Controllable Constructionof CeO<sub>2</sub> Shellswith a Nanoscale Thickness to Enhance the High-Voltage ElectrochemicalPerformance of Ni-Rich Cathodes

Surface coating with metal oxide shells has been widely adopted across various fields due to the exceptional advantages these materials offer. However, achieving the controllable construction of uniform metal oxide shells with nanoscale thickness through a simple and cost-effective method remains challenging, primarily due to the high activity of metal ions. In this work, we proposed a cooperative regulation strategy that was successfully applied to construct uniform CeO<sub>2</sub> shells. Anhydrous ethanol was used as the solvent to reduce the reactivity of Ce(III) ions, while hexamethylenetetramine acted as a precipitant, precisely controlling the precipitation kinetics through its unique slow-release effect. This strategy resulted in high uniformity of the CeO<sub>2</sub> shells and enabled precise regulation of their thickness at the nanoscale, along with control over their crystalline state. The method was successfully applied to coat the LiNi<sub>0.83</sub>Co<sub>0.11</sub>Mn<sub>0.06</sub>O<sub>2</sub> (N83) cathode. By leveraging the advantages of CeO<sub>2</sub> in chemical/thermal stability, oxygen storage capability, and electronic/ionic conductivity, the CeO<sub>2</sub> shell effectively protected the cathode and mitigated lattice oxygen release. As a result, the cycling performance, high-temperature stability, and rate capability of N83 exhibited significant improvements. This work presents a viable approach for the fabrication of controllable metal oxide shells with a nanoscale thickness.

Publication Details

Journal
Figshare
Published
2025-02-03
DOI
https://doi.org/10.1021/acsanm.4c06789.s001
Primary Topic
Diverse Scientific and Economic Studies
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article
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article

Controllable Constructionof CeO2 Shellswith a Nanoscale Thickness to Enhance the High-Voltage ElectrochemicalPerformance of Ni-Rich Cathodes

Figshare
Diverse Scientific and Economic Studies
article

Controllable Constructionof CeO2 Shellswith a Nanoscale Thickness to Enhance the High-Voltage ElectrochemicalPerformance of Ni-Rich Cathodes

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Abstract

Surface coating with metal oxide shells has been widely adopted across various fields due to the exceptional advantages these materials offer. However, achieving the controllable construction of uniform metal oxide shells with nanoscale thickness through a simple and cost-effective method remains challenging, primarily due to the high activity of metal ions. In this work, we proposed a cooperative regulation strategy that was successfully applied to construct uniform CeO<sub>2</sub> shells. Anhydrous ethanol was used as the solvent to reduce the reactivity of Ce(III) ions, while hexamethylenetetramine acted as a precipitant, precisely controlling the precipitation kinetics through its unique slow-release effect. This strategy resulted in high uniformity of the CeO<sub>2</sub> shells and enabled precise regulation of their thickness at the nanoscale, along with control over their crystalline state. The method was successfully applied to coat the LiNi<sub>0.83</sub>Co<sub>0.11</sub>Mn<sub>0.06</sub>O<sub>2</sub> (N83) cathode. By leveraging the advantages of CeO<sub>2</sub> in chemical/thermal stability, oxygen storage capability, and electronic/ionic conductivity, the CeO<sub>2</sub> shell effectively protected the cathode and mitigated lattice oxygen release. As a result, the cycling performance, high-temperature stability, and rate capability of N83 exhibited significant improvements. This work presents a viable approach for the fabrication of controllable metal oxide shells with a nanoscale thickness.

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