EAGER: Project for Preliminary Studies of Electrochemical Reduction of Carbon Dioxide: Nano-Particle and Mechanistic Studies

EAGER：二氧化碳电化学还原初步研究项目：纳米粒子和机理研究

• 批准号: 1047563
• 负责人: Robert Savinell
• 金额: $ 7.85万
• 依托单位: Case Western Reserve University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2010
• 资助国家: 美国
• 起止时间: 2010-09-01 至 2011-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1047563&HistoricalAwards=false
• 关键词: EAGER; Project; Preliminary; Studies; Electrochemical

1047563SavinellThe electrochemical reduction of carbon dioxide with renewable electrical energy sources, or by direct photoelectrocatalytic reduction, could provide a source of chemical feedstocks and high value chemicals of the future. Fundamental to photoelectrocatalytic reduction processes are electrochemical pathways. Past research on electrochemical reduction of CO2 showed low efficiency but demonstrated some success at forming hydrocarbons and C-C bonds. This research made clear that the electrochemical reduction mechanisms are complex and only sketchily understood.Although the mechanism of CO2 reduction to high value products and fuels isuncertain, it is apparent that it requires a balance between CO adsorption, H availability, and intermediates that facilitate C-C bond coupling. Thus, catalyst selection and properties are factors, and the PI Robert Savinell of Case Western Reserve University proposes preliminary experiments on model surfaces of selected metals and composite metals that would provide evidence that tailoring electrocatalysts for CO2 reduction is a feasible approach.The activity of an electrocatalyst towards electrochemical reduction of CO2cannot be measured through comparative voltammetry alone. Consequently, the interpretation of electrochemical data by itself can be ambiguous and misleading. Therefore, electrochemical CO2 reduction must be combined with direct product analysis. PI Savinell proposes to use a new approach, Differential Electrochemical Mass Spectrometry, for the capture and analysis of the volatile products evolving from an electrode surface as a function of potential. The current is recorded simultaneously with m/e signals so product efficiencies and selectivity can be estimated, thus providing detailed information leading to mechanistic understanding of the reactions. These experiments and the preparation of the electrocatalysts are a challenge to develop and require a focused effort, which is the basis of this EAGER award. The proposed research is designed to show that the electrocatalytic approaches and methodologies proposed are feasible and can have a major impact in understanding of electrochemical reduction of carbon dioxide.The preliminary data obtained from this research will provide the foundation of the experimental research program for the PhD dissertation studies of a chemical engineering/materials science graduate student. In addition, undergraduate students participating in this project will address experimental cell design and DEMS calibration. This EAGER project is likely to be helpful to attracting these undergraduate students to pursue graduate study because of their direct involvement in exciting experiments and socially relevant science.

[47563] savinell二氧化碳的电化学还原与可再生电力能源，或通过直接的光电催化还原，可以提供一个来源的化学原料和高价值的化学品的未来。光电催化还原过程的基础是电化学途径。过去的研究表明，电化学还原CO2的效率较低，但在形成碳氢化合物和C-C键方面取得了一些成功。这项研究表明，电化学还原机制是复杂的，只是粗略了解。虽然二氧化碳还原为高价值产品和燃料的机制尚不确定，但很明显，它需要CO吸附，H可用性和促进C-C键偶联的中间体之间的平衡。因此，催化剂的选择和性能是因素，凯斯西储大学的PI Robert Savinell提出在选定的金属和复合金属的模型表面上进行初步实验，这将提供证据，证明定制电催化剂以减少二氧化碳是一种可行的方法。电催化剂对co2的电化学还原活性不能仅通过比较伏安法来测量。因此，电化学数据本身的解释可能是含糊不清和误导。因此，电化学CO2还原必须与直接产物分析相结合。PI Savinell提出使用一种新的方法，微分电化学质谱法，用于捕获和分析从电极表面演变成电位函数的挥发性产物。电流与m/e信号同时记录，因此可以估计产物效率和选择性，从而提供详细的信息，从而导致对反应机理的理解。这些实验和电催化剂的制备是一项挑战，需要集中精力进行开发，这是本次EAGER奖的基础。所提出的研究旨在表明所提出的电催化方法和方法是可行的，并且可以对理解二氧化碳的电化学还原产生重大影响。本研究获得的初步数据将为化学工程/材料科学研究生的博士论文研究提供实验研究计划的基础。此外，参与本项目的本科生将负责实验单元设计和dem校准。由于这些本科生直接参与了令人兴奋的实验和与社会相关的科学，因此这个EAGER项目很可能有助于吸引他们攻读研究生。