Molecular space linkage of dipentacyclic anhydride additives for long-lifespan Li-metal batteries with Ni-rich cathode

IF 18.9 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Energy Storage Materials Pub Date : 2025-02-01 DOI:10.1016/j.ensm.2025.104033
Ridong Hu , Chong Mao , Hao Zhuo , Xiaobing Dai , Lewen Yang , Xugang Shu , Yang Li , Zhanqiang Li , Wenhong Ruan , Fujie Yang , Xudong Chen
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Abstract

The precarious interfacial chemistry between the electrode and electrolyte is the determining step that restricts the long cycle life of Ni-rich-based Li-metal batteries. Here we show that the robust cathode electrolyte interphase (CEI) and solid electrolyte interphase (SEI) layers can be engineered by tuning the spatial linking structure of dipentacyclic anhydride (DPA) additives. Specifically, an inorganic-rich CEI/SEI layer induced by CBDA (a DPA featuring a quaternary ring spatial linking structure) exhibits superior Li+ interfacial kinetics and an ultra-stable cycle performance, outperforming the other systems. As a result, the NCM811ǁLi cells containing CBDA show excellent long-term performances, even under high voltage, high load, and high charge-discharge current density, respectively. The coin-cell using a low-loading cathode exhibits 129 mAh g-1 discharged capacity for over 200 cycles at a 6 C rate. Moreover, The high-loading cathode retains 80 % capacity after 312 cycles at 1.0 C. Furthermore, the NCM811ǁLi pouch cell demonstrated a capacity retention rate of 99.8 % after 50 cycles. Prolonged stable cycling for 900 cycles (93 % capacity retention) in an NCM811ǁGraphite pouch cell is enabled by CBDA. The DPA-based additives in this work offer a highly promising and feasible route to achieving a long-term and high-capacity lithium battery featuring a Ni-rich cathode.

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长寿命富镍锂金属电池双五环酸酐添加剂的分子空间连接
电极与电解液之间不稳定的界面化学是制约富镍锂金属电池长循环寿命的决定性因素。本研究表明,可以通过调整双五环酸酐(DPA)添加剂的空间连接结构来设计坚固的阴极电解质界面层(CEI)和固体电解质界面层(SEI)。具体而言,CBDA(一种具有四环空间连接结构的DPA)诱导的富无机CEI/SEI层表现出优越的Li+界面动力学和超稳定的循环性能,优于其他体系。因此,含有CBDA的NCM811ǁLi电池即使在高电压、高负载和高充放电电流密度下也表现出优异的长期性能。使用低负荷阴极的硬币电池在6℃的倍率下具有129 mAh g-1放电容量超过200次。此外,在1.0℃下,高负载阴极在312次循环后保持80%的容量,NCM811ǁLi袋状电池在50次循环后的容量保持率为99.8%。延长稳定循环900周期(93%容量保留)在NCM811ǁGraphite袋电池是由CBDA启用。本研究中基于dpa的添加剂为实现具有富镍阴极的长期高容量锂电池提供了一条非常有前途和可行的途径。
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来源期刊
Energy Storage Materials
Energy Storage Materials Materials Science-General Materials Science
CiteScore
33.00
自引率
5.90%
发文量
652
审稿时长
27 days
期刊介绍: Energy Storage Materials is a global interdisciplinary journal dedicated to sharing scientific and technological advancements in materials and devices for advanced energy storage and related energy conversion, such as in metal-O2 batteries. The journal features comprehensive research articles, including full papers and short communications, as well as authoritative feature articles and reviews by leading experts in the field. Energy Storage Materials covers a wide range of topics, including the synthesis, fabrication, structure, properties, performance, and technological applications of energy storage materials. Additionally, the journal explores strategies, policies, and developments in the field of energy storage materials and devices for sustainable energy. Published papers are selected based on their scientific and technological significance, their ability to provide valuable new knowledge, and their relevance to the international research community.
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