• Energy Research

Atmospheric methane (CH4) is a potent greenhouse gas, and its mole fraction has more than doubled since the preindustrial era. Fossil fuel extraction and use are among the largest anthropogenic sources of CH4 emissions, but the precise magnitude of these contributions is a subject of debate. Carbon-14 in CH4 (14CH4) can be used to distinguish between fossil (14C-free) CH4 emissions and contemporaneous biogenic sources; however, poorly constrained direct 14CH4 emissions from nuclear reactors have complicated this approach since the middle of the 20th century. Moreover, the partitioning of total fossil CH4 emissions (presently 172 to 195 teragrams CH4 per year) between anthropogenic and natural geological sources (such as seeps and mud volcanoes) is under debate; emission inventories suggest that the latter account for about 40 to 60 teragrams CH4 per year. Geological emissions were less than 15.4 teragrams CH4 per year at the end of the Pleistocene, about 11,600 years ago, but that period is an imperfect analogue for present-day emissions owing to the large terrestrial ice sheet cover, lower sea level and extensive permafrost. Here we use preindustrial-era ice core 14CH4 measurements to show that natural geological CH4 emissions to the atmosphere were about 1.6 teragrams CH4 per year, with a maximum of 5.4 teragrams CH4 per year (95 per cent confidence limit)—an order of magnitude lower than the currently used estimates. This result indicates that anthropogenic fossil CH4 emissions are underestimated by about 38 to 58 teragrams CH4 per year, or about 25 to 40 per cent of recent estimates. Our record highlights the human impact on the atmosphere and climate, provides a firm target for inventories of the global CH4 budget, and will help to inform strategies for targeted emission reductions.

Abstract A simple climate model is used to calculate the benefit, over time, of geosequestration of CO2 that would otherwise be released to the atmosphere. The analysis is performed relative to two reference cases. The first case is defined by a CO2 concentration profile leading to stabilisation at 500 ppm. The second case is defined by ‘business-as-usual’ (IS92a) CO2 emissions until 2100. The benefits are considered in terms of incremental change (per unit of displaced emission) in temperature and its rate of change, concentrating on the period to 2200. An automatic differentiation procedure has proved a convenient way of performing the calculations. The ‘temperature benefit’ of avoided carbon emission is found to be of order 1 mK/GtC on the time-scale of decades to centuries. This result is model-specific and would scale in proportion to the climate sensitivity of the model. Because of non-linearities in carbon-climate processes, the results have a small dependence (of order 10–20%) on the future emission scenario with a rather smaller contribution to uncertainty arising from model calibration uncertainties that reflect uncertainties in the 20th century carbon budget. Analysis over the longer term, to 2500, considers the effect of leakage of geologically stored CO2 to the atmosphere, and shows that even at 0.1% per annum leakage, about half the climate benefit remains after 500 years.

A recent study by Keppler et al. (2006; Nature 439, 187–191) demonstrated CH4 emission from living and dead plant tissues under aerobic conditions. This work included some calculations to extrapolate the findings from the laboratory to the global scale and led various commentators to question the value of planting trees as a greenhouse mitigation option. The experimental work of Keppler et al. (2006) appears to be largely sound, although some concerns remain about the quantification of emission rates. However, whilst accepting their basic findings, we are critical of the method used for extrapolating results to a global scale. Using the same basic information, we present alternative calculations to estimate global aerobic plant CH4 emissions as 10–60 Mt CH4 year–1. This estimate is much smaller than the 62–236 Mt CH4 year–1 reported in the original study and can be more readily reconciled within the uncertainties in the established sources and sinks in the global CH4 budget. We also assessed their findings in terms of their possible relevance for planting trees as a greenhouse mitigation option. We conclude that consideration of aerobic CH4 emissions from plants would reduce the benefit of planting trees by between 0 and 4.4%. Hence, any offset from CH4 emission is small in comparison to the significant benefit from carbon sequestration. However, much critical information is still lacking about aerobic CH4 emission from plants. For example, we do not yet know the underlying mechanism for aerobic CH4 emission, how CH4 emissions change with light, temperature and the physiological state of leaves, whether emissions change over time under constant conditions, whether they are related to photosynthesis and how they relate to the chemical composition of biomass. Therefore, the present calculations must be seen as a preliminary attempt to assess the global significance from a basis of limited information and are likely to be revised as further information becomes available.

