EAGER: Influence of Ionic Liquids on Product Selectivity in CO2 Electroreduction over Copper Catalysts

二氧化碳（CO2）电还原有望从废弃的CO2和可再生电力中生产燃料和化学品。存在生产更多高阶烃和醇的机会，然而控制产物选择性和具有高活性仍然是需要克服的关键挑战。拟议的探索性研究项目旨在研究使用铜（Cu）和离子液体（IL）作为将CO2转化为有价值的化学品和燃料的助催化剂。这是一个高风险高回报的项目，可能会导致开发的技术，按需转换CO2的燃料和化学品使用可再生electrics. Breakbreakthreads在实现高的产品选择性的烃和醇是可能的，通过使用离子液体作为稀释的水性添加剂在CO2电解还原铜。所提出的EAGER项目的中心假设是，在含水电解质中以低浓度利用离子液体作为助催化剂可以抑制析氢反应并增强Cu催化剂上的CO2对高级烃和醇的电还原选择性。通过修饰IL阳离子-阴离子对，可以显著改变IL的热物理和化学性质。拟议的研究计划旨在确定IL必须具有的关键特性，以便成为用于增强对烃和醇的法拉第效率的良好助催化剂。为了验证这一假设，工作分为两个主要目标：1）确定影响CO2电还原法拉第效率的关键IL结构特性，以及2）确定IL和Cu形态对CO2电还原法拉第效率之间是否存在协同效应。根据离子液体的结构-性质关系选择离子液体的科学见解将可转移到其他电化学系统中，从而显著影响离子液体的使用方式。所提出的研究计划也可能适用于其他电化学合成方法，如电化学氨合成和电化学氢化，以及其他电化学系统，如电池，燃料电池和废物处理。该奖项反映了NSF的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。

Carbon dioxide (CO2) electroreduction holds promise for producing fuels and chemicals from waste CO2 and renewable electricity. Opportunities exist to produce more high order hydrocarbons and alcohols, however controlling product selectivity and having high activity remain as the key challenges to overcome. The proposed exploratory research project aims to investigate the use of copper (Cu) and ionic liquids (ILs) as co-catalysts for the conversion of CO2 to valuable chemicals and fuels. This is a high risk-high payoff project that may lead to the development of technologies for on-demand conversion of CO2 to fuels and chemicals using renewable electricity.Breakthroughs in achieving high product selectivity for hydrocarbons and alcohols are possible by using ILs as dilute aqueous additives in CO2 electroreduction over Cu. The central hypothesis of the proposed EAGER project is that the utilization of ILs as co-catalysts at low concentrations in aqueous electrolytes can suppress the hydrogen evolution reaction and enhance CO2 electroreduction selectivity towards higher order hydrocarbons and alcohols on Cu catalysts. By modifying the IL cation-anion pair, the thermophysical and chemical properties of the IL can be altered dramatically. The proposed research plan seeks to identify the key properties an IL must have in order to be a good co-catalyst for the enhancement of the faradaic efficiency towards hydrocarbons and alcohols. To test the hypothesis, the work is split into two main objectives: 1) Identify key IL structure properties that influence faradaic efficiency of CO2t electroreduction, and 2) Determine if there are synergistic effects between IL and Cu morphology on CO2 electroreduction faradaic efficiency. The scientific insights developed for selecting ILs based upon their structure-property relationships will be transferable to other electrochemical systems, significantly impacting the way ILs are used. The proposed research plan may also be applicable to other electrochemical synthesis methods, such as electrochemical ammonia synthesis and electrochemical hydrogenations, and other electrochemical systems, such as batteries, fuel cells and waste treatment. The educational broader impacts of the proposal include scientific workforce development, particularly of women in STEM fields.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.