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π-Interactive Additive Unlocks Enhanced Zinc Anode Rechargeability: Unveiling Critical Role of Adsorption Layer Dynamics
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DOI：10.1039/D5EE05206H.png)
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Abstract
En 中文
Aqueous zinc-ion batteries promise a safe; inexpensive; and sustainable platform for stationary energy storage; but their reversibility remains limited by dendrite and corrosion-mediated failure of the zinc anode. While low-concentration electrolyte additives have emerged as scalable solutions; the mechanistic underpinnings of their interfacial dynamics that dictate whether they enable long-term rechargeability or trigger premature dendritic failure remain poorly understood. Here; we investigate a series of π-interactive aromatic alcohols and a cycloaliphatic reference additive and uncover how additive–zinc and additive–additive interactions jointly govern the formation; spatial organization; packing density; and mobility of the additive film. These interfacial dynamics govern Zn²⁺ transport; corrosion suppression; and zinc deposition morphology. Phenol; which strikes a balance between adsorption strength and interfacial mobility; forms a thick yet dynamic layer that suppresses hydrogen evolution-mediated corrosion while promoting uniform zinc deposition. This leads to excellent cycling stability with nearly 2 Ah cm-2 cumulative plated capacity in practically relevant asymmetric configuration at 24% depth of discharge under a demanding 4 mA cm-2 - 4 mAh cm-2; including a thin separator and low electrolyte-to-capacity ratio; with the Coulombic efficiency reaching 99.89% under kinetic control compared to the 95.94% for the additive-free electrolyte. Full-cell and pouch-cell tests further validate phenol’s efficacy; establishing adsorption layer dynamics as a new paradigm for rationalizing electrolyte additives’ efficacy in regulating zinc anode reversibility in aqueous batteries.
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