A Fluorine-Free Binder with Organic–Inorganic Crosslinked Networks Enabling Structural Stability of Ni-Rich Layered Cathodes in Lithium-Ion Batteries

IF 18.5 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Advanced Functional Materials Pub Date : 2024-08-11 DOI:10.1002/adfm.202410866
Junho Jang, Junho Ahn, Jinho Ahn, Uktae Jeong, Jihee Yoon, Jun Kyu Park, Woohyeon Shin, Min Jeong Kang, Min-kyung Cho, Dong Jun Kang, Jongsoon Kim, Jung-Keun Yoo, Hyeon-Gyun Im
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Abstract

Although the high-energy Ni-rich layered cathodes suffer from undesirable surface reactions with the electrolyte, the polyvinylidene fluoride (PVDF) binder has a limitation on surface stabilization because of its weak affinity and low adhesion/cohesion. Here, it is demonstrated that the novel fluorine-free and hydroxyl-rich siloxane nanohybrid (SNH) binder can enhance the electrochemical performances of LiNi0.8Mn0.1Co0.1O2 cathode (NCM811) via successful surface stabilization. The high silanol content in the SNH binder enhances the affinity to both NCM811 and conductive agent, facilitating uniform electron/ion pathways with high mass loading, improved shear thinning, and superior mechanical properties. Moreover, the fluorine-free organic-inorganic hybrid structure prevents the dissolution of transition metals, active material structural changes, and electrolyte interaction, leading to greatly enhanced cyclability of the SNH-based NCM811 electrode (≈81.9% in half-cell; ≈87.82% in full-cell after 200 cycles) compared to PVDF-based NCM811 electrode (≈58.8% in half-cell; ≈61.24% in full-cell after 200 cycles). Various analyses also indicate that the application of the fluorine-free SNH binder successfully stabilizes both the surface and bulk structure of the NCM811 cathode during charge/discharge. The binder design represents a straightforward yet highly effective approach to achieving remarkably prolonged cyclability in lithium-ion batteries, surpassing the performance of other fluorine-based or polymer-based binders.

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一种具有有机-无机交联网络的无氟粘合剂,可确保锂离子电池中富镍层状阴极的结构稳定性
虽然高能富镍层状阴极会与电解质发生不良的表面反应,但聚偏二氟乙烯(PVDF)粘结剂因其亲和力弱、粘附力/内聚力低而在表面稳定方面存在局限性。本文证明,新型无氟且富含羟基的硅氧烷纳米杂化(SNH)粘结剂可通过成功的表面稳定化提高镍钴锰酸锂(NCM811)阴极的电化学性能。SNH 粘合剂中的高硅烷醇含量增强了与 NCM811 和导电剂的亲和力,从而促进了均匀的电子/离子通道,实现了高负载质量,改善了剪切稀化,并具有优异的机械性能。此外,无氟有机-无机杂化结构可防止过渡金属溶解、活性材料结构变化和电解质相互作用,从而大大提高了基于 SNH 的 NCM811 电极的可循环性(半电池≈81.9%;200 次循环后全电池≈87.82%),而基于 PVDF 的 NCM811 电极的可循环性仅为(半电池≈58.8%;200 次循环后全电池≈61.24%)。各种分析还表明,在充放电过程中,无氟 SNH 粘结剂的应用成功地稳定了 NCM811 阴极的表面和体积结构。这种粘合剂设计是实现锂离子电池显著延长循环性能的一种简单而高效的方法,其性能超过了其他氟基或聚合物基粘合剂。
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来源期刊
Advanced Functional Materials
Advanced Functional Materials 工程技术-材料科学:综合
CiteScore
29.50
自引率
4.20%
发文量
2086
审稿时长
2.1 months
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.
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