Novel Catalysts for Electrochemical Carbon Dioxide Conversion: from Bimetallic Surfaces to Gas Diffusion Electrodes

电化学二氧化碳转化的新型催化剂：从双金属表面到气体扩散电极

• 批准号: 1152778
• 负责人: Giovanni Zangari
• 金额: $ 31.87万
• 依托单位: University of Virginia Main Campus
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2012
• 资助国家: 美国
• 起止时间: 2012-08-15 至 2016-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1152778&HistoricalAwards=false
• 关键词: Novel; Catalysts; Electrochemical; Carbon; Dioxide

With this award from the Chemical Catalysis Program in the Chemistry Division at the National Science Foundation, Professor Giovanni Zangari of the University of Virginia will study new electrocatalyst materials and electrode configurations aimed at electrochemically reducing carbon dioxide. Hydrogenation of carbon dioxide is expected to provide a flexible, efficient route to the realization of a carbon neutral cycle for fuel production, potentially of enormous importance to effectively decrease carbon dioxide concentration in the atmosphere. While current catalysts suffer from poor selectivity and low conversion rates, bimetallic surfaces and surface alloys with lateral compositional gradients and tunable adsorption strength for the various reactants and intermediates have the potential to widely enhance catalyst selectivity and accelerate formation of selected fuels. These novel catalysts will be synthesized by electrochemical methods, and their catalytic activity and selectivity will be tested via product analysis and kinetic investigations of the reaction mechanism. In a successive stage, porous nanoparticle catalysts reproducing the optimized compositions identified previously will be synthesized and impregnated with ionic liquids with the objective of increasing carbon dioxide concentration at the catalytic surface to boost its conversion rate. Finally, gas diffusion electrodes will be fabricated using these porous nanoparticle catalysts and suitable electrode configurations will be developed with the aim of maximizing electrochemical fuel production rates.The proposed research targets the decrease of carbon dioxide concentration in the atmosphere via its electrochemical conversion to useful liquid fuels, potentially powered by renewable energy. By developing materials capable of accelerating carbon dioxide conversion, this research will develop a fundamental understanding of the mechanism of fuel formation by electrochemical processes. This will enable rational catalyst design and optimization as well as enhanced process selectivity. Investigation of various electrode configurations will provide a better insight on the transport of carbon dioxide through heterogeneous media, which could be used to optimize the overall reactor performance. The knowledge developed here will not only facilitate widespread implementation of new technologies for recycling of carbon dioxide, but has the potential to be transferred to a variety of electrochemical conversion processes. Additionally, this research will provide training opportunities for students at the intersection of electrochemistry and materials science, as well as an array of educational activities focused on environmental issues, including a university-wide seminar offering and unique laboratory experiences for undergraduates.

凭借国家科学基金会化学部化学催化计划的这一奖项，弗吉尼亚大学的Giovanni Zangari教授将研究旨在电化学还原二氧化碳的新型电催化剂材料和电极配置。二氧化碳的加氢有望为实现燃料生产的碳中和循环提供灵活、有效的途径，这对有效降低大气中的二氧化碳浓度可能具有巨大的重要性。虽然目前的催化剂存在选择性差和转化率低的问题，但具有横向组成梯度和对各种反应物和中间体的可调吸附强度的表面合金和表面合金具有广泛提高催化剂选择性和加速所选燃料形成的潜力。这些新型催化剂将通过电化学方法合成，并通过产物分析和反应机理的动力学研究来测试它们的催化活性和选择性。在连续的阶段中，将合成再现先前确定的优化组合物的多孔纳米颗粒催化剂，并用离子液体浸渍，目的是增加催化表面的二氧化碳浓度以提高其转化率。最后，气体扩散电极将使用这些多孔纳米颗粒催化剂和合适的电极配置将开发以最大化电化学燃料生产率的目的。拟议的研究目标是通过其电化学转化为有用的液体燃料，可能由可再生能源提供动力，降低大气中的二氧化碳浓度。通过开发能够加速二氧化碳转化的材料，这项研究将对电化学过程形成燃料的机制有一个基本的了解。这将使合理的催化剂设计和优化以及提高工艺选择性成为可能。各种电极配置的调查将提供一个更好的洞察二氧化碳通过非均相介质的传输，这可以用来优化整体反应器的性能。这里开发的知识不仅将促进二氧化碳再循环新技术的广泛实施，而且有可能转移到各种电化学转化过程中。此外，这项研究将为电化学和材料科学交叉点的学生提供培训机会，以及一系列专注于环境问题的教育活动，包括为本科生提供的全校范围的研讨会和独特的实验室体验。