Volume 136, Issue 41 e202401910
Forschungsartikel

Hydrogen-Bonded Organic Frameworks-based Electrolytes with Controllable Hydrogen Bonding Networks for Solid-State Lithium Batteries

Dr. Yue Wang

Dr. Yue Wang

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, 130012 P. R. China

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Dr. Li-Na Song

Dr. Li-Na Song

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, 130012 P. R. China

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Dr. Xiao-Xue Wang

Dr. Xiao-Xue Wang

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, 130012 P. R. China

International Center of Future Science, Jilin University, Changchun, 130012 P. R. China

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Dr. Yi-Feng Wang

Dr. Yi-Feng Wang

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, 130012 P. R. China

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Prof. Ji-Jing Xu

Corresponding Author

Prof. Ji-Jing Xu

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, 130012 P. R. China

International Center of Future Science, Jilin University, Changchun, 130012 P. R. China

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First published: 21 July 2024

Abstract

The lack of stable solid-state electrolytes (SSEs) with high-ionic conductivity and the rational design of electrode/electrolyte interfaces remains challenging for solid-state lithium batteries. Here, for the first time, a high-performance solid-state lithium-oxygen (Li−O2) battery is developed based on the Li-ion-conducted hydrogen-bonded organic framework (LHOF) electrolyte and the HOF-DAT@CNT composite cathode. Benefiting from the abundant dynamic hydrogen bonding network in the backbone of LHOF-DAT SSEs, fast Li+ ion transport (2.2×10−4 S cm−1), a high Li+ transference number (0.88), and a wide electrochemical window of 5.05 V are achieved. Symmetric batteries constructed with LHOF-DAT SSEs exhibit a stably cycled duration of over 1400 h with uniform deposition, which mainly stems from the jumping sites that promote a uniformly high rate of Li+ flux and the hydrogen-bonding network structure that can relieve the structural changes during Li+ transport. LHOF-DAT SSEs-based Li−O2 batteries exhibit high specific capacity (10335 mAh g−1), and stable cycling life up to 150 cycles. Moreover, the solid-state lithium metal battery with LHOF-DAT SSEs endow good rate capability (129.6 mAh g−1 at 0.5 C), long-term discharge/charge stability (210 cycles). The design of LHOF-DAT SSEs opens an avenue for the development of novel SSEs-based solid-state lithium batteries.

Conflict of Interests

The authors declare no conflict of interest.

Data Availability Statement

The data that support the findings of this study are available in the supplementary material of this article.

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