Development of Catalytic Metal-Coupled Electron-Transfer (MCET) for Sustainable Chemical and Electrochemical Oxygen Reduction

在美国国家科学基金会化学部的支持下，布朗大学的杰罗姆·罗宾逊教授正在研究储能技术。这一主题与风能和太阳能“间歇性能源”的有效利用有关。该项目侧重于以过氧化物的形式储存能量，即具有氧-氧键的化合物。氧气的使用是有吸引力的，因为它是地球大气中最丰富的元素之一。目前生产过氧化物的工业路线是能源密集型的。该项目还解决了与个性化能源存储相关的小规模应用。研究小组设计了金属催化剂，利用电化学手段产生过氧化物。该项目为研究生、本科生和高中水平的科学家提供可再生能源和绿色化学领域的实践培训机会。通过夏季研究机会和基于队列的导师和研究人员培训计划，旨在扩大化学领域历史上代表性不足的群体的代表性和保留率。有效和受控的电子和质子传递对于许多可持续能源应用至关重要。尽管取得了重大进展和广泛的研究兴趣，但在低过电位下实现高选择性和高活性仍然是一个艰巨的挑战。在化学部化学催化项目的资助下，布朗大学的Jerome Robinson教授正在推进对催化金属耦合电子转移（MCET）的基本理解，以实现利用地球上丰富的催化剂将氧可持续和选择性地还原为过氧化物。为了实现这一目标，该项目专注于开发电催化MCET工艺，将氧还原为过氧化物，确定和优化刘易斯酸活化剂的周转条件，并管理潜在的竞争途径，如质子耦合电子转移。该奖项反映了美国国家科学基金会的法定使命，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。

With support from the Chemistry Division of the National Science Foundation, Professor Jerome Robinson of Brown University is working on energy storage. This theme is relevant to the efficient use of "intermittent energy" from wind and solar sources. This project focuses on the storage of energy in the form of peroxides, compounds with oxygen-oxygen bonds. The use of oxygen is attractive since it is one of the most abundant elements in the earth's atmosphere. Current industrial routes to peroxides are energy-intensive. The project is also addressing small-scale applications relevant to personalized-energy storage. The research team designs metal catalysts to produce peroxides using electro-chemical means. This project provides hands-on training opportunities in the areas of renewable energy and green chemistry for scientists at the graduate, undergraduate, and high-school levels. Initiatives focusing on broadening representation and increasing retention in historically underrepresented groups in chemistry are being advanced through summer research opportunities and cohort-based mentor and researcher training programs.Efficient and controlled delivery of electrons and protons are critical to many sustainable energy applications. Despite significant advances and intensive research interest, achieving high selectivity and activity at low overpotentials with earth-abundant catalysts remains a formidable challenge. With funding from the Chemical Catalysis Program of the Chemistry Division, Professor Jerome Robinson of Brown University is advancing the fundamental understanding of catalytic metal-coupled electron transfer (MCET) to enable the sustainable and selective reduction of oxygen to peroxide using earth-abundant catalysts. To achieve this goal, this project is focused on developing electrocatalytic MCET processes for the reduction of oxygen to peroxide, identifying and optimizing conditions for turnover of the Lewis-acid activator, and managing potentially competitive pathways such as proton-coupled electron transfer.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.