Zn/MnO₂ batteries, driven by a dual deposition reaction, are a prominent avenue for achieving high energy density in aqueous systems. Introducing an initially dual-electrode-free (anode/cathode) configuration can further boost energy density to over 200 Wh kg⁻¹, but with limited cycle life due to the poor reversibility of Zn/MnO₂ deposition and stripping. Drawing inspiration from soft templating strategies in material synthesis, here we apply this approach to electrodeposition and stripping by designing an in situ formed liquid crystal interphase. This concept is achieved by incorporating just 0.1 mM of surfactant molecules into the electrolyte, which induces favourable c-axis orientations in depositing both hexagonal Zn and MnO₂. This enhancement subsequently increases the deposition/stripping reversibility and promotes the cycle life of the dual-electrode-free battery, achieving 80% capacity retention after ~950 cycles. This liquid crystal interphase chemistry also holds great promise for regulating deposition in other crystal systems, opening an exciting research direction for next-generation high-energy-density and long-duration energy storage based on aqueous chemistries.

由双沉积反应驱动的Zn/MnO ₂电池是在水系统中实现高能量密度的重要途径。引入最初的无双电极（阳极/阴极）配置可以进一步将能量密度提高到200 Wh kg ^-1以上，但由于Zn/MnO ₂沉积和剥离的可逆性较差，循环寿命有限。受到材料合成中软模板策略的启发，我们通过设计原位形成的液晶界面将这种方法应用于电沉积和剥离。这一概念是通过将仅 0.1 mM 的表面活性剂分子掺入电解质中来实现的，这在沉积六方 Zn 和 MnO ₂时诱导有利的c轴取向。这种增强随后提高了沉积/剥离的可逆性，并提高了双电极无电池的循环寿命，在约 950 次循环后实现了 80% 的容量保持率。这种液晶相间化学也为调节其他晶体系统中的沉积提供了广阔的前景，为基于水化学的下一代高能量密度和长时间储能开辟了令人兴奋的研究方向。