Volume 137, Issue 8 e202420284
Forschungsartikel

Polyoxotungstate Featuring Zinc-Ion-Triggered Structural Transformation as An Efficient Electrolyte Additive for Aqueous Zinc-Ion Batteries

Dr. Yi Chen

Dr. Yi Chen

Fujian Provincial Key Laboratory of Advanced Inorganic Oxygenated-Materials, State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, Fujian, 350108 China

College of Chemical Engineering, Fuzhou University, Fuzhou, Fujian, 350108 China

These authors contribute equally to this work.

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Ze-Xun Zhang

Ze-Xun Zhang

Fujian Provincial Key Laboratory of Advanced Inorganic Oxygenated-Materials, State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, Fujian, 350108 China

These authors contribute equally to this work.

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Prof. Dr. Ping-Wei Cai

Corresponding Author

Prof. Dr. Ping-Wei Cai

Fujian Provincial Key Laboratory of Advanced Inorganic Oxygenated-Materials, State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, Fujian, 350108 China

State Key Laboratory of Structural Chemistry, and Fujian Provincial Key Laboratory of Materials and Techniques toward Hydrogen Energy, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian, 350002 China

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Dr. Zheng-Wei Guo

Dr. Zheng-Wei Guo

Fujian Provincial Key Laboratory of Advanced Inorganic Oxygenated-Materials, State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, Fujian, 350108 China

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Zhi-Wen Lu

Zhi-Wen Lu

State Key Laboratory of Structural Chemistry, and Fujian Provincial Key Laboratory of Materials and Techniques toward Hydrogen Energy, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian, 350002 China

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Prof. Dr. Cai Sun

Prof. Dr. Cai Sun

Fujian Provincial Key Laboratory of Advanced Inorganic Oxygenated-Materials, State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, Fujian, 350108 China

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Prof. Dr. Xin-Xiong Li

Prof. Dr. Xin-Xiong Li

Fujian Provincial Key Laboratory of Advanced Inorganic Oxygenated-Materials, State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, Fujian, 350108 China

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Prof. Dr. Jun-Xiang Chen

Corresponding Author

Prof. Dr. Jun-Xiang Chen

State Key Laboratory of Structural Chemistry, and Fujian Provincial Key Laboratory of Materials and Techniques toward Hydrogen Energy, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian, 350002 China

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Prof. Dr. Zhen-Hai Wen

Prof. Dr. Zhen-Hai Wen

State Key Laboratory of Structural Chemistry, and Fujian Provincial Key Laboratory of Materials and Techniques toward Hydrogen Energy, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian, 350002 China

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Prof. Dr. Shou-Tian Zheng

Corresponding Author

Prof. Dr. Shou-Tian Zheng

Fujian Provincial Key Laboratory of Advanced Inorganic Oxygenated-Materials, State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, Fujian, 350108 China

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First published: 27 November 2024

Abstract

It is promising but still challenging for the widespread application of aqueous zinc batteries due to the poor reversibility of the zinc anode caused by prevalent dendrite growth and pronounced interfacial side reactions. Herein, we report a rare soluble and water-stable high-nuclearity {Nd9Si4W39} polyoxotungstate. Interestingly, upon encountering Zn2+ ions, the discrete {Nd9Si4W39} nanocluster undergoes a structural transformation to form an infinitely extended cluster-based {[Zn(H2O)4]3[Nd9Si4W39]2} two-dimensional honeycomb layer, with which atomic-level Zn2+ ion effects in reconstructing the layer are determined. More interestingly, we demonstrate that the structural transformation property renders the {Nd9Si4W39} cluster an efficient electrolyte additive for aqueous zinc batteries, enabling the formation of the 2D layer as a protective layer on the zinc anode, significantly enhancing the reversibility of the zinc anode. Compared to the pristine Zn//Zn symmetric battery, the Zn//Zn symmetric battery with the {Nd9Si4W39} additive exhibits an extended lifespan of over 2000 hours at a current density of 1 mA cm−2. In situ optical microscopy, Raman spectroscopy, and molecular dynamics simulations reveal that the formation of the protective layer effectively promotes uniform zinc deposition, and inhibits zinc agglomeration, dendrite growth, and side reactions, thereby enabling the zinc anode to exhibit high reversibility and long-term service life.

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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