Publication Type:Journal Article
Source:Atmos. Chem. Phys. Discuss., Volume 8, Issue 1, p.1191 - 1237 (2008)
Keywords:212Pb, 222Rn, CH4, CO, CO2, N2O
We estimated CO2, CH4, CO and N2O emission fluxes over the British Isles and Western Europe using atmospheric radon observations and concentrations recorded at the Mace Head Atmospheric Research Station between 1996 and 2005. We classified hourly concentration data into either long-range European or regional sources from Ireland and UK, by using local wind speed data in conjunction with 222Rn and 212Pb threshold criteria. This leads to the selection of about 7% of the total data for both sectors. We then used continuous 222Rn measurements and assumptions on the surface emissions of 222Rn to deduce the unknown fluxes of CO2, CH4, CO and N2O. Our results have been compared to the UNFCCC, EMEP and EDGAR statistical inventories and to inversion results for CH4. For Western Europe, we found yearly mean fluxes of 4.1±1.5 106 kg CO2 km−2 yr−1 , 11.9±2.0 103 kg CH4 km−2 yr−1, 12.8±4.2 103 kg CO km−2 yr−1 and 520.2±129.2 kg N2O km−2 yr−1, respectively, for CO2, CH4, CO and N2O over the period 1996–2005. The method based upon 222Rn to infer emissions has many sources of systematic errors, in particular its poorly known and variable footprint, uncertainties in 222Rn soil fluxes and in atmospheric mixing of air masses with background air. However, these biases are likely to remain constant in the long-term, which makes the method quite efficient to detect trends in fluxes. Over the last ten years period, the decrease of the anthropogenic CH4, CO and N2O emissions in Europe estimated by inventories (respectively −30%, −35% and −23%) is confirmed by the Mace Head data within 2%. Therefore, the 222Rn method provides an independent way of verification of changes in national emissions derived from inventories. Using European-wide estimates of the CO/CO2 emission ratio, we also found that it is possible to separate the fossil fuel CO2 emissions contribution from the one of total CO2 fluxes. The fossil fuel CO2 emissions and their trends derived in that manner agree very well with inventories.