Effect of oxidative degradation of benzoic acid simulated wastewater by VUV/air

doi:10.16085/j.issn.1000-6613.2016-2172

Abstract

Abstract: Effects of pH,aeration rate,initial concentration of pollutant and coexisting anions on the degradation of benzohydroxamic acid in wastewater by VUV/air (vacuum ultraviolet) were studied.The experimental results showed that the best degradation rate could reach 78.89% when the VUV light power 10W,benzohydroxamic acid concentration 30mg/L,wastewater pH 4,aeration rate 0.6L/min and the reaction time 120min.Among these coexisting anions,the influence on degradation from high to low was:SiO₃^2- > HCO₃^- > CO₃^2- > SO₄^2- > Cl^-.Based on the mechanism analysis for the degradation of benzohydroxamic acid by VUV/air,the direct photolysis and oxygenolysis of hydroxyl radical produced by vacuum ultraviolet radiation played the main role in this process.The degradation result was fitted to the first-order kinetic equation,ln (C_t/C₀)=-kt.

Key words: advanced oxidation progress, vacuum ultraviolet (VUV), benzoylhydroxamic acid, radica, reaction kinetics

摘要： 以真空紫外/曝气（vacuum ultraviolet/air，VUV/air）降解模拟废水中的苯甲羟肟酸为研究对象，考察了废水pH、曝气量、污染物初始浓度及共存阴离子等因素对VUV/air降解苯甲羟肟酸效果的影响。实验结果表明：在VUV光源功率10W、苯甲羟肟酸初始浓度30mg/L、废水初始pH=4、曝气量0.6L/min、反应时间120min的条件下，VUV/air对苯甲羟肟酸模拟废水的降解效果最好，降解率为78.89%；其中共存阴离子对VUV/air降解苯甲羟肟酸的影响作用大小顺序依次为：SiO₃^2- > HCO₃^- > CO₃^2- > SO₄^2- > Cl^-。通过对VUV/air降解苯甲羟肟酸的机理分析研究发现，VUV/air降解苯甲羟肟酸的过程中起主要作用的是直接光降解和真空紫外产生的羟基自由基氧化分解。VUV/air降解废水中苯甲羟肟酸的行为符合一级动力学方程ln（C_t/C₀）=-kt。

关键词: 高级氧化法, 真空紫外, 苯甲羟肟酸, 自由基, 反应动力学

CLC Number:

X783

ZHANG Dachao, CHEN Min, DAI Zhenpeng, WU Suying, WANG Chunying. Effect of oxidative degradation of benzoic acid simulated wastewater by VUV/air[J]. Chemical Industry and Engineering Progress, 2017, 36(07): 2639-2644.

张大超, 陈敏, 代振鹏, 吴速英, 王春英. 真空紫外/曝气氧化降解苯甲羟肟酸模拟废水[J]. 化工进展, 2017, 36(07): 2639-2644.

