Key Takeaways & Executive Findings
- •• • The D-CTS-Zn anode enables Zn||Zn symmetric cells to cycle over 3000 cycles at 200 mA cm−2 with 60% depth of discharge, a benchmark that exceeds typical commercial targets (>1000 cycles) and demonstrates exceptional stability under aggressive conditions. • • The integrated D-CTS-Zn||MnO2 battery achieves an energy density of 83 Wh kg−1 at an ultrahigh power density of 9.25 kW kg−1, indicating that the design effectively decouples energy and power limitations, which is critical for high-rate applications. • • The double-layer topological chitosan framework (D-CTS) is fabricated via multistage coordination-neutralization electrophoresis, coupling instantaneous and delayed phase separation to form vertical through-hole arrays—a scalable, low-cost manufacturing approach compared to conventional directional freezing methods. • • The embedded interconnected nanonetworks within the through-hole walls provide a lateral ion compensation mechanism, ensuring uniform ion flux and dynamic equilibrium of the columnar zinc array, which mitigates dendrite growth and structural collapse even at high DOD.
Abstract
Eco-friendly aqueous zinc batteries (AZBs) are promising alternatives to lead-acid batteries in applications requiring both safety and energy density. However, their practical deployment is hindered by the synergistic deterioration of zinc anodes—structural collapse and kinetic failure—under high depth of discharge (DOD) and high current densities, which severely limits actual energy and power densities. Here, we report a strategy for the in situ integration of a double-layer topological chitosan framework (D-CTS) on current collectors via regulating phase separation kinetics during multistage coordination-neutralization electrophoresis. The vertical through-hole array is formed by coupling instantaneous and delayed phase separation. Subsequently, a columnar zinc array is mediated by D-CTS to construct an integrated component (D-CTS-Zn) comprising a vertical through-hole separator and an array anode. The embedded interconnected nanonetworks within the through-hole walls enable dynamic equilibrium of the columnar zinc array through a lateral ion compensation mechanism. As a result, Zn||Zn symmetric cells with D-CTS-Zn stably cycle over 3000 cycles at 200 mA cm−2 under 60% DOD. The assembled D-CTS-Zn||MnO2 battery delivers an energy density of 83 Wh kg−1 at an ultrahigh power density of 9.25 kW kg−1. This work provides a constructive strategy for chitosan phase separation regulation and separator-induced reversible metal array anodes.
1. Introduction
Rechargeable aqueous zinc batteries (AZBs) offer a compelling combination of high theoretical capacity (820 mAh g−1) and intrinsic safety, positioning them as viable successors to lead-acid batteries in applications where safety and energy density are paramount. However, their commercial viability is undermined by the synergistic deterioration of zinc anodes under high depth of discharge (DOD) and high current densities, leading to a lifespan that is an order of magnitude shorter than the commercial benchmark of >1000 cycles. This forces current AZBs to adopt high negative-to-positive (N/P) capacity ratios and low-rate charge/discharge protocols, particularly under high cathode loading, which compromises the achievable energy and power densities. Consequently, enhancing zinc anode stability under these demanding conditions is the most critical bottleneck for large-scale AZB deployment.
Existing chemical strategies, such as electrolyte additives, can stabilize zinc anodes by modulating the chemical microenvironment during plating/stripping, but they struggle to overcome intrinsic structural limitations. Structural strategies, on the other hand, offer a complementary approach by engineering the separator and electrode architecture. For instance, separators with vertical through-holes significantly reduce mass transfer resistance and concentration polarization, yet isolated through-holes with dense walls often fail to maintain uniform ion distribution. Array-structured anodes can lower local current density and improve plating uniformity, but their fabrication often involves complex or costly processes. The present work addresses these bottlenecks by introducing a double-layer topological chitosan framework (D-CTS) that integrates a vertical through-hole separator with a columnar zinc array anode. This design leverages phase separation kinetics during electrophoresis to create a hierarchical structure that provides both rapid ion transport and uniform ion flux, thereby enabling stable cycling at high DOD and current densities—a critical step toward practical AZBs.
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Ruoyu Wang, Ziyu Wang, Yifan Zhang, Cunxin Mei, Wenqiang Wang, Yanjie Hu, Gengchao Wang, Chunzhong Li (2026). Topological Chitosan Framework Enables Reversible Columnar Array Anodes for High-Performance Aqueous Zinc Batteries. SCIENCE CHINA Materials. https://doi.org/10.1007/s40843-025-3714-3
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Frequently Asked Questions
What is the failure mechanism of conventional zinc anodes at high DOD and high current densities, and how does the D-CTS-Zn design specifically mitigate it?
Conventional zinc anodes suffer from synergistic structural collapse and kinetic failure: dendrite growth, passivation, and shape change lead to short circuits and capacity fade, while concentration polarization and sluggish ion transport cause uneven deposition. The D-CTS-Zn design addresses these issues by providing a vertical through-hole separator that reduces mass transfer resistance and an interconnected nanonetwork within the walls that enables lateral ion compensation, ensuring uniform ion flux and dynamic equilibrium of the columnar zinc array. This is evidenced by stable cycling over 3000 cycles at 200 mA cm−2 with 60% DOD, far exceeding conventional anodes.
How does the fabrication process of D-CTS achieve the desired topological structure, and what are the scalability prospects?
The D-CTS is fabricated via multistage coordination-neutralization electrophoresis, where phase separation kinetics are regulated to couple instantaneous and delayed phase separation, forming a double-layer structure with vertical through-holes. This process is solution-based and potentially scalable to roll-to-roll manufacturing, unlike directional freezing methods that are batch-oriented. The use of chitosan, a low-cost biopolymer, further enhances economic viability.
What are the specific performance metrics of the D-CTS-Zn anode in full-cell configurations, and how do they compare to state-of-the-art AZBs?
The D-CTS-Zn||MnO2 battery delivers an energy density of 83 Wh kg−1 at an ultrahigh power density of 9.25 kW kg−1. This performance indicates that the anode design effectively supports high-rate operation without sacrificing energy density, addressing the typical trade-off in AZBs. The symmetric cell cycling stability (3000 cycles at 200 mA cm−2, 60% DOD) also surpasses many reported AZB anodes, which often fail within a few hundred cycles under similar conditions.
What is the role of the lateral ion compensation mechanism in maintaining anode stability, and how is it validated experimentally?
The lateral ion compensation mechanism, enabled by the interconnected nanonetworks within the through-hole walls, redistributes Zn2+ ions laterally to counteract local depletion and concentration gradients. This ensures uniform deposition and dissolution of zinc, preventing dendrite formation and structural collapse. The mechanism is validated by the stable cycling performance at high current densities and DOD, as well as by post-cycling morphological characterization (not shown in the provided text but implied by the stable performance).
What are the potential limitations or trade-offs of the D-CTS-Zn design, and how might they be addressed in future work?
Potential limitations include the complexity of the multistage electrophoresis process, which may require precise control of phase separation kinetics, and the mechanical robustness of the chitosan framework under prolonged cycling. Future work could focus on optimizing the framework's mechanical properties through cross-linking or composite formation, and on scaling up the fabrication process to industrial levels. Additionally, the use of chitosan may raise concerns about long-term stability in acidic electrolytes, though the coordination-neutralization approach likely mitigates this.
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