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       Samuel Clegg1, Kristy Nowak-Lovato1, Robert Currier1, Julianna Fessenden2, and Ronald Martinez1

       1 Chemistry Division, Los Alamos National Laboratory, Los Alamos, New Mexico, USA

       2 Earth and Environmental Sciences, Los Alamos National Laboratory, Los Alamos, New Mexico, USA

      ABSTRACT

      Geologic sequestration of carbon dioxide (CO2) is one of the immediate solutions to the permanent storage of greenhouse gases. Geologic storage of CO2 requires monitoring, verification, and accounting (MVA) to assess the location of the sequestered material as well as track the plume movement. Surface MVA techniques have been developed to detect CO2 emissions should some of the injected CO2 migrate to the surface. Most of these techniques involve monitoring absolute changes in bulk CO2 concentration, which is complicated by the diurnal cycle. Changes in the carbon stable isotope ratio in CO2 has been shown to be a more sensitive diagnostic to distinguish anthropogenic and natural CO2. Both cavity ringdown spectroscopy (CRS) and frequency modulated spectroscopy (FMS) are sensitive spectroscopic techniques that have been developed to measure these stable isotope ratios. While CRS is limited to analysis of point source emission samples, field experiments of FMS instruments have been demonstrated in both captured samples and in remote configurations. In this chapter, the application of FMS to the MVA of carbon dioxide is reviewed.

      Methods to limit greenhouse gas emissions in an effort to arrest global warming are necessary and geological sequestration is immediately available. Geological sequestration involves pumping CO2 into deep geological reservoirs such as depleted oil and natural gas reservoirs (Rodosta et al., 2014, Rodosta & Ackiewicz, 2014). Geological sequestration has the benefit of accommodating any source of CO2 including any industrial process where the CO2 is collected. The expectation is that the sequestered CO2 will become mineralized over time resulting in the permanent CO2 storage.

      Monitoring, verification, and accounting (MVA) is a fundamental requirement for geological sequestration sites to ensure the permanent storage as well as ensure public health and environmental safety (Rodosta & Ackiewicz, 2014). In order to pay for sequestration, there is an interest in the development of a carbon economy where those that sequester CO2 would receive a financial gain. If a carbon economy is established, it is critical to verify that the CO2 is permanently stored. Furthermore, MVA methods are required to ensure that the CO2 or other hazardous gases within the reservoir are not mobilized beyond the reservoir into used water reservoirs or to the surface at dangerous concentrations.

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