In this study,a sulfur–phosphorus co-doped nanocarbon(SPC)catalyst was syn-thesized using a straightforward one-step colloidal carbonization method and demonstrated high performance in the metal-free direct oxidation...In this study,a sulfur–phosphorus co-doped nanocarbon(SPC)catalyst was syn-thesized using a straightforward one-step colloidal carbonization method and demonstrated high performance in the metal-free direct oxidation of alcohols to aldehydes.This metal-free SPC catalyst showed exceptional efficiency,achiev-ing a conversion rate of 90%for benzyl alcohol and a selectivity of 94%toward benzaldehyde within only 1 h at 130◦C.Moreover,it displays exceptional cycle stability and a high turnover frequency(17.1×10-3 mol g-1 h-1).Theoretical analysis suggested that the catalyst’s superior performance is attributed to the presence of unsaturated edge defects and S-P-moieties,which increase the density of states at the Fermi level,lower the band gap energy,and promote electron localization.Additionally,the doping introduces cooperative co-active S-P-C sites,facilitating a synergistic multisite catalytic effect that lowers the energy barriers.These findings represent a significant advancement in the field of metal-free direct alcohol oxidation.展开更多
基金National Natural Science Foundation of China,Grant/Award Numbers:31925028,32301541,22102019。
文摘In this study,a sulfur–phosphorus co-doped nanocarbon(SPC)catalyst was syn-thesized using a straightforward one-step colloidal carbonization method and demonstrated high performance in the metal-free direct oxidation of alcohols to aldehydes.This metal-free SPC catalyst showed exceptional efficiency,achiev-ing a conversion rate of 90%for benzyl alcohol and a selectivity of 94%toward benzaldehyde within only 1 h at 130◦C.Moreover,it displays exceptional cycle stability and a high turnover frequency(17.1×10-3 mol g-1 h-1).Theoretical analysis suggested that the catalyst’s superior performance is attributed to the presence of unsaturated edge defects and S-P-moieties,which increase the density of states at the Fermi level,lower the band gap energy,and promote electron localization.Additionally,the doping introduces cooperative co-active S-P-C sites,facilitating a synergistic multisite catalytic effect that lowers the energy barriers.These findings represent a significant advancement in the field of metal-free direct alcohol oxidation.
