


Assuntos
Aerossóis/toxicidade , Butadienos/toxicidade , Perfilação da Expressão Gênica , Hemiterpenos/toxicidade , Pentanos/toxicidade , Células Epiteliais/efeitos dos fármacos , Humanos , Pulmão/citologia
8.
Atmos Environ (1994) ; 148: 258-265, 2017 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-28848374

RESUMO

The regulatory Community Multiscale Air Quality (CMAQ) model is a means to understanding the sources, concentrations and regulatory attainment of air pollutants within a model's domain. Substantial resources are allocated to the evaluation of model performance. The Regionalized Air quality Model Performance (RAMP) method introduced here explores novel ways of visualizing and evaluating CMAQ model performance and errors for daily Particulate Matter ≤ 2.5 micrometers (PM2.5) concentrations across the continental United States. The RAMP method performs a non-homogenous, non-linear, non-homoscedastic model performance evaluation at each CMAQ grid. This work demonstrates that CMAQ model performance, for a well-documented 2001 regulatory episode, is non-homogeneous across space/time. The RAMP correction of systematic errors outperforms other model evaluation methods as demonstrated by a 22.1% reduction in Mean Square Error compared to a constant domain wide correction. The RAMP method is able to accurately reproduce simulated performance with a correlation of r = 76.1%. Most of the error coming from CMAQ is random error with only a minority of error being systematic. Areas of high systematic error are collocated with areas of high random error, implying both error types originate from similar sources. Therefore, addressing underlying causes of systematic error will have the added benefit of also addressing underlying causes of random error.

9.
Risk Anal ; 37(12): 2420-2434, 2017 12.
Artigo em Inglês | MEDLINE | ID: mdl-28244115

RESUMO

To quantify the on-road PM2.5 -related premature mortality at a national scale, previous approaches to estimate concentrations at a 12-km × 12-km or larger grid cell resolution may not fully characterize concentration hotspots that occur near roadways and thus the areas of highest risk. Spatially resolved concentration estimates from on-road emissions to capture these hotspots may improve characterization of the associated risk, but are rarely used for estimating premature mortality. In this study, we compared the on-road PM2.5 -related premature mortality in central North Carolina with two different concentration estimation approaches-(i) using the Community Multiscale Air Quality (CMAQ) model to model concentration at a coarser resolution of a 36-km × 36-km grid resolution, and (ii) using a hybrid of a Gaussian dispersion model, CMAQ, and a space-time interpolation technique to provide annual average PM2.5 concentrations at a Census-block level (∼105,000 Census blocks). The hybrid modeling approach estimated 24% more on-road PM2.5 -related premature mortality than CMAQ. The major difference is from the primary on-road PM2.5 where the hybrid approach estimated 2.5 times more primary on-road PM2.5 -related premature mortality than CMAQ due to predicted exposure hotspots near roadways that coincide with high population areas. The results show that 72% of primary on-road PM2.5 premature mortality occurs within 1,000 m from roadways where 50% of the total population resides, highlighting the importance to characterize near-road primary PM2.5 and suggesting that previous studies may have underestimated premature mortality due to PM2.5 from traffic-related emissions.


Assuntos
Mortalidade Prematura , Material Particulado/toxicidade , Emissões de Veículos/toxicidade , Adulto , Idoso , Idoso de 80 Anos ou mais , Poluição do Ar/efeitos adversos , Poluição do Ar/análise , Feminino , Avaliação do Impacto na Saúde/estatística & dados numéricos , Humanos , Masculino , Pessoa de Meia-Idade , Modelos Estatísticos , North Carolina/epidemiologia , Material Particulado/análise , Medição de Risco/estatística & dados numéricos , Emissões de Veículos/análise
10.
Environ Sci Technol ; 50(8): 4393-400, 2016 Apr 19.
Artigo em Inglês | MEDLINE | ID: mdl-26998937

