Understanding and Controlling Reactivity of Functionalized Alcohols on Metal Surfaces

在这个由化学催化计划资助的项目中，位于博尔德的科罗拉多大学的Will Medlin教授将研究功能醇在金属表面上的反应。 目的是确定方法来设计固体催化剂的生物质衍生化合物的选择性反应。 表面光谱将与量子化学建模结合使用，以了解醇的分子结构如何控制其在通常用作工业催化剂活性组分的金属表面上的反应性。 分子结构的作用将与侧基官能团对C-OH键强度和化学吸附醇的几何形状的影响有关。 为了控制反应选择性的目的，这项工作将调查使用的表面改性剂，有利于吸附功能醇在特定的几何形状以上的金属表面。 作为一个具有现实意义的特定模型系统，糠醇的选择性氢解将被用于测试本项目中开发的催化剂设计原则。本研究旨在为可再生生物质原料转化为燃料和化学品做出重要进展。功能醇如糠醇和5-羟甲基糠醛可以由生物质衍生的糖大量生产。 选择性地将这些中间体转化为所需产物的稳健固体催化剂的鉴定受到试剂复杂性的阻碍。 通过开发此类催化剂的基本设计原则，这项工作可以为燃料和有用化学品的生产带来新的可持续途径。 研究生将为该项目进行研究，他们的研究的影响将从与国家可再生能源实验室研究人员的持续合作中延伸出来。本科生还将在研究生的研究基础上，对自己的小规模项目进行独立研究。 最后，面向普通观众的推广活动将通过现有的方案组织，其中主要研究者发挥积极或领导作用，包括可再生能源材料研究科学与工程中心，科罗拉多生物精炼和生物燃料中心，以及可再生和可持续能源研究所。

In this project funded by the Chemical Catalysis Program, Prof. Will Medlin of the University of Colorado at Boulder will investigate the reactions of functional alcohols on metal surfaces. The objective is to identify methods to design solid catalysts for selective reactions of biomass-derived compounds. Surface spectroscopy will be used in conjunction with quantum chemical modeling to understand how the molecular structure of alcohols controls their reactivity on the surfaces of metals that are commonly used as active components in industrial catalysts. The role of molecular structure will be linked to the influence of pendant functional groups on C-OH bond strength and on the geometry of the chemisorbed alcohol. For the purpose of controlling reaction selectivity, this work will investigate the use of surface modifiers that favor the adsorption of functional alcohols in specific geometries above metal surfaces. As a specific model system of real-world importance, the selective hydrogenolysis of furfuryl alcohol will be used to test the catalyst design principles developed in this project.This research is directed toward making important advances for the conversion of renewable biomass feedstocks to fuels and chemicals. Functional alcohols such as furfuryl alcohol and 5-hydroxymethylfurfural can be produced in large volumes from biomass-derived sugars. Identification of robust solid catalysts that selectively convert these intermediates to desired products is hampered by the complexity of the reagents. By developing fundamental design principles for such catalysts, this work can lead to new, sustainable pathways for production of fuels and useful chemicals. Graduate students will conduct research for the project, and the impact of their research will be extended from ongoing collaborations with researchers at the National Renewable Energy Laboratory. Undergraduate students will also conduct independent research on their own small-scale projects that build on the research of graduate students. Finally, outreach activities oriented toward a general audience will be organized through existing programs in which the principal investigator plays an active or leadership role, including the Renewable Energy Materials Research Science and Engineering Center, the Colorado Center for Biorefining and Biofuels, and the Renewable and Sustainable Energy Institute.