Bimetallic nanocatalysts often have increased activities and stabilities over their monometallic counterparts due to surface strain effects and electron transfer between the two metals. Here, we demonstrate that the performance of a nanocatalyst can be precisely manipulated in shape‐controlled nanocrystals through a bimetallic core@shell architecture. This ability is achieved in a model core@shell Rh@Pt nanocube system through control of shell thickness. The enhanced performance with thin‐shelled nanocrystals is correlated with the weakening of surface–adsorbate interactions. In these thin‐shelled Rh@Pt nanocubes, the maximum current density achieved during formic acid oxidation was over 2 times greater than that achieved with similarly sized Pt nanocubes, with a decreased CO poisoning ratio as well. The strategy employed here should also enhance the performance of many other bimetallic nanomaterials composed of more cost‐effective metals too.

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The performance of nanocatalysts can be enhanced through precise control of bimetallic architecture. For core@shell metal nanocrystals, both the shell thickness and particle shape should be controlled for optimal activity and selectivity. This approach should be generalizable to any structure‐sensitive process when appropriate core and shell materials are selected to impart strain. More information can be found in the Full Paper by S. E. Skrabalak et al. on page 815 in Issue 11, 2017 (DOI: 10.1002/cnma.201700167).

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