Functional data analysis (FDA) studies data in the form of measurements over a domain as whole entities. Our first focus is on the post-hoc analysis with pairwise and contrast comparisons of the popular functional ANOVA model comparing groups of functional data. Existing contrast tests assume independent functional observations within group. In reality, this assumption may not be satisfactory since functional data are often collected continually overtime on a subject. In this work, we introduce a new linear contrast test that accounts for time dependency among functional group members. For a significant contrast test, it can be beneficial to identify the region of significant difference. In the second part, we propose a non-parametric regression procedure to obtain a locally sparse estimate of functional contrast. Our work is motivated by a biomedical study using Raman spectroscopy to monitor hemodialysis treatment near real-time. With contrast test and sparse estimation, practitioners can monitor the progress of the hemodialysis within session and identify important chemicals for dialysis adequacy monitoring. In the third part, we propose a functional data model for degradation analysis of functional data. Motivated by degradation analysis application of rechargeable Li-ion batteries, we combine state-of-the-art functional linear models to produce fully functional prediction for curves on heterogenous domains. Simulation studies and data analysis demonstrate the advantage of the proposed method in predicting degradation measure than existing method using aggregation method. / Doctor of Philosophy / Functional data analysis (FDA) studies complex data structure in the form of curves and shapes. Our work is motivated by two applications concerning data from Raman spectroscopy and battery degradation study. Raman spectra of a liquid sample are curves with measurements over a domain of wavelengths that can identify chemical composition and whose values signify the constituent concentrations in the sample. We first propose a statistical procedure to test the significance of a functional contrast formed by spectra collected at beginning and at later time points during a dialysis session. Then a follow-up procedure is developed to produce a sparse representation of the contrast functional contrast with clearly identified zero and nonzero regions. The use of this method on contrast formed by Raman spectra of used dialysate collected at different time points during hemodialysis sessions can be adapted for evaluating the treatment efficacy in real time. In a third project, we apply state-of-the-art methodologies from FDA to a degradation study of rechargeable Li-ion batteries. Our proposed methods produce fully functional prediction of voltage discharge curves allowing flexibility in monitoring battery health.

Lithium-ion batteries (LIBs) play a pivotal role in advancing transportation electrification, offering a crucial solution to address climate change and fossil fuel depletion, but the current energy density of LIBs remains unsatisfying, limiting electric transportation range. To address this limitation, extensive efforts focus on developing novel electrode materials, including high-voltage cathodes and high-specific-capacity electrodes. However, the pursuit of higher energy densities introduces safety concerns due to the higher possibility of thermal runaway and flammable nature of conventional liquid electrolytes. In this doctoral thesis, I will present several innovative strategies for high-performance lithium battery systems aimed at enhancing the mileage of electric transportation without compromising or even enhancing safety. The first part (Chapter 3) discusses a novel design for structural batteries. Structural batteries are the energy storage devices with enhanced mechanical properties integrated as structural components in vehicles to reduce vehicle weights and increase mileage. Through the development of a scalable and feasible tree-root-like lamination at the electrode/separator interface, an 11-fold enhancement in the flexural modulus of pouch cells is achieved, and the underlying mechanism is revealed by finite element simulations. This lamination has a minimal impact on the electrochemical performance of LIBs and the smallest reported specific energy reduction of ~3% in structural batteries. The prototype "electric wings" showcases stable flight for an aircraft model, highlighting the effectiveness and scalability of engineering interfacial adhesion in developing structural batteries with superior mechanical and electrochemical properties. The second part (Chapter 4) presents a design rule for polymer electrolytes to enhance lithium metal battery safety. Lithium metal batteries are attractive for electric transportation due to their high energy densities, but their application is hindered by the safety concerns from dendrite growth. In this work, we observe that if the compositions of polyethylene oxide (PEO) electrolytes are near the boundary between amorphous and polymer-rich regions, concentration polarization in electrolytes will induce a phase transformation and create a PEO-rich phase at the electrode surface. This new phase is mechanically rigid with a Young’s modulus of ∼1-3 GPa so that it can suppress lithium dendrites, which allows Li/PEO/LiFePO₄ cells with such a phase transformation demonstrate superior lithium reversibility without dendrites for 100 cycles. The third part (Chapter 5) proposes an innovative cathode design for all-solid-state Li-S batteries (ASSLSBs) which have ultra-high energy densities and enhanced battery safety. However, conventional cathode designs of filling sulfur in carbon hosts suffer from accelerated decomposition of electrolytes and sulfur detachment, leading to significant capacity loss. As a solution, I propose that nonconductive polar hosts allow long cycling life of ASSLSBs via stabilizing the adjacent electrolytes and bonding sulfur/Li₂S steadily to avoid detachment. By using a mesoporous SiO₂host filled with 70 wt.% sulfur as the cathode, we demonstrate steady cycling in ASSLSBs with a capacity reversibility of 95.1% in the initial cycle and a discharge capacity of 1446 mAh g-1 after 500 cycles at C/5.

