Recent studies based on observations have shown the impact of lockdown measures taken in various European countries to contain the Covid-19 pandemic on air quality. However, these studies are often ...limited to compare situations without and with lockdown measures, which correspond to different time periods and then under different meteorological conditions. We propose a modelling study with the WRF-CHIMERE modelling suite for March 2020, an approach allowing to compare atmospheric composition with and without lockdown measures without the biases of meteorological conditions. This study shows that the lockdown effect on atmospheric composition, in particular through massive traffic reductions, has been important for several short-lived atmospheric trace species, with a large reduction in NO2 concentrations, a lower reduction in Particulate Matter (PM) concentrations and a mitigated effect on ozone concentrations due to non-linear chemical effects.
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•Air pollution modelling•COVID19 epidemy•Regional modelling•Anthropogenic emissions scenario•Impact of emissions reduction
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
CHIMERE is a chemistry-transport model designed for regional atmospheric composition. It can be used at a variety of scales from local to continental domains. However, due to the model design and its ...historical use as a regional model, major limitations had remained, hampering its use at hemispheric scale, due to the coordinate system used for transport as well as to missing processes that are important in regions outside Europe. Most of these limitations have been removed in the CHIMERE-2017 version, allowing its use in any region of the world and at any scale, from the scale of a single urban area up to hemispheric scale, with or without polar regions included. Other important improvements have been made in the treatment of the physical processes affecting aerosols and the emissions of mineral dust. From a computational point of view, the parallelization strategy of the model has also been updated in order to improve model numerical performance and reduce the code complexity. The present article describes all these changes. Statistical scores for a model simulation over continental Europe are presented, and a simulation of the circumpolar transport of volcanic ash plume from the Puyehue volcanic eruption in June 2011 in Chile provides a test case for the new model version at hemispheric scale.
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IZUM, KILJ, NUK, PILJ, PNG, SAZU, UL, UM, UPUK
The kriging-based estimation of the different types of atmospheric particulate matter (PM) pollutions defined in the air quality regulation raises some operational problems because the (co)kriging ...equations are obtained by minimizing a linear combination of the estimation variances subject to unbiasedness constraints. As a consequence, the estimation process can result in total PM10 concentrations that are less than the PM2.5 concentrations which would be physically impossible. In a previous publication, it was shown that a convenient external drift modeling can reduce the number of spatial locations where the inequality constraint is not satisfied, without completely solving the problem. In this work, the formulation of the cokriging system is modified, inspired by previous works focusing on positive kriging. The introduction of additional constraints on the cokriging weights are presented, leading to a unique and optimal solution to the problem of cokriging under inequality constraints between two variables. Some computational and algorithmic details are introduced. An evaluation of the penalized cokriging is provided by using the European PM monitoring sites dataset: some maps and performance scores are given to assess the relevance of our iterative optimization scheme.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
•First epidemiological study with extended annual exposure data (up to 22 years).•Airborne BaP exposure was significantly associated with overall breast cancer risk.•The association was greater among ...women who underwent menopausal transition.•Positive associations were observed for ER+, PR+, ER+ PR+, and grade 3 breast cancer.•Significant effect modification was observed for tobacco smoking status.
Benzoapyrene (BaP) is an endocrine-disrupting pollutant formed during incomplete combustion of organic materials. It has been recognized as a reproductive and developmental toxicant, however epidemiological evidence of the long-term effect of ambient air BaP on breast cancer (BC) is limited. Thus we evaluated associations between ambient air BaP exposure and risk of BC, overall and according to menopausal status and molecular subtypes (estrogen receptor negative/positive (ER−/ER+) and progesterone receptor negative/positive (PR−/PR+)), stage and grade of differentiation of BC in the French E3N cohort study.
Within a nested case-control study of 5222 incident BC cases and 5222 matched controls, annual BaP exposure was estimated using a chemistry-transport model (CHIMERE) and was assigned to the geocoded residential addresses of participants for each year during the 1990–2011 follow-up period. Multivariable conditional logistic regression models were used to estimate odds ratios (ORs) and 95% confidence intervals (CIs).
Overall, cumulative airborne BaP exposure was significantly associated with the overall risk of BC, for each 1 interquartile range (IQR) increase in the concentration levels of BaP (1.42 ng/m3), the OR = 1.15 (95% CI: 1.04–1.27). However, by menopausal status, the significant positive association remained only in women who underwent menopausal transition (i.e. premenopausal women at inclusion who became postmenopausal at diagnosis), OR per 1 IQR = 1.20 (95% CI: 1.03–1.40). By hormone receptor status, positive associations were observed for ER+, PR + and ER + PR + BC, with ORs = 1.17 (95% CI: 1.04–1.32), 1.16 (95% CI: 1.01–1.33), and 1.17 (95% CI: 1.01–1.36) per 1 IQR, respectively. There was also a borderline positive association between BaP and grade 3 BC (OR per 1 IQR = 1.15 (95% CI: 0.99–1.34).
