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Catalytic ozonation of an azo-dye using a natural aluminosilicate
Catalysis Today ( IF 5.3 ) Pub Date : 2019-12-16 , DOI: 10.1016/j.cattod.2019.12.019
N. Inchaurrondo , C. di Luca , G. Žerjav , J.M. Grau , A. Pintar , P. Haure

Catalytic ozonation of Orange II (100 mg/L) was studied using aluminosilicate Montanit300® (M) modified with H2SO4 (MS) and HCl (MH). Characterization of these samples was performed through several techniques: SEM/EDX, FTIR, XRD, FRX, TPD pyridine, surface area, pHPZC. Acid treatment increased surface area, Si:Al ratio and quantity of acid sites, but reduced pHPZC and Fe and Mn content.

Ozonation experiments achieved complete decoloration and remarkable TOC conversions of 66, 65, 88 and 91 % by single ozonation and catalytic ozonation with MH, MS and M, respectively. Higher M and MS activity under acidic pH was attributed to Mn leaching. Decreased mineralization efficiency in the presence of tert-butanol suggested a radical mechanism. At neutral pH, M showed no activity, while MS presented mild activity owing to its enlarged hydrophobicity.

The M sample sustained mineralization levels over 20 h. Lower O3 dose caused quick MS deactivation. However, it was reversed through calcination and prevented with a higher oxidant dose.

Mn is naturally found in Montanit300®, thus making it an inexpensive catalyst. The development of a dynamic cycle combining reduced and oxidized forms of Mn was key to the outstanding activity observed.



中文翻译:

使用天然铝硅酸盐催化偶氮染料的臭氧氧化

使用经H 2 SO 4(MS)和HCl(MH)改性的铝硅酸盐Montanit300®(M),研究了Orange II(100 mg / L)的催化臭氧化作用。这些样品的表征通过几种技术进行:SEM / EDX,FTIR,XRD,FRX,TPD吡啶,表面积,pH PZC。酸处理增加了表面积,Si:Al比和酸位的数量,但降低了pH PZC以及Fe和Mn的含量。

臭氧化实验通过分别用MH,MS和M进行一次臭氧化和催化臭氧化分别实现了完全脱色和66%,65%,88%和91%的显着TOC转化率。酸性pH下较高的M和MS活性归因于Mn的浸出。在叔丁醇存在下矿化效率降低表明存在根本机理。在中性pH值下,M无活性,而MS由于疏水性增强,具有中等活性。

M样品在20小时内持续矿化水平。较低的O 3剂量会导致MS快速失活。然而,通过煅烧可以逆转,并通过较高的氧化剂剂量来防止。

Mn天然存在于Montanit300®中,因此使其成为廉价的催化剂。结合还原形式和氧化形式的Mn形成的动态循环是观察到的出色活性的关键。

更新日期:2019-12-16
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