Renkun Zhang

It is a challenging task for selective hydrogenation of cinnamaldehyde (CAL) to hydrocinnamaldehyde (HCAL) without additional by-product formation. In this work, a La₂O₃ supported high Ni content nanoparticle catalyst was prepared for CAL selective hydrogenation. Meanwhile, Co-La₂O₃ catalysts were used as a reference catalyst. XRD, TEM, STEM-HAADF, XPS, and H₂-TPR measurements were used to investigate the physicochemical properties of Ni-La₂O₃ catalysts. The experimental results confirmed that the CAL conversion and HCAL selectivity were effectively promoted with the increase of Ni loading amounts. At a Ni/La molar ratio of four, a high HCAL selectivity of 87.4% was obtained at a CAL conversion of 88.1% under mild reaction conditions. The catalyst was recycled five times without activity loss. Combined with various characterizations, it could be inferred that the good hydrogen adsorption and dissociation capacity of Ni and the presence of a certain amount of oxygen vacancies on the La₂O₃ support have a positive effect on the improvement of HCAL selectivity. This work provided an effective path to design transition-metal-based supported oxide catalyst for the cinnamaldehyde hydrogenation to hydrocinnamaldehyde.

Metal-supported catalyst with high activity and relatively simple preparation method is given priority to industrial production. In this work, this study reported an easily accessible synthesis strategy to prepare Mott-Schottky-type N-doped carbon encapsulated metallic Co (Co@N_p+gC) catalyst by high-temperature pyrolysis method in which carbon nitride (g-C₃N₄) and dopamine were used as support and nitrogen source. The prepared Co@N_p+gC presented a Mott-Schottky effect; that is, a strong electronic interaction of metallic Co and N-doped carbon shell was constructed to lead to the generation of Mott-Schottky contact. The metallic Co, due to high work function as compared to that of N-doped carbon, transferred electrons to the N-doped outer shell, forming a new contact interface. In this interface area, the positive and negative charges were redistributed, and the catalytic hydrogenation mainly occurred in the area of active charges. The Co@N_p+gC catalyst showed excellent catalytic activity in the hydrogenation of phenylacetylene to styrene, and the selectivity of styrene reached 82.4%, much higher than those of reference catalysts. The reason for the promoted semi-hydrogenation of phenylacetylene was attributed to the electron transfer of metallic Co, as it was caused by N doping on carbon.