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.

拟议的研究集中于用于修复氧化过程的发展地下水和土壤/沉积物，被卤代有机物污染可疑的生殖和发展后果。治疗依赖于催化铁试剂最好的操作模式是模仿生物氧酶（P-450，SMMO）的操作模式，并且是因此，比使用不加选择的羟基的其他晚期氧化技术更有选择性激进分子。具体而言，拟议的工作将为单人类家族提供新的，更强大的成员试剂（p-450类似物），由富含电子的三座配体支持，旨在稳定高价值铁氧氧化剂和以配体为中心的自由基同时。此外，一个新家庭将引入二铁试剂（SMMO类似物），以提供高度亲电的氧化剂供持续污染物底物的氧合。合适的试剂将在降解中研究广泛的底物，包括氯化溶剂，BTEX，邻苯二甲酸盐，MTBE和氯苯酚，AS 以及针对顽固的亲脂性底物，例如多氯联苯 - 二氧蛋白，二苯并呋喃和双苯基。与金属，配体和以底物为中心事件相关的机械研究将是追求报告手头试剂的适用性，并评估其仿生作用方式。预计机械工作还将提供与当前争论的氧合有关的见解生物氧酶（P-450，SMMO）的途径。最成功的试剂将成为主题台式尺寸，柱状可处理性研究，顺序还原（Fe（0））和氧化处理区旨在实现有机污染物的完全降解。氧化区将由这项研究中开发的氧合试剂，适当修改以提供异质化版本支撑惰性矩阵的催化剂。将详细研究对化学混合物的有效性。