Lanthanide Orbital Modulation Coupled With Entropy Increase Effect for Synergistically Enhanced Interfacial Stability and Ion Transport Kinetics in Halide Electrolytes.
basic_science · Level V
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- Record sourced from PubMed, PMID 42478357.
- Also identified by DOI 10.1002/adma.202523567.
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Abstract
The development of solid-state electrolytes (SSEs) integrating high ionic conductivity and a wide electrochemical window constitutes a critical challenge for all-solid-state lithium batteries (ASSLBs). Herein, we propose a multication mixing strategy of lanthanide elements, which introduces configurational entropy increase effect and electronic structure regulation into the Li<sub>3</sub>YCl<sub>6</sub>, achieving simultaneous enhancement of ion transport and oxidation resistance. Combined theoretical and experimental analyses verify that the entropy increase-driven local structural distortions effectively reduce the energy barrier for Li<sup>+</sup> migration and optimize ion-transport pathways. Concurrently, the unique electronic structure regulation of rare earth elements stabilizes the chemical environment of Cl<sup>-</sup>, significantly improving the intrinsic oxidation resistance. The full battery employing this optimized electrolyte demonstrates remarkable stability at 4.5 V, maintaining a capacity retention ratio of 74.3% after 800 cycles at 1C rate. This research provides innovative insights into designing advanced SSEs through entropy increase effect and electronic structure design.