Pd _1.5 H ₂ @PdO Nanoparticles Nanoconfined in Nitrogen‐Doped Carbon for the Aerobic Oxidation Benzaldehydes to Arylnitriles

ABSTRACT The design of efficient, sustainable catalytic systems for the aerobic oxidation of benzaldehyde to aryl nitriles is of great interest in organic synthesis. In this study, we introduce a novel catalyst confined in nitrogen‐doped carbon (NC), which combines palladium‐hydride (Pd _1.5 H ₂ ) and palladium oxide (PdO) nanoparticles, as Pd _1.5 H ₂ @PdO NC. This catalyst was synthesized via a simple cellulose collosol co‐doping carbonization strategy. The nitrogen‐doped carbon support features a high surface area and a well‐developed nanopore structure, significantly improving the dispersion and accessibility of the co‐active sites. When applied to the aerobic oxidation of benzaldehyde with ammonia, the catalyst demonstrated outstanding performance, achieving a benzaldehyde conversion rate of 99.89% using air as the oxidant. Additionally, the catalyst showed excellent versatility, maintaining high conversion rates across a wide range of substituted benzaldehydes. The observed catalytic efficiency is attributed to the synergy between the Pd‐H species, which promotes hydrogen transfer or hydrogen abstraction, and the PdO phase, which is effective in oxidation reactions. This study provides an eco‐friendly approach to nitrile synthesis and highlights the potential of optimizing multi‐active sites on high‐surface‐area supports for advanced catalytic applications in oxidation processes.