A series of bimetallic Au−Pd alloy nanoparticles (NPs) with varied Au/Pd molar ratios was supported on Gamma‐alumina (γ‐Al2O3) surface through the co‐impregnation‐reduction method using HAuCl4 and PdCl2 as metal precursors. Characterization results suggested the high dispersion of Au−Pd alloy NPs, as well as the interplay between the two compositions. Benefitting from the synergistic effects of Au−Pd alloying, the bimetallic Au‐Pdx@γ‐Al2O3 catalysts were highly efficient for selective aerobic oxidation of various alcohols either aromatic or aliphatic in water using air at atmospheric pressure as a sole oxidant without the need for any cocatalyst. Quantitative yields of corresponding aldehydes or ketones were achieved over Au‐Pd1.2@γ‐Al2O3 within 2 h, whereas pure Au@γ‐Al2O3 or Pd@γ‐Al2O3 was far less efficient. More importantly, the “alloying effect” appeared to stabilize the bimetallic NPs against aggregation and poisoning, which made the Au‐Pdx@γ‐Al2O3 more stable and reusable in the aerobic oxidation of alcohols.
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