RESUMO

To improve ozone exposure estimates for ambient concentrations at a national scale, we introduce our novel Regionalized Air Quality Model Performance (RAMP) approach to integrate chemical transport model (CTM) predictions with the available ozone observations using the Bayesian Maximum Entropy (BME) framework. The framework models the nonlinear and nonhomoscedastic relation between air pollution observations and CTM predictions and for the first time accounts for variability in CTM model performance. A validation analysis using only noncollocated data outside of a validation radius rv was performed and the R(2) between observations and re-estimated values for two daily metrics, the daily maximum 8-h average (DM8A) and the daily 24-h average (D24A) ozone concentrations, were obtained with the OBS scenario using ozone observations only in contrast with the RAMP and a Constant Air Quality Model Performance (CAMP) scenarios. We show that, by accounting for the spatial and temporal variability in model performance, our novel RAMP approach is able to extract more information in terms of R(2) increase percentage, with over 12 times for the DM8A and over 3.5 times for the D24A ozone concentrations, from CTM predictions than the CAMP approach assuming that model performance does not change across space and time.


Assuntos
Poluição do Ar/análise , Modelos Teóricos , Poluentes Atmosféricos/análise , Teorema de Bayes , Entropia , Monitoramento Ambiental , Modelos Químicos , Ozônio/análise , Estações do Ano , Estados Unidos
11.
Inhal Toxicol ; 28(6): 251-9, 2016.
Artigo em Inglês | MEDLINE | ID: mdl-27100558

RESUMO

CONTEXT: EpiAirway™ 3-D constructs are human-derived cell cultures of differentiated airway epithelial cells that may represent a more biologically relevant model of the human lung. However, limited information is available on their utility for exposures to air pollutants at the air-liquid interface (ALI). OBJECTIVE: To assess the biological responses of EpiAirway™ cells in comparison to the responses of A549 human alveolar epithelial cells after exposure to air pollutants at ALI. METHODS: Cells were exposed to filtered air, 400 ppb of ozone (O3) or a photochemically aged Synthetic Urban Mixture (SynUrb54) consisting of hydrocarbons, nitrogen oxides, O3 and other secondary oxidation products for 4 h. Basolateral supernatants and apical washes were collected at 9 and 24 h post-exposure. We assessed cytotoxicity by measuring lactate dehydrogenase (LDH) release into the culture medium and apical surface. Interleukin 6 (IL-6) and interleukin 8 (IL-8) proteins were measured in the culture medium and in the apical washes to determine the inflammatory response after exposure. RESULTS: Both O3 and SynUrb54 significantly increased basolateral levels of LDH and IL-8 in A549 cells. No significant changes in LDH and IL-8 levels were observed in the EpiAirway™ cells, however, IL-6 in the apical surface was significantly elevated at 24 h after O3 exposure. CONCLUSION: LDH and IL-8 are robust endpoints for assessing toxicity in A549 cells. The EpiAirway™ cells show minimal adverse effects after exposure suggesting that they are more toxicologically resistant compared to A549 cells. Higher concentrations or longer exposure times are needed to induce effects on EpiAirway™ cells.


Assuntos
Poluentes Atmosféricos/toxicidade , Células Epiteliais/efeitos dos fármacos , Hidrocarbonetos/toxicidade , Pulmão/efeitos dos fármacos , Óxidos de Nitrogênio/toxicidade , Ozônio/toxicidade , Biomarcadores/metabolismo , Técnicas de Cultura de Células , Linhagem Celular Tumoral , Sobrevivência Celular/efeitos dos fármacos , Relação Dose-Resposta a Droga , Células Epiteliais/metabolismo , Células Epiteliais/patologia , Humanos , Exposição por Inalação/efeitos adversos , Interleucina-6/metabolismo , Interleucina-8/metabolismo , L-Lactato Desidrogenase/metabolismo , Pulmão/metabolismo , Pulmão/patologia , Medição de Risco , Fatores de Tempo
12.
Proc Natl Acad Sci U S A ; 110(17): 6718-23, 2013 Apr 23.
Artigo em Inglês | MEDLINE | ID: mdl-23553832

