3 years ago

Nanoscale Manipulation of Spinel Lithium Nickel Manganese Oxide Surface by Multisite Ti Occupation as High-Performance Cathode

Nanoscale Manipulation of Spinel Lithium Nickel Manganese Oxide Surface by Multisite Ti Occupation as High-Performance Cathode
Ruying Li, Qian Sun, Mei Cai, Xueliang Sun, Hanshuo Liu, Gianluigi A. Botton, Biwei Xiao, Tsun-Kong Sham, Yang Zhao, Mohammad Norouzi Banis, Karthikeyan Kaliyappan, Biqiong Wang, Jian Liu, Yulong Liu
A novel two-step surface modification method that includes atomic layer deposition (ALD) of TiO2 followed by post-annealing treatment on spinel LiNi0.5Mn1.5O4 (LNMO) cathode material is developed to optimize the performance. The performance improvement can be attributed to the formation of a TiMn2O4 (TMO)-like spinel phase resulting from the reaction of TiO2 with the surface LNMO. The Ti incorporation into the tetrahedral sites helps to combat the impedance growth that stems from continuous irreversible structural transition. The TMO-like spinel phase also alleviates the electrolyte decomposition during electrochemical cycling. 25 ALD cycles of TiO2 growth are found to be the optimized parameter toward capacity, Coulombic efficiency, stability, and rate capability enhancement. A detailed understanding of this surface modification mechanism has been demonstrated. This work provides a new insight into the atomic-scale surface structural modification using ALD and post-treatment, which is of great importance for the future design of cathode materials. A novel method that combines atomic layer deposition of TiO2 and post-annealing has been developed to fully exploit the performance of LiNi0.5Mn1.5O4. The incorporation of Ti into both the tetrahedral and octahedral sites in the spinel structure suppresses the irreversible surface phase transition during initial charge and contributes to improved performance under both room temperature and 55 °C.

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

DOI: 10.1002/adma.201703764

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