Release, Transport, and accumulation of lithium in shale brines

Kyung Jae Lee; Jiahui You; Yongjun Gao; Tanguy Terlier

doi:10.1016/j.fuel.2023.129629

Release, Transport, and accumulation of lithium in shale brines

Kyung Jae Lee, Jiahui You, Yongjun Gao, Tanguy Terlier

Geochemistry & Interfacial Science

Research output: Contribution to journal › Article › peer-review

5 Scopus citations

Abstract

In order to mitigate climate change, diversifying the sources of lithium supply is crucial for the decarbonization of energy sector through enhanced renewable electricity generation and electrified transportation. Shale brines have been recently found to be containing significant amount of lithium, but relevant subsurface phenomena regarding its origin, fate, and transport are unknown. Here we present a suite of geochemical experiments to elucidate the initial presence of lithium in shale rocks and its release mechanism from solid phase into fluid, and numerical modeling to estimate the resources of lithium in shale brines by addressing its fate and transport. We find that the majority of lithium is inorganically bound as an interlayer cation of clay in shale rock, while a sparingly small portion is organically bound. Hydrothermal reaction experiments for leaching lithium reveal that calcium ion in fluid has strongest impact on lithium to be released into fluid, while sodium ion has minimal impact. From the numerical modeling combined with the experimental findings, average concentration of lithium in shale brines mimicking Marcellus Shale system is estimated to be about 135 ppm under calcium ion dominancy in pore fluid, which shows excellent match with actually measured values from produced Marcellus Shale brines. This study provides the understanding of fundamental phenomena addressing release, transport, and accumulation of lithium in geologic system, and hence contributes to the enhancement of sources of lithium supply for energy decarbonization.

Original language	English
Article number	129629
Journal	Fuel
Volume	356
DOIs	https://doi.org/10.1016/j.fuel.2023.129629
State	Published - Jan 15 2024

Funding

We appreciate the funding for this research from National Science Foundation under Award 2042504 (CAREER: Identifying a New Source of Lithium for Sustainable and Renewable Energy Storage). The paper was benefitted from the support of J. Casey and K. Bissada of Department of Earth and Atmospheric Sciences at the University of Houston, for letting us to utilize their laboratory facilities for elemental analysis and kerogen isolation, respectively. We also thank a company in Utah for providing Green River Shale samples, and another company in Pennsylvania for providing the produced water samples from Marcellus Shale. ToF–SIMS analysis was carried out with support provided by the National Science Foundation CBET-1626418, where it was conducted in part using the resources of the Shared Equipment Authority (SEA) at Rice University. We appreciate the funding for this research from National Science Foundation under Award 2042504 (CAREER: Identifying a New Source of Lithium for Sustainable and Renewable Energy Storage). The paper was benefitted from the support of J. Casey and K. Bissada of Department of Earth and Atmospheric Sciences at the University of Houston, for letting us to utilize their laboratory facilities for elemental analysis and kerogen isolation, respectively. We also thank a company in Utah for providing Green River Shale samples, and another company in Pennsylvania for providing the produced water samples from Marcellus Shale. ToF–SIMS analysis was carried out with support provided by the National Science Foundation CBET-1626418, where it was conducted in part using the resources of the Shared Equipment Authority (SEA) at Rice University.

Keywords

Critical minerals
Energy decarbonization
Lithium
Renewable energy storage
Shale brines
Sustainable energy system

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10.1016/j.fuel.2023.129629

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title = "Release, Transport, and accumulation of lithium in shale brines",

abstract = "In order to mitigate climate change, diversifying the sources of lithium supply is crucial for the decarbonization of energy sector through enhanced renewable electricity generation and electrified transportation. Shale brines have been recently found to be containing significant amount of lithium, but relevant subsurface phenomena regarding its origin, fate, and transport are unknown. Here we present a suite of geochemical experiments to elucidate the initial presence of lithium in shale rocks and its release mechanism from solid phase into fluid, and numerical modeling to estimate the resources of lithium in shale brines by addressing its fate and transport. We find that the majority of lithium is inorganically bound as an interlayer cation of clay in shale rock, while a sparingly small portion is organically bound. Hydrothermal reaction experiments for leaching lithium reveal that calcium ion in fluid has strongest impact on lithium to be released into fluid, while sodium ion has minimal impact. From the numerical modeling combined with the experimental findings, average concentration of lithium in shale brines mimicking Marcellus Shale system is estimated to be about 135 ppm under calcium ion dominancy in pore fluid, which shows excellent match with actually measured values from produced Marcellus Shale brines. This study provides the understanding of fundamental phenomena addressing release, transport, and accumulation of lithium in geologic system, and hence contributes to the enhancement of sources of lithium supply for energy decarbonization.",

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N2 - In order to mitigate climate change, diversifying the sources of lithium supply is crucial for the decarbonization of energy sector through enhanced renewable electricity generation and electrified transportation. Shale brines have been recently found to be containing significant amount of lithium, but relevant subsurface phenomena regarding its origin, fate, and transport are unknown. Here we present a suite of geochemical experiments to elucidate the initial presence of lithium in shale rocks and its release mechanism from solid phase into fluid, and numerical modeling to estimate the resources of lithium in shale brines by addressing its fate and transport. We find that the majority of lithium is inorganically bound as an interlayer cation of clay in shale rock, while a sparingly small portion is organically bound. Hydrothermal reaction experiments for leaching lithium reveal that calcium ion in fluid has strongest impact on lithium to be released into fluid, while sodium ion has minimal impact. From the numerical modeling combined with the experimental findings, average concentration of lithium in shale brines mimicking Marcellus Shale system is estimated to be about 135 ppm under calcium ion dominancy in pore fluid, which shows excellent match with actually measured values from produced Marcellus Shale brines. This study provides the understanding of fundamental phenomena addressing release, transport, and accumulation of lithium in geologic system, and hence contributes to the enhancement of sources of lithium supply for energy decarbonization.

AB - In order to mitigate climate change, diversifying the sources of lithium supply is crucial for the decarbonization of energy sector through enhanced renewable electricity generation and electrified transportation. Shale brines have been recently found to be containing significant amount of lithium, but relevant subsurface phenomena regarding its origin, fate, and transport are unknown. Here we present a suite of geochemical experiments to elucidate the initial presence of lithium in shale rocks and its release mechanism from solid phase into fluid, and numerical modeling to estimate the resources of lithium in shale brines by addressing its fate and transport. We find that the majority of lithium is inorganically bound as an interlayer cation of clay in shale rock, while a sparingly small portion is organically bound. Hydrothermal reaction experiments for leaching lithium reveal that calcium ion in fluid has strongest impact on lithium to be released into fluid, while sodium ion has minimal impact. From the numerical modeling combined with the experimental findings, average concentration of lithium in shale brines mimicking Marcellus Shale system is estimated to be about 135 ppm under calcium ion dominancy in pore fluid, which shows excellent match with actually measured values from produced Marcellus Shale brines. This study provides the understanding of fundamental phenomena addressing release, transport, and accumulation of lithium in geologic system, and hence contributes to the enhancement of sources of lithium supply for energy decarbonization.

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Release, Transport, and accumulation of lithium in shale brines

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