Cited by 851Advanced Battery Materials and TechnologiesAdvancements in Battery MaterialsAqueous and Flow Batteries

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Tailoring electrolyte solvation for Li metal batteries cycled at ultra-low temperature

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Holoubek, John, Liu, Haodong, Wu, Zhaohui, Yin, Yijie, Xing, Xing, Cai, Guorui, Yu, Sicen, Zhou, Hongyao, Pascal, Tod A., Chen, Zheng, Liu, Ping·2021·Nature Energy

DOI 10.1038/s41560-021-00783-zPMC PMC7954221

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Abstract

Lithium metal batteries (LMBs) hold the promise to pushing cell level energy densities beyond 300 Wh kg-1 while operating at ultra-low temperatures (< -30°C). Batteries capable of both charging and discharging at these temperature extremes are highly desirable due to their inherent reduction of external warming requirements. Here we demonstrate that the local solvation structure of the electrolyte defines the charge-transfer behavior at ultra-low temperature, which is crucial for achieving high Li metal coulombic efficiency (CE) and avoiding dendritic growth. These insights were applied to Li metal full cells, where a high-loading 3.5 mAh cm-2 sulfurized polyacrylonitrile (SPAN) cathode was paired with a one-fold excess Li metal anode. The cell retained 84 % and 76 % of its room temperature capacity when cycled at -40 and -60 °C, respectively, which presented stable performance over 50 cycles. This work provides design criteria for ultra-low temperature LMB electrolytes, and represents a defining step for the performance of low-temperature batteries.

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Influential
Hydrofluorocarbon electrolytes for energy-dense and low-temperature batteries
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Regulating the reduction reaction pathways via manipulating the solvation shell and donor number of the solvent in Li-CO 2 chemistry
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“To explain solvation structure–property correlations in depth, radial distribution function (RDF) calculations were conducted to further reveal detailed information on the solvation shell structure, which determines the different SEI formation mechanisms in DMSO- and TEGDME-based electrolytes (34, 35).”
Background
Revealing the evolution of solvation structure in low-temperature electrolytes for lithium batteries
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Electrolyte Chemistry Modulation Toward High‐Performance and Ultralow‐Temperature Silicon Anode
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A >200 Wh kg−1 anode-free Na pouch battery at −40°C enabled by manipulating electrolyte equilibrium
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“5 h) [6 ,22 ,39 ,56 ].”
Cyclopentylmethyl Ether, a Non‐Fluorinated, Weakly Solvating and Wide Temperature Solvent for High‐Performance Lithium Metal Battery
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Rational design of hierarchically-solvating electrolytes enabling highly stable lithium metal batteries with high-nickel cathodes
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Self-citation
A Polysiloxane-Enabled Ternary Eutectic Electrolyte with Fast Ion Transport under Extreme Conditions
Li, W., Wen, P., Ren, Y., Xie, W., Lin, J., Chen, M., Yang, Y., & Lin, X. (2023) · ACS Energy Letters · doi:10.1021/acsenergylett.3c01558 · Cited by 45
Partially Ion‐Paired Solvation Structure Design for Lithium‐Sulfur Batteries under Extreme Operating Conditions
Cai, G., Gao, H., Li, M., Gupta, V., Holoubek, J. J., Pascal, T. A., Liu, P., & Chen, Z. (2023) · Angewandte Chemie International Edition · doi:10.1002/anie.202316786 · Cited by 45
Self-citation
In Situ Orthogonal Polymerization for Constructing Fast-Charging and Long-Lifespan Li Metal Batteries with Topological Copolymer Electrolytes
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Reconstructing Inorganic‐Rich Interphases by Nonflammable Electrolytes for High‐Voltage and Low‐Temperature LiNi0.5Mn1.5O4 Cathodes
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Self-citation
Strongly and Weakly Solvating Solvents Co-Coordinated Electrolyte for Stable Lithium Metal Batteries
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Heterostructured Solid Electrolyte Interphase Enables Facilitated Kinetics for Low‐Temperature Sodium‐Ion Batteries
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Manipulating anion solvation competitiveness via a multifunctional additive toward robust low-temperature sodium metal batteries
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Electrolyte Design and Optimization for Alkali Metal‐Sulfur Batteries
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A Coordinated-Anion-Enriched Electrolyte for Lean-Electrolyte Li–S Batteries
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Carboxylate‐Based Electrolyte with Bilateral Functions Enable Working Sodium‐Metal Batteries at −60°C
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Predicting the Ion Desolvation Pathway of Lithium Electrolytes and Their Dependence on Chemistry and Temperature
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Self-citation
Tuning of electrolyte solvation structure for low-temperature operation of lithium–sulfur batteries
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Toward a quantitative interfacial description of solvation for Li metal battery operation under extreme conditions
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“Early works in this area demonstrated that applying solvents that bind weakly with Li in solution does so, where Li/anion coordination is observed in tandem with reduced charge- transfer impedance (28, 34).”
BackgroundSelf-citation
Reversible uniform and fine deposition stabilizing zinc anode at low temperature
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Tantalum oxide nanosheets/polypropylene composite separator constructing lithium-ion channels for stable lithium metal batteries
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Potassium‐Based Dual‐Ion Batteries Operating at −60 °C Enabled By Co‐Intercalation Anode Chemistry
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Electrolyte design weakens lithium-ion solvation for a fast-charging and long-cycling Si anode
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“32,33 The desolvation energy is closely related to the solvation structure of the electrolyte.”
Anion-Containing Solvation Structure Reconfiguration Enables Wide-Temperature Electrolyte for High-Energy-Density Lithium-Metal Batteries
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Spatially resolved structural order in low-temperature liquid electrolyte
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“…solids are found in the short-range order (SRO) regime of less than 5 Å. Mounting experimental evidence has confirmed the existence of SRO and its strong influence on electrical conduction ( 1 – 3 ), ion transport ( 4 , 5 ), mechanical strength ( 6 – 8 ), and crystallization processes ( 9 , 10 ).”
BackgroundSelf-citation

