Characterizing Surface Binding and Activation of Substrates in Aqueous-Phase Heterogeneous Catalysis (TSE03-C)

该项目解决了快速发展的生物可再生材料催化转化领域的关键研究需求。通过发酵产生的有机酸构成了一类重要的可再生资源衍生化合物;它们大量由生物质制成，可以转化为药物，食品，聚合物，溶剂和其他产品的各种构建模块。该研究将表征有机酸在水环境中在非均相金属催化剂上的吸附和氢化。 与有机酸和酸与其他物种的组合进行的反应和吸附的研究将开发一个更好的理解的结合强度和反应性的有机酸和它们的反应产物在不同的金属催化剂，从而提供了一个基础，最终定制催化剂的性能为特定的有机酸底物的氢化。 工作的其他方面将澄清关键问题，如水对催化剂金属的作用，如CO的毒物的影响，以及保留和生成的产品种类的手性。 此外，由于氢化和脱氢共享化学途径，这项工作对作为清洁能源的生物质制氢具有影响。 从环境的角度来看，与使用均相催化剂或传统的氢化物试剂化学相比，在水中通过金属催化剂的非均相氢化允许容易的催化剂分离和再利用，避免有机溶剂，并且大大减少了废物的产生。 因此，这种“绿色”氢化途径代表了未来“生物质炼油厂”所需的主要一类使能技术。最后，这项努力支持了教育下一代科学家的更大使命，他们将负责从可再生、可持续的资源中生产我们国家的化学品和燃料。

This project addresses critical research needs in the rapidly developing area of catalytic conversion of biorenewables. Organic acids produced via fermentation constitute an important class of renewable resource-derived compounds; they are made in large quantities from biomass and can be converted into a variety of building blocks for pharmaceuticals, foods, polymers, solvents, and other products. The research will characterize organic acid adsorption and hydrogenation on heterogeneous metal catalysts in an aqueous environment. The reaction and adsorption studies to be conducted with organic acids and combinations of acids with other species will develop a better understanding of binding strengths and reactivities of organic acids and their reaction products on different metal catalysts, thus providing a foundation for ultimately tailoring catalyst properties for hydrogenation of specific organic acid substrates. Additional aspects of the work will clarify key issues such as the role of water on the catalyst metal, the effect of poisons such as CO, and retention and generation of chirality in the product species. Further, because hydrogenation and dehydrogenation share chemical pathways, this work has implications for hydrogen generation from biomass as a clean energy source. From an environmental standpoint, heterogeneous hydrogenation over metal catalysts in water allows easy catalyst separation and reuse, avoids organic solvents, and greatly reduces waste generation in comparison to use of homogeneous catalysts or traditional hydride reagent chemistry. This "green" hydrogenation pathway thus represents a primary class of enabling technologies needed for the "biomass refinery" of the future. Finally, this effort supports the larger mission of educating the next generation of scientists, who will be responsible for producing our nation's chemicals and fuels from renewable, sustainable resources.