Key Takeaways & Executive Findings
- •• A rigid electrolyte container (SiO2@PVDF-hfp) was designed to immobilize the liquid halogen-ion electrolyte, enabling separator-free Zn-halogen batteries. • The container regulates Zn2+ solvation via hydrogen bonding regulation, while providing multi-channel structure for enhanced mass transfer, jointly enabling durable Zn plating/stripping. • Effective confinement of intermediates ensures high reversibility across multi-electron transfer mechanisms, achieving an exceptionally low-capacity decay of 0.02‰ over 4500 cycles and a high areal capacity of 11.9 mAh cm−2. • This work presents a novel “container engineering” approach to halogen-ion electrolyte design, providing fundamental insights into redox reversibility and reaction kinetics.
Abstract
Recent advancements in Zn-halogen batteries have focused on enhancing the adsorptive or catalytic capability of host materials and stabilizing complex intermediates with electrolyte additives, while the halogen-ion electrolyte modifications exhibit strong potential for integrated interfacial regulation. Herein, we design an electrically insulating rigid electrolyte container to immobilize a liquid halogen-ion electrolyte for separator-free Zn-halogen batteries with customizable electron transfer. Robust hydrogen bonding of hydroxyl groups in SiO2 with fluorinated moieties in PVDF-hfp regulates Zn2+ solvation and suppresses H2O activity, while multi-channels formed by microcracks and interparticle gaps not only enhance mass transfer but also buffer interfacial electric field, jointly enabling a durable Zn plating/stripping. Effective confinement of intermediates also ensures the high reversibility across single-(I−/I0), double-(I−/I0/I⁺), and triple-(I−/I0/I⁺, Cl−/Cl0) electron transfer mechanisms at cathode, as evidenced by the double-electron transfer systems exhibiting a low capacity decay rate of 0.02‰ over 4500 cycles at 10 mA cm−2 and a high areal capacity of 11.9 mAh cm−2 at 2 mA cm−2. This work presents a novel “container engineering” approach to halogen-ion electrolyte design and provides fundamental insights into the relationships between redox reversibility and reaction kinetics.
1. Introduction
The past decade has witnessed the explosive growth in Zn-based batteries and their potential for grid-scale energy storage [1]. Distinct from rocking-chair systems driven solely by Zn2+ transport, the Zn-halogen batteries operate on a dual-ion mechanisms involving independent interfacial reactions (i.e., Zn plating/stripping at anode and halogen redox at cathode) [2]. This configuration offers fast kinetics, high-energy efficiency, and design flexibility, yet the uncontrolled loss of active halogen species leads to short lifespan, thereby limiting their practical applications [3].
Halogens are incorporated into Zn-based batteries primarily through two strategies, including cathode blending and electrolyte additives [4]. The former is more commonly employed for higher utilization of charge carriers, while the latter streamlines the process by focusing optimization on the electrolyte itself [5]. Regarding physicochemical properties, halogen species such as I− and Cl− can form highly polar and unstable interhalogen compounds [6]. For instance, in a common double-electron system, I− can complex with I2 to form I3−, which impairs kinetics. Meanwhile, the oxidized ICl species is prone to decomposition, causing the collapse of high-voltage plateau [7]. Hence, designing a system that can effectively confine these reactive species to enable reversible, high utilization redox remains a central goal.
To address these issues, various modification strategies have been proposed. A wide range of carbon substrates, doped frameworks, and metal compound composites were introduced into the cathode to enhance halogen confinement through physical adsorption or chemical anchoring, while catalytic components such as heteroatom dopants and transition metal sites were incorporated to accelerate redox kinetics [8–10]. Additionally, surfactants, organic chelators and pH-responsive polymers were added into electrolyte to sta...
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Yifan Zhou, Yicai Pan, Yongqiang Yang, Taghreed F. Altamimi, Yunpeng Zhong, Dalal A. Alshammari, Zeinhom M. El-Bahy, Shuquan Liang, Jiang Zhou, Xinxin Cao (2026). Electrically Insulating Rigid Multi-Channel Electrolyte Container for Customizable Electron Transfer in Zn-Halogen Batteries. Nano-Micro Letters. https://doi.org/10.1007/s40820-025-02007-5
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Frequently Asked Questions
What is the main innovation of this paper?
The paper introduces a novel 'container engineering' approach using an electrically insulating rigid electrolyte container (SiO2@PVDF-hfp) to immobilize liquid halogen-ion electrolytes, enabling separator-free Zn-halogen batteries with customizable electron transfer.
How does the electrolyte container improve battery performance?
The container regulates Zn2+ solvation via hydrogen bonding, suppresses water activity, and provides multi-channels for enhanced mass transfer and electric field buffering, leading to durable Zn plating/stripping and high reversibility across multiple electron transfer mechanisms.
What are the key performance metrics achieved?
The double-electron transfer system exhibits a low capacity decay rate of 0.02‰ over 4500 cycles at 10 mA cm−2 and a high areal capacity of 11.9 mAh cm−2 at 2 mA cm−2.
What is the significance of customizable electron transfer?
The design allows for effective confinement of intermediates, enabling high reversibility across single-, double-, and triple-electron transfer mechanisms, which is crucial for high-energy and long-life Zn-halogen batteries.
What are the potential applications of this technology?
This technology is promising for grid-scale energy storage and other applications requiring high-energy, long-life, and safe battery systems.
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