表面活性剂淋溶-化学氧化处理焦化场地高环多环芳烃污染土壤

李伟; 王华伟; 孟祥宇; 杨乐巍; 丁浩然; 李书鹏; 刘渊文; 孙英杰; 刘鹏; 王亚楠

PDF(1358 KB)

中国环境科学 ›› 2023, Vol. 43 ›› Issue (12) : 6474-6481.

土壤污染与控制

表面活性剂淋溶-化学氧化处理焦化场地高环多环芳烃污染土壤

李伟¹, 王华伟¹, 孟祥宇¹, 杨乐巍^2,3, 丁浩然^2,3, 李书鹏^2,3, 刘渊文^2,3, 孙英杰¹, 刘鹏^2,3, 王亚楠¹

作者信息 +

Research on the efficiency of surfactant leaching coupled with chemical oxidation on high rings polycyclic aromatic hydrocarbons removal from coking contaminated soil

Li Wei¹, Wang Hua-wei¹, Meng Xiang-yu¹, Yang Yue-wei^2,3, DING Hao-ran^2,3, Li Shu-peng^2,3, Liu Yuan-wen^2,3, Sun Ying-jie¹, Liu Peng^2,3, Wang Ya-nan¹

Author information +

文章历史 +

摘要

为了探究表面活性剂淋溶-化学氧化技术对焦化场地有机污染土壤的修复效能,以安徽某焦化场地多环芳烃(PAHs)污染土壤为实验对象,分析了表面活性剂浓度、液固比、淋溶时间和淋溶次数等工艺参数对淋溶效果的影响,在优化工艺参数的基础上,进一步研究了化学氧化对PAHs的去除效能.结果表明:1)吐温80(TW80)对PAHs污染土壤的淋溶效果优于曲拉通和鼠李糖脂,用于后续实验; 2)当TW80浓度为6g/L,液固比为10:1,淋溶时间为4h时为最佳工艺参数,此时ΣPAHs的淋溶效率为43.5%; 3)多次淋溶有助于提高PAHs的淋溶效率,连续淋溶3次后ΣPAHs的淋溶效率为63.3%,淋溶5次时淋溶率升高至72.1%; 4)TW80淋溶5次,采用10%的H₂O₂氧化处理后ΣPAHs去除率为79.4%,而采用10% KMnO₄氧化处理后ΣPAHs去除率为81.2%,其中苯并[a]芘去除率为98.3%;5) TW80淋溶处理后,H₂O₂或KMnO₄氧化处理均能提高PAHs的去除效率,淋溶5次+1% H₂O₂和淋溶3次+1% KMnO₄处理后苯并[a]芘含量分别为0.39和0.46mg/kg,均满足《土壤环境质量建设用地土壤污染风险管控标准(试行)》(GB 36600-2018) 第一类用地筛选值要求; 6)表面活性剂淋溶+化学氧化技术对PAHs去除效果良好,该技术在PAHs污染土壤修复具有潜在的应用前景.

Abstract

In order to explore the remediation efficiency of surfactant leaching combined with chemical oxidation technology on the treatment of organic polluted soil in coking sites, the polycyclic aromatic hydrocarbons (PAHs) contaminated soil in a coking site in Anhui Province was taken as the experimental object, and the effect of process parameters such as surfactant concentration, liquid-solid ratio, leaching time and number of leaching on the leaching efficiency was analyzed. On the basis of optimizing the process parameters, the efficiency of chemical oxidation on the removal of PAHs was further investigated. The results showed that: 1) Tween 80 (TW80) was more effective than Triton and rhamnolipid in leaching PAHs from soil, which was used for subsequent experiments; 2) The removal efficiency of ΣPAHs was 43.5% when the concentration of TW80was 6g/L, the liquid-solid ratio was 10:1and the leaching time was 4h; 3) Multiple leaching was helpful for improving the leaching efficiency of PAHs, and the leaching efficiencies of ΣPAHs were 63.3% and 72.1% after three and five times leaching, respectively; 4) The removal efficiency of ΣPAHs increased to 79.4% after TW80 leaching five times combined with the oxidation of 10% H₂O₂, while the ΣPAHs removal efficiency increased to 81.2% after oxidation treatment with 10% KMnO₄, in which the benzo[a]pyrene removal efficiency was 98.3%; 5) After TW80 leaching treatment, the combination of H₂O₂ or KMnO₄ oxidation treatment can improve the removal efficiency of PAHs, the content of benzo[a]pyrene was 0.39mg/kg and 0.46mg/kg after five times leaching combined with 1% H₂O₂ and three times leaching combined with 1% KMnO₄, respectively, which can met the screening value requirement of soil environmental quality risk control standard for soil contamination of development land (GB36600-2018); 6) The combination of surfactant leaching with chemical oxidation technology has a good efficiency on PAHs removal. This technology has a potential application prospect on the remediation of PAHs contaminated soil.

