Study of the unknown HONO daytime source at a European suburban site during the MEGAPOLI summer and winter field campaigns

International audienceNitrous acid measurements were carried out during the MEGAPOLI summer and winter field campaigns at SIRTA observatory in Paris surroundings. Highly variable HONO levels were observed during the campaigns, ranging from 10 ppt to 500 ppt in summer and from 10 ppt to 1.7 ppb in winter. Significant HONO mixing ratios have also been measured during daytime hours, comprised between some tenth of ppt and 200 ppt for the summer campaign and between few ppt and 1 ppb for the winter campaign. Ancillary measurements, such as NOx , O3 , photolysis frequencies, meteorological parameters (pressure, temperature, relative humidity , wind speed and wind direction), black carbon concentration , total aerosol surface area, boundary layer height and soil moisture, were conducted during both campaigns. In addition, for the summer period, OH radical measurements were made with a CIMS (Chemical Ionisation Mass Spectrometer). This large dataset has been used to investigate the HONO budget in a suburban environment. To do so, calculations of HONO concentrations using PhotoStationary State (PSS) approach have been performed, for daytime hours. The comparison of these calculations with measured HONO concentrations revealed an underestimation of the calculations making evident a missing source term for both campaigns. This unknown HONO source exhibits a bell-shaped like average diurnal profile with a maximum around noon of approximately 0.7 ppb h−1 and 0.25 ppb h−1 , during summer and winter respectively. This source is the main HONO source during daytime hours for both campaigns. In both cases, this source shows a slight positive correlation with J (NO2) and the product between J (NO2) and soil moisture. This original approach had, thus, indicated that this missing source is photolytic and might be heterogeneous occurring at ground surface and involving water content available on the ground. Published by Copernicus Publications on behalf of the European Geosciences Union. 2806 V. Michoud et al.: Study of the unknown HONO daytime sourc

Particle and VOC emission factor measurements for anthropogenic sources in West Africa

A number of campaigns have been carried out to establish the emission factors of pollutants from fuel combustion in West Africa, as part of work package 2 ("Air Pollution and Health") of the DACCIWA (Dynamics-Aerosol-Chemistry-Cloud Interactions in West Africa) FP7 program. Emission sources considered here include wood (hevea and iroko) and charcoal burning, charcoal making, open trash burning, and vehicle emissions, including trucks, cars, buses and two-wheeled vehicles. Emission factors of total particulate matter (TPM), elemental carbon (EC), primary organic carbon (OC) and volatile organic compounds (VOCs) have been established. In addition, emission factor measurements were performed in combustion chambers in order to reproduce field burning conditions for a tropical hardwood (hevea), and obtain particulate emission factors by size (PM0.25, PM1, PM2.5 and PM10). Particle samples were collected on quartz fiber filters and analyzed using gravimetric method for TPM and thermal methods for EC and OC. The emission factors of 58 VOC species were determined using offline sampling on a sorbent tube. Emission factor results for two species of tropical hardwood burning of EC, OC and TPM are 0.98 ± 0.46 g kg-1 of fuel burned (g kg-1), 11.05 ± 4.55 and 41.12 ± 24.62 g kg-1, respectively. For traffic sources, the highest emission factors among particulate species are found for the two-wheeled vehicles with two-stroke engines (2.74 g kg-1 fuel for EC, 65.11 g kg-1 fuel for OC and 496 g kg-1 fuel for TPM). The largest VOC emissions are observed for two-stroke two-wheeled vehicles, which are up to 3 times higher than emissions from light-duty and heavy-duty vehicles. Isoprene and monoterpenes, which are usually associated with biogenic emissions, are present in almost all anthropogenic sources investigated during this work and could be as significant as aromatic emissions in wood burning (1 g kg-1 fuel). EC is primarily emitted in the ultrafine fraction, with 77 % of the total mass being emitted as particles smaller than 0.25 μm. The particles and VOC emission factors obtained in this study are generally higher than those in the literature whose values are discussed in this paper. This study underlines the important role of in situ measurements in deriving realistic and representative emission factors

Le comportement des hydrocarbures non-méthaniques en zone urbaine (identification et contributions des sources)

