Dissertation/Thesis Abstract

Diagnosing, Optimizing and Designing Ni & Mn based Layered Oxides as Cathode Materials for Next Generation Li-ion Batteries and Na-ion Batteries
by Liu, Haodong, Ph.D., University of California, San Diego, 2016, 217; 10161740
Abstract (Summary)

The progressive advancements in communication and transportation has changed human daily life to a great extent. While important advancements in battery technology has come since its first demonstration, the high energy demands needed to electrify the automotive industry have not yet been met with the current technology. One considerable bottleneck is the cathode energy density, the Li-rich layered oxide compounds xLi2MnO3.(1-x)LiMO 2 (M= Ni, Mn, Co) (0.5= Co) (0.5=discharge capacities greater than 280 mAh g-1 (almost twice the practical capacity of LiCoO 2).

In this work, neutron diffraction under operando battery cycling is developed to study the lithium and oxygen dynamics of Li-rich compounds that exhibits oxygen activation at high voltage. The measured lattice parameter changes and oxygen position show movement of oxygen and lattice contractions during the high voltage plateau until the end of charge. Lithium migration kinetics for the Li-rich material is observed under operando conditions for the first time to reveal the rate of lithium extraction from the lithium layer and transition metal layer are related to the different charge and discharge characteristics.

In the second part, a combination of multi-modality surface sensitive tools was applied in an attempt to obtain a complete picture to understand the role of NH4F and Al2O3 surface co-modification on Li-rich. The enhanced discharge capacity of the modified material can be primary assigned to three aspects: decreased irreversible oxygen loss, the activation of cathode material was facilitated with pre-activated Mn3+ on the surface, and stabilization of the Ni redox pair. These insights will provide guidance for the surface modification in high voltage cathode battery materials of the future.

In the last part, the idea of Li-rich has transferred to the Na-ion battery cathode. A new O3 - Na0.78Li0.18Ni0.25Mn 0.583Ow is prepared as the cathode material for Na-ion batteries, delivering exceptionally high energy density and superior rate performance. The single-slope voltage profile and ex situ synchrotron X-ray diffraction data demonstrate that no phase transformation happens through a wide range of sodium concentrations (0.8 Na removed). Further optimization could be realized by tuning the combination and ratio of transition metals.

Indexing (document details)
Advisor: Ying Shirley, Meng
Commitee: Chen, Renkun, Liu, Ping, Luo, Jian, Sinha, Sunil K.
School: University of California, San Diego
Department: NanoEngineering
School Location: United States -- California
Source: DAI-B 78/02(E), Dissertation Abstracts International
Subjects: Engineering, Energy, Materials science
Keywords: Layered oxide cathode, Li-excess, Li-ion batteries, Li-rich, Na-ion batteries, Operando neutron diffraction
Publication Number: 10161740
ISBN: 978-1-369-16602-6
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