2020
DOI: 10.1021/acsami.9b20436
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Single Lithium-Ion Conducting Solid Polymer Electrolyte with Superior Electrochemical Stability and Interfacial Compatibility for Solid-State Lithium Metal Batteries

Abstract: Lithium metal batteries are being explored in meeting ever-increasing energy density needs. Because of serious dendritic lithium issues in liquid-state electrolytes, it is generally thought that solid-state electrolytes are potential alternatives for lithium metal batteries. Herein, we design a new single lithium-ion conducting lithium poly­[(cyano)­(4-styrenesulfonyl)­imide] (LiPCSI) to replace the conventional dual-ion conducting salt for use in solid polymer electrolytes (SPEs) that successfully suppress th… Show more

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Cited by 99 publications
(66 citation statements)
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“…Lithium poly[(cyano)(4‐styrenesulfonyl)imide] (LiPCSI) comprising highly delocalized anions and antioxidant cyano groups was designed and synthesized, which was dispersed in PEO to construct a free‐standing and flexible electrolyte membrane (Figure 5c). [ 79 ] By optimizing the ratio of Li ions and ethylene oxide units (Li + /EO), high ionic conductivity of 7.33 × 10 −5 S cm −1 at 60 °C was obtained at EO/Li + = 8. This was ascribed to the strong electron‐withdrawing cyano groups in this PSE, which promoted anionic delocalization and thus liberation of lithium ions.…”
Section: Pses With An Architecturally Engineered Polymer Matrixmentioning
confidence: 99%
“…Lithium poly[(cyano)(4‐styrenesulfonyl)imide] (LiPCSI) comprising highly delocalized anions and antioxidant cyano groups was designed and synthesized, which was dispersed in PEO to construct a free‐standing and flexible electrolyte membrane (Figure 5c). [ 79 ] By optimizing the ratio of Li ions and ethylene oxide units (Li + /EO), high ionic conductivity of 7.33 × 10 −5 S cm −1 at 60 °C was obtained at EO/Li + = 8. This was ascribed to the strong electron‐withdrawing cyano groups in this PSE, which promoted anionic delocalization and thus liberation of lithium ions.…”
Section: Pses With An Architecturally Engineered Polymer Matrixmentioning
confidence: 99%
“…Li + ions can migrate from one anion group to another without the aid of segmental motion. [ 218 ] Also, Zhang and co‐workers developed lithium poly((4‐styrenesulfonyl) (trifluoromethanesulfonyl) imide) polysalts in PEO that are highly cationic conductive ( t Li + = 0.63) because only Li + ions located in the TFSI groups can easily jump between anion groups due to the low dissociation energy of Li + and high structural flexibility (Figure 9d). [ 219 ] The ion transfer mechanism of polymer electrolytes is still unclear and requires more research; however, these theories will be essential for the design of new electrolyte membranes with high σ.…”
Section: Spes For Li‐based Secondary Batteriesmentioning
confidence: 99%
“…[ 49–51 ] Besides, according to computational and experimental studies, SSEs with high t Li + s would benefit LMBs, help stabilize the electrodeposition process, and reduce concentration gradients. [ 52,53 ] Therefore, with cationic transference numbers close to unity combined with their intrinsic flexibility and processability, SICPEs may be an ideal SSE candidate for LMBs, achieving next‐generation energy storage devices with high‐energy density, improved safety, and prolonged lifetime. [ 54,55 ]…”
Section: Introductionmentioning
confidence: 99%