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1.
Environ Sci Technol ; 2024 Apr 11.
Artigo em Inglês | MEDLINE | ID: mdl-38602183

RESUMO

Tropospheric nitrogen dioxide (NO2) poses a serious threat to the environmental quality and public health. Satellite NO2 observations have been continuously used to monitor NO2 variations and improve model performances. However, the accuracy of satellite NO2 retrieval depends on the knowledge of aerosol optical properties, in particular for urban agglomerations accompanied by significant changes in aerosol characteristics. In this study, we investigate the impacts of aerosol composition on tropospheric NO2 retrieval for an 18 year global data set from Global Ozone Monitoring Experiment (GOME)-series satellite sensors. With a focus on cloud-free scenes dominated by the presence of aerosols, individual aerosol composition affects the uncertainties of tropospheric NO2 columns through impacts on the aerosol loading amount, relative vertical distribution of aerosol and NO2, aerosol absorption properties, and surface albedo determination. Among aerosol compositions, secondary inorganic aerosol mostly dominates the NO2 uncertainty by up to 43.5% in urban agglomerations, while organic aerosols contribute significantly to the NO2 uncertainty by -8.9 to 37.3% during biomass burning seasons. The possible contrary influences from different aerosol species highlight the importance and complexity of aerosol correction on tropospheric NO2 retrieval and indicate the need for a full picture of aerosol properties. This is of particular importance for interpreting seasonal variations or long-term trends of tropospheric NO2 columns as well as for mitigating ozone and fine particulate matter pollution.

2.
Nat Food ; 5(3): 251-261, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38486126

RESUMO

Food consumption contributes to the degradation of air quality in regions where food is produced, creating a contrast between the health burden caused by a specific population through its food consumption and that faced by this same population as a consequence of food production activities. Here we explore this inequality within China's food system by linking air-pollution-related health burden from production to consumption, at high levels of spatial and sectorial granularity. We find that low-income groups bear a 70% higher air-pollution-related health burden from food production than from food consumption, while high-income groups benefit from a 29% lower health burden relative to their food consumption. This discrepancy largely stems from a concentration of low-income residents in food production areas, exposed to higher emissions from agriculture. Comprehensive interventions targeting both production and consumption sides can effectively reduce health damages and concurrently mitigate associated inequalities, while singular interventions exhibit limited efficacy.


Assuntos
Poluição do Ar , Renda , Pobreza , Alimentos , Agricultura
3.
Environ Sci Technol ; 2024 Mar 14.
Artigo em Inglês | MEDLINE | ID: mdl-38485962

RESUMO

Ozone pollution is profoundly modulated by meteorological features such as temperature, air pressure, wind, and humidity. While many studies have developed empirical models to elucidate the effects of meteorology on ozone variability, they predominantly focus on local weather conditions, overlooking the influences from high-altitude and broader regional meteorological patterns. Here, we employ convolutional neural networks (CNNs), a technique typically applied to image recognition, to investigate the influence of three-dimensional spatial variations in meteorological fields on the daily, seasonal, and interannual dynamics of ozone in Shenzhen, a major coastal urban center in China. Our optimized CNNs model, covering a 13° × 13° spatial domain, effectively explains over 70% of daily ozone variability, outperforming alternative empirical approaches by 7 to 62%. Model interpretations reveal the crucial roles of 2-m temperature and humidity as primary drivers, contributing 16% and 15% to daily ozone fluctuations, respectively. Regional wind fields account for up to 40% of ozone changes during the episodes. CNNs successfully replicate observed ozone temporal patterns, attributing -5-6 µg·m-3 of interannual ozone variability to weather anomalies. Our interpretable CNNs framework enables quantitative attribution of historical ozone fluctuations to nonlinear meteorological effects across spatiotemporal scales, offering vital process-based insights for managing megacity air quality amidst changing climate regimes.

