应用于水溶液介质中喹啉氧化的电芬顿工艺实验设计方法(英文)

采用碳毡阴极和铂阳极的电芬顿工艺研究了喹啉模型分子8-羟基喹啉硫酸盐（8-HQS）在水溶液介质中的降解行为. 由于电化学诱导芬顿药剂（H2O2，Fe2+）产生大量的羟基活性基（OH），成为与有机物发生反应直到有机物完全矿化的强有力氧化剂，因此，电芬顿工艺具有很强的氧化能力. 采用正交实验设计确定了水溶液介质中8-HQS降解的操作参数. 结果表明，电流密度和8-HQS的初始浓度是影响降解速度的主要因素. 8-HQS浓度随着电解时间而减少，说明8-HQS的氧化遵循准一级反应动力学. 通过竞争动力学方法确定的由OH引起8-HQS氧化的绝对反应速度常数为1.62×109 mol^-1·L·s^-1. 通过Doehlert 矩阵研究了8-HQS矿化的最佳实验参数，由此确定最佳条件下电芬顿工艺能导致8-HQS在水溶液中的准完全矿化（总有机成分去除率95%）. 对8-HQS水溶液的处理，使得8-HQS矿化前的最终产物为短链羧酸. 同时研究了电芬顿处理中短链羧酸的演变行为. 溶液毒性演变的跟踪研究发现，中间产物的毒性比8-HQS强，但溶液的毒性在中间产物矿化后可以完全消除.

Experimental Design Methodology Applied to the Oxidation of Quinolines in Aqueous Medium by Electro-Fenton Process

The degradation behavior of 8-hydroxyquinoleine sulfate (8-HQS), a model molecule of quinolines, was studied in an aqueous medium by electro-Fenton process using a carbon felt cathode and a platinum anode. The great oxidation ability of this process is due to a large production of hydroxyl radical (OH) by electrochemically induced Fenton’s reagent (H2O2, Fe2+). Hydroxyl radicals are very powerful oxidizing agents which react on organics up to complete mineralization. A factorial experimental design was used for determining the operating parameters on the degradation of 8-HQS in an aqueous medium. The results showed that the current intensity and the initial concentration of 8-HQS were the main factors that influenced the degradation rate. The decay in concentration of 8-HQS with the electrolysis time shows that the oxidation of 8-HQS follows pseudo-first order kinetics. The absolute rate constant for the oxidation of 8-HQS by OH was determined by using competition kinetics method and found to be 1.62×109 mol^-1·L·s^-1. The optimal experimental parameters for the mineralization of 8-HQS have also been investigated by the use of Doehlert matrix. It has been demonstrated that under the optimal conditions determined by this method, electro-Fenton process can lead to a quasi-complete mineralization (95% of TOC removal) of 8-HQS aqueous solution. The treatment of 8-HQS aqueous solutions leads to the formation of short-chain carboxylic acids as end-products before mineralization. Their evolution during electro-Fenton treatment was studied. The follow-up of the solution toxicity evolution shows the formation of intermediates more toxic than 8-HQS. However, the solution toxicity was totally removed after mineralization of these intermediates.