材料科学
阳极
韧性
复合材料
硅
聚合物
压力(语言学)
电极
化学工程
光电子学
语言学
化学
哲学
物理化学
工程类
作者
Biao Zhang,Yanling Dong,Jingrui Han,Yunjing Zhen,Chuangang Hu,Dong Liu
标识
DOI:10.1002/adma.202301320
摘要
The poor interfacial stability and insufficient cycling performance caused by undesirable stress hinder the commercial application of silicon microparticles (µSi) as next-generation anode materials for high-energy-density lithium-ion batteries. Herein, a conceptionally novel physicochemical dual cross-linking conductive polymeric network is designed combining high strength and high toughness by coupling the stiffness of poly(acrylic acid) and the softness of carboxyl nitrile rubber, which includes multiple H-bonds, by introducing highly branched tannic acid as a physical cross-linker. Such a design enables effective stress dissipation by folded molecular chains slipping and sequential cleavage of H-bonds, thus stabilizing the electrode interface and enhancing cycle stability. As expected, the resultant electrode (µSi/PTBR) delivers an unprecedented high capacity retention of ≈97% from 2027.9 mAh g-1 at the 19th to 1968.0 mAh g-1 at the 200th cycle at 2 A g-1 . Meanwhile, this unique stress dissipation strategy is also suitable for stabilizing SiOx anodes with a much lower capacity loss of ≈0.012% per cycle over 1000 cycles at 1.5 A g-1 . Atomic force microscopy analysis and finite element simulations reveal the excellent stress-distribution ability of the physicochemical dual cross-linking conductive polymeric network. This work provides an efficient energy-dissipation strategy toward practical high-capacity anodes for energy-dense batteries.
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