RESUMO

Isoprene is a substantial contributor to the global secondary organic aerosol (SOA) burden, with implications for public health and the climate system. The mechanism by which isoprene-derived SOA is formed and the influence of environmental conditions, however, remain unclear. We present evidence from controlled smog chamber experiments and field measurements that in the presence of high levels of nitrogen oxides (NO(x) = NO + NO2) typical of urban atmospheres, 2-methyloxirane-2-carboxylic acid (methacrylic acid epoxide, MAE) is a precursor to known isoprene-derived SOA tracers, and ultimately to SOA. We propose that MAE arises from decomposition of the OH adduct of methacryloylperoxynitrate (MPAN). This hypothesis is supported by the similarity of SOA constituents derived from MAE to those from photooxidation of isoprene, methacrolein, and MPAN under high-NOx conditions. Strong support is further derived from computational chemistry calculations and Community Multiscale Air Quality model simulations, yielding predictions consistent with field observations. Field measurements taken in Chapel Hill, North Carolina, considered along with the modeling results indicate the atmospheric significance and relevance of MAE chemistry across the United States, especially in urban areas heavily impacted by isoprene emissions. Identification of MAE implies a major role of atmospheric epoxides in forming SOA from isoprene photooxidation. Updating current atmospheric modeling frameworks with MAE chemistry could improve the way that SOA has been attributed to isoprene based on ambient tracer measurements, and lead to SOA parameterizations that better capture the dependency of yield on NO(x).


Assuntos
Aerossóis/química , Poluentes Atmosféricos/análise , Atmosfera/análise , Butadienos/química , Compostos de Epóxi/química , Hemiterpenos/química , Modelos Químicos , Óxidos de Nitrogênio/química , Pentanos/química , Butadienos/efeitos da radiação , Simulação por Computador , Hemiterpenos/efeitos da radiação , Luz , Metacrilatos/química , North Carolina , Oxirredução , Pentanos/efeitos da radiação , Fotoquímica
13.
J Air Waste Manag Assoc ; 66(5): 456-69, 2016 May.
Artigo em Inglês | MEDLINE | ID: mdl-26796121

RESUMO

UNLABELLED: Electrical generation units (EGUs) are important sources of nitrogen oxides (NOx) that contribute to ozone air pollution. A dynamic management system can anticipate high ozone and dispatch EGU generation on a daily basis to attempt to avoid violations, temporarily scaling back or shutting down EGUs that most influence the high ozone while compensating for that generation elsewhere. Here we investigate the contributions of NOx from individual EGUs to high daily ozone, with the goal of informing the design of a dynamic management system. In particular, we illustrate the use of three sensitivity techniques in air quality models-brute force, decoupled direct method (DDM), and higher-order DDM-to quantify the sensitivity of high ozone to NOx emissions from 80 individual EGUs. We model two episodes with high ozone in the region around Pittsburgh, PA, on August 4 and 13, 2005, showing that the contribution of 80 EGUs to 8-hr daily maximum ozone ranges from 1 to >5 ppb at particular locations. At these locations and on the two high ozone days, shutting down power plants roughly 1.5 days before the 8-hr ozone violation causes greater ozone reductions than 1 full day before; however, the benefits of shutting down roughly 2 days before the high ozone are modest compared with 1.5 days. Using DDM, we find that six EGUs are responsible for >65% of the total EGU ozone contribution at locations of interest; in some locations, a single EGU is responsible for most of the contribution. Considering ozone sensitivities for all 80 EGUs, DDM performs well compared with a brute-force simulation with a small normalized mean bias (-0.20), while this bias is reduced when using the higher-order DDM (-0.10). IMPLICATIONS: Dynamic management of electrical generation has the potential to meet daily ozone air quality standards at low cost. We show that dynamic management can be effective at reducing ozone, as EGU contributions are important and as the number of EGUs that contribute to high ozone in a given location is small (<6). For two high ozone days and seven geographic regions, EGUs would best be shut down or their production scaled back roughly 1.5 days before the forecasted exceedance. Including online sensitivity techniques in an air quality forecasting model can provide timely and useful information on which EGUs would be most beneficial to shut down or scale back temporarily.


