Key Takeaways & Executive Findings
- •• A bilayer of zincophilic Cu and flexible polymer on Zn anode enables uniform Zn deposition and suppresses dendrites. • The Cu layer provides nucleation sites, while the polymer layer prevents side reactions, enhancing cycle stability. • Symmetric cells achieve over 2900 h cycling at 1 mA cm−2, and full cells retain 72% capacity after 500 cycles. • This strategy offers a simple, effective approach to improve aqueous zinc-ion battery performance for practical applications.
Abstract
Aqueous zinc-ion batteries are regarded as promising electrochemical energy-storage systems for various applications because of their high safety, low costs, and high capacities. However, dendrite formation and side reactions during zinc plating or stripping greatly reduce the capacity and cycle life of a battery and subsequently limit its practical application. To address these issues, we modified the surface of a zinc anode with a functional bilayer composed of zincophilic Cu and flexible polymer layers. The zincophilic Cu interfacial layer was prepared through CuSO4 solution pretreatment to serve as a nucleation site to facilitate uniform Zn deposition. Meanwhile, the polymer layer was coated onto the Cu interface layer to serve as a protective layer that would prevent side reactions between zinc and electrolytes. Benefiting from the synergistic effect of the zincophilic Cu and protective polymer layers, the symmetric battery exhibits an impressive cycle life, lasting over 2900 h at a current density of 1 mA·cm−2 with a capacity of 1 mA·h·cm−2. Moreover, a full battery paired with a vanadium oxide cathode achieves a remarkable capacity retention of 72% even after 500 cycles.
1. Introduction
The development of renewable energy sources, such as wind, hydropower, tidal energy, and biomass energy, is essential to reducing the consumption of limited fossil fuels and mitigating related greenhouse and air pollution [1]. However, the intermittency and fluctuation of renewable energy resources result in fluctuating frequency and voltage instability when these resources are integrated into power grids. Through peak shaving and valley filling, energy-storage devices can mitigate instability caused by renewable resources in power systems [2‒3]. The electrochemical energy-storage technology is relatively mature, and rechargeable batteries are electrochemical energy-storage devices that play a vital role in daily life [4‒5]. For 30 years, lithium-ion batteries (LIBs) have been extensively applied to transportable electronics and electric-powered vehicles because of their high energy densities and long cycle lifespans [6]. However, LIBs cause pollution because of their nickel, cobalt, and fluorine components and have safety issues. Additionally, the high costs of raw materials restrict their large-scale applications in smart grids [7]. Compared with LIBs, aqueous zinc-ion batteries have low cost, low toxicity, and high safety [8−11]. Moreover, they exhibit excellent theoretical capacity (5851 mA·h·mL−1), low oxidation-reduction potential (−0.76 V vs. standard hydrogen electrode) [12], and excellent ionic conductivity. These characteristics make them promising candidates as supplementary energy-storage devices for LIBs, thus drawing considerable attention [13‒14].
However, aqueous zinc-ion batteries are subject to many challenges, such as uncontrolled dendrite formation and side reactions [15]. A rough zinc metal surface and uneven electric field would cause the nonuniform deposition of Zn, which will evolve in protuberances. These protuberances act as charge centers during subsequent plating processes, triggering uncontrolled dendrite growth, which may break separators and cause a short circuit [16‒17]. In addition, active water molecules in electrolytes are electrolyzed to produce H+ and OH−, resulting in severe hydrogen evolution, anodic corrosion, and passivation [18‒19]. To solve the dendrite issue, one strategy is to introduce a metal coating with high zincophilicity, which provides nucleation sites, decreases nucleation overpotential, and facilitates uniform Zn deposition [20]. Such coating is typically composed of Au [21], Ag [22‒23], In [24], or Cu [23,25]. However, metal coatings undergo considerable volume expansion during Zn plating and stripping, leading to coating rupture and failure, and restricting stability performance [26]. Besides the dendrite’s issues, side reactions between deposited Zn on a nucleation site’s surface and an electrolyte require further attention. These reactions can be prevented on a metal anode surface by applying a shielding layer to prevent direct contact between a metal anode and an electrolyte. Therefore, various protective layers have been explored.
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Luyang Sun, Wenjia Zhang, Qiongqiong Lu, Pengfei Yue, Guoshang Zhang, Kexing Song, Yanqing Su (2025). Zincophilic Cu/flexible polymer heterogeneous interfaces ensuring the stability of zinc metal anodes. Int. Journal of Minerals, Metallurgy and Materials (矿物冶金与材料学报). https://doi.org/10.1007/s12613-024-3020-7
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Frequently Asked Questions
What is the main challenge in aqueous zinc-ion batteries?
The main challenges are uncontrolled dendrite formation and side reactions during zinc plating/stripping, which reduce capacity and cycle life.
How does the Cu/polymer bilayer improve zinc anode stability?
The zincophilic Cu layer provides nucleation sites for uniform Zn deposition, while the flexible polymer layer acts as a protective barrier to prevent side reactions between zinc and electrolyte, synergistically enhancing stability.
What performance was achieved with the modified zinc anode?
The symmetric battery lasted over 2900 hours at 1 mA cm−2 with 1 mAh cm−2, and a full battery with vanadium oxide cathode retained 72% capacity after 500 cycles.
Why is the polymer layer necessary in addition to the Cu layer?
The polymer layer prevents direct contact between the zinc anode and electrolyte, suppressing side reactions like hydrogen evolution and corrosion, which the Cu layer alone cannot fully address.
What is the significance of this research for practical applications?
This simple and effective surface modification strategy enhances the cycle life and capacity retention of aqueous zinc-ion batteries, making them more viable as safe, low-cost energy storage systems.
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