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Abstract:
Selective oxidation of alcohols to aldehydes is widely applicable to the synthesis of various green chemicals. The poor chemo-selectivity for complicated primary aldehydes over state-of-the-art metal-free or metal-based catalysts represents a major obstacle for industrial application. Here we report on bucky nanodiamond as a potential green catalyst which exhibits excellent chemo-selectivity and cycle stability in the selective oxidation of primary alcohols in diverse structures (22 examples, including aromatic, substituted aromatic, unsaturated, heterocycle and linear chain alcohols) to their corresponding aldehydes; the results are even comparable to the reported transition metal catalysts and conventional Pt/C and Ru/C catalysts for certain substrates under solvent-free conditions. The possible activation process of surface oxygen groups and defect species to oxidant and substrate are revealed with model catalysts, ex-situ electrochemical measurement and ex-situ attenuated total reflectance. The zigzag edges of sp2 carbon planes have been shown to play a key role in these reactions.
