Acidic mesoporous silica for the acetylation of glycerol: Synthesis of bioadditives to petrol fuel
Acidic mesoporous silica for the acetylation of glycerol: Synthesis of bioadditives to petrol fuel
复制标题
DOI：
10.1021/ef060647q
复制
发表时间：
2007-05-01
期刊：
影响因子：
5.3
通讯作者：
Paniagua, Marta
中科院分区：
文献类型：
--
作者：
Melero, Juan A.;van Grieken, Rafael;Paniagua, Marta
预计未来几年生物柴油产量将增加，这将导致主要副产品甘油的生产过剩。使用以甘油为基础的添加剂来改善汽油燃料的性能是目前正在探索的利用这种可再生原料的可能性之一。在此背景下，磺酸功能化的介孔结构材料在甘油和醋酸的酯化反应中表现出了良好的催化性能。二乙酰甘油(DAG)和三乙酰甘油(TAG，也称为三乙酸甘油)已被证明是有价值的汽油燃料添加剂，当与柴油混合时，可提高冷性和粘度性质，或当添加到汽油中时，可提高抗爆性。使用磺酸功能化的介孔材料作为催化剂，其活性和选择性与传统酸催化剂相当甚至更好，反应4h后，甘油转化率高达90%，对DAG和TAG的联合选择性超过80%。磺酸中心的酸强度也被发现是影响这些材料催化性能的一个重要因素。此外，这些磺化的介孔材料经过温和的溶剂洗涤再生步骤后，在重复催化运行中得到了与新鲜催化剂相似的催化性能。预计未来几年生物柴油产量将增加，这将导致主要副产品甘油的生产过剩。使用以甘油为基础的添加剂来改善汽油燃料的性能是目前正在探索的利用这种可再生原料的可能性之一。在此背景下，磺酸功能化的介孔结构材料在甘油和醋酸的酯化反应中表现出了良好的催化性能。二乙酰甘油(DAG)和三乙酰甘油(TAG，也称为三乙酸甘油)已被证明是有价值的汽油燃料添加剂，当与柴油混合时，可提高冷性和粘度性质，或当添加到汽油中时，可提高抗爆性。使用磺酸功能化的介孔材料作为催化剂，其活性和选择性与传统酸催化剂相当甚至更好，反应4h后，甘油转化率高达90%，对DAG和TAG的联合选择性超过80%。磺酸中心的酸强度也被发现是影响这些材料催化性能的一个重要因素。此外，这些磺化的介孔材料经过温和的溶剂洗涤再生步骤后，在重复催化运行中得到了与新鲜催化剂相似的催化性能。
Expected increasing biodiesel production during the next few years will lead to an overproduction of glycerol, which is the main byproduct. The use of glycerol-based additives to improve petrol fuel properties is one of the possibilities currently being explored to utilize this renewable feedstock. In this context, sulfonic acid functionalized mesostructured materials have demonstrated an excellent catalytic behavior in the esterification of glycerol with acetic acid to yield acetylated derivates. Diacetylglycerol (DAG) and triacetylglycerol (TAG, also called triacetin) have been shown to be valuable petrol fuel additives leading to either enhanced cold and viscosity properties when blended with diesel fuel or antiknocking properties when added to gasoline. The activities and selectivities achieved using sulfonic acid functionalized mesostructured materials as catalysts are comparable or even superior to those displayed by conventional acid catalysts, providing values up to 90% of glycerol conversion and over 80% of combined selectivity toward DAG and TAG after 4 h of reaction. The acid strength of the sulfonic acid site has also been found to be an important factor affecting the catalytic performance of these materials. Moreover, these sulfonated mesostructured materials have been reused in repeated catalytic runs after a mild solvent-washing regeneration step yielding similar catalytic performance to that of the fresh catalyst. Expected increasing biodiesel production during the next few years will lead to an overproduction of glycerol, which is the main byproduct. The use of glycerol-based additives to improve petrol fuel properties is one of the possibilities currently being explored to utilize this renewable feedstock. In this context, sulfonic acid functionalized mesostructured materials have demonstrated an excellent catalytic behavior in the esterification of glycerol with acetic acid to yield acetylated derivates. Diacetylglycerol (DAG) and triacetylglycerol (TAG, also called triacetin) have been shown to be valuable petrol fuel additives leading to either enhanced cold and viscosity properties when blended with diesel fuel or antiknocking properties when added to gasoline. The activities and selectivities achieved using sulfonic acid functionalized mesostructured materials as catalysts are comparable or even superior to those displayed by conventional acid catalysts, providing values up to 90% of glycerol conversion and over 80% of combined selectivity toward DAG and TAG after 4 h of reaction. The acid strength of the sulfonic acid site has also been found to be an important factor affecting the catalytic performance of these materials. Moreover, these sulfonated mesostructured materials have been reused in repeated catalytic runs after a mild solvent-washing regeneration step yielding similar catalytic performance to that of the fresh catalyst.