Volume 61, Issue 2 e202113086
Research Article

Eutectic Crystallization Activates Solid-State Zinc-Ion Conduction

Huayu Qiu

Huayu Qiu

College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao, 266042 China

Qingdao Industrial Energy Storage Research Institute, Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao, 266101 China

These authors contributed equally to this work.

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Rongxiang Hu

Rongxiang Hu

College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao, 266042 China

Qingdao Industrial Energy Storage Research Institute, Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao, 266101 China

These authors contributed equally to this work.

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Dr. Xiaofan Du

Dr. Xiaofan Du

Qingdao Industrial Energy Storage Research Institute, Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao, 266101 China

These authors contributed equally to this work.

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Zhou Chen

Zhou Chen

Qingdao Industrial Energy Storage Research Institute, Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao, 266101 China

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Dr. Jingwen Zhao

Corresponding Author

Dr. Jingwen Zhao

Qingdao Industrial Energy Storage Research Institute, Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao, 266101 China

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Guoli Lu

Guoli Lu

Qingdao Industrial Energy Storage Research Institute, Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao, 266101 China

School of Future Technology, University of Chinese Academy of Sciences, Beijing, 100190 China

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Meifang Jiang

Meifang Jiang

Qingdao Industrial Energy Storage Research Institute, Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao, 266101 China

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Prof. Qingyu Kong

Prof. Qingyu Kong

Société Civile Synchrotron SOLEIL, L'Orme des Merisiers, Saint-Aubin-BP 48, 91192 Gif-sur-Yvette Cedex, France

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Yiyuan Yan

Yiyuan Yan

Qingdao Industrial Energy Storage Research Institute, Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao, 266101 China

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Junzhe Du

Junzhe Du

Qingdao Industrial Energy Storage Research Institute, Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao, 266101 China

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Prof. Xinhong Zhou

Corresponding Author

Prof. Xinhong Zhou

College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao, 266042 China

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Prof. Guanglei Cui

Corresponding Author

Prof. Guanglei Cui

Qingdao Industrial Energy Storage Research Institute, Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao, 266101 China

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First published: 19 October 2021
Citations: 74

Graphical Abstract

Here, we discovered a novel crystallized Zn2+ conductor based on inducing crystallization of high-entropy, charge-separated eutectic liquids. To the best of our knowledge, it is the first introduction of the concept of a crystallized eutectic material to achieve dramatically enhanced multivalent-ion transport properties. This facile strategy may also open up opportunities for designing a wide variety of new solid ionic conductors.

Abstract

Solid-state zinc (Zn) batteries offer a new candidate for emerging applications sensitive to volume, safety and cost. However, current solid polymeric or ceramic electrolyte structures remain poorly conductive for the divalent Zn2+, especially at room temperature. Constructing a heterogeneous interface which allows Zn2+ percolation is a viable option, but this is rarely involved in multivalent systems. Herein, we construct a solid Zn2+-ion conductor by inducing crystallization of tailored eutectic liquids formed by organic Zn salts and bipolar ligands. High-entropy eutectic-networks weaken the ion-association and form interfacial Zn2+-percolated channels on the nucleator surfaces, resulting in a solid crystal with exceptional selectivity for Zn2+ transport (turn:x-wiley:14337851:media:anie202113086:anie202113086-math-0001 =0.64) and appreciable Zn2+ conductivity (σurn:x-wiley:14337851:media:anie202113086:anie202113086-math-0002 =3.78×10−5 S cm−1 at 30 °C, over 2 orders of magnitude higher than conventional polymers), and finally enabling practical ambient-temperature Zn/V2O5 metal solid cells. This design principle leveraged by the eutectic solidification affords new insights on the multivalent solid electrochemistry suffering from slow ion migration.

Conflict of interest

The authors declare no conflict of interest.

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