Rational Design of Selective Hydrodeoxygenation Catalysts for Organic Acids

有机酸选择性加氢脱氧催化剂的合理设计

• 批准号: 1153012
• 负责人: Andreas Heyden
• 金额: $ 40万
• 依托单位: University South Carolina Research Foundation
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2012
• 资助国家: 美国
• 起止时间: 2012-08-15 至 2015-07-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1153012&HistoricalAwards=false
• 关键词: Rational; Design; Selective; Hydrodeoxygenation; Catalysts

The Chemical Catalysis Program in the Chemistry Division at the National Science Foundation supports Professor Andreas Heyden and co-PIs Professor John R. Monnier and Professor Christopher T. Williams from the University of South Carolina to investigate the underlying science that can lead to the development of highly selective, catalytic materials for upgrading of bio-oils using fast pyrolysis of lignocellulosic biomass. A combined computational and experimental research approach will (a) obtain fundamental understanding of the reaction mechanism of the heterogeneous, catalytic hydrodeoxygenation (HDO) of organic acids on Group VIII transition metal catalysts in both a gas phase and liquid phase (water and n-butanol) environment and (b) rationally design novel supported metal catalysts for the selective conversion of organic acids into alcohols and alkanes. The research approach rigorously integrates (a) state-of-the-art computational heterogeneous catalysis tools such as plane wave density functional theory (DFT), implicit continuum solvation models, d-band models, Brønsted-Evans-Polanyi (BEP) relationships, scaling relations, microkinetic modeling, Campbell's degree of rate and selectivity control, and multi-dimensional volcano curves with (b) an experimental program that combines a novel bimetallic catalyst synthesis methodology (electrode less deposition) with structural and electronic characterization techniques, in-situ vibrational spectroscopy, and kinetic evaluation using state of the art single pass flow reactors and high pressure batch reactors. The computational studies will lead to hypotheses that motivate new experiments, while experimental observations will confirm theoretical findings and inspire new computational investigations. The conversion of biomass to useful fuels and chemicals is an essential goal of sustainable chemistry. The fundamental objective of this project is to establish a scientific basis for the rational design of novel heterogeneous catalysts with superior activity and selectivity for the HDO of organic acids relevant for upgrading of bio-oils obtained from lignocellulosic biomass. The aim is to increase the understanding of HDO reaction mechanisms and reduce the time and financial resources needed for the design of new heterogeneous catalysts tailored to meet the changing needs of a world with limited resources. Finally, the PhD students involved in this project will become experts in the practice and integration of computational and experimental catalysis. Graduate students from underrepresented groups will be attracted through the ongoing Sloan Minority Graduate Fellowship and Southeast Alliance for Graduate Education and the Professoriate (SEAGEP) programs that are available within Chemical Engineering at USC. Also, the research results will be integrated into the joint graduate and undergraduate electives"Multiscale Modeling: From Electrons to Chemical Reactors" and "Catalysis" and the core chemical engineering curriculum.

美国国家科学基金会化学部的化学催化项目支持南卡罗来纳大学的 Andreas Heyden 教授以及联合 PI 教授 John R. Monnier 和 Christopher T. Williams 来研究可导致发展的基础科学。利用木质纤维素生物质的快速热解来升级生物油的高选择性催化材料，结合计算和实验研究方法将（a）获得对异质反应机制的基本了解，有机酸在气相和液相（水和正丁醇）环境中在第 VIII 族过渡金属催化剂上的催化加氢脱氧（HDO），以及（b）合理设计新型负载金属催化剂，用于将有机酸选择性转化为醇和该研究方法严格集成了（a）最先进的计算多相催化工具，例如平面波密度泛函理论（DFT）、隐式连续溶剂化模型、 d 带模型、Brønsted-Evans-Polanyi (BEP) 关系、标度关系、微动力学建模、坎贝尔速率和选择性控制程度以及多维火山曲线，以及 (b) 结合新型双金属催化剂合成方法的实验程序（无电极沉积）采用结构和电子表征技术、原位振动光谱以及使用最先进的单程流反应器和高压间歇反应器的动力学评估计算研究。将产生激发新实验的假设，而实验观察将证实理论发现并激发新的计算研究将生物质转化为有用的燃料和化学品是可持续化学的基本目标。为合理设计新型多相催化剂提供基础，该催化剂对有机酸的 HDO 具有优异的活性和选择性，与从木质纤维素生物质中获得的生物油的升级有关，目的是增加对 HDO 反应机制的了解并减少时间和财务资源。最后，参与该项目的博士生将成为计算和实验催化实践和整合的专家。南加州大学化学工程系正在进行的斯隆少数族裔研究生奖学金和东南研究生教育联盟和教授 (SEAGEP) 项目吸引了人们的关注。此外，研究成果将被纳入研究生和本科生联合项目中。选修课“多尺度建模：从电子到化学反应器”和“催化”以及核心化学工程课程。