Boosting the interfacial superionic conduction of halide solid electrolytes for all-solid-state batteries

Hiram Kwak, Jae-Seung Kim, Daseul Han, Jong Seok Kim, Juhyoun Park, Gihan Kwon, Seong-Min Bak, Unseon Heo, Changhyun Park, Hyun-Wook Lee, Kyung-Wan Nam (), Dong-Hwa Seo () and Yoon Seok Jung ()
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Hiram Kwak: Yonsei University
Jae-Seung Kim: Ulsan National Institute of Science and Technology (UNIST)
Daseul Han: Dongguk University
Jong Seok Kim: Yonsei University
Juhyoun Park: Yonsei University
Gihan Kwon: Brookhaven National Laboratory
Seong-Min Bak: Brookhaven National Laboratory
Unseon Heo: Dongguk University
Changhyun Park: Ulsan National Institute of Science and Technology (UNIST)
Hyun-Wook Lee: Ulsan National Institute of Science and Technology (UNIST)
Kyung-Wan Nam: Dongguk University
Dong-Hwa Seo: Ulsan National Institute of Science and Technology (UNIST)
Yoon Seok Jung: Yonsei University

Nature Communications, 2023, vol. 14, issue 1, 1-14

Abstract: Abstract Designing highly conductive and (electro)chemical stable inorganic solid electrolytes using cost-effective materials is crucial for developing all-solid-state batteries. Here, we report halide nanocomposite solid electrolytes (HNSEs) ZrO2(-ACl)-A2ZrCl6 (A = Li or Na) that demonstrate improved ionic conductivities at 30 °C, from 0.40 to 1.3 mS cm−1 and from 0.011 to 0.11 mS cm−1 for Li+ and Na+, respectively, compared to A2ZrCl6, and improved compatibility with sulfide solid electrolytes. The mechanochemical method employing Li2O for the HNSEs synthesis enables the formation of nanostructured networks that promote interfacial superionic conduction. Via density functional theory calculations combined with synchrotron X-ray and 6Li nuclear magnetic resonance measurements and analyses, we demonstrate that interfacial oxygen-substituted compounds are responsible for the boosted interfacial conduction mechanism. Compared to state-of-the-art Li2ZrCl6, the fluorinated ZrO2−2Li2ZrCl5F HNSE shows improved high-voltage stability and interfacial compatibility with Li6PS5Cl and layered lithium transition metal oxide-based positive electrodes without detrimentally affecting Li+ conductivity. We also report the assembly and testing of a Li-In||LiNi0.88Co0.11Mn0.01O2 all-solid-state lab-scale cell operating at 30 °C and 70 MPa and capable of delivering a specific discharge of 115 mAh g−1 after almost 2000 cycles at 400 mA g−1.

Date: 2023
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DOI: 10.1038/s41467-023-38037-z

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