Ti/RuO_2-CoO电极制备及其氨氮降解性能
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摘要
采用热氧化法制备Ti/RuO_2-CoO电极,通过SEM和XRD对电极涂层的表面形貌和晶体结构进行表征;并利用最佳条件制备的电极开展电化学氧化氨氮模拟废水研究。实验研究了电流密度、初始pH值、Cl~-浓度和NH_3-N初始浓度对NH_3-N降解效果的影响。研究结果表明:当n(Ru)/n(Co)=7∶3时Ti/RuO_2-CoO电极对NH_3-N的去除效果较好。随着电流密度的增加,NH_3-N去除率随之升高;初始pH为碱性条件时,NH_3-N去除效果较好;NH_3-N去除率随Cl~-浓度的增加呈现先增大后减小,当Cl~-浓度为3 000 mg/L时,氨氮去除率达到97.95%。当电流密度为70 mA/cm~2、Cl~-浓度为3 000 mg/L、初始pH=9时,经过180 min电解后,氨氮初始浓度从500 mg/L降低至10.25 mg/L,且电化学氧化氨氮的产物主要为氮气和硝酸盐氮。
Ti/RuO_2-CoO anode was prepared by thermal oxidation method and was used to treat simulated wastewater which contained ammonia nitrogen(NH_3-N). The surface morphology and crystal structure of the electrode coating layer were analyzed by SEM and XRD. Effects of current density, initial pH, Cl~- concentration and initial NH_3-N concentration on removal efficiency of NH_3-N using Ti/RuO_2-CoO as anode were investigated.When n(Ru)/n(Co) was 7∶3, Ti/RuO_2-CoO anode exhibited good performance on degradation of NH_3-N. The increment of current density improved the removal rate of NH_3-N. The removal efficiency of NH_3-N was better in alkaline condition than that in acidic condition. The removal rate of NH_3-N increased firstly and then decreased along with the increment of Cl~- concentration. The NH_3-N removal rate was 97.75% in the condition that Clconcentration was 3 000 mg/L. When the current density was 70 mA/cm2, Cl~- concentration was 3 000 mg/L and the initial pH was 9, the NH_3-N concentration was degraded from 500 mg/L to 10.25 mg/L in electrolysis time of180 min. Main products during electrochemical oxidation of NH_3-N by Ti/RuO_2-CoO anode were nitrogen and nitrate.
Ti/RuO_2-CoO anode was prepared by thermal oxidation method and was used to treat simulated wastewater which contained ammonia nitrogen(NH_3-N). The surface morphology and crystal structure of the electrode coating layer were analyzed by SEM and XRD. Effects of current density, initial pH, Cl~- concentration and initial NH_3-N concentration on removal efficiency of NH_3-N using Ti/RuO_2-CoO as anode were investigated.When n(Ru)/n(Co) was 7∶3, Ti/RuO_2-CoO anode exhibited good performance on degradation of NH_3-N. The increment of current density improved the removal rate of NH_3-N. The removal efficiency of NH_3-N was better in alkaline condition than that in acidic condition. The removal rate of NH_3-N increased firstly and then decreased along with the increment of Cl~- concentration. The NH_3-N removal rate was 97.75% in the condition that Clconcentration was 3 000 mg/L. When the current density was 70 mA/cm2, Cl~- concentration was 3 000 mg/L and the initial pH was 9, the NH_3-N concentration was degraded from 500 mg/L to 10.25 mg/L in electrolysis time of180 min. Main products during electrochemical oxidation of NH_3-N by Ti/RuO_2-CoO anode were nitrogen and nitrate.
引文
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[2]Ting W H T,Tan I A W,Salleh S F,et al.Application of water hyacinth(eichhornia crassipes)for phytoremediation of ammoniacal nitrogen:A review[J].Journal of Water Process Engineering,2018(22):239-249.
[3]朱广伟.太湖富营养化现状及原因分析[J].湖泊科学,2008,20(1):21-26.
[4]马宏瑞,陈阳,马鹏飞.电化学氧化法处理高浓度氨氮废水研究[J].中国皮革,2018,47(3):50-56.
[5]刘晶冰,燕磊,白文荣,等.高级氧化技术在水处理的研究进展[J].水处理技术,2011,37(3):11-17.
[6]冯玉杰,崔玉虹,孙丽欣,等.电化学废水处理技术及高效电催化电极的研究与进展[J].哈尔滨工业大学学报,2004,36(4):450-455.
[7]孟惠民,史艳华,俞宏英,等.绿色环保的DSA电极的应用进展[J].材料保护,2007,40(11):53-55.
[8]Li G T,Zhu M Y,Chen J,et al.Production and contribution of hydroxyl radicals between the DSA anode and water interface[J].Journal of Environmental Sciences,2011,23(5):744-748.
[9]孔德生,吕文华,冯媛媛,等.DSA电极电催化性能研究及尚待深入探究的几个问题[J].化学进展,2009,21(6):1107-1117.
[10]尤宏,崔玉虹,冯玉杰,等.钛基Co中间层Sn O2电催化电极的制备及性能研究[J].材料科学与工艺,2004,12(3):230-233.
[11]Da S L M,Boodts J F C,De F L A.Chlorine evolution reaction at Ti/(RuO2+Co3O4)electrodes[J].Journal of the Brazilian Chemical Society,2003,14(3):388-395.
[12]Burke L D,Mccarthy M M.ChemInform abstract:Modification of the electronic transfer properties of Co3O4 as required for Its use in DSA-Type anodes[J].Cheminform,1988,19(34):1175-1179.
[13]Meher S K,Rao G R.Ultralayered Co3O4 for high-performance supercapacitor applications[J].Journal of Physical Chemistry C,2011,115(31):15646-15654.
[14]魏婕,黄胜,宋鹏程,等.热氧化法制备Ti/RuO2-TiO2-IrO2电极及处理亚甲基蓝废水[J].环境工程学报,2016,10(3):1289-1294.
[15]黄小清,甘卫平,杨杰,等.掺钴氧化钌(RuO2/Co3O4)·n H2O复合薄膜电极的制备与表征[J].粉末冶金材料科学与工程,2013,18(1):107-112.
[16]何潇,罗建中,蔡宗岳.微污染水源水中氨氮的危害与现代处理技术[J].工业水处理,2017,37(4):6-11.
[17]袁芳,代晋国,范洪波,等.老龄垃圾渗滤液高氨氮的电化学氧化及其能耗分析[J].水处理技术,2012,38(3):55-59.
[18]褚衍洋,杨波,李玲玲,等.氨氮在两种电解质体系下的电化学氧化[J].高校化学工程学报,2010,24(1):71-75.
[19]曾次元,李亮,赵心越,等.电化学氧化法除氨氮的影响因素[J].复旦学报(自然科学版),2006,45(3):348-352.
[20]鲁剑,张勇,吴盟盟,等.电化学氧化法处理高氨氮废水的试验研究[J].安全与环境工程,2010,17(2):51-53.
[21]Lin S H,Wu C L.Electrochemical removal of nitrite and ammonia for aquaculture[J].Water Research,1996,30(3):715-721.
[22]陈金銮,施汉昌,徐丽丽.pH值对氨氮电化学氧化产物与氧化途径的影响[J].环境科学,2008,29(8):2277-2281.
[23]Moran E,Cattaneo C,Mishima H,et al.Ammonia oxidation on electrodeposited Pt-Ir alloys[J].Journal of Solid State Electrochemistry,2008,12(5):583-589.
[24]邱勇萍,张国庆,杨晓青,等.光/电法氨氮降解过程中协同作用的研究[J].环境工程学报,2015,9(1):150-156.