Metallic lithium has been considered one of the most attractive anode materials for high-energy batteries because it has a low density (0.53 g cm8́23), the lowest reduction potential (8́23.04 V vs. the standard hydrogen electrode), and a high theoretical specific capacity (3,860 mAh g8́21). Chalcogen elements, such as sulfur and selenium, have been widely reported as promising cathode candidates for next-generation lithium-metal batteries (LMBs) that demonstrate much higher energy density than current lithium-ion batteries. However, lithium0́3chalcogen batteries still suffer from the loss of cathode active materials and the degradation of lithium metal anode owing to the shuttle effects of intermediate products (e.g., polysulfides and polyselenides), leading to fast capacity fading and poor cyclability. Moreover, for lithium metal anodes, the cracking of solid electrolyte interphase (SEI) layer during long cycling results in dead lithium formation and lithium dendrite growth, leading to poor Coulombic efficiency and potential safety issues. The abovementioned challenges hinder the commercialization of LMBs. To address these problems, various strategies have been developed to mitigate the dissolution/diffusion of redox intermediates and stabilize metallic lithium anodes. In this dissertation, sulfur- and selenium-based nanocomposites were synthesized and employed as advanced cathode materials for high-energy LMBs. The correlations between syntheses, properties, and performances of such chalcogen cathode materials were established by various characterization methods such as microstructural analyses, solid-state nuclear magnetic resonance, X-ray photoelectron spectroscopy, and nanoscale X-ray computed tomography. Additionally, the interfacial electrochemistry of lithium metal anodes and ionic liquid0́3based electrolytes is comprehensively investigated, revealing the effective stabilization and protection of lithium anode via the formation of an in situ SEI layer with specific compositions. Moreover, strategies for achieving novel solid polymer electrolytes with improved lithium-ion transference number were demonstrated, paving the way toward safe LMBs by mitigating lithium dendrite growth. This dissertation provides a combined strategy of advanced cathode design, electrolyte engineering, and lithium anode stabilization to develop high-energy LMBs for practical applications.

This thesis makes significant advances in the design of electrolytes and interfaces in electrochemical cells that utilize reactive metals as anodes. Such cells are of contemporary interest because they offer substantially higher charge storage capacity than state-of-the-art lithium-ion battery technology. Batteries based on metallic anodes are currently considered impractical and unsafe because recharge of the anode causes physical and chemical instabilities that produce dendritic deposition of the metal leading to catastrophic failure via thermal runaway. This thesis utilizes a combination of chemical synthesis, physical & electrochemical analysis, and materials theory to investigate structure, ion transport properties, and electrochemical behaviors of hybrid electrolytes and interfacial phases designed to prevent such instabilities. In particular, it demonstrates that relatively low-modulus electrolytes composed of cross-linked networks of polymer-grafted nanoparticles stabilize electrodeposition of reactive metals by multiple processes, including screening electrode electrolyte interactions at electrochemical interfaces and by regulating ion transport in tortuous nanopores. This discovery is significant because it overturns a longstanding perception in the field of nanoparticle-polymer hybrid electrolytes that only solid electrolytes with mechanical modulus higher than that of the metal electrode are able to stabilize electrodeposition of reactive metals.

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.

Liquid Electrolyte Chemistry for Lithium Metal Batteries An of-the-moment treatment of liquid electrolytes used in lithium metal batteries Considered by many as the most-promising next-generation batteries, lithium metal batteries have grown in popularity due to their low potential and high capacity. Crucial to the development of this technology, electrolytes can provide efficient electrode electrolyte interfaces, assuring the interconversion of chemical and electrical energy. The quality of electrode electrolyte interphase, in turn, directly governs the performance of batteries. In Liquid Electrolyte Chemistry, provides a comprehensive look at the current understanding and status of research regarding liquid electrolytes for lithium metal batteries. Offering an introduction to lithium-based batteries from development history to their working mechanisms, the book further offers a glimpse at modification strategies of anode electrolyte interphases and cathode electrolytic interphases. More, by discussing the high-voltage electrolytes from their solvents—organic solvents and ionic liquids—to electrolyte additives, the text provides a thorough understanding on liquid electrolyte chemistry in the remit of lithium metal batteries. Liquid Electrolyte Chemistry for Lithium Metal Batteries readers will also find: A unique focus that reviews the development of liquid electrolytes for lithium metal batteries State-of-the-art progress and development of electrolytes for lithium metal batteries Consideration of safety, focusing the design principles of flame retardant and non-flammable electrolytes Principles and progress on low temperature and high temperature electrolytes Liquid Electrolyte Chemistry for Lithium Metal Batteries is a useful reference for electrochemists, solid state chemists, inorganic chemists, physical chemists, surface chemists, materials scientists, and the libraries that supply them.

Electrochemical energy systems can successfully exploit beneficial characteristics of electrolyte and/or electrode membranes due to their intriguing peculiarities that make them well-established, standard components in devices such as fuel cells, electrolyzers, and flow batteries. Therefore, more and more researchers are attracted by these challenging yet important issues regarding the performance and behavior of the final device. This Special Issue of Membranes offers scientists and readers involved in these topics an appealing forum to bring and summarize the forthcoming Research & Development results, which stipulates that the composite electrolyte/electrode membranes should be tailored for lithium batteries and fuel cells. Various key aspects, such as synthesis/preparation of materials/components, investigation of the physicochemical and electrochemical properties, understanding of phenomena within the materials and electrolyte/electrode interface, and device manufacturing and performance, were presented and discussed using key research teams from internationally recognized experts in these fields.

Over-consumption of fossil fuels has caused deficiency of limited resources and environmental pollution. Hence, deployment and utilization of renewable energy become an urgent need. The development of next-generation rechargeable batteries that store more energy and last longer has been significantly driven by the utilization of renewable energy.This book starts with principles and fundamentals of lithium rechargeable batteries, followed by their designs and assembly. The book then focuses on the recent progress in the development of advanced functional materials, as both cathode and anode, for next-generation rechargeable batteries such as lithium-sulfur, sodium-ion, and zinc-ion batteries. One of the special features of this book is that both inorganic electrode materials and organic materials are included to meet the requirement of high energy density and high safety of future rechargeable batteries. In addition to traditional non-aqueous rechargeable batteries, detailed information and discussion on aqueous batteries and solid-state batteries are also provided.