References

[1] ZENG V,LI J Z,QIN S. Dioxygen affinites and biomimetic eatalytic performance of transtion metal hydroxamates[J]. Reaction Kinetics and Catalysis Letters,2003,79:111-117.
[2] 罗仙平,谢明辉. 金属矿山选矿废水净化与资源化利用现状与研究发展方向[J]. 中国矿业,2006,10(15):51-56. LUO X P, XIE M H. Situation of purifying and comprehensive utilizing mineral processing wastewate and its development trend in nonferrous nonferrous metal ore mining[J]. China Mining Magazine,2006,10(15):51-56.
[3] 邢瑞,温东辉,唐孝炎. 紫外与真空紫外深度处理焦化废水的试验研究[J]. 北京大学学报(自然科学版),2012,48(4):639-646. XING R,WEN D H,TANG X Y. Research on the advanced treatment of coking wastewater by ultraviolet or vacuum ultraviolet[J]. Acta Scientiarum Naturalium Universitatis Pekinensis,2012,48(4):639-646.
[4] 宋卫锋,唐铁柱,林梓河,等. 生物接触氧化法处理选矿废水的影响因素[J]. 环境工程学报,2013,2(7):603-607. SONG W F,TANG T Z,LIN Z H,et a1. Some influencing factors of flotation wastewater treatment with bio-contact oxidation method[J]. Chinese Journal of Environmental Engineering,2013,2(7):603-607.
[5] 王福奎,王忠诚,滕龙鱼,等. 黄药类捕收剂浮选时H₂O₂的应用[J]. 有色金属(选矿部分),2002(5):45-47. WANG F K,WANG Z C,TENG L Y,et a1. Xanthate type flotation collector when the application of H₂O₂[J]. Non-ferrous Metals(Mineral Processing Section),2002(5):45-47.
[6] 朱玉霜,朱建光.浮选药剂的化学原理(修订版)[M].长沙:中南工业大学出版社,1996. ZHU Y X,ZHU J G. The chemical principle of flotation reagents[M].Changsha:Central South University of Technology Press,1996.
[7] 顾浩飞,安太成,文晟,等. 超声光催化降解苯胺及其衍生物研究[J]. 环境科学学报,2003,23(5):593-597. GU H F,AN T C,WEN S,et a1.Sonophotocatalytic degradation of aniline and its derivatives[J]. Acta Scientiae Circumstantiae,2003,23(5):593-597.
[8] DOMBI A,ILISZ I,LASZLO Z,et a1. Comparison of ozone-based and other (VUV and TiO₂/UV)radical generation methods in phenol decomposition[J]. Ozone:Science & Engineering:The Journal of the International Ozone Association,2002,24(1):49-54.
[9] AN T C,GU H F,ZHU X H,et al. Decolorization and COD removal from reactive dye-containing waste water using sonophotocatalytic technology[J]. J. Chem. Technol. Biotechnol. Accepted,2003,78:1142-1148.
[10] 鄢恒珍,龚文琪,梅光军,等. 羟肟酸类捕收剂的生物降解性能及机理研究[J]. 中国给水排水,2010,26(15):89-91. YAN H Z,GONG W Q,MEI G J,et a1. Study on biodegradability and mechanism of hydroxamic acid collectors[J]. China Water Wastewater,2010,26(15):89-91.
[11] LUO X P,WANG J W,WANG C Y,et a1. Degradation and mineralization of benzohydroxamic acid by synthesi-zed mesoporpus La/TiO₂[J]. International Journal of Environmental Research and Public Health,2016,13:997-1010.
[12] 李文杰,洪添,胡勇有,等. UVU/UV耦合深度处理印染废水尾水的研究[J]. 环境科学学报,2014,34(7):1689-1695. LI W J,HONG T,HU Y Y,et a1. Advanced treatment of printing and dyeing wastewater by combination of vacuum ultraviolet and high frequent ultrasound irradiation[J]. Acta Scientiae Circumstantiae,2014,34(7):1689-1695
[13] CHEN C,CHEN H,GUO X,et al. Advanced ozone treatment of heavy oil refining wastewater by activated carbon supported iron oxide[J]. Journal of Industrial & Engineering Chemistry,2014,20(5):2782-2791.
[14] 宋宝旭,刘四清. 国内选矿厂废水处理现状与研究进展[J]. 矿冶,2012,21(2):97-103. SONG B X,LIU S Q. Domestic wastewater treatment status and research progress of concentrator[J]. Mining Metal,2012,21(2):97-103
[15] BABATUNDE A O,ZHAO Y Q,NEILL M O,et al. Constructed wetlands for environmental pollution control:a review of developments research and practice in Ireland[J]. Environment International,2008,1:116-126.
[16] MA J,GRAHAM N.Degradation of atrazine by manganese-catalysed ozonation:influence of humic substances[J].Water Research,1999,33(3):785-793.
[17] 尹平河,梁凤颜,赵玲. TiO₂/EP光催化降解水体中微污染磺胺嘧啶的研究[J]. 环境工程学报,2010,4(8):1704-1708. YIN P H,LIANG F Y,ZHAO L. Photocatalytic degradation of trace sulfadiazine in aqueous solution by TiO₂ imm obilized on expanded perlite[J]. Chinese Journal of Environmental Engineering,2010,4(8):1704-1708.
[18] KIM D H,ANDERSON M A. Solution factors affecting the photocatalytic and photoelectrocatalytic degradation of formic acid using supported TiO₂ thin films[J].Journal of Photochemistry and Photobiology A:Chemistry,1996,94(2/3):221-229.
[19] BELTRAN F J. Ozone reaction kinetics for water and wastewater systerms[M]. London:Lewis Publisher,2004:4-19.
[20] CHEN Q Q,WU P X,LI Y Y,et a1. Heterogeneous photo-Fenton photo degradation of reactive brilliant orange X-GN over iron-pillared montmorillonite under visible irradiation[J]. Journal of Hazardous Materials,2009,168(2/3):901-908.
[21] 白小霞,杨庆,丁昀,等. 催化臭氧氧化处理难降解石化废水技术的研究进展[J]. 化工进展,2016,35(1):263-268. BAI X X,YANG Q,DING Y,et a1.Research progress of catalytic ozonation process to treat refractory petrochemical wastewater[J]. Chenical Industry and Engineering Progress,2016,35(1):263-268.