Hydrogen gas-free processes for single-step preparation of transition-metal bifunctional catalysts and one-pot Γ-valerolactone synthesis in supercritical CO 2 -ionic liquid systems

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13 Citations (Scopus)

Abstract

Hydrothermal carbonization of glucose (180 °C, 4 h) with 5-sulfosalicylic acid and nickel or copper sulfate afforded transition-metal (Ni/NiO, Cu/CuO) functional carbon (FC) catalysts in a single-step without hydrogen gas. Hydrogenation of levulinic acid to γ-valerolactone (GVL) in supercritical carbon dioxide (scCO 2 )-ionic liquid ([BMIM]Cl) systems with formic acid as H-donor source and Ni/NiO-FC catalysts gave 97% GVL yields (170 °C, 3 h). The Ni/NiO-FC catalysts (d = 50 to 200 nm) had well-dispersed Ni/NiO particles (<5 nm) with –SO 3 H, COOH and phenolic −OH functional groups; Ni/NiO-FC catalysts were more effective than Cu/CuO-FC catalysts. Ni/NiO-FC catalysts were active for conversion of substrates (ethyl levulinate, fructose, cellobiose or cellulose) to respective products (GVL, 5-HMF, sugars). The role of scCO 2 in the reaction system is one of improving mass transport and suppressing side-reactions via GVL product removal. Proposed methods for catalyst synthesis and substrate hydrogenation do not require hydrogen gas and are widely applicable to processing biomass.

Original languageEnglish
Pages (from-to)263-270
Number of pages8
JournalJournal of Supercritical Fluids
Volume147
DOIs
Publication statusPublished - 2019 May

Keywords

  • Hydrogenation catalyst
  • Hydrothermal carbonization
  • Levulinic acid
  • Platform chemicals
  • γ-Valerolactone

ASJC Scopus subject areas

  • Chemical Engineering(all)
  • Condensed Matter Physics
  • Physical and Theoretical Chemistry

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