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Surface chemistry is important across diverse fields such as corrosion andnanostructure synthesis. Unfortunately, many as-synthesized nanomaterials,including partially dealloyed nanoparticle catalysts for fuel cells, withhighly active surfaces are not stable in their reactive environments,preventing widespread application. Thus, understanding instability by focusingon the structure-stability and defect-stability relationship at the nanoscaleis crucial and will likely play an important role in meeting grand challenges.To this end, recent advances in imaging nanostructure stability have come viaboth electron, x-ray, and other techniques such as atomic force microscopy, buttend to be limited to specific sample environments and/or two-dimensionalimages. Here, we report investigations into the defect-stability relationshipof silver nanoparticles to voltage-induced electrochemical dissolution imagedin-situ in three-dimensional (3D) detail by Bragg Coherent Diffractive Imaging(BCDI). We first determine the average dissolution kinetics by Stationary ProbeRotating Disk Electrode (SPRDE) in combination with inductively coupled plasmamass spectrometry (ICP-MS), which allows real-time in-situ measurement of Ag+ions formation and the corresponding electrochemical current. We then observethe dissolution and redeposition processes in 3D with BCDI in singlenanocrystals, providing unique insight about the role of surface strain,defects, and their coupling to the dissolution chemistry. The methods developedand the knowledge gained go well beyond a "simple" silver electrochemistry andare applicable to all electrocatalytic reactions where functional links betweenactivity and stability are controlled by structure and defect dynamics.

Stability Limits and Surface Chemistry of Ag Nanoparticles in Non-Adsorbing Electrolytes Probed by Bragg Coherent Diffractive Imaging