序批式复极性三维电催化反应器降解苯并噻唑的影响因素
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摘要
设计构建了序批式复极性三维电催化反应器,以自制的Fe/Fe2O_3/Fe3O_4/AC作为粒子电极,考察了电解质种类及浓度、进水pH、上升流速、进水时间和电催化反应时间多个因素对序批式复极性三维电催化反应器去除苯并噻唑的影响。通过对苯并噻唑的去除率、反应体系矿化度、矿化电流效率以及电能能耗多个指标进行评价,得到最佳运行条件:电解液为中性的0.1 mol·L~(-1)Na Cl溶液,进水时间为30 min,上升流速为8.333 m L·min~(-1),电催化反应时间为3 h。在该运行条件下,初始浓度为100 mg·L~(-1)的苯并噻唑最终被完全去除,反应体系中的矿化率达到92.0%,而消耗的电能较低仅为13.00 k W·h·(kg COD)-1。
A sequencing batch bipolar three-dimensional electrocatalytic reactor filled with modified particle electrodes was constructed and used for benzothiazole(BTH) degradation. The influence of multiple factors,including electrolyte species,concentration,pH,up-flow velocity,inflow duration,and electrocatalytic reaction time,on the BTH degradation performance were studied. The BTH removal rate,mineralization,mineralization current efficiency,and energy consumption were measured. The results showed that the optimal operating conditions of the reactor were: electrolyte of 0. 1 mol·L~(-1)Na Cl solution,pH of 7,inflow duration of 30 min,up-flow velocity of 8. 333 m L·min~(-1),and electrocatalytic reaction time of 3 h. When operated at these conditions,the reactor achieved complete degradation of BTH with an initial concentration of 100 mg·L~(-1)and 92% removal of mineralization with low energy consumption of 13 k W·h·(kg COD)-1.
A sequencing batch bipolar three-dimensional electrocatalytic reactor filled with modified particle electrodes was constructed and used for benzothiazole(BTH) degradation. The influence of multiple factors,including electrolyte species,concentration,pH,up-flow velocity,inflow duration,and electrocatalytic reaction time,on the BTH degradation performance were studied. The BTH removal rate,mineralization,mineralization current efficiency,and energy consumption were measured. The results showed that the optimal operating conditions of the reactor were: electrolyte of 0. 1 mol·L~(-1)Na Cl solution,pH of 7,inflow duration of 30 min,up-flow velocity of 8. 333 m L·min~(-1),and electrocatalytic reaction time of 3 h. When operated at these conditions,the reactor achieved complete degradation of BTH with an initial concentration of 100 mg·L~(-1)and 92% removal of mineralization with low energy consumption of 13 k W·h·(kg COD)-1.
引文
[1]GINSBERG G,TOAL B,KURLAND T.Benzothiazole Toxicity assessment in support of synthetic turf field human health risk assessment[J].Toxicology and Environmental Health,Part A:Current Issues,2011,74(17):1175-1183
[2]BELLAVIA V,NATANGEOLO M,FANELLI R,et al.Analysis of benzothiazole in Italian wines using headspace solid-phase microextraction and gass chromatography mass spectrometry[J].Journal of Agricultural&Food Chemistry,2000,48:1239-1242
[3]刘春苗,丁杰,刘先树,等.电辅助微生物反应器降解苯并噻唑效能的研究[J].环境科学,2014,35(11):4192-4197
