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

0328827 程 (1)本研究的目的是利用空气中的分子氧作为氧化剂，在温和的反应条件下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在室温和大气压下制取分子氧的方法。这种方案的显著之处在于仅需要空气、水、铁颗粒和合适的铁螯合剂（Fe（0）/EDTA/O2）。在该过程中不使用昂贵的贵金属催化剂。这一过程是一个罕见的非生物双氧在室温下激活的例子。据我们所知，这是在如此温和的反应条件下，用分子氧作为最终氧化剂完全降解氯化有机化合物的唯一实例。我们最近已经证明了这个系统的氧化能力，对各种替代品，包括4-氯苯酚，五氯苯酚，苯酚，硝基苯，马拉硫磷。在所有情况下，起始化合物降解成更简单的无毒羧酸和二氧化碳。在这项研究中，我们打算研究的机制，该系统是能够产生动力学上容易的氧化物种从O2，通过产品的元素平衡的反应途径的研究，该系统的氧化能力的调查。从科学和技术两个方面进行研究，还建议对该过程进行动力学研究。诸如Fe（0）溶解速率、O2需求和EDTA浓度的变量是感兴趣的，其最终目标是增加反应动力学。(2)拟议活动产生的更广泛影响：人们对发现一种在温和的反应条件下使用廉价试剂销毁有机污染物的方法很感兴趣。Fe（0）/EDTA/O2工艺满足这些标准。最后，希望这一系统将导致制定可迅速商业化并由非专业人员使用的实地便携式有机污染物销毁计划。Fe（0）/EDTA/O2工艺具有很强的放大可能性，因为不需要专门的催化剂或试剂来活化分子氧。

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.