Citation: Qiao Li, Yijian Chen, Meihua Zhu, Houhou Huang, Fu-Quan Bai, Linglong Hu, Rui Gao, Hongji Xu, Chaoqun Qu, Ming Feng. Constructing robust anode/electrolyte interface by additive in hydrogel to achieve high utilization of Zn anode[J]. Chinese Chemical Letters, ;2026, 37(4): 111754. doi: 10.1016/j.cclet.2025.111754 shu

Constructing robust anode/electrolyte interface by additive in hydrogel to achieve high utilization of Zn anode

Qiao Li ^a ,
Yijian Chen ^a ,
Meihua Zhu ^{a, *,} ,
Houhou Huang ^b ,
Fu-Quan Bai ^b ,
Linglong Hu ^a ,
Rui Gao ^c ,
Hongji Xu ^a ,
Chaoqun Qu ^{a, *,} ,
Ming Feng ^{a, *,}

a.
Key Laboratory of Functional Materials Physics and Chemistry of the Ministry of Education, Jilin Normal University, Changchun 130103, China
b.
College of Chemistry, Jilin University, Changchun 130012, China
c.
Institute for Clean Energy Technology, North China Electric Power University, Beijing 102206, China

zhumh18@mails.jlu.edu.cn

quchaoqun@jlnu.edu.cn

mingfeng@jlnu.edu.cn

Received Date: 20 July 2025
Revised Date: 15 August 2025
Accepted Date: 25 August 2025
Available Online: 26 August 2025

Figures(5)

Hydrogel electrolyte have attracted widely interest for aqueous zinc-ion batteries because of their multi-functionality and intrinsic safety. However, the unstable anode/electrolyte interface by dendrite and side reaction (HER) restricted the cycling of Zn anode, especially at high utilization. Herein, we propose an interface engineering strategy by introducing dimethylformamide (DMF) to polyacrylamide (PAM) electrolyte which could construct the polymer-inorganic bilayer solid electrolyte interphase (SEI) to improve the interface stability and compatibility. Internal Zn₅(OH)₆(CO₃)₂ provided high modulus to suppress the dendrite physically and external polymer exhibited flexibility to accommodate the volume change of Zn during cycles. Meanwhile, larger polymer clusters were induced by enhanced hydrogen-bond interactions, resulted in higher shear strength and interfacial adhesion. Additionally, DMF regulated the crystal orientation along (100) crystal plane and solvation structure of Zn²⁺ with PAM, enabling dense deposition and reduced by-products. Consequently, the Zn anode could provide an impressive lifespan (0.5 mA/cm²@0.5 mAh/cm², 4000 h; 30 mA/cm²@15 mAh/cm², 650 h). More importantly, high utilization (68%) was achieved using ultra-thin Zn (10 µm) with superior stability (2 mA/cm²@4 mAh/cm², 1200 h). Coupled with iodine cathode, the Zn-I₂ cell could provide an initial capacity of 184.5 mAh/g at the low ratio of anode/cathode capacity (N/P: 4.3) and ~86.4% retention over 500 cycles. This work provides a promising approach to construct robust interface by hydrogel electrolyte towards practical zinc-ion batteries.
- Aqueous zinc-ion battery,
- Zn anode,
- Hydrogel electrolyte,
- Polymer-inorganic solid electrolyte interface,
- Solvation structure
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