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Selective Hydrodeoxygenation of Vegetable Oils and Waste Cooking Oils to Green Diesel Using a Silica‐Supported Ir–ReOx Bimetallic Catalyst
ChemSusChem ( IF 7.5 ) Pub Date : 2018-04-19 , DOI: 10.1002/cssc.201800321 Sibao Liu 1 , Trent Simonetti 1 , Weiqing Zheng 1 , Basudeb Saha 1
ChemSusChem ( IF 7.5 ) Pub Date : 2018-04-19 , DOI: 10.1002/cssc.201800321 Sibao Liu 1 , Trent Simonetti 1 , Weiqing Zheng 1 , Basudeb Saha 1
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High yields of diesel‐range alkanes are prepared by hydrodeoxygenation of vegetable oils and waste cooking oils over ReOx‐modified Ir/SiO2 catalysts under mild reaction conditions. The catalyst containing a Re/Ir molar ratio of 3 exhibits the best performance, achieving 79–85 wt % yield of diesel‐range alkanes at 453 K and 2 MPa H2. The yield is nearly quantitative for the theoretical possible long‐chain alkanes on the basis of weight of the converted oils. The catalyst retains comparable activity upon regeneration through calcination. Control experiments using probe molecules as model substrates suggest that C=C bonds of unsaturated triglycerides and free fatty acids are first hydrogenated to their corresponding saturated intermediates, which are then converted to aldehyde intermediates through hydrogenolysis of acyl C−O bonds and subsequently hydrogenated to fatty alcohols. Finally, long‐chain alkanes without any carbon loss are formed by direct hydrogenolysis of the fatty alcohols. Small amounts of alkanes with one carbon fewer are also formed by decarbonylation of the aldehyde intermediates. A synergy between Ir and partially reduced ReOx sites is discussed to elucidate the high activity of Ir–ReOx/SiO2.
中文翻译：
使用二氧化硅负载的Ir-ReOx双金属催化剂对植物油和废食用油进行选择性加氢脱氧为绿色柴油
在温和的反应条件下，通过在ReO x改性的Ir / SiO 2催化剂上对植物油和废食用油进行加氢脱氧，可以制备高产率的柴油级烷烃。Re / Ir摩尔比为3的催化剂表现出最佳性能，在453 K和2 MPa H 2的条件下，柴油级烷烃的收率达到79-85 wt％。基于转化油的重量，理论上可能的长链烷烃的收率几乎是定量的。通过煅烧再生时，催化剂保持相当的活性。使用探针分子作为模型底物的对照实验表明，不饱和甘油三酸酯和游离脂肪酸的C = C键首先被氢化成其相应的饱和中间体，然后通过酰基C-O键的氢解将其转化为醛中间体，随后被氢化为脂肪族酒精。最后，脂肪醇直接氢解形成了无碳损失的长链烷烃。醛中间体的脱羰作用也形成少量少碳的烷烃。Ir与部分还原的ReO x之间的协同作用讨论了这些位点以阐明Ir–ReO x / SiO 2的高活性。
更新日期：2018-04-19
中文翻译：
使用二氧化硅负载的Ir-ReOx双金属催化剂对植物油和废食用油进行选择性加氢脱氧为绿色柴油
在温和的反应条件下，通过在ReO x改性的Ir / SiO 2催化剂上对植物油和废食用油进行加氢脱氧，可以制备高产率的柴油级烷烃。Re / Ir摩尔比为3的催化剂表现出最佳性能，在453 K和2 MPa H 2的条件下，柴油级烷烃的收率达到79-85 wt％。基于转化油的重量，理论上可能的长链烷烃的收率几乎是定量的。通过煅烧再生时，催化剂保持相当的活性。使用探针分子作为模型底物的对照实验表明，不饱和甘油三酸酯和游离脂肪酸的C = C键首先被氢化成其相应的饱和中间体，然后通过酰基C-O键的氢解将其转化为醛中间体，随后被氢化为脂肪族酒精。最后，脂肪醇直接氢解形成了无碳损失的长链烷烃。醛中间体的脱羰作用也形成少量少碳的烷烃。Ir与部分还原的ReO x之间的协同作用讨论了这些位点以阐明Ir–ReO x / SiO 2的高活性。
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