Energy storage is a necessity for the electrification of the modern world and the progression towards renewable energy. Designing new and innovative energy storage alternatives is one of the many challenges taken on by the Nuckolls group at Columbia University. More precisely, organic materials for energy storage with facile synthesis methods, non-toxic materials, and compatibility with aqueous electrolytes are a focus of this research. For this purpose, Perylenediimide (PDI) is the chosen primary molecular building block, that has enabled design of redox active materials due to its versatility as a structural unit, as well as its remarkable electrochemical performance. In this thesis 3 classes of materials based on PDI - small molecules, polymer networks, and COF materials - are compared; providing insights into how their design impacts electrochemical performance. Chapter 1 provides an overview of existing organic materials for energy storage. In particular, explaining the limitations, challenges, current landscape, and future of organic materials for battery and pseudocapacitive applications. This research area confronts current traditional energy storage strategies, such as lithium-ion batteries, with new organic alternatives that offer opportunities that could be more eco-friendly alternatives to lithium-ion batteries in specific applications. Chapter 2 describes the synthesis and characterization of PHATN, the highest performing aqueous n-type pseudocapacitor based on the PDI molecular backbone integrated into a 3-dimensional polymer network, and the relationship between electrochemical performance and structural contortion generated because of the molecular design. This is accomplished by benchmarking against a non-contorted linear polymer and comparing their electrochemical properties. This work provides the foundation for chapters 3 and 4. Chapter 3 expands on the use of molecular contortion as a design principle for molecular electronics, associating molecular contortion to electrochemical performance by generating helical inspired PDI polymers. This design reveals that the helical motif allows for enhanced electronic communication between the redox moieties and leads to higher device performance. Chapter 4 utilizes linear PDI polymers as a non-contorted control in comparison to the helical inspired polymers described in chapter 3. This linear motif reveals the competing design principle of increased surface area for electrolyte access to redox sites which is shown to increase device performance. Chapter 5 discusses a COF inspired redox active 2-dimensional polymers (RA-2DP) based on PDI materials and how the structural motif and conductive linkers can improve electrochemical performance. This chapter validates the design criteria outlined in chapter 4 and explains how these RA-2DPs and similar structures can enhance energy storage in organic materials. Collectively, this work provides a structured story of PDI materials, their potential as energy storage materials, and the design principles that have led to increased performance. The work completed in this thesis points towards structured and porous redox active organic materials as next generation energy storage alternatives. With the consideration of renewable energy and challenges with existing energy storage options, it is our hope that organic materials will contribute to this ever evolving and growing research area to create a more sustainable and environmentally friendly future.

