微纳铁活化过硫酸钠降解污染土壤中DDTs的效果研究
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摘要
作为典型的持久性有机污染物,DDTS尽管已被禁止使用,但由于其稳定的结构,土壤中仍然残留大量的DDTs,亟需开发快速高效的DDTs降解技术。基于此,本文研究了微米尺寸具有纳米单元的铁粉(微纳铁,micro/nano-Fe~Ⅱ)活化过硫酸钠(sodium persulfate,PS)降解场地污染土壤中DDTs的效果,并考察了微纳铁负载量、过硫酸钠浓度、反应时间及氧化-洗脱耦合对DDTs去除效率的影响。研究结果表明:微纳铁能有效活化Ps降解土壤中的DDTs,在Ps浓度为100mmol/L时,DDTs的降解率随着微纳铁负载量增加而增加,当微纳铁升高到44.8g/L时,p,p'-DDT和o,p'-DDT的降解率高达92.2%和95.1%。洗脱-氧化耦合实验中,3种表面活性剂Tween80、Brij35和SDBS,其中Brij35土壤洗脱液中DDTs的降解效率最高,微纳铁和Ps的摩尔比为4:1时,对DDTs有最佳的降解效果。以上研究结果为DDTs的去除提供了一种新的途径,也为其他有机污染场地的修复提供了一类新技术。
As typical persistent organic contaminants,DDTs pollution has received much attention due to their persistence and high toxicity although it has been banned for many years,so it is highly important to develop efficiently methods for DDTs remediation.In this study persulfate activated with micro/nano-Fe~0 particles for DDTs degradation in soil was investigated,and the effects of micro/nano-Fe~0 dosage,persulfate concentration,reaction time and combined elutes-oxidation on the removal efficiency of DDTs were also examined.The results indicated persulfate was activated efficiently with micro/nano-Fe~0 for DDTs degradation in soil.With persulfate concentration of 100 mmol/L and micro/nano-Fe~0 loading of 44.8 g/L,the degradation efficiencies of p,p'-DDT and o,p'-DDT were 92.2% and 95.1%,respectively.Combined elute-oxidation was also efficient for DDTs degradation in the elutes,and among the three surfactants including Tween80,Brij35 and SDBS,the highest degradation efficiency of DDTs was observed in Brij35 solution,which indicated that Brij35 is the best elute in the combination of elute-oxidation processes.This study provides a new method for the remediation of DDTs contaminated soil with persulfate activation technologies.
As typical persistent organic contaminants,DDTs pollution has received much attention due to their persistence and high toxicity although it has been banned for many years,so it is highly important to develop efficiently methods for DDTs remediation.In this study persulfate activated with micro/nano-Fe~0 particles for DDTs degradation in soil was investigated,and the effects of micro/nano-Fe~0 dosage,persulfate concentration,reaction time and combined elutes-oxidation on the removal efficiency of DDTs were also examined.The results indicated persulfate was activated efficiently with micro/nano-Fe~0 for DDTs degradation in soil.With persulfate concentration of 100 mmol/L and micro/nano-Fe~0 loading of 44.8 g/L,the degradation efficiencies of p,p'-DDT and o,p'-DDT were 92.2% and 95.1%,respectively.Combined elute-oxidation was also efficient for DDTs degradation in the elutes,and among the three surfactants including Tween80,Brij35 and SDBS,the highest degradation efficiency of DDTs was observed in Brij35 solution,which indicated that Brij35 is the best elute in the combination of elute-oxidation processes.This study provides a new method for the remediation of DDTs contaminated soil with persulfate activation technologies.
