Monopersulfate oxidation of tetrabromobisphenol A by an iron(III)-phthalocyaninetetrasulfate catalyst coordinated to imidazole functionalized silica particles

被引:51
作者
Maeno, Shohei [1 ]
Zhu, Qianqian [1 ]
Sasaki, Masahide [2 ]
Miyamoto, Takafumi [1 ]
Fukushima, Masami [1 ]
机构
[1] Hokkaido Univ, Div Sustainable Resources Engn, Lab Chem Resources, Fac Engn, Sapporo, Hokkaido 0608628, Japan
[2] Natl Inst Advanced Ind Sci & Technol, Toyohira Ku, Sapporo, Hokkaido 0628517, Japan
关键词
Iron(III)-phthalocyanine-4,4 ',4 '',4 '''-tetrasulfonic acid; Imidazole functionalized silica; Iron(III)-tetrakis(p-sulfonatephenyl)porphyrin; Catalytic oxidation; HYDROXYPROPYL-BETA-CYCLODEXTRIN; CONTAMINATED SOIL SUSPENSIONS; HUMIC-ACID; POTASSIUM MONOPERSULFATE; FORMALDEHYDE POLYCONDENSATION; PORPHYRIN COMPLEX; IRON(III)-PHTHALOCYANINE-TETRASULFONIC ACID; BIOMIMETIC CATALYSTS; HYDROGEN-PEROXIDE; FLAME RETARDANTS;
D O I
10.1016/j.molcata.2015.02.003
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
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 mu m) was more effective than larger sizes (145 mu m< and 45-145 mu m). 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 SO4 center 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 O-O bonding in the Fe(III)-peroxo species. (C) 2015 Elsevier B.V. All rights reserved.
引用
收藏
页码:56 / 63
页数:8
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