Molecular Tailoring of Helmholtz Plane by a Cyclic Imino Additive: Inhibiting Hydrogen Evolution Reaction and Enabling Dendrite-Free Zn Anodes for High-Performance Hybrid Zn/Na Aqueous Batteries

Menglu Lu; Zhong Qiu; Tianqi Yang; Zheyu Jin; Jiayuan Xiang; Jianping Xu; Fangfang Tu; Wenkui Zhang; Xinping He; Yang Xia; Hui Huang; Xinhui Xia; Jun Zhang

doi:10.1002/adfm.202518611

Molecular Tailoring of Helmholtz Plane by a Cyclic Imino Additive: Inhibiting Hydrogen Evolution Reaction and Enabling Dendrite-Free Zn Anodes for High-Performance Hybrid Zn/Na Aqueous Batteries

Menglu Lu
, Zhong Qiu
, Tianqi Yang^*
, Zheyu Jin
, Jiayuan Xiang
, Jianping Xu
, Fangfang Tu
, Wenkui Zhang
, Xinping He
, Yang Xia
, Hui Huang
, Xinhui Xia
, Jun Zhang^*

^*Corresponding author for this work

Department of Physics

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

4 Citations (Scopus)

Abstract

Aqueous zinc-sodium (Zn/Na) hybrid ion batteries (AZSIBs) combine the high energy density of aqueous Zn-ion batteries and the high safety of aqueous Na-ion batteries. However, AZSIBs suffer from rapid performance degradation because of unregulated zinc deposition and unwanted chemical reactions. To address these challenges, this study introduces a new type of additive, 5,5-dimethylhydantoin (DMH), which has a cyclic structure and an imine group. It can reconstruct the Helmholtz plane of the anode while inhibiting the hydrogen evolution reaction and promoting the epitaxial growth of the zinc (002) plane. Theoretical and experimental results reveal that DMH molecules preferentially adsorbed on the anode surface, displacing active H₂O from the inner Helmholtz Plane (IHP), and Zn²⁺is deposited in a compact and dense manner along the Zn (002) plane. As a result, Zn//Zn symmetric cell demonstrates stable cycling for 2400 h without a short circuit. Moreover, Zn//V₂O₅ full cell cycles stably for over 3,000 cycles at a current density of 3 A g^-1. This work establishes a paradigm of additive engineering for developing high-performance AZSIBs.

© 2025 Wiley-VCH GmbH

Original language	English
Article number	e18611
Number of pages	13
Journal	Advanced Functional Materials
DOIs	https://doi.org/10.1002/adfm.202518611
Publication status	Online published - 2 Sept 2025

Funding

M.L., and Z.Q. contributed equally to this work. The authors acknowledge the support by the Key Scientific Research Project of Hangzhou (No. 2024SZD1B12), Department of Science & Technology of Zhejiang Province (No. 2024C01095), the Fundamental Research Funds for the Provincial Universities of Zhejiang (RF-C2022008), Zhejiang Provincial Natural Science Foundation of China (No. LD22E020006), and the National Natural Science Foundation of China (NSFC, Nos. U20A20253, 22279116, and 52372235).

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

SDG 7 Affordable and Clean Energy

Research Keywords

5
5-dimethylhydantoin
helmholtz plane
hybrid Zn/Na aqueous batteries
Zinc anode
Zn (002) plane growth

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Lu, M., Qiu, Z., Yang, T., Jin, Z., Xiang, J., Xu, J., Tu, F., Zhang, W., He, X., Xia, Y., Huang, H., Xia, X., & Zhang, J. (2025). Molecular Tailoring of Helmholtz Plane by a Cyclic Imino Additive: Inhibiting Hydrogen Evolution Reaction and Enabling Dendrite-Free Zn Anodes for High-Performance Hybrid Zn/Na Aqueous Batteries. Advanced Functional Materials, Article e18611. Advance online publication. https://doi.org/10.1002/adfm.202518611

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title = "Molecular Tailoring of Helmholtz Plane by a Cyclic Imino Additive: Inhibiting Hydrogen Evolution Reaction and Enabling Dendrite-Free Zn Anodes for High-Performance Hybrid Zn/Na Aqueous Batteries",

abstract = "Aqueous zinc-sodium (Zn/Na) hybrid ion batteries (AZSIBs) combine the high energy density of aqueous Zn-ion batteries and the high safety of aqueous Na-ion batteries. However, AZSIBs suffer from rapid performance degradation because of unregulated zinc deposition and unwanted chemical reactions. To address these challenges, this study introduces a new type of additive, 5,5-dimethylhydantoin (DMH), which has a cyclic structure and an imine group. It can reconstruct the Helmholtz plane of the anode while inhibiting the hydrogen evolution reaction and promoting the epitaxial growth of the zinc (002) plane. Theoretical and experimental results reveal that DMH molecules preferentially adsorbed on the anode surface, displacing active H2O from the inner Helmholtz Plane (IHP), and Zn2+ is deposited in a compact and dense manner along the Zn (002) plane. As a result, Zn//Zn symmetric cell demonstrates stable cycling for 2400 h without a short circuit. Moreover, Zn//V2O5 full cell cycles stably for over 3,000 cycles at a current density of 3 A g-1. This work establishes a paradigm of additive engineering for developing high-performance AZSIBs. {\textcopyright} 2025 Wiley-VCH GmbH",

keywords = "5, 5-dimethylhydantoin, helmholtz plane, hybrid Zn/Na aqueous batteries, Zinc anode, Zn (002) plane growth",

