辉光放电电解等离子体降解水中阳离子红XL-GRL
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摘要
针对染料废水色度高、难生物降解等问题,提出了用辉光放电电解等离子体(GDEP)技术降解染料废水阳离子红XL-GRL的方法。研究了放电电压、溶液浓度对脱色率的影响;测定了GDEP产生的活性物质以及降解过程中溶液的电导率、pH和TOC去除率的变化;分析了降解中间产物成分。结果表明,在600 V电压下,GDEP产生了HO?、H?、O?等高活性物质,他们可使染料分子在130 min内的脱色率达到93.32%,在120 min内TOC去除率达到了65.80%。降解过程中产生了大量带电离子及酸性中间产物。推测可能的降解机理是,阳离子红XL-GRL分子在HO·作用下双键断裂,生成酚类等产物,接着继续降解为中间产物醌,并进一步氧化为小分子有机酸,最终矿化为CO_2、H_2O和简单的无机离子。GDEP在有机染料废水处理方面具有一定的应用前景。
For high chroma and refractory dye wastewater, a glow discharge electrolysis plasma(GDEP)technique was used to degrade cationic red XL-GRL in dye wastewater. The effects of discharge voltage and dye concentration on the decolorization rate were investigated. The active species produced by GDEP, solution conductivity, pH, TOC removal rate during degradation process were determined, as well as the intermediate products. The experimental results showed that highly active species such as HO·, O· and H· are produced at the 600 V, which could lead to 93.32% dye decolorization after 130 min treatment, and 65.80% TOC removal after 120 min treatment. A large number of charged ions and acidic intermediates were produced accordingly.Moreover, a possible degradation mechanism was that the double bonds in cationic red XL-GRL molecular were broken under the action of HO·, and phenols were formed. They were degraded into quinones, and further oxidized into small-molecule organic acids. Finally, these acids were completely mineralized into CO2, H2 O and simple inorganic salt. As an advanced oxidation technique, GDEP has a promising application prospect in organic dye wastewater treatment.
For high chroma and refractory dye wastewater, a glow discharge electrolysis plasma(GDEP)technique was used to degrade cationic red XL-GRL in dye wastewater. The effects of discharge voltage and dye concentration on the decolorization rate were investigated. The active species produced by GDEP, solution conductivity, pH, TOC removal rate during degradation process were determined, as well as the intermediate products. The experimental results showed that highly active species such as HO·, O· and H· are produced at the 600 V, which could lead to 93.32% dye decolorization after 130 min treatment, and 65.80% TOC removal after 120 min treatment. A large number of charged ions and acidic intermediates were produced accordingly.Moreover, a possible degradation mechanism was that the double bonds in cationic red XL-GRL molecular were broken under the action of HO·, and phenols were formed. They were degraded into quinones, and further oxidized into small-molecule organic acids. Finally, these acids were completely mineralized into CO2, H2 O and simple inorganic salt. As an advanced oxidation technique, GDEP has a promising application prospect in organic dye wastewater treatment.
引文
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[2]唐嘉丽,岳秀,于广平,等.双氧水协同生化法处理实际印染废水[J].环境工程学报,2018,12(7):1942-1950.
[3]中华人民共和国生态环境部.环境统计年报2015[EB/OL].[2017-02-23].http://www.zhb.gov.cn/gzfw_13107/hjtj/hjtjnb/201702/P020170223595802837498.pdf,2015.
[4]李敏睿,柳淑娟,班宁宁,等.辉光放电电解等离子体降解水体中的亚甲基蓝[J].西北师范大学学报(自然科学版),2015,51(2):42-46.
[5]孙华,洪英,高廷耀,等.染料生产废水处理工艺探讨[J].同济大学学报(自然科学版),2001,29(10):1246-1250.
[6]陆泉芳,俞洁.辉光放电等离子体降解模拟染料废水的研究[J].环境科学学报,2006,26(11):1799-1803.