Authors: Holoubek, J., Liu, H., Wu, Z., Yin, Y., Xing, X., Cai, G., Yu, S., Zhou, H., Pascal, T. A., Chen, Z., & Liu, P.
Affiliations: University of California San Diego (US)
Corresponding author: Pascal, Tod A.
Chen, Zheng
Liu, Ping
ORCID: Holoubek, John
Liu, Haodong
Wu, Zhaohui
Yin, Yijie
Xing, Xing
Cai, Guorui
Yu, Sicen
Zhou, Hongyao
Pascal, Tod A.
Chen, Zheng
Liu, Ping
Venue: Nature Energy
Publisher: Springer Science and Business Media LLC
Published: 2021-02-25
Volume: 6
Issue: 3
Pages: 303-313
ISSN: 2058-7546 (ISSN-L)
DOI: 10.1038/s41560-021-00783-z
PMC: PMC7954221
OpenAlex: W3134786422
Cited by: 851
References: 53
Citations by year: 2026: 98 · 2025: 210 · 2024: 184 · 2023: 176 · 2022: 140 · 2021: 43
FWCI: 39.93
Type: journal article
Language: en
Open access: green
www.ncbi.nlm.nih.gov
Licence: www.springernature.com/gp/researchers/text-and-data-mining (tdm)
www.springernature.com/gp/researchers/text-and-data-mining (vor)
Locations: Nature Energy (publishedVersion)
PubMed (publishedVersion)
PubMed Central (acceptedVersion)
eScholarship (California Digital Library) (submittedVersion)
RePEc: Research Papers in Economics (submittedVersion)
Funders: National Aeronautics and Space Administration (ECF 80NSSC18K1512)
U.S. Department of Energy (DE-EE0007764)
Topics: Physical Sciences › Engineering › Electrical and Electronic Engineering › Advanced Battery Materials and Technologies
Physical Sciences › Engineering › Electrical and Electronic Engineering › Advancements in Battery Materials
Physical Sciences › Engineering › Electrical and Electronic Engineering › Aqueous and Flow Batteries
Keywords: lithium metal batteries, electrolyte solvation structure, Coulombic efficiency, lithium dendrite suppression, lithium metal anode, low-temperature battery performance

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Tailoring electrolyte solvation for Li metal batteries cycled at ultra-low temperature

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