Laboratory of Chemical Resources, Division of Sustainable Resources Engineering, Graduate School of Engineering, Hokkaido University, Sapporo, Japan.
J Environ Sci Health A Tox Hazard Subst Environ Eng. 2013;48(13):1593-601. doi: 10.1080/10934529.2013.815078.
Iron(III)-porphyrin complexes are generally regarded as green catalysts, since they mimic the catalytic center of cytochrome-P450 and widely used as green catalysts for degrading halogenated phenols in wastewater, such as landfill leachates. However, iron(III)-porphyrins are deactivated by self-oxidation in the presence of an oxygen donor, such as KHSO5. In the present study, to enhance the reusability of an iron(III)-porphyrin catalyst, iron(III)-5,10,15,20-tetrakis(4-carboxyphenyl) porphyrin (FeTCPP) was immobilized on a functionalized silica gel. The oxidative degradation of 2,4,6-tribromophenol (TrBP), a widely used brominated flame retardant that is found in landfill leachates, was examined using the prepared catalyst. In addition, the influence of humic substances (HSs), major components of leachates, on the TrBP oxidation was investigated. Concerning the effect of pH, more than 90% of the TrBP was degraded in the pH range of 3-8 in the absence of HS, while the optimal pH for the reaction was in the range of pH 5-7 in the presence of HS. Although the oxidation of TrBP was inhibited in the presence of HSs, more than 90% of the TrBP was degraded in the presence of 50 mg L(-1) of HS. Thus, the prepared catalyst, SiO2-FeTCPP, showed a high catalytic activity and could be reused up to 10 times even in the presence of HS.
铁(III)-卟啉配合物通常被认为是绿色催化剂,因为它们模拟细胞色素 P450 的催化中心,并广泛用作降解废水中卤代酚(如垃圾渗滤液)的绿色催化剂。然而,在氧气供体(如 KHSO5)存在下,铁(III)-卟啉会自氧化而失活。在本研究中,为了提高铁(III)-卟啉催化剂的可重复使用性,将铁(III)-5,10,15,20-四(4-羧基苯基)卟啉(FeTCPP)固定在功能化硅胶上。使用制备的催化剂研究了 2,4,6-三溴苯酚(TrBP)的氧化降解,TrBP 是一种广泛用于垃圾渗滤液的溴化阻燃剂。此外,还研究了垃圾渗滤液主要成分腐殖质(HSs)对 TrBP 氧化的影响。关于 pH 的影响,在不存在 HS 的情况下,TrBP 在 3-8 的 pH 范围内降解超过 90%,而在存在 HS 的情况下,反应的最佳 pH 范围在 5-7。尽管 HSs 的存在抑制了 TrBP 的氧化,但在存在 50mg/L 的 HS 的情况下,仍有超过 90%的 TrBP 被降解。因此,即使在 HS 存在的情况下,制备的催化剂 SiO2-FeTCPP 也表现出很高的催化活性,可重复使用多达 10 次。