Date of Award
Doctor of Philosophy
Materials Science and Engineering
Claus Daniel, Claudia Rawn, Thomas Zawodzinski
Current demands on lithium ion battery (LIB) technology include high capacity retention over a life time of many charge and discharge cycles. Maximizing battery longevity is still a major challenge partly due to electrode degradation as a function of repeated cycling. The intercalation of lithium ions into an active material causes the development of stress and strain in active electrode materials which can result in fracture and shifting that can in turn lead to capacity fade and eventual cell failure. The processes leading to active material degradation in cycling LIBs has been studied using a combination of acoustic emission (AE) and in situ X-ray diffraction (XRD) techniques. Safe, low cost custom electrochemical cells were designed and developed for use in battery AE and XRD experiments. These tools were used to monitor the time of material fracture through AE and link these events to lattice strain and phase composition as determined by XRD. Both anode and cathode materials were studied with an emphasis on graphite, silicon, and Li(Mn1.5Ni0.5)O4, and tin. A thermal analogy model for lithiation/delithiation induced fracture of spherical particles capable of predicting when AE should be detected in a cell containing a composite silicon electrode. The results of this work were used to develop an understanding of when and how active materials are degrading as well as to suggest methods of improving their performance and operational longevity.
Rhodes, Kevin James, "Acoustic Emission and X-Ray Diffraction Techniques for the In Situ Study of Electrochemical Energy Storage Materials. " PhD diss., University of Tennessee, 2011.