Collaborative Research: Synergistic Actions of Peroxy Acids and Metals for Advanced Water Treatment: Delineating Multi-Oxidant Mechanisms

在美国国家科学基金会化学部环境化学科学项目的支持下，乔治亚理工学院的黄庆华教授和德克萨斯农工大学的Virender Sharma教授将研究涉及过氧酸（POA）和金属的多氧化系统在水处理中的应用。POA，高铁酸盐（VI）和高锰酸盐（VII）是公认的氧化剂，但它们各自都有一些局限性。该项目将探索POA与高价金属（HVM）或低价金属（LVM）离子在多氧化剂系统中的结合，可以降解水处理中的污染物并激活有机合成中的化学键。本项目旨在阐明其基本反应动力学和机理，以最大限度地发挥其应用潜力。此外，该项目将加强教育，扩大代表性不足群体的参与。例如，通过与乔治亚州和德克萨斯州的九所少数族裔机构合作，教授和招募少数族裔学生参与研究，并教授K-12 STEM（科学、技术、工程和数学）教师。POA与高价金属（HVM）（如高铁酸盐（VI）和高锰酸盐（VII））或低价金属（LVM）（如铁（II）和锰（II））的相互作用可以显著增强水污染物的降解。poa基自由基和中间高价金属氧的生成(如Fe（V， IV)=O, Mn(VI， V， IV)=O）可能提供了大大增强的多氧化剂条件。所提出的“POA-Metal”体系可以增强(i)碳氢化合物的C-H键活化和（ii）水的去污。该项目结合了互补的实验室实验、动力学建模和计算化学计算，努力阐明机理细节，以实现金属的催化循环和高效的有机氧化。对组合氧化剂的新见解有可能产生强大的催化氧化系统，用于合成化学和水处理。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 Environmental Chemical Sciences Program of the NSF Division of Chemistry, Professors Ching-Hua Huang of Georgia Institute of Technology and Virender Sharma of Texas A&M University will study multi-oxidant systems that involve peroxy acids (POA) and metals, for applications in water treatment. POA, ferrate(VI) and permanganate(VII) are well-recognized oxidants, but each shows some limitations individually. The project will explore the combination of POA with high valent metal (HVM) or low valent metal (LVM) ions in a multi-oxidant system that can degrade contaminants in water treatment and activate chemical bonds in organic synthesis. This project aims to elucidate the fundamental reaction kinetics and mechanisms to maximize the application potential. Additionally, this project will enhance education and broaden participation of underrepresented groups. Example activities include teaching and recruiting minority students to participate in research though partnerships with nine minority institutions in Georgia and Texas and teaching K-12 STEM (science, technology, engineering and mathematics) teachers. The interaction of POA with either high-valent metal (HVM) (e.g., ferrate(VI) and permanganate(VII)) or low-valent metal (LVM) (e.g., Fe(II) and Mn(II)) species can significantly enhance the degradation of water contaminants. The generation of POA-based radicals and intermediate high-valent metal oxo species (e.g., Fe(V, IV)=O, Mn(VI, V, IV)=O) likely provides the much enhanced multi-oxidants conditions. The proposed “POA-Metal” system can enhance (i) the C-H bond activation of hydrocarbons, and (ii) decontamination of water. This project combines complementary laboratory experiments, kinetic modeling, and computational chemistry calculations in an effort to elucidate mechanistic details to achieve catalytic cycling of the metal as well as high efficiency in the organic oxidation. The new insights into the combined oxidants have the possibility of generating robust catalytic oxidative systems for use in both synthetic chemistry and water treatment.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.