4.
Environ Sci Technol ; 58(12): 5430-5441, 2024 Mar 26.
Artigo em Inglês | MEDLINE | ID: mdl-38471097

RESUMO

The evaporative emissions of anthropogenic volatile organic compounds (AVOCs) are sensitive to ambient temperature. This sensitivity forms an air pollution-meteorology connection that has not been assessed on a regional scale. We parametrized the temperature dependence of evaporative AVOC fluxes in a regional air quality model and evaluated the impacts on surface ozone in the Beijing-Tianjin-Hebei (BTH) area of China during the summer of 2017. The temperature dependency of AVOC emissions drove an enhanced simulated ozone-temperature sensitivity of 1.0 to 1.8 µg m-3 K-1, comparable to the simulated ozone-temperature sensitivity driven by the temperature dependency of biogenic VOC emissions (1.7 to 2.4 µg m-3 K-1). Ozone enhancements driven by temperature-induced AVOC increases were localized to their point of emission and were relatively more important in urban areas than in rural regions. The inclusion of the temperature-dependent AVOC emissions in our model improved the simulated ozone-temperature sensitivities on days of ozone exceedance. Our results demonstrated the importance of temperature-dependent AVOC emissions on surface ozone pollution and its heretofore unrepresented role in air pollution-meteorology interactions.


Assuntos
Poluentes Atmosféricos , Poluição do Ar , Ozônio , Compostos Orgânicos Voláteis , Ozônio/análise , Poluentes Atmosféricos/análise , Compostos Orgânicos Voláteis/análise , Temperatura , Monitoramento Ambiental/métodos , China
5.
Environ Int ; 184: 108492, 2024 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-38350258

RESUMO

Water-soluble organic molecules (WSOMs) in inhaled PM2.5 can readily translocate from the lungs into the blood circulation, facilitating their distribution to and health effects on distant organs and tissues in the human body. Human serum albumin (HSA), the most abundant protein carrier in the blood, readily binds exogenous substances to form non-covalent adducts and subsequently transports them throughout the circulatory system, thereby indicating their internal exposure. The direct internal exposure of WSOMs in PM2.5 needs to be understood. In this study, the non-covalent HSA-WSOM adductome was developed as a dosimeter to evaluate the internal exposure potential of WSOMs in urban PM2.5. The WSOM composition was acquired from non-target high-resolution mass spectrometry analysis coupled with multiple ionizations. The binding level of HSA-WSOM non-covalent adducts was obtained from surface plasma resonance. Machine learning combined WSOM composition and the binding level of HSA-WSOM non-covalent adducts to screen bindable (also internalizable) WSOMs. The concentration of WSOM ranged from 4 to 13 µg/m3 during our observation period. Of the 17,513 mass spectral features detected, 9,484 contributed to the non-covalent adductome and possessed the internal exposure potential. 102 major contributors accounted for 90.6 % of the HSA-WSOM binding level. The fraction of internalizable WSOMs in PM2.5 varied from 11.9 % to 61.3 %, averaging 26.2 %. WSOMs that have internal exposure potential were primarily lignin-like and lipid-like substances. The HSA-WSOMs non-covalent adductome represents direct internal exposure potential, which can provide crucial insights into the molecular diagnosis of PM2.5 exposure and precise assessments of PM2.5 health effects.


Assuntos
Material Particulado , Água , Humanos , Material Particulado/análise , Albumina Sérica Humana , Espectrometria de Massas , Aerossóis/análise
6.
Environ Sci Technol ; 58(1): 628-638, 2024 Jan 09.
Artigo em Inglês | MEDLINE | ID: mdl-38153406

RESUMO

China's industrial restructuring and pollution controls have altered the contributions of individual sources to varying air quality over the past decade. We used the GEOS-Chem adjoint model and investigated the changing sensitivities of PM2.5 and ozone (O3) to multiple species and sources from 2010 to 2020 in the central Yangtze River Delta (YRDC), the largest economic region in China. Controlling primary particles and SO2 from industrial and residential sectors dominated PM2.5 decline, and reducing CO from multiple sources and ≥C3 alkenes from vehicles restrained O3. The chemical regime of O3 formation became less VOC-limited, attributable to continuous NOX abatement for specific sources, including power plants, industrial combustion, cement production, and off-road traffic. Regional transport was found to be increasingly influential on PM2.5. To further improve air quality, management of agricultural activities to reduce NH3 is essential for alleviating PM2.5 pollution, while controlling aromatics, alkenes, and alkanes from industry and gasoline vehicles is effective for O3. Reducing the level of NOX from nearby industrial combustion and transportation is helpful for both species. Our findings reveal the complexity of coordinating control of PM2.5 and O3 pollution in a fast-developing region and support science-based policymaking for other regions with similar air pollution problems.


