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Published on: August 12, 2013
Fluorinated Deep Eutectic Gel Electrolytes for Sustainable Lithium Metal Batteries
Tongrui Zhang1, Jiangtao Yu1, Tianxing Lin1
1Frontiers Science Center for New Organic Matter, State Key Laboratory of Advanced Chemical Power Sources, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), State Key Laboratory of Elemonto-organic Chemistry, Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Academy of Advanced Interdisciplinary Studies, College of Chemistry, Nankai University, Tianjin 300071, P. R. China.
Fluorinated amides in deep eutectic gel electrolytes (DEGEs) enhance lithium metal battery stability by forming robust solid electrolyte interphase (SEI) layers. This innovation improves battery lifespan and safety, paving the way for advanced energy storage solutions.
Area of Science:
- Materials Science
- Electrochemistry
- Energy Storage
Background:
- Deep eutectic gel electrolytes (DEGEs) offer high ionic conductivity and tunable interactions for lithium metal batteries (LMBs).
- Achieving high interfacial stability between DEGEs and lithium metal remains a significant challenge.
- Fluorinated compounds are explored to enhance electrolyte performance and stability.
Purpose of the Study:
- To develop novel DEGEs using fluorinated amides for improved interfacial stability in LMBs.
- To investigate the role of fluorine's electron-withdrawing effects on amide LUMO energy levels and Li+ binding.
- To establish a screening criterion for optimizing DEGEs based on LUMO levels and desolvation barriers.
Main Methods:
- Synthesis and characterization of a series of DEGEs based on fluorinated amides.
- Computational screening integrating amide LUMO energy levels and Li+ desolvation energy barriers.
- Electrochemical testing of symmetric Li||Li and Li||LiFePO4 batteries utilizing the developed DEGEs.
Main Results:
- 2,2,2-trifluoro-N-methylacetamide (C═Oα3F) based DEGE showed the lowest LUMO energy and desolvation barrier.
- C═Oα3F-DEGE facilitated uniform, robust SEI layers (LiF, Li3N) and synergistic solvent-anion-derived SEI mechanisms.
- The electrolyte exhibited nonflammability, high ionic conductivity (1.24 mS cm⁻¹), and enabled over 9000 h of stable cycling in Li||Li batteries.
- Li||LiFePO4 batteries demonstrated a 2500-cycle lifespan with 81.7% capacity retention.
Conclusions:
- Fluorinated amides, particularly C═Oα3F, significantly enhance interfacial stability and performance in DEGEs for LMBs.
- The proposed bidirectional screening criterion effectively guides the development of high-performance DEGEs.
- These findings offer valuable insights for designing advanced electrolytes for safer and more durable lithium metal batteries.
