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Simultaneously engineering the size and surface crystal facets of bimetallic core-shell nanocrystals offers an effective route to not only reduce the extravagance of innermost core metal and maximize the utilization efficiency of shell atoms but also strengthen the core-to-shell interaction via ligand and/or strain effects. Herein, we systematically study the architecture transition and crystal facet engineering at the atomic level on the surface of sub-5 nm Pd(111) tetrahedrons (Ths), aimed at embodying how the variations in the local

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