【摘要】 为进一步提高氯介导的电化学高级氧化（Cl-EAO）脱氨效率,本研究制备了一种新型TiO₂纳米线负载RuO₂阳极（TiO₂NBs-RuO₂）,在考察其材料及电化学性质的基础上,探讨了不同条件对该阳极氨氧化性能的影响,并结合电子顺磁共振（EPR）和自由基淬灭实验对氨氧化机理进行了探究.材料表征结果表明,RuO₂均匀的负载在了TiO₂纳米线的表面,形成了疏松多孔的稳定结构,纳米线直径在100nm以内.电化学表征结果表明,TiO₂NBs-RuO₂阳极能够抑制析氧反应从而提高析氯反应电流效率.TiO₂NBs-RuO₂阳极的氨氧化过程符合零级反应动力学特征,50min内氨氮去除效率可达99.6%以上,显著高于未改性的Ti-RuO₂阳极及TiO₂-RuO₂阳极,并且其氨氧化性能会随着初始氨氮浓度、初始氯浓度、初始pH值以及电流密度的增加而增加.机理探究结果表明ClO·在氨氮降解过程中发挥了最主要作用.此外,研究对比了最常见的商用Ti-RuO₂阳极,发现TiO₂NBs-RuO₂阳极较商用阳极氨氧化效率提高29.7%,且能耗比和硝态氮产率更低.更多还原

【Abstract】 In order to further improve the ammonia removal efficiency of the chlorine-mediated electrochemical advanced oxidation（Cl-EAO） technology, a new TiO₂ nanobelts loaded RuO₂ anode（TiO₂ NBs-RuO₂） was prepared in this study. Based on the investigation of its material and electrochemical properties, the ammonia oxidation performance of the anode was explored under different conditions, and the ammonia oxidation mechanism was explored by combining electron paramagnetic resonance（EPR） and free radical inhibition assays. The material characterization results indicated that RuO₂ was loaded on the surface of TiO₂ nanobelts uniformly, which formed a porous and stable structure, and the nanobelts diameter was within 100nm. The electrochemical characterization results indicated that TiO₂ NBs-RuO₂ anode has inhibited the oxygen evolution reaction and improved the current efficiency of the chlorine evolution reaction. The ammonia oxidation process of TiO₂ NBs-RuO₂ anode followed zero order reaction kinetics, and the ammonia nitrogen removal efficiency reached over 99.6% within 50min, which was significantly higher than unmodified Ti-RuO₂ anode and TiO₂-RuO₂ anode. Moreover, its ammonia oxidation rate increased with the increase of initial ammonia nitrogen concentration, initial chlorine concentration, initial pH, and current density. It was found that the ClO· played the most important role in the ammonia oxidation process. In addition, this study compared the TiO₂ NBs-RuO₂ anode and the most common commercial Ti-RuO₂ anode and found that the ammonia oxidation rate of TiO₂ NBs-RuO₂ anode was 29.7% higher than the commercial anode, and the energy consumption ratio and nitrate nitrogen yield of TiO₂ NBs-RuO₂ anode were also lower than the commercial one.更多还原