High-entropy solvent design enabling a universal electrolyte with a low freezing point for low-temperature aqueous batteries

Abstract

The amide additives acting as hydrogen-bonding ligands effectively break the cross-linking structures between water molecules and increase the entropy of mixed solvents, thus enabling the mixed solvent with an ultralow...

Formation of Polymer-like Nanochains with Short Lithium–Lithium Distances in a Water-in-Salt Electrolyte

“…In future studies of WiS systems, we encourage taking into account this effect either by reparameterization of classical force fields or by the use of machine-learning potentials. Future works should track the existence of similar effects in other ion-concentrated liquids, such as localized high-concentration electrolytes , or high entropy electrolytes − that have recently been introduced. The high impact of the presence of polymeric species on the interfacial properties is also to be expected since the concentration of ionic species within the electrochemical double-layer is known to drastically change the local reactivity, such as the formation of dendrites at the metal anodes.…”

Working Principles of High-Entropy Electrolytes in Rechargeable Batteries

“…However, there are some discrepancies in the definition and claim of high entropy. Wang et al 63 designed the mixed solvents of acetamide−water or formamide−water. The operating temperature range of zinc ion batteries with such mixed solvents was extended to −60 to 50 °C because of the increasing system entropy and destroyed water cross-linking structures.…”

Tuning of Molecular Water Organization in Water-in-Salt Electrolytes by Addition of Chaotropic Ionic Liquids

“…While the effects of chaotropic ions on the HBN and the macroscopic consequences of such interactions are still unclear, the importance of chaotropicity in the reactivity of aqueous electrolytes has clearly been demonstrated. 28,31,32 Recently, ILs have been used in a few formulations of hybrid WISEs for LIBs. In all those investigations, a combination of a nonflammable IL with a WISE has been proposed to both reduce the H 2 O activity and to improve the ionic conductivity.…”

“…Recently, different groups have developed cosalts of “high-entropy” aqueous electrolytes, leading to desolvation processes caused by the presence of hydrophobic cations at the electrode–electrolyte interface. , However, we anticipate distinct roles for entropic and chaotropic effects in solution, with the primary focus of this article being on the latter. While the effects of chaotropic ions on the HBN and the macroscopic consequences of such interactions are still unclear, the importance of chaotropicity in the reactivity of aqueous electrolytes has clearly been demonstrated. ,, …”