Abstract
Abstract. Measurements 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.
Highlights
In 2011 more than half of the world population was living in urban areas, and this proportion is expected to reach 67 % in 2050 (United Nations, 2012)
This study pioneered the measurement of CO to CO2 and Volatile Organic Compounds (VOCs) to CO2 ratios for traffic emissions in the Paris area. 15 co-emitted species characteristic of traffic emissions were found to strongly correlate with CO2
Differences from 9 % to more than 500 % were found between previous tunnel studies, only reporting CO to CO2 ratios, and the ratio inferred from our observations
Summary
In 2011 more than half of the world population was living in urban areas, and this proportion is expected to reach 67 % in 2050 (United Nations, 2012). First encouraging estimates of the total CO2 anthropogenic emissions of the Paris megacity by atmospheric inverse modelling have been obtained by Bréon et al (2014), who compared their results to the Airparif inventory. The study of VOCs and of tracers of anthropogenic CO2 like CO or NOx is motivated by their impact on human health and by their production of photo-oxidants (such as ozone) in ambient air. As they are major pollutants emitted by traffic activities, they are regulated by European emission standards. The long lifetime of some of the studied species, like CO2, induces a large variety of emission origins and potentially elevated background levels in the measured mole fractions. Apart from CO2 and CO, it was not possible to use the few measurements made outside the tunnel (Sect. 2.2) because they do not include all species and are not performed on a regular basis, while, according to previous measurements, ambient VOCs mole fractions vary significantly during the day and from one day to another (Gros et al, 2011)
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