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

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

doi:10.1038/s41560-021-00783-z

Cited by 851Advanced Battery Materials and TechnologiesAdvancements in Battery MaterialsAdvanced battery technologies research

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 +3 more·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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The Li/SPAN cell using 1 M LiFSI in DOL/DME failed immediately at -60 °C.
“In contrast, the Li/SPAN cell using 1 M LiFSI in DOL/DME failed immediately at -60 °C.”
From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [57]
The Full Cell Behavior section (Fig. 6g; page not provided) reports that the Li||SPAN cell using 1 M LiFSI in DOL/DME had no viable capacity output after two cycles at −60 °C. This supports failure at that temperature, but not the claim that it failed immediately. (LLM, conf=0.88)
Experimental — accuracy not yet measured
The low binding energy of Li+(DEE)1.8 provided a favorable desolvation energy barrier and resulted in excellent Coulombic efficiency (98.4%) of Li/Cu cells at -60 °C.
“The low binding energy of Li + (DEE) 1.8 provided a much favorable desolvation energy barrier to be overcome and resulted in excellent CE (98.4%) of Li/Cu cells at ultra-LTs (-60 °C), as shown in Fig. 8b.”
From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [57]
DEE electrolytes presented characteristic contact-ion pairs with 1.8 DEE oxygens and 2.0 FSI- oxygens per Li+.
“Different from typical solvent-separated ion pair (SSIP) solvation structure, DEE electrolytes presented characteristic CIPs with 1.8 DEE oxygens and 2.0 FSI -oxygens per Li + .”
From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [57]
Li+(DEE)1.8 complexes possessed a much lower binding energy of -280 kJ mol-1 than Li+(DME)2.3 (-414 kJ mol-1) formed in 1 M LiFSI in DOL-DME electrolytes.
“Meanwhile, the Li + (DEE) 1.8 complexes possessed a much lower binding energy of -280 kJ mol -1 than that of Li + (DME) 2.3 (-414 kJ mol -1 ) formed in 1 M LiFSI in DOL-DME electrolytes shown in Fig. 8a.”
From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [57]

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Electrolytes in Organic Batteries
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A Review on Regulating Li+Solvation Structures in Carbonate Electrolytes for Lithium Metal Batteries
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Ether‐Based Electrolyte Chemistry Towards High‐Voltage and Long‐Life Na‐Ion Full Batteries
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Electrode–Electrolyte Interfacial Chemistry Modulation for Ultra‐High Rate Sodium‐Ion Batteries
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Self‐Enhancing Gel Polymer Electrolyte by In Situ Construction for Enabling Safe Lithium Metal Battery
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External Li supply reshapes Li deficiency and lifetime limit of batteries
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Designing phosphazene-derivative electrolyte matrices to enable high-voltage lithium metal batteries for extreme working conditions
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Extending the low-temperature operation of sodium metal batteries combining linear and cyclic ether-based electrolyte solutions
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Enhancing Li+ Transport in NMC811||Graphite Lithium‐Ion Batteries at Low Temperatures by Using Low‐Polarity‐Solvent Electrolytes
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Designing Temperature-Insensitive Solvated Electrolytes for Low-Temperature Lithium Metal Batteries.
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Designing Weakly Solvating Solid Main-Chain Fluoropolymer Electrolytes: Synergistically Enhancing Stability toward Li Anodes and High-Voltage Cathodes
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Challenges and Breakthroughs in Enhancing Temperature Tolerance of Sodium‐Ion Batteries
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Restructuring Electrolyte Solvation by a Versatile Diluent Toward Beyond 99.9% Coulombic Efficiency of Sodium Plating/Stripping at Ultralow Temperatures
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Revealing the Anion–Solvent Interaction for Ultralow Temperature Lithium Metal Batteries
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Solvent Gaming Chemistry to Control the Quality of Halide Perovskite Thin Films for Photovoltaics
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“6,7 − 12 The ABX 3 structure of OIHPs is composed of a three-dimensional network of corner-shared BX 6 octahedra and A + counter cations situated in the voids.”
Fire-extinguishing, recyclable liquefied gas electrolytes for temperature-resilient lithium-metal batteries
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Advanced Ultralow‐Concentration Electrolyte for Wide‐Temperature and High‐Voltage Li‐Metal Batteries
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Fire‐Retardant, Stable‐Cycling and High‐Safety Sodium Ion Battery
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Synergy of Weakly‐Solvated Electrolyte and Optimized Interphase Enables Graphite Anode Charge at Low Temperature
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Balanced Interfacial Ion Concentration and Migration Steric Hindrance Promoting High‐Efficiency Deposition/Dissolution Battery Chemistry
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Atomic Insights into Advances and Issues in Low‐Temperature Electrolytes
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Asymmetric ether solvents for high-rate lithium metal batteries
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Toward High Temperature Sodium Metal Batteries via Regulating the Electrolyte/Electrode Interfacial Chemistries
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Promoting Mechanistic Understanding of Lithium Deposition and Solid‐Electrolyte Interphase (SEI) Formation Using Advanced Characterization and Simulation Methods: Recent Progress, Limitations, and Future Perspectives
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Multifunctional Additives to Realize Dendrite‐Free Lithium Deposition in Carbonate Electrolytes toward Low‐Temperature Li Metal Batteries
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Electrolyte Design for Lithium‐Ion Batteries for Extreme Temperature Applications
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Inhibiting gas generation to achieve ultralong-lifespan lithium-ion batteries at low temperatures
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“Also, it is essential to consider the effect of the interface on the solvation structure [ 33 ].”
Low Concentration Electrolyte Enabling Cryogenic Lithium–Sulfur Batteries
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Tailoring Electrolyte Solvation for Practical Li Metal Batteries Cycled at Ultra-Low Temperature
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Self-citation
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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 › Advanced battery technologies research
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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