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Facilitation of humification of recalcitrant chlorinated organic compounds via the catalytic oxidation and toxicity of humification products

通过腐殖化产物的催化氧化和毒性促进顽固氯化有机化合物的腐殖化

基本信息

批准号：
14380283
负责人：
FUKUSHIMA Masami
金额：
$ 6.85万
依托单位：
National Institute of Advanced Industrial Science and Technology (AIST)
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

Humic substances (HSs) were extracted from 14-types of soils, and the correlations between the parameters of humification (e.g. elemental composition and contents of acidic functional groups) and the percentages of pentachlorophenol (PCP) degradation were investigated in the catalytic oxidation system with iron(III)-porphyrin complex and KHSO_5. It found that the percentages of PCP degradation were largely reduced by the presence of HSs, which were of lower degree of humification (Environ.Sci.Technol. 2003,37,1031). On the other hand, PCP was oxidized to reaction intermediates, such as phenoxy radicals, and this resulted in the formation of humification products via the radical coupling. A bioassay (Microtox test) of the reaction products demonstrated that the toxicity of PCP was largely reduced by forming the humification products (Environ.Sci.Technol. 2003,37,386). When the catalytic system with iron(III)-porphyrin complex and KHSO_5 was applied to the PCP-contaminated soil, the PCP removal from the soil was enhanced by adding peat HS. This implies that the addition of HS with lower degree of humification is useful for the detoxification of PCP-contaminated soils (Toxicol.Environ.Chem. 2003,85,39). In addition, other biomimetic catalysts as well as iron(III)-porphyrin complex, such as iron(III)-phthalocyanine and manganese(III)-porphyrin complexes, were also useful for enhancing PCP degradation in the presence of peat HSs. I supposed from the model experiments using cyclodextrin that such effects of HS with lower degree of humification may be attributed to the interactions between biomimetic catalysts and the sugar moieties in HSs (J.Mol.Catal. A, in press).

从14类土壤中提取腐殖质(HSs)，研究铁(III)-卟啉络合物和KHSO_5催化氧化体系中腐殖化参数(元素组成、酸性官能团含量等)与五氯酚(PCP)降解率的相关性。结果发现，腐殖化程度较低的 HS 的存在大大降低了五氯苯酚的降解百分比（Environ.Sci.Technol. 2003,37,1031）。另一方面，PCP被氧化成反应中间体，例如苯氧基自由基，这导致通过自由基偶联形成腐殖化产物。反应产物的生物测定（Microtox 测试）表明，通过形成腐殖化产物，五氯苯酚的毒性大大降低（Environ.Sci.Technol. 2003,37,386）。当铁(III)-卟啉络合物和KHSO_5催化体系应用于PCP污染土壤时，添加泥炭HS增强了PCP从土壤中的去除。这意味着添加腐殖化程度较低的 HS 对于 PCP 污染土壤的解毒是有用的 (Toxicol.Environ.Chem. 2003,85,39)。此外，其他仿生催化剂以及铁(III)-卟啉络合物，例如铁(III)-酞菁和锰(III)-卟啉络合物，也可用于在泥炭HS存在下增强PCP降解。我从使用环糊精的模型实验中推测，腐殖化程度较低的 HS 的这种影响可能归因于仿生催化剂和 HS 中糖部分之间的相互作用（J.Mol.Catal.A，出版中）。