Assuntos
Poluentes Atmosféricos , Poluição do Ar , Ozônio , Ozônio/análise , Poluentes Atmosféricos/análise , Rios , Monitoramento Ambiental , Poluição do Ar/análise , China , Material Particulado/análise , Alcenos
7.
Sci Total Environ ; 912: 169555, 2024 Feb 20.
Artigo em Inglês | MEDLINE | ID: mdl-38157913

RESUMO

Antioxidants are typically seen as agents that mitigate environmental health risks due to their ability to scavenge free radicals. However, our research presents a paradox where these molecules, particularly those within lung fluid, act as prooxidants in the presence of airborne particulate matter (PM2.5), thus enhancing PM2.5 oxidative potential (OP). In our study, we examined a range of antioxidants found in the respiratory system (e.g., vitamin C, glutathione (GSH), and N-acetylcysteine (NAC)), in plasma (vitamin A, vitamin E, and ß-carotene), and in food (tert-butylhydroquinone (TBHQ)). We aimed to explore antioxidants' prooxidant and antioxidant interactions with PM2.5 and the resulting OP and cytotoxicity. We employed OH generation assays and electron paramagnetic resonance assays to assess the pro-oxidative and anti-oxidative effects of antioxidants. Additionally, we assessed cytotoxicity interaction using a Chinese hamster ovary cell cytotoxicity assay. Our findings revealed that, in the presence of PM2.5, all antioxidants except vitamin E significantly increased the PM2.5 OP by generating more OH radicals (OH generation rate: 0.16-24.67 pmol·min-1·m-3). However, it's noteworthy that these generated OH radicals were at least partially neutralized by the antioxidants themselves. Among the pro-oxidative antioxidants, vitamin A, ß-carotene, and TBHQ showed the least ability to quench these radicals, consistent with their observed impact in enhancing PM2.5 cytotoxicity (PM2.5 LC50 reduced to 91.2 %, 88.8 %, and 75.1 % of PM2.5's original level, respectively). Notably, vitamin A and TBHQ-enhanced PM2.5 OP were strongly associated with the presence of metals and organic compounds, particularly with copper (Cu) contributing significantly (35 %) to TBHQ's pro-oxidative effect. Our study underscores the potential health risks associated with the interaction between antioxidants and ambient pollutants.


Assuntos
Poluentes Atmosféricos , Antioxidantes , Hidroquinonas , Cricetinae , Animais , Antioxidantes/metabolismo , beta Caroteno , Poluentes Atmosféricos/toxicidade , Poluentes Atmosféricos/análise , Células CHO , Vitamina A , Cricetulus , Material Particulado/toxicidade , Material Particulado/análise , Vitamina E , Glutationa , Estresse Oxidativo
8.
Environ Sci Technol ; 57(50): 21295-21305, 2023 Dec 19.
Artigo em Inglês | MEDLINE | ID: mdl-38064660

RESUMO

The chemical industry is a significant source of nonmethane volatile organic compounds (NMVOCs), pivotal precursors to ambient ozone (O3), and secondary organic aerosol (SOA). Despite their importance, precise estimation of these emissions remains challenging, impeding the implementation of NMVOC controls. Here, we present the first comprehensive plant-level assessment of NMVOC emissions from the chemical industry in China, encompassing 3461 plants, 127 products, and 50 NMVOC compounds from 2010 to 2019. Our findings revealed that the chemical industry in China emitted a total of 3105 (interquartile range: 1179-8113) Gg of NMVOCs in 2019, with a few specific products accounting for the majority of the emissions. Generally, plants engaged in chemical fibers production or situated in eastern China pose a greater risk to public health due to their higher formation potentials of O3 and SOA or their proximity to residential areas or both. We demonstrated that targeting these high-risk plants for emission reduction could enhance health benefits by 7-37% per unit of emission reduction on average compared to the current situation. Consequently, this study provides essential insights for developing effective plant-specific NMVOC control strategies within China's chemical industry.


