Multi‐Layered Systems for Permanent Geologic Storage of CO2 at the Gigatonne Scale.

The effectiveness of Carbon Capture and Storage (CCS) as an imperative decarbonization technology relies on the sealing capacity of a fine‐grained caprock to permanently store CO2 deep underground. Uncertainties in assessing the caprock sealing capacity increase with the spatial and temporal scales and may delay CCS deployment at the gigatonne scale. We have developed a computationally efficient transport model to capture the dynamics of basin‐wide upward CO2 migration in a multi‐layered setting over geological time scales. We find that massive capillary breakthrough and viscous flow of CO2, even through pervasively fractured caprocks, are unlikely to occur and compromise the storage security. Potential leakage from the injection reservoir is hampered by repetitive layering of overlying caprocks. This finding agrees with geologic intuition and should be understandable by the public, contributing to the development of climate policies around this technology with increased confidence that CO2 will be indefinitely contained in the subsurface. Plain Language Summary: Massive and timely deployment of Carbon Capture and Storage (CCS) at the gigatonne scale is a critical component of the majority of pathways toward reaching the Paris Agreement emissions abatement targets to mitigate climate change. Although CCS has been successfully deployed at multiple sites around the world, concerns about long‐term containment, especially for gigatonne‐scale storage, are causing uncertainty about the ability of geological layers to permanently store CO2 underground. This uncertainty is delaying the widespread deployment of CCS. This paper focuses on assessing the possibility of basin‐wide CO2 leakage through a typical multi‐layered geological setting with a sequence of aquifers and fine‐grained caprocks (e.g., shales). Numerical transport models, constrained by hydraulic properties of intact and pervasively fractured caprocks (as the best‐ and worst‐case scenarios, respectively), enable us to draw unambiguous limits on the CO2 leakage rates over previously unexplored temporal and spatial scales. We show that CO2 leakage to shallow sediments in both extreme scenarios is quite unlikely and the injected CO2 will be contained in the subsurface over millions of years. These findings should offer confidence to industrial developers, policy‐makers, investors, and most importantly, the public that CCS provides a secure and environmentally sound carbon removal option. Key Points: We develop a numerical transport model to understand the long‐term fate of CO2 in gigatonne‐scale geologic carbon storageCO2 leakage is dominated by molecular diffusion at inherently slow rates, hardly approaching a meter per several thousands of yearsThe long‐term potential for CO2 leakage from a multi‐layered system is low, making geologic storage a secure decarbonization technology [ABSTRACT FROM AUTHOR]