Efficient solvent-free hydrogenation of levulinic acid to γ-valerolactone by pyrazolylphosphite and pyrazolylphosphinite ruthenium(II) complexes

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Abstract

Solvent-free conversion of bioderived levulinic acid (LA) to γ-valerolactone (GVL) has been achieved by new pyrazolylphosphite and pyrazolylphosphinite ruthenium(II) complexes as catalyst precursors, using both formic acid and molecular hydrogen as hydrogen sources. The reactions were very efficient at moderate temperatures of 100-120 °C. With a catalyst loading of 0.1%, 100% LA conversion (with hydrogen gas) was achieved with 100% GVL selectivity at 110 °C and 15 bar. The catalyst was recyclable up to three times without significant loss of activity and selectivity. The catalyst precursors are found to be more efficient when the hydrogen source was molecular hydrogen as compared to formic acid. NMR studies of reactions involving formic acid as a hydrogen source indicate that the initial step in the reaction involves the decomposition of formic acid to CO2 and H2.

Original languageEnglish
Pages (from-to)6010-6018
Number of pages9
JournalACS Sustainable Chemistry and Engineering
Volume4
Issue number11
DOIs
Publication statusPublished - 7 Nov 2016

Keywords

  • Hydrogenation
  • Levulinic acid
  • Ruthenium catalysts
  • Solvent-free
  • γ-Valerolactone

ASJC Scopus subject areas

  • General Chemistry
  • Environmental Chemistry
  • General Chemical Engineering
  • Renewable Energy, Sustainability and the Environment

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