Key Takeaways & Executive Findings
- •• Aspartame additive enables in situ formation of self-healing ZnO-based SEI, enhancing Zn anode corrosion resistance and stability. • Zn║Zn symmetric cells with APM-modified electrolyte operate stably for 6,400 h at −5 °C, 10,330 h at 25 °C, and 2,250 h at 40 °C, with a high DOD of 85.2%. • Achieves 99.59% Coulombic efficiency, suppresses dendrite growth, and maintains 150 mAh g−1 capacity after 1,750 cycles in NH4+-V2O5 full cells. • Provides a straightforward electrolyte engineering strategy for dendrite-free, wide-temperature aqueous Zn-ion batteries.
Abstract
Metallic Zn anodes suffer from hydrogen evolution and dendritic deposition in aqueous electrolytes, resulting in low Coulombic efficiency and poor cyclic stability for aqueous Zn-ion batteries (AZIBs). Constructing stable solid electrolyte interphase (SEI) with strong affinity for Zn and exclusion of water corrosion of Zn metal anodes is a promising strategy to tackle these challenges. In this study, we develop a self-healing ZnO-based SEI film on the Zn electrode surface by employing an aspartame (APM) as a versatile electrolyte additive. The hydrophobic nature and strong Zn affinity of APM can facilitate the dynamic self-healing of ZnO-based SEI film during cyclic Zn plating/stripping process. Benefiting from the superior protection effect of self-healing ZnO-based SEI, the Zn║Cu cells possess an average coulombic efficiency more than 99.59% over 1,000 cycles even at a low current density of 1 mA cm−2 − 1 mAh cm−2. Furthermore, the Zn║NH4+-V2O5 full cells display a large specific capacity of 150 mAh g−1 and high cyclic stability with a capacity retention of 77.8% after 1,750 cycles. In addition, the Zn║Zn cell delivers high temperature adaptability at a wide-temperature range from −5 to 40 °C even under a high DOD of 85.2%. The enhanced capability and durability originate from the self-healing SEI formation enabled by multifunctional APM additives mediating both corrosion suppression and interfacial stabilization. This work presents an inspired and straightforward approach to promote a dendrite-free and wide-temperature rechargeable AZIBs energy storage system.
1. Introduction
Aqueous Zn-ion batteries (AZIBs) are regarded as one of the most commercially viable options among the next-generation electrochemical energy storage systems. The high volumetric capacity and specific capacity of Zn metal endow AZIBs with unique advantages for large-scale applications [1–5]. However, the thermodynamic instability of Zn anode stemming from its low redox potential (−0.762 V vs SHE) persistently compromises electrochemical performance through irreversible side reactions [6, 7]. The inevitable hydrogen evolution reaction (HER) severely depletes the electrolytes [8] and generates loose, poorly conductive by-products, such as Zn4(OH)6SO4·xH2O (ZSH) [9]. Dendritic Zn is further exacerbated by the enhanced “tip effect,” where Zn2+ deposition mostly happens at a limited number of highly active sites [10]. The aforementioned fundamental issues lead to an unstable electrolyte/electrode interface and the puncturing of separator, ultimately resulting in cell failure.
Recent advances in addressing the above critical issues for Zn anodes mainly contain the following three aspects [11, 12], including using hydrogels to restrict the migration of free H2O [13, 14], modifying the Zn metal surface [15–17], and limiting harmful ion transport through the separator [18, 19]. Among them, electrolyte engineering is considered as one of the most straightforward and effective strategies to stabilize Zn electrode, which can directly change the deposition behavior of Zn2+ and affect the interface properties of Zn electrode [20, 21]. The common electrolyte modification methods include altering the solvation structure of Zn2+ [22–25], modifying the hydrogen bonding network of H2O molecules [26, 27], adjusting electric field distribution at the interface [28–30], and regulating the inner Helmholtz plane (IHP) [31, 32]. Previous research on electrolyte additives primarily concentrated on the bulk phase of the electrolyte and the interface between electrolyte and Zn electrode to mitigate Zn corrosion caused by the aqueous electrolyte [33, 34]. The effects of other solutes in the electrolyte except H2O and electrolyte salts on Zn metal are always ignored. However, because the anion decomposition voltage in the electrolyte is much higher than that in H2O, SEI formation on the surface of the Zn electrode is less studied [35]. Therefore, constructing SEI film with the a
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Yunyu Shi, Yingkang Liu, Ruirui Chang, Guilin Zhang, Yuqing Rang, Zheng-Long Xu, Qi Meng, Penghui Cao, Xiangyang Zhou, Jingjing Tang, Juan Yang (2025). Aspartame Endowed ZnO-Based Self-Healing Solid Electrolyte Interface Film for Long-Cycling and Wide-Temperature Aqueous Zn-Ion Batteries. Nano-Micro Letters. https://doi.org/10.1007/s40820-025-01765-6
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Frequently Asked Questions
What is the role of aspartame in the electrolyte for Zn-ion batteries?
Aspartame acts as a multifunctional electrolyte additive that facilitates the in situ formation of a self-healing ZnO-based solid electrolyte interphase (SEI) on the Zn anode. Its hydrophobic nature and strong Zn affinity help suppress water corrosion and dendrite growth, enhancing the stability and cycle life of the battery.
How does the self-healing SEI film improve battery performance?
The self-healing SEI film dynamically repairs itself during cycling, providing continuous protection against corrosion and dendrite formation. This results in high Coulombic efficiency (99.59%), long cycle life (up to 10,330 hours in symmetric cells), and stable operation over a wide temperature range (-5 to 40 °C).
What are the key performance metrics of the modified Zn-ion batteries?
The Zn║Cu cells achieve an average Coulombic efficiency of 99.59% over 1,000 cycles. The Zn║NH4+-V2O5 full cells deliver a specific capacity of 150 mAh g−1 with 77.8% capacity retention after 1,750 cycles. Zn║Zn symmetric cells operate stably for 6,400 h at -5 °C, 10,330 h at 25 °C, and 2,250 h at 40 °C, even at a high depth of discharge (DOD) of 85.2%.
Why is wide-temperature operation important for aqueous Zn-ion batteries?
Wide-temperature operation is crucial for practical applications in various climates and conditions. The aspartame-modified electrolyte enables stable performance from -5 to 40 °C, addressing the common issue of performance degradation at extreme temperatures, thus expanding the usability of AZIBs.
What is the significance of the self-healing mechanism in the SEI film?
The self-healing mechanism ensures that any damage to the SEI film during cycling is repaired, maintaining a robust protective layer. This prevents continuous corrosion and dendrite growth, leading to enhanced durability and longer cycle life, which is essential for commercial viability.
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