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八面体分子筛氧化锰催化剂的有机染料绿色分解。

Green decomposition of organic dyes using octahedral molecular sieve manganese oxide catalysts.

机构信息

Department of Chemistry, University of Connecticut, 55 North Eagleville Road, Storrs 06269-3060, USA.

出版信息

J Phys Chem A. 2009 Feb 26;113(8):1523-30. doi: 10.1021/jp807631w. Epub 2009 Jan 29.

DOI:10.1021/jp807631w
PMID:19178167
Abstract

The catalytic degradation of organic dye (methylene blue, MB) has been studied using green oxidation methods (tertiary-butyl hydrogen peroxide, TBHP, as the oxidant with several doped mixed-valent and regular manganese oxide catalysts in water) at room and higher temperatures. These catalysts belong to a class of porous manganese oxides known as octahedral molecular sieves (OMS). The most active catalysts were those of Mo(6+)- and V(5+)-doped OMS. Rates of reaction were found to be first-order with respect to the dye. TBHP has been found to enhance the MB decomposition, whereas H(2)O(2) does not. Reactions were studied at pH 3-11. The optimum pH for these reactions was pH 3. Dye-decomposing activity was proportional to the amount of catalyst used, and a significant increase in catalytic activity was observed with increasing temperature. X-ray diffraction (XRD), energy dispersive spectroscopy (EDX), and thermogravimetric analysis (TGA) studies showed that no changes in the catalyst structure occurred after the dye-degradation reaction. The products as analyzed by electrospray ionization mass spectrometry (ESI-MS) showed that MB was successively decomposed through different intermediate species.

摘要

采用绿色氧化法(叔丁基过氧化氢(TBHP)作为氧化剂,几种掺杂的混合价和常规氧化锰催化剂在水中)在室温及更高温度下研究了有机染料(亚甲基蓝,MB)的催化降解。这些催化剂属于一类称为八面体分子筛(OMS)的多孔锰氧化物。最活跃的催化剂是 Mo(6+)和 V(5+)掺杂的 OMS。反应速率与染料呈一级关系。发现 TBHP 增强了 MB 的分解,而 H(2)O(2)则没有。在 pH 3-11 下研究了反应。这些反应的最佳 pH 值为 pH 3。染料分解活性与所用催化剂的量成正比,并且随着温度的升高,观察到催化活性显著增加。X 射线衍射(XRD)、能谱(EDX)和热重分析(TGA)研究表明,在染料降解反应后,催化剂结构没有发生变化。通过电喷雾电离质谱(ESI-MS)分析的产物表明,MB 通过不同的中间物种依次分解。

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