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Fundamental researches on the novel process for laboratory waste treatment by supercritical water oxidation

超临界水氧化处理实验室废弃物新工艺的基础研究

基本信息

批准号：
14380264
负责人：
OSHIMA Yoshito
金额：
$ 10.82万
依托单位：
The University of Tokyo
依托单位国家：
日本
项目类别：
Grant-in-Aid for Scientific Research (B)
财政年份：
2002
资助国家：
日本
起止时间：
2002 至 2003
项目状态：
已结题

项目摘要

The objective of this project was to obtain the fundamental engineering information on the lab-waste treatment process by supercritical water oxidation (SCWO). The outreaches of this project are summarized as follows.(1)For the degradation of 2-chrolophenol (2-CP), chosen as a model compound of halogenated organic compounds, a consecutive combination of pyrolysis with oxidation was suggested to be effective to obtain high conversion of 2-CP and to avoid the formation of undesired by-products. In the decomposition of chrolobenzoic acid, very high selectivities for dechrolinated products can be achieved, particularly at lower temperatures. It was also found that addition of such alkali species as Na and K promotes dechlorination of 2-CP.(2)In the co-oxidation of such refractory compounds as acetic acid, phenol and methane with alcohol in supercritical water, it was experimentally suggested that the presence of alcohols enhanced the disappearance rate of the co-existing refractory compounds. The calculated results based on detailed chemical kinetics model suggest that the kinetic effect of such mixtures in SCWO is well characterized by the concentration of OH radical.(3)The catalytic oxidation of phenol in the presence of such heterogeneous catalyst as metal oxide or activated carbon was examined. A non-supported MnO, catalyst possessed a strong activity for promoting phenol oxidation, though the overall reaction rate was appreciably influenced by internal mass transfer resistance. From the kinetic analyses, the global rate expression of the surface reaction was determined, and a Langmuir-type mechanism was proposed to explain the reaction orders for phenol, oxygen and water. It was also experimentally demonstrated that phenol can be effectively oxidized with inexpensive carbon catalysts.

本项目的目的是获得有关超临界水氧化(SCWO)处理实验室垃圾的基本工程信息。本课题的主要工作如下：(1)对于作为卤代有机物模型化合物的2-氯苯酚(2-CP)的降解，建议采用热解与氧化相结合的方法，以获得较高的2-CP转化率，并避免产生有害副产物。在氯代苯甲酸的分解中，对脱铬产物的选择性很高，特别是在较低的温度下。在超临界水中，Na、K等碱性物种的加入促进了2-CP的脱氯。(2)在超临界水中乙醇与醋酸、苯酚、甲烷等难降解化合物的共氧化反应中，醇的存在提高了共存难降解化合物的消失率。基于详细的化学动力学模型的计算结果表明，这些混合物在超临界水中的动力学效应可以很好地用羟基自由基浓度来表征。(3)考察了金属氧化物或活性碳等多相催化剂对苯酚的催化氧化。非负载型MnO_2催化剂对苯酚氧化具有较强的催化活性，但总反应速率受内部传质阻力的影响较大。通过动力学分析，确定了表面反应的全局速率表达式，并提出了解释苯酚、氧气和水的反应级数的朗缪尔型反应机理。实验还证明，廉价的碳催化剂可以有效地氧化苯酚。