Date of Award
Open Access Dissertation
Chemistry and Biochemistry
The demand for fast, energy-dense storage has driven research into nanoscale intercalation materials. Nanoscale materials not only accelerate kinetics but also can modify reaction path thermodynamics, intercalant solubility, and diffusivity. Pioneering works have revealed such nanoscale changes, often without the need to separately probe each fundamental transport process. While electrodes can be designed to have one transport processes dominant, there remain opportunities to better understand energy-dense designs with multiple concomitant transport constraints. The contents herein highlight emerging an method using tailored, energy-dense nanomaterials and the process of elimination to clearly correlate architectural features to performance. For example, this method revealed the dependance of intercalation pseudocapacitive kinetics upon the intercalation length scale for multiple materials. In addition, this approach can isolate material-specific effects such as how amorphization modifies both insertion and diffusion kinetics for multiple materials exhibiting intercalation pseudocapacitance. A recently developed current-model deconvolves changes to surface-limited and diffusion-limited processes while at the same time revealing avenues to achieve markedly faster intercalation. Future directions are suggested including synthetic methods emphasizing tailored defects, characterization methods with minimal assumptions, and computer simulations that include diffusion with non-uniform concentrations.
van den Bergh, W.(2022). Tailored Nanomaterials for Advancing Fast-Charge Research. (Doctoral dissertation). Retrieved from https://scholarcommons.sc.edu/etd/6848