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pectroscopy) and microscopy (e.g., high-resolution transmission electron microscopy (HRTEM) and atomic force microscopy (AFM)) for gaining valuable insights into the qualitative and quantitative nature of not only the inner core and outer shell themselves but also their intervening interface. While probing the functional catalytic behavior of a few of these core-shell structures under realistic operando conditions, using dynamic, in situ characterization techniques, we found that local and subtle changes in chemical composition and phy