Assuntos
Poluentes Atmosféricos/análise , Monitoramento Ambiental/métodos , Óxidos de Nitrogênio/análise , Ozônio/análise , Modelos Teóricos , New England , Centrais Elétricas , Estados Unidos
14.
ACS EST Air ; 1(6): 511-524, 2024 Jun 14.
Artigo em Inglês | MEDLINE | ID: mdl-38884193

RESUMO

Secondary organic aerosol (SOA) from acid-driven reactive uptake of isoprene epoxydiols (IEPOX) contributes up to 40% of organic aerosol (OA) mass in fine particulate matter. Previous work showed that IEPOX substantially converts particulate inorganic sulfates to surface-active organosulfates (OSs). This decreases aerosol acidity and creates a viscous organic-rich shell that poses as a diffusion barrier, inhibiting additional reactive uptake of IEPOX. To account for this "self-limiting" effect, we developed a phase-separation box model to evaluate parameterizations of IEPOX reactive uptake against time-resolved chamber measurements of IEPOX-SOA tracers, including 2-methyltetrols (2-MT) and methyltetrol sulfates (MTS), at ~ 50% relative humidity. The phase-separation model was most sensitive to the mass accommodation coefficient, IEPOX diffusivity in the organic shell, and ratio of the third-order reaction rate constants forming 2-MT and MTS ( k M T / k M T S ). In particular, k M T / k M T S had to be lower than 0.1 to bring model predictions of 2-MT and MTS in closer agreement with chamber measurements; prior studies reported values larger than 0.71. The model-derived rate constants favor more particulate MTS formation due to 2-MT likely off-gassing at ambient-relevant OA loadings. Incorporating this parametrization into chemical transport models is expected to predict lower IEPOX-SOA mass and volatility due to the predominance of OSs.

15.
Environ Chem ; 10(3): 260-268, 2013 Jun 28.
Artigo em Inglês | MEDLINE | ID: mdl-24014080

RESUMO

Many of Houston's highest 8-h ozone (O3) peaks are characterised by increases in concentrations of at least 40 ppb in 1 h, or 60 ppb in 2 h. These rapid increases are called non-typical O3 changes (NTOCs). In 2004, the Texas Commission on Environmental Quality (TCEQ) developed a novel emissions control strategy aimed at eliminating NTOCs. The strategy limited routine and short-term emissions of ethene, propene, 1,3-butadiene and butene isomers, collectively called highly reactive volatile organic compounds (HRVOCs), which are released from petrochemical facilities. HRVOCs have been associated with NTOCs through field campaigns and modelling studies. This study analysed wind measurements and O3, formaldehyde (HCHO) and sulfur dioxide (SO2) concentrations from 2000 to 2011 at 25 ground monitors in Houston. NTOCs almost always occurred when monitors were downwind of petrochemical facilities. Rapid O3 increases were associated with low wind speeds; 75 % of NTOCs occurred when the 3-h average wind speed preceding the event was less than 6.5 km h-1. Statistically significant differences in HCHO concentrations were seen between days with and without NTOCs. Early afternoon HCHO concentrations were greater on NTOC days. In the morning before an observed NTOC event, however, there were no significant differences in HCHO concentrations between days with and without NTOCs. Hourly SO2 concentrations also increased rapidly, exhibiting behaviour similar to NTOCs. Oftentimes, the SO2 increases preceded a NTOC. These findings show that, despite the apparent success of targeted HRVOC emission controls, further restrictions may be needed to eliminate the remaining O3 events.

16.
J Air Waste Manag Assoc ; 63(1): 41-53, 2013 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-23447863

RESUMO

UNLABELLED: There currently exist a number of planetary boundary layer (PBL) schemes that can represent the effects of turbulence in daytime convective conditions, although these schemes remain a large source of uncertainty in meteorology and air quality model simulations. This study evaluates a recently developed combined local and nonlocal closure PBL scheme, the Asymmetric Convective Model, version 2 (ACM2), against PBL observations taken from radar wind profilers, a ground-based lidar, and multiple daytime radiosonde balloon launches. These observations were compared against predictions of PBLs from the Weather Research and Forecasting (WRF) model version 3.1 with the ACM2 PBL scheme option, and the Fifth-Generation Meteorological Model (MM5) version 3.7.3 with the Eta PBL scheme option that is currently being used to develop ozone control strategies in southeast Texas. MM5 and WRF predictions during the regulatory modeling episode were evaluated on their ability to predict the rise and fall of the PBL during daytime convective conditions across southeastern Texas. The MM5 predicted PBLs consistently underpredicted observations, and were also less than the WRF PBL predictions. The analysis reveals that the MM5 predicted a slower rising and shallower PBL not representative of the daytime urban boundary layer. Alternatively, the WRF model predicted a more accurate PBL evolution improving the root mean square error (RMSE), both temporally and spatially. The WRF model also more accurately predicted vertical profiles of temperature and moisture in the lowest 3 km of the atmosphere. Inspection of median surface temperature and moisture time-series plots revealed higher predicted surface temperatures in WRF and more surface moisture in MM5. These could not be attributed to surface heat fluxes, and thus the differences in performance of the WRF and MM5 models are likely due to the PBL schemes. IMPLICATIONS: An accurate depiction of the diurnal evolution of the planetary boundary layer (PBL) is necessary for realistic air quality simulations, and for formulating effective policy. The meteorological model used to support the southeast Texas 03 attainment demonstration made predictions of the PBL that were consistently less than those found in observations. The use of the Asymmetric Convective Model, version 2 (ACM2), predicted taller PBL heights and improved model predictions. A lower predicted PBL height in an air quality model would increase precursor concentrations and change the chemical production of O3 and possibly the response to control strategies.


