LaF3@SiO2 yolk–shell heterostructure nanofiber-modified separator enhances the long-cycling performance of lithium–sulfur batteries

IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL
Yingying Bao , Bin Yue , Lin Li , Hong Shao , Yunrui Xie , Qianli Ma , Wensheng Yu , Jinxian Wang , Xiangting Dong
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引用次数: 0

Abstract

High-energy–density lithium–sulfur (Li–S) cells are identified as one of the most prospective next-generation energy storage appliances owing to their numerous advantages. Nonetheless, their widespread applications are restricted by the unwanted shuttling effect and tardy conversion reaction kinetics of lithium polysulfides (LiPSs). To address these puzzles, we present an innovative strategy for the one-pot synthesis of LaF3@SiO2 yolk–shell heterostructure nanofibers (YSHNFs) through a straightforward uniaxial electrospinning process coupled with fluorination, avoiding the complexities of traditional methods. The specially designed LaF3@SiO2 YSHNFs are utilized as an interlayer to modify a polypropylene (PP) film, creating a LaF3@SiO2/PP separator for long-cycle Li–S batteries. Peculiar “3 + 1” mode anchoring (quadruplex anchoring) and “3 + 1” mode catalysis (quadruplex catalysis) are present in the LaF3@SiO2 YSHNFs, effectively inhibiting the LiPSs shuttling and enhancing their conversion reaction kinetics. Furthermore, the yolk–shell cavity acts as a nanoreactor, advancing the conversion of LiPSs on the LaF3@SiO2 heterostructure. Owing to the strategic design of components and the distinctive structure of LaF3@SiO2 YSHNFs, the combination of the quadruplex anchoring, the quadruplex catalysis, and the nanoreactor collectively contributes to a long-cyclic Li–S battery with high performances. The bare sulfur cathode using the LaF3@SiO2/PP separator exhibits an impressive incipient discharge capacity of 1514 mAh g−1 at 0.2 C and displays a decay rate of only 0.034 % per cycle at 2 C over 600 cycles with a distinguished stability. Density functional theory calculations offer insights into the mechanisms of quadruplex anchoring and catalytic conversion reactions involving the LaF3@SiO2 heterostructure for LiPSs redox process. The strategies for interlayer design, concepts and techniques proposed in this study provide valuable guidance for developing yolk–shell structured materials for advanced long-cyclic Li–S batteries.

Abstract Image

LaF3@SiO2蛋黄壳异质结构纳米纤维改性隔膜提高锂硫电池的长循环性能。
高能量密度锂硫(Li-S)电池由于其众多优点,被认为是最有前途的下一代储能设备之一。然而,它们的广泛应用受到多硫化锂(LiPSs)不必要的穿梭效应和缓慢的转化反应动力学的限制。为了解决这些难题,我们提出了一种创新的策略,通过简单的单轴静电纺丝工艺结合氟化,一锅合成LaF3@SiO2蛋黄壳异质结构纳米纤维(YSHNFs),避免了传统方法的复杂性。特别设计的LaF3@SiO2 YSHNFs用作修饰聚丙烯(PP)膜的中间层,为长周期Li-S电池创建LaF3@SiO2/PP隔膜。LaF3@SiO2 YSHNFs中存在特有的“3 + 1”模式锚定(四联锚定)和“3 + 1”模式催化(四联催化),有效抑制了LiPSs的穿梭,增强了其转化反应动力学。此外,蛋黄壳腔作为纳米反应器,促进了LiPSs在LaF3@SiO2异质结构上的转化。由于组件的战略性设计和LaF3@SiO2 YSHNFs的独特结构,四重锚定、四重催化和纳米反应器的结合共同促成了高性能的长循环Li-S电池。使用LaF3@SiO2/PP分离器的裸硫阴极在0.2 C时显示出令人印象深刻的1514 mAh g-1的初始放电容量,并且在2 C下超过600次循环时显示出每循环仅0.034%的衰减率,并具有出色的稳定性。密度泛函数理论计算提供了对LiPSs氧化还原过程中涉及LaF3@SiO2异质结构的四重锚定和催化转化反应机制的见解。本研究提出的层间设计策略、概念和技术为开发先进长循环锂电池的蛋黄壳结构材料提供了有价值的指导。
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来源期刊
CiteScore
16.10
自引率
7.10%
发文量
2568
审稿时长
2 months
期刊介绍: The Journal of Colloid and Interface Science publishes original research findings on the fundamental principles of colloid and interface science, as well as innovative applications in various fields. The criteria for publication include impact, quality, novelty, and originality. Emphasis: The journal emphasizes fundamental scientific innovation within the following categories: A.Colloidal Materials and Nanomaterials B.Soft Colloidal and Self-Assembly Systems C.Adsorption, Catalysis, and Electrochemistry D.Interfacial Processes, Capillarity, and Wetting E.Biomaterials and Nanomedicine F.Energy Conversion and Storage, and Environmental Technologies
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