[7]欧晓霞,张凤杰,王崇,等.芬顿氧化法处理水中酸性品红的研究[J].环境工程学报,2010,4(7):1453-1456.
[8]孙怡,于利亮,黄浩斌,等.高级氧化技术处理难降解有机废水的研发趋势及实用化进展[J].化工学报,2017,68(5):1743-1756.
[9]吴晴,刘金泉,王凯,等.高级氧化技术在难降解工业废水中的研究进展[J].水处理技术,2015,41(11):25-29.
[10]RIBEIRO A R,NUNES O C,PEREIRA M F R,et al.An overview on the advanced oxidation processes applied for the treatment of water pollutants defined in the recently launched directive 2013/39/EU[J].Environment International,2015,75(2):33-51.
[11]仙光,张光明,刘毓璨,等.Fenton法处理电镀有机废水[J].环境工程学报,2018,12(4):1007-1012.
[12]SENGUPTA S K,SINGH O P.Contact glow discharge electrolysis:A study of its chemical yields in a queous inert-type electrolysis[J].Journal of Electroanalytical Chemistry,1994,369(1/2):113-120.
[13]CHENG M,ZENG G,HUANG D,et al.Hydroxyl radicals based advanced oxidation processes(AOPs)for remediation of soils contaminated with organic compounds:A review[J].Chemical Engineering Journal,2016,284:582-598.
[14]郑继东,陆泉芳,俞洁,等.辉光放电电解等离子体降解水体中的罗丹明B[J].环境科学学报,2017,37(6):2164-2170.
[15]王凤秋.辉光放电等离子体技术在模拟废水降解过程中的应用研究[D].西安:西北大学,2013.
[16]陆泉芳,俞洁,刘永军,等.接触辉光放电等离子体降解水体中的对氯硝基苯[J].西北师范大学学报(自然科学版),2003,39(1):49-53.
[17]JAMRóZ P,GR?DA K,POHL P,et al.Atmospheric pressure glow discharges generated in contact with flowing liquid cathode:Production of active species and application in wastewater purification processes[J].Plasma Chemistry and Plasma Processing,2014,34(1):25-37.
[18]SUN B,KUNITOMO S,IGARASHI C.Characteristics of ultraviolet light and radicals formed by pulsed discharge in water[J].Journal of Physics D:Applied Physics,2006,39(17):3814-3820.
[19]LIU Y,SUN B,WANG L,et al.Characteristics of light emission and radicals formed by contact glow discharge electrolysis of an aqueous solution[J].Plasma Chemistry and Plasma Processing,2012,32(2):359-368.
[20]张亚平,韦朝海.光Fenton氧化降解染料阳离子红GTL[J].中南大学学报(自然科学版),2008,39(4):688-693.
[21]ZHAO W R,SHI H X,WANG D H.Ozonation of cationic X-GRL in aqueous solution:Degradation and mechanism[J].Chemosphere,2004,57(9):1189-1199.
[22]田东凡,王玉如,宋薇,等.UV/PMS降解水中罗丹明B的动力学及反应机理[J].环境科学学报,2018,38(5):1868-1876.
[23]JIANG B,ZHENG J T,QIU S,et al.Review on electrical discharge plasma technology for wastewater remediation[J].Chemical Engineering Journal,2014,236:348-368.
[24]罗汉金,刘佳乐,朝海,等.染料溶液的臭氧脱色效率和残留物的分析研究[J].环境化学,2006,25(5):602-605.
[25]GAO J Z,YU J,LU Q F,et al.Decoloration of alizarin red S in aqueous solution by glow discharge electrolysis[J].Dyes Pigments,2008,76(1):47-52.
[26]陆泉芳,俞洁,杨彩玲,等.辉光放电电解降解水体中阳离子桃红FG的机理[J].化工学报,2018,69(6):2664-2671.
[27]龚丹.蒽醌染料的TiO2光催化降解产物分析及其降解过程研究[D].武汉:武汉纺织大学,2013.