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Nano Research Energy 2023, 2: e9120064 https://doi.org/10.26599/NRE.2023.9120064
Research Article | Open Access | Issue | Published: 10 April 2023

Functional group differentiation of isomeric solvents enables distinct zinc anode chemistry

Show Author's Information Chao Liu1,2,§,  Qing Li3,§,  Yilun Lin1,2,  Zhiquan Wei2,3,  Yihan Yang2,  Cuiping Han5,  Minshen Zhu6,  Haiyan Zhang1( ),  Hongfei Li2,4( )
School of Materials and Energy, Guangdong University of Technology, Guangzhou 510006, China
Songshan Lake Materials Laboratory, Dongguan 523808, China
Department of Materials Science and Engineering, City University of Hong Kong, Hong Kong 999077, China
School of System Design and Intelligent Manufacturing, Southern University of Science and Technology, Shenzhen 518055, China
Faculty of Materials Science and Engineering/Institute of Technology for Carbon Neutrality, Shenzhen Institutes of Advanced Technology, Chinese Academy of Sciences, Shenzhen 518055, China
Research Center for Materials, Architectures, and Integration of Nanomembranes (MAIN), TU Chemnitz, Chemnitz 09126, Germany

Keywords:
functional group, isomeric solvents, zinc anode, solid electrolyte interphase (SEI) model
Cite this article:
Liu C, Li Q, Lin Y, et al. Functional group differentiation of isomeric solvents enables distinct zinc anode chemistry. Nano Research Energy, 2023, 2: e9120064. https://doi.org/10.26599/NRE.2023.9120064
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Abstract Full text Electronic supplementary material About this article

Electrolytes hold the key to realizing reliable zinc (Zn) anodes. Divergent organic molecules have been proven effective in stabilizing Zn anodes; however, irrational comparisons exist due to the uncontrolled molecular weights and functional group amounts. In this work, two “isomeric molecules”: 1,2-dimethoxyethane (DME) and 1-methoxy-2-propanol (PM), with identical molecular weights but different functional groups, have been studied as co-solvents in electrolytes, which have delivered distinct electrochemical performance. Experimental and simulative study indicates the dipole moment induced by the hydroxyl groups in PM (higher molecular polarity than ether groups in DME) reconstructs the space charge region, enhances the concentration of Zn2+ in the vicinity of Zn anodes, and in-situ derives different solid electrolyte interphase (SEI) models and electrode–electrolyte interfaces, resulting in exceptional cycling stability. Remarkably, the Zn||Cu cell with PM worked over 2000 cycles with high Coulombic efficiency (CE) of 99.7%. The Zn||Zn symmetric cell cycled over 2000 h at 1 mA·cm−2, and showed excellent stability at an ultrahigh current density of 10 mA·cm−2 and capacity of 20 mAh·cm−2 over 200 h (depth of discharge, DOD of 70%). The Zn||sodium vanadate pouch cell with a high mass loading of 6.3 mg·cm−2 and a high capacity of 24 mAh demonstrates superior cyclability after 570 h. This work can be a good starting point to provide reliable guidance on electrolyte design for practical aqueous Zn batteries.


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Electronic supplementary material
About this article

Functional group differentiation of isomeric solvents enables distinct zinc anode chemistry

Show Author's information Chao Liu1,2,§, Qing Li3,§, Yilun Lin1,2, Zhiquan Wei2,3, Yihan Yang2, Cuiping Han5, Minshen Zhu6, Haiyan Zhang1( ), Hongfei Li2,4( )
School of Materials and Energy, Guangdong University of Technology, Guangzhou 510006, China
Songshan Lake Materials Laboratory, Dongguan 523808, China
Department of Materials Science and Engineering, City University of Hong Kong, Hong Kong 999077, China
School of System Design and Intelligent Manufacturing, Southern University of Science and Technology, Shenzhen 518055, China
Faculty of Materials Science and Engineering/Institute of Technology for Carbon Neutrality, Shenzhen Institutes of Advanced Technology, Chinese Academy of Sciences, Shenzhen 518055, China
Research Center for Materials, Architectures, and Integration of Nanomembranes (MAIN), TU Chemnitz, Chemnitz 09126, Germany

Abstract

Electrolytes hold the key to realizing reliable zinc (Zn) anodes. Divergent organic molecules have been proven effective in stabilizing Zn anodes; however, irrational comparisons exist due to the uncontrolled molecular weights and functional group amounts. In this work, two “isomeric molecules”: 1,2-dimethoxyethane (DME) and 1-methoxy-2-propanol (PM), with identical molecular weights but different functional groups, have been studied as co-solvents in electrolytes, which have delivered distinct electrochemical performance. Experimental and simulative study indicates the dipole moment induced by the hydroxyl groups in PM (higher molecular polarity than ether groups in DME) reconstructs the space charge region, enhances the concentration of Zn2+ in the vicinity of Zn anodes, and in-situ derives different solid electrolyte interphase (SEI) models and electrode–electrolyte interfaces, resulting in exceptional cycling stability. Remarkably, the Zn||Cu cell with PM worked over 2000 cycles with high Coulombic efficiency (CE) of 99.7%. The Zn||Zn symmetric cell cycled over 2000 h at 1 mA·cm−2, and showed excellent stability at an ultrahigh current density of 10 mA·cm−2 and capacity of 20 mAh·cm−2 over 200 h (depth of discharge, DOD of 70%). The Zn||sodium vanadate pouch cell with a high mass loading of 6.3 mg·cm−2 and a high capacity of 24 mAh demonstrates superior cyclability after 570 h. This work can be a good starting point to provide reliable guidance on electrolyte design for practical aqueous Zn batteries.

Keywords: functional group, isomeric solvents, zinc anode, solid electrolyte interphase (SEI) model

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Publication history

Received: 07 February 2023
Revised: 05 March 2023
Accepted: 08 March 2023
Published: 10 April 2023
Issue date: June 2023

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© The Author(s) 2023. Published by Tsinghua University Press.

Acknowledgements

Acknowledgements

We acknowledge the financial support from the Open Research Fund of Songshan Lake Materials Laboratory (No. 2021SLABFN04), the National Natural Science Foundation of China (Nos. 22005207 and U20A20249), the Regional Innovation and Development Joint Fund, and the Science and Technology Program of Guangdong Province of China (No. 2022A0505030028).

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