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Abstract The ability to control the electrode interfaces in an electrochemical energy storage system is essential for achieving the desired electrochemical performance. However, achieving this ability requires an in-depth understanding of the detailed interfacial nanostructures of the electrode under electrochemical operating conditions. In-situ transmission electron microscopy (TEM) is one of the most powerful techniques for revealing electrochemical energy storage mechanisms with high spatiotemporal resolution and high sensitivity in complex electrochemical environments. These attributes play a unique role in understanding how ion transport inside electrode nanomaterials and across interfaces under the dynamic conditions within working batteries. This review aims to gain an in-depth insight into the latest developments of in-situ TEM imaging techniques for probing the interfacial nanostructures of electrochemical energy storage systems, including atomic-scale structural imaging, strain field imaging, electron holography, and integrated differential phase contrast imaging. Significant examples will be described to highlight the fundamental understanding of atomic-scale and nanoscale mechanisms from employing state-of-the-art imaging techniques to visualize structural evolution, ionic valence state changes, and strain mapping, ion transport dynamics. The review concludes by providing a perspective discussion of future directions of the development and application of in-situ TEM techniques in the field of electrochemical energy storage systems. 

Abstract The ability to control phase structures and surface sites of ultrasmall alloy nanoparticles under reaction conditions is essential for preparing catalysts by design. This is, however, challenging due to limited understanding of the atomic‐scale phases and their correlation with the ensemble‐averaged structures and activities of catalysts during catalytic reactions. We reveal here a dynamic structural stability of alumina‐supported ultrasmall and equiatomic copper‐gold alloy nanoparticles under reaction conditions as a model system in the in situ/operando study. In situ atomic‐scale morphological tracking under oxygen reveals temperature‐dependent dynamic crystalline‐amorphous dual‐phase structures, showing dynamic stability over an elevated temperature range. This atomic‐scale dynamic phase stability coincides with a “conversion plateau” observed for carbon monoxide oxidation on the catalyst. It is substantiated by the stable lattice ordering/disordering structures and surface sites with oscillatory characteristics shown by operando ensemble‐average structural tracking of the catalyst during the oxidation reaction. The understanding of the atomic‐scale dynamic phase structures in correlation with the ensemble‐average dynamic ordering/disordering phase structures and surface sites provides fresh insights into the unique synergy of the supported alloy nanoparticles. This understanding has implications for the design and structural tuning of active and stable ultrasmall alloy catalysts under elevated temperatures.