{"title":"Advanced Hierarchical Lithiophilic Scaffold Design to Facilitate Synchronous Deposition for Dendrite-Free Lithium Metal Batteries","authors":"Jinlong Jiang, Didi Wang, Huakun Liu, Kuan Wu, Xianzhong Yang, Yaru Shi, Bing Zhao, Yong Jiang, Xueliang Sun, Jiujun Zhang, Shixue Dou, Chao Wu","doi":"10.1002/adfm.202417296","DOIUrl":null,"url":null,"abstract":"<p>Localized deposition behavior tends to induce the growth of lithium dendrite and hinder the the full utilization of lithium storage space, significantly impeding the practical application of 3D conductive hosts. Here, a novel synchronous deposition mode is proposed for the first time through hierarchical structure design of 3D Li host. The top-down gradually enhanced lithiophilicity and conductivity of 3D scaffold provide sufficient driving force for Li<sup>+</sup> to migrate downward, promoting synchronous Li deposition within the entire space of the host. Notably, the novel deposition mode has been theoretically and experimentally validated through finite element simulation and in situ optical microscopy, respectively. The meticulously designed strategy not only maximizes the utilization of the entire 3D scaffold space but also prevents the formation of Li dendrites under high current rate. Consequently, the symmetric Li//Li cell exhibits a long-term cycling lifespan over 3700 h with a low overpotential of 15.6 mV, together with a Coulombic efficiency as high as 99.5% over 300 cycles at 3 mA cm<sup>−2</sup>. The full cell paired with LiFePO<sub>4</sub> cathode demonstrates a cycling lifespan of 1000 cycles with a capacity retention rate of 91.6%. The proposed synchronous deposition strategy opens up a new paradigm for the design and construction of 3D hosts for dendrite-free Li metal anode.</p>","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"35 11","pages":""},"PeriodicalIF":18.5000,"publicationDate":"2024-11-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Advanced Functional Materials","FirstCategoryId":"88","ListUrlMain":"https://onlinelibrary.wiley.com/doi/10.1002/adfm.202417296","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
Abstract
Localized deposition behavior tends to induce the growth of lithium dendrite and hinder the the full utilization of lithium storage space, significantly impeding the practical application of 3D conductive hosts. Here, a novel synchronous deposition mode is proposed for the first time through hierarchical structure design of 3D Li host. The top-down gradually enhanced lithiophilicity and conductivity of 3D scaffold provide sufficient driving force for Li+ to migrate downward, promoting synchronous Li deposition within the entire space of the host. Notably, the novel deposition mode has been theoretically and experimentally validated through finite element simulation and in situ optical microscopy, respectively. The meticulously designed strategy not only maximizes the utilization of the entire 3D scaffold space but also prevents the formation of Li dendrites under high current rate. Consequently, the symmetric Li//Li cell exhibits a long-term cycling lifespan over 3700 h with a low overpotential of 15.6 mV, together with a Coulombic efficiency as high as 99.5% over 300 cycles at 3 mA cm−2. The full cell paired with LiFePO4 cathode demonstrates a cycling lifespan of 1000 cycles with a capacity retention rate of 91.6%. The proposed synchronous deposition strategy opens up a new paradigm for the design and construction of 3D hosts for dendrite-free Li metal anode.
局部沉积行为容易诱导锂枝晶生长,阻碍锂存储空间的充分利用,严重阻碍了三维导电主体的实际应用。本文首次提出了一种新型的同步沉积模式,该模式通过三维锂基体的分层结构设计实现。3D支架自上而下逐渐增强的亲石性和电导率为Li+向下迁移提供了足够的动力,促进了整个宿主空间内Li的同步沉积。值得注意的是,这种新的沉积模式已经分别通过有限元模拟和原位光学显微镜进行了理论和实验验证。精心设计的策略不仅可以最大限度地利用整个3D支架空间,还可以防止高电流下锂枝晶的形成。因此,对称锂//锂电池具有超过3700 h的长期循环寿命,过电位低至15.6 mV,在3 mA cm−2下,300次循环的库仑效率高达99.5%。与LiFePO4阴极配对的完整电池循环寿命为1000次,容量保持率为91.6%。所提出的同步沉积策略为无枝晶锂金属阳极三维主体的设计和构建开辟了新的范式。
期刊介绍:
Firmly established as a top-tier materials science journal, Advanced Functional Materials reports breakthrough research in all aspects of materials science, including nanotechnology, chemistry, physics, and biology every week.
Advanced Functional Materials is known for its rapid and fair peer review, quality content, and high impact, making it the first choice of the international materials science community.