Key Takeaways & Executive Findings
- •• An organic-assisted solid electrolyte interface pre-construction creates a functional organic interfacial layer (OIL-IPS@Zn) with aligned zwitterionic structures, suppressing side reactions and enhancing Zn2+ transport. • OIL-IPS@Zn shows superior electrolyte affinity, enabling symmetric cells to operate stably for 3500 h at 1 mA cm−2/1 mAh cm−2 and 3200 h at 50 mA cm−2/10 mAh cm−2. • With 99.90% Zn plating/stripping efficiency, full cells paired with H2V3O8 cathodes achieve over 7000 cycles. • Density functional theory calculations and experiments confirm that immobilized organic propane sulfonate lowers energy barriers and increases Zn2+ transport kinetics.
Abstract
Rechargeable zinc-ion batteries have emerged as one of the most promising candidates for large-scale energy storage applications due to their high safety and low cost. However, the use of Zn metal in batteries suffers from many severe issues, including dendrite growth and parasitic reactions, which often lead to short cycle lives. Herein, we propose the construction of functional organic interfacial layers (OIL) on the Zn metal anodes to address these challenges. Through a well-designed organic-assist pre-construction process, a densely packed artificial layer featuring the immobilized zwitterionic molecular brush can be constructed, which can not only efficiently facilitate the smooth Zn plating and stripping, but also introduce a stable environment for battery reactions. Through density functional theory calculations and experimental characterizations, we verify that the immobilized organic propane sulfonate on Zn anodes can significantly lower the energy barrier and increase the kinetics of Zn2+ transport. Thus, the Zn metal anode with the functional OIL can significantly improve the cycle life of the symmetric cell to over 3500 h stable operation. When paired with the H2V3O8 cathode, the aqueous Zn-ion full cells can be continuously cycled over 7000 cycles, marking an important milestone for Zn anode development for potential industrial applications.
1. Introduction
Electrochemical energy storage devices play a crucial role in the utilization of renewable energy sources, thereby making the development of renewable clean energy strategically important for establishing a sustainable society [1–6]. Aqueous zinc-ion (Zn-ion) batteries, which directly use metallic zinc as the anode, are considered one of the ideal batteries due to their abundance, non-toxicity, high safety, and high theoretical capacity (820 mAh g−1) [7–11]. Despite the extensive research on aqueous zinc-ion batteries for large-scale energy storage systems, the potential commercial application of these batteries faces various challenges, such as dendrite growth and parasitic reactions at the zinc anode, which often lead to low capacity, poor cycling performance, and even safety issues [12–17]. Therefore, it is highly desirable to develop stable Zn anodes with high plating/stripping efficiency, dendritic growth suppression, and alleviated parasitic reactions, to enhance the overall electrochemical performance and cycling stability.
Up to now, several strategies have been proposed to improve the reversibility and stability of Zn electrodes for Zn-ion batteries, including hierarchical structural design [18, 19], artificial protective layer design [20], electrolyte modification [21], and separator modification [22, 23]. In particular, introducing an artificial protective layer on the Zn anodes, such as TiO2 [24], BTO@Zn [25], Zn3(PO4)2·4H2O [26], and NaC(CN)3 [27], shows robust potential, which can significantly improve the stability of the Zn metal anode by reducing parasitic reactions and dendrite formation. For instance, Li et al. [28] reported the design of the MOF-CeO2 artificial protection layer on the zinc anode, which promoted the dissolution process of [Zn(H2O)6]2+ and balanced the flux of Zn ions through the pore channels, leading to improved Coulombic efficiency and cycle stability. Nevertheless, introducing foreign layers on Zn surface often faces interfacial issues that may cause insufficient contact and a low Zn2+ transport rate [29–31]. Therefore, in situ constructing artificial solid electrolyte interface (SEI) derived from electrolytes can be an alternative strategy to maintain excellent interfacial contact [32, 33]. However, due to the constant h
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Limeng Sun, Xianjun Cao, Li Gao, Jiayi Li, Chen Qian, Jinhu Wu, Xinming Nie, Hong Gao, Peng Huang, Yufei Zhao, Yong Wang, Jinqiang Zhang, Guoxiu Wang, Hao Liu (2025). Immobilizing Zwitterionic Molecular Brush in Functional Organic Interfacial Layers for Ultra-Stable Zn-Ion Batteries. Nano-Micro Letters. https://doi.org/10.1007/s40820-025-01782-5
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Frequently Asked Questions
What is the main challenge addressed in this paper?
The paper addresses the severe issues of dendrite growth and parasitic reactions in zinc metal anodes, which lead to short cycle lives in rechargeable zinc-ion batteries.
How does the proposed functional organic interfacial layer (OIL) improve battery performance?
The OIL, featuring immobilized zwitterionic molecular brushes, facilitates smooth Zn plating/stripping, lowers energy barriers for Zn2+ transport, and creates a stable environment, resulting in over 3500 h of stable symmetric cell operation and over 7000 cycles in full cells.
What are the key experimental results reported?
Symmetric cells with OIL-IPS@Zn operate stably for 3500 h at 1 mA cm−2/1 mAh cm−2 and 3200 h at 50 mA cm−2/10 mAh cm−2, with a Zn plating/stripping efficiency of 99.90%. Full cells with H2V3O8 cathodes achieve over 7000 cycles.
What methods were used to verify the effectiveness of the OIL?
Density functional theory (DFT) calculations and experimental characterizations were used to confirm that the immobilized organic propane sulfonate lowers energy barriers and increases Zn2+ transport kinetics.
What is the significance of this work for industrial applications?
The work marks an important milestone for Zn anode development, offering a promising strategy to enhance the cycling stability and efficiency of zinc-ion batteries, which are considered ideal for large-scale energy storage due to their safety and low cost.
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