导出引用

李伟, 王华伟, 孟祥宇, 杨乐巍, 丁浩然, 李书鹏, 刘渊文, 孙英杰, 刘鹏, 王亚楠. 表面活性剂淋溶-化学氧化处理焦化场地高环多环芳烃污染土壤[J]. 中国环境科学. 2023, 43(12): 6474-6481

Li Wei, Wang Hua-wei, Meng Xiang-yu, Yang Yue-wei, DING Hao-ran, Li Shu-peng, Liu Yuan-wen, Sun Ying-jie, Liu Peng, Wang Ya-nan. Research on the efficiency of surfactant leaching coupled with chemical oxidation on high rings polycyclic aromatic hydrocarbons removal from coking contaminated soil[J]. China Environmental Science. 2023, 43(12): 6474-6481

中图分类号： X53

参考文献

[1] Zhang F Y, Yang L, Sheng Z Y, et al. Physicochemical characteristics of polycyclic aromatic hydrocarbons in condensable particulate matter from coal-fired power plants: A laboratory simulation[J]. Environmental Pollution, 2022,318:120944.
[2] 代朝猛,童汪凯,胡佳俊,等.开关表面活性剂对土壤及地下水中多环芳烃污染的增效修复研究进展[J]. 环境科学研究, 2022,35(8): 1925-1934. Dai Z M, Tong W K, Hu J J, et al. Switchable surfactant-enhanced remediation of polycyclic aromatic hydrocarbons in soil and groundwater: A review[J]. Research of Environmental Sciences, 2022, 35(8):1925-1934.
[3] Xie B X, Qin J H, Sun H, et al. Release characteristics of polycyclic aromatic hydrocarbons (PAHs) leaching from oil-based drilling cuttings[J]. Chemosphere, 2021,291:132711.
[4] Mojiri A, Zhou J L, Ohashi A, et al. Comprehensive review of polycyclic aromatic hydrocarbons in water sources, their effects and treatments[J]. Science of the Total Environment, 2019,696:133971.
[5] 孟祥帅,陈鸿汉,郑从奇,等.焦化厂不同污染源作用下土壤PAHs污染特征[J]. 中国环境科学, 2020,40(11):4857-4864. Meng X S, Chen H H, Zheng C Q, et al. Pollution characteristics of PAHs in soil at an abandoned coking plant affected by different sources. China Environmental Science, 2020,40(11):4857-4864.
[6] 张灿灿,郭书海,李婷婷,等.焦化厂高环PAHs污染土壤的电动-微生物修复[J]. 环境工程, 2014,32(7):150-154. Zhang C C, Guo S H, Li T T, et al. Electric microbial remediation of high environmental PAHs contaminated soil in coking plants[J]. Environmental Engineering, 2014,32(7):150-154.
[7] 陈倩,蔡武,陈杰,等.不同化学氧化剂对土壤中多环芳烃的降解效果[J]. 浙江大学学报(工学版), 2019,53(12):2437-2444. Chen Q, Cai W, Chen J, et al. Degradation effects of different chemical oxidants on polycyclic aromatic hydrocarbons in soil. Journal of ZheJiang University (Engineering Science), 2019,53(12):2437-2444.
[8] Zhang W H, Wei C, Feng C, et al. Distribution and health-risk of polycyclic aromatic hydrocarbons in soils at a coking plant[J]. Journal of Environmental Monitoring, 2011,13(12):3429-3436.
[9] Han C, Zhang Y, Redmile-Gordon M, et al. Organic and inorganic model soil fractions instigate the formation of distinct microbial biofilms for enhanced biodegradation of benzo[a] pyrene[J]. Journal of Hazardous Materials, 2021,404:124071.
[10] Gou Y L, Ma J S, Yang S C, et al. Insights into the effects of Fenton oxidation on PAH removal and indigenous bacteria in aged subsurface soil[J]. Environmental Pollution, 2022,298:118872.
[11] Liao X Y, Wu Z Y, Li Y, et al. Effect of various chemical oxidation reagents on soil indigenous microbial diversity in remediation of soil contaminated by PAHs[J]. Chemosphere, 2019,226:483-491.
[12] Patel A B, Shaikh S, Jain K R, et al. Polycyclic aromatic hydrocarbons: sources, toxicity, and remediation approaches[J]. Frontiers in Microbiology, 2020,11:562813.
[13] Liu J F, Wang Y R, Li H F. Synergistic solubilization of phenanthrene by mixed micelles composed of biosurfactants and a conventional non-ionic surfactant[J]. Molecules, 2020,25(18):4327.