Formula SAE (FSAE) vehicle systems are very complex. Understanding how subsystems effect the overall vehicle is essential for making design trade-offs. FSAE is a competitive environment. Teams need to have reliable and high performing vehicles to do well in competition. The Virginia Tech (VT) FSAE team has produced a prototype electric powertrain (EPT) vehicle, VTM16e, and will take their first EPT vehicle, VTM17e, to competition in 2017. The use of model-based design (MBD) for an EPT FSAE vehicle is investigated through this thesis. The goal of the research is to build the framework of a full vehicle simulation to take knowledge gained from the VTM16e prototype vehicle, and apply it to the VTM17e competition vehicle. A top-down, bottom-up approach is taken to build a full vehicle model of an EPT FSAE vehicle. A full vehicle simulation is built with subsystems to establish an overall structure and subsystem interactions. Individual subsystems are then focused on for testing and validation. Breaking the vehicle down into subsystems allows the overall model to be incrementally improved. The battery subsystem is focused on in this thesis. Extensive testing is performed on the batteries to characterize their performance. Computer models are generated from empirical data through parameter estimation techniques. Validation of the battery models is performed and the resulting model is incorporated into the overall vehicle model. Performance limits of the vehicle are determined through model exploration, and design modifications to increase the reliability and performance for the VTM17e vehicle are proposed. / Master of Science

<p dir="ltr">This study investigates the electrochemical behavior of molybdenum disulfide (MoS₂) when utilized as an anode material in Li-ion batteries, particularly focusing on the intriguing phenomenon of extra capacity observed beyond theoretical expectations and the unique discharge curve of the first cycle. Employing a robust suite of advanced characterization methods such as in situ and ex situ X-ray diffraction (XRD), Raman spectroscopy, X-ray photoelectron spectroscopy (XPS), and transmission electron microscopy (TEM), the research unravels the complex structural and chemical evolution of MoS₂ throughout its cycling process. A pivotal discovery of the research is the identification of a distinct lithium intercalation mechanism in MoS₂, which leads to the formation of reversible Li_xMoS₂. These phases play a crucial role in contributing to the extra capacity observed in the MoS₂ electrode. Additionally, density functional theory (DFT) calculations have been utilized to explore the potential for overlithiation within MoS₂, suggesting that Li₅MoS₂ could be the most energetically favorable phase during the lithiation-delithiation process. This study also explores the energetics of a Li-rich phase forming on the surface of Li₄MoS2, indicating that this configuration is energetically advantageous and could contribute further to the extra capacity. The incorporation of reduced graphene oxide (RGO) as a conductive additive in MoS₂ electrodes, demonstrating that RGO notably improves the electrochemical performance, rate capability, and durability of the electrodes. These findings are supported by experimental observations and are crucial for advancing the understanding of MoS₂ as a high-capacity anode material. The implications of this research are significant, offering a pathway to optimize the design and composition of electrode materials to exceed traditional performance and longevity limits in Li-ion batteries.</p>

This thesis investigates the lithium-ion dynamics and structural changes in the novel cathode material LiFeV2O7 by solid-state NMR spectroscopy and density functional theory (DFT). With the escalating demand for high-performance lithium-ion batteries (LIBs), exploring cathode materials that can offer superior energy density, cycle stability, and safety is crucial. LiFeV2O7 presents a fascinating structure because it incorporates two transition metals capable of undergoing redox processes, a feature highly beneficial for lithium-ion batteries. The research employs advanced DFT calculations to predict the electronic structure and 7Li NMR shifts. These theoretical insights are essential for understanding how structural disorder influences NMR results and how the oxidation state of transition metal impacts the Fermi contact shift. Experimental techniques, including solid-state NMR spectroscopy and diffraction methods, are applied to study the lithium-ion exchange process and structural evolution during electrochemical cycling. Selective inversion NMR experiments were used to quantify the exchange rates relative to lithiation levels, and in combination with diffraction methods and DFT calculations, enabled the development of a structure model that elucidates the corresponding phase changes in the material. Moreover, the thesis discusses the impact of structural modifications on the lithium-ion dynamics within Li1.71FeV2O7, revealing a direct link between specific crystallographic changes and enhanced lithium mobility. The integration of DFT calculations with experimental observations provides a comprehensive understanding of the material's behavior, paving the way for improvements in cathode design. Overall, this research contributes significantly to the field of LIBs, offering novel insights into the complex interplay between structure, dynamics, and electrochemical performance in cathode materials. / Thesis / Doctor of Science (PhD) / This thesis explores the lithium-ion dynamics and structural changes in the new cathode material LiFeV2O7 using solid-state NMR spectroscopy and density functional theory (DFT). As the demand for high-performance lithium-ion batteries (LIBs) grows, discovering cathode materials with better energy density, stability, and safety becomes crucial. LiFeV2O7 is particularly interesting due to its structure, which includes two transition metals that undergo redox processes. This study combines advanced DFT calculations with experimental techniques to understand how structural disorder and the oxidation state of transition metals affect NMR results. Solid-state NMR spectroscopy and diffraction methods are used to examine lithium-ion exchange and structural changes during battery cycling. The research identifies how specific crystallographic changes enhance lithium mobility, providing insights that can improve cathode design. This comprehensive study contributes to the development of more efficient and stable LIBs by revealing the complex interplay between structure, dynamics, and electrochemical performance.

