Frameworked electrolytes: Ionic transport behavior and high mobility for solid state batteries

IF 22.7 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Infomat Pub Date : 2023-12-18 DOI:10.1002/inf2.12487
Jianguo Sun, Hao Yuan, Jing Yang, Tuo Wang, Yulin Gao, Qi Zhao, Ximeng Liu, Haimei Wang, Yong-Wei Zhang, John Wang
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Abstract

All solid-state batteries (ASSBs) are the holy grails of rechargeable batteries, where extensive searches are ongoing in the pursuit of ideal solid-state electrolytes. Nevertheless, there is still a long way off to the satisfactorily high (enough) ionic conductivity, long-term stability and especially being able to form compatible interfaces with the solid electrodes. Herein, we have explored ionic transport behavior and high mobility in the sub-nano pore networks in the framework structures. Macroscopically, the frameworked electrolyte behaves as a solid, and however in the (sub)-nano scales, the very limited number of solvent molecules in confinement makes them completely different from that in liquid electrolyte. Differentiated from a liquid-electrolyte counterpart, the interactions between the mobile ions and surrounding molecules are subject to dramatic changes, leading to a high ionic conductivity at room temperature with a low activation energy. Li+ ions in the sub-nano cages of the network structure are highly mobile and diffuse rather independently, where the rate-limiting step of ions crossing cages is driven by the local concentration gradient and the electrostatic interactions between Li+ ions. This new class of frameworked electrolytes (FEs) with both high ionic conductivity and desirable interface with solid electrodes are demonstrated to work with Li-ion batteries, where the ASSB with LiFePO4 shows a highly stable electrochemical performance of over 450 cycles at 2°C at room temperature, with an almost negligible capacity fade of 0.03‰ each cycle. In addition, the FE shows outstanding flexibility and anti-flammability, which are among the key requirements of large-scale applications.

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框架电解质:固态电池的离子传输行为和高迁移率
全固态电池(ASSB)是可充电电池中的 "圣杯",目前正在广泛寻找理想的固态电解质。然而,要达到令人满意的高(足够)离子电导率、长期稳定性,特别是能与固体电极形成兼容界面,还有很长的路要走。在此,我们探索了框架结构中亚纳米孔隙网络的离子传输行为和高迁移率。从宏观上看,框架电解质的行为类似于固体,但在(亚)纳米尺度上,溶剂分子的数量非常有限,这使得它们与液态电解质完全不同。与液态电解质不同的是,移动离子与周围分子之间的相互作用发生了巨大变化,从而在室温下以较低的活化能实现了较高的离子电导率。网络结构亚纳米笼中的 Li+ 离子具有高度流动性,扩散相当独立,离子穿过笼子的限速步骤是由局部浓度梯度和 Li+ 离子之间的静电作用驱动的。这种新型框架电解质(FEs)具有高离子电导率和与固体电极的理想界面,已在锂离子电池中得到证实,其中含有 LiFePO4 的 ASSB 在室温 2°C 下显示出高度稳定的电化学性能,循环次数超过 450 次,每次循环的容量衰减几乎可以忽略不计,仅为 0.03‰。此外,FE 还具有出色的柔韧性和抗燃性,而这正是大规模应用的关键要求之一。
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
Infomat
Infomat MATERIALS SCIENCE, MULTIDISCIPLINARY-
CiteScore
37.70
自引率
3.10%
发文量
111
审稿时长
8 weeks
期刊介绍: InfoMat, an interdisciplinary and open-access journal, caters to the growing scientific interest in novel materials with unique electrical, optical, and magnetic properties, focusing on their applications in the rapid advancement of information technology. The journal serves as a high-quality platform for researchers across diverse scientific areas to share their findings, critical opinions, and foster collaboration between the materials science and information technology communities.
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