定制用于可充电高性能全固态锂电池的阴极有机硫化物外围脂肪族基团

IF 13 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Energy & Environmental Materials Pub Date : 2024-08-06 DOI:10.1002/eem2.12819
Yan Chen, Mingcong Yang, Wei Hu, Tao Chen, Jun Li, Shun Wang, Huile Jin, Jichang Wang
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引用次数: 0

摘要

有机阴极材料具有更高的储能能力,但由于溶解在液态有机电解质中,其循环性较差,这仍然是一个挑战。然而,最近,含有 N-杂环的有机多硫化物的电化学行为揭示了具有稳定循环性能的阴极材料的前景。本文以二硫代烯丙基(甲基)氨基甲酸钠和二乙基二硫代氨基甲酸钠与聚氧化乙烯和 LiTFSI 的聚合物固体电解质的结合为例,介绍了有机硫化物盐作为阴极与固体电解质的结合,解决了有机电极电化学稳定性差的问题。对比分析显示,与二乙基二硫代氨基甲酸钠相比,烯丙基(甲基)二硫代磷酸碳酸钠的电化学性能和稳定性更优越,从而强调了外围脂肪族改性在提高全固态有机锂电池中有机硫化物材料的电极容量、速率性能和电化学稳定性方面的功效。我们还通过动力学分析和热力学分析,探讨了外围脂肪族改性在提高电化学性能方面的作用。此外,利用密度泛函理论计算和原位傅立叶变换红外光谱实验,阐明了 N-C=S 结构在储能机制中的关键作用。这项研究推动了有机硫化物材料的有机正极设计,释放了全固态有机锂电池的潜力,提高了电池的循环能力,推动了下一代储能系统的发展。
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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Tailoring the Periphery Aliphatic Group of Cathode Organosulfide for Rechargeable High-Performance All-Solid-State Lithium Battery
Organic cathode materials exhibit higher energy storage capacity, their poor cyclability due to dissolution in liquid organic electrolytes remains a challenge. However, recently, the electrochemical behavior of organopolysulfides incorporating N-heterocycles unveils promising cathode materials with stable cycling performance. Herein, the integration of organosulfides salt as cathodes with solid electrolytes, exemplified by sodium allyl(methyl)carbamodithioate and sodium diethylcarbamodithioate with a polymer solid electrolyte of polyethylene oxide and LiTFSI, addresses the poor electrochemical stability of organic electrodes. Comparative analysis highlights sodium allyl(methyl)carbamodithioate's superior electrochemical performance and stability compared with sodium diethylcarbamodithioate, emphasizing the efficacy of periphery aliphatic modification in enhancing electrode capacity, rate performance, and electrochemical stability for organosulfide materials within all-solid-state lithium organic batteries. We also explore the origin of periphery aliphatic modification in these enhancing electrochemical performances by kinetic analysis and thermodynamic analysis. Furthermore, employing density functional theory calculations and ex situ FTIR experiments elucidates the critical role of the N–C=S structure in the energy storage mechanism. This research advances organic cathode design within organosulfide materials, unlocking the potential of all-solid-state lithium organic batteries with enhanced cyclability, propelling the development of next-generation energy storage systems.
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来源期刊
Energy & Environmental Materials
Energy & Environmental Materials MATERIALS SCIENCE, MULTIDISCIPLINARY-
CiteScore
17.60
自引率
6.00%
发文量
66
期刊介绍: Energy & Environmental Materials (EEM) is an international journal published by Zhengzhou University in collaboration with John Wiley & Sons, Inc. The journal aims to publish high quality research related to materials for energy harvesting, conversion, storage, and transport, as well as for creating a cleaner environment. EEM welcomes research work of significant general interest that has a high impact on society-relevant technological advances. The scope of the journal is intentionally broad, recognizing the complexity of issues and challenges related to energy and environmental materials. Therefore, interdisciplinary work across basic science and engineering disciplines is particularly encouraged. The areas covered by the journal include, but are not limited to, materials and composites for photovoltaics and photoelectrochemistry, bioprocessing, batteries, fuel cells, supercapacitors, clean air, and devices with multifunctionality. The readership of the journal includes chemical, physical, biological, materials, and environmental scientists and engineers from academia, industry, and policy-making.
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