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Hydrogenation of biomass-derived ethyl levulinate into gamma-valerolactone by activated carbon supported bimetallic Ni and Fe catalysts

机译:活性炭负载的镍和铁双金属催化剂将生物质衍生的乙酰丙酸乙酯加氢成γ-戊内酯

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摘要

Gamma-valerolactone (GVL) has been identified as a sustainable high-value platform molecular for the production of fuels and carbon-based chemicals. In this work, a series of activated carbon supported low-cost bimetallic Ni-Fe catalysts (Ni-Fe/AC) with different molar content of Fe species were prepared by using co-precipitation method for the liquid phase hydrogenation of ethyl levulinate (EL) to produce gamma-valerolactone. The Ni-Fe0.5/AC exhibited the highest activity among the bimetallic or monometallic catalysts under mild reaction conditions (100 degrees C, 4 MPa H2, 6 h) and achieved 99.3% conversion of EL and 99.0% yield of GVL. Under more mild conditions (60 degrees C, 2 MPa H-2) and prolonging the reaction time to 24 h, EL could be converted completely and the obtained GVL yield was more than 98%. The catalysts were characterized by various techniques including XRD, TEM, HRTEM, EDX, XPS, H-2-TPR and NH3-TPD. Based on the structure and activity relationship study, the formation of highly dispersed Ni-Fe alloy structure and the co-presented FeOx nanoparticles could be responsible for the high catalytic hydrogenation activity. (C) 2017 Elsevier Ltd. All rights reserved.
机译:伽马-戊内酯(GVL)被确定为生产燃料和碳基化学品的可持续的高价值平台分子。本文采用共沉淀法制备乙酰丙酸乙酯(EL)液相加氢制备了一系列活性炭负载的不同摩尔比的Fe物种的低成本双金属Ni-Fe催化剂(Ni-Fe / AC)。 )产生γ-戊内酯。 Ni-Fe0.5 / AC在温和的反应条件下(100℃,4 MPa H2、6 h)在双金属或单金属催化剂中表现出最高的活性,并实现了99.3%的EL转化率和99.0%的GVL收率。在更温和的条件下(60摄氏度,2 MPa H-2)并将反应时间延长至24小时,EL可以完全转化,获得的GVL产率超过98%。通过多种技术对催化剂进行了表征,包括XRD,TEM,HRTEM,EDX,XPS,H-2-TPR和NH3-TPD。基于结构和活性关系的研究,高分散的镍铁合金结构的形成和共同存在的FeOx纳米颗粒可能是高催化加氢活性的原因。 (C)2017 Elsevier Ltd.保留所有权利。

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