Measuring the Stable Isotope Composition of Water in Brine from Halite Fluid Inclusions and Borehole Brine Seeps Using Cavity Ring-Down Spectroscopy

Eldridge, Daniel L.; Mills, Melissa M.; Miller, Hayden D.; Otto, Shawn; Davis, Jon E.; Guiltinan, Eric J.; Rahn, Thom; Kuhlman, Kristopher L.; Stauffer, Philip H.

doi:10.1021/acsearthspacechem.4c00107

Measuring the Stable Isotope Composition of Water in Brine from Halite Fluid Inclusions and Borehole Brine Seeps Using Cavity Ring-Down Spectroscopy

Journal Article · Tue Dec 17 04:00:00 EST 2024 · ACS Earth and Space Chemistry

DOI:https://doi.org/10.1021/acsearthspacechem.4c00107· OSTI ID:2496663

^[1]; Mills, Melissa M. ^[2]; Miller, Hayden D. ^[1]; Otto, Shawn ^[3]; Davis, Jon E. ^[3]; Guiltinan, Eric J. ^[1]; Rahn, Thom ^[1]; ^[2]; Stauffer, Philip H. ^[1]

Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)
Carlsbad Field Office (CBFO), NM (United States)

Naturally occurring bedded salt deposits are considered robust for the permanent disposal of heat-generating nuclear waste due to their unique physical and geological properties. The Brine Availability Test in Salt (BATS) is a US-DOE Office of Nuclear Energy funded project that uses heated borehole experiments underground (~655 meters depth) at the Waste Isolation Pilot Plant (WIPP) in the bedded salt deposits of the Salado Formation to investigate the capacity for safe disposal of high-level, heat generating nuclear waste in salt. Uncertainties associated with brine mobility near heat-generating waste motivates the need to characterize the processes and sources of brine in salt deposits. Intragranular halite fluid inclusions are a potential source of brine that can migrate under temperature gradients toward heat sources. We developed a methodology to measure the stable isotopic compositions of water (δD_VSMOW, δ¹⁸O_VSMOW) in brine from halite fluid inclusions using Cavity Ring-Down Spectroscopy that accounts for memory effects using a unique reference-sample-reference bracketing approach and that minimizes sample size requirements. We applied this approach to halite samples obtained from WIPP and compare these data to seeped brines collected from horizontal boreholes at WIPP after drilling at ambient conditions. Here, the stable isotope compositions that we obtain for halite fluid inclusions (δ¹⁸O_VSMOW = +3.24 ± 0.53‰, δD_VSMOW = -25.3 ± 5.1‰, ±1σ, n = 5) generally agree with previous measurements and likely reflect a combination of syn-depositional and/or postdepositional processes. The seep brines are isotopically distinct (δ18OVSMOW = +3.46 ± 0.84‰, δD_VSMOW = +7.3 ± 3.5‰, ±1σ, n = 35) and instead resemble evaporated seawater. We discuss our results in the context of prior WIPP-proximal waters and lay the groundwork for using stable isotopes of water in brine as a tool to assess the heat-induced mobilization of halite fluid inclusions in ongoing heating experiments that comprise the Brine Availability Test in Salt.

View Accepted Manuscript (DOE)

Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE Office of Nuclear Energy (NE), Office of Spent Fuel and Waste Disposition. Office of Spent Fuel and Waste Science and Technology; USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: NA0003525; 89233218CNA000001

OSTI ID:: 2496663

Alternate ID(s):: OSTI ID: 2482103

Report Number(s):: LA-UR--24-23008

Journal Information:: ACS Earth and Space Chemistry, Journal Name: ACS Earth and Space Chemistry Journal Issue: 1 Vol. 9; ISSN 2472-3452

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

References (41)

