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

合作研究：过氧酸和金属在高级水处理中的协同作用：描述多氧化剂机制

• 批准号: 2107967
• 负责人: Virender Sharma
• 金额: $ 20万
• 依托单位: The Texas A&M University System HSC
• 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: 2021-09-01 至 2024-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2107967&HistoricalAwards=false
• 关键词: Collaborative; Research; Synergistic; Actions; Peroxy

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.

在NSF化学部的环境化学科学计划的支持下，德克萨斯州A＆M大学的佐治亚州技术研究所和Virender Sharma教授将研究涉及过氧酸（POA）和金属的多氧化系统，用于水处理。 POA，Ferrate（VI）和锰酸盐（VII）是公认的氧化物，但每种都会单独显示一些局限性。该项目将在多氧化剂系统中探索POA与高价值金属（HVM）或低价值金属（LVM）离子的组合，该系统可以在水处理中降解污染物并激活有机合成中的化学键。该项目旨在阐明基本反应动力学和机制，以最大程度地发挥应用潜力。此外，该项目将增强教育并扩大代表性不足的群体的参与。示例活动包括教学和招募少数民族学生，通过与佐治亚州和德克萨斯州的九个少数族裔机构的合作伙伴关系，以及教学K-12 STEM（科学，技术，工程和数学）教师。 POA与高价值金属（HVM）（例如Ferrate（VI）和高烷酸（VII））或低价值金属（LVM）（例如Fe（II）和Mn（II）和Mn（II））物种的相互作用可以显着增强水污染物的降解。基于POA的自由基和中间高价值金属氧物种（例如Fe（V，IV）= O，Mn（VI，V，IV，IV）= O）的产生可能提供了大大增强的多氧化剂条件。所提出的“ POA-METAL”系统可以增强（i）碳氢化合物的C-H键激活，以及（ii）水对水的污染。该项目结合了完整的实验室实验，动力学建模和计算化学计算，以阐明机械细节以实现金属的催化循环以及有机氧化的高效率。对合并氧化物的新见解具有在合成化学和水处理中生成可靠的催化氧化系统。该奖项反映了NSF的法定任务，并被认为是通过基金会的智力优点和更广泛的影响审查标准通过评估来获得的支持。

项目成果

Enhanced Oxidation of Antibiotics by Ferrate Mediated with Natural Organic Matter: Role of Phenolic Moieties

• DOI: 10.1021/acs.est.3c03165
• 发表时间: 2023-06
• 期刊: Environmental Science & Technology
• 影响因子: 11.4
• 作者: B. Guo;Junyue Wang;K. Sathiyan;Xingmao Ma;E. Lichtfouse;Ching-Hua Huang;V. Sharma

Oxidation of Pharmaceuticals by Ferrate(VI)–Amino Acid Systems: Enhancement by Proline

• DOI: 10.1021/acs.jpca.3c00134
• 发表时间: 2023-03
• 期刊: The Journal of Physical Chemistry. a
• 作者: V. Sharma;Junyue Wang;Mingbao Feng;Ching-Hua Huang

Overlooked Role of Chromium(V) and Chromium(IV) in Chromium Redox Reactions of Environmental Importance

• DOI: 10.1021/acsestwater.1c00409
• 发表时间: 2022-05
• 期刊: ACS ES&T Water
• 作者: Joshua Bell;Xingmao Ma;T. McDonald;Ching-Hua Huang;V. Sharma

Interaction of peracetic acid with chromium(III): Understanding degradation of coexisting organic pollutants in water

过氧乙酸与铬(III) 的相互作用：了解水中共存有机污染物的降解

• DOI: 10.1016/j.jhazmat.2022.129537
• 发表时间: 2022
• 期刊: Journal of Hazardous Materials
• 影响因子: 13.6
• 作者: Bell, Joshua;Wen, Yinghao;Ma, Xingmao;McDonald, Thomas J.;Huang, Ching-Hua;Sharma, Virender K.
• 通讯作者: Sharma, Virender K.