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在层柱蒙脱石负载的钴基催化剂存在下用 Oxone®降解食用柠檬黄-即使在极端条件下也很有效的技术。

Degradation of tartrazine by Oxone® in the presence of cobalt based catalyst supported on pillared montmorillonite - Efficient technology even in extreme conditions.

机构信息

University of Belgrade-Institute of Chemistry, Technology and Metallurgy, Njegoševa 12, Belgrade, Serbia.

University of Belgrade-Faculty of Physics, Studentski Trg 12, Belgrade, Serbia.

出版信息

Environ Pollut. 2023 Aug 15;331(Pt 1):121863. doi: 10.1016/j.envpol.2023.121863. Epub 2023 May 22.

DOI:10.1016/j.envpol.2023.121863
PMID:37225074
Abstract

The catalytic degradation of hazardous organic contaminants in industrial wastewater is a promising technology. Reactions of tartrazine, the synthetic yellow azo dye, with Oxone® in the presence of catalyst in strong acidic condition (pH 2), were detected by using UV-Vis spectroscopy. In order to extend the applicability profile of Co-supported Al-pillared montmorillonite catalyst an investigation of Oxone® induced reactions were performed in extreme acidic environment. The products of the reactions were identified by liquid chromatography-mass spectrometry (LC-MS). Along with the catalytic decomposition of tartrazine induced by radical attack (confirmed as unique reaction path under neutral and alkaline conditions), the formation of tartrazine derivatives by reaction of nucleophilic addition was also detected. The presence of derivatives under acidic conditions slowed down the hydrolysis of tartrazine diazo bond in comparison to the reactions in neutral environment. Nevertheless, the reaction in acidic conditions (pH 2) is faster than the one conducted in alkaline conditions (pH 11). Theoretical calculations were used to complete and clarify the mechanisms of tartrazine derivatization and degradation, as well as to predict the UV-Vis spectra of compounds which could serve as predictors of certain reaction phases. ECOSAR program, used to estimate toxicological profile of compounds to aquatic animals, indicated an increase in the harmfulness of the compounds identified by LC-MS as degradation products from the reaction conducted for 240min. It could be concluded that an intensification of the process parameters (higher concentration of Oxone®, higher catalyst loading, increased reaction time, etc.) is needed in order to obtain only biodegradable products.

摘要

工业废水中有害有机污染物的催化降解是一种很有前途的技术。在酸性条件(pH 2)下,使用紫外-可见光谱法检测到了合成黄色偶氮染料酒石黄在催化剂存在下与 Oxone®的反应。为了扩展 Co 负载的 Al 柱撑蒙脱石催化剂的适用性,在极端酸性环境下进行了 Oxone®诱导反应的研究。通过液相色谱-质谱联用(LC-MS)鉴定了反应产物。除了由自由基攻击引起的酒石黄的催化分解(在中性和碱性条件下被确认为唯一的反应途径)之外,还检测到亲核加成反应形成的酒石黄衍生物。在酸性条件下存在衍生物会使酒石黄重氮键的水解速度减慢,与中性环境下的反应相比。然而,在酸性条件(pH 2)下的反应比在碱性条件(pH 11)下的反应更快。理论计算用于完成和澄清酒石黄衍生化和降解的机制,并预测可作为某些反应阶段预测指标的化合物的紫外-可见光谱。ECOSAR 程序用于估计化合物对水生动物的毒理学特征,表明通过 LC-MS 鉴定为反应产物的化合物的危害性增加了,这些化合物是在 240min 的反应中产生的。可以得出结论,需要强化工艺参数(增加 Oxone®的浓度、增加催化剂的负载量、增加反应时间等),以获得仅可生物降解的产物。

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