Volume 135, Issue 35 e202306948
Forschungsartikel

Supramolecular Polymer Ion Conductor with Weakened Li Ion Solvation Enables Room Temperature All-Solid-State Lithium Metal Batteries

Dr. Hang-Yu Zhou

Dr. Hang-Yu Zhou

Department of Chemical Engineering, Tsinghua University, Beijing, 100084 China

National Academy of Safety Science and Engineering, China Academy of Safety Science and Technology, Beijing, 100012 China

Contribution: Data curation (lead), Formal analysis (lead), ​Investigation (lead), Methodology (lead), Writing - original draft (lead), Writing - review & editing (lead)

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Yu Ou

Yu Ou

Department of Chemical Engineering, Tsinghua University, Beijing, 100084 China

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

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Shuai-Shuai Yan

Shuai-Shuai Yan

Department of Chemical Engineering, Tsinghua University, Beijing, 100084 China

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

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Dr. Jin Xie

Dr. Jin Xie

Department of Chemical Engineering, Tsinghua University, Beijing, 100084 China

Contribution: Data curation (supporting)

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Pan Zhou

Pan Zhou

Department of Chemical Engineering, Tsinghua University, Beijing, 100084 China

Contribution: Data curation (supporting)

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Lei Wan

Lei Wan

Department of Chemical Engineering, Tsinghua University, Beijing, 100084 China

Contribution: Data curation (supporting)

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Zi-Ang Xu

Zi-Ang Xu

Department of Chemical Engineering, Tsinghua University, Beijing, 100084 China

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

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Dr. Feng-Xiang Liu

Dr. Feng-Xiang Liu

Department of Chemical Engineering, Tsinghua University, Beijing, 100084 China

Contribution: Data curation (supporting), Formal analysis (supporting)

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Dr. Wei-Li Zhang

Dr. Wei-Li Zhang

Department of Chemical Engineering, Tsinghua University, Beijing, 100084 China

Contribution: Data curation (supporting)

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Dr. Yin-Chun Xia

Dr. Yin-Chun Xia

Department of Chemical Engineering, Tsinghua University, Beijing, 100084 China

Contribution: Data curation (supporting)

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Prof. Kai Liu

Corresponding Author

Prof. Kai Liu

Department of Chemical Engineering, Tsinghua University, Beijing, 100084 China

Contribution: Conceptualization (lead), Supervision (lead), Writing - review & editing (lead)

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First published: 05 July 2023
Citations: 5

Abstract

Improved durability, enhanced interfacial stability, and room temperature applicability are desirable properties for all-solid-state lithium metal batteries (ASSLMBs), yet these desired properties are rarely achieved simultaneously. Here, in this work, it is noticed that the huge resistance at Li metal/electrolyte interface dominantly impeded the normal cycling of ASSLMBs especially at around room temperature (<30 °C). Accordingly, a supramolecular polymer ion conductor (SPC) with “weak solvation” of Li+ was prepared. Benefiting from the halogen-bonding interaction between the electron-deficient iodine atom (on 1,4-diiodotetrafluorobenzene) and electron-rich oxygen atoms (on ethylene oxide), the O-Li+ coordination was significantly weakened. Therefore, the SPC achieves rapid Li+ transport with high Li+ transference number, and importantly, derives a unique Li2O-rich SEI with low interfacial resistance on lithium metal surface, therefore enabling stable cycling of ASSLMBs even down to 10 °C. This work is a new exploration of halogen-bonding chemistry in solid polymer electrolyte and highlights the importance of “weak solvation” of Li+ in the solid-state electrolyte for room temperature ASSLMBs.

Conflict of interest

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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