首页> 美国卫生研究院文献>Molecules >Oxidative Debromination and Degradation of Tetrabromo-bisphenol A by a Functionalized Silica-Supported Iron(III)-tetrakis(p-sulfonatophenyl)porphyrin Catalyst
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Oxidative Debromination and Degradation of Tetrabromo-bisphenol A by a Functionalized Silica-Supported Iron(III)-tetrakis(p-sulfonatophenyl)porphyrin Catalyst

机译:功能化二氧化硅负载的铁(III)-四(对磺酰基苯基)卟啉催化剂对四溴双酚A的氧化脱溴和降解

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摘要

Tetrabromobisphenol A (TBBPA), a commonly used brominated flame retardant, also functions as an endocrine disruptor. Thus, the degradation of TBBPA has attracted considerable interest among the scientific community. Iron(III)-porphyrin complexes are generally regarded as “green” catalysts and have been reported to catalyze the efficient degradation and dehalogenation of halogenated phenols in environmental wastewaters. However, they are quickly deactivated due to self-degradation in the presence of an oxygen donor, such as KHSO5. In the present study, an iron(III)-tetrakis(p-sulfonatophenyl)-porphyrin (FeTPPS) was immobilized on imidazole-modified silica (FeTPPS/IPS) via coordination of the Fe(III) with the nitrogen atom in imidazole to suppress self-degradation and thus enhance the catalyst reusability. The oxidative degradation and debromination of TBBPA and the influence of humic acid (HA), a major component in leachates, on the oxidation of TBBPA was investigated. More than 95% of the TBBPA was degraded in the pH range from 3 to 8 in the absence of HA, while the optimal pH for the reaction was at pH 8 in the presence of HA. Although the rate of degradation was decreased in the presence of HA, over 95% of the TBBPA was degraded within 12 h in the presence of 28 mg-C L−1 of HA. At pH 8, the FeTPPS/IPS catalyst could be reused up to 10 times without any detectable loss of activity for TBBPA for degradation and debromination, even in the presence of HA.
机译:四溴双酚A(TBBPA),一种常用的溴化阻燃剂,也可作为内分泌干扰物。因此,TBBPA的降解引起了科学界的极大兴趣。铁(III)-卟啉配合物通常被认为是“绿色”催化剂,据报道可催化环境废水中卤代酚的有效降解和脱卤。但是,由于在氧气供体(例如KHSO5)存在下的自降解作用,它们会迅速失活。在本研究中,通过Fe(III)与咪唑中的氮原子的配位,将铁(III)-四(对磺酰基苯基)-卟啉(FeTPPS)固定在咪唑改性的二氧化硅(FeTPPS / IPS)上自降解,从而提高催化剂的可重复使用性。研究了TBBPA的氧化降解和脱溴作用以及浸出液中主要成分腐殖酸(HA)对TBBPA氧化的影响。在不存在HA的情况下,pH在3至8范围内,超过95%的TBBPA降解,而在存在HA的情况下,该反应的最佳pH值为8。尽管在HA存在下降解速率降低,但是在28 mg-C L -1 HA存在下12小时内,超过95%的TBBPA降解。在pH为8的情况下,即使在存在HA的情况下,FeTPPS / IPS催化剂也可以重复使用多达10次,而对TBBPA降解和脱溴的活性没有任何可检测的损失。

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