京都大学 / 新制・課程博士 / 博士(エネルギー科学) / 甲第23295号 / エネ博第420号 / 新制||エネ||80(附属図書館) / 京都大学大学院エネルギー科学研究科エネルギー基礎科学専攻 / (主査)教授 萩原 理加, 教授 野平 俊之, 教授 坂口 浩司 / 学位規則第4条第1項該当 / Doctor of Energy Science / Kyoto University / DFAM

Les accumulateurs commerciaux à base de lithium-ion (LIB) utilisent des matériaux à base de carbone (graphite) comme électrode négative; cependant, la technologie atteint sa limite en raison de la faible capacité spécifique théorique. L'objectif de cette thèse est d'étudier le comportement électrochimique de trois nouvelles anodes à haute capacité (SnSb microsturé, Ti3SiC2 anodisé et nanotubes de Si poreux) comme alternatives au graphite, d'identifier les principaux paramètres responsables de la perte de capacité et de proposer une solution commune pour améliorer leurs performances électrochimiques. Ces matériaux d'électrode présentent une bonne performance électrochimique qui les rend prometteurs pour remplacer le carbone en tant qu'électrode négative pour batteries au Li-ion. Cependant, ils présentent une perte de capacité initiale importante qui doit être résolue avant la commercialisation. Les limitations observées sont attribuées à de nombreux facteurs, et en particulier à la formation et la croissance d’une SEI à la surface des matériaux. En raison de la forte perte de la capacité et du manque d’études détaillées sur les matériaux à base d’étain, en particulier le SnSb, nous avons concentré la suite du travail à la formation et la croissance de la SEI sur cette électrode négative. L'évolution des propriétés électriques, de la composition chimique et de la morphologie du SnSb microstructuré a été étudiée en détail pour comprendre son comportement électrochimique. Pour limiter l’effet de la SEI, nous avons proposé d’appliquer un film protecteur à la surface de l'électrode. / Currently, commercial lithium ion batteries (LIBs) use carbon based materials as negative electrode; however the technology is reaching its limit because of the low theoretical specific capacity. The objective of this thesis is to study the electrochemical behaviour of three different new high capacity anodes (SnSb alloy, anodized Ti3SiC2, and Si nanotubes) as alternative to graphite, identify the main parameters responsible for the capacity fading, and propose a versatile solution to improve their electrochemical performance. These electrode materials exhibit good electrochemical performance which makes them promising candidates to replace carbon as a negative electrode for LIBs. However, their limitation due to capacity fading and the large initial irreversible capacity loss must be resolved before commercialization. The observed limitations are attributed to many factors, and particularly, to the formation and growth of SEI layer which is the common factor for all the three electrode materials. Because of the strong capacity fade and lack of many detailed studies on the Sn-based materials, specifically SnSb, we focus our study to investigate the formation and growth of SEI layer on SnSb electrode. The evolution of the electrical, compositional, and morphological properties have been investigated in detail to understand the electrochemical behavior of micron-sized SnSb. To limit the capacity fade, we propose the use of a protective film on the electrode surface. The electrochemical performance of micron-sized SnSb electrode coated with thermoplastic elastomer protective film, namely poly(styrene-b-2-hydroxyethyl acrylate) PS-b-PHEA has been achieved.

Indiana University-Purdue University Indianapolis (IUPUI) / In recent years Lithium-Ion battery as an alternate energy source has gathered lot of importance in all forms of energy requiring applications. Due to its overwhelming benefits over a few disadvantages Lithium Ion is more sought of than any other Battery types. Any battery pack alone cannot perform or achieve its maximum capacity unless there is some robust, efficient and advanced controls developed around it. This control strategy is called Battery Management System or BMS. Most BMS performs the following activity if not all Battery Health Monitoring, Temperature Monitoring, Regeneration Tactics, Discharge Profiles, History logging, etc. One of the major key contributor in a better BMS design and subsequently maintaining a better battery performance and EUL is Regeneration Tactics. In this work, emphasis is laid on understanding the prevalent methods of regeneration and designing a new strategy that better suits the battery performance. A performance index is chosen which aims at minimizing the effort of regeneration along with a minimum deviation from the rated maximum thresholds for cell temperature and regeneration current. Tuning capability is provided for both temperature deviation and current deviation so that it can be tuned based on requirement and battery chemistry and parameters. To solve the optimization problem, Pontryagin's principle is used which is very effective for constraint optimization with both state and input constraints. Simulation results with different sets of tuning shows that the proposed method has a lot of potential and is capable of introducing a new dynamic regeneration tactic for Lithium Ion cells. With the current optimistic results from this work, it is strongly recommended to bring in more battery constraints into the optimization boundary to better understand and incorporate battery chemistry into the regeneration process.

