Research Project 9: Biomimetic Remediation of Hazardous Substances

研究项目9：有害物质的仿生修复

基本信息

批准号：
7799056
负责人：
Pericles Stavropoulos
金额：
$ 21.51万
依托单位：
BOSTON UNIVERSITY MEDICAL CAMPUS
依托单位国家：
美国
项目类别：
财政年份：
资助国家：
美国
起止时间：
至 2012-09-19
项目状态：
已结题

来源：
https://reporter.nih.gov/project-details/7799056
关键词：
Accounting Air Aromatic Hydrocarbons Basic Science Biological Biomimetics Bioremediations Boston Capital Case Study Chemicals Chemistry Chlorophenols Coupled Decontamination Deposition Development Dioxins Drug Metabolic Detoxication Effectiveness Electrons Ensure Equilibrium Event Family Generations Hand Hazardous Substances Hydroxyl Radical In Situ Intervention Investigation Iron Kinetics Ligands Maintenance Metabolic Metals Methane hydroxylase Methods Modification Mono-S Mononuclear Operative Surgical Procedures Oxidants Oxygenases Pathway interactions Petroleum Plant Resins Polychlorinated Biphenyls Population Principal Investigator Process Property Pump Reagent Reporting Reproduction Research Research Project Grants Site Soil Solvents Superfund System Technology Toxicology Toxin Universities Vinyl Chloride Water Work Xenobiotics analog base catalyst cost cost effective dechlorination design dibenzo(1,4)dioxin dibenzofuran diphenyl field study insight interest member microbial novel organic contaminant oxidation phthalates pollutant programs remediation reproductive success vapor

项目摘要

The proposed research concentrates on the development of oxidative processes for remediation of groundwater and soils/sediments contaminated with halogenated and non-halogenated organics with suspected reproductive and developmental consequences. The treatment relies on catalytic iron reagents whose mode of operation is preferably mimicking that of biological oxygenases (P-450, sMMO), and are thus more selective than other advanced oxidative technologies that make use of indiscriminate hydroxyl radicals. Specifically, the proposed work will provide new and more robust members of a family of monoiron reagents (P-450 analogs), which are supported by electron-rich tripodal ligands designed to stabilize high-valent iron-oxo oxidants and ligand-centered radicals simultaneously. In addition, a new family of diiron reagents (sMMO analogs) will be introduced to afford highly electrophilic oxidants for use in oxygenations of persistent pollutant substrates. Suitable reagents will be investigated in the degradation of a wide range of substrates, including chlorinated solvents, BTEX, phthalates, MTBE and chlorophenols, as well as against recalcitrant lipophilic substrates such as polychlorinated dibenzo-p-dioxins, dibenzofurans and biphenyls. Mechanistic studies associated with metal, ligand, and substrate-centered events will be pursued to report on the suitability of the reagents at hand and evaluate their biomimetic mode of action. The mechanistic work is also expected to provide insights in relation to the currently debated oxygenation pathways of biological oxygenases (P-450, sMMO). The most successful reagents will become the subject of bench-scale, column treatability studies in sequential reductive (Fe(0)) and oxidative treatment zones designed to effect complete degradation of organic contaminants. The oxidative zone will be composed of the oxygenation reagents developed in this study, suitably modified to afford heterogeriized versions of the catalysts supported on inert matrices. The effectiveness on chemical mixtures will be studied in detail.

拟议的研究集中于氧化过程的开发以修复被卤化和非卤化有机物污染的地下水和土壤/沉积物疑似生殖和发育后果。治疗依赖于催化铁试剂其操作模式优选模仿生物加氧酶（P-450，sMMO），并且是因此比其他利用不加选择的羟基的先进氧化技术更具选择性部首。具体来说，拟议的工作将为单铁家族提供新的、更强大的成员试剂（P-450 类似物），由富电子三足配体支持，旨在稳定同时产生高价铁氧氧化剂和配体中心自由基。此外，还有一个新的家庭将引入二铁试剂（sMMO 类似物）以提供高亲电子氧化剂，用于持久性污染物底物的氧化。将研究合适的试剂的降解多种基材，包括氯化溶剂、BTEX、邻苯二甲酸盐、MTBE 和氯酚，以及对抗顽固的亲脂性底物，例如多氯二苯并-对-二恶英、二苯并呋喃和联苯。与金属、配体和底物中心事件相关的机理研究将致力于报告现有试剂的适用性并评估其仿生作用模式。机械工作也有望提供有关当前有争议的氧合的见解生物加氧酶途径（P-450，sMMO）。最成功的试剂将成为主题连续还原 (Fe(0)) 和氧化处理区的小台规模、柱可处理性研究旨在实现有机污染物的完全降解。氧化区将由以下部分组成本研究中开发的氧化试剂经过适当修改以提供杂化版本负载在惰性基质上的催化剂。将详细研究对化学混合物的有效性。