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

用可再生电能或通过直接光电催化还原对二氧化碳进行电化学还原，可以提供未来化学原料和高价值化学品的来源。光电催化还原过程的基础是电化学途径。过去对CO2电化学还原的研究显示效率较低，但在形成烃和C-C键方面取得了一些成功。本研究表明，电化学还原机理是复杂的，只是粗略地了解，虽然CO2还原为高价值产品和燃料的机制是不确定的，很明显，它需要一个平衡之间的CO吸附，H的可用性，和中间体，促进C-C键耦合。因此，催化剂的选择和性能是影响因素，凯斯西储大学的PI Robert Savinell提出了对所选金属和复合金属的模型表面进行初步实验，这将提供证据，证明为CO2还原定制电催化剂是一种可行的方法。因此，电化学数据本身的解释可能是模糊和误导的。因此，电化学CO2还原必须与直接产物分析相结合。PI Savinell建议使用一种新的方法，差分电化学质谱法，用于捕获和分析从电极表面作为电势的函数演变的挥发性产物。电流与m/e信号同时记录，因此可以估计产品效率和选择性，从而提供详细信息，从而了解反应的机理。这些实验和电催化剂的制备是一个挑战，需要集中精力，这是EAGER奖的基础。该研究旨在表明所提出的电催化方法和方法是可行的，可以在理解电化学还原二氧化碳产生重大影响，从这项研究中获得的初步数据将提供基础的实验研究计划的博士论文研究的化学工程/材料科学研究生。此外，参与该项目的本科生将解决实验室设计和DEMS校准。这个EAGER项目可能有助于吸引这些本科生继续研究生学习，因为他们直接参与了令人兴奋的实验和社会相关的科学。

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.