Anionic Effects on Concentrated Aqueous Lithium Ion Dynamics

Felsted, Robert G.; Graham, Trent R.; Zhao, Yatong; Bazak, J. David; Nienhuis, Emily T.; Pauzauskie, Peter J.; Joly, Alan G.; Pearce, Carolyn I.; Wang, Zheming; Rosso, Kevin M.

doi:10.1021/acs.jpclett.4c00585

Title: Anionic Effects on Concentrated Aqueous Lithium Ion Dynamics

Journal Article · 06 May 2024 · Journal of Physical Chemistry Letters

DOI: https://doi.org/10.1021/acs.jpclett.4c00585 · OSTI ID:2448369

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Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); University of Washington, Seattle, WA (United States)
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Washington State University, Pullman, WA (United States)

In this article, the structural dynamics, chemical reactivity, anisotropy, diffusivity, viscosity, and density were measured for concentrated lithium salt solutions, including lithium chloride (LiCl), lithium bromide (LiBr), lithium nitrite (LiNO₂), and lithium nitrate (LiNO₃), with methyl thiocyanate as an infrared vibrational probe molecule, using two-dimensional infrared spectroscopy (2D IR), nuclear magnetic resonance (NMR) spectroscopy, and viscometry. 2D IR, NMR, and viscosity results show that LiNO₂ exhibits longer correlation times, lower diffusivity, and nearly four times greater viscosity when compared to the other lithium salt solutions of the same concentration, suggesting that nitrite anions may strongly facilitate structure formation via strengthening water-ion interactions, directly impacting bulk solution properties at sufficiently high concentrations. Additionally, the LiNO₂ and LiNO₃ solutions show significantly reduced chemical reactivity with respect to lithium cations coordinating with the methyl thiocyanate when compared to the lithium halide salts.

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Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Biological and Environmental Research (BER); Energy Frontier Research Centers (EFRC) (United States). Interfacial Dynamics in Radioactive Environments and Materials (IDREAM)

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 2448369

Report Number(s):: PNNL-SA--195392

Journal Information:: Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Journal Issue: 19 Vol. 15; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Anionic Effects on Concentrated Aqueous Lithium Ion Dynamics

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