LILLE1-BU (590092102) / SudocSudocFranceF

Impact de la mousson sur la chimie photooxydante en Afrique de l'Ouest

Le changement climatique est relié à l évolution de la composition chimique de l atmosphère et de sa capacité oxydante, impliquant le système COV-NOy-HOx-O3. La troposphère tropicale, de l Afrique de l Ouest en particulier, joue un rôle critique sur la composition atmosphérique globale pour trois raisons majeures : (1) l existence d importantes sources de précurseurs d espèces photooxydantes, (2) une photochimie active, (3) une activité convective intense en période de mousson. Pour évaluer son rôle, il est nécessaire de bien caractériser ces différents processus et leur interaction. Cette question est au coeur du programme international AMMA (Analyse Multidisciplinaire de la Mousson Africaine) dans lequel s inscrit cette thèse. Ce travail a pour objectif de caractériser et d évaluer l impact de la convection nuageuse profonde sur la chimie photooxydante de la troposphère libre en Afrique de l Ouest, en particulier pour les composés organiques volatils (COV), qui sont d importants précurseurs d ozone. Ce travail s appuie sur les données physico-chimiques recueillies sur les deux avions de recherche français au cours de la campagne d observation intensive de l été 2006 de AMMA. Afin de compléter le dispositif instrumental embarqué, une nouvelle instrumentation de mesure indirecte des COV a été d abord développée. Puis, l utilisation de traceurs physico-chimiques et la mise en place d outils diagnostiques appliqués aux COV (profils verticaux de concentrations, rapport de concentration de COV ad hoc, horloge photochimique, réactivité totale vis-à-vis de OH) ont montré que la convection profonde assure un transport vertical rapide et efficace des espèces gazeuses réactives émises près de la surface vers la haute troposphère. Enfin, un modèle photochimique de boîte 0D a permis de renseigner l évolution de la composition chimique des masses d air post-convectives. Les simulations montrent que les espèces transportées par la convection participent activement à la chimie et conduisent à une production nette et significative d ozone dans la haute troposphère. La sensibilité de la production d ozone aux précurseurs gazeux (COV et NOx) a été également évaluéeRecent climatic change is tightly linked to the evolution of the chemical composition of the atmosphere and its oxidizing capacity through VOC-NOy-HOx-O3 system. The tropical troposphere, in particular of West Africa, plays a major role in the global atmospheric composition for three major reasons: (1) the existence of important ozone precursor sources, (2) an active photochemistry, (3) an intense convective activity during the monsoon period. To evaluate its role, it is necessary to characterize these processes and their interactions. This is one of the main objectives of the AMMA (African Monsoon Multidisciplinary Analyzes) international program. The present work goes through the frame of AMMA. Its main objective is to characterize and evaluate deep convection impact on the upper troposphere chemistry of West Africa, in particular for volatile organic compounds (VOC). This work is based on the data collected on the two French research aircrafts during the special observation period of AMMA in summer 2006. In order to enhance the instrumental device deployed onboard, a new offline instrumentation for non-methane hydrocarbons (NMHC) measurement was developed. Then, various physical and chemical tracers and several diagnostic tools applied to VOC data (vertical profiles, concentration ratios, photochemical clock, OH reactivity) showed that deep convection provides a fast and effective vertical transfer of reactive species emitted near the surface to the upper troposphere. At last, a photochemical box model 0D was used to simulate the chemical evolution of the composition of postconvective air masses. Simulations showed that reactive species transported by deep convection participate actively to the upper troposphere chemistry and lead to a significant and net ozone production. Ozone production sensitivity to VOC and NOx was also evaluated in the modelPARIS-EST-Université (770839901) / SudocSudocFranceF

Light oxygenated volatile organic compound concentrations in an Eastern Mediterranean urban atmosphere rivalling those in megacities

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One decade of VOCs measurements in São Paulo megacity: Composition, variability, and emission evaluation in a biofuel usage context

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Safire : des avions au service de la recherche en environnement

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Source apportionment vs. emission inventories of non-methane hydrocarbons (NMHC) in an urban area of the Middle East: local and global perspectives

International audienceWe applied the positive matrix factorization model to two large data sets collected during two intensive measurement campaigns (summer 2011 and winter 2012) at a suburban site in Beirut, Lebanon, in order to identify NMHC (non-methane hydrocarbons) sources and quantify their contribution to ambient levels. Six factors were identified in winter and five factors in summer. PMF-resolved source profiles were consistent with source profiles established by near-field measurements. The major sources were traffic-related emissions (combustion and gasoline evaporation) in winter and in summer accounting for 51 and 74 wt %, respectively, in agreement with the national emission inventory. The gasoline evaporation related to traffic source had a significant contribution regardless of the season (22 wt % in winter and 30 wt % in summer). The NMHC emissions from road transport are estimated from observations and PMF results, and compared to local and global emission inventories. The PMF analysis finds reasonable differences on emission rates, of 20-39 % higher than the national road transport inventory. However, global inventories (ACCMIP, EDGAR, MACC-ity) underestimate the emissions up to a factor of 10 for the transportation sector. When combining emission inventory to our results, there is strong evidence that control measures in Lebanon should be targeted on mitigating the NMHC emissions from the traffic-related sources. From a global perspective , an assessment of VOC (volatile organic compounds) an-thropogenic emission inventories for the Middle East region as a whole seems necessary as these emissions could be much higher than expected at least from the road transport sector