A novel cyclopentyl methyl ether electrolyte solvent with a unique solvation structure for subzero (−40 °C) lithium-ion batteries

Ramasamy, Hari Vignesh; Kim, Soohwan; Adams, Ethan; Rao, Harsha; Pol, Vilas G.

doi:10.1039/d2cc00188h

Cited by 19 publications

(24 citation statements)

References 30 publications

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“…Lithium bis(flourosulfonyl)imide (LiFSI) and cyclopentyl methyl ether (CPME) were both obtained from Sigma Aldrich. To synthesize the 1 m LiFSI CPME electrolyte, LiFSI (187.1 mg) was added to CPME (1 mL) [12a] . The salt and solvent were mildly shaken in a rotating fashion until the LiFSI was completely dissolved in the CPME in an Ar‐filled glovebox.…”

Section: Methodsmentioning

confidence: 99%

“…The LIB cells that were tested comprised of an LTO material and 1 м lithium bis(fluorosulfonyl)imide (LiFSI) in cyclopentyl methyl ether (CPME) electrolyte were utilized due to their excellent low‐temperature performance. [ 12 ] The LTO has a low Li + desolvation energy (52 kJ mol −1 ) and high Li + reaction potential (≈1.5 V vs Li/Li + ), which can facilitate Li + transport and prevent Li plating on the electrode surface at cold temperatures. The distinct solvation structures, low melting/freezing point (−140 °C), and relatively high low‐temperature ionic conductivities of the CPME electrolyte minimize electrolyte‐related issues at cold temperatures (Table S1, Supporting Information).…”

Section: Introductionmentioning

confidence: 99%

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Lithium‐Ion Battery Testing Capable of Simulating “Ultralow” Lunar Temperatures

et al. 2022

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The first‐ever lithium‐ion battery cycler capable of testing the coin and pouch cells under ultralow (≤40 °C) temperatures down to −175 °C to simulate extreme climates found in the lunar and space missions, high‐altitude air vehicles, polar regions of Earth, and military expeditionary missions is enthusiastically reported. The extremely cold temperatures are achieved through a tailored extreme low‐temperature system (ELTS) with liquid nitrogen flow and the ability to reach temperatures between −175 and 25 °C, using 1 kΩ and 1 MΩ resistors at varying currents of 1–4 mA and 1–4 μA, respectively, is validated. Employing the ELTS, Li4Ti5O12 (LTO)||Li cells with 1 m lithium bis(fluorosulfonyl)imide in cyclopentyl methyl ether as an electrolyte developed in this research group are charged and discharged at room temperature (cycling rate C/5), −20 (C/10), −40 (C/40), and −60 °C (C/50), which exhibited discharge capacities of 159.04, 119.12, 101.79, and 33.06 mAh g−1, respectively. Moreover, the LTO||Li cell produced a reversible capacity of 7.12 mAh g−1 tested at −100 °C for the first time.

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Section: Methodsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Lithium‐Ion Battery Testing Capable of Simulating “Ultralow” Lunar Temperatures

et al. 2022

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“…The CPME (ether) solvent mixture with PC induces lower desolvation energy, which is attributed to faster charge-transfer kinetic and is partially responsible for excellent performance. 21,22 The charge/discharge profile shows that the WPET-HC exhibits a greater plateau region, significantly below 0.1 V, indicating intercalation followed by closed-pore filling. To quantify the maximum plateaubased capacity for WPET-based HC, typical derivative capacity (dQ/dV) curves were analyzed, as shown in Figure 2c.…”

Section: Electrochemical Characterizationmentioning

confidence: 99%

“…But the unstable (dissolving), richer organic SEI layer results in poor initial Coulombic efficiency (ICE) and capacity decay during cycling. 20,21 The low-temperature performance of EC is worse (liquid temperature range is poor) and is used in combination with other co-solvents for lowtemperature battery applications. Recently, CPME-based solvents were reported for lowtemperature Li-ion and ambient Li-metal batteries.…”

Section: Introductionmentioning

confidence: 99%

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Role of Cyclopentyl methyl ether co-solvent in Improving SEI layer stability in Hard Carbon Anode for Sodium-ion Batteries

