TiO_(2)纳米线负载RuO_(2)阳极制备及其氨氧化性能  

Preparation of TiO2 nanobelts loaded RuO2 anode and the research of its ammonia oxidation performance

作　　者：刘国华[1] 李乾岗 张彤彤 杜洪彪 仙光 曾凡刚[1,2] 齐鲁[1] LIU Guo-hua;LI Qian-gang;ZHANG Tong-tong;DU Hong-biao;XIAN Guang;ZENG Fan-gang;QI Lu(Research Center for Carbon Technology of Water Environment,School of Chemistry and Life Resource,Renmin University of China,Beijing 100872,China;School of Ecology&Environment,Renmin University of China,Beijing 100872,China;Army Logistics Academy,Chongqing 401331,China)

机构地区：[1]中国人民大学,化学与生命资源学院低碳水环境技术研究中心,北京100872 [2]中国人民大学生态环境学院,北京100872 [3]陆军勤务学院勤务指挥系,重庆401331

出　　处：《中国环境科学》2024年第11期6181-6193,共13页China Environmental Science

基　　金：中国人民大学2022年度拔尖创新人才培育资助计划成果;重庆市教委科学技术研究项目(KJQN202212902)。

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TiO_(2)纳米线负载RuO_(2)阳极(TiO_(2)NBs-RuO_(2)),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,RuO_(2)均匀的负载在了TiO_(2)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,TiO_(2)NBs-RuO_(2)阳极能够抑制析氧反应从而提高析氯反应电流效率.TiO_(2)NBs-RuO_(2)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-RuO_(2)阳极及TiO_(2)-RuO_(2)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-RuO_(2)阳极,发现TiO_(2)NBs-RuO_(2)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.In order to further improve the ammonia removal efficiency of the chlorine-mediated electrochemical advanced oxidation(Cl-EAO)technology,a new TiO_(2)nanobelts loaded RuO_(2)anode(TiO_(2)NBs-RuO_(2))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 RuO_(2)was loaded on the surface of TiO_(2)nanobelts uniformly,which formed a porous and stable structure,and the nanobelts diameter was within 100nm.The electrochemical characterization results indicated that TiO_(2)NBs-RuO_(2)anode has inhibited the oxygen evolution reaction and improved the current efficiency of the chlorine evolution reaction.The ammonia oxidation process of TiO_(2)NBs-RuO_(2)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-RuO_(2)anode and TiO_(2)-RuO_(2)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 TiO_(2)NBs-RuO_(2)anode and the most common commercial Ti-RuO_(2)anode and found that the ammonia oxidation rate of TiO_(2)NBs-RuO_(2)anode was 29.7%higher than the commercial anode,and the energy consumption ratio and nitrate nitrogen yield of TiO_(2)NBs-RuO_(2)anode were also lower than the commercial one.

关 键 词：氨氮 活性氯 氯自由基 二氧化钛 电化学高级氧化 

分 类 号：X703.1[环境科学与工程—环境工程]