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Determining Atomic Structure of Grain Boundaries and Heterostructure Interfaces at Solid-State Electrode/Electrolyte Heterostructures in Lithium Based Oxides

Improving upon the current generation of lithium-ion batteries requires a holistic understanding of electrochemical and structural/chemical changes due to work-cycles of the electrodes/electrolyte heterostructure. Multiple mechanisms exist for cell degradation, whether this be through structural fatigue in the bulk of the electrodes or via formation of solid electrolyte interfaces (SEIs). With resolutions achievable below 1 Å in aberration corrected transmission electron microscopy (TEM), structural analysis of grains, grain boundaries, as well as interfaces between electrode (LiCoO 2 , LCO) and electrolyte (Li 7 La 3 Zr 2 O 12 , LLZO) as well as formed current induced SEIs is possible on atomic scale. In this work we focus on the atomic structure of grain boundaries of LCO and LLZO, and the interface between LCO and LLZO with the goal of determining the atomistic structure of the boundaries and interfaces that will allow us to build atomistic models for calculating the electronic properties (including barrier heights etc.) for Li transport/diffusion. The observation of defects and interfacial composition down to atomic resolutions is fundamental to understanding the specific characteristics changing the efficiency of lithium-ion movement through the device. Hence, atomic analysis of working and as prepared devices is the key for understanding the processes that lead to SEIs which will ultimately lead to improved design of solid state battery devices. By combining SEM/EDX/EBSD with HRTEM and STEM/EELS we will present structural and chemical analysis of the