Solid‐state electrolyte materials are attractive options for meeting the safety and performance needs of advanced lithium‐based rechargeable battery technologies because of their improved mechanical and thermal stability compared to liquid electrolytes. However, there is typically a tradeoff between mechanical and electrochemical performance. Here an elastic Li‐ion conductor with dual covalent and dynamic hydrogen bonding crosslinks is described to provide high mechanical resilience without sacrificing the room‐temperature ionic conductivity. A solid‐state lithium‐metal/LiFePO4cell with this resilient electrolyte can operate at room temperature with a high cathode capacity of 152 mAh g−1for 300 cycles and can maintain operation even after being subjected to intense mechanical impact testing. This new dual crosslinking design provides robust mechanical properties while maintaining ionic conductivity similar to state‐of‐the‐art polymer‐based electrolytes. This approach opens a route toward stable, high‐performance operation of solid‐state batteries even under extreme abuse.
The emergence of wearable electronics puts batteries closer to the human skin, exacerbating the need for battery materials that are robust, highly ionically conductive, and stretchable. Herein, we introduce a supramolecular design as an effective strategy to overcome the canonical tradeoff between mechanical robustness and ionic conductivity in polymer electrolytes. The supramolecular lithium ion conductor utilizes orthogonally functional H-bonding domains and ion-conducting domains to create a polymer electrolyte with unprecedented toughness (29.3 MJ m−3) and high ionic conductivity (1.2 × 10−4S cm−1at 25 °C). Implementation of the supramolecular ion conductor as a binder material allows for the creation of stretchable lithium-ion battery electrodes with strain capability of over 900% via a conventional slurry process. The supramolecular nature of these battery components enables intimate bonding at the electrode-electrolyte interface. Combination of these stretchable components leads to a stretchable battery with a capacity of 1.1 mAh cm−2that functions even when stretched to 70% strain. The method reported here of decoupling ionic conductivity from mechanical properties opens a promising route to create high-toughness ion transport materials for energy storage applications.
more » « less- NSF-PAR ID:
- 10153769
- Publisher / Repository:
- Nature Publishing Group
- Date Published:
- Journal Name:
- Nature Communications
- Volume:
- 10
- Issue:
- 1
- ISSN:
- 2041-1723
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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