1Institute of Biogeochemistry and Pollutant Dynamics, ETH Zurich, Universitätstrasse 16, 8092 Zurich, Switzerland
*now at: Scripps Institution of Oceanography, University of California-San Diego, 9500 Gilman Dr., La Jolla, CA 92093-0244, USA
Received: 26 Apr 2011 – Published in Atmos. Chem. Phys. Discuss.: 12 May 2011
Abstract. The 14C-free fossil carbon added to atmospheric CO2 by combustion dilutes the atmospheric 14C/C ratio (Δ14C), potentially providing a means to verify fossil CO2 emissions calculated using economic inventories. However, sources of 14C from nuclear power generation and spent fuel reprocessing can counteract this dilution and may bias 14C/C-based estimates of fossil fuel-derived CO2 if these nuclear influences are not correctly accounted for. Previous studies have examined nuclear influences on local scales, but the potential for continental-scale influences on Δ14C has not yet been explored. We estimate annual 14C emissions from each nuclear site in the world and conduct an Eulerian transport modeling study to investigate the continental-scale, steady-state gradients of Δ14C caused by nuclear activities and fossil fuel combustion. Over large regions of Europe, North America and East Asia, nuclear enrichment may offset at least 20% of the fossil fuel dilution in Δ14C, corresponding to potential biases of more than −0.25 ppm in the CO2 attributed to fossil fuel emissions, larger than the bias from plant and soil respiration in some areas. Model grid cells including high 14C-release reactors or fuel reprocessing sites showed much larger nuclear enrichment, despite the coarse model resolution of 1.8°×1.8°. The recent growth of nuclear 14C emissions increased the potential nuclear bias over 1985–2005, suggesting that changing nuclear activities may complicate the use of Δ14C observations to identify trends in fossil fuel emissions. The magnitude of the potential nuclear bias is largely independent of the choice of reference station in the context of continental-scale Eulerian transport and inversion studies, but could potentially be reduced by an appropriate choice of reference station in the context of local-scale assessments.
Revised: 15 Sep 2011 – Accepted: 25 Nov 2011 – Published: 09 Dec 2011
Citation: Graven, H. D. and Gruber, N.: Continental-scale enrichment of atmospheric 14CO2 from the nuclear power industry: potential impact on the estimation of fossil fuel-derived CO2, Atmos. Chem. Phys., 11, 12339-12349, doi:10.5194/acp-11-12339-2011, 2011.