优化过硫酸盐体系处理石油类污染土壤
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摘要
以提高过硫酸盐体系处理效果为目标,研究了活化剂(FeSO_4、CuSO_4、Fe_3O_4)、络合剂(柠檬酸,CA)和沙粒对实际污染土壤中石油类污染物(TPH)处理效果的影响。结果表明:当n(活化剂)∶n(氧化剂)=1∶1,反应时间为48 h,初始pH为4,水∶土=2∶1(以质量比计),温度为20℃时,3种活化剂对TPH去除效果依次为FeSO_4>CuSO_4>Fe_3O_4;当n(过硫酸钠)∶n(硫酸亚铁)∶n(柠檬酸)为4∶1∶1时,柠檬酸的添加使污染土壤中TPH去除率提高了9.82%;在Na_2S_2O_8/FeSO_4、Na_2S_2O_8/FeSO_4/CA体系中添加沙粒(土壤∶沙粒=5∶1)(以质量比计)后,TPH的去除率分别提高了1.8%和3.8%。利用过硫酸钠进行化学氧化修复石油污染土壤,以Fe~(2+)作为活化剂,同时添加沙粒时TPH去除效果较好,且土壤不会过度酸化。研究结果可为开展石油污染土壤的原位化学氧化修复技术提供参考。
Persulfate is a common oxidant used in in-situ chemical oxidation remediation(ISCO) for petroleum-contaminated soil, and with improving the efficiency of persulfate oxidation as the objective, the effects of activating agents(FeSO_4, CuSO_4, Fe_3O_4), chelating agents(citric acid, CA) and sand addition on the removal efficiency of total petroleum hydrocabons(TPH) in an actually contaminated soil were studied. The results showed that the removal efficiency of the three activating agents were in the order of FeSO_4>CuSO_4>Fe_3O_4, when activating agent∶oxidant=1∶1, reaction time was 48 h, initial pH was 4, n(water)∶n(soil)=2∶1, and temperature was 20 ℃; when the ratio of sodium persulfate/ferrous sulfate/citric acid was 4∶1∶1, the TPH removal rate in contaminated soil was increased by 9.82% with addition of citric acid; the addition of sand(n(soil)∶n(grain)=5∶1) in the Na_2S_2O_8/FeSO_4 and Na_2S_2O_8/FeSO_4/CA systems increased the TPH removal efficiency by 1.8% and 3.8%, respectively. When using sodium persulfate for chemical oxidation remediation of petroleum-contaminated soil, if taking Fe~(2+) as the activator and adding sand, better TPH removal efficiency could be achieved without causing excessive acidation. The research results would provide basic data for carrying out ISCO for petroleum-contaminated soil.
Persulfate is a common oxidant used in in-situ chemical oxidation remediation(ISCO) for petroleum-contaminated soil, and with improving the efficiency of persulfate oxidation as the objective, the effects of activating agents(FeSO_4, CuSO_4, Fe_3O_4), chelating agents(citric acid, CA) and sand addition on the removal efficiency of total petroleum hydrocabons(TPH) in an actually contaminated soil were studied. The results showed that the removal efficiency of the three activating agents were in the order of FeSO_4>CuSO_4>Fe_3O_4, when activating agent∶oxidant=1∶1, reaction time was 48 h, initial pH was 4, n(water)∶n(soil)=2∶1, and temperature was 20 ℃; when the ratio of sodium persulfate/ferrous sulfate/citric acid was 4∶1∶1, the TPH removal rate in contaminated soil was increased by 9.82% with addition of citric acid; the addition of sand(n(soil)∶n(grain)=5∶1) in the Na_2S_2O_8/FeSO_4 and Na_2S_2O_8/FeSO_4/CA systems increased the TPH removal efficiency by 1.8% and 3.8%, respectively. When using sodium persulfate for chemical oxidation remediation of petroleum-contaminated soil, if taking Fe~(2+) as the activator and adding sand, better TPH removal efficiency could be achieved without causing excessive acidation. The research results would provide basic data for carrying out ISCO for petroleum-contaminated soil.
