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A novel approach in revealing mechanisms and particular step predictors of pH dependent tartrazine catalytic degradation in presence of Oxone®
Chemosphere ( IF 8.8 ) Pub Date : 2021-05-05 , DOI: 10.1016/j.chemosphere.2021.130806
Marko G Popadić 1 , Sanja R Marinović 2 , Tihana M Mudrinić 2 , Aleksandra D Milutinović-Nikolić 2 , Predrag T Banković 2 , Ivana S Đorđević 2 , Goran V Janjić 2
Affiliation  

The degradation of tartrazine in the presence of cobalt activated Oxone® (potassium peroxymonosulfate) was investigated at different initial pH values. Aluminum pillared clay had the role of a support for catalytically active cobalt oxide species. The degradation of tartrazine and the formation of a mixture of degradation products were monitored using the Ultraviolet–Visible (UV–Vis) spectroscopy and gas chromatography–mass spectrometry (GC-MS). The exact qualitative composition of this mixture and the determination of the most probable mechanism of degradation (the primary goal) were obtained using GC-MS. Besides, the main reaction pathway (reaction with SO4˙ˉ radical anion) and secondary pathways were proposed depending on the pH value. At pH = 6 the reaction with HO˙ radical was proposed. At pH = 11 decarboxilation was suggested as the first step of the secondary proposed reaction pathway. The combination of results acquired from the deconvolution of UV–Vis spectra and the theoretical UV–Vis spectra of degradation products, whose occurrence was predicted by quantum-chemical calculations, was proven to be beneficial for the identification of tartrazine degradation products and for defining UV–Vis predictors of particular degradation steps. An additional contribution of this paper, from the reactivity aspect, was the establishment of the critical structural demand for the radical degradation of any diazo compound. The existence of a hydrogen atom bound to a diazo group was found to be the essential prerequisite for the radical cleavage of diazo compounds.



中文翻译:

在存在Oxone®的情况下揭示pH依赖的酒石黄催化降解的机理和特定步骤预测因子的新方法

在不同的初始pH值下,研究了钴活化Oxone®(过氧一硫酸钾)存在下酒石黄的降解情况。铝柱状粘土具有催化活性氧化钴物质的支撑作用。使用紫外-可见(UV-Vis)光谱和气相色谱-质谱(GC-MS)监测酒石黄的降解和降解产物混合物的形成。使用GC-MS获得了该混合物的确切定性组成,并确定了最可能的降解机理(主要目标)。此外,主要反应途径(与SO 4反应˙ˉ自由基阴离子)和次级途径被提出,具体取决于pH值。建议在pH = 6时与HO +自由基反应。在pH = 11时,建议将去羧化作为第二步建议的反应途径的第一步。从UV-Vis光谱的去卷积和降解产物的理论UV-Vis光谱获得的结果相结合,其发生是通过量子化学计算预测的,被证明对鉴定酒石黄降解产物和定义UV很有帮助。 –查看特定降解步骤的预测因子。从反应性的角度来看,本文的另一项贡献是确立了对任何重氮化合物进行自由基降解的关键结构要求。

更新日期:2021-05-15
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