[14] 王永剑,单广波,徐佰青,等.表面活性剂在石油烃污染土壤修复中的应用研究进展[J]. 当代化工, 2021,50(6):1425-1430. Wang Y J, Shan G B, Xu B Q, et al. Research progress on the application of surfactants in the remediation of petroleum hydrocarbon contaminated soil[J]. Contemporary Chemical Industry, 2021,50(6): 1425-1430.
[15] 可欣,周燕,张飞杰,等.污染场地修复药剂安全利用问题及对策[J]. 环境科学研究, 2021,34(6):1473-1481. Ke X, Zhou Y, Zhang F J, et al. Problems and strategies of safe utilization of agents for contaminated sites[J]. Research of Environmental Sciences, 2021,34(6):1473-1481.
[16] 王忠旺,韩玮,陈雨龙,等.表面活性剂对焦化污染土壤中多环芳烃淋溶修复研究[J]. 环境污染与防治, 2020,42(6):690-695. Wang Z W, Han W, Chen Y L, et al. Study on the leaching and remediation of polycyclic aromatic hydrocarbons in coking contaminated soil by surfactants[J]. Environmental Pollution and Prevention, 2020,42(6):690-695.
[17] Wei W, Ran Z X, He H, et al. Desorption process and morphological analysis of real polycyclic aromatic hydrocarbons contaminated soil by the heterogemini surfactant and its mixed systems[J]. Chemosphere, 2020,254:126854.
[18] 吉红军,龙涛,陈墙,等.Tween 80强化-活化过硫酸钠氧化修复多环芳烃污染土壤[J]. 化工学报, 2016,67(9):3879-3887. Ji H J, Long T, Chen Q, Yue HE, et al. Tween 80 enhanced-activated sodium persulfate oxidation of PAHs contaminated soil[J]. CIESC Journal, 2016,67(9):3879-3887.
[19] 勾立争,刘长波,刘诗诚,等.热脱附法修复多环芳烃和汞复合污染土壤实验研究[J]. 环境工程, 2018,36(2):184-187,146. Gou L Z, Liu C B, Liu S C, et al. Experimental study on the remediation of polycyclic aromatic hydrocarbons and mercury contaminated soil by thermal desorption method[J]. Environmental Engineering, 2018,36(2):184-187,146.
[20] Wei M, Xia T X, He Y. Remediation of polycyclic aromatic hydrocarbons by thermal desorption from a coking plant soil: effects of vacuum-enhanced and alkali-assisted on removal efficiencies[J]. Environmental Engineering Science, 2022,39(1):48-55.
[21] 赵涛,马刚平,周宇,等.多环芳烃类污染土壤热脱附修复技术应用研究[J]. 环境工程, 2017,35(11):178-181. Zhao T, Ma G P, Zhou Y, et al. Application of thermal desorption remediation technology for polycyclic aromatic hydrocarbon polluted soil[J]. Environmental Engineering, 2017,35(11):178-181.
[22] Gou Y L, Song Y, Yang S C, et al. Low-temperature thermal- enhanced anoxic biodegradation of polycyclic aromatic hydrocarbons in aged subsurface soil[J]. Chemical Engineering Journal, 2023,454: 140143.
[23] Wei K H, Ma J, Xi B D, et al. Recent progress on in-situ chemical oxidation for the remediation of petroleum contaminated soil and groundwater[J]. Journal of Hazardous Materials, 2022,432:128738.
[24] 廖用开,刘爽,钟雅琪,等.高锰酸钾修复PAHs污染土壤过程中Mn迁移转化规律[J]. 环境工程学报, 2022,16(10):3374-3380. Liao Y K, Liu S, Zhong Y Q, et al. Migration and transformation of Mn during remediation process of soil contaminated with PAHs by potassium permanganate oxidation[J]. Journal of Environmental Engineering, 2022,16(10):3374-3380.
[25] Derudi M, Venturini G, Lombardi G, et al. Biodegradation combined with ozone for the remediation of contaminated soils[J]. European Journal of Soil Biology, 2007,43(5/6):297-303.
[26] Gou Y L, Zhao Q Y, Yang S C, et al. Enhanced degradation of polycyclic aromatic hydrocarbons in aged subsurface soil using integrated persulfate oxidation and anoxic biodegradation[J]. Chemical Engineering Journal, 2020,394:125040.
[27] GB 36600-2018土壤环境质量建设用地土壤污染风险管控标准(试行)[S]. GB 36600-2018 Soil environmental quality standard for soil pollution risk control of construction land (Trial)[S].
