CAS:Improving the Activity of Homogeneous Mn Catalysts for the Oxygen Reduction Reaction

CAS：提高均相锰催化剂的氧还原反应活性

• 批准号: 2348515
• 负责人: Charles Machan
• 金额: $ 48.1万
• 依托单位: University of Virginia Main Campus
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2024
• 资助国家: 美国
• 起止时间: 2024-06-01 至 2027-05-31
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2348515&HistoricalAwards=false
• 关键词: CAS; Improving; Activity; Homogeneous; Mn; CAS; Improving; Activity; Homogeneous; Mn

With the support of the Chemical Catalysis program in the Division of Chemistry, Charles W. Machan of the University of Virginia is studying the catalytic reduction of dioxygen by molecular manganese compounds. The reduction of dioxygen can be used for energy production from chemical bonds in devices such as fuel cells, where it is the preferred reaction to pair with the oxidation of chemical fuels to produce power. In order to make these systems deployable and scalable, it is essential to develop catalysts made from earth abundant materials. Although Mn is known to have strong interactions with dioxygen, catalysts made from this metal are relatively rare because effective strategies to accelerate catalysis based on Mn are underdeveloped. These studies on dioxygen reduction are aimed at developing design principles for better manganese catalysts, to achieve sufficient performance metrics to compete with other transition metals. An important part of these efforts is a research-focused educational outreach program to provide students with training in science communication. Kits will also be developed to provide research-based lab experience for undergraduates at all levels. The research goals under study and the educational components under development are addressing important priorities for society by meeting the growing needs for new energy technologies and familiarizing students with energy research at early career stages.Under this award, the Machan research team at the University of Virginia is studying the catalytic reduction of dioxygen by molecular manganese compounds. As an earth abundant transition metal that binds strongly to dioxygen, manganese has great potential to be an effective catalyst for dioxygen reduction. However, to achieve sufficient reaction rates, there is a need to develop strategies for destabilizing the intermediate species. This is an ongoing challenge, since far less is known about the use of manganese as a catalyst for dioxygen reduction than is known for approaches employing other transition metals. These research efforts will address this need by investigating how the primary environment of the manganese active site regulates dioxygen binding, how the transfer of substrate to the active site can be controlled to select for specific reduction products, and how the use of secondary metal ions can disrupt stable manganese dioxygen adducts to accelerate the observed reactions. Overall, these studies on manganese-based dioxygen reduction are evaluating the structure-function parameters that regulate the reaction pathways for the two possible reaction products: hydrogen peroxide and water. By improving the activity of manganese-based electrocatalysts through this iterative design strategy, these studies are addressing the ongoing need for the fundamental understanding of dioxygen reduction, which is required for better renewable energy utilization in the long term.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.

在化学催化计划的支持下，弗吉尼亚大学的Charles W. Machan正在研究分子锰化合物对二氧化物的催化减少。二氧化碳的还原可用于从燃料电池等设备中的化学键产生能源，在这种燃料电池等设备中，这是与化学燃料氧化以产生功率的首选反应。为了使这些系统可部署和可扩展，必须开发由地球丰富材料制成的催化剂。尽管已知MN与二氧化物具有很强的相互作用，但用这种金属制成的催化剂相对较少，因为基于MN加速催化的有效策略欠发达。这些关于二氧化碳减少的研究旨在制定设计原理，以实现更好的锰催化剂，以实现足够的性能指标来与其他过渡金属竞争。这些努力的重要组成部分是以研究为重点的教育外展计划，旨在为学生提供科学传播方面的培训。 还将开发套件，以为各个级别的本科生提供基于研究的实验室经验。正在研究的研究目标和正在开发的教育组成部分通过满足新能量技术的不断增长的需求并在职业生涯早期阶段熟悉能源研究，从而解决了社会的重要重点。在此奖项之后，弗吉尼亚大学的Machan研究团队正在研究分子锰化合物对二氧化基因的催化减少。 作为与二氧化物强烈结合的地球丰富的过渡金属，锰具有很大的潜力，可以成为二氧化物还原的有效催化剂。但是，为了达到足够的反应速率，有必要制定破坏中间物种稳定的策略。这是一个持续的挑战，因为对于使用其他过渡金属的方法所知，使用锰作为二氧化物减少的催化剂知之甚少。这些研究工作将通过调查锰活性位点的主要环境调节二恶英结合，如何控制底物转移到活性位点以选择特定的还原产物以及如何破坏稳定的锰二氧化加合物来调节相对的反应。总体而言，这些对基于锰的二恶英还原的研究正在评估调节两种可能反应产物的反应途径的结构功​​能参数：过氧化氢和水。通过通过这种迭代设计策略改善基于锰的电催化剂的活动，这些研究正在解决对减少二氧化物的基本了解的持续需求，这是长期更好地可再生能源利用所必需的。这项奖项反映了NSF的法定任务，反映了通过评估基金会的智力效果，并通过评估了基金会的范围。