3 years ago

Synthesis and formation mechanism of carbonate precursor for the fabrication of LiNi0.5Mn1.5O4 material with hierarchical micro/nano architecture

Li Wang, Xing Qin, Guangchuan Liang, Bo Zong, Jianling Guo, Mushang Zhou
Spinel LiNi0.5Mn1.5O4 cathode material with porous hierarchical micro/nano architecture has been successfully prepared by a urea-assisted hydrothermal method followed by high-temperature calcination process. The effects of hydrothermal duration on the structure, morphology and electrochemical performance of carbonate precursor and LiNi0.5Mn1.5O4 cathode material were investigated. The results show that with the hydrothermal duration increasing, the cation disordering degree (Mn3+ content) first decreases and then increases, among which, the LiNi0.5Mn1.5O4 sample synthesized with the carbonate precursor hydrothermally treated 10 h has the lowest Mn3+ content. However, this sample exhibits optimal electrochemical performance, which can be mainly attributed to its smaller particle size and more homogeneous distribution. Based on time-dependent observation, the formation mechanism and phase composition of carbonate precursor have been tentatively explored. The carbonate precursor actually consists of three parts: the inner core MnCO3, the interlayer MnCO3/NiCO3, and the outer shell NiCO3. The formation pathway of the carbonate precursor can be generalized as a mechanism of nucleation-growth-self-assembly-Ostwald ripening for MnCO3 and a mechanism of dissolution-reaction-crystallization for NiCO3.

Publisher URL: http://onlinelibrary.wiley.com/resolve/doi

DOI: 10.1002/ejic.201701196

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