Enhanced stability of nitrogen-doped carbon-supported palladium catalyst for oxidative carbonylation of phenol

Enhancing the stability of supported noble metal catalysts emerges is a major challenge in both science and industry.Herein,a heterogeneous Pd catalyst(Pd/NCF)was prepared by supporting Pd ultrafine metal nanoparticles(NPs)on nitrogen-doped carbon;synthesized by using F127 as a stabilizer,as well as chitosan as a carbon and nitrogen source.The Pd/NCF catalyst was efficient and recyclable for oxidative carbonylation of phenol to diphenyl carbonate,exhibiting higher stability than Pd/NC prepared without F127 addition.The hydrogen bond between chitosan(CTS)and F127 was enhanced by F127,which anchored the N in the free amino group,increasing the N content of the carbon material and ensuring that the support could provide sufficient N sites for the deposition of Pd NPs.This process helped to improve metal dispersion.The increased metal-support interaction,which limits the leaching and coarsening of Pd NPs,improves the stability of the Pd/NCF catalyst.Furthermore,density functional theory calculations indicated that pyridine N stabilized the Pd^(2+)species,significantly inhibiting the loss of Pd^(2+)in Pd/NCF during the reaction process.This work provides a promising avenue towards enhancing the stability of nitrogen-doped carbon-supported metal catalysts.

Effect of Alkali Carbonate/Bicarbonate on Citral Hydrogenation over Pd/Carbon Molecular Sieves Catalysts in Aqueous Media

The efficient citral hydrogenation was achieved in aqueous media using Pd/CMS and alkali additives like K2CO3. The alkali concentrations, reaction temperature and the Pd metal content were optimized to enhance the citral hydrogenation under aqueous media. In the absence of alkali, citral hydrogenation was low and addition of alkali promoted to ~92% hydrogenation without reduction in the selectivity to citronellal. The alkali addition appears to be altered the palladium sites. The pore size distribution reveals that the pore size of these catalysts is in the range of 0.96 to 0.7 nm. The palladium active sites are also quite uniform based on the TPR data. The catalytic parameters are correlated well with the activity data.

Pd/TiN nanocomposite catalysts for selective hydrogenation of phenol and its derivatives

Pd/TiN nanocomposite catalysts were fabricated for one-step selective hydrogenation of phenol to cyclohexanone successfully. High conversion of phenol （99%） and selectivity of cyclohexanone （98%） were obtained at 30 ℃ and 0.2 MPa H2 for 12 h in the mixed solvents of H20 and CH2C12. The Pd nanoparticles were stable in the reaction, and no aggregation was detected after four successive runs. The catalytic activity and selectivity depended on slightly the Pd particle sizes. The generality of the catalysts for this reaction was demonstrated by the selective hydrogenation of phenol derivatives, which showed that the catalyst was selective for the formation of cyclohexanone.

CO catalytic oxidation over Pd/CeO2 with different chemical states of Pd

Three Pd/CeO2 catalysts were,respectively,prepared by reduction-deposition and impregnation method(IMP)to investigate the effect of chemical state of Pd on CO oxidation.Two kinds of surface Pd species,namely PdO and Pdδ+(2<δ≤4)in PdxCe1-xO2,were identified in all Pd/CeO2 samples although their relative ratios in each sample were different.Surface PdxCe1-xO2 species were found to be very active for CO oxidation,and it could act as a channel by which active oxygen species can be transferred from CeO2 to Pd species for CO oxidation.Our results reveal that the preparation method can severely influence the chemical state of Pd which can further determine the activity for CO oxidation.