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Pt‐based electrocatalysts are considered as one of the most promising choices to facilitate the oxygen reduction reaction (ORR), and the key factor enabling their success is to reduce the required amount of platinum. Herein, we focus on illuminating both the theoretical mechanisms which enable enhanced and sustained ORR activity and the practical methods to achieve them in catalysts. The various multi‐step pathways of ORR are firstly reviewed and the rate‐determining steps based on the reaction intermediates and their binding energies are analyzed. We then explain the critical aspects of Pt‐based electrocatalysts to tune oxygen reduction properties from the viewpoints of active sites exposure and altering the surface electronic structure, and further summarize representative research progress towards practically achieving these activity enhancements with a focus on platinum size reduction, shape control and core Pt elimination methods. We finally outline the remaining challenges and provide our perspectives with regard to further enhancing their activities. [ABSTRACT FROM AUTHOR]

In article number 1802427, Zhengyu Bai, Zhongwei Chen, and co‐workers reveal orbital interactions of Bi‐Sn nanostructures, leading to the electrocatalytic conversion of CO2 to formate with high selectivity, activity, and durability. This is attributed to the electronic states of Sn upshifting away from the Fermi level due to the coupling with Bi, making the HCOO* intermediate adsorb more favorably on Bi‐Sn than on pure Sn surfaces. This study provides sub‐atomic level insights into bimetallic catalyst development for highly selective CO2 reduction. [ABSTRACT FROM AUTHOR]