Spatially resolved structural order in low-temperature liquid electrolyte

Xie, Yujun; Wang, Jingyang; Savitzky, Benjamin H.; Chen, Zheng; Wang, Yu; Betzler, Sophia B.; Bustillo, Karen C.; Persson, Kristin A.; Cui, Yi; Wang, Lin‐Wang; Ophus, Colin; Ercius, Peter; Zheng, Haimei

doi:10.1126/sciadv.adc9721

Cited by 18 publications

(10 citation statements)

References 60 publications

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“…Therefore, it is natural to define a EC/PC solvent molecule to be in the coordination shell if the Li-O (carbonyl) separation is less than 2.5 Å. Whereas, the Li-F pair correlation function (cumulative coordination number) often has much smaller peak(s) (much steadier increase) at 3 − 4 Å, despite the van der Waals radius of F (in the employed MD simulation) only being only slightly larger than O [41,44,87]. Therefore, we shall focus solely on the solvents in the cation coordination shell, not delving into the information about cation-anion association in this section.…”

Section: Cation Solvation In Classical Non-aqueous Electrolytesmentioning

confidence: 99%

Theory of Cation Solvation and Ionic Association in Non-Aqueous Solvent Mixtures

Goodwin¹,

McEldrew²,

Kozinsky³

et al. 2023

Preprint

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Conventional lithium-ion batteries, and many next-generation technologies, rely on organic electrolytes with multiple solvents to achieve the desired physicochemical and interfacial properties. The complex interplay between these physicochemical and interfacial properties can often be elucidated via the coordination environment of the cation. We develop a theory for the coordination shell of cations in non-aqueous solvent mixtures that can be applied with high fidelity, up to very high salt concentrations. Our theory can naturally explain simulation and literature values of cation solvation in "classical" non-aqueous electrolytes. Moreover, we utilise our theory to understand general design principles of emerging classes of non-aqueous electrolyte mixtures. It is hoped that this theory provides a systematic framework to understand simulations and experiments which engineer the solvation structure and ionic associations of concentrated non-aqueous electrolytes.

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Section: Cation Solvation In Classical Non-aqueous Electrolytesmentioning

confidence: 99%

Theory of Cation Solvation and Ionic Association in Non-Aqueous Solvent Mixtures

Goodwin¹,

McEldrew²,

Kozinsky³

et al. 2023

Preprint

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show abstract

“…SolvationAnalysis was designed to free researchers from laboriously implementing and validating common analyses. In addition to routine properties like coordination numbers, solute-solvent pairing, and solute speciation, SolvationAnalysis uses tools from the SciPy ecosystem (Harris et al, 2020) (Virtanen et al, 2020) to implement analyses of network formation (Xie et al, 2023) and residence times (Self et al, 2019), summarized in Figure 1. To make visualization fast, the package includes a robust set of plotting tools built on top of Matplotlib and Plotly (Hunter, 2007) (Plotly, 2015).…”

Section: Statement Of Needmentioning

confidence: 99%

SolvationAnalysis: A Python toolkit for understanding liquid solvation structure in classical molecular dynamics simulations

Cohen¹,

MacDermott-Opeskin²,

Lee³

et al. 2023

JOSS

Self Cite

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The macroscopic behavior of matter is determined by the microscopic arrangement of atoms, but this arrangement is often difficult or impossible to observe experimentally. Instead, researchers use simulation techniques like molecular dynamics to probe the microscopic structure and dynamics of everything from proteins to battery electrolytes. SolvationAnalysis extracts solvation information from completed molecular dynamics simulations, letting researchers access key solvation structure statistics with minimal effort and accelerating scientific research.

