Catalytic transfer hydrogenation of biomass-derived levulinic acid and its esters to γ-valerolactone over ZrO 2 catalyst supported on SBA-15 silica
| Autor: | Tadahiro Fujitani, Hiromi Yamashita, Wako Kaburagi, Yasutaka Kuwahara, Yohsuke Osada |
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| Rok vydání: | 2017 |
| Předmět: |
Reaction mechanism
Zirconium Hydrogen 010405 organic chemistry Chemistry chemistry.chemical_element General Chemistry Mesoporous silica 010402 general chemistry 01 natural sciences Catalysis 0104 chemical sciences Reaction rate chemistry.chemical_compound Levulinic acid Organic chemistry Mesoporous material |
| Zdroj: | Catalysis Today. 281:418-428 |
| ISSN: | 0920-5861 |
| DOI: | 10.1016/j.cattod.2016.05.016 |
| Popis: | A series of ZrO2 catalysts supported on mesoporous SBA-15 silica were synthesized and examined as catalysts in the production of γ-valerolactone (GVL) from biomass-derived levulinic acid and its esters via a catalytic transfer hydrogenation (CTH) using several alcohols as hydrogen donors. Among the catalysts examined, ZrO2 supported on high-surface-area SBA-15 silica bearing highly-dispersed zirconium species exhibited the highest catalytic activity, of which reaction rate was 1.7 times higher than that of the conventional bulk ZrO2 catalyst. Zr K-edge XAFS analysis revealed that Zr4+-oxide species with a low-coordination state anchored on silica surface is the dominant active species. Such a Zr species efficiently converted levulinic acid and its esters to GVL (∼95% yields) under mild reaction conditions (150 °C, 1.0 MPa Ar), and was reusable over multiple catalytic cycles without significant loss of catalytic performances. Comparative experiments, combined with detailed characterizations using NH3/CO2-TPD and in-situ FTIR, proposed a plausible reaction mechanism where basic Zr OH site triggers the CTH reaction involving a six-member ring transition state. |
| Databáze: | OpenAIRE |
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