期刊
NATIONAL SCIENCE REVIEW
卷 10, 期 3, 页码 -出版社
OXFORD UNIV PRESS
DOI: 10.1093/nsr/nwac272
关键词
all-solid-state batteries; thick electrodes; lithiation; delithiation heterogeneity; tortuosity gradient; synchrotron techniques
A tortuosity-gradient thick electrode was developed to promote fast ion transport and mitigate the heterogeneous solid-state reaction, leading to excellent electrochemical performance for solid-state batteries.
A tortuosity-gradient thick electrode was developed to promote fast ion transport and mitigate the heterogeneous solid-state reaction, leading to excellent electrochemical performance for solid-state batteries. Simultaneously achieving high electrochemical activity and high loading for solid-state batteries has been hindered by slow ion transport within solid electrodes, in particular with an increase in electrode thickness. Ion transport governed by 'point-to-point' diffusion inside a solid-state electrode is challenging, but still remains elusive. Herein, synchronized electrochemical analysis using X-ray tomography and ptychography reveals new insights into the nature of slow ion transport in solid-state electrodes. Thickness-dependent delithiation kinetics are spatially probed to identify that low-delithiation kinetics originate from the high tortuous and slow longitudinal transport pathways. By fabricating a tortuosity-gradient electrode to create an effective ion-percolation network, the tortuosity-gradient electrode architecture promotes fast charge transport, migrates the heterogeneous solid-state reaction, enhances electrochemical activity and extends cycle life in thick solid-state electrodes. These findings establish effective transport pathways as key design principles for realizing the promise of solid-state high-loading cathodes.
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