ALBERT

Description: Radiocarbon analyses are commonly used in a broad range of fields, including earth science, archaeology, forgery detection, isotope forensics, and physiology. Many applications are sensitive to the radiocarbon (14C) content of atmospheric CO2, which has varied since 1890 as a result of nuclear weapons testing, fossil fuel emissions, and CO2...

Description: Two independent programs have collected and analyzed atmospheric CO2 samples from Point Barrow, Alaska, for radiocarbon content (Δ14C) over the period 2003–2007. In one program, flask collection, stable isotope analysis, and CO2 extraction are performed by the Scripps Institution of Oceanography's CO2 Program and CO2 is graphitized and measured by accelerator mass spectrometry (AMS) at Lawrence Livermore National Laboratory. In the other program, the University of California, Irvine, performs flask collection, sample preparation, and AMS. Over 22 common sample dates spanning 5 yr, differences in measured Δ14C are consistent with the reported uncertainties and there is no significant bias between the programs.

Description: This paper presents a step in the development of a top-down method to complement the bottom-up inventories of halocarbon emissions in California using high frequency observations, forward simulations and inverse methods. The Scripps Institution of Oceanography high-frequency atmospheric halocarbons measurement sites are located along the California coast and therefore the evaluation of transport in the chosen Weather Research Forecast (WRF) model at these sites is crucial for inverse modeling. The performance of the transport model has been investigated by comparing the wind direction and speed and temperature at four locations using aircraft weather reports as well at all METAR weather stations in our domain for hourly variations. Different planetary boundary layer (PBL) schemes, horizontal resolutions (achieved through nesting) and two meteorological datasets have been tested. Finally, simulated concentration of an inert tracer has been briefly investigated. All the PBL schemes present similar results that generally agree with observations, except in summer when the model sea breeze is too strong. At the coarse 12 km resolution, using ERA-interim (ECMWF Re-Analysis) as initial and boundary conditions leads to improvements compared to using the North American Model (NAM) dataset. Adding higher resolution nests also improves the match with the observations. However, no further improvement is observed from increasing the nest resolution from 4 km to 0.8 km. Once optimized, the model is able to reproduce tracer measurements during typical winter California large-scale events (Santa Ana). Furthermore, with the WRF/CHEM chemistry module and the European Database for Global Atmospheric Research (EDGAR) version 4.1 emissions for HFC-134a, we find that using a simple emission scaling factor is not sufficient to infer emissions, which highlights the need for more complex inversions.

Description: 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.

Description: CH4 and CO2 emissions from geologic sources, which are devoid of radiocarbon (14C), dilute the atmospheric 14C/C ratio. Observations of 14C/C can be used to estimate fossil fuel-derived CH4 and CO2. However, the atmospheric 14C/C ratio is perturbed by emissions of 14C from nuclear power plants (NPPs) and fuel reprocessing sites, which may affect such 14C/C-based estimation if they are not correctly quantified. We calculate NPP 14C emissions for CO2 and CH4 from 1972–2016 using standard emission factors (14C emitted per unit of power produced) and analyze trends in global and regional emissions. We use available observations of 14C emissions and power generation in Europe to assess emission factors for different reactor types, as well as potential differences related to the age or manufacturer of the NPPs. Globally, nuclear 14C emissions increase until 2005 and then decrease, mostly because of the closure of gas-cooled reactors in the United Kindom and the shutdown of light water reactors after the Fukushima nuclear accident in March 2011. Observed emission factors in Europe show strong variability, spanning values from 0.003 to 2.521 TBq/GWa for PWR and from 0.007 to 1.732 TBq/GWa for BWR reactors, suggesting more information and more sophisticated models are needed to improve estimates of 14C emissions.

