Designing Novel Types of Cooperative Effects to Influence Catalytic Performance

这项研究旨在设计一种固体催化剂替代液体催化过程，用于将果糖(从生物可再生资源中获得)转化为5-羟甲基呋喃(HMF)-一种关键的中间化学物质，可进一步加工成一系列燃料和化工产品。固体催化剂方法有可能降低生物可再生能源加工的成本和复杂性，从而使生物燃料和生物化学品与化石衍生的类似物更具竞争力。这项研究还将包括一项教育推广计划，该计划将增加妇女和代表不足的少数群体在STEM领域的参与。具体地说，PI寻求将传统液相过程中的两种元素(二甲基亚砜(DMSO)溶剂中的磺酸)共同固定在固体二氧化硅载体上，以实现高选择性地将果糖脱水为HMF的合作催化中心。拟议的工作将集中在有机硅烷链接剂在二氧化硅载体上的精确接枝上，以达到预期的协同效果。通过改变系链基团的几个性质，如长度和分子结构，将实现最优化。这项研究还将讨论束缚物种在水反应环境中的稳定性。如果该项目能够打开水基过程的大门，消除目前从DMSO溶剂中分离产品HMF所需的能源密集型(和昂贵的)蒸馏过程，那么该项目的技术影响可能是巨大的。总体而言，这将创造一条从生物质到HMF的更直接的路线--一种多功能平台化学品，可用于制造生物质衍生聚合物、合成燃料添加剂或利用可再生资源生产商品化学品。除了本科和研究生教育机会，该项目还将与俄亥俄州立大学现有的几个项目相结合，为学生创建一个课堂模块，以及一个向小学生介绍酸和碱概念的项目。

This study seeks to design a solid-catalyst substitute for a liquid-phase catalytic process used to convert fructose (obtained from biorenewable sources) to 5-hydroxymethylfurfural (HMF) - a key intermediate chemical that can be further processed to a range of fuel and chemical products. The solid-catalyst approach has the potential to reduce the cost and complexity of biorenewables processing, thereby making bio-fuels and bio-chemicals more competitive with fossil-derived analogs. The study will also include an educational outreach plan that will increase the participation of women and underrepresented minorities in STEM fields. Specifically, the PI seeks to co-immobilize the two elements of the conventional liquid-phase process (sulfonic acids in a dimethylsulfoxide (DMSO) solvent) on a solid silica support to achieve cooperative catalytic sites that dehydrate fructose to HMF with high selectivity. The proposed work will focus on the precise grafting of organosilane tethering agents onto the silica support to achieve the desired cooperative effects. Optimization will be achieved by varying several properties of the tethered groups such as length and molecular structure. The study will also address the stability of the tethered species in the aqueous reaction environment. The technological impact of the project can be substantial if it can open the door to a water-based process that eliminates the energy intensive (and expensive) distillation process currently needed to separate the product HMF from the DMSO solvent. Overall, this would create a more direct route from biomass to HMF - a versatile platform chemical that can be used to create biomass-derived polymers, to synthesize fuel additives, or to produce commodity chemicals from renewable sources. In addition to undergraduate and graduate education opportunities, the project will interface with several existing programs at Ohio State University to create a classroom module for students and a project to introduce the concepts of acids and bases to elementary school children.