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An economically efficient and operationally simple ligand‐free protocol for the chemoselective oxidation of benzylic alcohols to carbonyl compounds has been developed using alumina‐supported nickel nanoparticles as a stable recyclable heterogeneous catalyst along with potassium tert‐butoxide in the presence of aerial oxygen as an eco‐friendly oxidant. The aliphatic alcohols remained unaffected under the present condition. Excellent chemoselectivity has also been demonstrated through intermolecular and intramolecular competition experiments. This protocol accommodates a diverse range of substituents with the tolerance of various sensitive moieties during the reaction. The catalyst could be recovered by filtration and reused consecutively without any significant loss in the catalytic activity. Moreover, the heterogeneity of the catalyst has also been established by the “hot filtration method (Sheldon's test)”.

An economically efficient ligand-free oxidative conversion of aldehydes to nitriles has been achieved using Cu(OAc)2 and NH4OAc as inexpensive materials of low toxicity in the presence of aerial oxygen as an eco-friendly oxidant.

A novel and transition-metal-free strategy has been developed for the synthesis of aryl esters starting from corresponding benzylic primary alcohols as the exclusive substrates using tert-butyl hydroperoxide (TBHP) as a terminal oxidant in the presence of catalytic amount of tetrabutylammonium iodide (TBAI) and imidazole, where the aliphatic alcohols remained unaffected. These reactions are highly chemoselective and associated with high yield and wide applicability accommodating a wide range of substituents. Excellent chemoselectivity has also been demonstrated through intramolecular competition experiments. This protocol can be considered as an important analogue of Tishchenko reaction using benzylic alcohols as the substrates instead of benzaldehydes.