Solvent-free γ-valerolactone hydrogenation to 2-methyltetrahydrofuran catalysed by Ru/C: a reaction network analysis

Solvent-free γ-valerolactone hydrogenation to 2-methyltetrahydrofuran catalysed by Ru/C: a reaction network analysis
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DOI:
10.1039/c3gc41803k
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发表时间:
2014-01-01
期刊:
影响因子:
9.8
通讯作者:
Palkovits, Regina
Palkovits, Regina
中科院分区:
化学1区
文献类型:
--
作者:
Al-Shaal, Mohammad G.;Dzierbinski, Adam;Palkovits, Regina

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2-甲基四氢呋喃(2-MTHF)被认为是一种很有吸引力的生物质平台化学品,作为生物燃料化合物和绿色溶剂具有很大的潜力。以生物基乙酰丙酸(LA)和丙戊内酯(GVL)为原料合成2-MTHF。本文研究了Ru/C催化剂上GVL加氢的最佳反应条件。在无溶剂条件下,GVL完全转化,2-MTHF的最高产率为43%。优化后的反应条件已用于合成2-甲基呋喃的反应机理研究。考察了几个副反应,以探索该多相催化体系的完整反应网络,并阐明了影响产物选择性的因素。此外,通过两步除水的方法,可以实现高效的LA无溶剂加氢反应生成2-MTHF,转化率为90%,2-MTHF的产率为61%。
2-Methyltetrahydrofuran (2-MTHF) is considered to be an attractive biomass based platform chemical with high potential as a biofuel compound and as a green solvent. 2-MTHF can be synthesised from biobased levulinic acid (LA) and gamma-valerolactone (GVL). Herein the optimum reaction conditions for the hydrogenation of GVL over Ru/C have been studied. A full conversion of GVL has been obtained under solvent free conditions with a maximum yield of 2-MTHF of 43%. The optimized conditions have been employed in a mechanistic study of the synthesis of 2-MTHF. Several side reactions have been investigated to explore the full reaction network of this heterogeneously catalysed system and to elucidate the factors influencing product selectivity. Additionally an efficient solvent-free hydrogenation reaction of LA into 2-MTHF could be achieved delivering 90% conversion of LA with a yield of 2-MTHF of 61% by removing water from the system in a two-step approach.