Design Stable Solid Electrolyte Interphase For Anodes In Rechargeable Lithium Batteries

Solid-electrolyte interphase (SEI) is a nanoscale composite layer of organic and inorganic lithium (Li) salts formed on the electrode surface by electrolyte decomposition. It is ionically conductive and electrically insulating, thus allowing facile Li-ion transport and preventing further electrolyte decomposition. Owing to these features, SEI stability is crucial to the performance of rechargeable Li batteries. Unfortunately, SEI layer are unstable for most advanced battery materials, including high-capacity anodes materials (e.g., silicon (Si) and Li) in liquid electrolyte and Li anodes in solid electrolytes (e.g., Li10GeP2S12 (LGPS)). An unstable SEI layer may cause poor battery performance including consumption of active materials and electrolyte, capacity fading, resistance increase., etc. The structure and property of SEI have generally eluded rational control since its formation and growth processes involve a series of complex and competitive electrochemical reactions. The main efforts to addressing this issue have been made on the development of new electrolyte systems to form alternative SEI layers and preformed artificial SEI layers on the electrode surface to replace the electrolyte-derived SEI.This dissertation focuses on intrinsically regulating the chemical composition and nanostructure of SEI for advanced battery materials in conventional electrolyte systems, which enables not only optimized chemical and physical properties of SEI but improved battery performance. This is realized by developing chemical and electrochemical reactive materials and allowing them to participate in the SEI formation. These materials can contribute functional components in the SEI layer and therefore alter the structure and property of the SEI deliberately. The design of functional material is based on the requirement of SEI layers for different anodes. In Chapters 2 and 3, I presented approaches to manipulating the formation process, chemical composition, and morphology of SEI for nano-sized and micro-sized Si anodes, respectively. The SEI layers were fabricated through a covalent anchoring of multiple functional components onto the Si surface, followed by electrochemical decomposition of the functional components and conventional electrolyte. We showed that to covalently bond organic oligomeric species at the surface of nano-sized Si anodes can effectively increase its SEI flexibility and realized an intimate contact between SEI and Si surface (Chapter 2). In the case of micro-sized Si anodes, we reported that to covalently bond a functional salt, N-methyl-N-propyl pyrrolidinium bis(fluorosulfonyl)imide (PYR13FSI), at the surface of micro-sized Si anodes can effectively stabilize the interface and SEI (Chapter 3). In Chapters 4 and 5, we designed chemically and electrochemically active organic polymer, namely poly((N-2,2-dimethyl-1,3-dioxolane-4-methyl)-5-norbornene-exo-2,3-dicarboximide), and polymeric composite containing poly(vinylsulfonyl fluoride-ran-2-vinyl-1,3-dioxolane) and graphene oxide (GO) nanosheets to alter SEI formation process and regulate the composition and nanostructure of SEI for Li metal anodes. The reactive organic polymer and polymeric composite can generate stable SEI layers in situ by reacting with Li to occupy surface sites and then electrochemically decomposing to form nanoscale SEI components. The formed SEI layers presented excellent surface passivation, homogeneity, and mechanical strength. Using the polymer, we can implant polymeric ether species in the electrolyte-derived SEI, enabling improved SEI flexibility and homogeneity. In the case of polymeric composite, the SEI is mainly generated by the composite instead of electrolyte. In this way, we realized an intrinsic control of SEI structure and property. The formed SEI presented excellent homogeneity, mechanical strength, ionic conductivity, and surface passivation.In Chapter 6, we reported a novel approach based on the use of a nanocomposite consisting of organic elastomeric salts (LiO-(CH2O)n-Li) and inorganic nanoparticle salts (LiF, -NSO2-Li, Li2O), which serve as an interphase to protect Li10GeP2S12 (LGPS), a highly conductive but reducible SSE. The nanocomposite is formed in situ on Li via the electrochemical decomposition of a liquid electrolyte, therefore possessing excellent chemical and electrochemical stability, affinity for Li and LGPS, and limited interfacial resistance. We concluded this dissertation work in Chapter 7 and briefly discussed the possible future work.

This invaluable book focuses on the mechanisms of formation of a solid-electrolyte interphase (SEI) on the electrode surfaces of lithium-ion batteries. The SEI film is due to electromechanical reduction of species present in the electrolyte. It is widely recognized that the presence of the film plays an essential role in the battery performance, and its very nature can determine an extended (or shorter) life for the battery. In spite of the numerous related research efforts, details on the stability of the SEI composition and its influence on the battery capacity are still controversial. This book carefully analyzes and discusses the most recent findings and advances on this topic.

This book provides the first complete and up-to-date summary of the state of the art in HAXPES and motivates readers to harness its powerful capabilities in their own research. The chapters are written by experts. They include historical work, modern instrumentation, theory and applications. This book spans from physics to chemistry and materials science and engineering. In consideration of the rapid development of the technique, several chapters include highlights illustrating future opportunities as well.