The invention of the lithium-ion battery has revolutionized the passenger transportation field in recent years, and it has emerged as one of the state-of-the-art solutions to address greenhouse gases emission and air pollution issues. Layered oxide lithium-ion battery cathode materials have become commercially successful in the past few decades due to their high energy density, high power density, long cycle life, and low cost. Yet, with the increasing demand for battery performance, it is crucial to understand the material fading mechanisms further to improve layered oxide materials' performance. A heterogeneous redox reaction is a dominant fading mechanism, which limits the utilization percentage of a battery materials' redox capability and leads to adverse effects such as detrimental interfacial reactions, lattice oxygen release, and chemomechanical breakdown. Crystallographic defects, such as dislocations and grain boundaries, are rich in battery materials. These crystallographic defects change the local lithium-ion diffusivity and have a dramatic effect on the redox reactions. To date, there is still a knowledge gap on how various crystallographic defects affect electrochemistry at the microscopic scale. Herein, we adopted synchrotron-based diffraction, imaging, and spectroscopic techniques to systematically study the correlation between crystallographic defects and redox chemistries in the nanodomain. Our studies shed light on design principles of next-generation battery materials. In Chapter 1, we first provide a comprehensive background introduction on the battery chemistry at various length scales. We then introduce the heterogeneous redox reactions in layered oxide cathode materials, including a discussion on the impacts of heterogeneous redox reactions. Finally, we present the different categories of crystallographic defects in layered oxide materials and how these crystallographic defects affect electrochemical performance. In Chapter 2, we use LiCoO2, a representative layered oxide cathode material, as the material platform to quantify the categories and densities of various crystallographic defects. We then focus on geometrically necessary dislocations as they represent a major class of crystallographic defects in LiCoO2. Combining synchrotron-based X-ray fluorescence mapping, micro-diffraction, and spectroscopic techniques, we reveal that geometrically necessary dislocations can facilitate the charging reactions in LiCoO2 grains. Our study illustrates that the heterogeneous redox chemistries can be potentially mitigated by precisely controlling the defects. In Chapter 3, we systematically investigated how grain boundaries affect redox reactions. We reveal that grain boundaries can guide redox reactions in LiNixMnyCo1-x-yO2 (NMC) materials. Specifically, NMC materials with radially aligned grains have a more uniform charge distribution, less stress mismatch, and better cycling performance. NMC materials with randomly orientated grains have a more heterogeneous redox reaction. These heterogeneous redox reactions are related to the lattice strain mismatch and worse cycling performance. Our study emphasizes the importance of tuning grain orientations to achieve improved performance. Chapter 4 systematically investigated how the grain boundaries and crystallographic orientations affect the thermal stability of layered oxide cathode materials. Combining diffraction, spectroscopic, and imaging techniques, we reveal that a cathode materials' microstructure plays a significant role in determining the lattice oxygen release behavior and, therefore, determines cathode materials' thermal stability. Our study provides a fundamental understanding of how the grain boundaries and crystallographic orientations can be tuned to develop better cathode materials for the next-generation Li-ion batteries. Chapter 5 summarizes the contributions of our work and provides our perspective on future research directions. / Doctor of Philosophy / Lithium-ion battery technology has revolutionized the portable electronic device and electric vehicle markets in recent years. Yet, the performance of current lithium-ion batteries still cannot satisfy customer demands. To further improve battery performance, we need a deeper understanding of why battery materials degrade over long-term cycling. One of the fading mechanisms in lithium-ion batteries is heterogeneous redox reactions, i.e., charge or discharge reactions do not proceed at the same pace at different locations in the electrode materials. Herein, we utilize layered oxide cathode materials as an example to systematically investigate how crystallographic defects in the cathode materials lead to heterogeneous redox reactions. Our study indicates that crystallographic defects, such as geometrically necessary dislocations, contribute positively to the charging reaction of the cathode materials. We also unveil that the grain crystallographic orientations of the primary particles affect the redox reactions directly. By aligning the single grains in the radial direction, the volumetric-change-induced stress can be effectively mitigated to ensure prolonged cycling performance. Our study also points out that the single grain orientations are related to the thermal stability of the battery materials. To summarize, our studies provide new insights into the heterogeneous redox reactions in battery materials and offer critical material design criteria to improve battery performance further.

