CAS: Developing Homogeneous Mn Catalyst Systems for the Oxygen Reduction Reaction
CAS:开发用于氧还原反应的均相锰催化剂体系
基本信息
- 批准号:2102156
- 负责人:
- 金额:$ 47.5万
- 依托单位:
- 依托单位国家:美国
- 项目类别:Standard Grant
- 财政年份:2021
- 资助国家:美国
- 起止时间:2021-05-01 至 2025-04-30
- 项目状态:未结题
- 来源:
- 关键词:
项目摘要
With the support of the Chemical Catalysis program in the Division of Chemistry, Dr. Charles W. Machan of the University of Virginia is studying the catalytic reduction of dioxygen by molecular manganese compounds. The reduction of dioxygen is important for producing energy from chemical bonds. Fuel cells, for example, often employ the reduction of dioxygen to water to generate clean energy. The current best catalysts for this reaction are based on platinum metal, which is rare and expensive. In the search for earth-abundant alternatives, systems containing iron and cobalt have been studied extensively, however, manganese versions of these systems are more poorly understood. Manganese generally interacts strongly with dioxygen and has the potential to rival or exceed the catalytic activity of iron or cobalt. These studies will achieve this by developing design principles for dioxygen reduction by manganese complexes, thus enabling optimized systems with improved performance. Integrated into these efforts is a research-focused educational outreach program, which will develop a scientific communication training program and a research-based lab experience. The integrated research and educational components will address fundamental challenges for the field and priorities of the current NSF Strategic Plan, with the goal of maximizing the health, environmental and economic benefits of renewable energy technologies.With the support of the Chemical Catalysis program in the Division of Chemistry, Dr. Charles W. Machan of the University of Virginia is studying the catalytic reduction of dioxygen by molecular manganese compounds. When paired with the oxidation of energy rich molecules, dioxygen reduction is a convenient way to drive oxidation reactions or to convert chemical energy to electrical energy. Manganese metal centers, while underrepresented as molecular catalyst active sites, have strong interactions with dioxygen and could demonstrate catalytic activity that rivals or exceeds the activity of more well-understood iron and cobalt species. A coordination chemistry-based approach will be used to enhance the binding and activation of dioxygen by tuning electronic properties at the Mn center, with the ultimate goal of improving catalytic performance. In initial studies, conditions for the selective generation of hydrogen peroxide or water as the reaction product have been developed: hydrogen peroxide is a valuable chemical oxidant and water is the desired half-reaction for fuel cells. Understanding how to achieve high selectivity and activity for each of these products has implications for renewable energy utilization. To address the ongoing need for fundamental understanding of the reduction of dioxygen by manganese complexes, the role of axial ligands in dioxygen binding and activation will be quantified, the catalytic response will be improved by synthetically modifying the ligand framework, and conditions for selective hydrogen peroxide and water production will be sought using redox mediators.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.
在化学系化学催化项目的支持下,查尔斯W。弗吉尼亚大学的Machan正在研究分子锰化合物对分子氧的催化还原。分子氧的还原对于从化学键产生能量是重要的。例如,燃料电池通常利用分子氧还原为水来产生清洁能源。目前用于该反应的最好的催化剂是基于铂金属,其稀有且昂贵。在寻找地球上丰富的替代品时,对含有铁和钴的系统进行了广泛的研究,然而,对这些系统的锰版本了解甚少。锰通常与分子氧强烈相互作用,并且具有竞争或超过铁或钴的催化活性的潜力。这些研究将通过开发锰络合物还原分子氧的设计原理来实现这一目标,从而使优化的系统具有更好的性能。这些努力中包括一个以研究为重点的教育推广计划,该计划将开发一个科学交流培训计划和一个以研究为基础的实验室体验。综合研究和教育部分将解决该领域的基本挑战和当前NSF战略计划的优先事项,以最大限度地提高可再生能源技术的健康,环境和经济效益为目标。弗吉尼亚大学的Machan正在研究分子锰化合物对分子氧的催化还原。当与富含能量的分子的氧化配对时,分子氧还原是驱动氧化反应或将化学能转化为电能的方便方式。锰金属中心,虽然作为分子催化剂活性位点的代表性不足,但与分子氧具有很强的相互作用,并且可以表现出与更好理解的铁和钴物种的活性相媲美或超过其活性的催化活性。基于配位化学的方法将用于通过调节Mn中心的电子性质来增强分子氧的结合和活化,最终目标是提高催化性能。在最初的研究中,已经开发了选择性生成过氧化氢或水作为反应产物的条件:过氧化氢是有价值的化学氧化剂,水是燃料电池所需的半反应。了解如何实现这些产品的高选择性和活性对可再生能源的利用具有重要意义。为了解决对锰络合物还原分子氧的基本理解的持续需求,将量化轴向配体在分子氧结合和活化中的作用,将通过合成修饰配体框架来改善催化响应,该奖项反映了NSF的法定使命,并被认为是值得的,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来提供支持。
项目成果
期刊论文数量(9)
专著数量(0)
科研奖励数量(0)
会议论文数量(0)
专利数量(0)
Controlling Product Selectivity During Dioxygen Reduction with Mn Complexes Using Pendent Proton Donor Relays and Added Base
使用悬垂质子供体继电器和添加碱在锰配合物还原过程中控制产物选择性
- DOI:10.1039/d3sc02611f
- 发表时间:2024
- 期刊:
- 影响因子:8.4
- 作者:Cook, Emma N.;Courter, Ian M.;Dickie, Diane A.;Machan, Charles W.
- 通讯作者:Machan, Charles W.
Bioinspired mononuclear Mn complexes for O 2 activation and biologically relevant reactions
用于 O 2 活化和生物学相关反应的仿生单核锰配合物
- DOI:10.1039/d1dt03178c
- 发表时间:2021
- 期刊:
- 影响因子:4
- 作者:Cook, Emma N.;Machan, Charles W.
- 通讯作者:Machan, Charles W.
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Charles Machan其他文献
Charles Machan的其他文献
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{{ truncateString('Charles Machan', 18)}}的其他基金
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 - 财政年份:2024
- 资助金额:
$ 47.5万 - 项目类别:
Standard Grant
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