Ab initio calculations of the atomic and electronic structures of crystalline PEO3:LiCF3SO3 electrolytes

Abstract

The PEO3:LiCF3SO3 polymer electrolyte has attracted significant research due to its enhanced stability at the lithium/polymer interface of high conductivity polymer batteries. Experimental studies have shown that, depending on the preparation conditions, both the PEO3:LiCF3SO3 crystalline complex and the PEO3:LiCF3SO3 amorphous phase can be formed. However, previous theoretical investigations focused on the short chain amorphous PEO3:LiCF3SO3 system. We report ab initio density-functional-theory calculations of crystalline PEO3:LiCF3SO3. The calculated results about the bonding configuration, electronic structures, and conductivity properties are in good agreement with the experimental measurements.

Composite electrolyte with polyethylene oxide and metal–organic framework for lithium‐ion conduction

“…17 PEO 3 is another type of polymer-salt cocrystal, where one helical polymer chain, with conformation similar to PEO, intertwines with a chain of alternating anions and cations. [66][67][68] In PEO 3 , each lithium-ion coordinates with three ether oxygens in a single turn of the PEO helix and two anions, which bridge two consecutive lithium ions, thus forming an ion chain. 67 The formation of PEO 3 at 6:1 composition (y = 6) came as a surprise because PEO 3 typically forms in the range of 2 < y < 6 in PEO y /LiClO 4 (Figure S1).…”

“…The peak positions at 2 θ = 11.3°and 12.2° in XRD (Figure 6A) suggested the formation of PEO 3 along with PEO 6 in the unfilled electrolyte 17 . PEO 3 is another type of polymer‐salt cocrystal, where one helical polymer chain, with conformation similar to PEO, intertwines with a chain of alternating anions and cations 66–68 . In PEO 3 , each lithium‐ion coordinates with three ether oxygens in a single turn of the PEO helix and two anions, which bridge two consecutive lithium ions, thus forming an ion chain 67 .…”

High ionic conductivity materials Li3YBr6 and Li3LaBr6 for solid-state batteries: first-principles calculations

“…However, the low ionic conductivity of the solid-state electrolyte at room temperature is challenging. Numerous research focus on finding high ionic conductivity materials for solid-state electrolyte batteries [9][10][11][12][13][14][15][16].…”