Assuntos
Movimentos do Ar , Convecção , Modelos Teóricos , Umidade , Radar , Temperatura , Texas
17.
J Air Waste Manag Assoc ; 73(4): 321-332, 2023 04.
Artigo em Inglês | MEDLINE | ID: mdl-36730104

RESUMO

In 2019, an air emissions field sampling study was conducted by the Colorado Department of Public Health and Environment's Air Pollution Control Division (APCD) at four commercial cannabis cultivation facilities. Measurements of ambient biogenic volatile organic compounds (VOC) concentrations were collected from various growing stages of cannabis (vegetative and flowering) and during post-harvest activities (drying and trimming). These data were then used to determine room-specific biogenic VOC emission rates for three of the facilities from the vegetative stage of the life cycle through post-harvest activities. This study shows that the magnitude of biogenic VOC emissions within a cannabis cultivation facility varies widely with the highest emission rates of up to 7.18E-1 kg/hr found during mechanical trimming and up to 2.33E-1 kg/hr in the drying rooms. These were up to an order of magnitude higher than emission rates found in the cultivation rooms. For example, Facility A vegetative room had an emissions rate of 1.46E-2 kg/hr. Normalized by the amount of biomass present, the drying rooms had the highest VOC emissions rates, with a maximum rate of 1.6E-3 kg/hr/kg biomass. The flowering room rates were found to be up to 3.25E-4 kg/hr/kg biomass and drying rooms up to 1.16E-3 kg/hr/kg biomass. When normalized by plant count, emission rates in the flower rooms ranged from 8.11E-6 to 3.62E-4 kg/hr/plant. The dominant monoterpenes from sampling were ß-myrcene, terpinolene, and D-limonene. These data suggest that the variability in emission rates across cannabis production will create a challenge in establishing a generalized emission factor for all facilities. Across the industry, cannabis cultivation conditions and strategies can vary widely impacting the amount and type of VOC emissions. Minimizing uncertainties for VOC emission from cannabis facilities requires site-specific information on air exchange rates, plant counts, cannabis strains, biomass, and if hand or mechanical processing is used.Implications: This study found that the magnitude of biogenic VOC emissions within a cannabis cultivation varies widely throughout rooms found in the facility, with the highest emissions found during post-harvest activities (i.e. trimming) and the lowest rates in the vegetative room. These data suggest that the large emission sources of VOCs are found post-harvest and emission inventories based solely on cultivation emissions will underestimate total biogenic VOC emissions from indoor cannabis cultivation facilities. The dominant measured terpenes throughout all facilities from cultivation to post harvest were: ß-myrcene, terpinolene, and D-limonene.


