Aqueous Zn metal batteries (ZBs) have obtained increasing attention recently owing to their low-cost and environmentally friendly nature. Unfortunately, the sluggish Zn²⁺ de/intercalation in hosts often requires the nanostructural tailoring of cathode materials, which however degrades the tap density and accelerates the dissolution of active species. Herein, we propose a shallow-layer pillaring strategy to drive the superior zinc storage performance of V₂O₅ monolithic grains without the prerequisite of intentional nanoscale attenuation. The in situ polymerized 3,4-ethylenedioxythiophene chains only in the near-surface V₂O₅ interlayers are sufficient to activate a cascading effect to successively open the deeper interlayers during Zn intercalation. This synergic interlayer expansion mechanism leads to a thorough and quick redox process of bulk phase V₂O₅ even with micro-sized grains as opposed to the poor reaction kinetics in the non-pillared one. In contrast to excess pillaring or cation doping, the shallow-layer hybridization with a hydrophobic conductive polymer can suppress the dissolution of active species, reinforce the conductive contact between grains, lower the Zn²⁺ diffusion barrier (0.39 eV) and absorption energy (0.17 eV), and upgrade the pseudocapacitance contribution (>67%) and Zn²⁺ diffusion coefficient (1.43 × 10⁻⁹–1.81 × 10⁻⁸ cm² s⁻¹). This composite cathode enables an unprecedented cycling/rate performance (e.g. 388, 367 and 351 mA h g⁻¹ even at 5, 8 and 10 A g⁻¹ respectively, and 269 mA h g⁻¹ after 4500 cycles at 10 A g⁻¹), corresponding to high energy densities of 280.2 and 205.8 W h kg⁻¹ under ultrahigh power densities of 700.5 and 5960 W kg⁻¹, respectively. This concept of shallow-layer pillaring activation (especially via rich organic molecules) can be extended to more electrode systems with the preservation of the grain integrity.

中文翻译：

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整体聚合物颗粒中的导电聚合物的浅层立柱，通过级联效应来驱动出色的锌储存

锌水金属电池（ZBs）近年来因其低成本和环保特性而受到越来越多的关注。不幸的是，寄主中缓慢的Zn ²⁺脱除/嵌入通常需要对阴极材料进行纳米结构调整，但是这会降低振实密度并加速活性物质的溶解。在本文中，我们提出了一种浅层柱化策略，以驱动V ₂ O ₅整体晶粒的优异锌存储性能，而无需故意进行纳米级衰减。在原位仅在近面V聚合3,4-亚乙基链₂ ö ₅中间层足以激活级联效应，从而在Zn插入过程中依次打开较深的中间层。这种协同的层间膨胀机理甚至导致了微细晶粒，也使块状相V ₂ O ₅发生了彻底，快速的氧化还原过程，这与非立柱中的不良反应动力学相反。与过量柱化或阳离子掺杂相比，与疏水性导电聚合物的浅层杂交可抑制活性物质的溶解，增强晶粒之间的导电接触，降低Zn ²⁺扩散势垒（0.39 eV）和吸收能（0.17） eV），并提升伪电容贡献（> 67％）和Zn ²⁺扩散系数（1.43×10 ^-9–1.81×10 ^-8 cm ² s ^-1）。该复合阴极使前所未有的循环/速率的性能（例如388，367和351毫安汞柱^-1即使在5,8和10 A G ^-1分别与269毫安汞柱^-1以10 A G 4500次循环后^-1）分别对应于700.5和5960 W kg ^-1的超高功率密度下的280.2和205.8 W h kg ^-1的高能量密度。可以通过保留晶粒完整性将这种浅层支柱激活（尤其是通过富有机分子）的概念扩展到更多的电极系统。