Towards a quantification of the CO2 emission sectors of the Paris megacity

En réponse aux changements climatiques avérés et à une qualité de l'air qui se dégrade, la quantification des émissions de gaz à effet de serre et des polluants atmosphériques des régions urbanisées suscite un intérêt croissant. La meilleure description des émissions anthropiques actuellement disponible est proposée par les inventaires d'émission. Mais leurs estimations, fournies par secteur, reposent sur la combinaison de données d'activité et de facteurs d'émission déterminés sur bancs d'essai et qui ne représentent pas forcément bien les conditions réelles d'émission. Paris, en tant que 3e mégapole européenne, se place dans ce contexte et nous avons choisi d'utiliser des méthodes reposant sur l'acquisition de mesures in situ en région parisienne pour caractériser le signal urbain et vérifier les estimations de l'inventaire régional haute résolution d'Airparif. Les méthodes mises en place dans ce travail de thèse reposent sur l'utilisation conjointe de différents traceurs atmosphériques (CO, NOx, COV). En effet, ils sont co-émis au CO2 lors des processus de combustions incomplètes dans des proportions supposées caractéristiques du secteur d'émission. Les rapports de concentration entre les différentes espèces co-émises sont donc un outil de choix pour cette étude. Nous avons alors développé différentes méthodes d'évaluation de ces rapports pour caractériser les émissions pour l'une des sources prédominantes de CO2 à Paris (le trafic routier) ou dans le panache parisien. Les variabilités spatiale et saisonnière des rapports ont notamment pu être étudiées et les conclusions obtenues n'étaient pas forcément référencées dans les estimations des inventaires ou d'études antérieures. Nous avons comparé nos résultats aux estimations fournies par l'inventaire le plus récent d'Airparif qui apparait généralement surestimer ces rapports. Enfin, nous avons combiné les résultats de l'approche multi-espèces à ceux fournis par l'analyse des isotopes du carbone dans le CO2 (souvent utilisés comme référence pour l'étude des émissions anthropiques). D'après leur analyse, les émissions de CO2 à Paris sont majoritairement d'origine fossile (81 %) et l'utilisation des combustibles fossiles est répartie quasi équitablement. Finalement, l'accord satisfaisant trouvé entre les deux démarches (multi-espèces et isotopique) a permis d'affirmer leur pertinence pour l'étude des signaux urbains moyens.In response to changing air quality and climate, there is a growing interest in quantifying emissions ofatmospheric pollutants and greenhouse gases from urban areas. Currently emission inventories provide the most detailed description of anthropogenic emissions. However, their estimates rely on the combination of activity proxies and emission factors for individual source sectors calibrated for benchmarck situations that may significantly differ from real conditions. Paris, the third largest megacity in Europe, can be considered in this context. We used methods based on in situ measurements in this region to characterise the urban signal and independently assess the latest estimates from the regional inventory. The methods we developed rely on the joint analysis of atmospheric tracers (CO, NOx, VOCs) which are co-emitted with CO2 during incomplete combustion processes in ratios that are characteristic of each emission sector. These ratios between co-emitted species are thus an appropriate tool to study the urban signal. During this PhD, we developed several methods to evaluate the ratios using measurements for a major CO2 emission source in Paris (road traffic) or for measurements acquired in the urban atmosphere. We revealed spatial and seasonal variabilities in these ratios and the main conclusions were not necessarily in complete accordance with the ones from inventories or previous studies. We also compared our results to the estimates provided by the latest regional inventory, which appears to overestimate them in most cases. Finally, we combined the results obtained with the multi-species analysis to the ones provided by isotopic analyses (which are often used as a reference to study anthropogenic emissions). According to the analyses of these measurements, CO2 emissions in Paris came mostly from combustion of fossil fuels (81 %) and the use of each fossil fuel is almost equally distributed. Finally, the satisfactory agreement found between the two approaches (multi-species and isotopic one) confirmed their relevancefor the analysis of mean urban signals

Vers une quantification des secteurs d’émission de CO2 de l’agglomération parisienne

