Measurement of fossil fuel carbon dioxide and other anthropogenic trace gases from MEGAPOLI intensive campaign in Paris during winter 2010

The Paris agglomeration is the third biggest megacity in Europe (12 million inhabitants) and according to national emission inventories, is responsible for 15 % of the French anthropogenic CO2 emissions mainly originating from road transport, residential and industrial energy consumption. The objective of our feasibility study was to design an efficient monitoring strategy in order to quantify future trends in anthropogenic CO2 emission in Paris area. During the winter campaign of the European project MEGAPOLI and French project CO2-MEGAPARIS, we performed measurements of CO2 and related trace gases from January to February 2010. The RAMCES (Atmospheric Network for Greenhouse Gases Monitoring) team at LSCE monitored CO2 and CO mixing ratio with high temporal resolution using instruments based on Cavity Ring Down Spectroscopy (CRDS) in the thirteenth arrondissement of Paris (south). We also sampled air in more than fifty flasks covering three full days at the same place. Flasks were analysed in the RAMCES central laboratory with a Gas Chromatograph system for CO2, CO, CH4, N2O, SF6 and H2 mixing ratios and also by Mass Spectroscopy for CO2 isotopic ratios (δ13C and δ18O). In order to quantify the fossil fuel CO2 (CO2ff) most flasks were analysed at INSTAAR for Δ14C in CO2. In addition, 13CO2 isotopic ratio and total CO2 concentration were measured at high temporal resolution (< 1 min) over three days at Paris with Tunable Diode Laser Spectroscope developed at LPMAA. In parallel with the Paris measurements, in-situ CO2, CO and other trace gases were monitored at Gif-sur-Yvette, a semi urban station 20km south west of Paris. Similar synoptic variations of CO2 and CO mixing ratios were found in Paris and Gif with maximum mixing ratio up to 495 ppm CO2 and 1000 ppb CO downtown Paris. The mean diurnal variation during this winter period shows peak to peak amplitude of 15 ppm CO2 and 150 ppb CO at Paris and 10 ppm CO2 and 40 CO ppb at Gif station. We focused on CO and NOx as tracer of fossil fuel emission to estimate CO2ff. We calibrated these tracers against CO2ff estimates based on Δ14C. Moreover, δ13C measurements were used to quantify the contribution of the different combustion sources for CO2 emission. Finally, we compared our results to the emission inventories from EDGAR 4.2 (global inventories), IER (European inventory) and the national ones from CITEPA and AirParif.