Synergistic effects of La loading on furfural hydrogenation using wrinkled silica-supported Pd catalysts: Role of partially oxidized Pd and base sites

Abstract

The catalytic hydrogenation of furfural (FF) to tetrahydrofurfuryl alcohol (THFAL) is complicated by competing hydrogenation reactions involving the carbonyl group and furan ring. To address this challenge, we developed Pd/xLa@wrinkled silica (Pd/xLa@KCC) catalysts exhibiting excellent efficiency via the optimization of La/Si molar ratios, improved Pd dispersion, and stabilization of partially oxidized Pd particles (Pdδ+). These catalysts were designed for the selective hydrogenation of FF to THFAL. Pd/0.2La@KCC, characterized by a high level of oxygen defects, good basicity, and abundant Pdδ+ species, achieved complete conversion and 91.2 % THFAL selectivity at 45 °C within 6 h. Pd/0.2La@KCC exhibited a THFAL formation rate of 100.9 mmol/g/h, 10.8 times higher than that of Pd/0.02La@KCC. Improved Pd dispersion increased the available metallic surface area for H2 dissociations, whereas abundant Lewis-base sites and Pdδ+ species served as adsorption sites for the carbonyl group and furan ring, respectively. The catalyst facilitated the activation and conversion of the furan ring and carbonyl group to THFAL owing to the parallel adsorption geometry of FF. This approach highlights the importance of the surface characteristics of the catalyst for achieving exceptional selectivity and efficiency. Our findings provide valuable insights into the development of advanced catalysts exhibiting excellent selectivity for biomass-derived chemicals.