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Solid-state sulfur cathodes based on inorganic sulfide solid electrolytes can enable energy-dense lithium batteries. However, volume changes and chemical decomposition can drive delamination and degradation during cycling. To overcome these challenges, this paper reports an in situ approach to encapsulate the solid-state sulfur cathode with a gel polymer electrolyte (GPE). The GPE is covalently bonded with the sulfide solid electrolyte and acts as a barrier that suppresses chemical decomposition between the sulfide solid electrolyte and cathode active material. The elastic GPE maintains interfacial contact within the sulfur cathode allowing for greater sulfur utilization. The solid-state sulfur cathode with GPE demonstrates capacities nearing 700 mAh g −1 and capacity retention over 100 cycles. 

A continuum of water populations can exist in nanoscale layered materials, which impacts transport phenomena relevant for separation, adsorption, and charge storage processes. Quantification and direct interrogation of water structure and organization are important in order to design materials with molecular-level control for emerging energy and water applications. Through combining molecular simulations with ambient-pressure X-ray photoelectron spectroscopy, X-ray diffraction, and diffuse reflectance infrared Fourier transform spectroscopy, we directly probe hydration mechanisms at confined and nonconfined regions in nanolayered transition-metal carbide materials. Hydrophobic (K + ) cations decrease water mobility within the confined interlayer and accelerate water removal at nonconfined surfaces. Hydrophilic cations (Li + ) increase water mobility within the confined interlayer and decrease water-removal rates at nonconfined surfaces. Solutes, rather than the surface terminating groups, are shown to be more impactful on the kinetics of water adsorption and desorption. Calculations from grand canonical molecular dynamics demonstrate that hydrophilic cations (Li + ) actively aid in water adsorption at MXene interfaces. In contrast, hydrophobic cations (K + ) weakly interact with water, leading to higher degrees of water ordering (orientation) and faster removal at elevated temperatures. 

Electrification of the transportation sector relies on radical re-imagining of energy storage technologies to provide affordable, high energy density, durable and safe systems. Next generation energy storage systems will need to leverage high energy density anodes and high voltage cathodes to achieve the required performance metrics (longer vehicle range, long life, production costs, safety). Solid-state batteries (SSBs) are promising materials technology for achieving these metrics by enabling these electrode systems due to the underlying material properties of the solid electrolyte ( viz. mechanical strength, electrochemical stability, ionic conductivity). Electro-chemo-mechanical degradation in SSBs detrimentally impact the Coulombic efficiencies, capacity retention, durability and safety in SSBs restricting their practical implementation. Solid|solid interfaces in SSBs are hot-spots of dynamics that contribute to the degradation of SSBs. Characterizing and understanding the processes at the solid|solid interfaces in SSBs is crucial towards designing of resilient, durable, high energy density SSBs. This work provides a comprehensive and critical summary of the SSB characterization with a focus on in situ and operando studies. Additionally, perspectives on experimental design, emerging characterization techniques and data analysis methods are provided. This work provides a thorough analysis of current status of SSB characterization as well as highlights important avenues for future work. 

Polymer-based hybrid electrolytes are a promissing class of materials for solid-state batteries due to their mechanical, physico-chemical and electrochemical properties. This paper gives an in-depth overview of possible ionic conduction mechanisms essential for good battery performance, and related relevant contemporary materials. The materials' preparation and characterization techniques are given in the light of necessity for deeper understanding of the structure–property relationship in such composites. 

Engineering energy dense electrodes (e.g. lithium metal, conversion cathodes, etc.) with solid electrolytes is important for enhancing the practical energy density of solid-state batteries. However, large electrode volumetric strain can cause significant drive fracture, delamination, and accelerate degradation. This review discusses transport and chemo-mechanical challenges associated with energy dense solid state batteries. In particular, this review focuses on summarizing work which provides design strategies for implementation on energy dense anodes with rigid solid electrolytes. This review further assesses the properties which impact the elasticity of inorganic solid electrolytes and inorganic/organic hybrid electrolyte. Finally, this review discusses the advanced characterization approaches for analyzing the coupled electrochemistry/transport/mechanical phenomena that occur at buried solid-solid interfaces