Orientational Electrodeposition of Highly (002)-Textured Zinc Metal Anodes Enabled by Iodide Ions for Stable Aqueous Zinc Batteries

Abstract

Regulating the crystallographic texture of the zinc (Zn) metal anode is promising to promote Zn reversibility in aqueous electrolytes, but the direct fabrication of specific textured Zn still remains challenging. Herein, we report a facile iodide ion (I–)-assisted electrodeposition strategy that can scalably fabricate highly (002) crystal plane-textured Zn metal anode (H-(002)-Zn). Theoretical and experimental characterizations demonstrate that the presence of I– additives can significantly elevate the growth rate of the Zn (100) plane, homogenize the Zn nucleation, and promote the plating kinetics, thus enabling the uniform H-(002)-Zn electrodeposition. Taking the electrolytic cell with the conventional ZnSO4-based electrolyte and commercial Cu substrate as a model system, the Zn texture gradually transforms from (101) to (002) as the increase of NaI additive concentration. In the optimized 1 M ZnSO4 + 0.8 M NaI electrolyte, the as-prepared H-(002)-Zn features a compact structure and an ultrahigh intensity ratio of (002) to (101) signal without containing the (100) signal. The free-standing H-(002)-Zn electrode manifests stronger resistance to interfacial side reactions than the conventional (101)-textured Zn electrode, thus delivering a high efficiency of 99.88% over 400 cycles and ultralong cycling lifespan over 6700 h (>9 months at 1 mA cm–2) and assuring the stable operation of full Zn batteries. This work will enlighten the efficient electrosynthesis of high-performance Zn anodes for practical aqueous Zn batteries.

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“…Over the next 20 cycles, the diffraction intensity of (002) lattice plane on the reed membrane modified Zn rose more dramatically to 1.80 (Figure 3f), whereas that of its counterpart experienced a negligible growth. This elucidates the reed interlayers' capability to promote dendrite-free Zn(002) electrodeposition, attributed to the reduction in desolvation energy and the uniform distribution of current density on the surface of the Zn anode, [39,61,62] which is conducive to achieving smooth and uniform zinc depositions, as well as a prolonged cycle life.…”

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“…Figure a shows the cyclic voltammetry (CV) profiles of the as-assembled coin cells. 3DOM MnO 2 /Ni shows a higher current density than the 2D MnO 2 /Ni cathode, which means a larger electrochemical active surface area is provided by the 3DOM structured skeleton . Further, in conjunction with the 3DOM Sn@Zn anode, the full battery delivers a polarization decrease of 29 mV owing to the improved reaction kinetics at the anode side.…”

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“…Another notable advancement in ZIB anode research involves refining manufacturing processes to lower costs and enhance overall performance. Examples of this are the creation of a scalable and cost-efficient method for producing Zn anodes through a straightforward electroplating process, roll-to-roll processing and 3D printing [238,263,264]. Furthermore, the integration of advanced characterization techniques, such as in situ microscopy and spectroscopy, has empowered researchers to deepen their understanding of the fundamental processes related to Zn deposition [265][266][267].…”