Assuntos
Poluentes Atmosféricos , Cannabis , Compostos Orgânicos Voláteis , Monoterpenos , Compostos Orgânicos Voláteis/análise , Colorado , Limoneno , Monitoramento Ambiental , Poluentes Atmosféricos/análise
18.
Environ Sci Technol ; 46(16): 9062-70, 2012 Aug 21.
Artigo em Inglês | MEDLINE | ID: mdl-22834915

RESUMO

One of the most widely used in vitro particulate matter (PM) exposures methods is the collection of PM on filters, followed by resuspension in a liquid medium, with subsequent addition onto a cell culture. To avoid disruption of equilibria between gases and PM, we have developed a direct in vitro sampling and exposure method (DSEM) capable of PM-only exposures. We hypothesize that the separation of phases and post-treatment of filter-collected PM significantly modifies the toxicity of the PM compared to direct deposition, resulting in a distorted view of the potential PM health effects. Controlled test environments were created in a chamber that combined diesel exhaust with an urban-like mixture. The complex mixture was analyzed using both the DSEM and concurrently collected filter samples. The DSEM showed that PM from test atmospheres produced significant inflammatory response, while the resuspension exposures at the same exposure concentration did not. Increasing the concentration of resuspended PM sixteen times was required to yield measurable IL-8 expression. Chemical analysis of the resuspended PM indicated a total absence of carbonyl compounds compared to the test atmosphere during the direct-exposures. Therefore, collection and resuspension of PM into liquid modifies its toxicity and likely leads to underestimating toxicity.


Assuntos
Poluentes Atmosféricos/toxicidade , Emissões de Veículos/toxicidade , Poluentes Atmosféricos/análise , Atmosfera , Linhagem Celular Tumoral , Ciclo-Oxigenase 2/genética , Humanos , Interleucina-8/genética , RNA Mensageiro/genética , Emissões de Veículos/análise
19.
J Air Waste Manag Assoc ; 62(6): 696-706, 2012 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-22788108

RESUMO

In Houston, some of the highest measured 8-hr ozone (O3) peaks are characterized by sudden increases in observed concentrations of at least 40 ppb in 1 hr or 60 ppb in 2 hr. Measurements show that these large hourly changes appear at only a few monitors and span a narrow geographic area, suggesting a spatially heterogeneous field of O3 concentrations. This study assessed whether a regulatory air quality model (AQM) can simulate this observed behavior. The AQM did not reproduce the magnitude or location of some of the highest observed hourly O3 changes, and it also failed to capture the limited spatial extent. On days with measured large hourly changes in O3 concentrations, the AQM predicted high O3 over large regions of Houston, resulting in overpredictions at several monitors. This analysis shows that the model can make high O3, but on these days the predicted spatial field suggests that the model had a different cause. Some observed large hourly changes in O3 concentrations have been linked to random releases of industrial volatile organic compounds (VOCs). In the AQM emission inventory, there are several emission events when an industrial point source increases VOC emissions in excess of 10,000 mol/hr. One instance increased predicted downwind O3 concentrations up to 25 ppb. These results show that the modeling system is responsive to a large VOC release, but the timing and location of the release, and meteorological conditions, are critical requirements. Attainment of the O3 standard requires the use of observational data and AQM predictions. If the large observed hourly changes are indicative of a separate cause of high O3, then the model may not include that cause, which might result in regulators enacting control strategies that could be ineffective.


Assuntos
Poluentes Atmosféricos/química , Monitoramento Ambiental , Modelos Químicos , Ozônio/química , Poluição do Ar , Cidades , Texas , Fatores de Tempo
20.
ACS Omega ; 7(23): 19043-19047, 2022 Jun 14.
Artigo em Inglês | MEDLINE | ID: mdl-35722010

RESUMO

Although the "skunky" odor characteristic of cannabis has been widely referenced, its cause has been historically misassigned to unspecified "skunky terpenes". Recent reports from two independent research groups, the Koziel team (March and April 2021) and Oswald team (August and November 2021), have corrected this misassignment by linking the "skunky" character of industrial hemp and cannabis to 3-methyl-2-butene-1-thiol (321MBT). A recent USPTO patent application review clearly indicated that the Oswald team should take full credit for the discovery of this link with respect to cannabis. However, the August 19, 2021 publication of their patent application appears to be their formal public disclosure of 321MBT as the primary source odorant which is responsible for the targeted "skunky" odor. This date is well after the March and April 2021 public disclosures by the Koziel team for the 321MBT/"skunky" odor link relative to both cannabis and industrial hemp. This Viewpoint summarizes the investigative strategy leading to the public disclosure of this historically elusive link. It is presented from the perspective of the rapid multidimensional-gas chromatography-mass spectrometry-olfactometry (i.e., MDGC-MS-O) based odorant-prioritization "screening" approach, as applied by the Koziel team.

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