Department of Chemistry and Earth Sciences, College of Arts and Sciences, Qatar University, Doha, Qatar.
Department of Chemistry, Faculty of Sciences of Gabes, University of Gabes, 6072, Zrig, Gabes, Tunisia.
J Environ Sci (China). 2016 Jul;45:115-23. doi: 10.1016/j.jes.2015.10.015. Epub 2016 Jan 4.
In this work, the contribution of mediated oxidation mechanisms in the electrolytic degradation of cyanuric acid using boron-doped diamond (BDD) anodes was investigated in different electrolytes. A complete mineralization of cyanuric acid was obtained in NaCl; however lower degrees of mineralization of 70% and 40% were obtained in Na2SO4 and NaClO4, respectively. This can be explained by the nature of the oxidants electrogenerated in each electrolyte. It is clear that the contribution of active chlorine (Cl2, HClO, ClO(-)) electrogenerated from oxidation of chlorides on BDD is much more important in the electrolytic degradation of cyanuric acid than the persulfate and hydroxyl radicals produced by electro-oxidation of sulfate and water on BDD anodes. This could be explained by the high affinity of active chlorine towards nitrogen compounds. No organic intermediates were detected during the electrolytic degradation of cyanuric acid in any the electrolytes, which can be explained by their immediate depletion by hydroxyl radicals produced on the BDD surface. Nitrates and ammonium were the final products of electrolytic degradation of cyanuric acid on BDD anodes in all electrolytes. In addition, small amounts of chloramines were formed in the chloride medium. Low current density (≤10mA/cm(2)) and neutral medium (pH in the range 6-9) should be used for high efficiency electrolytic degradation and negligible formation of hazardous chlorate and perchlorate.
在这项工作中,研究了在不同电解质中,介体氧化机制在使用掺硼金刚石(BDD)阳极电解降解三聚氰胺中的贡献。在 NaCl 中可以完全矿化三聚氰胺;然而,在 Na2SO4 和 NaClO4 中,矿化度分别为 70%和 40%。这可以通过在每种电解质中电生成的氧化剂的性质来解释。很明显,从 BDD 上氯化物氧化产生的活性氯(Cl2、HClO、ClO(-))比 BDD 阳极上硫酸盐和水的电氧化产生的过硫酸盐和羟基自由基对三聚氰胺的电解降解贡献更大。这可以解释为活性氯对含氮化合物的高亲和力。在任何电解质中,在三聚氰胺的电解降解过程中都没有检测到有机中间体,这可以解释为它们立即被 BDD 表面产生的羟基自由基消耗。硝酸盐和铵盐是所有电解质中 BDD 阳极上三聚氰胺电解降解的最终产物。此外,在氯化物介质中形成了少量的氯胺。在高效率电解降解和可忽略不计的亚氯酸盐和高氯酸盐形成的情况下,应使用低电流密度(≤10mA/cm(2))和中性介质(pH 值在 6-9 范围内)。