Assuntos
Poluentes Atmosféricos , Ozônio , Compostos Orgânicos Voláteis , Poluentes Atmosféricos/análise , Compostos Orgânicos Voláteis/análise , Compostos Orgânicos Voláteis/química , Indústria Química , Monitoramento Ambiental , Ozônio/análise , China , Aerossóis/análise , Plantas
9.
PNAS Nexus ; 2(11): pgad391, 2023 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-38034090

RESUMO

Maritime trade and associated emissions are dynamic in nature. Although shipping emissions contribute significantly to air quality and climate change, their trade-governed dynamics remain less explored due to the lack of observational evidence. Here, we use satellite measurements to capture the redistribution of shipping nitrogen oxides (NOx) emissions from Shanghai port, the world's busiest port, during a natural experiment posted by the localized COVID-19 lockdown in 2022. Viewing the ports as nodes in a network linked by ship journeys, we quantify a lockdown-induced -42% reduction in shipping NOx emissions for Shanghai port. We further identify an emission transfer to its neighboring connected ports, confirmed by comprehensive vessel activity observations. Our study highlights the socioeconomic drivers of shipping emissions, which may add additional layers of complexity to air quality management.

10.
Natl Sci Rev ; 10(12): nwad244, 2023 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-37954202

RESUMO

Atmospheric deposition of particulate organic nitrogen (ONp) is a significant process in the global nitrogen cycle and may be pivotally important for N-limited ecosystems. However, past models largely overlooked the spatial and chemical inhomogeneity of atmospheric ONp and were thus deficient in assessing global ONp impacts. We constructed a comprehensive global model of atmospheric gaseous and particulate organic nitrogen (ON), including the latest knowledge on emissions and secondary formations. Using this model, we simulated global atmospheric ONp abundances consistent with observations. Our estimated global atmospheric ON deposition was 26 Tg N yr-1, predominantly in the form of ONp (23 Tg N yr-1) and mostly from wildfires (37%), oceans (22%) and aqueous productions (17%). Globally, ONp contributed as much as 40% to 80% of the total N deposition downwind of biomass-burning regions. Atmospheric ONp deposition thus constituted the dominant external N supply to the N-limited boreal forests, tundras and the Arctic Ocean, and its importance may be amplified in a future warming climate.

11.
Environ Sci Technol ; 57(43): 16477-16488, 2023 10 31.
Artigo em Inglês | MEDLINE | ID: mdl-37867432

RESUMO

The iron and steel industry (ISI) is important for socio-economic progress but emits greenhouse gases and air pollutants detrimental to climate and human health. Understanding its historical emission trends and drivers is crucial for future warming and pollution interventions. Here, we offer an exhaustive analysis of global ISI emissions over the past 60 years, forecasting up to 2050. We evaluate emissions of carbon dioxide and conventional and unconventional air pollutants, including heavy metals and polychlorinated dibenzodioxins and dibenzofurans. Based on this newly established inventory, we dissect the determinants of past emission trends and future trajectories. Results show varied trends for different pollutants. Specifically, PM2.5 emissions decreased consistently during the period 1970 to 2000, attributed to adoption of advanced production technologies. Conversely, NOx and SO2 began declining recently due to stringent controls in major contributors such as China, a trend expected to persist. Currently, end-of-pipe abatement technologies are key to PM2.5 reduction, whereas process modifications are central to CO2 mitigation. Projections suggest that by 2050, developing nations (excluding China) will contribute 52-54% of global ISI PM2.5 emissions, a rise from 29% in 2019. Long-term emission curtailment will necessitate the innovation and widespread adoption of new production and abatement technologies in emerging economies worldwide.


Assuntos
Poluentes Atmosféricos , Poluição do Ar , Humanos , Poluição do Ar/análise , Ferro , Material Particulado/análise , Aço , Poluentes Atmosféricos/análise , China
12.
Environ Sci Technol ; 57(44): 16999-17010, 2023 11 07.
Artigo em Inglês | MEDLINE | ID: mdl-37856868

RESUMO

In early 2020, two unique events perturbed ship emissions of pollutants around Southern China, proffering insights into the impacts of ship emissions on regional air quality: the decline of ship activities due to COVID-19 and the global enforcement of low-sulfur (<0.5%) fuel oil for ships. In January and February 2020, estimated ship emissions of NOx, SO2, and primary PM2.5 over Southern China dropped by 19, 71, and 58%, respectively, relative to the same period in 2019. The decline of ship NOx emissions was mostly over the coastal waters and inland waterways of Southern China due to reduced ship activities. The decline of ship SO2 and primary PM2.5 emissions was most pronounced outside the Chinese Domestic Emission Control Area due to the switch to low-sulfur fuel oil there. Ship emission reductions in early 2020 drove 16 to 18% decreases in surface NO2 levels but 3.8 to 4.9% increases in surface ozone over Southern China. We estimated that ship emissions contributed 40% of surface NO2 concentrations over Guangdong in winter. Our results indicated that future abatements of ship emissions should be implemented synergistically with reductions of land-borne anthropogenic emissions of nonmethane volatile organic compounds to effectively alleviate regional ozone pollution.


