High Chaos Induced Multiple-Anion-Rich Solvation Structure Enabling Ultrahigh Voltage and Wide Temperature Lithium-Metal Batteries

Cheng, Fangyuan; Zhang, Wen; Li, Qing; Fang, Chun; Han, Jiantao; Huang, Yunhui

doi:10.1021/acsnano.3c09759

Cited by 18 publications

(6 citation statements)

References 50 publications

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“…24,67,68 Han et al calculated the entropy of the system using first-principles and the Castep module of density functional theory. 69 This method can only estimate the entropy change of the system under different external environment. Moreover, variations in the temperature coefficient and the heat of the electrolytes are also used to estimate the entropy of liquid HEEs.…”

Section: ■ Features Of Heesmentioning

confidence: 99%

“…Han et al dissolved 0.5 M Li difluoro(oxalic acid)borate, 0.3 M Li hexafluorophosphate, and 0.2 M Li difluorophosphate in dimethyl carbonate and ethyl methyl carbonate to form a HEE operating in a wide temperature range from −30 to 45 °C. 69 The multiple-anionrich solvation sheath promotes the formation of weak solvation structures. This renders faster desolvation of Li + , thus dramatically improving the charge transfer kinetics and inhibiting the growth of Li dendrites.…”

Section: ■ Hees In Working Batteriesmentioning

confidence: 99%

“…Currently, the entropy value of liquid HEEs is mainly calculated based on the molecular dynamics simulation, density functional theory, etc. Molecular dynamics simulation show that HEE is more likely to form a solvated structure, endowing the solvated sheath of Li ions rich in anions, thus reflecting the entropy enhancement. ,, Han et al calculated the entropy of the system using first-principles and the Castep module of density functional theory . This method can only estimate the entropy change of the system under different external environment.…”

Section: Features Of Heesmentioning

confidence: 99%

Section: Hees In Working Batteriesmentioning

confidence: 99%

“…High entropy also functions to improve the performance of batteries at high temperatures. Han et al dissolved 0.5 M Li difluoro(oxalic acid)borate, 0.3 M Li hexafluorophosphate, and 0.2 M Li difluorophosphate in dimethyl carbonate and ethyl methyl carbonate to form a HEE operating in a wide temperature range from −30 to 45 °C . The multiple-anion-rich solvation sheath promotes the formation of weak solvation structures.…”

Section: Hees In Working Batteriesmentioning

confidence: 99%

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Working Principles of High-Entropy Electrolytes in Rechargeable Batteries

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Section: ■ Features Of Heesmentioning

confidence: 99%

Section: ■ Hees In Working Batteriesmentioning

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Section: Features Of Heesmentioning

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Section: Hees In Working Batteriesmentioning

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Working Principles of High-Entropy Electrolytes in Rechargeable Batteries

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Liu,

Guo

et al. 2024

ACS Energy Lett.

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Tuning the Nucleophilicity of Anion in Lithium Salt to Enable an Anion‐Rich Solvation Sheath for Stable Lithium Metal Batteries

Zhou,

Ou,

Feng

et al. 2024

Adv Funct Materials

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Traditional lithium salts typically adhere to the designing principles of enhancing cation‐anion dissociation degree to obtain a high electrolyte conductivity. This promotes the invention of lithium bis(trifluoromethanesulfonyl)imide (LiTFSI), where the symmetric electron‐withdrawing trifluoromethanesulfonyl groups significantly delocalize the negative charge density around the nitrogen atom, thereby weakening the electrostatic interaction between Li+ and the anion. Herein, deviating from the general principle, lithium (methanesulfonyl)(trifluoromethanesulfonyl) imide (LiMTFSI) is deliberately designed by substituting a unilateral electron‐withdrawing trifluoromethyl (─CF3) group of LiTFSI with an electron‐donating methyl (─CH3) group, to tune the nucleophilicity of the anion. This modification enhances Li‐anion interaction, causing the anion to replace the solvent molecules in the Li+ solvation shell. Additionally, the MTFSI− anion exhibits an elevated donor number to facilitate the solubility of LiNO3 in carbonate‐based electrolytes. The synergistic effect of these changes suppresses the decomposition of solvent and helps construct a stable solid electrolyte interphase (SEI) enriched with multiple inorganic lithium salts (e.g., Li2S, Li3N, and LiNxOy) on the Li metal anode, which enables the 500 mAh Li||LiNi0.5Co0.2Mn0.3O2 pouch cell to operate steadily for 150 cycles. It is believed this work would provide new insights and another dimension for designing functional anions beyond their role as charge carriers.

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Lithium Batteries Operating at Wide Temperatures: Opportunities and Challenges

Chen,

Yang,

Zhai

et al. 2024

Adv Funct Materials

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The development of rechargeable lithium batteries (RLBs) has made a great contribution in solving the problems in the current era, such as energy shortage and climate change. With the expanding of application field of RLBs from portable device to large‐scale electric equipment, it is an urgent demand for RLBs to operate in a wide range of temperature. More and more attention has been paid to the design of wide‐temperature RLBs. Therefore, a timely and critical overview of the latest development in the field of RLBs operating at wide temperatures is needed. In this review, an in‐depth understanding on how the temperature affects the thermodynamics of lithium‐ion transport at electrodes, electrolytes, and electrode/electrolyte interfaces is emphasized. Recent progress in probing the temperature effects on electrochemical performance fading is comprehensively discussed. Different strategies to widen the working temperature of RLBs, including regulating the electrode degradation, interface evolution, and electrolyte solvation chemistry are also reviewed. Finally, an outlook of potential future research directions is also proposed, which sheds light on the design of novel electrodes and electrolytes for next‐generation RLBs operating at wide temperatures.

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High Chaos Induced Multiple-Anion-Rich Solvation Structure Enabling Ultrahigh Voltage and Wide Temperature Lithium-Metal Batteries

Cited by 18 publications

References 50 publications

Working Principles of High-Entropy Electrolytes in Rechargeable Batteries

Working Principles of High-Entropy Electrolytes in Rechargeable Batteries

Tuning the Nucleophilicity of Anion in Lithium Salt to Enable an Anion‐Rich Solvation Sheath for Stable Lithium Metal Batteries

Lithium Batteries Operating at Wide Temperatures: Opportunities and Challenges

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