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Electric vehicles contain hundreds of high-energy density lithium-ion batteries. The crashworthiness of these vehicles can be improved by better understanding the response of these batteries in an event of an accident or abusive loads. These loads can induce short-circuit and thermal runways in extreme cases. Therefore, an efficient finite element model of a battery that can precisely predict the coupled multi-physics behavior of a cell in a real-world application is desired. This investigation incorporates detailed and homogenized multi-physics modeling of various form factors of lithium-ion batteries. In the first two chapters of this thesis, a multi-physics homogenized model of a pouch cell was developed and validated in a wide range of multi-disciplines of the battery. In contrast to other similar models described in the literature, which are only applicable in certain scenarios, this model has a much broader range of applications due to the innovative techniques developed for material calibration and cell modeling. In addition, due to the homogenized nature and computational cost efficiency of this technique, the developed model has significance in the crashworthiness analysis of battery packs and electric vehicles where hundreds of these batteries exist. In the final chapter, a detailed layered model of an 18650 cylindrical cell was developed. Component and cell-level tests were performed on the cell to calibrate the material properties and extract the geometries of all the components of the cell. This model is the first of its kind that precisely predicts the load-displacement response and shape of deformation in various loading scenarios. This developed model has crucial importance in the safety assessment of the batteries by providing insight into the sequence of deformation of the internal layers and components and their interplay during mechanical abuse loadings. Overall, the two developed models in this thesis provide battery-related industries with a tool to improve the safety of future electrified industries. / Mechanical Engineering

The pursuit of sustainable and high-performance materials is of utmost significance in driving the progress of battery technologies. Solid-state technology represents a promising avenue for the development of batteries with improved sustainability and performance. In this context, the present study delves into the examination of composition and the substitution of oxygen with nitrogen within the 50Li2O-xSiO2-(50-x)P2O5 glass system, specifically as applied to Solid-State electrolytes. The objective is to evaluate the influence of these factors on the electrical properties of the glass and their potential implications for Solid-State battery technology. The glass matrix was obtained through the melt-quenching technique, followed by comprehensive characterization using electrochemical impedance spectroscopy. The influence of varying silica content on the conductivity of the glass was investigated. This led to the selection of the glass system with the highest conductivity for further experiments involving nitridation. Subsequent experiments on nitridation aimed to explore the impact of nitrogen incorporation on the conductivity of the glass. By systematically varying the nitrogen content at different temperatures, the study sought to elucidate the relationship between nitrogen content and the resulting increase in glass conductivity.    The study reveals a noteworthy finding regarding the impact of nitrogen content on the conductivity of the glass. Specifically, when the nitrogen content was increased, the conductivity increased. In the case of a similar glass composition in pellet form, the conductivity at room temperature increased from Log σ = -8,009 (for glass without nitrogen) to Log σ = -6,951 (for nitrided glass). Additionally, the introduction of nitrogen into the glass resulted in a decrease in activation energy, being reduced from 0,66 eV (for oxide glass) to 0,60 eV (for oxynitride glass). These results indicate a clear correlation between increased nitrogen content and enhanced electrical properties of the investigated glasses; although obtaining a homogeneous bulk glass after nitridation was not feasible. Therefore, the nitrided samples were pelletized and sintered under different thermal conditions to obtain characterizable samples. The findings suggest that nitrogen substitution could be a promising approach for enhancing the electrical properties of the glasses of the title system of composition. Further investigation is required to optimize the process and achieve homogeneous bulk oxynitride glass.