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 化学部环境化学科学项目的支持下，佐治亚理工学院的 Ching-Hua Huang 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) 和金属的多氧化剂系统，以供应用POA、高铁酸盐(VI)和高锰酸盐(VII)是公认的氧化剂，但各自都显示出一些局限性，该项目将探索POA与高浓度氧化剂的组合。多氧化剂系统中的价金属（HVM）或低价金属（LVM）离子可以降解水处理中的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，以最大限度地发挥应用潜力。此外，该项目将加强教育并扩大代表性不足群体的参与，示例活动包括通过与佐治亚州和德克萨斯州的 9 个少数族裔机构合作，教授和招募少数族裔学生参与研究，以及教授 K-12 STEM（科学、技术、 POA 与高价金属 (HVM)（例如高铁酸盐 (VI) 和高锰酸盐 (VII)）或低价金属 (LVM)（例如 Fe(II) 和 Mn( II)) 物质可以显着增强水污染物的降解，产生基于 POA 的自由基和中间高价金属氧代物质（例如 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-金属”系统可以增强(i)碳氢化合物的C-H键活化，以及(ii)水的净化。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，旨在阐明实现金属催化循环以及有机氧化的高效率的机制细节。组合氧化剂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 NSF 的法定使命，并通过使用基金会的智力价值和更广泛的影响审查标准进行评估，被认为值得支持。

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.