Solid-state batteries are considered the holy grail of next-generation battery technology, meeting the ever-increasing demand for energy storage that is affordable and safe, with high energy density and long cycle life. Materials and interfaces play a critical role for their eventual success and mass commercialization. This issue of MRS Bulletin focuses on the current state of the art of solid-state electrolytes and device architectures and provides a perspective into the various materials and interfacial challenges that limit its performance and stability.

All-solid-state batteries utilizing a ceramic instead of an organic liquid as an electrolyte have the potential to be safer and more energy dense than traditional rechargeable lithium-ion batteries. This emergent energy-storage technology, however, is still critically limited by the performance of the solid electrolyte and its interface with electrodes. Here, we present a review of recent efforts in predictive modeling and materials design for lithium and sodium solid electrolytes using advanced computational approaches. These approaches have enabled the efficient design and discovery of new functional materials with desired properties, such as high alkali ionic conductivity, good phase and electrochemical stability, and low cost, accelerating the development of all-solid-state alkali batteries.

Historically, batteries with lithium metal anodes have been a hazard, as the lithium becomes rough and eventually finely divided during cycling. The promise of higher energy density, however, continues to drive the search for novel approaches to manage this light and reactive material. Significant improvement has been achieved by designing new liquid-electrolyte compositions and interface barriers to stabilize the lithium in traditional batteries, but it is clear that solid-state batteries ensure a higher level of safety and perhaps higher energy density and lifetimes. The materials challenge then is to fabricate a cost-effective solid electrolyte that effectively maintains lithium as a dense uniform metal layer. This article describes the ideal cycling behavior of lithium and progress toward this goal of a solid electrolyte using glassy, ceramic, polymer, and composite electrolytes, as well as the challenges that continue to arise toward long-term, high-rate, and efficient cycling of lithium metal.

Solid inorganic and polymeric electrolytes have the potential to enable rechargeable batteries with higher energy densities, compared to current lithium-ion technology, which uses liquid electrolyte. Inorganic materials such as ceramics and glasses conduct lithium ions well, but they are brittle, which makes incorporation into a battery difficult. Polymers have the flexibility for facile use in a battery, but their transport properties tend to be inferior to inorganics. Thus, there is growing interest in composite electrolytes with inorganic and organic phases in intimate contact. This article begins with a discussion of ion transport in single-phase electrolytes. A dimensionless number (the Newman number) is presented for quantifying the efficacy of electrolytes. An effective medium framework for predicting transport properties of composite electrolytes containing only one conducting phase is then presented. The opportunities and challenges presented by composite electrolytes containing two conducting phases are addressed. Finally, the importance and status of reaction kinetics at the interfaces between solid electrolytes and electrodes are covered, using a lithium-metal electrode as an example.

Solid-state electrolytes can offer improved lithium-ion battery safety while potentially increasing the energy density by enabling alkali metal anodes. There have been significant research efforts to improve the ionic conductivity of solid-state electrolytes and the electrochemical performance of all-solid-state batteries; however, the root causes of their poor performance—interfacial reaction and subsequent impedance growth—are poorly understood. This is due to the dearth of effective characterization techniques for probing these buried interfaces. In situ and operando methodologies are currently under development for solid-state interfaces, and they offer the potential to describe the dynamic interfacial processes that serve as performance bottlenecks. This article highlights state-of-the-art solid–solid interface probing methodologies, describes practical limitations, and describes a future for dynamic interfacial characterization.

Solid-state batteries are promising candidates for energy storage due to their potential advantages in safety, working temperature range, and energy density compared to traditional liquid-electrolyte-based batteries. Rational battery architecture design and a scalable fabrication approach are critical to realize solid-state batteries. In this article, we present the architecture, fabrication procedure, and related challenges of sulfide and oxide electrolyte-based solid-state batteries. Approaches toward intimate solid−solid contact, thin solid-electrolyte fabrication, and scale-up production are discussed. Finally, we discuss the future research directions of solid-state batteries.

The flow of heat in materials is generally perceived to be a slow process and, therefore, pump-probe techniques originally developed for ultrafast time-resolved optical spectroscopy are not an obvious source of technologies for advances in thermal-property measurements. Nevertheless, over the past 18 years, the work of approximately 30 dedicated students and postdoctoral researchers at the University of Illinois at Urbana-Champaign has developed time-domain thermoreflectance (TDTR) into a nearly universal, high-throughput tool for measuring the thermal conductivity of materials and the thermal conductance of materials interfaces. This article illustrates the utility of TDTR and surveys current topics in the science of heat conduction in materials with recent examples drawn from high-thermal-conductivity crystals of cubic boron phosphide and boron arsenide, structure–property relationships for thermal conductivity of amorphous polymers, and thermal conductivity switching in liquid-crystal networks.