Chloro-Functionalized Ether-Based Electrolyte for High-Voltage and Stable Potassium-Ion Batteries

YY Hu and HW Fu and YH Geng and XT Yang and L Fan and J Zhou and BG Lu, ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 63, e202403269 (2024).

DOI: 10.1002/anie.202403269

Ether-based electrolyte is beneficial to obtaining good low-temperature performance and high ionic conductivity in potassium ion batteries. However, the dilute ether-based electrolytes usually result in ion- solvent co-intercalation of graphite, poor cycling stability, and hard to withstand high voltage cathodes above 4.0 V. To address the aforementioned issues, an electron-withdrawing group (chloro- substitution) was introduced to regulate the solid-electrolyte interphase (SEI) and enhance the oxidative stability of ether-based electrolytes. The dilute (similar to 0.91 M) chloro-functionalized ether-based electrolyte not only facilitates the formation of homogeneous dual halides-based SEI, but also effectively suppress aluminum corrosion at high voltage. Using this functionalized electrolyte, the K||graphite cell exhibits a stability of 700 cycles, the K||Prussian blue (PB) cell (4.3 V) delivers a stability of 500 cycles, and the PB||graphite full-cell reveals a long stability of 6000 cycles with a high average Coulombic efficiency of 99.98 %. Additionally, the PB||graphite full-cell can operate under a wide temperature range from -5 degrees C to 45 degrees C. This work highlights the positive impact of electrolyte functionalization on the electrochemical performance, providing a bright future of ether-based electrolytes application for long-lasting, wide-temperature, and high Coulombic efficiency PIBs and beyond.

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