Stable isotopes in atmospheric water vapor and applications to the hydrologic cycle: ISOTOPES IN THE ATMOSPHERIC WATER CYCLE Galewsky, Joseph; Steen-Larsen, Hans Christian; Field, Robert D. Reviews of Geophysics, Vol. 54, Issue 4 https://doi.org/10.1002/2015RG000512	journal	November 2016
A Newly Designed Analytical Line to Examine Fluid Inclusion Isotopic Compositions in a Variety of Carbonate Samples Dassié, Emilie P.; Genty, Dominique; Noret, Aurélie Geochemistry, Geophysics, Geosystems, Vol. 19, Issue 4 https://doi.org/10.1002/2017GC007289	journal	April 2018
Demonstration of high-precision continuous measurements of water vapor isotopologues in laboratory and remote field deployments using wavelength-scanned cavity ring-down spectroscopy (WS-CRDS) technology Gupta, Priya; Noone, David; Galewsky, Joseph Rapid Communications in Mass Spectrometry, Vol. 23, Issue 16 https://doi.org/10.1002/rcm.4100	journal	August 2009
Hydrogen and oxygen isotopes of water from inclusions in minerals: design of a new crushing system and on‐line continuous‐flow isotope ratio mass spectrometric analysis Dublyansky, Yuri V.; Spötl, Christoph Rapid Communications in Mass Spectrometry, Vol. 23, Issue 17 https://doi.org/10.1002/rcm.4155	journal	July 2009
Improved water δ²H and δ¹⁸O calibration and calculation of measurement uncertainty using a simple software tool Gröning, Manfred Rapid Communications in Mass Spectrometry, Vol. 25, Issue 19 https://doi.org/10.1002/rcm.5074	journal	September 2011
Doubly Labelled Water analysis: Preparation, memory correction, calibration and quality assurance for δ²H and δ¹⁸O measurements over four orders of magnitudes Guidotti, S.; Jansen, H. G.; Aerts‐Bijma, A. T. Rapid Communications in Mass Spectrometry, Vol. 27, Issue 9 https://doi.org/10.1002/rcm.6540	journal	April 2013
Lake Louise Water (USGS47): A new isotopic reference water for stable hydrogen and oxygen isotope measurements Qi, Haiping; Lorenz, Jennifer M.; Coplen, Tyler B. Rapid Communications in Mass Spectrometry, Vol. 28, Issue 4 https://doi.org/10.1002/rcm.6789	journal	December 2013
LIMS for Lasers 2015 for achieving long-term accuracy and precision ofδ²H,δ¹⁷O, andδ¹⁸O of waters using laser absorption spectrometry Coplen, Tyler B.; Wassenaar, Leonard I. Rapid Communications in Mass Spectrometry, Vol. 29, Issue 22 https://doi.org/10.1002/rcm.7372	journal	October 2015
A comparison of isotope ratio mass spectrometry and cavity ring‐down spectroscopy techniques for isotope analysis of fluid inclusion water de Graaf, Stefan; Vonhof, Hubert B.; Weissbach, Therese Rapid Communications in Mass Spectrometry, Vol. 34, Issue 16 https://doi.org/10.1002/rcm.8837	journal	July 2020
Isotope ratio infrared spectroscopy analysis of water samples without memory effects de Graaf, Stefan; Vonhof, Hubert B.; Levy, Elan J. Rapid Communications in Mass Spectrometry, Vol. 35, Issue 8 https://doi.org/10.1002/rcm.9055	journal	February 2021
Temperature response and brine availability to heated boreholes in bedded salt Guiltinan, Eric J.; Kuhlman, Kristopher L.; Rutqvist, Jonny Vadose Zone Journal, Vol. 19, Issue 1 https://doi.org/10.1002/vzj2.20019	journal	January 2020
Stable isotope fractionation factors of water in hydrated saline mineral-brine systems Horita, Juske Earth and Planetary Science Letters, Vol. 95, Issue 1-2 https://doi.org/10.1016/0012-821X(89)90175-1	journal	October 1989
Variation of O18 content of waters from natural sources Epstein, S.; Mayeda, T. Geochimica et Cosmochimica Acta, Vol. 4, Issue 5 https://doi.org/10.1016/0016-7037(53)90051-9	journal	November 1953
Deuterium content of natural waters and other substances Friedman, Irving Geochimica et Cosmochimica Acta, Vol. 4, Issue 1-2 https://doi.org/10.1016/0016-7037(53)90066-0	journal	August 1953
