More is better: high-entropy electrolyte design in rechargeable batteries

Abstract

The field of rechargeable batteries has witnessed significant advancements driven by the increasing demand for efficient and sustainable energy technologies. As a key component of rechargeable battery systems, electrolytes play...

Working Principles of High-Entropy Electrolytes in Rechargeable Batteries

“…This will lead to a clearer classification of the HEEs. Additionally, Kang et al also argued that the concept of entropy is ambiguous, and theoretical studies of entropy need to be supported by rich and accurate calculations and modeling . More effort is required to reveal the basic physicochemical parameters and the intrinsic relationship between the phase, structure, and property variations of the different components in HEEs.…”

Entropy-Driven Hybrid Gel Electrolyte Enables Practical High-Voltage Lithium Metal Batteries

“…The high-entropy design concept, successfully applied to alloys and ceramics, leverages a magnitude of components to increase configurational entropy contribution to free energy, with the intention to yield unexpected properties that surpass those of individual components. , Herein, the solubilities of LiNO 3 and LiPO 2 F 2 are substantially improved in carbonate-based electrolytes by increasing the entropy of mixing which represents the uncertainty or disorder in mixed systems. , This yields a highly hybrid electrolyte boasting enhanced diversity in solvation structures, fostering increased interaction between salt anions and Li + (Figure ). These Li + solvation structures facilitate the preferential decomposition of numerous anions (PF 6 – , NO 3 – , and PO 2 F 2 – ) to construct protective, robust electrode–electrolyte interfaces.…”

“…24,25 Herein, the solubilities of LiNO 3 and LiPO 2 F 2 are substantially improved in carbonatebased electrolytes by increasing the entropy of mixing which represents the uncertainty or disorder in mixed systems. 26,27 This yields a highly hybrid electrolyte boasting enhanced diversity in solvation structures, fostering increased interaction between salt anions and Li + (Figure 1). These Li + solvation structures facilitate the preferential decomposition of numerous anions (PF 6 − , NO 3 − , and PO 2 F 2 − ) to construct protective, robust electrode−electrolyte interfaces.…”

Osteoporosis Failure of Aluminum Current Collector Induced Crosstalk Degradation at the Imide-Type Lithium Salt Comprised Practical-Level Lithium-Ion Batteries

“…The advancement of the electrolyte composition for the highperformance lithium secondary batteries are attempted by the new lithium salt introduction, which substitutes typical lithium hexafluorophospate (LiPF 6 ) salt. [1][2][3][4][5][6][7][8][9][10][11] The incorporation of newly designed lithium salts typically enhances the ionic conductivity and transference number of lithium ions, as well as the chemical stability of electrolytes, [12][13][14][15][16] particularly those of the imide-type lithium salts. Notably, lithium bis(fluorosulfonyl)imide (LiFSI), an imide-type salt, has garnered attention in the lithium secondary battery industry due to its facile ionic conduction and improved chemical stability at moderately high temperature compared to typical LiPF 6 salt.…”