UNS: Selective Catalytic Conversion of Syngas-Derived Dimethyl Oxalate to Ethylene Glycol: Mechanistic Insights from In-Situ Surface Vibrational Spectroscopy

1510157 Williams，Christopher t这项拟议的工作将研究从合成气中通过草酸二烷基酯的催化脱氢反应生产乙二醇(EG)的反应，乙二醇是一种重要的工业化学品。这为从煤炭、天然气和生物质等非传统来源生产乙烷打开了大门，而不是基于石油资源生产环氧乙烷的传统工艺。尽管该技术已经使用了几十年，但新的催化剂配方以及更先进的适合在反应条件下进行分析的表征技术，为更详细地了解催化机理提供了机会，从而进一步发展了催化剂技术。作为该项目的一部分开发的技术将广泛适用于一系列催化过程--特别是那些在液体中进行的过程。首席研究员还将把国际研究机会和针对代表性不足的基团的研究机会纳入该项目。该项目将研究各种二烷基草酸盐在铜、银、金-铜和金-银催化剂上加氢所涉及的表面化学，包括负载型和非负载型催化剂，以及气相和液相中的表面化学。该项目的关键将是实施一种新的备受关注的全反射红外光谱仪(ATR-IR)作为主要工具，并通过设计一种新的高压高温ATR-IR池。新的ATR-IR电池的应用，以及在相同条件下获得的反应动力学，将对催化反应机理和影响催化剂稳定性和中毒的因素有新的认识。这项研究的一个独特特点是，实验将在接近工业实践的条件下在气相和液体环境中进行。该项目的基本性质涉及相对复杂的有机化学品和多个反应路径，以及在水和气相环境中的反应，使其成为高压/高温ATR-IR池改进实验能力的重要试验台。这项研究提供的信息应有助于深入了解从电催化到光催化再到生物质中间产品催化转化等广泛的催化过程。通过本项目中演示的工具和技术，将特别适合研究液体环境中的催化作用。国际和平研究所还将在拟议的研究项目中纳入几个新的教育机会，包括为他的研究生提供国际研究经验，以及为研究生和本科生中代表性不足的群体提供研究机会。

1510157Williams, Christopher TThe proposed work will examine the reactions involved in producing ethylene glycol (EG) - an important industrial chemical - from synthesis gas via catalytic dehydrogenation reactions of dialkyl oxalate intermediates. This opens the door to EG production from non-conventional sources such as coal, natural gas, and biomass instead of the conventional process based on ethylene oxide produced from petroleum resources. Although the technology has been used for several decades, new catalyst formulations, as well as more advanced characterization techniques suitable for analysis under reaction conditions, present an opportunity to obtain a more detailed understanding of the catalytic mechanism, and thereby further develop the catalyst technology. The techniques developed as part of the project will be broadly applicable to a range of catalytic processes - especially those carried out in liquids. The principal investigator will also integrate international research opportunities and research opportunities targeting underrepresented groups into the project.The project will examine the surface chemistry involved in the hydrogenation of various dialkyl oxalate species on Cu, Ag, Au-Cu, and Au-Ag catalysts - both supported and unsupported - and both in the gas and liquid phases. Critical to the project will be the implementation of a new attentuated total reflection infrared spectrophotometer (ATR-IR) as the primary tool and through design of a new high-pressure and high-temperature ATR-IR cell. Application of the new ATR-IR cell, together with reaction kinetics obtained under the same conditions, should shed new insight on the catalytic reaction mechanism and factors affecting catalyst stability and poisoning. A unique feature of the study is that experiments will be conducted in both gas phase and liquid phase environments under conditions close to those utilized in industrial practice.The fundamental nature of the project, involving relatively complex organic chemicals and multiple reaction pathways, as well as reaction in both aqueous and gas phase environments, makes it an important test-bed for the improved experimental capabilities offered by the high pressure/temperature ATR-IR cell. Information derived from the study should offer insight into a broad range of catalytic processes ranging from electrocatalysis to photocatalysis and to catalytic conversion of biomass intermediate products. Catalysis in liquid phase environments will be particularly amenable to study by the tools and techniques demonstrated in this project. The PI will also integrate several novel educational opportunities into the proposed research project, including an international research experience for his graduate students, and research opportunities for underrepresented groups at both the graduate and undergraduate levels.