Doctor of Philosophy, The Ohio State University, 2024, Mechanical Engineering
To meet the growing demands of electric vehicles and energy storage devices, it is essential to develop advanced lithium-ion batteries (LIBs) that not only provide high energy density but also affordability and rapid charging and discharging capabilities. Cathode materials account for over 40% of the total cost of a battery and directly determine the battery's voltage and capacity. Therefore, it is imperative to develop low-cost cathode materials with high electrochemical performance. In this dissertation, we explored several cobalt-free cathode materials, including spinel-structured LiNi0.5Mn1.5O4 (LNMO), nickel-rich cobalt-free LiNi0.95M0.05O2 (M=Al, Mn, Mg, and Ti) layered oxides and xLi2MnO3·(1 – x)LiMO2 (M = Ni and Mn) layered oxides (LMR), which have the advantage of low raw materials price compared to commercialized cathode materials, such as LiCoO2 and cobalt-rich LiNi0.33Co0.33Mn0.33O2 (NMC111) layered oxides. However, like most cathode materials, they also encounter significant challenges, including low thermal stability, an unstable internal structure, and rapid capacity fading, which is caused by serious anisotropic volume changes during cycling, continuous electrolyte decomposition, and transition metal dissolution, particularly at high operating voltages.
To overcome these challenges, we present three advanced strategies aimed at producing intergranular-crack-free cathode materials with superior cycling performance, high internal structure stability, and minimal parasitic reactions even under severe cycling conditions. Firstly, employing solid-state electrolytes as Li-ion conductors to form a stable cathode electrolyte interphase (CEI) layer. Secondly, establishing a concentration-gradient layered oxide with a Ni-rich core and an enrichment of substituted elements in the surface region through a co-precipitation reactor. The presence of a Ni-rich core enhances the material's capacity, while the transition elements at the surface ensure excellent cycla (open full item for complete abstract)
Committee: Jung-Hyun Kim Dr. (Advisor); Jay Sayre Dr. (Committee Member); Stephanie Stockar Dr. (Committee Member); Lei Raymond Cao Dr. (Committee Member)
Subjects: Materials Science; Mechanical Engineering