Granularity control enables high stability and elevated-temperature properties of micron-sized single-crystal LiNi0.5Mn1.5O4 cathodes at high voltage

• Published in: Journal of Materiomics Vol. 7; no. 5; pp. 1049 - 1060
• Main Authors: Liang, Wenbiao, Wang, Peng, Ding, Hao, Wang, Bo, Li, Shiyou
• Format: Journal Article
• Language: English
• Published: Elsevier B.V 01.09.2021; Elsevier
• Subjects: 5 V cathode; Facile synthesis; In-situ EIS; LiNi0.5Mn1.5O4; Micron-sized materials; Single crystals; Single crystals; Facile synthesis; LiNi0.5Mn1.5O4; In-situ EIS; 5 V cathode; Micron-sized materials
• ISSN: 2352-8478
• DOI: 10.1016/j.jmat.2021.02.003

The development of high energy density LiNi0.5Mn1.5O4 (LNMO) cathode materials for lithium-ion batteries are challenged by capacity degradation, which becomes more aggravated particularly at elevated temperatures. Thus, the practical strategy with facile craft and the viability of large-scale preparation for industrialized applications should be developed urgently. In this work, a micron-sized LNMO single crystals is synthesized by a facile two-step method consisting of an alcohol gel solvent method and a segmented sintering reaction. Results show that the truncated polyhedron LNMO-900 sample, with the moderate D50 characteristic value of 4.429 μm and the highest tap density of 2.31 g cm−3, provides a stable structural and chemical stability even at elevated testing temperature due to its moderate specific surface area and the few Fd-3m phase. The LNMO/Li half-cells display more excellent capacity retention (87.3% at 1C and 25 °C after 500 cycles) and better thermal stability (76.65% at 1C and 55 °C after 200 cycles) than those of the single crystals of LNMO-850 and LNMO-950. Besides, the XPS, in-situ EIS and electrochemical tests results also prove that the LNMO-900 exhibits the lowest electrolyte decomposition degree, owing to a thin and effective solid-electrolyte interfacial film formed after cycles. [Display omitted] •Micron-sized LNMO single crystals are synthesized by a facile two-step method.•Truncated polyhedron sample with D50 of 4.429 μm shows a stable structural and chemical stability even at 55 °C.•LNMO-900 sample forms a thin and effective CEI film after cycles.