Abstract
The conversion of levulinic acid (LA) to -valerolactone (GVL) was investigated by employing the homogeneous Shvo catalyst (Ru-1) and iron Knolker-type catalysts, in order to evaluate the possibility to replace ruthenium with cheap, earth-abundant iron for this catalytic reaction. While the ruthenium-catalyzed reactions readily proceed, the activating agent required for the iron complex was found to interfere with the LA. This problem could be circumvented by pre-activating the original Knolker complex (Fe-1) into the corresponding dicarbonyl mono-acetonitrile iron species (Fe-3). The pre-activated iron catalyst deactivated after a few turn-overs in transfer hydrogenation reactions with isopropyl alcohol; however, highly improved GVL yields were achieved under H-2 pressure to a notable maximum of 570 turn-overs for Fe-3. Nevertheless, comparative screening experiments with various solvents and kinetic studies showed that Ru-1 is still superior over Fe-3 in terms of catalytic activity.
Original language | English |
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Pages (from-to) | 694-702 |
Number of pages | 9 |
Journal | European Journal of Inorganic Chemistry |
Issue number | 6 |
DOIs | |
Publication status | Published - 14 Feb 2018 |
Keywords
- Ruthenium
- Iron
- Homogeneous catalysis
- Hydrogenation
- Levulinic acid
- COOPERATIVE TRANSITION-METAL
- LIGAND-EXCHANGE REACTION
- SITU GENERATED CATALYST
- GAMMA-VALEROLACTONE
- ENANTIOSELECTIVE HYDROGENATION
- FORMIC-ACID
- ASYMMETRIC HYDROGENATION
- HETEROGENEOUS CATALYSTS
- FRUCTOSE DEHYDRATION
- TRANSPORTATION FUELS