UNS:Catalysis at Acid-Base Site Pairs: Thermodynamic and Kinetic Studies of Aldol Additions to Upgrade Biofuels on Metal and Mixed Metal Oxides

Flaherty，1511819全球能源消费将在未来几十年内急剧增加，从而刺激对可再生能源（如生物质）生产的燃料和化学品的需求。 虽然将生物质转化为化学品如乙醇的方法是众所周知的，但将这些发酵产物进一步加工成构成燃料和化学品的更大分子目前效率低下且不太清楚。 该项目将研究专门设计的催化材料的新组合，以促进发酵产物偶联成柴油燃料，润滑油和化学原料。 通过了解详细的催化化学及其与催化材料的结构和组成的关系，该研究将为一类新的催化剂材料奠定基础，这些材料可以将发酵产品转化为更高价值的产品，与现有工艺相比，更有效地节省能源。 这项工作还将为科学、技术和工程方面的研究生和本科生提供培训机会，特别强调为女生提供机会。 由于与发酵过程相关的水和二氧化碳的中毒，通常避免使用碱性催化剂。 这些研究人员已经认识到有机会将酸性和碱性催化功能联合收割机结合到单一催化剂中，以促进羟醛型缩合（即链增长）反应而没有通常的中毒效应。 他们将通过研究超过25种技术相关的催化剂来实现这一目标，这些催化剂包含一系列酸位点，碱位点和酸碱位点对。 使用实验工具的组合，他们将表征酸，碱和酸碱对位点的数量和强度，然后将这些位点上的醇和醛吸附与详细的羟醛缩合动力学和临界过渡态的识别相关联。 这项工作的更广泛的科学影响将是为生产碳中性生物燃料和化学品设计更活跃和稳定的催化剂提供指导原则。 此外，首席研究员正在建立一个本科生研究计划，重点是培养研究生女导师，与STEM领域的本科生学员合作。

Flaherty, 1511819Global energy consumption will increase dramatically in the next several decades, thus stimulating demand for fuels and chemicals produced from renewable sources such as biomass. While the processes for converting biomass to chemicals such as ethanol are well-known, the further processing of those fermentation products to the larger molecules that make up fuels and chemicals is presently inefficient and not well understood. This project will investigate new combinations of catalytic materials specifically designed to promote the coupling of fermentation products into diesel fuel, lubricants and chemical feedstocks. By understanding the detailed catalytic chemistry and its relationship to the structure and composition of the catalytic materials, the research will lay the groundwork for a new class of catalyst materials that can convert fermentation products into higher-value products both more efficiently and with significant energy savings compared to existing processes. The work will also provide opportunities for the training of both graduate students and undergraduates in science, technology, and engineering, with special emphasis on providing opportunities to female students.Most biomass upgrading processes rely on acidic catalysts. Basic catalysts have generally been avoided because of poisoning by water and carbon dioxide associated with fermentation processes. These researchers have recognized an opportunity to combine both acidic and basic catalytic functions into a single catalyst in a way that promotes aldol type condensation (i.e. chain growth) reactions without the usual poisoning effects. They will do this by investigating more than 25 technologically relevant catalysts containing a range of acid sites, base sites, and acid-base site pairs. Using a combination of experimental tools, they will characterize the number and strength of acid, base, and acid-base pair sites and then relate alcohol and aldehyde adsorption on those sites to detailed aldol condensation kinetics and identification of critical transition states. The broader scientific impact of this work will be to produce guiding principles for the design of more active and stable catalysts for the production of carbon-neutral biofuels and chemicals. In addition, the principal investigator is building an undergraduate research program that focuses on developing graduate-student female mentors to work with undergraduate mentees in the STEM areas.