引文
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[18] 孙威,刘春婷,李娜.金属离子在过硫酸盐降解甲基橙染料废水中活化作用的比较分析[J].辽宁化工,2014,43(11):1373-1375.
[19] 张宏玲,李森,张杨,等.过渡金属离子活化过硫酸盐去除土壤中的芘[J].环境工程学报,2016,10(10):6010-6014.
[20] Haizhou L, Bruton T A, Doyle F M, et al. In situ chemical oxidation of contaminated groundwater by persulfate: decomposition by Fe(Ⅲ)-and Mn(Ⅳ)-containing oxides and aquifer materials[J].Environmental Science & Technology,2014,48(17):10330-10336.
[2] 韩妮.新疆石油污染土壤修复技术研究[D].乌鲁木齐: 新疆农业大学, 2014.
[3] 胡迪,李川,董倩倩,等.油田区土壤石油烃组分残留特性研究[J].环境科学, 2014, 35(1): 227-232.
[4] Li X, Wang X, Ren Z J, et al. Sand amendment enhances bioelectrochemical remediation of petroleum hydrocarbon contaminated soil[J]. Chemosphere, 2015, 141: 62-70.
[5] 刘五星,骆永明,王殿玺.石油污染场地土壤修复技术及工程化应用[J].环境监测管理与技术,2011,23(3):47-51.
[6] 李政,顾贵州,宁春莹,等.固体微生物菌剂在克拉玛依石油污染土壤生物修复中的应用[J]. 石油学报(石油加工),2016,32(6):1195-1204.
[7] 苏增建,李敏,王颖.土壤石油污染的生物修复原理及研究进展[J].安徽农业科学,2007,35(6):1742-1744.
[8] 李佳,曹兴涛,隋红,等.石油污染土壤修复技术研究现状与展望[J].石油学报(石油加工),2017,33(5):812-833.
[9] Watts R J, Teel A L. Treatment of contaminated soils and groundwater using in situ chemical oxidation[J]. Haz Waste Manag,2006,10 (1): 2-9.
[10] 吴昊,孙丽娜,王辉,等.活化过硫酸钠原位修复石油类污染土壤研究进展[J].环境化学,2015,34(11): 2085-2095.
[11] 吴昊.大连某TPH污染场地原位强化过硫酸钠修复技术研究[D].沈阳:沈阳大学,2017.
[12] 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.
[13] Pardo F, Rosas J M, Santos A, et al. Remediation of a biodiesel blend-contaminated soil by using a modified Fenton process[J]. Environmental Science and Pollution Research, 2014, 21(21): 12198-12207.
[14] 土壤石油类的测定红外光度法(征求意见稿)[S].中华人民共和国国家环境保护标准.
[15] 杨焱明,冷艳秋,林欣,等.Fe3O4/石墨烯活化过硫酸盐降解罗丹明B废水的研究[J].环境科学与管理,2014,39(4):80-84.
[16] 晏井春.含铁化合物活化过硫酸盐及其在有机污染修复中的应用[D].武汉:华中科技大学,2012.
[17] 吴昊,孙丽娜,李玉双,等.活化过硫酸钠去除长期污染土壤中的TPH[J].环境工程学报,2016,10(9):5232-5237.
[18] 孙威,刘春婷,李娜.金属离子在过硫酸盐降解甲基橙染料废水中活化作用的比较分析[J].辽宁化工,2014,43(11):1373-1375.
[19] 张宏玲,李森,张杨,等.过渡金属离子活化过硫酸盐去除土壤中的芘[J].环境工程学报,2016,10(10):6010-6014.
[20] Haizhou L, Bruton T A, Doyle F M, et al. In situ chemical oxidation of contaminated groundwater by persulfate: decomposition by Fe(Ⅲ)-and Mn(Ⅳ)-containing oxides and aquifer materials[J].Environmental Science & Technology,2014,48(17):10330-10336.