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Hydrogenation of levulinic acid to γ-valerolactone over Fe-Re/TiO2 catalysts
Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2020-07-06 , DOI: 10.1016/j.apcatb.2020.119314
Xiaoming Huang , Kaituo Liu , Wilbert L. Vrijburg , Xianhong Ouyang , A. Iulian Dugulan , Yingxin Liu , M.W.G.M. Tiny Verhoeven , Nikolay A. Kosinov , Evgeny A. Pidko , Emiel J.M. Hensen

Hydrogenation of levulinic acid to γ-valerolactone is a key reaction in the valorization of carbohydrates to renewable fuels and chemicals. State-of-the-art catalysts are based on supported noble metal nanoparticle catalysts. We report the utility of a bimetallic Fe-Re supported on TiO2 for this reaction. A strong synergy was observed between Fe and Re for the hydrogenation of levulinic acid in water under mild conditions. Fe-Re/TiO2 shows superior catalytic performance compared to monometallic Fe and Re catalysts at similar metal content. The hydrogenation activity of the bimetallic catalysts increased with Re content. H2-TPR, XPS, XANES, EXAFS, Mössbauer spectroscopy, TEM, and low-temperature CO IR spectroscopy show that the bimetallic catalysts contain metallic Re nanoparticles covered by FeOx species and small amounts of a Fe-Re alloy. Under reaction conditions, the partially reduced surface FeOx species adsorb water and form Brønsted acidic OH groups, which are involved in dehydration of reaction intermediates. Under optimized conditions, nearly full conversion of levulinic acid with a 95 % yield of γ-valerolactone could be achieved at a temperature as low as 180 °C in water at a H2 pressure of 40 bar.



中文翻译:

Fe-Re / TiO 2催化剂上乙酰丙酸加氢成γ-戊内酯

乙酰丙酸加氢为γ-戊内酯是碳水化合物向可再生燃料和化学物质增值的关键反应。最先进的催化剂是基于负载的贵金属纳米颗粒催化剂。我们报告了在此反应中负载在TiO 2上的双金属Fe-Re的效用。在温和的条件下,观察到Fe和Re之间有很强的协同作用,可以在水中对乙酰丙酸进行氢化。与单金属的Fe和Re催化剂相比,Fe-Re / TiO 2在相似的金属含量下显示出优异的催化性能。双金属催化剂的氢化活性随Re含量的增加而增加。高2-TPR,XPS,XANES,EXAFS,穆斯堡尔光谱,TEM和低温CO IR光谱显示,双金属催化剂包含被FeO x物种覆盖的金属Re纳米颗粒和少量的Fe-Re合金。在反应条件下,部分还原的表面FeO x物质吸附水并形成布朗斯台德酸性OH基团,这些基团参与反应中间体的脱水。在优化的条件下,在低至180°C的水中,H 2压力为40 bar的情况下,可以实现乙酰丙酸的几乎完全转化,并具有95%的γ-戊内酯收率。

更新日期:2020-07-10
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