We provide evidence of increased risk of BC associated with cumulative BaP exposure, which varied according to menopausal status, hormone receptor status, and grade of differentiation of BC. Our results add further epidemiological evidence to the previous experimental studies suggesting the adverse effects of BaP.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
In the framework of the FAIRMODE initiative, a set of simulations was performed using the WRF and CHIMERE models. The simulation period is chosen to cover a Particulate Matter (PM) pollution episode ...that happened in February 2015 over the Parisian area. A thorough validation of the reference simulation is presented, showing a good agreement between the measurements and the model both for PM components and major gaseous species. The PM composition analysis shows that the major contributors to the PM total concentration are nitrates and organic aerosols, followed by ammonium. An analysis of emission reduction scenarios compared to the reference simulation is also presented and different configurations of these scenarios are analyzed. Exceedances regarding to the last World Health Organization (WHO) guidelines are assessed, concluding that even if the most severe mitigation analyzed here (−50% emissions reduction) was applied over Paris, exceedances would still happen for PM. Emission reduction scenarios show that ozone concentrations are sensitive to NOx reductions inside the city with an increase in concentrations, while for PM a systematic decrease is observed whichever precursor emission is reduced. Coupling effects are explored and the impact of PM concentrations on the radiative and thermodynamic budgets is quantified. Scenarios are repeated both with different durations and different intensities and the most efficient configuration leading to exceedances reduction is discussed.
Dry deposition of semi-volatile organic compounds (SVOC) is not currently treated in most chemical transport models of air quality and this omission has been identified as a possible major source of ...uncertainty. The effect of dry deposition of SVOC on the concentration of secondary organic aerosols (SOA) is investigated in summertime with the chemical transport model CHIMERE that simulates SOA concentrations by means of molecular SOA surrogate species. Omitting dry deposition could overestimate SOA concentrations by as much as 50%. This overestimation is larger during nighttime due to higher relative humidity.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UL, UM, UPCLJ, UPUK
Airborne particulate matter (PM) is a pollutant of concern not only because of its adverse effects on human health but also on visibility and the radiative budget of the atmosphere. PM can be ...considered as a sum of solid/liquid species covering a wide range of particle sizes with diverse chemical composition. Organic aerosols may be emitted (primary organic aerosols, POA), or formed in the atmosphere following reaction of volatile organic compounds (secondary organic aerosols, SOA), but some of these compounds may partition between the gas and aerosol phases depending upon ambient conditions. This review focuses on carbonaceous PM and gaseous precursors emitted by road traffic, including ultrafine particles (UFP) and polycyclic aromatic hydrocarbons (PAHs) that are clearly linked to the evolution and formation of carbonaceous species. Clearly, the solid fraction of PM has been reduced during the last two decades, with the implementation of after-treatment systems abating approximately 99% of primary solid particle mass concentrations. However, the role of brown carbon and its radiative effect on climate and the generation of ultrafine particles by nucleation of organic vapour during the dilution of the exhaust remain unclear phenomena and will need further investigation. The increasing role of gasoline vehicles on carbonaceous particle emissions and formation is also highlighted, particularly through the chemical and thermodynamic evolution of organic gases and their propensity to produce particles. The remaining carbon-containing particles from brakes, tyres and road wear will still be a problem even in a future of full electrification of the vehicle fleet. Some key conclusions and recommendations are also proposed to support the decision makers in view of the next regulations on vehicle emissions worldwide.
NOx emissions from lightning have been added to the CHIMERE v2020r1 model using a parameterization based on convective clouds. In order to estimate the impact of these emissions on pollutant ...concentrations, two simulations, using the online coupled WRF-CHIMERE models with and without NOx emissions from lightning, have been carried out over the months of July and August 2013 and over a large area covering Europe and the northern part of Africa. The results show that these emissions modify the pollutant concentrations as well as the meteorology. The changes are most significant where the strongest emissions are located. Adding these emissions improves Aerosol Optical Depth in Africa but has a limited impact on the surface concentrations of pollutants in Europe. For the two-month average we find that the maximum changes are localized and may reach ±0.5 K for 2 m temperature, ±0.5 m s−1 for 10 m wind speed, 10 W m−2 for short wave radiation surface flux, and 50 and 2 μg m−3 for dust and sea salt surface concentrations, respectively. This leads to maximum changes of 1 μg m−3 for surface concentrations of PM2.5.