This case study investigates the potential graphite circular economy within the lithium-ion battery industry, intending to create sustainable management of graphite waste streams. The improper handling of graphite as waste amplifies the carbon footprint and incurs additional costs for battery recyclers. Unlike cathode materials in batteries, graphite regeneration into battery-grade material has not beenindustrialized. Therefore, the study investigates recycling and other alternative approaches to obtain the circularity of graphite. The research explores downcycling, recycling, and upcycling business modelsfor graphite from lithium batteries. With the aim to maximize value and minimize efforts and associated costs. As per methods, an exploratory qualitative method was employed with the data mainly collected through interviews with actors in the graphite sector and recycling technologies. The findings showeconomic viability, feasibility, market dynamic, and regulatory aspects as crucial considerations for the decision-making of battery recyclers. Given the novelty of the material, evaluating technical feasibility through research and development requires coordination with potential partners. Several potential customer options, including graphene applications, steel and refineries, and refractory products, are proposed, each involving a respective business model. Furthermore, the study suggests diversifying partners and establishing partnerships with material receivers as a short-term strategy while awaiting advancements in recycling and upcycling technologies.

<p dir="ltr">Lithium-ion batteries (LIBs) are integral to modern energy storage, with graphite serving as the preferred anode material due to its high conductivity, stability, and affordability. However, challenges related to irreversible initial lithium loss, electrolyte compatibility, and lithium-ion transport kinetics limit the performance and efficiency of graphite anodes. This dissertation addresses these critical issues by exploring novel approaches to enhance the functionality of graphite anodes. The first part of the research investigates the loss of lithium during the formation of the solid electrolyte interphase (SEI) on the graphite anode during the initial charge process. To counter this loss, a new method of graphite pre-SEI is introduced. By preforming SEI layers electrochemically on graphite powders, this technique improves the initial Coulombic efficiency of full cells without sacrificing active cathode material, providing a practical solution for offsetting lithium loss. The second part focuses on overcoming the limitations of traditional electrolyte systems. Graphite's tendency to exfoliate in the presence of organic solvents restricts electrolyte choices, particularly those beyond ethylene carbonate (EC)-based solvents. This chapter presents a new electrolyte design featuring nanoscale anion networks formed by concentrated lithium salts. These networks stabilize graphite by preventing solvent co-intercalation, offering new opportunities for LIBs to operate with a broader range of electrolytes while maintaining electrode integrity. The final chapter of this dissertation re-examines the conventional understanding of lithium-ion transport through the SEI. By constructing SEI-rich structures on a niobium oxide (Nb₂O₅) anode, a new mechanism of lithium transport is proposed. Contrary to the widely accepted two-step diffusion model, findings indicate that lithium transport can occur via a one-step pore diffusion process, eliminating the kinetic limitations previously associated with the SEI and enhancing fast-charging capabilities. In the fourth chapter, a surface modification on graphite surface with a electrochemically active layer is demonstrated to improve the surface diffusion of lithium and thus enhance the low-temperature performance of graphite anodes. The next chapter the high energy density V₂O₅ cathode is revisited with multi-nonmetal doping with improved cycling stability. Overall, this dissertation advances the understanding of graphite anodes in lithium-ion batteries by providing innovative solutions to SEI formation, electrolyte design, and lithium-ion transport, paving the way for more efficient and high-performance energy storage systems.</p>

