Volume 135, Issue 51 e202314883
Forschungsartikel

Engineering Fluorine-rich Double Protective Layer on Zn Anode for Highly Reversible Aqueous Zinc-ion Batteries

Titi Li

Titi Li

School of Physics and Technology, University of Jinan, Shandong, 250022 China

Faculty of Materials Science and Energy Engineering/Institute of Technology for Carbon Neutrality, Shenzhen Institute of Advanced Technology, Chinese Academy of Sciences, Shenzhen, 518055 China

These authors contributed equally to this work.

Contribution: Conceptualization (lead), Data curation (lead), ​Investigation (lead), Resources (lead), Writing - original draft (lead)

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Sanlue Hu

Sanlue Hu

Faculty of Materials Science and Energy Engineering/Institute of Technology for Carbon Neutrality, Shenzhen Institute of Advanced Technology, Chinese Academy of Sciences, Shenzhen, 518055 China

Shenzhen Key Laboratory of Energy Materials for Carbon Neutrality, Shenzhen Institute of Advanced Technology, Chinese Academy of Sciences, Shenzhen, 518055 China

These authors contributed equally to this work.

Contribution: Methodology (lead), Software (lead), Writing - review & editing (equal)

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Chenggang Wang

Chenggang Wang

School of Physics and Technology, University of Jinan, Shandong, 250022 China

These authors contributed equally to this work.

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

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Dun Wang

Dun Wang

Faculty of Materials Science and Energy Engineering/Institute of Technology for Carbon Neutrality, Shenzhen Institute of Advanced Technology, Chinese Academy of Sciences, Shenzhen, 518055 China

Contribution: Data curation (lead), Formal analysis (lead), ​Investigation (lead), Methodology (lead)

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Minwei Xu

Minwei Xu

Faculty of Materials Science and Energy Engineering/Institute of Technology for Carbon Neutrality, Shenzhen Institute of Advanced Technology, Chinese Academy of Sciences, Shenzhen, 518055 China

Shenzhen Key Laboratory of Energy Materials for Carbon Neutrality, Shenzhen Institute of Advanced Technology, Chinese Academy of Sciences, Shenzhen, 518055 China

Contribution: Resources (lead), Supervision (lead)

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Caiyun Chang

Corresponding Author

Caiyun Chang

Faculty of Materials Science and Energy Engineering/Institute of Technology for Carbon Neutrality, Shenzhen Institute of Advanced Technology, Chinese Academy of Sciences, Shenzhen, 518055 China

Shenzhen Key Laboratory of Energy Materials for Carbon Neutrality, Shenzhen Institute of Advanced Technology, Chinese Academy of Sciences, Shenzhen, 518055 China

Contribution: Conceptualization (lead), Data curation (lead), ​Investigation (lead), Methodology (lead), Resources (equal), Writing - review & editing (equal)

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Xijin Xu

Corresponding Author

Xijin Xu

School of Physics and Technology, University of Jinan, Shandong, 250022 China

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

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Cuiping Han

Corresponding Author

Cuiping Han

Faculty of Materials Science and Energy Engineering/Institute of Technology for Carbon Neutrality, Shenzhen Institute of Advanced Technology, Chinese Academy of Sciences, Shenzhen, 518055 China

Shenzhen Key Laboratory of Energy Materials for Carbon Neutrality, Shenzhen Institute of Advanced Technology, Chinese Academy of Sciences, Shenzhen, 518055 China

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

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First published: 04 November 2023
Citations: 1

Abstract

The high thermodynamic instability and side reactions of Zn-metal anode (ZMA), especially at high current densities, greatly impede the commercialization of aqueous zinc-ion batteries (AZIBs). Herein, a fluorine-rich double protective layer strategy is proposed to obtain the high reversibility of AZIBs through the introduction of a versatile tetradecafluorononane-1,9-diol (TDFND) additive in aqueous electrolyte. TDFND molecule with large adsorption energy (−1.51 eV) preferentially absorbs on the Zn anode surface to form a Zn(OR)2 (R=−CH2−(CF2)7−CH2−) cross-linking complex network, which balances space electric field and controls the Zn2+ ion flux, thus enabling the uniform and compact deposition of Zn (002) crystal planes. Meanwhile, TDFND with low Lowest unoccupied molecular orbital (LUMO, 0.10 eV) energy level is priorly decomposed to regulate the interfacial chemistry of ZMA by building a ZnF2-rich solid electrode/electrolyte interface (SEI) layer. It is found that a 14 nm-thick SEI layer delivers excellent structural integrity to suppress parasitic reactions by blocking the direct contact of active water and ZMA. Consequently, the Zn electrode exhibits a superior cycling life over 430 h at 10 mA cm−2 and a high average Coulombic efficiency of 99.8 % at 5 mA cm−2. Furthermore, a 68 mAh pouch cell delivers 80.3 % capacity retention for 1000 cycles.

Conflict of interest

The authors declare no conflict of interest.

Data Availability Statement

Research data are not shared.

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