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 futuremore »
This content will become publicly available on June 22, 2023
Kinetics or Transport: Whither Goes the Solid-State Battery Cathode?
Solid-state batteries (SSBs) hold the potential to enhance the energy density, power density, and safety of conventional lithium-ion batteries. The theoretical promise of SSBs is predicated on the mechanistic design and comprehensive analysis of various solid–solid interfaces and microstructural features within the system. The spatial arrangement and composition of constituent phases (e.g., active material, solid electrolyte, binder) in the solid-state cathode dictate critical characteristics such as solid–solid point contacts or singularities within the microstructure and percolation pathways for ionic/electronic transport. In this work, we present a comprehensive mesoscale discourse to interrogate the underlying microstructure-coupled kinetic-transport interplay and concomitant modes of resistances that evolve during electrochemical operation of SSBs. Based on a hierarchical physics-based analysis, the mechanistic implications of solid–solid point contact distribution and intrinsic transport pathways on the kinetic heterogeneity is established. Toward designing high-energy-density SSB systems, the fundamental correlation between active material loading, electrode thickness and electrochemical response has been delineated. We examine the paradigm of carbon-binder free cathodes and identify design criteria that can facilitate enhanced performance with such electrode configurations. A mechanistic design map highlighting the dichotomy in kinetic and ionic/electronic transport limitations that manifest at various SSB cathode microstructural regimes is established.
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- ACS Applied Materials & Interfaces
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- National Science Foundation
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