电-多相臭氧催化技术处理金刚烷胺制药废水
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摘要
采用电-多相臭氧催化(E-catazone)技术处理高COD、高含盐、难生化的金刚烷胺制药废水.对比研究电-多相臭氧催化、多相臭氧催化(Catazone)、电催化氧化(EO)对金刚烷胺制药废水的处理效果,在此基础上进一步研究了电流密度、pH值以及气相O_3浓度对电-多相臭氧催化技术处理效果的影响,同时优化实验条件.实验结果表明,在原水pH值为12.5,电流密度为15mA/cm~2,O_3进气流速0.4L/min,O_3浓度为60mg/L的条件下,经过60min反应,电-多相臭氧催化技术获得了62%的COD去除和44%的总有机碳(TOC)去除,其效果显著优于多相臭氧催化(COD 44%,TOC 29%)与电催化氧化(COD13%,TOC 17%);同时,电-多相臭氧催化不仅氧化能力强,而且氧化速率快,获得的伪一级COD去除速率常数k是多相臭氧催化和电催化氧化的1.81倍和8.22倍,更为重要的是,电-多相臭氧催化技术还可以高效、快速地提高废水的生化性,提高约2个数量级,结果表明,电-多相臭氧催化技术是一种有潜力的高级氧化技术,可以实现高效、快速去除有机污染物以及提高废水的可生化性.
Electrochemical heterogeneous catalytic ozonation(E-catazone)process was studied for treating amantadine wastewater,which was of high COD,high salinity and nonbiodegradable.The amantadine removal efficiency of E-catazone process was compared with catalytic ozonation(Catazone)and electrochemical oxidation(EO)processes,Besides,the effects of current density,pH and ozone concentration on the amahadine treatment efficiency were further investigated to obtain optimized experimental conditions.Electro-catalytic ozonation obtained 62%of the COD removal efficiency and 44%removal of TOC under pH 12.5,current density 15mA/cm~2,O_3flow rate 0.4L/min and O_3concentration 60mg/L,The performance was significantly better than that of Catazone(COD 44%,TOC 29%)and EO(COD 13%,TOC 17%),E-catazone process demonstrated strong oxidizing power and fast oxidation rate,and the pseudo-first order of COD removal rate constant k was 1.81times and 8.22times of Catazone and EO,More importantly,the E-catazone could improve the biochemical properties of wastewater efficiently and rapidly,and increased by about two order of magnitude.The results showed that the E-catazone was a potential advanced oxidation technology,which could realize high efficiency,fast removal of organic pollutants and improve the biodegradability of wastewater.
Electrochemical heterogeneous catalytic ozonation(E-catazone)process was studied for treating amantadine wastewater,which was of high COD,high salinity and nonbiodegradable.The amantadine removal efficiency of E-catazone process was compared with catalytic ozonation(Catazone)and electrochemical oxidation(EO)processes,Besides,the effects of current density,pH and ozone concentration on the amahadine treatment efficiency were further investigated to obtain optimized experimental conditions.Electro-catalytic ozonation obtained 62%of the COD removal efficiency and 44%removal of TOC under pH 12.5,current density 15mA/cm~2,O_3flow rate 0.4L/min and O_3concentration 60mg/L,The performance was significantly better than that of Catazone(COD 44%,TOC 29%)and EO(COD 13%,TOC 17%),E-catazone process demonstrated strong oxidizing power and fast oxidation rate,and the pseudo-first order of COD removal rate constant k was 1.81times and 8.22times of Catazone and EO,More importantly,the E-catazone could improve the biochemical properties of wastewater efficiently and rapidly,and increased by about two order of magnitude.The results showed that the E-catazone was a potential advanced oxidation technology,which could realize high efficiency,fast removal of organic pollutants and improve the biodegradability of wastewater.
引文
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[2]宋永会,魏健,马印臣,等,金刚烷胺制药胺化废水与溴化废水的中和络合萃取处理[J].中国环境科学,2014,34(10):2522-2527.
[3]樊杰,金刚烷胺制药废水Fenton-超声氧化处理及溴化氢双极膜电渗析回收[D].北京:北京林业大学,2013.
[4]Bobu M,Yediler A,Siminiceanu I,et al,Comparison of different advanced oxidation processes for the degradation of two fluoroquinolone antibiotics in aqueous solutions,Journal of environmental science and health[J].Part A,Toxic/hazardous substances&environmental engineering,2002,36(4):1034-1042.
[5]宋永会,魏健,马印臣,等.络合萃取法处理金刚烷胺制药废水[J].环境科学研究,2014,27(12):1513-1518.
[6]曾萍,宋永会,樊杰,等,超声、Fenton及其联合工艺预处理金刚烷胺制药废水效果对比[C]//北京:中国环境科学学会学术年会论文A集,2014:4492-4496.
[7]Wang Y J,Li X Y,Zhen L M,et al.Electro-Fenton treatment of concentrates generated in nanofiltration of biologically pretreated landfill leachate[J].Journal of Hazardous Materials,2012,115(3):229-230.
[8]刘永泽,高级氧化过程中OH?和SO4-定量分析及溴代副产物生成规律研究[D].哈尔滨:哈尔滨工业大学,2015.
[9]Li X Y,Liu G C,Shi M,et al,A novel electro-catalytic ozonation process for treating Rhodamine B using mesoflower-structured TiO2-coated porous titanium gas diffuser anode[J].Water Science and Technology,2016,165(1):154-159.
[10]倪金雷.不同物相TiO2催化臭氧(/H2O2)体系的氧化效能[D].浙江:浙江工业大学,2015.
[11]Li X Y,Sun S B,Zhang X,et al,Combined electro-catazone/electroperoxone process for rapid and effective Rhodamine B degradation[J].Separation and Purification Technology,2017,178:189-192.
[12]Li X Y,Liu G C,Shi M,et al.Using TiO2 Mesoflower Interlayer in Tubular Porous Titanium Membranes for Enhanced Electrocatalytic Filtratio[J].Electrochimica Acta,2016,218:318-324.
[13]Chemlal R,Azzouz L,Kernani R,et al.Combination of advanced oxidation and biological processes for the landfill leachate treatment[J].Ecological Engineering,2014,73:281-289.
[14]李兆欣,甄丽敏,李新洋,等.BDD电极阳极氧化垃圾渗滤液纳滤浓缩液[J].环境工程学报,2014,8(11):4662-4668.
[15]Wang H J,Yuan S,Zhan J H,et al.Mechanisms of enhanced total organic carbon elimination from oxalic acid solutions by electroperoxone process[J].Water Research,2015,80:20-29.
[16]Komtchou S,Dirany A,Drogui P,et al,Removal of atrazine and its by-products from water using electrochemical advanced oxidation processes[J].Water Research,2017,125:91-103.
[17]Oulego P,Collado S,Laca A,et al.Impact of leachate composition on the advanced oxidation treatment[J].Water Research,2016,88:389-402.
[18]Li X Y,Zhu W,Wang C G,et al.The electrochemical oxidation of biologically treated citric acid wastewater in a continuous-flow threedimensional electrode reactor(CTDER)[J].Chemical Engineering Journal,2013,232(10):495-502.
[19]Kishimoto N,Sugimura E,Feasibility of an electrochemically assisted Fenton method using Fe2+/HOCl system as an advanced oxidation process[J].Water Science and Technology,2010,62(10):2321-2329.
[20]Yao W K,Wang X F,Yang H G,et al,Removal of pharmaceuticals from secondary effluents by an electroperoxone process[J].Water Research 2015,88:826-83.
[21]袁实.电催化臭氧水处理技术的开发和研究[D].北京:清华大学,2014.