Selective hydroconversion of levulinic acid to γ-valerolactone or 2-methyltetrahydrofuran over silica-supported cobalt catalysts

Gyula Novodárszki, Hanna E. Solt, J. Valyon, F. Lónyi, J. Hancsók, Dhanapati Deka, Róbert Tuba, Magdolna R. Mihályi

Research output: Contribution to journalArticle

4 Citations (Scopus)

Abstract

Solvent-free hydroconversion of levulinic acid (LA) was studied over Co/silica catalysts by applying a flow-through fixed-bed microreactor. Consecutive hydrogenation/hydrogenolysis and dehydration reactions proceeded over the catalyst having Co 0 metal and CoO x Lewis acid active sites. As a first step, LA was dehydrated to form an angelica lactone (AL) intermediate. Because dehydration of LA is a facile reaction, the selectivity was controlled by the hydrogenation/hydrogenolysis activity of the catalyst. At 200 °C and 30 bar total pressure in the steady state, the catalyst could only saturate the double bond of the AL ring. Thus, γ-valerolactone (GVL) was obtained with 98 mol% yield at full LA conversion. However, at temperatures ≥225 °C, the hydrogenation activity was high enough to cleave the GVL ring and obtain 2-methyltetrahydrofuran (2-MTHF) with a stable yield of about 70 mol%. FT-IR spectroscopic examination of the adsorbed LA showed the formation of H-bound LA and also surface carboxylate. 4-Hydroxy-3-pentenoate and 4-hydroxypentanoate were substantiated as surface intermediates of lactone formation by dehydration.

Original languageEnglish
Pages (from-to)2291-2304
Number of pages14
JournalCatalysis Science and Technology
Volume9
Issue number9
DOIs
Publication statusPublished - Jan 1 2019

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Cobalt
Silicon Dioxide
Silica
Catalysts
Acids
Dehydration
Hydrogenation
Hydrogenolysis
Lewis Acids
Lactones
levulinic acid
2-methyltetrahydrofuran
Thermodynamic properties
Metals
Temperature

ASJC Scopus subject areas

  • Catalysis

Cite this

Selective hydroconversion of levulinic acid to γ-valerolactone or 2-methyltetrahydrofuran over silica-supported cobalt catalysts. / Novodárszki, Gyula; Solt, Hanna E.; Valyon, J.; Lónyi, F.; Hancsók, J.; Deka, Dhanapati; Tuba, Róbert; Mihályi, Magdolna R.

In: Catalysis Science and Technology, Vol. 9, No. 9, 01.01.2019, p. 2291-2304.

Research output: Contribution to journalArticle

Novodárszki, Gyula ; Solt, Hanna E. ; Valyon, J. ; Lónyi, F. ; Hancsók, J. ; Deka, Dhanapati ; Tuba, Róbert ; Mihályi, Magdolna R. / Selective hydroconversion of levulinic acid to γ-valerolactone or 2-methyltetrahydrofuran over silica-supported cobalt catalysts. In: Catalysis Science and Technology. 2019 ; Vol. 9, No. 9. pp. 2291-2304.
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