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Single atom tailored metal nanoparticles represent a new type of catalysts. Herein, we demonstrate a single atom-cavity coupling strategy to regulate performance of single atom tailored nano-catalysts. Selective atomic layer deposition (ALD) was conducted to deposit Ru single atoms on the surface concavities of PtNi nanoparticles (Ru-ca-PtNi). Ru-ca-PtNi exhibits a record-high activity for methanol oxidation reaction (MOR) with 2.01 A mg À 1 Pt . Also, Ru-ca-PtNi showcases a significant durability with only 16 % activity loss. Operando electrochemical Fourier transform infrared spectroscopy (FTIR) and theoretical calculations demonstrate Ru single atoms coupled to cavities accelerate the CO removal by regulating d-band center position. Further, the high diffusion barrier of Ru single atoms in concavities accounts for excellent stability. The developed Ru-ca-PtNi via single atom-cavity coupling opens an encouraging pathway to design highly efficient single atom-based (electro)catalysts.

Non‐precious metal‐based catalysts for oxygen evolution reaction (OER) have been extensively studied, among which the transition metal X‐ides (including phosph‐ides, sulf‐ides, nitr‐ides, and carb‐ides) materials are emerging as promising candidates to replace the benchmark Ir/Ru‐based materials in alkaline media. However, it is controversial whether the metal Xides host the real active sites since these metal Xides are thermodynamically unstable under a harsh OER environment—it has been reported that the initial metal Xides can be electrochemically oxidized and transformed into corresponding oxides and (oxy)hydroxides. Therefore, the metal Xides are argued as “pre‐catalysts”; the electrochemically formed oxides and (oxy)hydroxides are believed as the real active moieties for OER. Herein, the recent advances in understanding the transformation behavior of metal Xides during OER are re‐looked; importantly, hypotheses are provided to understand why the electrochemically formed oxides and (oxy)hydroxides catalysts derived from metal Xides are superior for OER to the as‐prepared metal oxides and (oxy)hydroxides catalysts.