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Examples will highlight Pt- or Pd-based nanoparticles and nanowires alloyed with different 3d-TMs with a focus to their architectural evolution under reaction problems. Whilst the dynamic procedure is complex, the capability to gain an insight to the evolution of core-shell and alloy structures underneath the catalytic response problem is essential for advancing the look of multimetallic nanocatalysts. This Account functions as a springboard from fundamental knowledge of the core-shell and alloy