Volume 64, Issue 24 e202501721
Research Article

Interfacial H-bond Network/Concentration Fields/Electric Fields Regulation Achieved by D-Valine Anions Realizes the Highly Efficient Aqueous Zinc Ion Batteries

Jiadong Lin

Jiadong Lin

State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources, Key Laboratory of Oil and Gas Fine Chemicals of Ministry of Education, School of Chemical Engineering and Technology, Xinjiang University, Urumqi, 830017 China

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Chenchen Ji

Corresponding Author

Chenchen Ji

State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources, Key Laboratory of Oil and Gas Fine Chemicals of Ministry of Education, School of Chemical Engineering and Technology, Xinjiang University, Urumqi, 830017 China

E-mail: [email protected]; [email protected]; [email protected]

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Gaozhi Guo

Gaozhi Guo

State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources, Key Laboratory of Oil and Gas Fine Chemicals of Ministry of Education, School of Chemical Engineering and Technology, Xinjiang University, Urumqi, 830017 China

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Yulu Luo

Yulu Luo

State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources, Key Laboratory of Oil and Gas Fine Chemicals of Ministry of Education, School of Chemical Engineering and Technology, Xinjiang University, Urumqi, 830017 China

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Pengru Huang

Pengru Huang

Guangxi Key Laboratory of Information Materials, Guangxi Collaborative Innovation Center of Structure and Property for New Energy Materials, School of Materials Science and Engineering, Guilin University of Electronic Technology, Guilin, 541004 China

Institute for Functional Intelligent Materials, National University of Singapore, Singapore, 117544 Singapore

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Fen Xu

Fen Xu

Guangxi Key Laboratory of Information Materials, Guangxi Collaborative Innovation Center of Structure and Property for New Energy Materials, School of Materials Science and Engineering, Guilin University of Electronic Technology, Guilin, 541004 China

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Lixian Sun

Corresponding Author

Lixian Sun

Guangxi Key Laboratory of Information Materials, Guangxi Collaborative Innovation Center of Structure and Property for New Energy Materials, School of Materials Science and Engineering, Guilin University of Electronic Technology, Guilin, 541004 China

E-mail: [email protected]; [email protected]; [email protected]

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Wilhelm Pfleging

Wilhelm Pfleging

Institute for Applied Materials, Karlsruhe Institute of Technology, Hermann von Helmholtz Platz 1, Eggenstein Leopoldshafen, 76344 Germany

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Kostya S. Novoselov

Corresponding Author

Kostya S. Novoselov

Institute for Functional Intelligent Materials, National University of Singapore, Singapore, 117544 Singapore

School of Physics & Astronomy, The University of Manchester, Manchester, M13 9PL United Kingdom

E-mail: [email protected]; [email protected]; [email protected]

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First published: 09 April 2025
Citations: 3

Graphical Abstract

A D-valine anion interfacial layer reversely regulates the interfacial H-bond network and the interfacial concentration/electric fields, which realizes the synchronous occurrence of inhibition (suppressing H+ migration by disrupting the interfacial H-bond interaction and restraining the anion depletion layer formation) and optimization effects (homogenizing the interfacial Zn2+ flow and electric field).

Abstract

Uncontrolled mobile anions and proton transport result in many issues, including interfacial anion depletion, irregular multiphysics fields fluctuations, space charge layer-induced interfacial Zn dendrites, and hydrogen evolution reaction (HER), which seriously exacerbates the cycling stability of zinc-ion batteries. Herein, this work constructs an efficient D-valine anion interface structure to reversely regulate the Zn2+/H+ dynamic chemistry and unlocks the multiple regulation effects of this anionic interface by investigating interfacial proton transport and complex concentration/electric fields distribution of Zn anode through dynamic in-situ spectroscopy analysis, static energy calculations, and molecular dynamics simulation. We unravel core factors affecting complicated interfacial HER processes and the generation of the space charge layer. This anionic interfacial layer severs proton hopping transport by rupturing the initial water–water hydrogen bond, which effectively restrains uncontrolled HER processes. Further, the anion-immobilized interfacial layer accelerates Zn2+ transfer to optimize the interfacial concentration fields. Also, the anionic interface restrains the formation of the anion depletion layer by relieving rapid Zn2+ ions exhaustion and strengthening the uniformity of interfacial electrical field distribution, which suppresses space charges-induced Zn dendrite growth. Consequently, Zn||Zn symmetric cells deliver an ultralong cycle life of 4150 h. Importantly, the multiple regulation effects enable Zn||I2 cells exhibit long-term stable 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 from the corresponding author upon reasonable request.

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