[4]李鹏宇,李江胜,刘卫东,等.苯并噻唑类杂环合成最新进展[J].精细化工中间体,2011,41(4):8-11
[5]BESSE P,COMBOURIEU B,BOYSE G,et al.Long-Range1H-15N heteronuclear shift correlation at natural abundance:A tool to study benzothiazole biodegradation by two Rhodococcus strains[J].Applied and Environmental Microbiology,2001,67:1412-1417
[6]KLOEPFER A,JEKEL M,REETSMA T.Occurrence,sources,and fate of benzothiazoles in municipal wastewater treatment plants[J].Environmental Science&Technology,2005,39(10):3792-3798
[7]QIN Y H,SUN M,LIU H J,et al.Au Pd/Fe3O4-based three-dimensional electrochemical system for efficiently catalytic degradation of 1-butyl-3-methylimidazolium hexafluorophosphate[J].Electrochimica Acta,2015,186:328-336
[8]汪巡,朱友利,施永生,等.三维电解法处理有机废水的研究进展[J].化工新型材料,2011,39(11):39-41
[9]陈沛.高级催化反应器在印染废水中应用[D].武汉:武汉纺织大学,2014
[10]乔启成.新型填充床电化学反应器电极材料制备、表征及对酸性橙II的催化氧化性能研究[D].徐州:中国矿业大学,2014
[11]张建刚.不溶性催化电极的制备及其对废水中有机物、菌藻和纤维素类物质的催化降解作用[D].北京:北京化工大学,2010
[12]李新洋.填充负载型活性炭三维电极反应器的开发与试验研究[D].北京:清华大学,2013
[13]李艳.阴阳极共同作用体系电催化降解邻硝基苯酚的研究[D].哈尔滨:哈尔滨工业大学,2008
[14]任文鑫.吸附—催化剂吸附苯酚及干催化氧化所吸附苯酚行为的研究[D].西安:西北大学,2012
[15]MURUGANANTHAN M,YOSHIHARA S,RAKUMA T,et al.Mineralization of bispheol A(BPA)by anodic oxidation with boron-doped diamond(BDD)electrode[J].Hazardous Materials,2008,154:213-220
[16]GUINEA E,ARIAS C,Cabot P L,et al.Mineralization of salicylic acid in acidic aqueous medium by electrochemical advanced oxidation processes using platinum and boron-doped diamond as anode and cathodically generated hydrogen peroxide[J].Water Research,2008,42:499-511
[17]魏金枝.电催化-生物氧化组合工艺构建及处理除草剂废水研究[D].哈尔滨:哈尔滨工业大学,2011
[18]李弘.电催化氧化法用于制药废水预处理与深度处理的实验研究[D].哈尔滨:哈尔滨工业大学,2013
[19]毕强.电化学处理有机废水电极材料的制备与性能研究[D].西安:西安建筑科技大学,2014
[20]李鹏.有机污染物电催化氧化有效电流表征及其阶段反应动力学[D].徐州:中国矿业大学,2015
[21]LIU Yuan,LIU Huiling.Comparative studies on the electrocatalytic properties of modified Pb O2anodes[J].Electrochimica Acta,2008,53(16):5077-5083
[22]RICHARD S,NICHOLSON.Theory and application of cyclic voltammetry formeasurement of electrode reaction kinetics[J].Analytical Chemistry,1965,37(11):1351-1355
[23]李海涛.循环伏安法对PAN基高模碳纤维阳极氧化的研究[D].北京:北京化工大学,2010
[24]季跃飞,魏杰,徐笑华,等.电解质种类对电催化氧化降解苯酚的影响[J].环境工程学报,2010,4(9):2000-2004
[25]于明瑞.电催化氧化体系阳极的制备及在维尼纶废水处理中的应用[D].哈尔滨:哈尔滨工业大学,2009
[26]SHAN Danna,DENG Shub,ZHAO Tianning,et al.Preparation of ultrafine magnetic biochar and activated carbon for pharmaceutical adsorption and subsequent degradation by ball milling[J].Hazardous Materials,2016,305:156-163
[27]WANG Ying,SHEN Zhenya,CHEN Xiaochun.Effects of experimental parameters on 2,4-dichlorphenol degradation over ErChitosan-Pb O2electrode[J].Hazardous Materials,2010,178(1-3):867-874
[2]BELLAVIA V,NATANGEOLO M,FANELLI R,et al.Analysis of benzothiazole in Italian wines using headspace solid-phase microextraction and gass chromatography mass spectrometry[J].Journal of Agricultural&Food Chemistry,2000,48:1239-1242
