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Multifunctional Subnanowires Modulating In Situ Polymerization for High-Voltage Solid-State Batteries.
Haoran Xu1, Hong Zhang1, Wei Peng1
1State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, School of Materials Science and Engineering, Wuhan University of Technology, Wuhan 430070, China.
ACS Applied Materials & Interfaces
|May 30, 2025
Summary
Subnanowires enhance poly(1,3-dioxolane) (PDOL) electrolytes for lithium metal batteries (LMBs). This strategy improves oxidative stability, enabling high-voltage applications and better battery performance.
Area of Science:
- Materials Science
- Electrochemistry
- Polymer Chemistry
Background:
- In situ polymerized poly(1,3-dioxolane) (PDOL) electrolytes offer good interfacial contact but suffer from limited oxidative stability, restricting their use with high-voltage cathodes in lithium metal batteries (LMBs).
- Developing electrolytes with enhanced oxidative stability is crucial for advancing high-performance LMBs.
Purpose of the Study:
- To improve the oxidative stability of in situ polymerized PDOL electrolytes by modulating their molecular weight distribution (MWD).
- To introduce a novel strategy using multifunctional subnanowires (SNWs) to control PDOL polymerization and enhance electrolyte performance.
Main Methods:
- Utilized multifunctional subnanowires (SNWs) to promote and regulate the ring-opening polymerization of 1,3-dioxolane (DOL).
- Leveraged oxygen vacancies (Ov) and protonated oleylamine (PO) on SNWs to enhance monomer conversion, control polymerization speed, and facilitate lithium salt dissociation.
- Characterized the resulting PDOL electrolytes for their MWD, oxidative stability, and ionic conductivity.
Main Results:
- Achieved a narrow MWD of 1.42 in PDOL electrolytes through the SNW-induced polymerization strategy.
- Demonstrated superior oxidative stability exceeding 5.1 V for the modified PDOL electrolytes.
- Obtained a high lithium-ion transference number of 0.81, indicating efficient ion transport.
- NCM811||Li cells using these electrolytes maintained stable operation for 100 cycles at 4.5 V with 89.2% capacity retention.
Conclusions:
- The molecular weight modulation strategy using SNWs effectively enhances the oxidative stability of in situ polymerized PDOL electrolytes.
- This approach provides a unique pathway for developing advanced electrolytes for high-voltage lithium metal batteries.
- The findings offer significant potential for the next generation of high-performance and stable energy storage devices.
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