4.7 Article

Influence of the surface hydroxyl groups of MnOx/SBA-15 on heterogeneous catalytic ozonation of oxalic acid

期刊

CHEMICAL ENGINEERING JOURNAL
卷 242, 期 -, 页码 348-356

出版社

ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2013.12.097

关键词

MnOx/SBA-15; Catalytic ozonation; Surface hydroxyl groups; Oxalic acid; Reaction mechanism

资金

  1. National High-Tech Research and Development Program [2013AA06A305]
  2. National Natural Science Foundation of China [20977036, 21247004]
  3. Science & Technology Office of Guangdong Province [2010B030900006]

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Comparative ozonation experiments were carried out to investigate the catalytic ability and mechanism of SBA-15 supported manganese oxide (MnOx/SBA-15) for the degradation of oxalic acid (OA) in aqueous solution. The results showed that MnOx/SBA-15 possessed good catalytic capacity for the ozonation of OA. The influences of tert-butanol and phosphate on OA removal and ozone equilibrium concentration in aqueous solution demonstrated that initiation of hydroxyl radicals ((OH)-O-center dot) was involved and surface reaction played the major role in O-3/MnOx/SBA-15. The effects of manganese content and initial solution pH verified that surface hydroxyl groups affected by the pH of solution and the point of zero charge (pH(PZC)) of catalysts, were closely related to OA adsorption and (OH)-O-center dot initiation on the surface of MnOx/SBA-15. The pre-ozonated catalyst improved its catalytic activity a little due to the enhancement of electron transfer in the presence of higher multivalent MnOx (Mn(III)/Mn(IV)). It was concluded that the protonated surface hydroxyl groups were the main reaction sites and a possible catalytic ozonation mechanism of OA over MnOx/SBA-15 was proposed. (C) 2014 Elsevier B.V. All rights reserved.

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