Abstract. Methane is a strong greenhouse gas and large uncertainties exist concerning the future evolution of its atmospheric abundance. Analyzing methane atmospheric mixing and stable isotope ratios in air trapped in polar ice sheets helps in reconstructing the evolution of its sources and sinks in the past. This is important to improve predictions of atmospheric CH4 mixing ratios in the future under the influence of a changing climate. The aim of this study is to assess whether past atmospheric δ13C(CH4) variations can be reliably reconstructed from firn air measurements. Isotope reconstructions obtained with a state of the art firn model from different individual sites show unexpectedly large discrepancies and are mutually inconsistent. We show that small changes in the diffusivity profiles at individual sites lead to strong differences in the firn fractionation, which can explain a large part of these discrepancies. Using slightly modified diffusivities for some sites, and neglecting samples for which the firn fractionation signals are strongest, a combined multi-site inversion can be performed, which returns an isotope reconstruction that is consistent with firn data. However, the isotope trends are lower than what has been concluded from Southern Hemisphere (SH) archived air samples and high-accumulation ice core data. We conclude that with the current datasets and understanding of firn air transport, a high precision reconstruction of δ13C of CH4 from firn air samples is not possible, because reconstructed atmospheric trends over the last 50 yr of 0.3–1.5 ‰ are of the same magnitude as inherent uncertainties in the method, which are the firn fractionation correction (up to ~2 ‰ at individual sites), the Kr isobaric interference (up to ~0.8 ‰, system dependent), inter-laboratory calibration offsets (~0.2 ‰) and uncertainties in past CH4 levels (~0.5 ‰).

AbstractMonitoring is essential for the approval and control of geological storage of carbon dioxide and to judge the effectiveness of the technology in mitigating CO2 emissions and climate change. We present a strategy for monitoring the atmosphere in the vicinity of a geological storage project that is designed to detect and quantify potential emissions. The strategy includes measurements of CO2, CO2 fluxes and tracers, combined with model simulations of atmospheric dispersion and ecosystem CO2 fluxes. We applied an atmospheric monitoring program to the CO2CRC Otway Project where large amounts of CO2 have been stored in a deep depleted natural gas reservoir. The sensitivity of the monitoring is tested by detecting emissions from surface activities at the Otway facility, including a scheduled release of injected gas.

Carbon capture and storage (CCS) is vital to reduce CO 2 emissions to the atmosphere, potentially providing 20% of the needed reductions in global emissions. Research and demonstration projects are important to increase scientific understanding of CCS, and making processes and results widely available helps to reduce public concerns, which may otherwise block this technology. The Otway Project has provided verification of the underlying science of CO 2 storage in a depleted gas field, and shows that the support of all stakeholders can be earned and retained. Quantitative verification of long-term storage has been demonstrated. A direct measurement of storage efficiency has been made, confirming that CO 2 storage in depleted gas fields can be safe and effective, and that these structures could store globally significant amounts of CO 2 .

AbstractAtmospheric CO2 perturbations from simulated leaks have been used to determine the minimum statistically significant emissions that can be detected above background concentrations using a single atmospheric station. The study uses high precision CO2 measurements from the Arcturus atmospheric monitoring station in the Bowen Basin, Australia. A statistical model of the observed CO2 signal was constructed, combining both a regression and a time series model. A non-parametric goodness of fit approach using the Kolmogorov-Smirnoff (KS) test was then used to test whether simulated perturbations can be detected against the modelled expected value of the background for certain hours of the day and for particular seasons.The KS test calculates the probability that the modelled leak perturbation could be caused by natural variation in the background. Using pre-whitened data and selecting optimum test conditions, minimum detectable leaks located 1km from the measurement station were estimated at 22 tpd for an area source of size 100 m x 100 m and 14 tpd for a point source at a KS cutoff defined by using the formal p-value of 0.05. These are very large leaks located only 1km from the station and have a high false alarm rate of 56%. An alternative p-value could be chosen to reduce the false alarm rate but then the minimum detectable leaks are larger. A long term, single measurement station monitoring program that is unconstrained by prior information on the possible direction or magnitude of a leak, and based solely on detection of perturbations of CO2 due to leakage above a (naturally noisy) background signal, is likely to take one or more years to detect leaks of the order of 10 kt p.a. The sensitivity of detection of a leak above a background signal could be greatly improved through the installation of additional atmospheric monitoring stations or through greater prior knowledge about the location and size of a suspected leak.