Description: The global ocean is a significant sink for anthropogenic carbon (Cant), absorbing roughly a third of human CO2 emitted over the industrial period. Robust estimates of the magnitude and variability of the storage and distribution of Cant in the ocean are therefore important for understanding the human impact on climate. In this synthesis we review observational and model-based estimates of the storage and transport of Cant in the ocean. We pay particular attention to the uncertainties and potential biases inherent in different inference schemes. On a global scale, three data based estimates of the distribution and inventory of Cant are now available. While the inventories are found to agree within their uncertainty, there are considerable differences in the spatial distribution. We also present a review of the progress made in the application of inverse and data-assimilation techniques which combine ocean interior estimates of Cant with numerical ocean circulation models. Such methods are especially useful for estimating the air-sea flux and interior transport of Cant, quantities that are otherwise difficult to observe directly. However, the results are found to be highly dependent on modeled circulation, with the spread due to different ocean models at least as large as that from the different observational methods used to estimate Cant. Our review also highlights the importance of repeat measurements of hydrographic and biogeochemical parameters to estimate the storage of Cant on decadal timescales in the presence of the variability in circulation that is neglected by other approaches. Data-based Cant estimates provide important constraints on ocean forward models, which exhibit both broad similarities and regional errors relative to the observational fields. A compilation of inventories of Cant gives us a "best" estimate of the global ocean inventory of anthropogenic carbon in 2010 of 155 Pg C with an uncertainty of ±20%. This estimate includes a broad range of values suggesting that a combination of approaches is necessary in order to achieve a robust quantification of the ocean sink of anthropogenic CO2.

Description: The global ocean is a significant sink for anthropogenic carbon (Cant), absorbing roughly a third of human CO2 emitted over the industrial period. Robust estimates of the magnitude and variability of the storage and distribution of Cant in the ocean are therefore important for understanding the human impact on climate. In this synthesis we review observational and model-based estimates of the storage and transport of Cant in the ocean. We pay particular attention to the uncertainties and potential biases inherent in different inference schemes. On a global scale, three data-based estimates of the distribution and inventory of Cant are now available. While the inventories are found to agree within their uncertainty, there are considerable differences in the spatial distribution. We also present a review of the progress made in the application of inverse and data assimilation techniques which combine ocean interior estimates of Cant with numerical ocean circulation models. Such methods are especially useful for estimating the air–sea flux and interior transport of Cant, quantities that are otherwise difficult to observe directly. However, the results are found to be highly dependent on modeled circulation, with the spread due to different ocean models at least as large as that from the different observational methods used to estimate Cant. Our review also highlights the importance of repeat measurements of hydrographic and biogeochemical parameters to estimate the storage of Cant on decadal timescales in the presence of the variability in circulation that is neglected by other approaches. Data-based Cant estimates provide important constraints on forward ocean models, which exhibit both broad similarities and regional errors relative to the observational fields. A compilation of inventories of Cant gives us a "best" estimate of the global ocean inventory of anthropogenic carbon in 2010 of 155 ± 31 PgC (±20% uncertainty). This estimate includes a broad range of values, suggesting that a combination of approaches is necessary in order to achieve a robust quantification of the ocean sink of anthropogenic CO2.

Description: Since aged carbon in fossil fuel contains no 14C, 14C/C ratios (Δ14C) measured in atmospheric CO2 can be used to estimate CO2 added by combustion and, potentially, provide verification of fossil CO2 emissions calculated using economic inventories. Sources of 14C from nuclear power generation and spent fuel reprocessing can counteract dilution by fossil CO2. Therefore, these nuclear sources can bias observation-based estimates of fossil fuel-derived CO2 if they are not correctly accounted for or included as a source of uncertainty. 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 Europe, North America and East Asia, nuclear enrichment may offset 0–260 % of the fossil fuel dilution in Δ14C, corresponding to potential biases of 0 to −8 ppm in the CO2 attributed to fossil fuel emissions, larger than the bias from respiration in some areas. Growth of 14C emissions increased the potential nuclear bias over 1985–2005. The magnitude of this potential bias is largely independent of the choice of reference station in the context of Eulerian transport and inversion studies, but could potentially be reduced by an appropriate choice of reference station in the context of local-scale assessments.