Constraining the effectiveness of inherent tracers of captured CO2 for tracing CO2 leakage: Demonstration in a controlled release site.

Geological storage of carbon dioxide (CO2) is an integral component of cost-effective greenhouse gas emissions reduction scenarios. However, a robust monitoring regime is necessary for public and regulatory assurance that any leakage from a storage site can be detected. Here, we present the results from a controlled CO2 release experiment undertaken at the K-COSEM test site (South Korea) with the aim of demonstrating the effectiveness of the inherent tracer fingerprints (noble gases, δ13C) in monitoring CO2 leakage. Following injection of 396 kg CO2(g) into a shallow aquifer, gas release was monitored for 2 months in gas/water phases in and above the injection zone. The injection event resulted in negative concentration changes of the dissolved gases, attributed to the stripping action of the depleted CO2. Measured fingerprints from inherent noble gases successfully identified solubility-trapping of the injected CO2 within the shallow aquifer. The δ13C within the shallow aquifer could not resolve the level of gas trapping, due to the interaction with heterogeneous carbonate sources in the shallow aquifer. The time-series monitoring of δ13CDIC and dissolved gases detected the stripping action of injected CO2(g), which can provide an early warning of CO2 arrival. This study highlights that inherent noble gases can effectively trace the upwardly migrating and fate of CO2 within a shallow aquifer.

Storage of Carbon Dioxide in Saline Aquifers: Physicochemical Processes, Key Constraints, and Scale-Up Potential.

CO2 storage in saline aquifers offers a realistic means of achieving globally significant reductions in greenhouse gas emissions at the scale of billions of tonnes per year. We review insights into the processes involved using well-documented industrial-scale projects, supported by a range of laboratory analyses, field studies, and flow simulations. The main topics we address are (a) the significant physicochemical processes, (b) the factors limiting CO2 storage capacity, and (c) the requirements for global scale-up.Although CO2 capture and storage (CCS) technology can be considered mature and proven, it requires significant and rapid scale-up to meet the objectives of the Paris Climate Agreement. The projected growth in the number of CO2 injection wells required is significantly lower than the historic petroleum industry drill rates, indicating that decarbonization via CCS is a highly credible and affordable ambition for modern human society. Several technology developments are needed to reduce deployment costs and to stimulate widespread adoption of this technology, and these should focus on demonstration of long-term retention and safety of CO2 storage and development of smart ways of handling injection wells and pressure, cost-effective monitoring solutions, and deployment of CCS hubs with associated infrastructure.

Author Correction: 420,000 year assessment of fault leakage rates shows geological carbon storage is secure.

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

420,000 year assessment of fault leakage rates shows geological carbon storage is secure.

Carbon capture and storage (CCS) technology is routinely cited as a cost effective tool for climate change mitigation. CCS can directly reduce industrial CO2 emissions and is essential for the retention of CO2 extracted from the atmosphere. To be effective as a climate change mitigation tool, CO2 must be securely retained for 10,000 years (10 ka) with a leakage rate of below 0.01% per year of the total amount of CO2 injected. Migration of CO2 back to the atmosphere via leakage through geological faults is a potential high impact risk to CO2 storage integrity. Here, we calculate for the first time natural leakage rates from a 420 ka paleo-record of CO2 leakage above a naturally occurring, faulted, CO2 reservoir in Arizona, USA. Surface travertine (CaCO3) deposits provide evidence of vertical CO2 leakage linked to known faults. U-Th dating of travertine deposits shows leakage varies along a single fault and that individual seeps have lifespans of up to 200 ka. Whilst the total volumes of CO2 required to form the travertine deposits are high, time-averaged leakage equates to a linear rate of less than 0.01%/yr. Hence, even this natural geological storage site, which would be deemed to be of too high risk to be selected for engineered geologic storage, is adequate to store CO2 for climate mitigation purposes.

Estimating geological CO2 storage security to deliver on climate mitigation.

Carbon capture and storage (CCS) can help nations meet their Paris CO2 reduction commitments cost-effectively. However, lack of confidence in geologic CO2 storage security remains a barrier to CCS implementation. Here we present a numerical program that calculates CO2 storage security and leakage to the atmosphere over 10,000 years. This combines quantitative estimates of geological subsurface CO2 retention, and of surface CO2 leakage. We calculate that realistically well-regulated storage in regions with moderate well densities has a 50% probability that leakage remains below 0.0008% per year, with over 98% of the injected CO2 retained in the subsurface over 10,000 years. An unrealistic scenario, where CO2 storage is inadequately regulated, estimates that more than 78% will be retained over 10,000 years. Our modelling results suggest that geological storage of CO2 can be a secure climate change mitigation option, but we note that long-term behaviour of CO2 in the subsurface remains a key uncertainty.

Inherent Tracers for Carbon Capture and Storage in Sedimentary Formations: Composition and Applications.

Inherent tracers-the "natural" isotopic and trace gas composition of captured CO2 streams-are potentially powerful tracers for use in CCS technology. This review outlines for the first time the expected carbon isotope and noble gas compositions of captured CO2 streams from a range of feedstocks, CO2-generating processes, and carbon capture techniques. The C-isotope composition of captured CO2 will be most strongly controlled by the feedstock, but significant isotope fractionation is possible during capture; noble gas concentrations will be controlled by the capture technique employed. Comparison with likely baseline data suggests that CO2 generated from fossil fuel feedstocks will often have δ(13)C distinguishable from storage reservoir CO2. Noble gases in amine-captured CO2 streams are likely to be low concentration, with isotopic ratios dependent on the feedstock, but CO2 captured from oxyfuel plants may be strongly enriched in Kr and Xe which are potentially valuable subsurface tracers. CO2 streams derived from fossil fuels will have noble gas isotope ratios reflecting a radiogenic component that will be difficult to distinguish in the storage reservoir, but inheritance of radiogenic components will provide an easily recognizable signature in the case of any unplanned migration into shallow aquifers or to the surface.

Solubility trapping in formation water as dominant CO(2) sink in natural gas fields.

Injecting CO(2) into deep geological strata is proposed as a safe and economically favourable means of storing CO(2) captured from industrial point sources. It is difficult, however, to assess the long-term consequences of CO(2) flooding in the subsurface from decadal observations of existing disposal sites. Both the site design and long-term safety modelling critically depend on how and where CO(2) will be stored in the site over its lifetime. Within a geological storage site, the injected CO(2) can dissolve in solution or precipitate as carbonate minerals. Here we identify and quantify the principal mechanism of CO(2) fluid phase removal in nine natural gas fields in North America, China and Europe, using noble gas and carbon isotope tracers. The natural gas fields investigated in our study are dominated by a CO(2) phase and provide a natural analogue for assessing the geological storage of anthropogenic CO(2) over millennial timescales. We find that in seven gas fields with siliciclastic or carbonate-dominated reservoir lithologies, dissolution in formation water at a pH of 5-5.8 is the sole major sink for CO(2). In two fields with siliciclastic reservoir lithologies, some CO(2) loss through precipitation as carbonate minerals cannot be ruled out, but can account for a maximum of 18 per cent of the loss of emplaced CO(2). In view of our findings that geological mineral fixation is a minor CO(2) trapping mechanism in natural gas fields, we suggest that long-term anthropogenic CO(2) storage models in similar geological systems should focus on the potential mobility of CO(2) dissolved in water.