Ti_nO_(2n-1)电极电催化氧化有机污水中二甲基苯酚的探究
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摘要
从Ti_nO_(2n-1)电极的制备入手,以Ti H2与Ti O2为合成原料,采用高温压片-真空烧结法制得Ti_nO_(2n-1)多孔电极。通过SEM、XRD技术对电极进行了表征,随后利用电化学测试方法考察了Ti_nO_(2n-1)电极的性能,并设计了有机污染物处理试验考察了电极的电催化氧化效能。结果显示:自制得到了主相为Ti4O7的Ti_nO_(2n-1)多孔电极,将自制的Ti_nO_(2n-1)多孔电极与石墨电极分别进行电化学测试,Ti_nO_(2n-1)电极的析氧电位保持在2.25 V左右,石墨电极仅为1.60 V、电化学稳定性等指标均优于石墨电极。在二甲基苯酚(DPM)模拟污水的电催化氧化过程中,Ti_nO_(2n-1)电极在105 min内对DPM的消解率达到93.1%,对COD的去除率达到84%,反应过程符合一级动力学过程。
In this paper,starting from the preparation of Ti_nO_(2n-1) electrode,using Ti H2 and TiO_2 as synthetic raw materials,Ti_nO_(2n-1) electrode was prepared by the high-temperature compression-vacuum sintering method. The characterization of the material was carried out by SEM and XRD techniques,and the performance of the Ti_nO_(2n-1) electrode was investigated using an electrochemical test method. Moreover,an organic pollutant treatment experiment was designed to investigate the electrocatalytic oxidation performance of the electrode. Results showed that the homemade porous Ti_nO_(2n-1) electrode possessed the main phase of Ti4 O7. The as-prepared Ti_nO_(2n-1) porous electrode and the graphite electrode were tested by electrochemical methods. The oxygen evolution potential of the Ti_nO_(2n-1) electrode was maintained at about 2.25 V,while that of graphite electrode was only at 1.60 V,revealing that the catalytic activity,electrochemical stability,and electrochemical window of the Ti_nO_(2n-1) electrode were superior to those of the graphite electrode. Furthermore,in the process of electrocatalytic oxidation of organic pollutants,the dissolution efficiency of dimethylphenol( DPM) reached 93.1% within 105 min and the removal efficiency of COD reached 84%. The reaction process conformed to the first-order kinetics process.
In this paper,starting from the preparation of Ti_nO_(2n-1) electrode,using Ti H2 and TiO_2 as synthetic raw materials,Ti_nO_(2n-1) electrode was prepared by the high-temperature compression-vacuum sintering method. The characterization of the material was carried out by SEM and XRD techniques,and the performance of the Ti_nO_(2n-1) electrode was investigated using an electrochemical test method. Moreover,an organic pollutant treatment experiment was designed to investigate the electrocatalytic oxidation performance of the electrode. Results showed that the homemade porous Ti_nO_(2n-1) electrode possessed the main phase of Ti4 O7. The as-prepared Ti_nO_(2n-1) porous electrode and the graphite electrode were tested by electrochemical methods. The oxygen evolution potential of the Ti_nO_(2n-1) electrode was maintained at about 2.25 V,while that of graphite electrode was only at 1.60 V,revealing that the catalytic activity,electrochemical stability,and electrochemical window of the Ti_nO_(2n-1) electrode were superior to those of the graphite electrode. Furthermore,in the process of electrocatalytic oxidation of organic pollutants,the dissolution efficiency of dimethylphenol( DPM) reached 93.1% within 105 min and the removal efficiency of COD reached 84%. The reaction process conformed to the first-order kinetics process.
引文
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[2]钱易.水体颗粒物和难降解有机物的特性与控制技术原理.下卷:难降解有机物[M].北京:中国环境科学出版社,2000:45-60.
[3]肖宏康,肖书虎,张国芳,等.电化学氧化法处理模拟黄连素制药废水的研究[J].环境工程学报,2011,5(1):987-991.
[4]MAIKE R,TEIXEIRA M A,CARNEIRO A E,et al.Performance of constructed wetlands in the treatment of aerated coffee processing wastewater:Removal of nutrients and phenoliccompounds[J].Ecol Eng,2012,49:264-269.
[5]POLCARO A M,PALMAS S,RENOLDI F,et al.On the performance of Ti/Sn O2and Ti/PbO2anodesin electrochemical degradation of 2-chlorophenolfor wastewater treatment[J].Journal of Applied Electrochemistry,1999,29(2):147-151.
[6]WANG G,LIU Y,YE J,et al.Fabrication of Rod-like Ti4O7with High Conductivity by Molten Salt Synthesis[J].Materials Letters,2017,186:361-363.
[7]WALSH F C,WILLS R G A.The continuing development of Magnéli phase titanium sub-oxides and Ebonex electrodes[J].Electrochimica Acta,2010,55(22):6 342-6 351.
[8]李联,何平,李洪,等.Ti5O9-Ti4O7电极电化学处理2,4,6-三硝基苯酚废水[J].化工环保,2015,35(4):420-425.
[9]应杭君,田华军,孟阵,等.TinO2n-1系列氧化物的特性、制备方法及应用[J].化学进展,2015,27(4):361-372.
[10]DJADJEV I.How to comply with MARPOL 73/78:A commentary on the IMO’s pollution-prevention instrument and the implications for the shipping industry[J].Koelner Zeitschrift Fuer Soziologie Und Sozialpsychologie,2015,63(1):424-446.
[11]唐超.Magneli相低价钛氧化物的制备及其作为析氧材料的应用研究[J].化学教育,2011(3):65-66.
[12]任一鸣,唐定兴,丁纯梅,等.浅谈应用Woodward-Fieser规则的常见错误[M].长沙:中南大学,2013:40-63.
[13]ZAKY A M,CHAPLIN B P.Porous Substoichiometric Ti O2Anodes as Reactive Electrochemical Membranes for Water Treatment[J].Environmental Science&Technology,2013,47(12):6 554-6 563.