Three-dimensional networking binders prepared in situ during wet-slurry process for all-solid-state batteries operating under low external pressure

Tae Young Kwon, Kyu Tae Kim, Dae Yang Oh, Yong Bae Song, Seunggoo Jun, Yoon Seok Jung

Research output: Contribution to journalArticlepeer-review

8 Citations (Scopus)


For all-solid-state Li batteries (ASLBs), the external operating pressure offsets the detrimental electrochemo-mechanical effects. In this work, a new scalable in situ protocol to reinforce binders for sulfide-electrolyte-based ASLBs operating under low or no external pressures is reported. The vulcanization of butadiene rubber (BR) using elemental sulfur proceeds in situ during the wet-slurry fabrication process for electrodes, forming a mechanically resilient crosslinked structure. The electrochemical performance of LiNi0.70Co0.15Mn0.15O2 electrodes fabricated using pristine or vulcanized BR diverge significantly as the operating pressure is lowered from 70 MPa to a practically acceptable value of 2 MPa. Complementary analysis using cross-sectional scanning electron microscopy and operando electrochemical pressiometry measurements confirms that the vulcanization of BR suppresses the electrochemo-mechanical degradation of electrodes, which suggests that the scaffolding structure of the vulcanized BR helps maintain the microstructural integrity of the electrodes upon charge and discharge. The significantly enhanced performance of the vulcanized BR is also demonstrated for pouch-type LiNi0.70Co0.15Mn0.15O2/Li4Ti5O12 full cells operated under no external pressure (reversible capacity of 121 vs. 150 mA h g−1 at 0.2C for electrodes with pristine vs. vulcanized BR, respectively).

Original languageEnglish
Pages (from-to)219-226
Number of pages8
JournalEnergy Storage Materials
Publication statusPublished - 2022 Aug

Bibliographical note

Funding Information:
This work was supported by the Technology Development Program to Solve Climate Changes and by the Basic Science Research Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Science, ICT & Future Planning (NRF-2018R1A2B6004996 and 2017M1A2A2044501), and by the Technology Innovation Program (20007045 and 20012216) funded by the Ministry of Trade, Industry & Energy (MOTIE, Korea). The work was also funded by the Yonsei University Research Fund of 2021 (2021-22-0326).

Publisher Copyright:
© 2022 Elsevier B.V.

All Science Journal Classification (ASJC) codes

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


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