Assuntos
Poluentes Atmosféricos , Poluição do Ar , Óleos Combustíveis , Ozônio , Poluentes Atmosféricos/análise , Navios , Emissões de Veículos/análise , Material Particulado/análise , Dióxido de Nitrogênio , Poluição do Ar/análise , China , Ozônio/análise , Enxofre , Monitoramento Ambiental/métodos
13.
Environ Sci Technol ; 57(33): 12341-12350, 2023 08 22.
Artigo em Inglês | MEDLINE | ID: mdl-37552529

RESUMO

As the main anthropogenic source in open seas and coastal areas, ship emissions impact the climate, air quality, and human health. The latest marine fuel regulation with a sulfur content limit of 0.5% went into effect globally on January 1, 2020. Investigations of ship emissions after fuel switching are necessary. In this study, online field measurements at an urban coastal site and modeling simulations were conducted to detect the impact of ship emissions on air quality in the Greater Bay Area (GBA) in China under new fuel regulation. By utilizing a high mass-resolution single particle mass spectrometer, the vanadium(V) signal was critically identified and was taken as a robust indicator for ship-emitted particles (with relative peak area > 0.1). The considerable number fractions of high-V particles (up to 30-40% during ship plumes) indicated that heavy fuel oils via simple desulfurization or blending processes with low-sulfur fuels were extensively used in the GBA to meet the global 0.5% sulfur cap. Our results showed that ship-emitted particulate matter and NOx contributed up to 21.4% and 39.5% to the ambient, respectively, in the summertime, significantly affecting the air quality in the GBA. The sea-land breeze circulation also played an important role in the transport pattern of ship-emitted pollutants in the GBA.


Assuntos
Poluentes Atmosféricos , Poluição do Ar , Humanos , Poluentes Atmosféricos/análise , Emissões de Veículos/análise , Navios , Poluição do Ar/análise , Material Particulado/análise , China , Enxofre
14.
Huan Jing Ke Xue ; 44(6): 3117-3129, 2023 Jun 08.
Artigo em Chinês | MEDLINE | ID: mdl-37309931

RESUMO

The short-term reduction of air pollutant emissions is an important emergency control measure for avoiding air pollution exceedances in Chinese cities. However, the impacts of short-term emission reductions on the air qualities in southern Chinese cities in spring has not been fully explored. We analyzed the changes in air quality in Shenzhen, Guangdong before, during, and after a city-wide lockdown associated with COVID-19 control during March 14 to 20, 2022. Stable weather conditions prevailed before and during the lockdown, such that local air pollution was strongly affected by local emissions. In-situ measurements and WRF-GC simulations over the Pearl River Delta (PRD) both showed that, due to reductions in traffic emissions during the lockdown, the concentrations of nitrogen dioxide (NO2), respirable particulate matter (PM10), and fine particulate matters (PM2.5) in Shenzhen decreased by (-26±9.5)%, (-28±6.4)%, and (-20±8.2)%, respectively. However, surface ozone (O3) concentration did not change significantly[(-1.0±6.5)%]. TROPOMI satellite observations of formaldehyde and nitrogen dioxide column concentrations indicated that the ozone photochemistry in the PRD in spring 2022 was mainly controlled by the volatile organic compound (VOCs) concentrations and was not sensitive to the reduction in nitrogen oxide (NOx) concentrations. Reduction in NOx may even have increased O3, because the titration of O3 by NOx was weakened. Due to the small spatial-temporal extent of emission reductions, the air quality effects caused by this short-term urban-scale lockdown were weaker than the air quality effects across China during the widespread COVID-19 lockdown in 2020. Future air quality management in South China cities should consider the impacts of NOx emission reduction on ozone and focus on the co-reduction scenarios of NOx and VOCs.