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“…However, the traditional solvents still have some drawbacks that restrict the scope of applications for LIBs. For example, for single solvents, high melting points result in LIBs’ poor properties at low temperatures; low dielectric constants result in low solubility; and high viscosity causes the cells to have a high internal resistance and low voltage platforms, severely restricting the performance of cells and the range of their applications. − The root cause of these problems is mainly dependent on the electrolyte of LIBs. These issues will ultimately result in decreased low-temperature performance or even functional failure. − In addition, lithium salt is another crucial component of the lithium-ion battery electrolyte because the electrolyte’s ionic conductivity is essential to the battery’s low temperature, which can be impacted by the lithium salt solubility. − LiPF 6 is currently regarded as the most practical lithium salt and frequently used in industrial solvents.…”

Section: Introductionmentioning

confidence: 99%

EB (Ethyl Butyrate) as a Cosolvent of Electrolyte Tuning an Ultrathin CEI Membrane for Improving the Ultralow-Temperature Behaviors of LiNi_0.8Co_0.1Mn_0.1O₂ Batteries

Li,

Lv,

Chen

et al. 2023

ACS Sustainable Chem. Eng.

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Adding lithium difluorophosphate into the original electrolyte results in outstanding eletrochemical performances among low temperatures, as documented in our earlier published work; therefore, to be able to gain more stability in lowtemperature performances, in this work, a kind of linear carboxylate cosolvent, EB (ethyl butyrate), is introduced, which has low viscosity (0.639 mPa s), high ion conductivity (5.18 mS cm −1 ), and ultralow melting point (−93 °C). The study's results show that the basic electrolyte's conductivity and viscosity are correspondingly 2.9 mS cm −1 and 3.34 mPa s at −40 °C; however, comparing under the same condition, after adding 16% EB into the baseline, the conductivity and viscosity are 3.37 mS cm −1 and 3.07 mPa s, whose amplitude changes show that the conductivity has increased by 16.2% and the viscosity has dropped by 8% in the interim. Therefore, the addition of EB can clearly boost conductivity, also drastically decreasing the electrolyte's viscosity, further to signify that the addition of EB can contribute to the decrease in the resistance during lithium-ion transport in cold conditions. Besides, the electrochemical properties of the batteries during cold conditions can be obviously improved by adding EB. In addition, after 50 cycles of −40 °C, the basic electrolyte has a discharge capacity of 81.94 mAh g −1 ; on the contrary, the cells using the 16 EB-modified coreagent maintains a discharge capacity of 112.3 mAh g −1 under the same conditions. Overall, the cells containing EB perform exceptionally well at low temperatures and are capable of meeting the appliance of Li-ion batteries in a cool environment.

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Spatially resolved structural order in low-temperature liquid electrolyte

Cited by 18 publications

References 60 publications

Theory of Cation Solvation and Ionic Association in Non-Aqueous Solvent Mixtures

Theory of Cation Solvation and Ionic Association in Non-Aqueous Solvent Mixtures

SolvationAnalysis: A Python toolkit for understanding liquid solvation structure in classical molecular dynamics simulations

EB (Ethyl Butyrate) as a Cosolvent of Electrolyte Tuning an Ultrathin CEI Membrane for Improving the Ultralow-Temperature Behaviors of LiNi_0.8Co_0.1Mn_0.1O₂ Batteries

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Spatially resolved structural order in low-temperature liquid electrolyte

Cited by 18 publications

References 60 publications

Theory of Cation Solvation and Ionic Association in Non-Aqueous Solvent Mixtures

Theory of Cation Solvation and Ionic Association in Non-Aqueous Solvent Mixtures

SolvationAnalysis: A Python toolkit for understanding liquid solvation structure in classical molecular dynamics simulations

EB (Ethyl Butyrate) as a Cosolvent of Electrolyte Tuning an Ultrathin CEI Membrane for Improving the Ultralow-Temperature Behaviors of LiNi0.8Co0.1Mn0.1O2 Batteries

Contact Info

Product

Resources

About

EB (Ethyl Butyrate) as a Cosolvent of Electrolyte Tuning an Ultrathin CEI Membrane for Improving the Ultralow-Temperature Behaviors of LiNi_0.8Co_0.1Mn_0.1O₂ Batteries