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Understanding the electrochemical oxidation of dyes on platinum and boron–doped diamond electrode surfaces: experimental and computational study
Journal of Solid State Electrochemistry ( IF 2.5 ) Pub Date : 2020-09-07 , DOI: 10.1007/s10008-020-04813-w
Izabelle Cristina da Costa Soares , Ámison Rick Lopes da Silva , Elaine Cristina Martins de Moura Santos , Elisama Vieira dos Santos , Djalma Ribeiro da Silva , Carlos A. Martínez-Huitle

Anodic oxidation (AO) approach proceeds via direct and indirect electrochemical pathways and their subsequent reactions. The interest to elucidate the mechanisms for removing dyes from water contributes to the understanding of more complex reactions involving organic pollutants towards anode surfaces. The present study was motivated by the reports that promote the use of AO for removing different organic compounds but no considerations about the influence of different functional groups in their structure have been discussed. Therefore, we have evaluated the influence of different functional groups in the dye structure (Reactive Orange 16, Reactive Violet 4, Reactive Red 228, and Reactive Black 5) by potentiodynamic measurements and by computational analyzes using density functional theory (DFT). The computational studies have allowed to carry out morphological studies on the frontier orbitals where the electrons are more energetic and then, the electron-transfer to electrode surface is achieved, which was associated to the electrochemical measurements (current-potential profiles). Also, the theoretical studies were used to understand the bulk electrolysis, in terms of mineralization. The results clearly demonstrate that organic molecules can be degraded in different way and level due to the oxidants electrochemically generated as well as the interaction of dyes with anode surface by adsorbed/non-adsorbed intermediates. Conversely, the decolorization mechanisms, which are related to the fragmentation of chromophore group, are associated to the direct AO approach, favoring different order of elimination, as already reported in our previous work. The results were discussed in light of the existing literature.



中文翻译:

了解染料在铂和硼掺杂的金刚石电极表面上的电化学氧化:实验和计算研究

阳极氧化(AO)方法通过直接和间接电化学途径及其后续反应进行。阐明从水中去除染料的机理的兴趣有助于理解涉及阳极污染物的有机污染物的更复杂的反应。本研究是受到促进使用AO去除不同有机化合物的报道的推动,但尚未讨论不同官能团对其结构的影响。因此,我们通过电位动力学测量和使用密度泛函理论(DFT)的计算分析,评估了染料结构中不同官能团(活性橙16,活性紫4,活性红228和活性黑5)的影响。通过计算研究,可以对前沿轨道进行形态学研究,在前沿轨道中,电子的能量更高,然后实现了电子向电极表面的转移,这与电化学测量(电流势分布)相关。同样,理论研究被用来理解矿化方面的本体电解。结果清楚地表明,由于电化学生成的氧化剂以及染料通过吸附/未吸附中间体与阳极表面的相互作用,有机分子可以以不同的方式和水平降解。相反,与发色团断裂相关的脱色机制与直接AO方法相关,有利于不同的消除顺序,正如我们先前工作中已经报道的那样。根据现有文献讨论了结果。

更新日期:2020-09-08
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