Assuntos
Poluentes Atmosféricos , Poluição do Ar , COVID-19 , Ozônio , Compostos Orgânicos Voláteis , Humanos , Dióxido de Nitrogênio , Controle de Doenças Transmissíveis , Óxido Nítrico , Material Particulado
15.
Sci Total Environ ; 862: 160771, 2023 Mar 01.
Artigo em Inglês | MEDLINE | ID: mdl-36513240

RESUMO

Reactive oxygen species (ROS) play a central role in health effects of ambient fine particulate matter (PM2.5). In this work, we screened for efficient and complementary oxidative potential (OP) measurements by comparing the response values of multiple chemical probes (OPDTT, OPOH, OPGSH) to ambient PM2.5 in Shenzhen, China. Combined with meteorological condition and PM2.5 chemical composition analysis, we explored the effects of different chemical components and emission sources on the ambient PM2.5 OP and analyzed their seasonal variations. The results show that OPmDTT(mass-normalized) and OPmGSH-SLF were highly correlated (r = 0.77). OPDTT was mainly influenced by organic carbon, while OPOH was highly dominated by heavy metals. The combination of OPDTT and OPOH provides an efficient and comprehensive measurement of OP. Temporally, the OPs were substantially higher in winter than in summer (1.4 and 4 times higher for OPmDTT and OPmOH, respectively). The long-distance transported biomass burning sources from the north dominated the OPDTT in winter, while the ship emissions mainly influenced the summer OP. The OPmDTT increased sharply with the decrease of PM2.5 mass concentration, especially when the PM2.5 concentration was lower than 30 µg/m3. The huge differences in wind fields between the winter and summer cause considerable variations in PM2.5 concentrations, components, and OP. Our work emphasizes the necessity of long-term, multi-method, multi-component assessment of the OP of PM2.5.


Assuntos
Poluentes Atmosféricos , Poluentes Atmosféricos/análise , Estações do Ano , Monitoramento Ambiental/métodos , Material Particulado/análise , China , Estresse Oxidativo
16.
Environ Sci Technol ; 56(10): 6243-6252, 2022 05 17.
Artigo em Inglês | MEDLINE | ID: mdl-35482889

RESUMO

We developed a regional atmospheric transport model for microplastics (MPs, 10 µm to 5 mm in size) over Asia and the adjacent Pacific and Indian oceans, accounting for MPs' size- and shape-dependent aerodynamics. The model was driven by tuned atmospheric emissions of MPs from the land and the ocean, and the simulations were evaluated against coastal (n = 19) and marine (n = 56) observations. Our tuned atmospheric emissions of MPs from Asia and the adjacent oceans were 310 Gg y-1 (1 Gg = 1 kton) and 60 Gg y-1, respectively. MP lines and fragments may be transported in the atmosphere >1000 km; MP pellets in our model mostly deposited near-source. We estimated that 1.4% of the MP mass emitted into the Asian atmosphere deposited into the oceans via atmospheric transport; the rest deposited over land. The resulting net atmospheric transported MP flux from Asia into the oceans was 3.9 Gg y-1, twice as large as a previous estimate for the riverine-transported MP flux from Asia into the oceans. The uncertainty of our simulated atmospheric MP budget was between factors of 3 and 7. Our work highlighted the impacts of the size and morphology on the aerodynamics of MPs and the importance of atmospheric transport in the source-to-sink relationship of global MP pollution.


Assuntos
Microplásticos , Poluentes Químicos da Água , Ásia , Monitoramento Ambiental , Oceano Índico , Plásticos , Poluentes Químicos da Água/análise
17.
Environ Sci Technol ; 56(3): 1586-1593, 2022 02 01.
Artigo em Inglês | MEDLINE | ID: mdl-35038862

RESUMO

Atmospheric black carbon (BC) has a large yet highly uncertain contribution to global warming. When mixed with non-BC/coating material during atmospheric aging, the BC light absorption can be enhanced through the lensing effect. Laboratory and modeling studies have consistently found strong BC absorption enhancement, while the results in ambient measurements are conflicting, with some reporting weak absorption enhancement even for particles with large bulk coating amounts. Here, from our direct field observations, we report both large and minor absorption enhancement factors for different BC-containing particle populations with large bulk non-BC-to-BC mass ratios. By gaining insights into the measured coating material distribution across each particle population, we find that the level of absorption enhancement is strongly dependent on the particle-resolved mixing state. Our study shows that the greater mixing-state heterogeneity results in the larger difference between observed and predicted absorption enhancement. We demonstrate that by considering the variability in coating material thickness in the optical model, the previously observed model measurement discrepancy of absorption enhancement can be reconciled. The observations and improved optical models reported here highlight the importance of mixing-state heterogeneity on BC's radiative forcing, which should be better resolved in large-scale models to increase confidence when estimating the aerosol radiation effect.


