Key Takeaways & Executive Findings
- •• Electric ambipolar effect motivates strong dipole interactions reorganized primary cations solvation sheath. • Electrostatic shielding homogenized the distribution for nucleated Zn and facilized the orientated Zn deposition. • The eutectic network of Zn2+ ternary hydrated eutectic electrolytes enables highly reversible and noteworthy Br2/Br− reaction kinetics. • The ZTE electrolyte achieves a broadened electrochemical window of 2.9 V and enables Zn anode plating/stripping reversibly for over 2400 h.
Abstract
The coupling of fast redox kinetics, high-energy density, and prolonged lifespan is a permanent aspiration for aqueous rechargeable zinc batteries, but which has been severely hampered by a narrow voltage range and suboptimal compatibility between the electrolytes and electrodes. Here, we unprecedentedly introduced an electric ambipolar effect for synergistic manipulation on Zn2+ ternary-hydrated eutectic electrolyte (ZTE) enabling high-performance Zn-Br2 batteries. The electric ambipolar effect motivates strong dipole interactions among hydrated perchlorates and bipolar ligands of L-carnitine (L-CN) and sulfamide, which reorganized primary cations solvation sheath in a manner of forming Zn[(L-CN)(SA)(H2O)4]2+ configuration and dynamically restricting desolvated H2O molecules, thus ensuring a broadened electrochemical window of 2.9 V coupled with high ionic conductivity. Noticeably, L-CN affords an electrostatic shielding effect and an in situ construction of organic–inorganic interphase, endowing oriented Zn anode plating/stripping reversibly for over 2400 h. Therefore, with the synergy of electro/nucleophilicity and exceptional compatibility, the ZTE electrolyte dynamically boosts the conversion redox of Zn-Br2 batteries in terms of high specific capacity and stable cycling performance. These findings open a window for designing electrolytes with synergetic chemical stability and compatibility toward advanced zinc-ion batteries.
1. Introduction
The integration of cost-effective, high-safety, and environmentally friendly battery systems with the electrical grid has proven beneficial, especially in ensuring continuous energy supply and addressing the intermittency challenges associated with renewable energy [1, 2]. Recently, rechargeable aqueous zinc-ion batteries have garnered considerable attention owing to their immense advantages in terms of exceptional safety, outstanding theoretical energy density, and economically sustainable raw materials [3–5]. Despite that, the practical implementation of aqueous zinc-ion batteries still remains hindered by several primary obstacles of thermodynamic and kinetic instability [6]. Specifically, conventional aqueous electrolytes frequently result in a shortened lifespan attributed to the uncontrolled formation of dendrites and the occurrence of competitive corrosion at interfaces on Zn anodes [7–9]. Moreover, the inherently narrow electrochemical stable window (ESW) of the electrolyte along with its poor compatibility with high-voltage cathodes prevents the achievement of high-energy density [10, 11].
Noticeably, as a representative of a high-energy density battery system, the two-electrons conversion reaction of a Zn-Br2 battery (ZBBs) based on the Br2/Br− redox couple is appealing due to its exhibition of a high redox potential (1.7 V vs. Zn/Zn2+) alongside an impressive specific capacity of 335 mAh g−1 [12, 13]. Although ZBBs demonstrate intriguing advantages, the matching traditional aqueous electrolyte faces serious side reactions especially upon redox conversion under high voltage [14, 15]. To address these problems, it is crucial to design a compatible aqueous electrolytes system that realizes collaborative benefits in both the cathode and anode aspects, which contributes to fully demonstrating the potential.
Considering the aforementioned challenges linked to high-energy–density ZBBs, a thorough understanding and modulation of the cation solvation-interphase chemistry intimately associated with electrolytes become crucial for reversible Br2/Br− conversion and stabilizing the Zn plating/stripping [16]. Although several strategies, such as component manipulation motivated water-in-salt electrolytes or introducing additives, to diminish the activity of the free water mo
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Wenda Li, Hengyue Xu, Shanzhe Ke, Hongyi Zhang, Hao Chen, Gaijuan Guo, Xuanyi Xiong, Shiyao Zhang, Jianwei Fu, Chengbin Jing, Jiangong Cheng, Shaohua Liu (2025). Integrating Electric Ambipolar Effect for High-Performance Zinc Bromide Batteries. Nano-Micro Letters. https://doi.org/10.1007/s40820-024-01636-6
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Frequently Asked Questions
What is the electric ambipolar effect in the context of zinc bromide batteries?
The electric ambipolar effect refers to the synergistic manipulation of ion transport and solvation structure in the electrolyte, which enhances the performance of zinc bromide batteries by reorganizing the primary cation solvation sheath and restricting water activity.
How does the ZTE electrolyte improve the electrochemical stability window?
The ZTE electrolyte, through the electric ambipolar effect, forms a Zn[(L-CN)(SA)(H2O)4]2+ configuration that dynamically restricts desolvated water molecules, thereby broadening the electrochemical stability window to 2.9 V.
What role does L-carnitine play in the electrolyte?
L-carnitine provides an electrostatic shielding effect and facilitates the in situ construction of an organic–inorganic interphase, which promotes oriented Zn deposition and enhances the reversibility of Zn plating/stripping for over 2400 hours.
What are the key performance metrics of the Zn-Br2 battery using ZTE electrolyte?
The ZTE electrolyte enables high specific capacity and stable cycling performance in Zn-Br2 batteries, with a high redox potential of 1.7 V vs. Zn/Zn2+ and a specific capacity of 335 mAh g−1.
What is the significance of the electric ambipolar effect for future battery design?
The findings open a window for designing electrolytes with synergetic chemical stability and compatibility, which is crucial for advancing high-energy-density zinc-ion batteries and other aqueous battery systems.
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