Thesis (Ph.D.)--University of Wollongong, 2003. / Typescript. Includes bibliographical references: leaf 151-160.

Thesis (Ph.D.)--Rochester Institute of Technology, 2008. / Typescript. Includes bibliographical references (leaves 151-155).

Thesis (Ph. D.)--Columbia University, 1931. / Vita. Bibliography: p. [40].

Thesis (M.S. in Electrical Engineering)--Naval Postgraduate School, June 2002. / Thesis advisor(s): John Ciezki, Sherif Michael. Includes bibliographical references (p. 101-102). Also available online.

Thesis (M. S.)--Electrical and Computer Engineering, Georgia Institute of Technology, 2009. / Committee Chair: Gregory Durgin; Committee Member: Andrew Peterson; Committee Member: Bernard Kippelen.

Thesis (Ph. D.)--Brigham Young University Dept. of Chemical Engineering, 2006. / Includes bibliographical references (p. 155-165).

Thesis (M.Phil.)--University of Hong Kong, 2003. / Includes bibliographical references. Also available in print.

Thesis (Ph. D.)--Florida State University, 2006. / Advisor: Srinivas Palanki, Florida State University, FAMU-FSU College of Engineering, Dept. of Chemical Engineering. Title and description from dissertation home page (viewed June 8, 2006). Document formatted into pages; contains xi, 145 pages. Includes bibliographical references.

Lithium-ion (Li-ion) batteries are the most popular energy storage technology in consumer electronics and electric vehicles and are increasingly applied in stationary storage systems. Yet, concerns about safety and reliability remain major obstacles, which must be addressed in order to improve the acceptance of this technology. The gradual degradation of Li-ion cells over time lies at the heart of this problem. Time, usage and environmental conditions lead to performance deterioration and cell failures, which, in rare cases, can be catastrophic due to res or explosions. The physical and chemical mechanisms responsible for degradation are numerous, complex and interdependent. Our understanding of degradation and failure of Li-ion cells is still very limited and more limited yet are reliable and practical methods for the detection and prediction of these phenomena. This thesis presents a comprehensive approach for the diagnosis and prognosis of degradation in Li-ion cells. The key to this approach is the extraction of information on electrode-speci c degradation through open circuit voltage (OCV) measurements. This is achieved in three stages. Firstly, a parametric OCV model is created, which computes the OCV of each electrode. Secondly, a diagnostic algorithm is devised, through which the OCV model is tted to OCV measurements recorded on Li-ion cells at various stages throughout their cycle life. The algorithm identi es the nature and quanti es the extent of degradation experienced by the cells. Lastly, the outputs of the algorithm are used to identify the likely failure modes of the cells and predict their end-of-life. The presented methods improve safe operation and predictions of remaining useful cycle life for commercial Li-ion cells. Greater certainty about the reliability, safety, required maintenance and depreciation of Li-ion battery systems can signi cantly enhance the competitiveness of battery electric storage in both automotive and stationary applications. The ndings presented in this work are therefore not only of technological but also of commercial interest.

This thesis uses first principles techniques, mainly the ab initio random structure searching method (AIRSS), to study anode materials for lithium- and sodium- ion batteries (LIBs and NIBs, respectively). Initial work relates to a theoretical structure prediction study of the lithium and sodium phosphide systems in the context of phosphorus anodes as candidates for LIBs and NIBs. The work reveals new Li-P and Na-P phases, some of which can be used to better interpret previous experimental results. By combining AIRSS searches with a high-throughput screening search from structures in the Inorganic Crystal Structure Database (ICSD), regions in the phase diagram are correlated to different ionic motifs and NMR chemical shielding is predicted from first principles. An electronic structure analysis of the Li-P and Na-P compounds is performed and its implication on the anode performance is discussed. The study is concluded by exploring the addition of aluminium dopants to the Li-P compounds to improve the electronic conductivity of the system. The following work deals with a study of tin anodes for NIBs. The structure prediction study yields a variety of new phases; of particular interest is a new NaSn$_2$ phase predicted by AIRSS. This phase plays a crucial role in understanding the alloying mechanism of high-capacity tin anodes, work which was done in collaboration with experimental colleagues. Our predicted theoretical voltages give excellent agreement with the experimental electrochemical cycling curve. First principles molecular dynamics is used to propose an amorphous Na$_1$Sn$_1$ model which, in addition to the newly derived NaSn$_2$ phase, provides help in revealing the electrochemical processes. In the subsequent work, we study Li-Sn and Li-Sb intermetallics in the context of alloy anodes for LIBs. A rich phase diagram of Li-Sn is present, exhibiting a variety of new phases. The calculated voltages show excellent agreement with previously reported cycling measurements and a consistent structural evolution of Li-Sn phases as Li concentration increases is revealed. The study concluded by calculating NMR parameters on the hexagonal- and cubic-Li$_3$Sb phases which shed light on the interpretation of reported experimental data. We conclude with a structure prediction study of the pseudobinary Li-FeS$_2$ system, where FeS$_2$ is considered as a potential high-capacity electrochemical energy storage system. Our first principles calculations of intermediate structures help to elucidate the mechanism of charge storage observed by our experimental collaborators via $\textit{in operando}$ studies.