Insights into electrode architectures and lithium-ion transport in polycrystalline V2O5 cathodes of solid-state batteries

Yu, Zhenjiang, Shan, Hongmei, Zhong, Yunlei, Hong, Guo, Hui, Kwan San ORCID:, Zhang, Xia and Hui, Kwun Nam (2023) Insights into electrode architectures and lithium-ion transport in polycrystalline V2O5 cathodes of solid-state batteries. Small, 19 (43). ISSN 1613-6810

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Polymer-based solid-state batteries (SSBs) have received increasing attentions due to the absence of interfacial problems in sulfide/oxide-type SSBs, but the lower oxidation potential of polymer-based electrolytes greatly limits the application of conventional high-voltage cathode such as LiNixCoyMnzO2 (NCM) and lithium-rich NCM. Herein, this study reports on a lithium-free V2O5 cathode that enables the applications of polymer-based solid-state electrolyte (SSE) with high energy density due to the microstructured transport channels and suitable operational voltage. Using a synergistic combination of structural inspection and non-destructive X-ray computed tomography (X-CT), it interprets the chemo–mechanical behavior that determines the electrochemical performance of the V2O5 cathode. Through detailed kinetic analyses such as differential capacity and galvanostatic intermittent titration technique (GITT), it is elucidated that the hierarchical V2O5 constructed through microstructural engineering exhibits smaller electrochemical polarization and faster Li-ion diffusion rates in polymer-based SSBs than those in the liquid lithium batteries (LLBs). By the hierarchical ion transport channels created by the nanoparticles against each other, superior cycling stability (≈91.7% capacity retention after 100 cycles at 1 C) is achieved at 60 °C in polyoxyethylene (PEO)-based SSBs. The results highlight the crucial role of microstructure engineering in designing Li-free cathodes for polymer-based SSBs.

Item Type: Article
Additional Information: Funding Information: This work was funded by The Science and Technology Development Fund, Macau SAR (File no. 046/2019/AFJ, 0007/2021/AGJ, and 006/2022/ALC), the Multi‐Year Research Grants (MYRG2020‐00187‐IAPME and MYRG2022‐00223‐IAPME) from the Research Services and Knowledge Transfer Office at the University of Macau, and the UEA funding. This work is supported by the Science and Technology Program of Guangdong Province of China (Grant No. 2022A0505030028), the Natural Science Foundation of Shandong Province (File. no. ZR2022QB178). Publisher Copyright: © 2023 Wiley-VCH GmbH.
Uncontrolled Keywords: li-free cathodes,li-ion diffusion,microstructural transmission channels,solid-state batteries,x-ray tomography,biotechnology,chemistry(all),biomaterials,materials science(all),engineering (miscellaneous) ,/dk/atira/pure/subjectarea/asjc/1300/1305
Faculty \ School: Faculty of Science > School of Engineering
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Depositing User: LivePure Connector
Date Deposited: 25 Apr 2024 10:31
Last Modified: 25 Apr 2024 10:31
DOI: 10.1002/smll.202303046

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