Catalytic transfer hydrogenation of furfural using mechanically activated MgO as catalyst†

Antonio Manuel Pérez-Merchán, Benjamín Torres-Olea, Marcella Scala, Nikolaos Dimitratos, Irene Malpartida, Cristina García-Sancho, Josefa M. Mérida-Robles, Pedro Maireles-Torres, Ramón Moreno-Tost and Juan Antonio Cecilia
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Abstract

Several MgO materials have been prepared throughout wet flow semi-continuous mechanochemical treatment of the Mg(OH)2 precursors and their subsequent calcination. This mechanochemical treatment of the precursors has shown a clear influence on the textural properties and the amount and strength of basic sites of the MgO catalysts after its calcination, obtaining higher values than that observed in a MgO sample synthesized without mechanochemical treatment. An in-depth investigation was conducted on the effects of the mechanochemical treatment on the catalytic performance in the catalytic transfer hydrogenation of furfural, and a positive effect on the activity of the catalysts was found after short mechanochemical treatment times. The highest conversion values at shorter reaction times were obtained after a mechanochemical treatment of 15 min, reaching a furfuryl alcohol yield of 79% after 2 h of reaction at 90 °C, using 2-propanol as both hydrogen donor and solvent. This data notably improves that obtained for the untreated material, which only reaches a conversion of 48% under the same experimental conditions. The stability of the material in the reaction media as well as their reusability were also investigated, and the interaction nature of 2-propanol with the MgO surface has been elucidated by attenuated total reflection spectroscopy and 2-propanol adsorption studies.

机械活化氧化镁催化糠醛转移加氢
通过对Mg(OH)2前驱体的湿流半连续机械化学处理及其随后的煅烧,制备了几种MgO材料。前驱体的机械化学处理对煅烧后MgO催化剂的结构性能和碱性位的数量和强度有明显的影响,其数值高于未经机械化学处理的MgO样品。深入考察了机械化学处理对糠醛催化转移加氢催化性能的影响,发现机械化学处理时间短对催化剂活性有积极影响。在机械化学处理15 min后,在较短的反应时间内获得了最高的转化率,在90℃条件下,以2-丙醇为供氢剂和溶剂,反应2 h后糠醇收率达到79%。这一数据明显改善了未经处理的材料,在相同的实验条件下,未经处理的材料的转化率仅为48%。研究了材料在反应介质中的稳定性及其可重复使用性,并通过衰减全反射光谱和2-丙醇吸附研究阐明了2-丙醇与MgO表面的相互作用性质。
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