Liquid-Phase Synthesis of Highly Deformable and Air-Stable Sn-Substituted Li3PS4 for All-Solid-State Batteries Fabricated and Operated under Low Pressures

Jehoon Woo, Yong Bae Song, Hiram Kwak, Seunggoo Jun, Bo Yeong Jang, Juhyoun Park, Kyu Tae Kim, Changhyun Park, Chanhee Lee, Kern Ho Park, Hyun Wook Lee, Yoon Seok Jung

Research output: Contribution to journalArticlepeer-review


The liquid-phase synthesis (LS) of sulfide solid electrolytes (SEs) has promising potential for mass production of practical all-solid-state Li batteries (ASLBs). However, their accessible SE compositions are mostly metal-free. Moreover, liquid-phase-synthesized-SEs (LS-SEs) suffer from high electronic conductivity due to carbon impurities, resulting in below-par electrochemical performance of ASLBs. Here, the LS of highly deformable and air-stable Li3+xP1-xSnxS4 (0.19 mS cm−1) using 1,2-ethylene diamine-1,2-ethanedithiol with tetrahydrofuran is reported. A low heat-treatment temperature (260 °C) prevents the carbonization of organic residues. Importantly, a remarkable enhancement in the deformability of LS-SEs compared to that of conventional solid-state-synthesized SEs (SS-SEs) is identified for the first time. LiNi0.7Co0.15Mn0.15O2 electrodes employing LS-SEs in ASLBs significantly outperform those using SS-SEs, notably when assembled under a low fabricating pressure (148 vs 370 MPa, e.g., capacity loss: 2 vs 41 mA h g−1) or tested under a low operating pressure (12 or 3 MPa), which is attributed to reduced electrochemo-mechanical effects. Finally, when employing SEs that are exposed to air (dew point of −20 °C), LiNi0.7Co0.15Mn0.15O2 electrodes employing SEs with Sn-substituted composition or prepared by LS exhibit significantly better capacity retention than conventional SEs with Sn-free composition or prepared by SS (e.g., 92.2% for LS-Li3.2P0.8Sn0.2S4 vs 32.5% for SS-Li3PS4).

Original languageEnglish
Article number2203292
JournalAdvanced Energy Materials
Issue number8
Publication statusPublished - 2023 Feb 24

Bibliographical note

Funding Information:
This work was supported by the program of phased development of carbon neutral technologies through the National Research Foundation of Korea (NRF), funded by the Ministry of Science and ICT (NRF‐2022M3J1A1085397), and the Korea Institute of Energy Technology Evaluation and Planning (KETEP) grant funded by the Ministry of Trade, Industry & Energy (No. 20007045 and 20214000000320). The work was also funded by the Yonsei University Research Fund of 2021 (2021‐22‐0326).

Publisher Copyright:
© 2022 Wiley-VCH GmbH.

All Science Journal Classification (ASJC) codes

  • Renewable Energy, Sustainability and the Environment
  • Materials Science(all)


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