Atomic Origin of Chemomechanical Failure of Layered Cathodes in All-Solid-State Batteries

doi:10.1021/jacs.4c02198

IMR OpenIR

	Atomic Origin of Chemomechanical Failure of Layered Cathodes in All-Solid-State Batteries
	Wang, Chunyang 1,2; Jing, Yaqi 1; Zhu, Dong 1; Xin, Huolin L.1
通讯作者	Xin, Huolin L.(huolin.xin@uci.edu)
	2024-06-14
发表期刊	JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
ISSN	0002-7863
卷号	146 期号:26 页码:17712-17718
摘要	The ever-increasing demand for safety has thrust all-solid-state batteries (ASSBs) into the forefront of next-generation energy storage technologies. However, the atomic mechanisms underlying the failure of layered cathodes in ASSBs, as opposed to their counterparts in liquid electrolyte-based lithium-ion batteries (LIBs), have remained elusive. Here, leveraging artificial intelligence-enhanced super-resolution electron microscopy, we unravel the atomic origins dictating the chemomechanical degradation of technologically crucial high-Ni layered oxide cathodes in ASSBs. We reveal that the coupling of surface frustration and interlayer-shear-induced phase transformation exacerbates the chemomechanical breakdown of layered cathodes. Surface frustration, a phenomenon previously unobserved in liquid electrolyte-based LIBs, emerges through electrochemical processes involving surface nanocrystallization coupled with rock salt transformation. Simultaneously, delithiation-induced interlayer shear yields the formation of chunky O1 phases and intricate interfaces/transition motifs, distinct from scenarios observed in liquid electrolyte-based LIBs. Bridging the knowledge gap between the failure mechanisms of layered cathodes in solid-state electrolytes and conventional liquid electrolytes, our study provides unprecedented atomic-scale insights into the degradation pathways of layered cathodes in ASSBs.
资助者	Basic Energy Sciences ; Office of Basic Energy Sciences of the U.S. Department of Energy ; National Science Foundation through the UC Irvine Materials Research Science and Engineering Center ; UC Irvine
DOI	10.1021/jacs.4c02198
收录类别	SCI
语种	英语
资助项目	Basic Energy Sciences[DE-SC0021204] ; Office of Basic Energy Sciences of the U.S. Department of Energy[DMR-2011967] ; National Science Foundation through the UC Irvine Materials Research Science and Engineering Center ; UC Irvine
WOS研究方向	Chemistry
WOS类目	Chemistry, Multidisciplinary
WOS记录号	WOS:001248680100001
出版者	AMER CHEMICAL SOC
引用统计	被引频次：11[WOS] [WOS记录] [WOS相关记录]
文献类型	期刊论文
条目标识符	http://ir.imr.ac.cn/handle/321006/187176
专题	中国科学院金属研究所
通讯作者	Xin, Huolin L.
作者单位	1.Univ Calif Irvine, Dept Phys & Astron, Irvine, CA 92697 USA 2.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China
推荐引用方式 GB/T 7714	Wang, Chunyang,Jing, Yaqi,Zhu, Dong,et al. Atomic Origin of Chemomechanical Failure of Layered Cathodes in All-Solid-State Batteries[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2024,146(26):17712-17718.
APA	Wang, Chunyang,Jing, Yaqi,Zhu, Dong,&Xin, Huolin L..(2024).Atomic Origin of Chemomechanical Failure of Layered Cathodes in All-Solid-State Batteries.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,146(26),17712-17718.
MLA	Wang, Chunyang,et al."Atomic Origin of Chemomechanical Failure of Layered Cathodes in All-Solid-State Batteries".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 146.26(2024):17712-17718.