{"title":"Origami Silicon Anodes: Geometric Design for Structural Elasticity and Connectivity","authors":"Haimei Li, Ziyun Zhao, Mengwei Sun, Nannan Kuang, Yingxin Liu, Yong Guo, Yibo Zhang, Fanqi Chen, Qinyi Zhan, Anni Liu, Yue Zhai, Qing He, Yunpei Yue, Yun Tian, Shichao Wu, Quan‐Hong Yang","doi":"10.1002/adma.202503745","DOIUrl":null,"url":null,"abstract":"Achieving stable cycling of high‐capacity battery electrodes with large volume changes remains a significant challenge, with their mechanical failure and sluggish kinetics, primarily due to inadequate structural accommodation and inefficient transport pathways. Here, a magnesiothermic crystallization approach is presented to construct origami capsule (OC) architectures, imparting flexibility and conformability to inherently brittle silicon, featuring highly interconnected 2D silicon nanosheets (2.5 nm thickness) with built‐in nanopores encapsulated within a pressure‐tolerant conformal microshell. The design leverages geometric features at both the nanoscale (within nanosheets) and microscale (capsule assembly) to impart structural elasticity and connectivity for efficient stress dissipation, enhancing mechanical integrity and rapid transport kinetics. Consequently, the OC anode exhibits low electrode swelling (14.7%) at 2945 mAh g<jats:sup>−1</jats:sup> and exceptional rate capability, delivering a high capacity and ≈100% retention after 470 cycles at a large current density of 6 A g<jats:sup>−1</jats:sup>. This work bridges geometric design and materials science, opening new avenues for high‐performance energy storage solutions.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"51 1","pages":""},"PeriodicalIF":27.4000,"publicationDate":"2025-05-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Advanced Materials","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1002/adma.202503745","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
Achieving stable cycling of high‐capacity battery electrodes with large volume changes remains a significant challenge, with their mechanical failure and sluggish kinetics, primarily due to inadequate structural accommodation and inefficient transport pathways. Here, a magnesiothermic crystallization approach is presented to construct origami capsule (OC) architectures, imparting flexibility and conformability to inherently brittle silicon, featuring highly interconnected 2D silicon nanosheets (2.5 nm thickness) with built‐in nanopores encapsulated within a pressure‐tolerant conformal microshell. The design leverages geometric features at both the nanoscale (within nanosheets) and microscale (capsule assembly) to impart structural elasticity and connectivity for efficient stress dissipation, enhancing mechanical integrity and rapid transport kinetics. Consequently, the OC anode exhibits low electrode swelling (14.7%) at 2945 mAh g−1 and exceptional rate capability, delivering a high capacity and ≈100% retention after 470 cycles at a large current density of 6 A g−1. This work bridges geometric design and materials science, opening new avenues for high‐performance energy storage solutions.
实现大体积变化的高容量电池电极的稳定循环仍然是一个重大挑战,其机械失效和缓慢的动力学,主要是由于结构调节不足和低效的运输途径。本文提出了一种镁热结晶方法来构建折纸胶囊(OC)结构,赋予固有脆性硅的灵活性和一致性,具有高度互连的2D硅纳米片(2.5 nm厚度),内置纳米孔封装在耐压的保形微壳内。该设计利用了纳米尺度(纳米片内)和微尺度(胶囊组装)的几何特征,赋予结构弹性和连接性,以实现有效的应力消散,增强机械完整性和快速运输动力学。因此,OC阳极在2945 mAh g - 1时表现出低电极膨胀(14.7%)和卓越的倍率能力,在6 a g - 1的大电流密度下,在470次循环后提供高容量和≈100%的保留率。这项工作连接了几何设计和材料科学,为高性能储能解决方案开辟了新的途径。
期刊介绍:
Advanced Materials, one of the world's most prestigious journals and the foundation of the Advanced portfolio, is the home of choice for best-in-class materials science for more than 30 years. Following this fast-growing and interdisciplinary field, we are considering and publishing the most important discoveries on any and all materials from materials scientists, chemists, physicists, engineers as well as health and life scientists and bringing you the latest results and trends in modern materials-related research every week.