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相催化过程，用于将果糖（从生物可再生来源获得）转化为5-羟甲基糠醛（HMF）-一种关键的中间体化学品，可以进一步加工成一系列燃料和化学产品。 固体催化剂方法有可能降低生物可再生材料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。 该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性不足的少数民族在STEM领域的参与。 具体而言，PI旨在将常规液相工艺的两种元素（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，以实现协同催化位点，从而以高选择性将果糖转化为HMF。 所提出的工作将集中在有机硅烷栓系剂到二氧化硅载体上的精确接枝，以实现所需的合作效果。 通过改变栓系基团的几种性质，如长度和分子结构，可以实现优化。 该研究还将解决在水反应环境中的系留物种的稳定性。 该项目的技术影响可能是巨大的，如果它可以打开大门，以水基工艺，消除能源密集型（和昂贵的）蒸馏过程目前需要从DMSO溶剂中分离产品HMF。 总的来说，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的聚合物，合成燃料添加剂，或从可再生资源生产商品化学品。 除了本科和研究生教育机会，该项目将与俄亥俄州州立大学的几个现有项目对接，为学生创建一个课堂模块，并为小学生介绍酸和碱的概念。

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.