Regulating Li2S Deposition and Accelerating Conversion Kinetics through Intracavity ZnS toward Low-Temperature Lithium–Sulfur Batteries

IF 9.6 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nano Letters Pub Date : 2024-11-15 DOI:10.1021/acs.nanolett.4c04427

Hao Ding, Zhonghui Chen, Huiyu Li, Huadong Suo, Chaozhong Liu, Huanan Yu, Jingkun Yuan, Zixu Sun, Yanyan Zhu, Bo Song

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Abstract

The uncontrolled deposition behavior and sluggish conversion kinetics of the discharging product (solid Li₂S) severely deteriorate the electrochemical performance of lithium–sulfur (Li–S) batteries, especially under high S loading and low-temperature conditions. Herein, a multifunctional S cathode host consisting of ZnS nanoparticles (NPs) confined in hollow porous carbon spheres (ZnS@HPCS) is synthesized via a unique capillary force-driven melting-diffusion strategy. The porous carbon shell of ZnS@HPCS provides a space-confined reservoir for soluble polysulfides and solid Li₂S, while the intracavity ZnS NPs trap polysulfides, induce Li₂S inside deposition, and accelerate conversion kinetics. Thus, Li–S batteries with ZnS@HPCS-S cathodes exhibit excellent electrochemical performance at both room and low temperatures (−40 °C) and high reversible capacities under high S loading (5.2 mg cm^–2). Furthermore, Li₂S nucleation/deposition, in situ Raman, and theoretical analyses reveal the underlying mechanism. This work offers fundamental insights into regulating Li₂S deposition and designing S hosts for high-performance Li–S batteries.

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通过腔内 ZnS 调节 Li2S 沉积并加速转换动力学，实现低温锂硫电池的目标

放电产物（固态 Li2S）不受控制的沉积行为和缓慢的转化动力学严重恶化了锂硫（Li-S）电池的电化学性能，尤其是在高 S 负载和低温条件下。本文通过一种独特的毛细管力驱动的熔融扩散策略，合成了一种多功能硫阴极宿主，该宿主由封闭在空心多孔碳球（ZnS@HPCS）中的 ZnS 纳米颗粒（NPs）组成。ZnS@HPCS 的多孔碳壳为可溶性多硫化物和固态 Li2S 提供了一个空间封闭的储层，而腔内 ZnS NPs 则捕获多硫化物，诱导 Li2S 在内部沉积，并加速转换动力学。因此，采用 ZnS@HPCS-S 阴极的锂-S 电池在室温和低温（-40 °C）条件下均表现出优异的电化学性能，并且在高 S 负载（5.2 mg cm-2）条件下具有高可逆容量。此外，Li2S 成核/沉积、原位拉曼和理论分析揭示了其基本机制。这项研究为调节 Li2S 沉积和设计高性能锂-S 电池的 S 宿主提供了基本见解。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Nano Letters 工程技术-材料科学：综合

CiteScore

16.80

自引率

2.80%

发文量

1182

审稿时长

1.4 months

期刊介绍： Nano Letters serves as a dynamic platform for promptly disseminating original results in fundamental, applied, and emerging research across all facets of nanoscience and nanotechnology. A pivotal criterion for inclusion within Nano Letters is the convergence of at least two different areas or disciplines, ensuring a rich interdisciplinary scope. The journal is dedicated to fostering exploration in diverse areas, including: - Experimental and theoretical findings on physical, chemical, and biological phenomena at the nanoscale - Synthesis, characterization, and processing of organic, inorganic, polymer, and hybrid nanomaterials through physical, chemical, and biological methodologies - Modeling and simulation of synthetic, assembly, and interaction processes - Realization of integrated nanostructures and nano-engineered devices exhibiting advanced performance - Applications of nanoscale materials in living and environmental systems Nano Letters is committed to advancing and showcasing groundbreaking research that intersects various domains, fostering innovation and collaboration in the ever-evolving field of nanoscience and nanotechnology.