Search results

(1 - 2 of 2)
EXAMINING PERFORMANCE DEGRADATION OF LI-ION BATTERIES WITH SILICON-BASED ANODE AND POSSIBLE SOLUTIONS TO IMPROVE THE SILICON ANODE BEHAVIOR
Title
EXAMINING PERFORMANCE DEGRADATION OF LI-ION BATTERIES WITH SILICON-BASED ANODE AND POSSIBLE SOLUTIONS TO IMPROVE THE SILICON ANODE BEHAVIOR
Creator
Luo, Mei
Date
2022
Description
Si has been investigated as a promising alternative to conventional graphite because of its high specific capacity and wide operating voltage;...
Show moreSi has been investigated as a promising alternative to conventional graphite because of its high specific capacity and wide operating voltage; however, technical challenges related to volume change in the silicon anode have hampered their practical application. In this work, the effects of silicon volume change on electrochemical performance has been studied in NMC532/Si full cells. First, different area specific capacity ratios of the negative to positive electrode (N:P ratio) were investigated using three-electrode cells. With individual electrode potentials monitored by a reference electrode, different depths of lithiation/delithiation at the anode and cathode were found to play an important role on cell performance; the cell with higher N:P ratio displays superior electrochemical performance due to its smaller silicon volume change. Further, calendar-life aging and cycle-life aging of NMC532/Si cells were compared with their electrode potentials monitored using a reference electrode. The observation of larger capacity decay and impedance growth of cycle-life aging cells illustrates the important effect of silicon volume change; significant capacity decay of calendar-life aged cell was observed as well, revealing an essential role of chemical effect of ongoing side reactions at Si anode. Specially-designed silicon with different protocols and electrolyte additives were investigated to address the intrinsic challenges of Si anodes for lithium-ion batteries.
Show less
High-Entropy Stabilization as a Designing Tool for Li-Ion Electrodes
Title
High-Entropy Stabilization as a Designing Tool for Li-Ion Electrodes
Creator
Bandeira Jovino Marques, Otavio Jose
Date
2023
Description
High-Entropy oxides (HEOs) form a new class of materials where the configurational entropy plays the stabilizing role of multicomponent...
Show moreHigh-Entropy oxides (HEOs) form a new class of materials where the configurational entropy plays the stabilizing role of multicomponent systems at high temperatures. Recently, it raised much attention for energy storage applications, especially on Li-ion batteries, where the combination of several different elements in a single solid solution can synergistically act to overcome some of its main drawbacks, improving the battery’s performance. The entropy stabilization opens new boundaries on electrode’s design by increasing the compositional space available for different structures and compounds. Not long ago, the high-entropy oxide (Mg0.2Co0.2Ni0.2Cu0.2Zn0.2)O demonstrated a big potential as anode material in Li-ion batteries. Its high capacity and long cycling stability raised a lot of questions about the role of the transition metals in the conversion reaction, and the configurational entropy contribution to the electrochemical reaction, further supporting the electrode’s stability. In order to investigate the structural evolution, the role of the multicomponent oxides and structures on the battery’s performance, and the entropic contribution to the electrode’s stability, this research proposes a systematic and robust methodology around the (Mg0.2Co0.2Ni0.2Cu0.2Zn0.2)O high-entropy oxide (HEO). The project heavily relies on the EXAFS ability to determine the short-range structure and the chemical sensitivity to isolate the elemental contribution of the compound at different cycling and charging states. First, the role of different metallic cations on the electrochemical reaction mechanism of the HEO was analyzed by the change in local structure during different charging steps of a Li-ion battery (Chapter 3). Secondly, the entropy contribution and tunability effects on electrochemical performance were tested in a series of medium and high-entropy oxides derived from the seminal HEO. Mg, Co, Ni, Cu, and Zn were individually removed from the HEO’s composition at a time and tested as Li-ion electrode. Fe was also added to the HEO’s composition (HEO+Fe) in order to prove the tunability effects and entropy contribution (Chapter 4). Operando x-ray absorption spectroscopy (XAS) was used to capture the short lived phases and the transient nature of the conversion reaction, to explain the origins of the extra storage capacity encountered on entropy stabilized systems (Chapter 5). Finally, the role of the high-entropy oxide initial structure was investigated and compared, to check versatility of the elements that can be used on a high-entropy system (Chapter 6).
Show less