author = "Menglu Lu and Zhong Qiu and Tianqi Yang and Zheyu Jin and Jiayuan Xiang and Jianping Xu and Fangfang Tu and Wenkui Zhang and Xinping He and Yang Xia and Hui Huang and Xinhui Xia and Jun Zhang",

year = "2025",

month = sep,

day = "2",

doi = "10.1002/adfm.202518611",

language = "English",

journal = "Advanced Functional Materials",

issn = "1616-301X",

publisher = "Wiley-VCH Verlag GmbH",

}

Lu, M, Qiu, Z, Yang, T, Jin, Z, Xiang, J, Xu, J, Tu, F, Zhang, W, He, X, Xia, Y, Huang, H, Xia, X & Zhang, J 2025, 'Molecular Tailoring of Helmholtz Plane by a Cyclic Imino Additive: Inhibiting Hydrogen Evolution Reaction and Enabling Dendrite-Free Zn Anodes for High-Performance Hybrid Zn/Na Aqueous Batteries', Advanced Functional Materials. https://doi.org/10.1002/adfm.202518611

Molecular Tailoring of Helmholtz Plane by a Cyclic Imino Additive: Inhibiting Hydrogen Evolution Reaction and Enabling Dendrite-Free Zn Anodes for High-Performance Hybrid Zn/Na Aqueous Batteries. / Lu, Menglu; Qiu, Zhong; Yang, Tianqi et al.
In: Advanced Functional Materials, 02.09.2025.

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

TY - JOUR

T1 - Molecular Tailoring of Helmholtz Plane by a Cyclic Imino Additive: Inhibiting Hydrogen Evolution Reaction and Enabling Dendrite-Free Zn Anodes for High-Performance Hybrid Zn/Na Aqueous Batteries

AU - Lu, Menglu

AU - Qiu, Zhong

AU - Yang, Tianqi

AU - Jin, Zheyu

AU - Xiang, Jiayuan

AU - Xu, Jianping

AU - Tu, Fangfang

AU - Zhang, Wenkui

AU - He, Xinping

AU - Xia, Yang

AU - Huang, Hui

AU - Xia, Xinhui

AU - Zhang, Jun

PY - 2025/9/2

Y1 - 2025/9/2

N2 - Aqueous zinc-sodium (Zn/Na) hybrid ion batteries (AZSIBs) combine the high energy density of aqueous Zn-ion batteries and the high safety of aqueous Na-ion batteries. However, AZSIBs suffer from rapid performance degradation because of unregulated zinc deposition and unwanted chemical reactions. To address these challenges, this study introduces a new type of additive, 5,5-dimethylhydantoin (DMH), which has a cyclic structure and an imine group. It can reconstruct the Helmholtz plane of the anode while inhibiting the hydrogen evolution reaction and promoting the epitaxial growth of the zinc (002) plane. Theoretical and experimental results reveal that DMH molecules preferentially adsorbed on the anode surface, displacing active H2O from the inner Helmholtz Plane (IHP), and Zn2+ is deposited in a compact and dense manner along the Zn (002) plane. As a result, Zn//Zn symmetric cell demonstrates stable cycling for 2400 h without a short circuit. Moreover, Zn//V2O5 full cell cycles stably for over 3,000 cycles at a current density of 3 A g-1. This work establishes a paradigm of additive engineering for developing high-performance AZSIBs. © 2025 Wiley-VCH GmbH

AB - Aqueous zinc-sodium (Zn/Na) hybrid ion batteries (AZSIBs) combine the high energy density of aqueous Zn-ion batteries and the high safety of aqueous Na-ion batteries. However, AZSIBs suffer from rapid performance degradation because of unregulated zinc deposition and unwanted chemical reactions. To address these challenges, this study introduces a new type of additive, 5,5-dimethylhydantoin (DMH), which has a cyclic structure and an imine group. It can reconstruct the Helmholtz plane of the anode while inhibiting the hydrogen evolution reaction and promoting the epitaxial growth of the zinc (002) plane. Theoretical and experimental results reveal that DMH molecules preferentially adsorbed on the anode surface, displacing active H2O from the inner Helmholtz Plane (IHP), and Zn2+ is deposited in a compact and dense manner along the Zn (002) plane. As a result, Zn//Zn symmetric cell demonstrates stable cycling for 2400 h without a short circuit. Moreover, Zn//V2O5 full cell cycles stably for over 3,000 cycles at a current density of 3 A g-1. This work establishes a paradigm of additive engineering for developing high-performance AZSIBs. © 2025 Wiley-VCH GmbH

KW - 5

KW - 5-dimethylhydantoin

KW - helmholtz plane

KW - hybrid Zn/Na aqueous batteries

KW - Zinc anode

KW - Zn (002) plane growth

UR - https://www.webofscience.com/wos/woscc/full-record/WOS:001562147800001

U2 - 10.1002/adfm.202518611

DO - 10.1002/adfm.202518611

M3 - RGC 21 - Publication in refereed journal

SN - 1616-301X

JO - Advanced Functional Materials

JF - Advanced Functional Materials

M1 - e18611

ER -

Molecular Tailoring of Helmholtz Plane by a Cyclic Imino Additive: Inhibiting Hydrogen Evolution Reaction and Enabling Dendrite-Free Zn Anodes for High-Performance Hybrid Zn/Na Aqueous Batteries

Abstract

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Research Keywords

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