Monopersulfate oxidation of tetrabromobisphenol A by an iron(III)-phthalocyaninetetrasulfate catalyst coordinated to imidazole functionalized silica particles
Monopersulfate oxidation of tetrabromobisphenol A by an iron(III)-phthalocyaninetetrasulfate catalyst coordinated to imidazole functionalized silica particles
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DOI：
10.1016/j.molcata.2015.02.003
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发表时间：
2015-05
影响因子：
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通讯作者：
Shohei Maeno;Qianqian Zhu;M. Sasaki;Takafumi Miyamoto;M. Fukushima
中科院分区：
文献类型：
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作者：
Shohei Maeno;Qianqian Zhu;M. Sasaki;Takafumi Miyamoto;M. Fukushima
将四硫酸酞菁铁（FePcTS）轴向配位到一系列咪唑功能化的3-（1-咪唑基）丙基氨甲酰基-3 ′-氨丙基二氧化硅（IPS）粒子上。在所制备的FePcTS/IPS催化剂中，最小粒径（<30 μm）的FePcTS/IPS催化剂对四溴双酚A（TBBPA）的氧化活性高于较大粒径（<145 μm和45-145 μm）的FePcTS/IPS催化剂。比较了FePcTS/IPS与结构类似物四（对磺酸基苯基）卟啉铁（FeTPPS）负载IPS（FeTPPS/IPS）的催化活性。FePcTS/IPS氧化TBBPA的TOF值（11-17 h-1）远大于FeTPPS/IPS在不存在和存在腐殖酸（垃圾渗滤液中的主要共存物质）时的相应值（0.7-3.5 h-1）。为了研究FePcTS和FeTPPS体系催化活性差异的原因，测试了SO 4自由基点清除剂乙醇对TBBPA氧化的影响。FePcTS/IPS的TOF值随乙醇浓度的增加而降低，而FeTPPS/IPS的催化活性不受乙醇的影响。这些结果表明，FePcTS催化体系的高催化活性可以归因于自由基物种的贡献，自由基物种可以通过Fe（III）-过氧物种中O单键O键的均裂产生。
An iron(III)-phthalocyaninetetrasulfate (FePcTS) was axially coordinated to a series of imidazole functionalized silica, 3-(1-imidazolyl)propylcarbamoyl-3′-aminopropylsilica (IPS) particles. Among the prepared FePcTS/IPS catalysts, catalytic activity for the oxidation of tetrabromobisphenol A (TBBPA) for the smallest sized particle (<30 μm) was more effective than larger sizes (145 μm< and 45–145 μm). The catalytic activity of FePcTS/IPS was compared with that of a structural analogue, iron(III)-tetrakis(p-sulfonatephenyl)porphyrin (FeTPPS) supported IPS (FeTPPS/IPS). The TOF values for the oxidation of TBBPA by FePcTS/IPS (11–17 h−1) were much larger than the corresponding values for FeTPPS/IPS (0.7–3.5 h−1) in the absence and presence of humic acid, a major coexistent substance in landfill leachates. To investigate the reasons for the differences in catalytic activities between the FePcTS and FeTPPS systems, the influence of ethanol, a SO4radical dot−scavenger, on the oxidation of TBBPA oxidation was tested. The TOF values for FePcTS/IPS decreased with increasing ethanol concentration, while the catalytic activities for FeTPPS/IPS were not affected by adding ethanol. These results suggest that the higher catalytic activity of the FePcTS catalytic system can be attributed to the contribution of radical species, which can be generated via the homolysis of Osingle bondO bonding in the Fe(III)-peroxo species.