Isotope geochemistry of fluid inclusions in Permian halite with implications for the isotopic history of ocean water and the origin of saline formation waters Knauth, L. Paul; Beeunas, Mark A. Geochimica et Cosmochimica Acta, Vol. 50, Issue 3 https://doi.org/10.1016/0016-7037(86)90195-X	journal	March 1986
A model for the evolution of brines in salt from the lower Salado Formation, southeastern New Mexico Stein, C. L.; Krumhansl, J. L. Geochimica et Cosmochimica Acta, Vol. 52, Issue 5 https://doi.org/10.1016/0016-7037(88)90258-X	journal	May 1988
The composition of Permian seawater Horita, Juske; Friedman, Thomas J.; Lazar, Boaz Geochimica et Cosmochimica Acta, Vol. 55, Issue 2 https://doi.org/10.1016/0016-7037(91)90001-L	journal	February 1991
Liquid-vapor fractionation of oxygen and hydrogen isotopes of water from the freezing to the critical temperature Horita, Juske; Wesolowski, David J. Geochimica et Cosmochimica Acta, Vol. 58, Issue 16 https://doi.org/10.1016/0016-7037(94)90096-5	journal	August 1994
Automatic δD and δ18O analyses of multi-water samples using H2- and CO2-water equilibration methods with a common equilibration set-up Horita, Juske; Ueda, Akira; Mizukami, Kanae International Journal of Radiation Applications and Instrumentation. Part A. Applied Radiation and Isotopes, Vol. 40, Issue 9 https://doi.org/10.1016/0883-2889(89)90100-7	journal	January 1989
The origin of fluids in the salt beds of the Delaware Basin, New Mexico and Texas O'Neil, James R.; Johnson, Clark M.; White, Llyod D. Applied Geochemistry, Vol. 1, Issue 2 https://doi.org/10.1016/0883-2927(86)90011-9	journal	March 1986
Geochemistry of the waste isolation pilot plant (WIPP) site, southestern New Mexico, U.S.A. Lambert, Steven J. Applied Geochemistry, Vol. 7, Issue 6 https://doi.org/10.1016/0883-2927(92)90068-E	journal	November 1992
40Ar/39Ar dating of Late Permian evaporites, southeastern New Mexico, USA Renne, Paul R.; Sharp, Warren D.; Montañez, Isabel P. Earth and Planetary Science Letters, Vol. 193, Issue 3-4 https://doi.org/10.1016/S0012-821X(01)00525-8	journal	December 2001
Development of the conceptual models for chemical conditions and hydrology used in the 1996 performance assessment for the Waste Isolation Pilot Plant Larson, K. W. Reliability Engineering & System Safety, Vol. 69, Issue 1-3 https://doi.org/10.1016/S0951-8320(00)00025-9	journal	September 2000
Triple oxygen isotopes in the water cycle Aron, Phoebe G.; Levin, Naomi E.; Beverly, Emily J. Chemical Geology, Vol. 565 https://doi.org/10.1016/j.chemgeo.2020.120026	journal	March 2021
Precise oxygen and hydrogen isotope determination in nanoliter quantities of speleothem inclusion water by cavity ring-down spectroscopic techniques Uemura, Ryu; Nakamoto, Masashi; Asami, Ryuji Geochimica et Cosmochimica Acta, Vol. 172 https://doi.org/10.1016/j.gca.2015.09.017	journal	January 2016
Precise and accurate isotope fractionation factors (α17O, α18O and αD) for water and CaSO4·2H2O (gypsum) Gázquez, Fernando; Evans, Nicholas P.; Hodell, David A. Geochimica et Cosmochimica Acta, Vol. 198 https://doi.org/10.1016/j.gca.2016.11.001	journal	February 2017
A unified Craig-Gordon isotope model of stable hydrogen and oxygen isotope fractionation during fresh or saltwater evaporation Gonfiantini, Roberto; Wassenaar, Leonard I.; Araguas-Araguas, Luis Geochimica et Cosmochimica Acta, Vol. 235 https://doi.org/10.1016/j.gca.2018.05.020	journal	August 2018
Synthesis of results for Brine Availability Test in Salt (BATS) DECOVALEX-2023 Task E Kuhlman, Kristopher L.; Bartol, Jeroen; Benbow, Steven J. Geomechanics for Energy and the Environment, Vol. 39 https://doi.org/10.1016/j.gete.2024.100581	journal	September 2024
Conversion of Hydrogenic Materials to Hydrogen for Isotopic Analysis Bigeleisen, Jacob; Perlman, M. L.; Prosser, H. C. Analytical Chemistry, Vol. 24, Issue 8 https://doi.org/10.1021/ac60068a025	journal	August 1952
