Abstract
Independent estimates of fossil fuel CO2 (CO2ff) emissions are key to ensuring that emission reductions and regulations are effective and provide needed transparency and trust. Point source emissions are a key target because a small number of power plants represent a large portion of total global emissions. Currently, emission rates are known only from self-reported data. Atmospheric observations have the potential to meet the need for independent evaluation, but useful results from this method have been elusive, due to challenges in distinguishing CO2ff emissions from the large and varying CO2 background and in relating atmospheric observations to emission flux rates with high accuracy. Here we use time-integrated observations of the radiocarbon content of CO2 ((14)CO2) to quantify the recently added CO2ff mole fraction at surface sites surrounding a point source. We demonstrate that both fast-growing plant material (grass) and CO2 collected by absorption into sodium hydroxide solution provide excellent time-integrated records of atmospheric (14)CO2 These time-integrated samples allow us to evaluate emissions over a period of days to weeks with only a modest number of measurements. Applying the same time integration in an atmospheric transport model eliminates the need to resolve highly variable short-term turbulence. Together these techniques allow us to independently evaluate point source CO2ff emission rates from atmospheric observations with uncertainties of better than 10%. This uncertainty represents an improvement by a factor of 2 over current bottom-up inventory estimates and previous atmospheric observation estimates and allows reliable independent evaluation of emissions.