期刊
INORGANICA CHIMICA ACTA
卷 482, 期 -, 页码 460-468出版社
ELSEVIER SCIENCE SA
DOI: 10.1016/j.ica.2018.06.050
关键词
Solvent-free reactions; Formic acid; Hydrogen generation; Levulinic acid; Gamma-valerolactone; Arene ruthenium(II) complexes
资金
- University of Johannesburg' Centre for Synthesis and Catalysis
- National Research Foundation of South Africa (NRF) [99269, 105556]
- SASOL LTD.
The selective and efficient solvent-free hydrogenation of bio-based levulinic acid (LA) to gamma-valerolactone (GVL) was achieved with new pyridylimine ruthenium(II) complexes as catalyst precursors. The hydrogenation reactions were performed in the presence of formic acid as hydrogen source using a catalyst loading as low as 0.1 mol % with potassium hydroxide or triethylamine (Et3N). 4-Hydroxyvaleric acid (HVA) was produced only when KOH was used, whereas reactions involving Et3N were selective to GVL. At 150 degrees C, > 96% LA conversions were achieved with 100% GVL selectivity. Recyclability of catalyst precursors was demonstrated by running three consecutive reactions where 100% conversion and selectivity was maintained. In-situ NMR studies show that hydrogen gas is formed by the decomposition of formic acid to carbon dioxide and hydrogen. Ru-hydride species have been detected, by H-1 NMR, and are believed to be the catalytically active species, and a mechanism of the reaction has been proposed.
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