CAREER: Increasing Catalytic Selectivity for Isomerization of Glucose to Fructose using Paired Lewis Acid Sites

该研究的目标是设计葡萄糖液相异构化为果糖的非均相催化剂，这是生物质向化学品和燃料转化的关键步骤。作者利用生物启发的催化剂设计方法，该方法有可能降低生物可再生加工的成本，提高生物衍生化学品和燃料与化石燃料来源的经济竞争力。在催化剂设计方法中，还包括一项教育推广计划，旨在提高妇女和代表性不足的少数民族在STEM领域的参与度。具体而言，PI旨在合成在固体二氧化硅载体上含有明确的成对催化位点的催化材料，以提高葡萄糖异构化为果糖的催化活性和选择性。配对位点设计利用生物启发的方法，将酶的配对催化位点转化为非均相催化材料。拟议的工作将集中在开发一种水热合成方法，将结合成对的网站到沸石框架。这项工作将寻求通过改变成对的组成来调整催化性能，以证明成对位点的机械影响。该研究还将开发先进的光谱方法，以帮助识别成对催化位点的形成。该项目的技术影响可能是巨大的，因为它将为调整催化性能的能力增加一个新的层面，并提供一种方法来提高生物质转化为果糖的选择性，并降低相关的能源成本。总的来说，这将创造一种比目前生产高果糖玉米糖浆、生物质衍生聚合物或商品化学品更经济可行的路线。这项工作将由一个多元化的学生团队进行，他们将接受先进的催化材料合成和测试培训。除了本科生和研究生教育机会，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，并介绍沸石材料的尺寸选择性分离的概念。这些材料的一个重要特征小学生，以激励后代追求STEM相关领域的教育。过滤模块将通过PI网站提供，以扩大外联工作的影响。

The study targets design of heterogeneous catalysts for the liquid-phase isomerization of glucose to fructose, a key step in the valorization of biomass to chemicals and fuels. The authors utilize a bio-inspired catalyst design approach that has the potential to reduce cost of bio-renewable processing, increasing the economic competitiveness with fossil fuel sources of bio-derived chemicals and fuels. Integrated into the catalyst design approach is an educational outreach program that will increase participation of women and underrepresented minorities in STEM fields.Specifically, the PI seeks to synthesize catalytic materials containing well-defined paired catalytic sites on a solid silica support to increase the catalytic activity and selectivity for the isomerization of glucose to fructose. The paired site design utilizes a bio-inspired approach, translating the paired catalytic site of enzymes into a heterogeneous catalytic material. The proposed work will focus on developing a hydrothermal synthesis method that will incorporate paired sites into the zeolite framework. The work will seek to tune the catalytic performance through changing the composition of the pairs to demonstrate the mechanistic impact of paired sites. The study will also develop advanced spectroscopic methods to help identify the formation of paired catalytic sites. The technological impact of the project can be substantial since it will add a new dimension to the ability to tune catalytic performance and provide a method to increase the selectivity for biomass conversion to fructose and decrease associated energy costs. Overall, this would create a more economically viable route than currently available to produce high fructose corn syrup, biomass-derived polymers, or commodity chemicals. The work will be performed by a diverse team of students that will be trained in advanced catalytic material synthesis and testing. 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 size-selective separation of zeolitic materials ? a critical feature of these materials ? to elementary school children to inspire future generations to pursue education in STEM-related fields. The filtration module will be made available through the PI website to expand the impact of the outreach efforts.