This work presents a comprehensive investigation into optimizing cathode formulations for lithium-ion batteries (LIBs), focusing on advancing energy density, C-rate capability, and cost efficiency. A special focus was on the measurement and assessment of the electronic conductivity of cathodes. Electrode slurries with varying formulations were prepared and coated, examining the effects of cathode active materials (CAMs), binders, and conductive additives (CAs). Variations in electrode loading and density were done to provide a holistic perspective on electrode production parameters. Electrochemical performance was evaluated through half-coin cells (HCC), electronic resistance meas-urement (ERM), and electrochemical impedance spectroscopy (EIS) using three-electrode cells. Experimental data were used to develop semi-empirical models and behavioral schemes, offering new insights into cathode design. The first key outcome highlights a holistic understanding of cathode development. Comparisons of CAMs such as Lithium-Nickel-Cobalt-Manganese oxide (NCM) and Lith-ium-Manganese-Iron phosphate (LMFP) emphasized the impact of crystal density, press density and specific capacity on the reachable volumetric energy density. Electrode de-sign parameters like electrode loading, press density and porosity were assessed for their impact on C-rate capability, cost and volumetric energy density. Temperature and state-of-charge (SoC) effects on resistance types were characterized, revealing essential impacts on electrode kinetics. Secondly, the thesis focuses on characterizing electronic resistance at the electrode compound and electrode/current collector interface and its correlation with typically used performance indicators such as half coin cells. Using a newly commercially availa-ble electronic resistance measurement device (HIOKI RM2610), electronic resistances were measured, and important impact factors were identified. A total electronic re-sistance (TER) threshold of 0.25 Ω∙cm² was established, below which further perfor-mance gains were not measurable in half coin cells. These findings can enable predic-tions of cathode performance based on electronic resistance measurement (ERM) re-sults, a major contribution to the field of cathode development. Lastly, the gained insights were applied to develop a more efficient cathode optimiza-tion strategy. The integration of electronic resistance measurement (ERM) can signifi-cantly reduce the need for extensive electrochemical testing and can therefore help to make electrode development more time and cost efficient.:1 TABLE OF CONTENTS Danksagung I Abstract II 1 Table of contents 3 2 Symbols and Abbreviations 6 2.1 Formula Symbols and Constants 6 2.2 Abbreviations 7 3 Introduction 9 3.1 Motivation and Aims of the Thesis 9 3.2 Structure of This Thesis 11 4 Fundamentals and State of the Art 13 4.1 Function Principle and Components of a LIB 13 4.1.1 Cathode 15 4.1.2 Anode 15 4.1.3 Electrolyte 15 4.1.4 Separator and Current Collector 16 4.2 Thermodynamics 17 4.2.1 Energy Storage Principle of a LIB 17 4.2.2 Electrical Potential of a LIB 20 4.2.3 Li-Capacity 23 4.3 LIB Cell Kinetics 25 4.3.1 Electronic Resistances in the Cell 29 4.3.2 Electrolyte Resistance 30 4.3.3 Charge-Transfer Resistance 36 4.3.4 Solid State Diffusion Resistance 38 4.4 Cathode Development in LIB 39 4.4.1 Cathode Active Materials (CAM) 39 4.4.2 Conductive Additives (CA) and Binder 41 4.4.3 Cathode Electrode Development 43 4.5 LIB in Automotive Use 44 4.6 Definitions and Relevant Quantities 47 4.6.1 C-rate 47 4.6.2 SoC 47 4.6.3 Cycle Life and State of Health (SoH) 47 4.6.4 Area Types 47 4.6.5 Resistance Normalization 48 4.6.6 Calculation Boundaries 48 5 Materials and Methods 50 5.1 Materials and Electrode Production 50 5.1.1 Active Materials 50 5.1.2 Inactive Materials 50 5.1.3 Electrode Preparation 51 5.2 Cells and Test Methods 52 5.2.1 Thickness Measurement, Press Density and Porosity Calculation 52 5.2.2 Electrode Peel Test 53 5.2.3 Electronic Resistance Measurement (ERM) 53 5.2.4 HCC – C-rate (and OCV) Testing 55 5.2.5 Sandwich Pouch (SWP) – and Testing 55 5.2.6 3-Electrode Cells and EIS Measurements 56 6 Cathode Design Influence Factors 58 6.1 Qualitative Understanding of Cathode Design Influence Factors 58 6.2 Quantifying Influence of Loading, Porosity and C-rate 67 6.3 Quantifying Temperature and SoC Dependencies of Resistance Types 73 6.4 Cathode Design Schematics 85 7 Electronic Resistances in Cathodes 89 7.1 ERM Methods and Their Advantages and Disadvantages 89 7.2 Utilizing and Understanding Dry Multi-point Measurements 97 7.3 Correlation of ERM With HCC Performance 104 7.4 CAs Specific Strengths and Weaknesses 109 7.5 Synergy Effects of CA-mixtures and its Predictability 111 8 Tailored Cathode Designs with Help of ERM 117 8.1 On the Relevance and Need for Binder in a Cathode 117 8.2 Impact of Binder and CA Reduction on Cycle Life 121 8.3 Cathode Optimization Calculations 124 9 Summary and Outlook 131 10 References 135 11 Table of Figures 141 12 Table of Tables 148 13 List of scientific Contributions 149 Appendix 150 Appendix A: Capacities Influenced by CAM Cracking and Diffusion at High Degree of Lithiation 150 Appendix B: Different Operating Windows of LMFP 152 Appendix C: Additional Results for Electronic Resistance in Cathode Measurements 153 Appendix D: Price Assumptions and Calculations 155 Appendix E: Use of Writing Tools for this Work 156 Appendix F: Curriculum vitae 157