Nagmani

Das

Puravankara

2023

Preprint

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The conversion of polyethylene terephthalate (PET) municipal waste via the carbonization process into hard carbon (WPET-HC) delivers a high-performing, low-cost, sustainable anode material for sodium-ion batteries (SIBs). To further optimize the anode, electrolytes and interfacial chemistry are critical in improving cycling stability and rate capability. Herein, cyclopentyl methyl ether (CPME), a weakly solvating and a wide temperature solvent, is used as an alternative co-solvent to ethylene carbonate (EC) to deliver a high initial coulombic efficiency (ICE) up to 75%. The larger interlayer spacing, low surface area, and slit-shaped micro and mesoporous presence in the WPET-HC structure enhance the low potential plateau capacity to 68%, showing a more battery-type anode material from plastic trash. The WPET-HC delivered the excellent reversible capacity of 356 mAh g-1 at the current density of 30 mA g-1 with superior cycling of 91% after 100 cycles using CPME-PC-based electrolyte. The reduction of CPME co-solvent forms a more inorganic SEI than EC-generated SEI, providing a stable and thin SEI layer boosting the ICE and cycling stability of the anode. The low-temperature battery metric for CPME-PC-based electrolytes showed ~30% added capacity and improved ICE value compared to EC-PC-based electrolytes. The CPME-PC-based electrolyte maintained the higher capacity retention of 88% and 74% at 10℃ and 0℃, respectively, with a coulombic efficiency of 100%, revealing the excellent stability of the electrolyte with the HC anode. The work provides an eco-friendly approach to developing hard carbons from plastic trash and reports for the first time the use of greener, low-solvating CPME in improving the reversible capacity and ICE for low-temperature applications of SIBs.

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Nonpolar Cosolvent Driving LUMO Energy Evolution of Methyl Acetate Electrolyte to Afford Lithium‐Ion Batteries Operating at −60 °C

Lei

Zeng

Yan

et al. 2023

Adv Funct Materials

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The operation of lithium‐ion batteries (LIBs) at low temperatures (<−20 °C) is hindered by the low conductivity and high viscosity of conventional carbonate electrolytes. Methyl acetate (MA) has proven to be a competitive low‐temperature electrolyte solvent with low viscosity and low freezing point, but its interfacial stability is poor and remains elusive until now. Here, it is revealed thaat the reductive stability of MA‐based electrolytes is fundamentally governed by the anion‐prevailed solvation structure. Based on this framework, fluorobenzene is employed in the electrolyte to promote the entry of anions into the solvation shell via dipole‐dipole interactions and the generation of free MA, thus enhancing the lowest unoccupied molecular orbital energy of MA. The designed electrolyte enables LiCoO2 (LCO)/graphite cells to exhibit excellent cycling performance at −20 °C (90% retention after 1000 cycles at 1 C) and to remain 91% of their room‐temperature capacity at a super‐low temperature of −60 °C at 0.05 C. Thanks to the plentiful free MA, this electrolyte has a high conductivity (2.61 mS cm−1) at −60 °C and allows LCO/graphite cell to charge at −60 °C. This study offers the possibility of practical applications for those solvents with poor reductive stability and provides new approaches to designing advanced electrolytes for low‐temperature applications.

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A novel cyclopentyl methyl ether electrolyte solvent with a unique solvation structure for subzero (−40 °C) lithium-ion batteries

Abstract: 1M LiFSI in Cyclopentyl methyl ether is shown as novel electrolyte with unique solvation structure to form a thin robust multilayer solid electrolyte interface with inorganic LiF rich inner layer....

Cited by 19 publications

References 30 publications

Lithium‐Ion Battery Testing Capable of Simulating “Ultralow” Lunar Temperatures

Lithium‐Ion Battery Testing Capable of Simulating “Ultralow” Lunar Temperatures

Role of Cyclopentyl methyl ether co-solvent in Improving SEI layer stability in Hard Carbon Anode for Sodium-ion Batteries

Nonpolar Cosolvent Driving LUMO Energy Evolution of Methyl Acetate Electrolyte to Afford Lithium‐Ion Batteries Operating at −60 °C

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