Hydrogenation of 4-(2-furyl)-3-buten-2-one using Cu-double layered hydroxides modified with Zr and Ce

Abstract

The hydrogenation of 4-(2-furyl)-3-buten-2-one (FAc), derived from biomass through the aldol condensation of furfural and acetone, to obtain jet-fuel precursors and high-value products has been primarily performed using noble metals. In this study, the hydrogenation of FAc was studied using modified catalysts in which aluminum in CuMgAl double-layered hydroxides was partially or fully substituted with cerium (Ce) and zirconium (Zr) to induce oxygen vacancies. These vacancies were introduced to enhance catalytic performance by modifying the hydroxide structure. Characterization techniques, including N₂ adsorption–desorption, H₂-temperature-programmed reduction (TPR-H₂), N₂O-chemisorption, O₂-temperature-programmed desorption (TPD-O₂), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS), were employed to characterize catalysts. The complete substitution of the Al layer with Ce or Zr significantly enhanced activity due to increased oxygen vacancy formation and improved electronic density at copper sites, resulting from variations in electronegativity. A similar product distribution at iso-conversions suggests consistent active sites across catalysts. Additionally, the Ce- and Zr-modified catalysts (CuMgCe and CuMgZr) increased selectivity toward 4-(2-furyl)-butan-2-ol, which subsequently led to the formation of 2-methyl-1,6-dioxaspiro[4,4]nonane through an intermolecular addition reaction was observed at 6 h reaction time.