改性钯阴极电-芬顿法降解菲那西汀模拟废水
Degradation of phenacetin wastewater by E-Fenton from modified palladium cathode
张永刚,黄耀霈,刘莹
摘要(Abstract):
为提高对菲那西汀制药废水的处理效果,采用钛盐光度法、电子顺磁共振法(ESR)和重铬酸钾滴定法等方法对不同电极在电-芬顿法中H_2O_2产量、·OH生成量和化学需氧量(COD)的影响,并且考察降解菲那西汀的最佳反应条件。结果表明:在电流密度=2.5 mA/cm~2、[Fe~(2+)]=0.10 mmol/L、pH值=3和[Na_2SO_4]=0.1 mol/L的操作条件下,H_2O_2的质量浓度达最大值为6.91 mg/L;改性后的电极比未改性电极具有更高的DMPO-OH相应电流,同时可产生更多的羟基自由基(·OH);经120 min电催化处理后,PNT的去除率达到了81.2%;电-芬顿降解菲那西汀过程符合降解一级反应动力学,动力学常数为0.049 3。该结果验证了该电极可以显著提高菲那西汀的降解效能、提升H_2O_2和·OH产率、缩短反应时间。
关键词(KeyWords): 电-芬顿;菲那西汀;过氧化氢;羟基自由基;制药废水处理
基金项目(Foundation): 天津市科技计划项目(17YFCZZC00360)
作者(Author): 张永刚,黄耀霈,刘莹
参考文献(References):
- [1]BOCOS E,IGLESIAS O,PAZOS M,et al.Nickel foam a suitable alternative to increase the generation of Fenton's reagents[J].Process Safety and Environmental Protection,2016,101:34-44.
- [2]GARC魱A O,ISARAIN-CH魣VEZ E,GARCIA-SEGURA S,et al.Degradation of 2,4-dichlorophenoxyacetic acid by electro-oxidation and electro-Fenton/BDD processes using a pre-pilot plant[J].Electrocatalysis,2013,4(4):224-234.
- [3]张锋.电芬顿法降解苯酚废水的研究[J].广州化工,2014,42(10):116-117,141.ZHANG F.Degradation of phenol wastewater by electro-Fenton process[J].Guangzhou Chemical Industry,2014,42(10):116-117,141(in Chinese).
- [4]FAN Y,AI Z H,ZHANG L Z.Design of an electro-Fenton system with a novel sandwich film cathode for wastewater treatment[J].Journal of Hazardous Materials,2010,176(1/2/3):678-684.
- [5]HAIDER M R,JIANG W L,HAN J L,et al.In-situ electrode fabrication from polyaniline derived N-doped carbon nanofibers for metal-free electro-Fenton degradation of organic contaminants[J].Applied Catalysis B:Environmental,2019,256:117774.
- [6]JONOUSH Z A,REZAEE A,GHAFFARINEJAD A.Electrocatalytic nitrate reduction using Fe0/Fe3O4nanoparticles immobilized on nickel foam:Selectivity and energy consumption studies[J].Journal of Cleaner Production,2020,242:118569.
- [7]KANG Y J,YANG P D,MARKOVIC N M,et al.Shaping electrocatalysis through tailored nanomaterials[J].Nano Today,2016,11(5):587-600.
- [8]马楠,田耀金,杨广平,等.改性活性碳纤维电芬顿降解苯酚废水性能研究[J].环境科学,2014,35(7):2627-2632.MA N,TIAN Y J,YANG G P,et al.Modification of activated carbon fiber for electro-Fenton degradation of phenol[J].Environmental Science,2014,35(7):2627-2632(in Chinese).
- [9]LI D,SUN T Y,WANG L,et al.Enhanced electro-catalytic generation of hydrogen peroxide and hydroxyl radical for degradation of phenol wastewater using MnO2/Nano-G|FoamNi/Pd composite cathode[J].Electrochimica Acta,2018,282:416-426.
- [10]LI G S,ZHANG Y G.Highly selective two-electron oxygen reduction to generate hydrogen peroxide using graphite felt modified with N-doped graphene in an electro-Fenton system[J].New Journal of Chemistry,2019,43(32):12657-12667.
- [11]LIANG J Y,WANG Y Z,WANG C C,et al.In situ formation of NiO on Ni foam prepared with a novel leaven dough method as an outstanding electrocatalyst for oxygen evolution reactions[J].Journal of Materials Chemistry A,2016,4(25):9797-9806.
- [12]LIU W,AI Z H,ZHANG L Z.Design of a neutral three-dimensional electro-Fenton system with foam nickel as particle electrodes for wastewater treatment[J].Journal of Hazardous Materials,2012,243:257-264.
- [13]MANIAM K K,CHETTY R.Electrodeposited palladium nanoflowers for electrocatalytic applications[J].Fuel Cells,2013,13(6):1196-1204.
- [14]OU B,WANG J X,WU Y,et al.A highly efficient cathode based on modified graphite felt for aniline degradation by electro-Fenton[J].Chemosphere,2019,235:49-57.
- [15]PRIYADARSHINI P,FLAHERTY D W.Form of the catalytically active Pd species during the direct synthesis of hydrogen peroxide[J].AIChE Journal,2019,65(12):.
- [16]REN G B,ZHOU M H,SU P,et al.Simultaneous sulfadiazines degradation and disinfection from municipal secondary effluent by a flow-through electro-Fenton process with graphenemodified cathode[J].Journal of Hazardous Materials,2019,368:830-839.
- [17]SONG S Q,WU M M,LIU Y H,et al.Efficient and stable carbon-coated nickel foam cathodes for the electro-Fenton process[J].Electrochimica Acta,2015,176:811-818.
- [18]WANG H,WANG J L.Comparative study on electrochemical degradation of 2,4-dichlorophenol by different Pd/C gas-diffusion cathodes[J].Applied Catalysis B:Environmental,2009,89(1/2):111-117.
- [19]马放,徐炳乾,邱珊,等.泡沫铜阴极电芬顿氧化降解焦化废水研究[J].给水排水,2018,44(S2):170-173.MA F,XU B Q,QIU S,et al.Study on degradation of coking wastewater by ElectroFenton oxidation of copper foam cathode[J].Water&Wastewater Engineering,2018,44(S2):170-173(in Chinese).
- [20]班福忱,赵晓彤,武玉萍,等.三维电极/电Fenton法处理苯酚废水机理研究[J].沈阳建筑大学学报(自然科学版),2014,30(1):137-141.BAN F C,ZHAO X T,WU Y P,et al.Study on mechanism of phenol wastewater degradation by three-dimensional/electrode-Fenton method[J].Journal of Shenyang Jianzhu University(Natural Science),2014,30(1):137-141(in Chinese).
- [21]YE Z H,GUELFI D R V,魣LVAREZ G,et al.Enhanced electrocatalytic production of H2O2at Co-based air-diffusion cathodes for the photoelectro-Fenton treatment of bronopol[J].Applied Catalysis B:Environmental,2019,247:191-199.
- [22]YU F K,ZHOU M H,YU X M.Cost-effective electro-Fenton using modified graphite felt that dramatically enhanced on H2O2electro-generation without external aeration[J].Electrochimica Acta,2015,163:182-189.