Anionic Effects on Concentrated Aqueous Lithium Ion Dynamics

The dynamics, orientational 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...

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Published in:	The journal of physical chemistry letters Vol. 15; no. 19; pp. 5076 - 5087
Main Authors:	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.
Format:	Journal Article
Language:	English
Published:	United States American Chemical Society 16-05-2024
Subjects:	2D IR anions concentrated electrolyte dynamics ion-pair ions lithium Physical Insights into Materials and Molecular Properties salts solution chemistry viscosity
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Abstract	The dynamics, orientational 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. The 2D IR, NMR, and viscosity results show that LiNO2 exhibits longer correlation times, lower diffusivity, and nearly 4 times greater viscosity compared to those of the other lithium salt solutions of the same concentration, suggesting that nitrite anions may strongly facilitate structure formation via strengthening water–ion network interactions, directly impacting bulk solution properties at sufficiently high concentrations. Additionally, the LiNO2 and LiNO3 solutions show significantly weakened chemical interactions between the lithium cations and the methyl thiocyanate when compared with those of the lithium halide salts.
AbstractList	The dynamics, orientational anisotropy, diffusivity, viscosity, and density were measured for concentrated lithium salt solutions, including lithium chloride (LiCl), lithium bromide (LiBr), lithium nitrite (LiNO ), and lithium nitrate (LiNO ), with methyl thiocyanate as an infrared vibrational probe molecule, using two-dimensional infrared spectroscopy (2D IR), nuclear magnetic resonance (NMR) spectroscopy, and viscometry. The 2D IR, NMR, and viscosity results show that LiNO exhibits longer correlation times, lower diffusivity, and nearly 4 times greater viscosity compared to those of the other lithium salt solutions of the same concentration, suggesting that nitrite anions may strongly facilitate structure formation via strengthening water-ion network interactions, directly impacting bulk solution properties at sufficiently high concentrations. Additionally, the LiNO and LiNO solutions show significantly weakened chemical interactions between the lithium cations and the methyl thiocyanate when compared with those of the lithium halide salts. 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. The dynamics, orientational 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. The 2D IR, NMR, and viscosity results show that LiNO2 exhibits longer correlation times, lower diffusivity, and nearly 4 times greater viscosity compared to those of the other lithium salt solutions of the same concentration, suggesting that nitrite anions may strongly facilitate structure formation via strengthening water–ion network interactions, directly impacting bulk solution properties at sufficiently high concentrations. Additionally, the LiNO2 and LiNO3 solutions show significantly weakened chemical interactions between the lithium cations and the methyl thiocyanate when compared with those of the lithium halide salts.
Author	Rosso, Kevin M. Graham, Trent R. Joly, Alan G. Zhao, Yatong Pearce, Carolyn I. Wang, Zheming Pauzauskie, Peter J. Bazak, J. David Felsted, Robert G. Nienhuis, Emily T.
AuthorAffiliation	Department of Crop and Soil Sciences Materials Science and Engineering Department Washington State University Pacific Northwest National Laboratory
AuthorAffiliation_xml	– name: Washington State University – name: Pacific Northwest National Laboratory – name: Department of Crop and Soil Sciences – name: Materials Science and Engineering Department
Author_xml	– sequence: 1 givenname: Robert G. orcidid: 0000-0001-9395-2112 surname: Felsted fullname: Felsted, Robert G. email: Robert.Felsted@pnnl.gov organization: Pacific Northwest National Laboratory – sequence: 2 givenname: Trent R. orcidid: 0000-0001-8907-8004 surname: Graham fullname: Graham, Trent R. organization: Pacific Northwest National Laboratory – sequence: 3 givenname: Yatong surname: Zhao fullname: Zhao, Yatong organization: Pacific Northwest National Laboratory – sequence: 4 givenname: J. David orcidid: 0000-0002-4599-3208 surname: Bazak fullname: Bazak, J. David organization: Pacific Northwest National Laboratory – sequence: 5 givenname: Emily T. orcidid: 0000-0003-4348-5506 surname: Nienhuis fullname: Nienhuis, Emily T. organization: Pacific Northwest National Laboratory – sequence: 6 givenname: Peter J. orcidid: 0000-0002-1554-5949 surname: Pauzauskie fullname: Pauzauskie, Peter J. organization: Materials Science and Engineering Department – sequence: 7 givenname: Alan G. orcidid: 0000-0003-2931-4524 surname: Joly fullname: Joly, Alan G. organization: Pacific Northwest National Laboratory – sequence: 8 givenname: Carolyn I. orcidid: 0000-0003-3098-1615 surname: Pearce fullname: Pearce, Carolyn I. organization: Washington State University – sequence: 9 givenname: Zheming orcidid: 0000-0002-1986-4357 surname: Wang fullname: Wang, Zheming email: Zheming.Wang@pnnl.gov organization: Pacific Northwest National Laboratory – sequence: 10 givenname: Kevin M. orcidid: 0000-0002-8474-7720 surname: Rosso fullname: Rosso, Kevin M. email: Kevin.Rosso@pnnl.gov organization: Pacific Northwest National Laboratory
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Snippet	The dynamics, orientational anisotropy, diffusivity, viscosity, and density were measured for concentrated lithium salt solutions, including lithium chloride... In this article, the structural dynamics, chemical reactivity, anisotropy, diffusivity, viscosity, and density were measured for concentrated lithium salt...
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SubjectTerms	2D IR anions concentrated electrolyte dynamics ion-pair ions lithium Physical Insights into Materials and Molecular Properties salts solution chemistry viscosity
Title	Anionic Effects on Concentrated Aqueous Lithium Ion Dynamics
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