Advanced Water Management Centre, The University of Queensland, St Lucia, QLD 4072, Australia.
Water Res. 2012 Nov 15;46(18):6104-12. doi: 10.1016/j.watres.2012.08.038. Epub 2012 Sep 6.
Electrochemical processes have been widely investigated for degrading organic contaminants present in wastewater. This study evaluated the performance of electrochemical oxidation using boron-doped diamond (BDD) electrodes by forming OH() for the treatment of reverse osmosis concentrate (ROC) from secondary-treated wastewater effluents. Since oxidation by OH() and active chlorine species (HClO/ClO(-)) is influenced by pH, the electrochemical oxidation of ROC was evaluated at controlled pH 6-7 and at pH 1-2 (no pH adjustment). A high concentration of chloride ions in the ROC enhanced the oxidation, and 7-11% of Coulombic efficiency for chemical oxygen demand (COD) removal was achieved with 5.2 Ah L(-1) of specific electrical charge. Complete COD removal was observed after 5.2 and 6.6 Ah L(-1), yet the corresponding dissolved organic carbon (DOC) removal was only 48% (at acidic pH) and 59% (at circumneutral pH). Although a higher operating pH seemed to enhance the participation of OH() in oxidation mechanisms, high concentrations of chloride resulted in the formation of significant concentrations of adsorbable organic chlorine (AOCl) after electrochemical oxidation at both pH. While adsorbable organic bromine (AOBr) was degraded at a higher applied electrical charge, a continuous increase in AOCl concentration (up to 0.88 mM) was observed until the end of the experiments (i.e. 10.9 Ah L(-1)). In addition, total trihalomethanes (tTHMs) and total haloacetic acids (tHAAs) were further degraded with an increase in electrical charge under both pH conditions, to final total concentrations of 1 and 4 μM (tTHMs), and 12 and 22 μM (tHAAs), at acidic and circumneutral pH, respectively. In particular, tHAAs were still an order of magnitude above their initial concentration in ROC after further electrooxidation. Where high chloride concentrations are present, it was found to be necessary to separate chloride from ROC prior to electrochemical oxidation in order to avoid the formation of chlorinated by-products.
电化学过程已被广泛研究用于降解废水中存在的有机污染物。本研究评估了使用掺硼金刚石(BDD)电极形成 OH()进行电化学氧化的性能,以处理来自二级处理废水出水的反渗透浓缩物(ROC)。由于 OH()和活性氯物种(HClO/ClO(-))的氧化受 pH 影响,因此在控制 pH 6-7 和 pH 1-2(不进行 pH 调节)下评估了 ROC 的电化学氧化。ROC 中高浓度的氯离子增强了氧化作用,在 5.2 Ah L(-1)的特定电荷下,化学需氧量(COD)去除的库仑效率达到了 7-11%。在 5.2 和 6.6 Ah L(-1)时观察到完全去除 COD,但相应的溶解有机碳(DOC)去除率仅为 48%(在酸性 pH 下)和 59%(在近中性 pH 下)。尽管较高的操作 pH 似乎增强了 OH()在氧化机制中的参与,但在两种 pH 下进行电化学氧化后,高浓度的氯离子导致可吸附有机氯(AOCl)的形成浓度显著增加。虽然在较高的施加电荷下可降解吸附性有机溴(AOBr),但在实验结束时观察到 AOCl 浓度持续增加(最高达 0.88 mM)(即 10.9 Ah L(-1))。此外,在两种 pH 条件下,随着电荷的增加,总三卤甲烷(tTHMs)和总卤乙酸(tHAAs)进一步降解,最终总浓度分别为 1 和 4 μM(tTHMs)以及 12 和 22 μM(tHAAs),在酸性和近中性 pH 下。特别是,在进一步电氧化后,tHAAs 的浓度仍然比 ROC 中的初始浓度高出一个数量级。在存在高浓度氯离子的情况下,发现有必要在电化学氧化之前将氯离子从 ROC 中分离出来,以避免形成氯化副产物。