A Liquid/Liquid Electrolyte Interface that Inhibits Corrosion and Dendrite Growth of Lithium in Lithium‐Metal Batteries

Abstract

A proof‐of‐concept study on a liquid/liquid (L/L) two‐phase electrolyte interface is reported by using the polarity difference of solvent for the protection of Li‐metal anode with long‐term operation over 2000 h. The L/L electrolyte interface constructed by non‐polar fluorosilicane (PFTOS) and conventionally polar dimethyl sulfoxide solvents can block direct contact between conventional electrolyte and Li anode, and consequently their side reactions can be significantly eliminated. Moreover, the homogeneous Li‐ion flow and Li‐mass deposition can be realized by the formation of a thin and uniform solid‐electrolyte interphase (SEI) composed of LiF, LixC, LixSiOy between PFTOS and Li anode, as well as the super‐wettability state of PFTOS to Li anode, resulting in the suppression of Li dendrite formation. The cycling stability in a lithium–oxygen battery as a model is improved 4 times with the L/L electrolyte interface.

Development and Challenges of Biphasic Membrane‐Less Redox Batteries

“…it enabled a wider potential range for the stripping/plating of lithium metal. As a result, the proposed battery exhibited a high voltage of 3.47 V. Similar examples are also found in metal air batteries, [ 101 ] the non‐polar electrolyte (perfluorooctyltrimethoxysilane, PFTOS) and the polar one (dimethyl sulfoxide, DMSO) were applied to build two‐phase electrolyte interface, which could block the direct contact between Li‐metal electrode and the electrolyte to form a super‐wettability state of PFTOS to Li anode, resulting in the suppression of Li dendrite growth, thereby significantly improving the cycle life of the battery.…”

Starving Free Solvents: Toward Immiscible Binary Liquid Electrolytes for Li‐Metal Full Cells

“…However, ensuring that the two liquid electrolytes in the binary electrolytes do not mix is a significant challenge. To address this issue, several approaches have been explored, including the introduction of solid electrolyte interlayers [14,15] or thick glass fiber membranes [16,17] between the two liquid electrolytes, and the gelation of liquid electrolytes. [18][19][20] However, these approaches often encounter an unwanted increase in the thickness of the solid electrolyte interlayers, glass fiber membranes, and gel electrolytes and interfacial contact resistance between heterolayers, as well as a decrease in the bulk ionic conduction, which result in the loss of energy densities, rate capability, and cycling retention of resulting cells.…”

Regulating the Architecture of a Solid Electrolyte Interface on a Li-Metal Anode of a Li–O2 Battery by a Dithiobiuret Additive

“…Exploring a suitable additive for Li-metal in the O 2 environment for Li–O 2 cells is extremely urgent. It has been potentially regarded as an effective solution by regulating the distribution state between solvent molecules and the lithium salt in the Li + solvated sheath configuration, in order to effectively induce an antioxidative (against oxygen, high stability, not easily decomposed) SEI film architecture and obtain dendrite-free morphology. ,,,− …”