Abstract
Hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL) was studied by using mono- and bidentate p-cymene ruthenium(ii) N-heterocyclic carbene (NHC) complexes as catalyst precursors. In water, all complexes were found to be reduced in situ to form ruthenium nanoparticles (RuNPs) with a high hydrogenation activity. In organic solvents, complexes with monodentate NHC ligands also formed nanoparticles, while complexes with bidentate ligands gave rise to stable homogeneous catalysts with moderate hydrogenation activities.
Highlights
Fossil fuel has always been the main source of energy since the 18th century
We found that in water, the Ru–N-heterocyclic carbene (NHC) complexes were reduced in situ by dihydrogen to form ruthenium
The monocarbene ruthenium(II) complexes [RuCl2( p-cymene)(iPr2-imy)] (1), [RuCl2( p-cymene)] (2) and [RuCl2( p-cymene)(Bn2-bimy)] (3) derived from imidazole[10] and benzimidazole[11] were prepared as previously reported by deprotonation of the respective azolium salts A–C using Ag2O followed by transmetallation of the resulting silver NHC complexes to [RuCl2( p-cymene)]2
Summary
Fossil fuel has always been the main source of energy since the 18th century. due to its depletion and related chemical concerns, there has been a shift towards renewable sources of energy and chemicals. We report the synthesis of six p-cymene ruthenium(II) mono- and bidentate diNHC complexes and their applications as catalyst precursors in the hydrogenation of LA to GVL. Complexes with monodentate NHC ligands decomposed to form nanoparticles, while complexes with bidentate ligands formed stable homogeneous catalysts with moderate hydrogenation activities.
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