Fukushima Masami, Shigematsu Satoko, Nagao Seiya
Division of Solid Waste, Resources and Geoenvironmental Engineering, Graduate School of Engineering, Hokkaido University, Sapporo, Japan.
J Environ Sci Health A Tox Hazard Subst Environ Eng. 2009 Sep;44(11):1088-97. doi: 10.1080/10934520903005079.
A supramolecular catalyst consisting of 5,10,15,20-tetrakis(p-hydroxyphenyl)porphine-iron(III) (FeTPP(OH)(4)) bound to humic acid (HA) was synthesized via formaldehyde polycondensation. The catalytic system, which included the synthesized catalyst (resol) and an oxygen donor (KHSO(5)), was applied to the oxidative degradation of 2,4,6-trichlorophenol (TrCP) and pentachlorophenol (PCP) in contaminated soil suspensions. The optimal conditions (catalyst, KHSO(5) and substrate concentrations) were investigated. In both FeTPP(OH)(4) and resol catalytic systems, more than 95% of TrCP (100 microM) and PCP (25 microM) degraded at pH 4, [catalyst] 20 microM and [KHSO(5)] 1 mM. When initial concentrations of TrCP and PCP were increased to TrCP 200 micro M and PCP 50 micro M, the percent degradation of the CPs and the levels of dechlorination in the resol catalytic system were significantly greater than the values obtained using the FeTPP(OH)(4) system. These results show that the synthesized resol catalyst effectively enhances oxidative degradation of TrCP and PCP in contaminated soil suspensions. The resol catalysts adsorbed to contaminated soils were at levels that were significantly greater than those of FeTPP(OH)(4). Therefore, the enhanced degradation of CPs by resol catalysts can be attributed to the interactions between adsorbed CPs on the soil surface and the catalytic center of the resol catalysts.
通过甲醛缩聚反应合成了一种由与腐殖酸（HA）结合的5,10,15,20-四（对羟基苯基）卟啉铁（III）（FeTPP(OH)(4)）组成的超分子催化剂。该催化体系包括合成的催化剂（甲阶酚醛树脂）和氧供体（KHSO(5)），用于污染土壤悬浮液中2,4,6-三氯苯酚（TrCP）和五氯苯酚（PCP）的氧化降解。研究了最佳条件（催化剂、KHSO(5)和底物浓度）。在FeTPP(OH)(4)和甲阶酚醛树脂催化体系中，在pH值为4、[催化剂]为20μM和[KHSO(5)]为1 mM的条件下，超过95%的TrCP（100μM）和PCP（25μM）发生了降解。当TrCP和PCP的初始浓度增加到TrCP 200μM和PCP 50μM时，甲阶酚醛树脂催化体系中CPs的降解百分比和脱氯水平显著高于使用FeTPP(OH)(4)体系获得的值。这些结果表明，合成的甲阶酚醛树脂催化剂有效地增强了污染土壤悬浮液中TrCP和PCP的氧化降解。吸附在污染土壤上的甲阶酚醛树脂催化剂的含量显著高于FeTPP(OH)(4)。因此，甲阶酚醛树脂催化剂对CPs降解的增强作用可归因于土壤表面吸附的CPs与甲阶酚醛树脂催化剂催化中心之间的相互作用。