引文
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[16]Tan C,Gao N,Chu W,et al.Degradation of diuron by persulfete activated with ferrous ion[J].Separation and Purification Technology,2012,95:44-48
[17]Zhang Y,Xie X,Huang W,et al.Degradation of aniline by Fe~(2+)-activated pereulface oxidation at ambient temperature[J].Joumal of Central South University,2013,20:1010-1014
[18]Liang C,Lai M C.Trichloroethylene degradation by zero valent iron activated persulfate oxidation[J].Environmental Engineering Science,2008,25(7):1071-1078
[19]Hussain I,Zhang Y,Huang S,et al.Degradation of p-chloroaniline by persulfate activated with zero-valent iron[J].Chemical Engineering Journal,2012,203:269-276
[20]Kang S,Liu S,Wang H,Cai W.Enhanced degradation performances of plate-likemicro/nanostructured zero valent iron to DDT[J].Journal of Hazardous Materials,2016,307:145-153
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[22]Zhu C Y,Fang G D,Dionysiou D D,et al.Efficient transformation of DDTs with persulfate activation by zero-valent iron nanoparticles:A Mechanistic study[J].Journal of Hazardous Materials,2016,316:232-241
[23]Wolcott A R,Shin Y O,Chodan J J.Adsorption of DDT by soils,soil fractions,and biological materials[J].Journal of Agricultural and Food Chemistry,1970,18(6):1129-1133
[24]刘衡锡,张乃东,朱正江.硫酸自由基在水处理中的反应特性[J].科学通报,2012,36:3493-3499
[25]朱长银,方国东,司友斌,等.洗脱-过硫酸钠氧化联合去除土壤中PCBs的研究[J].土壤,2015,47(6):1125-1131
[2]李孟楠,雷磊,刘欣,DDT毒性及毒理机制的研究进展[J].绿色科技,2011(10):114-116
[3]任仁.《斯德哥尔摩公约》禁用的12种持久性有机污染物[J].大学化学,2003,18(3):37-41
[4]王瑛,李扬,黄启飞,等.温度和停留时间对DDT污染土壤热脱附效果的影响[J].环境工程,2012(1):116-120
[5]叶茂,杨兴伦,魏海江,等.持久性有机污染场地土壤淋洗法修复进展[J].土壤学报,2012,49(4):803-814
[6]罗飞,宋静,潘云雨,等.典型滴滴涕废弃生产场地污染土壤的人体健康风险评估[J],土壤学报,2012,49(1):26-31
[7]Passatore L,Rossetti S,Juwarkar A A,et al.Phytoremediation and bioremediation of polychlorinated biphenyls(PCBs):State of knowledge and research perspectives[J].Journal of Hazardous Materials,2014,278:189-202
[8]洪青,蒋新,李顺鹏.微生物降解DDT研究进展[J].土壤,2008,40(3):329-334
[9]Gillham R W,O'Hannesin S F.Enhanced degradation of halogenated aliphatics by zerovalent iron[J].Ground Water,1994:958-967
[10]Kim Y,Carraway E R.Dechlorination of pentachlorophenol by zero valent iron and modified zero valent Irons[J].Eovironmcaital Science&Technology,2000,34(10):2014-2017
[11]Quinn J,Geiger C,Clausen C,et al.Field demonstration of DNAPL debalogenation using emulsified zero-valent iron[J].Environmental Science&Technology,2005,39(5):1309-1318
[12]Sayles G D,You O,Wang M,et al.DDT,DDD,and DDE dechlorination by zero-valent iron[J].Environmental Science&Technology,1997,31(12):3448-3454
[13]Tsitonaki A,Petri B,Crimi M,et al.In situ chemical oxidation of contaminated soil and groundwater using persulfate:a review[J].Critical Reviews in Environmental Science and Technology,2010,40(1):55-91
[14]Cao J,Zhang W X,Brown D G,et al.Oxidation of lindane with Fe(Ⅱ)-activated sodium persulfete[J],Envircmmental Engineering Science,2008,25(2):221-228
[15]Chen K F,Kao C M,Wu L C,et al.Methyl tert-butyl ether(MTBE)degradation by ferrous ion-activated persulfate oxidation:feasibility and kinetics studies[J].Water Environment Research,2009,81(7):687-694
[16]Tan C,Gao N,Chu W,et al.Degradation of diuron by persulfete activated with ferrous ion[J].Separation and Purification Technology,2012,95:44-48
[17]Zhang Y,Xie X,Huang W,et al.Degradation of aniline by Fe~(2+)-activated pereulface oxidation at ambient temperature[J].Joumal of Central South University,2013,20:1010-1014
[18]Liang C,Lai M C.Trichloroethylene degradation by zero valent iron activated persulfate oxidation[J].Environmental Engineering Science,2008,25(7):1071-1078
[19]Hussain I,Zhang Y,Huang S,et al.Degradation of p-chloroaniline by persulfate activated with zero-valent iron[J].Chemical Engineering Journal,2012,203:269-276
[20]Kang S,Liu S,Wang H,Cai W.Enhanced degradation performances of plate-likemicro/nanostructured zero valent iron to DDT[J].Journal of Hazardous Materials,2016,307:145-153
[21]魏海江,杨兴伦,叶茂,等.活化过硫酸钠氧化法修复DDTs污染场地土壤研究[J].土壤,2014,46(3):504-511
[22]Zhu C Y,Fang G D,Dionysiou D D,et al.Efficient transformation of DDTs with persulfate activation by zero-valent iron nanoparticles:A Mechanistic study[J].Journal of Hazardous Materials,2016,316:232-241
[23]Wolcott A R,Shin Y O,Chodan J J.Adsorption of DDT by soils,soil fractions,and biological materials[J].Journal of Agricultural and Food Chemistry,1970,18(6):1129-1133
[24]刘衡锡,张乃东,朱正江.硫酸自由基在水处理中的反应特性[J].科学通报,2012,36:3493-3499
[25]朱长银,方国东,司友斌,等.洗脱-过硫酸钠氧化联合去除土壤中PCBs的研究[J].土壤,2015,47(6):1125-1131