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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. 

Activity, cost, and durability are the trinity of catalysis research for the electrochemical oxygen reduction reaction (ORR). While studies towards increasing activity and reducing cost of ORR catalysts have been carried out extensively, much effort is needed in durability investigation of highly active ORR catalysts. In this work, we examined the stability of a trimetallic PtPdCu catalyst that has demonstrated high activity and incredible durability during ORR using density functional theory (DFT) based computations. Specifically, we studied the processes of dissolution/deposition and diffusion between the surface and inner layer of Cu species of Pt 20 Pd 20 Cu 60 catalysts at electrode potentials up to 1.2 V to understand their role towards stabilizing Pt 20 Pd 20 Cu 60 catalysts. The results show there is a dynamic Cu surface composition range that is dictated by the interplay of the four processes, dissolution, deposition, diffusion from the surface to inner layer, and diffusion from the inner layer to the surface of Cu species, in the stability and observed oscillation of lattice constants of Cu-rich PtPdCu nanoalloys.