[28] 肖锟,刘聪洋,王仁女,等.表面活性剂影响微生物降解多环芳烃的研究进展[J]. 微生物学通报, 2021,48(2):582-595. Xiao K, Liu C Y, Wang R N, et al. Research progress on the effect of surfactants on microbial degradation of polycyclic aromatic hydrocarbons[J]. Microbiology Bulletin, 2021,48(2):582-595.
[29] 袁笑,相雷雷,赵振华,等.表面活性剂增溶洗脱土壤中多环芳烃的效果研究[J]. 环境科学研究, 2022,35(8):1885-1892. Yuan X, Xiang L L, Zhao Z H, et al. Surfactant-enhanced solubilization and elution of polycyclic aromatic hydrocarbons in soil[J]. Research of Environmental Sciences, 2022,35(8):1885-1892.
[30] HJ 761-2015固体废物有机质的测定灼烧减量法[S]. HJ 761-2015 Determination of organic matter in solid waste by ignition reduction method[S].
[31] Li S, Pi Y, Bao M, et al. Effect of rhamnolipid biosurfactant on solubilization of polycyclic aromatic hydrocarbons[J]. Marine Pollution Bulletin, 2015,101(1):219-225.
[32] 李看看,吴娟,马东,等.表面活性剂对土壤中多环芳烃(PAHs)纵向迁移的影响[J]. 环境化学, 2018,37(7):1545-1553. Li K K, Wu J, Ma D, et al. Effects of surfactant on longitudinal migration of polycyclic aromatic hydrocarbons in soil[J]. Environmental Chemistry, 2018,37(7):1545-1553.
[33] 伍剑博.烷基糖苷在土壤上的吸附及应用研究[D]. 海口:海南大学, 2016. Wu J B. Study on the adsorption and application of alkyl glycosides on soil[D] Haikou: Hainan University, 2016.
[34] 金柱,张军,周媛,等.烷基糖苷柠檬酸单酯盐水溶液表面张力研究[J]. 应用化工, 2016,45(9):1614-1618. Jin Z, Zhang J, Zhou Y, et al. Study on the surface tension of alkyl glucoside citrate monoester saline solution[J]. Applied Chemistry, 2016,45(9):1614-1618.
[35] Edwards, D A., Luthy, R G., Liu, Z B. Solubilization of polycyclic aromatic hydrocarbons in micellar nonionic surfactant solutions[J]. Environmental Science & Technology, 1991,25(1):127-133.
[36] 肖鹏飞,王剑桥.Tween系列表面活性剂对东北黑土中多环芳烃的淋溶[J]. 水土保持学报, 2013,27(5):267-272. Xiao P F, Wang J Q. The leaching of polycyclic aromatic hydrocarbons in Northeast black soil by Tween series surfactants[J]. Journal of Soil and Water Conservation, 2013,27(5):267-272.
[37] Rathankumar A K, Saikia K K, Kumar P S, et al. Surfactant-aided mycoremediation of soil contaminated with polycyclic aromatic hydrocarbon (PAHs): progress, limitation, and countermeasures[J]. Journal of Chemical Technology & Biotechnology, 2022,97(2):391-408.
[38] Zeng G L, Yang R M, Fu X T, et al. Naphthalene degradation in aqueous solution by Fe(II) activated persulfate coupled with citric acid[J]. Separation and Purification Technology, 2021,264:118441.
[39] 李爽,胡晓钧,李玉双,等.表面活性剂对多环芳烃的淋溶修复[J]. 环境工程学报, 2017,11(3):1899-1905. Li S, Hu X J, Li Y S, et al. Washing remediation of PAHs with surfactants[J]. Journal of Environmental Engineering, 2017,11(3): 1899-1905.
[40] 钟金魁,赵保卫,朱琨,等.表面活性剂对菲的增溶动力学及质量增溶比(WSR)与亲水亲油平衡值(HLB)的关系[J]. 环境化学, 2011, 30(10):1737-1742. Zhong J K, Zhao B W, Zhu K, et al. Solubilization kinetics of surfactants on phenanthrene and the relationship between mass solubilization ratio (WSR) and hydrophilic lipophilic equilibrium value (HLB)[J]. Environmental Chemistry, 2011,30(10):1737-1742.
[41] Gou Y L, Yang S C, Cheng Y J, et al. Enhanced anoxic biodegradation of polycyclic aromatic hydrocarbons (PAHs) in aged soil pretreated by hydrogen peroxide[J]. Chemical Engineering Journal, 2019,356:524-533.
[42] Li Y, Liao X Y, Huling S G. et al. The combined effects of surfactant solubilization and chemical oxidation on the removal of polycyclic aromatic hydrocarbon from soil[J]. Science of the Total Environment, 2019,647:1106-1112.
[43] Liao X Y, Wu Z Y, Li Y, et al. Effect of various chemlical oxidation reagents on soil indigenous microbial diversity in remediation of soil contaminated by PAHs[J]. Chemosphere, 2019,226:438-491.