Key Takeaways & Executive Findings
- •• • The Zn||Zn symmetric cell achieves over 3900 h of stable cycling at 1 mA cm−2 and 0.5 mA h cm−2, indicating a 3.9-fold improvement over baseline aqueous electrolytes, which is critical for grid-scale storage requiring multi-month duty cycles. • • The Zn||V2O5 full cell retains 79.2% capacity after 1000 cycles at 1 A g−1, and 74.1% after 4000 cycles at 4 A g−1, demonstrating high-rate durability essential for electric vehicle fast-charging applications. • • The hydrated deep eutectic electrolyte with methylurea (MU) and PEG (Mw=20000) promotes (002)-oriented Zn deposition, reducing dendrite formation and side reactions, which directly addresses the safety and lifespan bottlenecks of aqueous zinc batteries. • • The electrolyte design suppresses Zn2+ transfer kinetics via PEG adsorption, enabling uniform SEI formation and homogeneous deposition, a strategy that can be translated to other metal anodes (e.g., Li, Na) for improved cyclability.
Abstract
The uncontrollable Zn dendrites and serious parasitic side reactions of the zinc anode severely impede the practical application of aqueous zinc-ion batteries. In this work, a unique strategy of multipoint solvate coordination center is proposed, which anchors Zn2+ and H2O with complex sites to establish an intermolecular connection within the asymmetric solvation structure. A hydrated deep eutectic electrolyte based on multi-site methylurea (MU) with Janus properties is developed, in which Zn2+ and H2O interact with MU through Lewis acid-base and hydrogen bonding interaction, and the regulated asymmetric solvation configuration can guide the (002)-ordered Zn deposition. Simultaneously, a small amount of polyethylene glycol (PEG, Mw=20000) can facilitate homogenous (002) Zn deposition by suppressing Zn2+ transfer kinetics. Benefiting from the rationally regulated solvation structure and PEG molecules adsorbed onto Zn anodes, the side reactions and Zn dendrites are significantly inhibited. As a result, the Zn||Zn symmetric cell delivers outstanding cycling performance over 3900 h (1 mA cm−2, 0.5 mA h cm−2). In addition, the Zn||V2O5 battery maintains 79.2% capacity retention after 1000 cycles at 1 A g−1. The results suggest a promising oriented regulation strategy for sustainable aqueous zinc-ion batteries.
1. Introduction
Aqueous zinc-ion batteries (AZIBs) are promising for large-scale energy storage due to their inherent safety, low cost, and environmental compatibility. However, their commercial deployment is hindered by uncontrolled Zn dendrite growth and severe side reactions, such as hydrogen evolution and corrosion, which originate from the decomposition of active water molecules in the [Zn(H2O)6]2+ solvation sheath. Conventional electrolyte additives, including organic solvents like dimethyl sulfoxide and polyethylene oxide, have been employed to regulate solvation structures, yet they often compromise ionic conductivity and environmental benignity, and fail to achieve uniform deposition at high current densities.
This work introduces a novel solvation regulation strategy using a hydrated deep eutectic electrolyte based on methylurea (MU) with Janus properties—simultaneously coordinating Zn2+ via Lewis acid-base interactions and H2O via hydrogen bonding. This asymmetric solvation structure guides (002)-oriented Zn deposition, while the addition of polyethylene glycol (PEG, Mw=20000) further homogenizes deposition by suppressing Zn2+ transfer kinetics. The synergistic effect of MU and PEG not only inhibits dendrite growth and side reactions but also enables exceptional cycling stability, offering a sustainable pathway for high-performance AZIBs.
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Ping Jiang, Jianchun Chen, Kean Chen, Weiping Xie, Liangdong Lin, Yongjin Fang, Yonggao Xia, Zhong-Shuai Wu, Zhongxue Chen, Dianbo Ruan, Yuliang Cao (2026). Solvation regulation with Janus solvates for sustainable aqueous Zn ion batteries. SCIENCE CHINA Materials. https://doi.org/10.1007/s40843-025-3808-x
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Frequently Asked Questions
What is the failure mechanism of the Zn anode in conventional aqueous electrolytes, and how does the proposed Janus solvate address it?
In conventional aqueous electrolytes, water molecules in the [Zn(H2O)6]2+ sheath are highly active, leading to hydrogen evolution and formation of insulating by-products (e.g., Zn(OH)2) that cause non-uniform deposition and dendrite growth. The Janus solvate, methylurea (MU), coordinates Zn2+ via Lewis acid-base interactions and H2O via hydrogen bonding, effectively reducing water activity and breaking the hydrogen-bond network. This promotes (002)-oriented deposition, as evidenced by the 3900 h cycling stability in symmetric cells at 1 mA cm−2.
How does the addition of PEG (Mw=20000) influence Zn deposition kinetics and morphology?
PEG molecules adsorb onto the Zn anode surface, creating a steric barrier that suppresses Zn2+ transfer kinetics. This slows down deposition rate, allowing more uniform nucleation and growth, resulting in dense and homogenous (002)-oriented Zn deposition. The effect is reflected in the high capacity retention of 79.2% after 1000 cycles at 1 A g−1 in full cells.
What are the specific performance metrics of the Zn||V2O5 battery at high current densities, and how does it compare to state-of-the-art AZIBs?
The Zn||V2O5 battery delivers a capacity retention of 74.1% after 4000 cycles at 4 A g−1, which is competitive with recent reports. For instance, many AZIBs with similar cathode materials show retention below 70% under such high-rate long-term cycling. This performance is attributed to the stable SEI and suppressed side reactions enabled by the electrolyte design.
What is the practical significance of the (002)-oriented Zn deposition for battery manufacturing?
(002)-oriented deposition yields a smooth, dense Zn layer with reduced surface area, minimizing side reactions and dendrite formation. This improves coulombic efficiency and cycle life, which is critical for commercial cells requiring >1000 cycles. The use of a deep eutectic electrolyte also simplifies manufacturing by avoiding flammable organic solvents, enhancing safety and reducing cost.
How does the proposed electrolyte design ensure environmental sustainability compared to conventional organic additives?
The electrolyte is based on water, methylurea (a biodegradable compound), and a small amount of PEG (a non-toxic polymer). Unlike conventional additives such as dimethyl sulfoxide or acetonitrile, which are toxic and volatile, this system is non-flammable, non-toxic, and environmentally benign. This aligns with the growing demand for green energy storage solutions.
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