Dynamic interface engineering of softening metal-inorganic framework for dendrite-free zinc anodes

IF 20.2 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials Pub Date : 2025-10-04 DOI:10.1016/j.ensm.2025.104656

Yuqing Luo, Jiugang Hu, Jia Luo, Shan Cai, Lili He, Chengguo Wei, Guoqiang Zou, Hongshuai Hou, Xiaobo Ji

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引用次数: 0

Abstract

Rechargeable aqueous zinc-ion batteries (AZIBs) face significant challenges from zinc dendrites and side reactions, causing capacity decay and poor cycling stability. Herein, a dynamically softening zincophilic Zn(CN)₂ metal-inorganic framework was in situ constructed on zinc foil (Zn(CN)₂-Zn) via a vapor-phase etching strategy. In situ Raman monitoring revealed the dynamic interfacial transition from dense nonporous Pn3m phase to hexagonal P6₃/mmc phase (Lon-Zn(CN)₂) during cycling. The resulting Lon-Zn(CN)₂ framework features nanoconfined hexagonal linear channels that accelerate Zn²⁺ desolvation and enable uniform ion transport. In situ synchrotron radiation X-ray imaging and COMSOL simulations further confirmed that this structural transition homogenizes interfacial electric field and ensures excellent plating/stripping reversibility. Moreover, the high lattice matching between Lon-Zn(CN)₂ (001) and Zn(002) planes promotes epitaxial zinc deposition while suppressing dendrite formation. Consequently, the Zn(CN)₂-Zn electrode achieves stable cycling for over 3200 hours at 0.5 mA cm⁻² in symmetrical cells and superior rate performance with a capacity retention rate of 99.6% in full cells. This work demonstrates synergistic regulation of ion transport and crystallographic orientation via dynamic metal-inorganic framework engineering, providing a novel strategy for durable and dendrite-free AZIBs.

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无枝晶锌阳极软化金属-无机骨架的动态界面工程

可充电水性锌离子电池（azib）面临着锌枝晶和副反应的重大挑战，导致容量衰减和循环稳定性差。本文采用气相蚀刻技术，在锌箔（Zn(CN)2-Zn）上原位构建了动态软化的亲锌Zn(CN)2金属-无机骨架。原位拉曼监测揭示了循环过程中致密无孔Pn3m相向六方P63/mmc相（Lon-Zn(CN)2）的动态界面转变。得到的Lon-Zn(CN)2骨架具有纳米限制的六边形线性通道，加速了Zn2+的脱溶并实现了均匀的离子传输。原位同步辐射x射线成像和COMSOL模拟进一步证实了这种结构转变使界面电场均匀化，并确保了优异的镀/剥离可逆性。此外，Zn(CN)2（001）和Zn（002）平面之间的高晶格匹配促进了外延锌沉积，同时抑制了枝晶的形成。因此，Zn(CN)2-Zn电极在对称细胞中可以在0.5 mA cm⁻²下稳定循环3200小时以上，并且在满细胞中具有优异的倍率性能，容量保持率为99.6%。这项工作通过动态金属-无机框架工程证明了离子传输和晶体取向的协同调节，为耐用和无枝晶的azib提供了一种新的策略。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Energy Storage Materials Materials Science-General Materials Science

CiteScore

33.00

自引率

5.90%

发文量

652

审稿时长

27 days

期刊介绍： Energy Storage Materials is a global interdisciplinary journal dedicated to sharing scientific and technological advancements in materials and devices for advanced energy storage and related energy conversion, such as in metal-O2 batteries. The journal features comprehensive research articles, including full papers and short communications, as well as authoritative feature articles and reviews by leading experts in the field. Energy Storage Materials covers a wide range of topics, including the synthesis, fabrication, structure, properties, performance, and technological applications of energy storage materials. Additionally, the journal explores strategies, policies, and developments in the field of energy storage materials and devices for sustainable energy. Published papers are selected based on their scientific and technological significance, their ability to provide valuable new knowledge, and their relevance to the international research community.