Showing papers by "Karine Sartelet published in 2021"

Simulation of primary and secondary particles in the streets of Paris using MUNICH

Abstract: High particle concentrations are observed in the streets. Regional-scale chemistry-transport models are not able to reproduce these high concentrations, because their spatial resolution is not fine enough. Local-scale models are usually employed to simulate the high concentrations in street networks, but they often adopt substantial simplifications to determine background concentrations and use simplified chemistry. This study presents the new version of the local-scale Model of Urban Network of Intersecting Canyons and Highways (MUNICH) that integrates background concentrations simulated by the regional-scale chemistry-transport model Polair3D, and uses the same complex chemistry module as Polair3D, SSH-aerosol, to represent secondary aerosol formation. Gas and aerosol concentrations in Paris streets are simulated with MUNICH, considering a street-network with more than 3800 street segments, between 3 May and 30 June. Comparisons with PM10 and PM2.5 measurements at several locations of Paris show that the high PM10 and PM2.5 concentrations are well represented. Furthermore, the simulated chemical composition of fine particles corresponds well to a yearly measured composition. To understand the influence of the secondary pollutant formation, several sensitivity simulations are conducted. Simulations with and without gas-phase chemistry show that the influence of gas-phase chemistry on the formation of NO2 is large (37% on average over May and across all modelled streets), but the influence on condensables is lower (less than 2% to 3% on average at noon for inorganics and organics), but may reach more than 20% depending on the street. The assumption used to compute gas/particle mass transfer by condensation/evaporation is important for inorganic and organic compounds of particles, as using the thermodynamic equilibrium assumption leads to an overestimation of the organic concentrations by 4.7% on average (up to 31% at noon depending on the streets). Ammonia emissions from traffic lead to an increase in inorganic concentrations by 3% on average, reaching 26% depending on the street segments. Not taking into account gas-phase chemistry and aerosol dynamics in the modelling leads to an underestimation of organic concentrations by about 11% on average over the streets and time, but this underestimation may reach 51% depending on the streets and the time of the day.

Black carbon modeling in urban areas: investigating the influence of resuspension and non-exhaust emissions in streets using the Street-in-Grid model for inert particles (SinG-inert)

Abstract: . Black carbon (BC) is a primary and inert pollutant often used as a traffic tracer. Even though its concentrations are generally low at the regional scale, BC presents very high concentrations in streets (at the local scale), potentially with important effects on human health and the environment. Modeling studies of BC concentrations usually underestimate BC concentrations due to uncertainties in both emissions and modeling. Both exhaust and non-exhaust traffic emissions present uncertainties, but the uncertainties with respect to non-exhaust emissions, such as tire, brake, and road wear as well as particle resuspension, are particularly high. In terms of modeling, street models do not always consider the two-way interactions between the local and regional scales. Using a two-way modeling approach, a street with high BC concentrations may influence urban background concentrations above the street, which can subsequently enhance the BC concentrations in the same street. This study uses the multiscale Street-in-Grid model (SinG) to simulate BC concentrations in a suburban street network in Paris, taking the two-way coupling between local and regional scales into account. The BC concentrations in streets proved to have an important influence on urban background concentrations. The two-way dynamic coupling leads to an increase in BC concentrations in large streets with high traffic emissions (with a maximal increase of about 48 %) as well as a decrease in narrow streets with low traffic emissions and low BC concentrations (with a maximal decrease of about 50 %). A new approach to estimate particle resuspension in streets is implemented, strictly respecting the mass balance on the street surface. The resuspension rate is calculated from the available deposited mass on the street surface, which is estimated based on particle deposition and wash-off parameterizations adapted to street-canyon geometries. The simulations show that particle resuspension presents a low contribution to BC concentrations, as the deposited mass is not significant enough to justify high resuspension rates. Non-exhaust emissions, such as brake, tire, and road wear, may largely contribute to BC emissions, with a contribution that is equivalent to exhaust emissions. Here, a sensitivity analysis of BC concentrations is performed by comparing simulations with different emission factors of tire, brake, and road wear. The different emission factors considered are estimated based on the literature. We found a satisfying model–measurement comparison using high tire wear emission factors, which may indicate that the tire emission factors usually used in Europe are probably underestimated. These results have important policy implications: public policies replacing internal combustion engines with electric vehicles may not eliminate BC air pollution but only reduce it by half.

