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Sulfonic Mesostructured SBA-15 Silicas for the Solvent-Free Production of Bio-Jet Fuel Precursors via Aldol Dimerization of Levulinic Acid
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2021-04-16 , DOI: 10.1021/acssuschemeng.1c00378 Marta Paniagua 1 , Florentina Cuevas 1 , Gabriel Morales 1 , Juan A. Melero 1
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2021-04-16 , DOI: 10.1021/acssuschemeng.1c00378 Marta Paniagua 1 , Florentina Cuevas 1 , Gabriel Morales 1 , Juan A. Melero 1
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Sulfonic acid-functionalized mesostructured silicas have been evaluated in the solvent-free aldol dimerization of biomass-derived levulinic acid into bio-jet fuel precursors. These compounds produce branched alkanes in a subsequent hydrodeoxygenation process, with suitable properties for being a renewable alternative to conventional fossil aviation fuels. The combination of activity and selectivity toward the desired condensation products achieved over sulfonic acid-functionalized SBA-15 materials is superior to those displayed by other commercial solid acid catalysts. Enhanced textural properties provided by the mesoporous SBA-15 support contribute to such improved catalytic performance. The strength and loading of the mesoporous silica-supported sulfonic acid moieties are also important factors affecting the catalytic performance of the materials. Reaction conditions (temperature, time, and catalyst loading) have been optimized for propylsulfonic acid-functionalized mesostructured silica (Pr-SBA-15) by means of a response surface methodology, leading to a maximum yield to levulinic acid dimerization products of 58.4% (145 °C, 0.15 g of catalyst, 24 h, no solvent). Under these reaction conditions, conversion of levulinic acid is 61.1%, indicating excellent selectivity toward bio-jet fuel precursors. A small catalytic activity decay has been detected in reutilization experiments, attributed to the formation of organic deposits onto the catalyst surface. A mild acid washing of the catalyst allowed a significant recovery of the initial activity.
中文翻译：
磺酸介孔结构的SBA-15二氧化硅，可通过戊二酸的醛醇二聚法无溶剂生产生物喷气燃料前体
磺酸官能化的介孔结构二氧化硅已在无溶剂的醛醇二聚反应中得到了评估，该醇将生物质衍生的乙酰丙酸转化为生物喷气燃料前体。这些化合物在随后的加氢脱氧过程中产生支链烷烃，具有合适的性质，可作为常规化石航空燃料的可再生替代品。通过磺酸官能化的SBA-15材料获得的针对所需缩合产物的活性和选择性的结合优于其他商用固体酸催化剂所展示的那些。由中孔SBA-15载体提供的增强的织构性质有助于这种改进的催化性能。介孔二氧化硅负载的磺酸部分的强度和负载也是影响材料催化性能的重要因素。已通过响应表面方法对丙磺酸官能化的介孔结构二氧化硅（Pr-SBA-15）的反应条件（温度，时间和催化剂负载）进行了优化，从而使乙酰丙酸二聚产物的最大收率达58.4％（ 145°C，0.15 g催化剂，24小时，无溶剂）。在这些反应条件下，乙酰丙酸的转化率为61.1％，表明其对生物喷气燃料前体的优异选择性。在再利用实验中检测到小的催化活性衰减，这归因于在催化剂表面上形成了有机沉积物。
更新日期：2021-05-03
中文翻译：
磺酸介孔结构的SBA-15二氧化硅，可通过戊二酸的醛醇二聚法无溶剂生产生物喷气燃料前体
磺酸官能化的介孔结构二氧化硅已在无溶剂的醛醇二聚反应中得到了评估，该醇将生物质衍生的乙酰丙酸转化为生物喷气燃料前体。这些化合物在随后的加氢脱氧过程中产生支链烷烃，具有合适的性质，可作为常规化石航空燃料的可再生替代品。通过磺酸官能化的SBA-15材料获得的针对所需缩合产物的活性和选择性的结合优于其他商用固体酸催化剂所展示的那些。由中孔SBA-15载体提供的增强的织构性质有助于这种改进的催化性能。介孔二氧化硅负载的磺酸部分的强度和负载也是影响材料催化性能的重要因素。已通过响应表面方法对丙磺酸官能化的介孔结构二氧化硅（Pr-SBA-15）的反应条件（温度，时间和催化剂负载）进行了优化，从而使乙酰丙酸二聚产物的最大收率达58.4％（ 145°C，0.15 g催化剂，24小时，无溶剂）。在这些反应条件下，乙酰丙酸的转化率为61.1％，表明其对生物喷气燃料前体的优异选择性。在再利用实验中检测到小的催化活性衰减，这归因于在催化剂表面上形成了有机沉积物。
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