Deposition of the gas fraction of Semi-Volatile Organic Compounds (SVOC) may be an important removal pathway and may strongly influence concentrations of organic aerosols due to the gas-particle ...partitioning of SVOC. All the studies on this process are based on the classic Wesely resistance approach that uses Henry's law constants to calculate a deposition rate scaled on the deposition rate of SO2. However, even highly hydrophobic SVOC could be efficiently removed by the vegetation and soils as shown by numerous studies on Persistent Organic Pollutant (POP) modeling. Moreover, the re-volatilization of deposited SVOC is possible and could influence organic aerosol concentrations.
An atmosphere-soil-vegetation module was developed and implemented in the 3D air quality model CHIMERE 2017β to represent the accumulation of compounds in the different compartments of the biosphere and the exchanges between them. The soil compartment was represented with a multi-layer approach (the layers corresponding to different in-soil depths) to simulate the multiphase diffusion of compounds inside the soil. Exchanges of SVOC between the air, soil and vegetation compartments were simulated using bi-directional approaches based on Rg (the gas-phase partitioning in the soil compartment) and Kva the vegetation-air partitioning coefficient. Parameters were estimated based on the physical properties of the compounds and their molecular structure.
Simulations performed over Europe show that air-vegetation-soil exchanges may be a more efficient removal pathway than dry deposition of particles for SVOC with a gas-phase fraction above 10%. Considering air-vegetation-soil exchanges in the simulations lead to a decrease of organic aerosol concentrations by 15% and primary SVOC (considered as hydrophobic compounds) may be efficiently removed by those pathways (contrary to what is calculated with the Wesely approach). This decrease of concentrations is mainly due to air-vegetation exchanges. During summer, the use of the Wesely approach may lead to a slight overestimation of deposition fluxes (leading to an underestimation of concentration by 1%).
Re-volatilization may limit the amount of deposited SVOC. Depending on assumptions, simulations showed that re-emissions (inversion of exchanges toward the emissions) in summer of SVOC accumulated during winter is theoretically possible and may be a minor source of organic aerosol.
•A module for air/soil/vegetation exchanges of SVOC have been implemented into CHIMERE.•Strong deposition of primary SVOC from biomass burning in winter was simulated with the exchange module contrary to the Wesely approach.•However, similar concentrations of secondary organic aerosols were simulated in summer with the Wesely approach and the exchange module.•Re-emissions (inversion of the exchange flux toward emissions) of SVOC accumulated in ecosystems are theoretically possible.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UL, UM, UPCLJ, UPUK
The accurate simulation of meteorological conditions, especially within the planetary boundary layer (PBL), is of major importance for air quality modeling. In the present work, we have used the ...Weather Research and Forecast (WRF) model coupled with the chemistry transport model (CTM) CHIMERE to understand the impact of physics parameterizations on air quality simulation during a short-term pollution episode on the Paris region. A lower first model layer with a 4 m surface layer could better reproduce the transport and diffusion of pollutants in a real urban environment. Three canopy models could better reproduce a 2 m temperature (T2) in the daytime but present a positive bias from 1 to 5 °C during the nighttime; the multi-urban canopy scheme “building effect parameterization” (BEP) underestimates the 10 m windspeed (W10) around 1.2 m s−1 for the whole episode, indicating the city cluster plays an important role in the diffusion rate in urban areas. For the simulation of pollutant concentrations, large differences were found between three canopy schemes, but with an overall overestimation during the pollution episode, especially for NO2 simulation, the average mean biases of NO2 prediction during the pollution episode were 40.9, 62.2, and 29.7 µg m−3 for the Bulk, urban canopy model (UCM), and BEP schemes, respectively. Meanwhile, the vertical profile of the diffusion coefficients and pollutants indicated an important impact of the canopy model on the vertical diffusion. The PBL scheme sensitivity tests displayed an underestimation of the height of the PBL when compared with observations issued from the Lidar. The YonSei University scheme YSU and Boulac PBL schemes improved the PBL prediction compared with the Mellor–Yamada–Janjic (MYJ) scheme. All the sensitivity tests, except the Boulac–BEP, could not fairly reproduce the PBL height during the pollution episode. The Boulac–BEP scheme had significantly better performances than the other schemes for the simulation of both the PBL height and pollutants, especially for the NO2 and PM2.5 (particulate matter 2.5 micrometers or less in diameter) simulations. The mean bias of the NO2, PM2.5, and PM10 (particulate matter 10 micrometers or less in diameter) prediction were −5.1, 1.2, and −8.6 µg m−3, respectively, indicating that both the canopy schemes and PBL schemes have a critical effect on air quality prediction in the urban region.
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