Evolution under dark conditions of particles from old and modern diesel vehicles, in a new environmental chamber characterized with fresh exhaust emissions

Abstract: . Atmospheric particles have several impacts on health and environment, especially in urban areas. Part of those particles is not fresh, and has undergone atmospheric chemical and physical processes. Due to not representative experimental conditions, and experimental artifacts such as particle wall losses in chambers, there are uncertainties on the effects of physical processes (condensation, nucleation and coagulation) and how they act on particles from modern vehicles. This study develops a new method to correct wall losses, accounting for size dependence and experiment-to-experiment variations, and applies it to the evolution of fresh diesel exhaust particles to characterize the physical processes acting on them. The correction method is based on the black carbon decay and a size-dependent coefficient to correct particle distributions. Exhaust from 6 diesel passenger cars, Euro 3 to Euro 6, driven on a chassis dynamometer with Artemis Urban cold start and Artemis Motorway cycles, was injected in an 8 m3 chamber with Teflon walls. The physical evolution of particles was characterized during 6 to 10 hours. Condensation occurs even without photochemical reactions, due to the presence of intermediate volatility organic compounds and semi-volatile organic compounds which were quantified at emission, and induces a particle mass increase up to 17 %.h−1, mainly for the older vehicles (Euro 3 and Euro 4). Condensation is 4 times faster when the available particle surface if multiplied by 3. If initial particle number concentration is below [8–9] × 104 #.cm−3, it can increase up to 25 %.h−1 due to nucleation or condensation on particles below 14 nm. Above this threshold, particle number concentration decreases due to coagulation, up to −27 %.h−1.

Improvement in Modeling of OH and HO2 Radical Concentrations during Toluene and Xylene Oxidation with RACM2 Using MCM/GECKO-A

Abstract: Due to their major role in atmospheric chemistry and secondary pollutant formation such as ozone or secondary organic aerosols, an accurate representation of OH and HO2 (HOX) radicals in air quality models is essential. Air quality models use simplified mechanisms to represent atmospheric chemistry and interactions between HOX and organic compounds. In this work, HOX concentrations during the oxidation of toluene and xylene within the Regional Atmospheric Chemistry Mechanism (RACM2) are improved using a deterministic-near-explicit mechanism based on the Master Chemical Mechanism (MCM) and the generator of explicit chemistry and kinetics of organics in the atmosphere (GECKO-A). Flow tube toluene oxidation experiments are first simulated with RACM2 and MCM/GECKO-A. RACM2, which is a simplified mechanism, is then modified to better reproduce the HOX concentration evolution simulated by MCM/GECKO-A. In total, 12 reactions of the oxidation mechanism of toluene and xylene are updated, making OH simulated by RACM2 up to 70% more comparable to the comprehensive MCM/GECKO-A model for chamber oxidation simulations.

Combining homogeneous and heterogeneous chemistry to model inorganic compound concentrations in indoor environments: the H 2 I model (v1.0)

Abstract: . Homogeneous reactivity has been extensively studied in recent years through outdoor air-quality simulations. However, indoor atmospheres are known to be largely influenced by another type of chemistry, which is their reactivity with surfaces. Despite progress in the understanding of heterogeneous reactions, such reactions remain barely integrated into numerical models. In this paper, a room-scale, indoor air-quality (IAQ) model is developed to represent both heterogeneous and homogeneous chemistry. Thanks to the introduction of sorbed species, deposition and surface reactivity are treated as two separate processes, and desorption reactions are incorporated. The simulated concentrations of inorganic species are compared with experimental measurements acquired in a real room, thus allowing calibration of the model's undetermined parameters. For the duration of the experiments, the influence of the simulation's initial conditions is strong. The model succeeds in simulating the four inorganic species concentrations that were measured, namely NO, NO 2 , HONO and O 3 . Each parameter is then varied to estimate its sensitivity and to identify the most prevailing processes. The air-mixing velocity and the building filtration factor are uncertain parameters that appear to have a strong influence on deposition and on the control of transport from outdoors, respectively. As expected, NO 2 surface hydrolysis plays a key role in the production of secondary species. The secondary production of NO by the reaction of sorbed HONO with sorbed HNO 3 stands as an essential component to integrate into IAQ models.