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Tracking the paths for the sucrose transformations over bifunctional Ru-POM/AC catalysts

机译:跟踪双功能Ru-POM / AC催化剂的蔗糖变换的路径

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摘要

The possible pathways of sugars transformation into 1,2-propanediol (PDO) have been studied, using new bifunctional catalysts for this catalytic multistep reaction. The catalysts are based on an acidic active phase (polyoxometalates, POMs) and a metallic function (Ru nanoparticles) supported over activated carbon (AC, SBET = 1190 m(2)/g). This support was loaded with 15 wt% of polyoxometalate, either phosphotungstic acid (TPA) or tungstosilicic acid (STA), while the amount of loaded ruthenium was close to 2 wt%. The catalytic materials were characterized by X-ray diffraction and electron microscopy techniques (SEM and TEM), while the surface active sites were evaluated using model reaction tests: cyclohexane dehydrogenation for metallic surface sites and isomerization of 3,3-dimethyl-1-butene for acid sites. For different sugars (sucrose, pentoses or hexoses) hydrogenation/hydrogenolysis using these catalysts in batch reactor was studied. The higher PDO selectivity was obtained in ethanol:water media and this study aims to establish the possible ways that sugars follow to achieve this transformation. The best catalytic material, 2%Ru-15%STA supported on AC, yields up to 50% of PDO selectivity when fructose is used as reactant, under moderate reaction conditions (413 K and 30 bar H-2).
机译:利用新型双功能催化剂对糖转化为1,2-丙二醇(PDO)的可能途径进行了研究。这些催化剂基于酸性活性相(多金属氧酸盐、POMs)和金属功能(钌纳米颗粒)支撑在活性炭上(AC,SBET=1190 m(2)/g)。该载体负载15 wt%的多金属氧酸盐,即磷钨酸(TPA)或钨硅酸(STA),而负载钌的量接近2 wt%。通过X射线衍射和电子显微镜技术(SEM和TEM)对催化材料进行了表征,同时通过模型反应测试对表面活性中心进行了评估:金属表面中心为环己烷脱氢,酸中心为3,3-二甲基-1-丁烯异构化。在间歇反应器中研究了不同糖(蔗糖、戊糖或己糖)的加氢/氢解反应。在乙醇:水介质中获得了较高的PDO选择性,本研究旨在确定糖实现这种转化的可能途径。在中等反应条件下(413K和30bar H-2),以果糖为反应物时,2%Ru-15%STA负载在AC上的最佳催化材料可产生高达50%的PDO选择性。

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