Solvent–Binder Engineering for a Practically Viable Solution Process for Fabricating Sulfide-Based All-Solid-State Batteries

The commercial viability of sulfide all-solid-state batteries (ASSBs) has been hindered by limited solvent compatibility in solution processing as sulfide solid electrolytes (SEs) degrade in polar solvents. This constraint significantly restricts binder selection, which is critical for both performance─particularly at low pressures─and processability. This study addresses this critical issue by investigating thermoplastic polyurethane (TPU) as a binder dissolved in 1,6-dichlorohexane (DCH), a solvent specifically tailored for sulfide ASSBs. TPU demonstrates outstanding adhesion properties in composite anode, cathode, and SE layers, which not only enhance the long-term cycling performance but also enable double-cast solution processing with minimal binder content for electrode-SE layer manufacturing. A silicon-graphite (Si-Gr)-based pouch-cell fabricated through this solution process maintained 80% capacity retention over 100 cycles under practical conditions (40 μm SE layer, 25 °C, and 2 MPa), validating its practical feasibility. The successful implementation of this optimized solvent–binding system for solution processing represents a significant advancement toward practical ASSB technologies.

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Institutions

Publication Details

Journal
ACS Energy Letters
Published
2025-05-17
DOI
https://doi.org/10.1021/acsenergylett.5c00762
Citations
12
Primary Topic
Advanced Battery Materials and Technologies
Type
article
Field-Weighted Citation Impact
8.77

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article

Solvent–Binder Engineering for a Practically Viable Solution Process for Fabricating Sulfide-Based All-Solid-State Batteries

Taeyong Lee, Seung Ho Choi, Inwoo Kim, Jihoon Oh et al.
12 citations
ACS Energy Letters
Advanced Battery Materials and Technologies
8.77
article

Solvent–Binder Engineering for a Practically Viable Solution Process for Fabricating Sulfide-Based All-Solid-State Batteries

Taeyong Lee, Seung Ho Choi, Inwoo Kim, Jihoon Oh, Dong-Ok Kim, Jang Wook Choi, Jieun Lee, Dong‐Hoon Kim, Heejin Kim, Minkwan Kim, Woo Jun Chung, Sun-ung Moon
article en
12 citations

Abstract

The commercial viability of sulfide all-solid-state batteries (ASSBs) has been hindered by limited solvent compatibility in solution processing as sulfide solid electrolytes (SEs) degrade in polar solvents. This constraint significantly restricts binder selection, which is critical for both performance─particularly at low pressures─and processability. This study addresses this critical issue by investigating thermoplastic polyurethane (TPU) as a binder dissolved in 1,6-dichlorohexane (DCH), a solvent specifically tailored for sulfide ASSBs. TPU demonstrates outstanding adhesion properties in composite anode, cathode, and SE layers, which not only enhance the long-term cycling performance but also enable double-cast solution processing with minimal binder content for electrode-SE layer manufacturing. A silicon-graphite (Si-Gr)-based pouch-cell fabricated through this solution process maintained 80% capacity retention over 100 cycles under practical conditions (40 μm SE layer, 25 °C, and 2 MPa), validating its practical feasibility. The successful implementation of this optimized solvent–binding system for solution processing represents a significant advancement toward practical ASSB technologies.

ACS Energy LettersVol. 10(6)
Seoul National University (KR), Hyundai Motor Group (South Korea) (KR), Energy Storage Systems (United States) (US), Bio Pharm Dongsung (South Korea) (KR), Korea Electronics Technology Institute (KR), Korea Basic Science Institute (KR), Korea Institute of Science and Technology (KR)
Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung, Korea Institute of Machinery and Materials, National Research Foundation of Korea, Institute of Engineering Research, Seoul National University
Openalex Percentile: Top 2%
Advanced Battery Materials and Technologies
8.77
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