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Measuring Gas Transport and Sorption in Large Intact Geologic Specimens via the Piezometric Method

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Abstract

Uptake of noble gases into heterogeneous geologic core samples was measured using a piezometric methodology. In addition to measuring accessible porosity—as with gas pycnometry—by monitoring the rate of pressure decay, this method can also be used to estimate the gas effective diffusivity in the sample. In contrast to previous applications of this method, where milligram quantities of fractured grains are characterized, here approximately kilogram core samples were left intact when tested. In doing so, a more representative sample of the heterogeneous field geology is provided. Additionally, alteration of the pore structure and connectivity during sample preparation is avoided. To scale the piezometric method from milligrams to kilograms, the system was designed to operate at medium vacuum (1 to 100 Pa) to restrict transport in pores less than approximately 60 µm to large Knudsen numbers. To test the system performance, two samples of interest were selected: a rhyolitic welded tuff from Blue Canyon Dome at the Energetic Materials Research and Testing Center and a zeolitized non-welded rhyolitic tuff from the Nevada National Security Site. Three noble gases were utilized in this test series; Argon and xenon as they are of direct interest to nuclear monitoring efforts and helium as it is a weakly adsorbing reference standard. Additionally, mercury intrusion porosimetry measurements were made on subsamples of the core to compare the observed porosity by the two methods and to discuss gas transport rates in the context of the measured pore distribution.

Article Highlights

  • The piezometric method was extended to measure transport in intact geologic core samples between 800 and 1400 g.

  • Transport in the pores spaces was restricted to Knudsen flow using medium vacuum, enabling a closed-form solution.

  • Argon and xenon in a zeolitized tuff core exhibited significant adsorption and enhanced transport relative to helium.

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The raw data are available upon reasonable request.

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Curve fitting was performed using MATLAB and the scripts written are available upon reasonable request.

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Acknowledgements

The authors would like to thank Scott Broome for his support of this work, as well as Kris Kuhlman for his valuable feedback. This research was funded by the National Nuclear Security Administration, Defense Nuclear Nonproliferation Research and Development (NNSA DNN R&D). The authors acknowledge important interdisciplinary collaboration with scientists and engineers from LANL, LLNL, MSTS, PNNL, and SNL. This paper describes technical results and analysis. Any subjective views or opinions that might be expressed in the paper do not necessarily represent the views of the U.S. Department of Energy or the United States Government. Sandia National Laboratories is a multi-mission laboratory managed and operated by National Technology & Engineering Solutions of Sandia, LLC, a wholly owned subsidiary of Honeywell International Inc., for the U.S. Department of Energy's National Nuclear Security Administration under contract DE-NA0003525, SAND2021-7800 J.

Funding

All work was funded by the United States National Nuclear Security Administration, Defense Nuclear Nonproliferation Research and Development (NNSA DNN R&D).

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Correspondence to Matthew Paul.

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Paul, M., Feldman, J. Measuring Gas Transport and Sorption in Large Intact Geologic Specimens via the Piezometric Method. Transp Porous Med 139, 1–20 (2021). https://doi.org/10.1007/s11242-021-01627-w

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  • DOI: https://doi.org/10.1007/s11242-021-01627-w

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