In response to changing air quality and climate, there is a growing interest in quantifying emissions ofatmospheric pollutants and greenhouse gases from urban areas. Currently emission inventories provide the most detailed description of anthropogenic emissions. However, their estimates rely on the combination of activity proxies and emission factors for individual source sectors calibrated for benchmarck situations that may significantly differ from real conditions. Paris, the third largest megacity in Europe, can be considered in this context. We used methods based on in situ measurements in this region to characterise the urban signal and independently assess the latest estimates from the regional inventory. The methods we developed rely on the joint analysis of atmospheric tracers (CO, NOx, VOCs) which are co-emitted with CO2 during incomplete combustion processes in ratios that are characteristic of each emission sector. These ratios between co-emitted species are thus an appropriate tool to study the urban signal. During this PhD, we developed several methods to evaluate the ratios using measurements for a major CO2 emission source in Paris (road traffic) or for measurements acquired in the urban atmosphere. We revealed spatial and seasonal variabilities in these ratios and the main conclusions were not necessarily in complete accordance with the ones from inventories or previous studies. We also compared our results to the estimates provided by the latest regional inventory, which appears to overestimate them in most cases. Finally, we combined the results obtained with the multi-species analysis to the ones provided by isotopic analyses (which are often used as a reference to study anthropogenic emissions). According to the analyses of these measurements, CO2 emissions in Paris came mostly from combustion of fossil fuels (81 %) and the use of each fossil fuel is almost equally distributed. Finally, the satisfactory agreement found between the two approaches (multi-species and isotopic one) confirmed their relevancefor the analysis of mean urban signals.En réponse aux changements climatiques avérés et à une qualité de l'air qui se dégrade, la quantification des émissions de gaz à effet de serre et des polluants atmosphériques des régions urbanisées suscite un intérêt croissant. La meilleure description des émissions anthropiques actuellement disponible est proposée par les inventaires d'émission. Mais leurs estimations, fournies par secteur, reposent sur la combinaison de données d'activité et de facteurs d'émission déterminés sur bancs d'essai et qui ne représentent pas forcément bien les conditions réelles d'émission. Paris, en tant que 3e mégapole européenne, se place dans ce contexte et nous avons choisi d'utiliser des méthodes reposant sur l'acquisition de mesures in situ en région parisienne pour caractériser le signal urbain et vérifier les estimations de l'inventaire régional haute résolution d'Airparif. Les méthodes mises en place dans ce travail de thèse reposent sur l'utilisation conjointe de différents traceurs atmosphériques (CO, NOx, COV). En effet, ils sont co-émis au CO2 lors des processus de combustions incomplètes dans des proportions supposées caractéristiques du secteur d'émission. Les rapports de concentration entre les différentes espèces co-émises sont donc un outil de choix pour cette étude. Nous avons alors développé différentes méthodes d'évaluation de ces rapports pour caractériser les émissions pour l'une des sources prédominantes de CO2 à Paris (le trafic routier) ou dans le panache parisien. Les variabilités spatiale et saisonnière des rapports ont notamment pu être étudiées et les conclusions obtenues n'étaient pas forcément référencées dans les estimations des inventaires ou d'études antérieures. Nous avons comparé nos résultats aux estimations fournies par l'inventaire le plus récent d'Airparif qui apparait généralement surestimer ces rapports. Enfin, nous avons combiné les résultats de l'approche multi-espèces à ceux fournis par l'analyse des isotopes du carbone dans le CO2 (souvent utilisés comme référence pour l'étude des émissions anthropiques). D'après leur analyse, les émissions de CO2 à Paris sont majoritairement d'origine fossile (81 %) et l'utilisation des combustibles fossiles est répartie quasi équitablement. Finalement, l'accord satisfaisant trouvé entre les deux démarches (multi-espèces et isotopique) a permis d'affirmer leur pertinence pour l'étude des signaux urbains moyens

Exploiting stagnant conditions to derive robust emission ratio estimates for CO₂, CO and volatile organic compounds in Paris

International audienceWe propose an approach to estimate urban emission ratios that takes advantage of the enhanced local urban signal in the atmosphere at low wind speed. We apply it to estimate monthly ratios between CO 2 , CO and some VOCs from several atmospheric concentration measurement datasets acquired in the centre of Paris between 2010 and 2014. We find that this approach is not very sensitive to the regional background level definition and that, in the case of Paris, it samples all days (weekdays and weekends) and all hours of the day evenly. A large seasonal variability of the CO / CO 2 ratio in Paris is shown, with a difference of around 60 % between the extreme values and a strong anti-correlation (r 2 = 0.75) with atmospheric temperature. The comparison of the ratios obtained for two short measurement campaigns conducted in two different districts and two different periods (autumn and winter) shows differences ranging from −120 to +63 %. A comparison with a highly resolved regional emission inventory suggests some spatial variations of the ratio within the city

A new method for estimating emission ratios in the urban atmosphere: examples of ratios to CO2, CO and volatile organic compounds in Paris

We propose a new approach to estimate urban emission ratios that takes advantage of the enhanced local urban signal in the atmosphere at low wind speed. We apply it to estimate monthly ratios between CO2, CO and some VOCs from several atmospheric concentration measurement datasets acquired in the centre of Paris between 2010 and 2014. We find that this approach is little sensitive to the regional background level definition and that, in the case of Paris, it samples all days (weekdays and weekends) and all hours of the day evenly. A large seasonal variability of the DeltaCO/DeltaCO2 ratio in Paris is shown, with a difference of around 60 % between the extreme values and a strong anti-correlation (r2 = 0.75) with atmospheric temperature. The comparison of the ratios obtained for two short measurement campaigns conducted in two different districts and two different periods (fall and winter) shows differences ranging from -120 to 63 %. A comparison with a highly resolved regional emission inventory suggests some spatial variations of the ratio within the city, although most of these differences seem to be rather driven by the seasonal variability

A new method for estimating emission ratios in the urban atmosphere: examples of ratios to CO2, CO and volatile organic compounds in Paris

