High Configuration Entropy Promises Electrochemical Stability of Chloride Electrolytes for High-Energy, Long-Life All-Solid-State Batteries.

Angew Chem Int Ed Engl

Tianjin Key Laboratory of Advanced Carbon and Electrochemical Energy Storage, School of Chemical Engineering and Technology, Tianjin University, Tianjin, 300350, China.

Published: October 2024

AI Article Synopsis

  • High-entropy solid-state electrolytes (HE-SSEs) show enhanced ionic conductivity and electrochemical stability, crucial for developing efficient all-solid-state batteries (ASSBs).
  • The study demonstrates that HE-SSE (LiInZrScErYCl) maintains high voltage stability, achieving 250 cycles with 81.4% capacity retention at 4.8V and 5000 cycles at 4.6V.
  • Findings suggest that the high entropy design effectively reduces high-voltage degradation at the interface, providing a promising approach to improve both stability and conductivity in solid-state batteries.

Article Abstract

Solid-state electrolytes (SSEs) with high ionic conductivity, stability, and interface compatibility are indispensable for high-energy-density and long-life all-solid-state batteries (ASSBs), yet there are scarce SSEs with sufficient ionic conductivity and electrochemical stability. In this study, with a high-entropy SSE (HE-SSE, LiInZrScErYCl), we show the high configuration entropy has a thermodynamically positive relationship with the high-voltage stability. As a result, the ASSBs with HE-SSE and high-voltage cathode materials exhibit superior high-voltage and long-cycle stability, achieving 250 cycles with 81.4 % capacity retention when charged to 4.8 V (vs. Li/Li), and even 5000 cycles if charged to 4.6 V (vs. Li/Li). Experimental characterizations and density functional theory calculations confirm that the HE-SSE greatly suppresses the high-voltage degradation of SSE at the interface, promoting the high-voltage stability coordinately through high entropy and interface stability. The high entropy design offers a general strategy to simultaneously improve the high-voltage stability and ionic conductivity of SSEs, creating an avenue to building high-energy and long-life ASSBs.

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Source
http://dx.doi.org/10.1002/anie.202419735DOI Listing

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