Assuntos
Carbono , Fuligem , Aerossóis/análise , Aquecimento Global
18.
Environ Pollut ; 292(Pt A): 118266, 2022 Jan 01.
Artigo em Inglês | MEDLINE | ID: mdl-34610414

RESUMO

Cooking is an important source of organic aerosols (OA), particularly in urban areas, but it has not been explicitly included in current emission inventories in China. This study estimated the organic aerosol emissions from cooking during winter over the Pearl River Delta (PRD) region, China. Using the retrieved hourly cooking organic aerosol (COA) concentrations at two sites in Hong Kong and Guangzhou, population density, and daily per capita COA emissions, we determined the spatial and temporal distribution of COA emissions over the PRD region based on two approaches by treating COA as non-volatile (NVCOA) and semi-volatile (SVCOA), respectively. By using the estimated COA emissions and the Weather Research and Forecasting model coupled with chemistry (WRF-Chem) model, we reproduced the diurnal cycles of COA concentrations at the PolyU site in Hong Kong and Panyu site in Guangzhou. We also resolved the different patterns of COA between weekdays and weekends. The mean COA concentration during wintertime over the urban areas of the PRD region was 0.7 µg m-3 and 0.9 µg m-3 for the NVCOA and SVCOA cases, respectively, contributing 5.1% and 6.9% to the urban OA concentrations. The total COA emissions in winter over the PRD region were estimated to be 3.5 × 108 g month-1 and 3.8 × 108 g month-1 for the NVCOA and SVCOA cases, respectively, adding 34.8% and 37.8% to the total primary organic aerosol emissions. Considering COA emissions in the model increased the mean regional OA concentrations by 4.6% and 7.4% for the NVCOA and SVCOA cases, respectively. Our study therefore highlights the importance of cooking activities to OA concentrations in winter over the PRD region.


Assuntos
Poluentes Atmosféricos , Material Particulado , Aerossóis/análise , Poluentes Atmosféricos/análise , China , Culinária , Monitoramento Ambiental , Material Particulado/análise
19.
China CDC Wkly ; 3(23): 500-506, 2021 Jun 04.
Artigo em Inglês | MEDLINE | ID: mdl-34594922

RESUMO

What is already known about this topic? Climate change and air pollution are two important environmental issues in China. It is important to investigate particulate matter with aerodynamic diameter less than 2.5 µm (PM2.5)-related health impacts from climate change and air pollution emission control. What is added by this report? Deaths and years of life lost related to PM2.5 would increase in climate change scenario, although emission control would outweigh the influence of climate change. What are the implications for public health practice? More targeted actions should be taken to meet challenges of exacerbated PM2.5 pollutions and its health impacts related to climate change in the future.

20.
Environ Sci Technol ; 55(9): 5711-5720, 2021 05 04.
Artigo em Inglês | MEDLINE | ID: mdl-33861585

RESUMO

Particulate nitrate photolysis can produce oxidants (i.e., OH, NO2, and NO2-/HNO2) in aqueous droplets and may play a potential role in increased atmospheric oxidative capacity. Our earlier works have reported on the SO2 oxidation promoted by nitrate photolysis to produce sulfate. Here, we used glyoxal as a model precursor to examine the role of particulate nitrate photolysis in the formation of secondary organic aerosol (SOA) from particle-phase oxidation of glyoxal by OH radicals. Particles containing sodium nitrate and glyoxal were irradiated at 300 nm. Interestingly, typical oxidation products of oxalic acid, glyoxylic acid, and higher-molecular-weight products reported in the literature were not found in the photooxidation process of glyoxal during nitrate photolysis in the particle phase. Instead, formic acid/formate production was found as the main oxidation product. At glyoxal concentration higher than 3 M, we found that the formic acid/formate production rate increases significantly with increasing glyoxal concentration. Such results suggest that oxidation of glyoxal at high concentrations by OH radicals produced from nitrate photolysis in aqueous particles may not contribute significantly to SOA formation since formic acid is a volatile species. Furthermore, recent predictions of formic acid/formate concentration from the most advanced chemical models are lower than ambient observations at both the ground level and high altitude. The present study reveals a new insight into the production of formic acid/formate as well as a sink of glyoxal in the atmosphere, which may partially narrow the gap between model predictions and field measurements in both species.


Assuntos
Glioxal , Nitratos , Aerossóis , Formiatos , Fotólise
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