Angewandte Chemie, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 11, 2024

Abstract Regulating lithium salt dissociation kinetics by enhancing the interaction between inorganic fillers and salts is vital for ionic conductivity in solid‐state composite polymer electrolytes (CPEs). However, influence of fillers’ external electronic environments on dynamics remains unclear. Here, we design single‐atom sites metal–organic framework poly(ethylene oxide) (PEO)‐based CPEs, boosting through an electrocatalytic strategy. This strategy enhances lithium‐ion tuning coupling strength d p orbitals fillers, as captured a newly identified descriptor ( λ ) via high‐throughput density functional theory (DFT) calculations machine learning. The optimal single atom (Ti) are incorporated into ZIF‐8 matrix PEO‐based achieving exceeding 10 −3 S cm −1 at 30 °C. Additionally, electrolyte forms robust solid interphase compatible with LiCoO 2 , LiNi 0.9 Co 0.05 Mn0.05O sulfur cathodes. Consequently, metal battery demonstrates excellent cycling stability, maintaining performance over 5000 cycles C LiFePO4 cathodes stable operation −30 These findings highlight transformative potential engineering ‐ orbital hybridization incorporating designing highly ion‐conductive CPEs.

Language: Английский