The Synergy Between In Situ Gradient Polymerization and Phase Separation Enables Practical Solid-State Ni-Rich Lithium-Ion Batteries.

IF 27.4 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Advanced Materials Pub Date : 2025-07-21 DOI:10.1002/adma.202507621

Hao Zhang,Yalan Zhang,Xiaofan Du,Xuesong Ge,Zhixiang Yuan,Shijie Zhang,Duo Wang,Zhaolin Lv,Xinhong Zhou,Jianjun Zhang,Guanglei Cui

{"title":"The Synergy Between In Situ Gradient Polymerization and Phase Separation Enables Practical Solid-State Ni-Rich Lithium-Ion Batteries.","authors":"Hao Zhang,Yalan Zhang,Xiaofan Du,Xuesong Ge,Zhixiang Yuan,Shijie Zhang,Duo Wang,Zhaolin Lv,Xinhong Zhou,Jianjun Zhang,Guanglei Cui","doi":"10.1002/adma.202507621","DOIUrl":null,"url":null,"abstract":"Solid polymer electrolytes (SPEs) have garnered significant attention due to their exceptional safety property. However, most of the previously reported SPEs cannot well match with high-loading and high-voltage cathodes due to their low ionic conductivity and limited anodic stability. Herein, a SPE with superior compatibility with high-loading Ni-rich cathodes is generated by in situ gradient polymerization of a deep eutectic electrolyte. Besides, a polymerization-induced petaloid phase separation structure enhances interfacial ion transport, resulting in a high room temperature ionic conductivity of 1.5 × 10-3 S cm-1. As a result, the as-assembled high-loading (19.5 mg cm-2) NCM811||graphite full battery exhibites a high capacity retention of 85.3% after 200 cycles and outstanding rate performance (1 C). Industrial 1.2 Ah NCM811||SiOx pouch cell demonstrates unprecefented energy density of 382 Wh kg-1. Moreover, this SPE also exhibits significantly enhanced safety characteristics, delaying the onset temperature of heat release from 157 °C to 266 °C and thermal runaway temperature from 198 °C to 312 °C. This study provides a general and practical avenue to high-energy-density lithium-ion batteries.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"94 1","pages":"e07621"},"PeriodicalIF":27.4000,"publicationDate":"2025-07-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Advanced Materials","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1002/adma.202507621","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}

引用次数: 0

Abstract

Solid polymer electrolytes (SPEs) have garnered significant attention due to their exceptional safety property. However, most of the previously reported SPEs cannot well match with high-loading and high-voltage cathodes due to their low ionic conductivity and limited anodic stability. Herein, a SPE with superior compatibility with high-loading Ni-rich cathodes is generated by in situ gradient polymerization of a deep eutectic electrolyte. Besides, a polymerization-induced petaloid phase separation structure enhances interfacial ion transport, resulting in a high room temperature ionic conductivity of 1.5 × 10-3 S cm-1. As a result, the as-assembled high-loading (19.5 mg cm-2) NCM811||graphite full battery exhibites a high capacity retention of 85.3% after 200 cycles and outstanding rate performance (1 C). Industrial 1.2 Ah NCM811||SiOx pouch cell demonstrates unprecefented energy density of 382 Wh kg-1. Moreover, this SPE also exhibits significantly enhanced safety characteristics, delaying the onset temperature of heat release from 157 °C to 266 °C and thermal runaway temperature from 198 °C to 312 °C. This study provides a general and practical avenue to high-energy-density lithium-ion batteries.

查看原文本刊更多论文

原位梯度聚合和相分离之间的协同作用使实用的固态富镍锂离子电池成为可能。

固体聚合物电解质（spe）由于其特殊的安全性能而引起了人们的广泛关注。然而，先前报道的大多数spe由于其低离子电导率和有限的阳极稳定性而不能很好地与高负载和高压阴极匹配。本文通过深层共晶电解质的原位梯度聚合制备了一种与高负载富镍阴极具有优越相容性的SPE。此外，聚合诱导的花瓣状相分离结构增强了界面离子传输，导致室温离子电导率高达1.5 × 10-3 S cm-1。结果表明，组装后的高负载（19.5 mg cm-2） NCM811||石墨全电池在200次循环后的容量保持率高达85.3%，并且具有出色的倍率性能（1c）。工业1.2 Ah NCM811||SiOx袋电池具有前所未有的382 Wh kg-1能量密度。此外，该SPE还表现出显著增强的安全特性，将热释放的起始温度从157°C推迟到266°C，将热失控温度从198°C推迟到312°C。本研究为高能量密度锂离子电池提供了一条通用实用的途径。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

求助全文

约1分钟内获得全文求助全文

来源期刊

Advanced Materials 工程技术-材料科学：综合

CiteScore

43.00

自引率

4.10%

发文量

2182

审稿时长

2 months

期刊介绍： Advanced Materials, one of the world's most prestigious journals and the foundation of the Advanced portfolio, is the home of choice for best-in-class materials science for more than 30 years. Following this fast-growing and interdisciplinary field, we are considering and publishing the most important discoveries on any and all materials from materials scientists, chemists, physicists, engineers as well as health and life scientists and bringing you the latest results and trends in modern materials-related research every week.