Stable Isotope Analysis of Saline Water Samples on a Cavity Ring-down Spectroscopy Instrument Skrzypek, Grzegorz; Ford, Douglas Environmental Science & Technology, Vol. 48, Issue 5 https://doi.org/10.1021/es4049412	journal	February 2014
How old are bacteria from the Permian age? Hazen, Robert M.; Roedder, Edwin Nature, Vol. 411, Issue 6834 https://doi.org/10.1038/35075663	journal	May 2001
High-precision timeline for Earth’s most severe extinction Burgess, Seth D.; Bowring, Samuel; Shen, Shu-zhong Proceedings of the National Academy of Sciences, Vol. 111, Issue 9 https://doi.org/10.1073/pnas.1317692111	journal	February 2014
USGS48 Puerto Rico precipitation – a new isotopic reference material for δ²H and δ¹⁸O measurements of water Qi, Haiping; Coplen, Tyler B.; Tarbox, Lauren Isotopes in Environmental and Health Studies, Vol. 50, Issue 4 https://doi.org/10.1080/10256016.2014.905555	journal	April 2014
Isotopic Variations in Meteoric Waters Craig, H. Science, Vol. 133, Issue 3465 https://doi.org/10.1126/science.133.3465.1702	journal	May 1961
Isotopic Composition and Origin of the Red Sea and Salton Sea Geothermal Brines Craig, H. Science, Vol. 154, Issue 3756 https://doi.org/10.1126/science.154.3756.1544	journal	December 1966
Origin of depositional cycles in a Permian "saline giant": The Salado (McNutt zone) evaporites of New Mexico and Texas Lowenstein, Tim K. Geological Society of America Bulletin, Vol. 100, Issue 4 https://doi.org/10.1130/0016-7606(1988)100<0592:OODCIA>2.3.CO;2	journal	April 1988
Isotopes in the Water Cycle: Regional- to Global-Scale Patterns and Applications Bowen, Gabriel J.; Cai, Zhongyin; Fiorella, Richard P. Annual Review of Earth and Planetary Sciences, Vol. 47, Issue 1 https://doi.org/10.1146/annurev-earth-053018-060220	journal	May 2019
Rb-Sr Ages of Diagenesis of Mg-rich Clay in Permian Sediments, Palo Duro Basin, Texas Panhandle, U.S.A. No authors listed SEPM Journal of Sedimentary Research, Vol. Vol. 67 https://doi.org/10.1306/D426853B-2B26-11D7-8648000102C1865D	journal	January 1997
Salt disposal of heat-generating nuclear waste. Leigh, Christi D.; Hansen, Francis D. https://doi.org/10.2172/1005078	report	January 2011
Optimization of instrument setup and post-run corrections for oxygen and hydrogen stable isotope measurements of water by isotope ratio infrared spectroscopy (IRIS): Water stable isotope analysis with IRIS van Geldern, Robert; Barth, Johannes A. C. Limnology and Oceanography: Methods, Vol. 10, Issue 12 https://doi.org/10.4319/lom.2012.10.1024	journal	December 2012
New online method for water isotope analysis of speleothem fluid inclusions using laser absorption spectroscopy (WS-CRDS) Affolter, S.; Fleitmann, D.; Leuenberger, M. Climate of the Past, Vol. 10, Issue 4 https://doi.org/10.5194/cp-10-1291-2014	journal	July 2014

Similar Records

Conclusions after eleven years of studying brine at the Waste Isolation Pilot Plant

Technical Report · Fri Dec 30 23:00:00 EST 1994 · OSTI ID:111737

Brine inclusions in halite and the origin of the Middle Devonian Prairie evaporites of Western Canada

Journal Article · Sun Sep 01 00:00:00 EDT 1996 · Journal of Sedimentary Research, Section A: Sedimentary Petrology and Processes · OSTI ID:445630

Chemistry of brines in salt from the Waste Isolation Pilot Plant (WIPP), southeastern New Mexico: a preliminary investigation

Technical Report · Fri Feb 28 23:00:00 EST 1986 · OSTI ID:6061544

Related Subjects

58 GEOSCIENCES
BATS
Brines
CRDS
Earth Sciences
Halite Fluid Inclusions
Nuclear Waste
Repository Science
Stable Isotopes

Measuring the Stable Isotope Composition of Water in Brine from Halite Fluid Inclusions and Borehole Brine Seeps Using Cavity Ring-Down Spectroscopy

Citation Formats

References (41)

Similar Records

Related Subjects