[3]刘春苗,丁杰,刘先树,等.电辅助微生物反应器降解苯并噻唑效能的研究[J].环境科学,2014,35(11):4192-4197
[4]李鹏宇,李江胜,刘卫东,等.苯并噻唑类杂环合成最新进展[J].精细化工中间体,2011,41(4):8-11
[5]BESSE P,COMBOURIEU B,BOYSE G,et al.Long-Range1H-15N heteronuclear shift correlation at natural abundance:A tool to study benzothiazole biodegradation by two Rhodococcus strains[J].Applied and Environmental Microbiology,2001,67:1412-1417
[6]KLOEPFER A,JEKEL M,REETSMA T.Occurrence,sources,and fate of benzothiazoles in municipal wastewater treatment plants[J].Environmental Science&Technology,2005,39(10):3792-3798
[7]QIN Y H,SUN M,LIU H J,et al.Au Pd/Fe3O4-based three-dimensional electrochemical system for efficiently catalytic degradation of 1-butyl-3-methylimidazolium hexafluorophosphate[J].Electrochimica Acta,2015,186:328-336
[8]汪巡,朱友利,施永生,等.三维电解法处理有机废水的研究进展[J].化工新型材料,2011,39(11):39-41
[9]陈沛.高级催化反应器在印染废水中应用[D].武汉:武汉纺织大学,2014
[10]乔启成.新型填充床电化学反应器电极材料制备、表征及对酸性橙II的催化氧化性能研究[D].徐州:中国矿业大学,2014
[11]张建刚.不溶性催化电极的制备及其对废水中有机物、菌藻和纤维素类物质的催化降解作用[D].北京:北京化工大学,2010
[12]李新洋.填充负载型活性炭三维电极反应器的开发与试验研究[D].北京:清华大学,2013
[13]李艳.阴阳极共同作用体系电催化降解邻硝基苯酚的研究[D].哈尔滨:哈尔滨工业大学,2008
[14]任文鑫.吸附—催化剂吸附苯酚及干催化氧化所吸附苯酚行为的研究[D].西安:西北大学,2012
[15]MURUGANANTHAN M,YOSHIHARA S,RAKUMA T,et al.Mineralization of bispheol A(BPA)by anodic oxidation with boron-doped diamond(BDD)electrode[J].Hazardous Materials,2008,154:213-220
[16]GUINEA E,ARIAS C,Cabot P L,et al.Mineralization of salicylic acid in acidic aqueous medium by electrochemical advanced oxidation processes using platinum and boron-doped diamond as anode and cathodically generated hydrogen peroxide[J].Water Research,2008,42:499-511
[17]魏金枝.电催化-生物氧化组合工艺构建及处理除草剂废水研究[D].哈尔滨:哈尔滨工业大学,2011
[18]李弘.电催化氧化法用于制药废水预处理与深度处理的实验研究[D].哈尔滨:哈尔滨工业大学,2013
[19]毕强.电化学处理有机废水电极材料的制备与性能研究[D].西安:西安建筑科技大学,2014
[20]李鹏.有机污染物电催化氧化有效电流表征及其阶段反应动力学[D].徐州:中国矿业大学,2015
[21]LIU Yuan,LIU Huiling.Comparative studies on the electrocatalytic properties of modified Pb O2anodes[J].Electrochimica Acta,2008,53(16):5077-5083
[22]RICHARD S,NICHOLSON.Theory and application of cyclic voltammetry formeasurement of electrode reaction kinetics[J].Analytical Chemistry,1965,37(11):1351-1355
[23]李海涛.循环伏安法对PAN基高模碳纤维阳极氧化的研究[D].北京:北京化工大学,2010
[24]季跃飞,魏杰,徐笑华,等.电解质种类对电催化氧化降解苯酚的影响[J].环境工程学报,2010,4(9):2000-2004
[25]于明瑞.电催化氧化体系阳极的制备及在维尼纶废水处理中的应用[D].哈尔滨:哈尔滨工业大学,2009
[26]SHAN Danna,DENG Shub,ZHAO Tianning,et al.Preparation of ultrafine magnetic biochar and activated carbon for pharmaceutical adsorption and subsequent degradation by ball milling[J].Hazardous Materials,2016,305:156-163
[27]WANG Ying,SHEN Zhenya,CHEN Xiaochun.Effects of experimental parameters on 2,4-dichlorphenol degradation over ErChitosan-Pb O2electrode[J].Hazardous Materials,2010,178(1-3):867-874