Room Temperature and Atmospheric Pressure Dioxygen Activation for the Deep Oxidation of Organic Wastes (TSE03-O)

本研究的目的是在温和的反应条件下，利用空气中的二氧作为氧化剂来破坏有机污染物及其替代物。我们最近发现了一种从空气中提取含水、室温和常压双氧的方法。该方案的优点在于只需要空气、水、铁颗粒和合适的铁螯合剂（Fe(0)/EDTA/O2）。该工艺不使用昂贵的贵金属催化剂。这一过程是罕见的室温下非生物双氧活化的实例。据我们所知，这是在如此温和的反应条件下，以双氧作为最终氧化剂进行氯化有机化合物完全降解的唯一实例。我们最近证明了该系统对多种代物的氧化能力，包括4-氯酚、五氯酚、苯酚、硝基苯和马拉硫磷。在所有情况下，起始化合物都被分解成更简单的无毒羧酸和二氧化碳。在这项研究中，我们打算研究该系统能够从O2中产生动力学上容易氧化的物质的机制，通过产物的元素平衡研究反应途径，调查该系统的氧化能力。在科学和技术两方面的研究方面，还提出了该过程的动力学研究。诸如Fe(0)溶解速率、O2需求和EDTA浓度等变量都是提高反应动力学的最终目标。(2)拟议活动所产生的更广泛影响。人们对发现一种在温和反应条件下用廉价试剂破坏有机污染物的方法非常感兴趣。Fe(0)/EDTA/O2工艺符合这些标准。最终，希望该系统将导致现场便携式有机污染物销毁方案的发展，可以迅速商业化和非专业人员使用。Fe(0)/EDTA/O2工艺有很大的扩大可能性，因为不需要专门的催化剂或试剂来激活二氧。

0328827 Cheng (1) Intellectual merit of the proposed activityThe aim of this investigation is to use dioxygen from air as the oxidizing agent for the destruction of organic pollutants and their surrogates under mild reaction conditions. We have recently discovered a method for the aqueous, room temperature, and atmospheric pressure of dioxygen from air. Such scheme is remarkable in that only air, water, iron particles, and a suitable iron chelation agent are required (Fe(0)/EDTA/O2). No expensive precious metal catalysts are used in the process. This process is a rare instance of abiotic dioxygen activation at room temperature. To our knowledge this is the only instance in which complete degradation of chlorinated organics compounds proceeds with dioxygen as the ultimate oxidant under such mild reaction conditions. We have recently demonstrated this system's oxidizing capabilities on a variety of surrogates including 4-chlorophenol, pentachlorophenol, phenol, nitrobenzene, and malathion. In all cases the starting compounds were degraded into simpler non-toxic carboxylic acids, and carbon dioxide. In this study we intend to examine the mechanism by which this system is able to generate kinetically facile oxidizing species from O2, a study of the reaction pathways through an elemental balance of the products, a survey of the oxidizing capabilities of this system. In terms of a study with both scientific and technical aspects, kinetic studies of the process are also proposed. Variables such as Fe(0) dissolution rate, O2 demand, and EDTA concentration are of interest with the eventual goal of increasing reaction kinetics.(2) Broader impacts resulting from the proposed activity.There is a significant interest in the discovery of a method for the destruction of organic pollutants under mild reaction conditions with inexpensive reagents. The Fe(0)/EDTA/O2 process fulfills these criteria. Ultimately, it is hoped that this system will lead to the development of field portable organic pollutant destruction schemes that can be rapidly commercialized and used by non-specialized personnel. The Fe(0)/EDTA/O2 process has a strong possibility for scale-up since there are no specialized catalysts or reagents required to activate dioxygen.