期刊
CATALYSIS SCIENCE & TECHNOLOGY
卷 9, 期 9, 页码 2291-2304出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c9cy00168a
关键词
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资金
- Economic Development and Innovation Operative Program of Hungary [GINOP-2.3.2-15-2016-00053]
- European Union
- Indo-Hungarian project [TET_15_IN-1-2016-0034]
- Argentine-Hungarian project [TET_15-1-2016-0089]
- Slovenian-Hungarian project - National Research, Development and Innovation Office of Hungary [TET_16-1-2016-0054]
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 CoOx 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 degrees C and 30 bar total pressure in the steady state, the catalyst could only saturate the double bond of the AL ring. Thus, gamma-valerolactone (GVL) was obtained with 98 mol% yield at full LA conversion. However, at temperatures >= 225 degrees 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.
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