Volume 63, Issue 48 e202409965
Research Article

A Supramolecular Deep Eutectic Electrolyte Enhancing Interfacial Stability and Solution Phase Discharge in Li−O2 Batteries

Wen Sun

Wen Sun

Beijing Key Laboratory of Environmental Science and Engineering, School of Materials Science and Engineering, Beijing Institute of Technology, 100081 Beijing, China

These authors contributed equally to this work.

Contribution: Conceptualization (lead), Data curation (lead), Formal analysis (lead), ​Investigation (lead), Supervision (lead), Writing - original draft (lead)

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Fengling Zhang

Fengling Zhang

Beijing Key Laboratory of Environmental Science and Engineering, School of Materials Science and Engineering, Beijing Institute of Technology, 100081 Beijing, China

These authors contributed equally to this work.

Contribution: Data curation (equal), Formal analysis (equal), ​Investigation (equal), Visualization (equal)

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Dr. Jingning Lai

Corresponding Author

Dr. Jingning Lai

Beijing Key Laboratory of Environmental Science and Engineering, School of Materials Science and Engineering, Beijing Institute of Technology, 100081 Beijing, China

Contribution: Conceptualization (equal), Funding acquisition (lead), Supervision (lead), Visualization (lead), Writing - review & editing (lead)

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Bohua Li

Bohua Li

Beijing Key Laboratory of Environmental Science and Engineering, School of Materials Science and Engineering, Beijing Institute of Technology, 100081 Beijing, China

Contribution: Data curation (supporting), ​Investigation (supporting), Resources (supporting)

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Xin Hu

Xin Hu

Beijing Key Laboratory of Environmental Science and Engineering, School of Materials Science and Engineering, Beijing Institute of Technology, 100081 Beijing, China

Contribution: Formal analysis (supporting), Supervision (supporting), Visualization (supporting)

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Boshun Gui

Boshun Gui

Beijing Key Laboratory of Environmental Science and Engineering, School of Materials Science and Engineering, Beijing Institute of Technology, 100081 Beijing, China

Contribution: Data curation (supporting), ​Investigation (supporting)

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Nuo Chen

Nuo Chen

Beijing Key Laboratory of Environmental Science and Engineering, School of Materials Science and Engineering, Beijing Institute of Technology, 100081 Beijing, China

Contribution: ​Investigation (supporting)

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Prof. Xingming Guo

Corresponding Author

Prof. Xingming Guo

Beijing Key Laboratory of Environmental Science and Engineering, School of Materials Science and Engineering, Beijing Institute of Technology, 100081 Beijing, China

Contribution: Project administration (equal), Supervision (equal), Validation (lead)

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Prof. Zhujie Li

Prof. Zhujie Li

Advanced Technology Research Institute, Beijing Institute of Technology, 250300 Jinan, China

Contribution: Resources (equal), Software (equal), Validation (supporting)

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Prof. Nan Chen

Prof. Nan Chen

Beijing Key Laboratory of Environmental Science and Engineering, School of Materials Science and Engineering, Beijing Institute of Technology, 100081 Beijing, China

Advanced Technology Research Institute, Beijing Institute of Technology, 250300 Jinan, China

Contribution: Funding acquisition (supporting), Project administration (supporting), Validation (supporting)

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Prof. Li Li

Prof. Li Li

Beijing Key Laboratory of Environmental Science and Engineering, School of Materials Science and Engineering, Beijing Institute of Technology, 100081 Beijing, China

Advanced Technology Research Institute, Beijing Institute of Technology, 250300 Jinan, China

Collaborative Innovation Center of Electric Vehicles in Beijing, 100081 Beijing, China

Contribution: Funding acquisition (supporting), Project administration (equal), Validation (equal)

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Prof. Feng Wu

Prof. Feng Wu

Beijing Key Laboratory of Environmental Science and Engineering, School of Materials Science and Engineering, Beijing Institute of Technology, 100081 Beijing, China

Advanced Technology Research Institute, Beijing Institute of Technology, 250300 Jinan, China

Collaborative Innovation Center of Electric Vehicles in Beijing, 100081 Beijing, China

Contribution: Funding acquisition (equal), Resources (equal), Validation (equal)

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Prof. Renjie Chen

Corresponding Author

Prof. Renjie Chen

Beijing Key Laboratory of Environmental Science and Engineering, School of Materials Science and Engineering, Beijing Institute of Technology, 100081 Beijing, China

Advanced Technology Research Institute, Beijing Institute of Technology, 250300 Jinan, China

Collaborative Innovation Center of Electric Vehicles in Beijing, 100081 Beijing, China

Contribution: Conceptualization (lead), Funding acquisition (lead), Project administration (lead), Supervision (lead), Validation (lead), Writing - review & editing (lead)

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First published: 02 September 2024
Citations: 5

Graphical Abstract

The proposed supramolecular deep eutectic electrolyte (DEE) based on LiTFSI, acetamide and boric acid, improving the oxidation voltage up to 4.5 V, and enhancing the solution phase discharge mechanism by forming Li-bonds and H-bonds with Li+ and O2. The introduction of boric acid also promotes the formation of inorganic-rich SEI, which induces Li+ uniform deposition. The Li−O2 battery with this DEE delivers ultrahigh discharge capacity, improved cycling performance and intrinsic safety.

Abstract

Li−O2 batteries (LOBs) have gained widespread recognition for their exceptional energy densities. However, a major challenge faced by LOBs is the lack of appropriate electrolytes that can effectively balance reactant transport, interfacial compatibility, and non-volatility. To address this issue, a novel supramolecular deep eutectic electrolyte (DEE) has been developed, based on synergistic interaction between Li-bonds and H-bonds through a combination of lithium salt (LiTFSI), acetamide (Ace) and boric acid (BA). The incorporation of BA serves as an interface modification additive, acting as both Li-bonds acceptor and H-bonds donor/acceptor, thereby enhancing the redox stability of the electrolyte, facilitating a solution phase discharge process and improving compatibility with the Li anode. Our proposed DEE demonstrates a high oxidation voltage of 4.5 V, an ultrahigh discharge capacity of 15225 mAh g−1 and stable cycling performance of 196 cycles in LOBs. Additionally, the intrinsic non-flammability and successful operation of a Li−O2 pouch cell indicate promising practical applications of this electrolyte. This research broadens the design possibilities for LOBs electrolytes and provides theoretical insights for future studies.

Conflict of Interests

The authors declare no conflict of interest.

Data Availability Statement

The data that support the findings of this study are available from the corresponding author upon reasonable request.

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