We propose a new approach to estimate urban emission ratios that takes advantage of the enhanced local urban signal in the atmosphere at low wind speed. We apply it to estimate monthly ratios between CO2, CO and some VOCs from several atmospheric concentration measurement datasets acquired in the centre of Paris between 2010 and 2014. We find that this approach is little sensitive to the regional background level definition and that, in the case of Paris, it samples all days (weekdays and weekends) and all hours of the day evenly. A large seasonal variability of the DeltaCO/DeltaCO2 ratio in Paris is shown, with a difference of around 60 % between the extreme values and a strong anti-correlation (r2 = 0.75) with atmospheric temperature. The comparison of the ratios obtained for two short measurement campaigns conducted in two different districts and two different periods (fall and winter) shows differences ranging from -120 to 63 %. A comparison with a highly resolved regional emission inventory suggests some spatial variations of the ratio within the city, although most of these differences seem to be rather driven by the seasonal variability

Atmospheric measurements of ratios between CO2 and co-emitted species from traffic: a tunnel study in the Paris megacity

International audienceMeasurements of CO2, CO, NOx and selected Volatile Organic Compounds (VOCs) mole fractions were performed continuously during a 10-day period in the Guy Môquet tunnel in Thiais, a peri-urban area about 15 km south of the centre of Paris, between 28 September and 8 October 2012. This data set is used here to identify the characteristics of traffic-emitted CO2 by evaluating its ratios to co-emitted species for the first time in the Paris region. High coefficients of determination (r2 > 0.7) are observed between CO2 and certain compounds that are characteristic of the traffic source (CO, NOx, benzene, xylenes and acetylene). Weak correlations (r2 < 0.2) are found with species such as propane, n-butane and i-butane that are associated with fuel evaporation, an insignificant source for CO2. To better characterise the traffic signal we focus only on species that are well-correlated with CO2 and on rush-hour periods characterised by the highest traffic-related mole fractions. From those mole fractions we remove the nighttime-average weekday mole fraction obtained for each species that we infer to be the most appropriate background signal for our study. Then we calculate observed Δspecies / ΔCO2 ratios, which we compare with the ones provided by the 2010 bottom–up high-resolved regional emission inventory from Airparif (the association in charge of monitoring the air quality in Île-de-France), focusing on local emission data for the specific road of the tunnel. We find an excellent agreement (2%) between the local inventory emission CO / CO2 ratio and our observed ΔCO / ΔCO2 ratio. Former tunnel experiments carried out elsewhere in the world provided observed ΔCO / ΔCO2 ratios that differ from 49 to 592% to ours. This variability can be related to technological improvement of vehicles, differences in driving conditions, and fleet composition. We also find a satisfactory agreement with the Airparif inventory for n-propylbenzene, n-pentane and xylenes to CO2 ratios. For most of the other species, the ratios obtained from the local emission inventory overestimate the observed ratios to CO2 by 34 to more than 300%. However, the emission ratios of NOx, o-xylene and i-pentane are underestimated by 30 to 79%. One main cause of such high differences between the inventory and our observations is likely the obsolete feature of the VOCs speciation matrix of the inventory that has not been updated since 1998, although law regulations on some VOCs have occurred since that time. Our study bears important consequences, discussed in the conclusion, for the characterisation of the urban CO2 plume and for atmospheric inverse modelling of urban CO2 emissions

Characterization of traffic-emitted CO2 determined from road tunnel measurements in the region of Paris

With more than 10 million inhabitants (20% of the French population), Great Paris is the 3rd largest megacity in Europe. According to emission inventories, CO2 emissions of the Paris region represent about 15 % of the total French anthropogenic CO2 emissions whereas its surface extends over only 2% of the French territory. However, the assessment of such inventory is quite difficult and uncertainties are poorly constrained. During the incomplete combustion processes of fossil fuels, CO2 is co-emitted with other trace species in ratios that are characteristic of each emission sector and fuel type. Simultaneous measurements of CO2 and co-emitted species can thus allow the quantification of the relative contribution of each emission sector to the total amount of CO2 emitted. These ratios can be obtained from inventories. However, they are given for benchmark conditions that often may not represent well real world conditions. These ratios should thus also be assessed independently. Road traffic is one of the main sources of CO2 emitted by the Paris region : according to the regional French emission inventory (Airparif), 29% of CO2 emissions in the region of Paris are due to traffic which is also responsible for emissions of more than half of the CO (56%) and nearly 20% of the volatile organic compounds (VOCs) . As part of the PRIMEQUAL 'PREQUALIF' project, CO2 to co-emitted species emission factors were determined for the traffic sector. A 12-day measurement campaign was performed in a highway tunnel located in a peri-urban area about 15 km south of the Paris center. Several atmospheric compounds were monitored simultaneously with CO2, including CO, black carbon, NO-NO2 and VOCs. We will present here preliminary results from this campaign, based on the study of correlations between the concentrations of CO2 and co-emitted species, but also using information such as velocity, traffic rate, vehicle type and day of the week. Depending on these parameters, a classification of the different CO2 to co-species concentration ratios will be proposed. A first comparison will be provided with available inventories