CAREER: Control of surface reactivity for catalyzing hydrocarbon formation from CO2

职业：控制表面反应性以催化二氧化碳形成碳氢化合物

• 批准号: 1455162
• 负责人: Anne Co
• 金额: $ 65.17万
• 依托单位: Ohio State University
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2015
• 资助国家: 美国
• 起止时间: 2015-07-01 至 2022-06-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1455162&HistoricalAwards=false
• 关键词: CAREER; Control; surface; reactivity; catalyzing

CAREER: Control of Surface Reactivity for Catalyzing Hydrocarbon Formation from CO2 Scientific studies have predicted that converting carbon dioxide to fuels and chemical feedstocks, or using them directly as solvents, has the potential to reduce carbon dioxide (CO2) emission by 4,000,000,000 tons per year. Electrochemical synthesis is amongst the most promising chemical process for CO2 conversion, since the technology can be readily added to our existing industrial infrastructure without major disruptions. An economically-relevant electrocatalyst has certain requirements to be effective. It must possess high current densities, low specific electricity consumption, high selectivity, and a sustained electrode lifetime. Currently no electrocatalyst for carbon dioxide conversion meets all of these requirements. The carefully designed surface structures under investigation in this the project can help understand these catalyst limitations through a systematic investigation of the relationship between the surface structure and the electrocatalytic reactivity. Integrated with the research activities are a series of educational and outreach efforts that build upon existing infrastructure at The Ohio State University (OSU). A research-intensive undergraduate laboratory module in electrocatalysis is being developed as part of the OSU Research Experience to Enhance Learning (REEL) program. Professor Co and members of her group also participate in outreach activities to increase interest of underrepresented groups in science and to engage the public through OSU's STEAM Factory.With this award, the Chemical Catalysis Program of the Chemistry Division is funding Dr. Anne Co of The Ohio State University in the systematic investigation of the electrochemical conversion of carbon dioxide to hydrocarbons. A series of highly-controlled surfaces, designed to promote adsorption of specific intermediates, are being produced by underpotential deposition of strained copper monolayers and by porous copper-based bimetallic films, in designs chosen to facilitate the selective formation of C-H and C-C bonds. A combination of electrochemical and in situ spectroscopic measurements, complemented by theoretical modelling, are used to elucidate the mechanistic pathways and the chemical environments around the active center under electrochemical reaction conditions. The knowledge gained from the investigation of surface structure and reactivity relationships in this project has direct impact on the general understanding of surface electrocatalytic processes, and in the specific reaction of CO2 electroreduction.

科学研究预测，将二氧化碳转化为燃料和化学原料，或直接将其用作溶剂，每年有可能减少40亿吨二氧化碳的排放。电化学合成是最有前途的二氧化碳转化化学过程之一，因为该技术可以很容易地添加到我们现有的工业基础设施中，而不会造成重大破坏。与经济相关的电催化剂必须具备一定的有效性要求。它必须具有高电流密度、低比电耗、高选择性和持续的电极寿命。目前还没有一种用于二氧化碳转化的电催化剂能满足所有这些要求。通过系统地研究表面结构与电催化反应性之间的关系，本项目所研究的精心设计的表面结构可以帮助理解这些催化剂的局限性。与研究活动相结合的是俄亥俄州立大学（OSU）现有基础设施的一系列教育和推广工作。作为俄勒冈州立大学加强学习研究经验（REEL）计划的一部分，正在开发电催化研究密集型本科实验室模块。柯教授和她的小组成员也参与外展活动，以提高代表性不足的群体对科学的兴趣，并通过俄勒冈州立大学的STEAM工厂吸引公众参与。通过这个奖项，化学学部的化学催化项目资助俄亥俄州立大学的Anne Co博士对二氧化碳到碳氢化合物的电化学转化进行系统的研究。一系列高度可控的表面，旨在促进特定中间体的吸附，通过低电位沉积应变铜单层和多孔铜基双金属膜，在设计中选择促进C-H和C-C键的选择性形成。电化学和原位光谱测量相结合，辅以理论建模，用于阐明电化学反应条件下活性中心周围的机理途径和化学环境。本项目对表面结构和反应性关系的研究所获得的知识，直接影响到对表面电催化过程的一般理解，以及对CO2电还原具体反应的理解。