The role of Mn-doping for catalytic ozonation of phenol using Mn/γ-Al2O3 nanocatalyst: Performance and mechanism

催化作用 化学 苯酚 激进的 水溶液 无机化学 羟基自由基 X射线光电子能谱 氧气 零电荷点 化学工程 光化学 有机化学 工程类
作者
Ye Wang,Wenzhong Yang,Xiaoshuang Yin,Ying Liu
出处
期刊:Journal of environmental chemical engineering [Elsevier BV]
卷期号:4 (3): 3415-3425 被引量:95
标识
DOI:10.1016/j.jece.2016.07.016
摘要

Abstract Comparative ozonation experiments were carried out to investigate the catalytic ability and mechanism of γ-Al2O3 supported manganese oxide (Mn/γ-Al2O3) for the degradation of phenol in aqueous solution. The results showed that 4% Mn/γ-Al2O3 possessed highest catalytic efficiency for the ozonation of phenol than that of other catalysts. The influences of manganese content and catalyst dosage verified that surface hydroxyl groups affected by the solution pH and the point of zero charge (pHPZC) of catalysts. The Mn/γ-Al2O3 exerted the strongest catalytic activity at initial solution pH of 3.45. The strong interaction between ozone and Mn/γ-Al2O3 was observed and confirmed as a critical step for the catalysis reaction. The surface hydroxyl groups and chemisorbed water acted as the active sites in promoting hydroxyl radicals, while Bronsted acid sites were confirmed as reactive centres for catalytic ozonation in the aqueous phase. The influence of tert-butanol showed that hydroxyl radicals and active oxygen species were involved in the catalytic ozonation of phenol. According to the X-ray photoelectron spectroscopy (XPS) results, the enhancement of electron transfer on the surface manganese oxides were responsible for the catalysis and promoting the formation of active oxygen species. A possible catalytic ozonation mechanism of phenol over Mn/γ-Al2O3 was proposed.
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