A lithium-ion battery comprises essentially three components: two intercalation compounds as positive and negative electrodes, separated by an ionic-electronic electrolyte. Each component is discussed in sufficient detail to give the practising engineer an understanding of the subject, providing guidance on the selection of suitable materials in actual applications. Each topic covered is written by an expert, reflecting many years of experience in research and applications. Each topic is provided with an extensive list of references, allowing easy access to further information. Readership: Research students and engineers seeking an expert review. Graduate courses in electrical drives can also be designed around the book by selecting sections for discussion. The coverage and treatment make the book indispensable for the lithium battery community.

This book covers both the fundamental and applied aspects of advanced Na-ion batteries (NIB) which have proven to be a potential challenger to Li-ion batteries. Both the chemistry and design of positive and negative electrode materials are examined. In NIB, the electrolyte is also a crucial part of the batteries and the recent research, showing a possible alternative to classical electrolytes – with the development of ionic liquid-based electrolytes – is also explored. Cycling performance in NIB is also strongly associated with the quality of the electrode-electrolyte interface, where electrolyte degradation takes place; thus, Na-ion Batteries details the recent achievements in furthering knowledge of this interface. Finally, as the ultimate goal is commercialization of this new electrical storage technology, the last chapters are dedicated to the industrial point of view, given by two startup companies, who developed two different NIB chemistries for complementary applications and markets.

This richly illustrated book written by Professor Kai Peter Birke and several co-authors addresses both scientific and engineering aspects of modern batteries in a unique way. Emphasizing the engineering part of batteries, the book acts as a compass towards next generation batteries for automotive and stationary applications. The book provides distinguished answers to still open questions on how future batteries look like.Modern Battery Engineering explains why and how batteries have to be designed for successful commercialization in e-mobility and stationary applications. The book will help readers understand the principle issues of battery designs, paving the way for engineers to avoid wrong paths and settle on appropriate cell technologies for next generation batteries. This book is ideal for training courses for readers interested in the field of modern batteries.

This book covers the most recent advances in the science and technology of nanostructured materials for lithium-ion application. With contributions from renowned scientists and technologists, the chapters discuss state-of-the-art research on nanostructured anode and cathode materials, some already used in commercial batteries and others still in development. They include nanostructured anode materials based on Si, Ge, Sn, and other metals and metal oxides together with cathode materials of olivine, the hexagonal and spinel crystal structures.

Solid-state batteries hold the promise of providing energy storage with high volumetric and gravimetric energy densities at high power densities, yet with far less safety issues relative to those associated with conventional liquid or gel-based lithium-ion batteries. Solid-state batteries are envisioned to be useful for a broad spectrum of energy storage applications, including powering automobiles and portable electronic devices, as well as stationary storage and load-leveling of renewably generated energy. This comprehensive handbook covers a wide range of topics related to solid-state batteries, including advanced enabling characterization techniques, fundamentals of solid-state systems, novel solid electrolyte systems, interfaces, cell-level studies, and three-dimensional architectures. It is directed at physicists, chemists, materials scientists, electrochemists, electrical engineers, battery technologists, and evaluators of present and future generations of power sources. This handbook serves as a reference text providing state-of-the-art reviews on solid-state battery technologies, as well as providing insights into likely future developments in the field. It is extensively annotated with comprehensive references useful to the student and practitioners in the field.

The Handbook of Lithium-Ion Battery Pack Design: Chemistry, Components, Types and Terminology,?Second Edition provides a clear and concise explanation of EV and Li-ion batteries for readers that are new to the field. The second edition expands and updates all topics covered in the original book, adding more details to all existing chapters and including major updates to align with all of the rapid changes the industry has experienced over the past few years. This handbook offers a layman’s explanation of the history of vehicle electrification and battery technology, describing the various terminology and acronyms and explaining how to do simple calculations that can be used in determining basic battery sizing, capacity, voltage, and energy. By the end of this book the reader will have a solid understanding of the terminology around Li-ion batteries and be able to undertake simple battery calculations. The book is immensely useful to beginning and experienced engineers alike who are moving into the battery field. Li-ion batteries are one of the most unique systems in automobiles today in that they combine multiple engineering disciplines, yet most engineering programs focus on only a single engineering field. This book provides the reader with a reference to the history, terminology and design criteria needed to understand the Li-ion battery and to successfully lay out a new battery concept. Whether you are an electrical engineer, a mechanical engineer or a chemist, this book will help you better appreciate the inter-relationships between the various battery engineering fields that are required to understand the battery as an Energy Storage System. It gives great insights for readers ranging from engineers to sales, marketing, management, leadership, investors, and government officials. Adds a brief history of battery technology and its evolution to current technologies? Expands and updates the chemistry to include the latest types Discusses thermal runaway and cascading failure mitigation technologies? Expands and updates the descriptions of the battery module and pack components and systems?? Adds description of the manufacturing processes for cells, modules, and packs? Introduces and discusses new topics such as battery-as-a-service, cell to pack and cell to chassis designs, and wireless BMS?