CO, NOx and 13CO2 as tracers for fossil fuel CO2: results from a pilot study in Paris during winter 2010

Measurements of the mole fraction of the CO2 and its isotopes were performed in Paris during the MEGAPOLI winter campaign (January-February 2010). Radiocarbon ((CO2)-C-14) measurements were used to identify the relative contributions of 77% CO2 from fossil fuel consumption (CO(2)ff from liquid and gas combustion) and 23% from biospheric CO2 (CO2 from the use of biofuels and from human and plant respiration: CO(2)bio). These percentages correspond to average mole fractions of 26.4 ppm and 8.2 ppm for CO(2)ff and CO(2)bio, respectively. The (CO2)-C-13 analysis indicated that gas and liquid fuel contributed 70% and 30 %, respectively, of the CO2 emission from fossil fuel use. Continuous measurements of CO and NOx and the ratios CO/CO(2)ff and NOx/CO(2)ff derived from radiocarbon measurements during four days make it possible to estimate the fossil fuel CO2 contribution over the entire campaign. The ratios CO/CO(2)ff and NOx/CO(2)ff are functions of air mass origin and exhibited daily ranges of 7.9 to 14.5 ppb ppm(-1) and 1.1 to 4.3 ppb ppm(-1), respectively. These ratios are consistent with different emission inventories given the uncertainties of the different approaches. By using both tracers to derive the fossil fuel CO2, we observed similar diurnal cycles with two maxima during rush hour traffic.