Ultralow-Temperature Li/CF<sub>x</sub> Batteries Enabled by Fast-Transport and Anion-Pairing Liquefied Gas Electrolytes.

Yin, Yijie; Holoubek, John; Liu, Alex; Sayahpour, Baharak; Raghavendran, Ganesh; Cai, Guorui; Han, Bing; Mayer, Matthew et al. · Adv Mater · 2023

basic_science · Level V

Where this comes from

Abstract

Lithium fluorinated-carbon (Li/CF<sub>x</sub> ) is one of the most promising chemistries for high-energy-density primary energy-storage systems in applications where rechargeability is not required. Though Li/CF<sub>x</sub> demonstrates high energy density (>2100 Wh kg<sup>-1</sup> ) under ambient conditions, achieving such a high energy density when exposed to subzero temperatures remains a challenge, particularly under high current density. Here, a liquefied gas electrolyte with an anion-pair solvation structure based on dimethyl ether with a low melting point (-141 °C) and low viscosity (0.12 mPa s, 20 °C), leading to high ionic conductivity (>3.5 mS cm<sup>-1</sup> ) between -70 and 60 °C is reported. Besides that, through systematic X-ray photoelectron spectroscopy integrated with transmission electron microscopy characterizations, the interface of CF<sub>x</sub> is evaluated for low-temperature performance. The fast transport and anion-pairing solvation structure of the electrolyte are concluded to bring about reduced charge-transfer resistance at low temperatures, which results in significantly enhanced performance of Li/CF<sub>x</sub> cells (1690 Wh kg<sup>-1</sup> , -60 °C based on active materials). Utilizing 50 mg cm<sup>-2</sup> loading electrodes, the Li/CF<sub>x</sub> still displays 1530 Wh kg<sup>-1</sup> at -60 °C. This work provides insights into the electrolyte design that may overcome the operational limits of batteries in extreme environments.