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

UNS：合成气衍生的草酸二甲酯选择性催化转化为乙二醇：来自原位表面振动光谱的机理见解

• 批准号: 1510157
• 负责人: Christopher Williams
• 金额: $ 34.82万
• 依托单位: University of South Carolina at Columbia
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2015
• 资助国家: 美国
• 起止时间: 2015-09-01 至 2019-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1510157&HistoricalAwards=false
• 关键词: UNS; Selective; Catalytic; Conversion; Syngas

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.

1510157 Williams，Christopher T拟议的工作将研究通过草酸二烷基酯中间体的催化脱氢反应从合成气生产乙二醇（EG）-一种重要的工业化学品-所涉及的反应。这为从煤、天然气和生物质等非常规来源生产EG打开了大门，而不是基于从石油资源生产环氧乙烷的常规工艺。虽然该技术已经使用了几十年，但新的催化剂配方以及适用于反应条件下分析的更先进的表征技术提供了一个机会，可以更详细地了解催化机理，从而进一步发展催化剂技术。作为该项目一部分开发的技术将广泛适用于一系列催化过程，特别是在液体中进行的催化过程。 主要研究者还将把国际研究机会和针对代表性不足的群体的研究机会整合到该项目中。该项目将研究各种草酸二烷基酯物种在Cu、Ag、Au-Cu和Au-Ag催化剂上（包括负载和非负载的）以及气相和液相中的氢化所涉及的表面化学。 该项目的关键将是采用一种新的衰减全反射红外分光光度计作为主要工具，并设计一种新的高压和高温衰减全反射红外单元。 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，应该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。该研究的一个独特之处在于，实验将在接近工业实践的条件下在气相和液相环境中进行，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途径，以及在水相和气相环境中的反应，使其成为一个重要的测试平台，用于提高高压/高温ATR-IR单元的实验能力。从研究中获得的信息应提供深入了解广泛的催化过程，从电催化到生物质中间产品的催化转化。液相环境中的催化作用将特别适合于本项目中所展示的工具和技术的研究。PI还将把几个新的教育机会整合到拟议的研究项目中，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水平代表性不足的群体提供研究机会。