优化SO4-·高级氧化技术修复PAHs复合污染土壤

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摘要

采用硫酸根自由基高级氧化技术（SR-AOPs）修复南京某炼钢厂附近PAHs复合土壤，通过调整过硫酸钠（Na2S2O8）和亚铁离子（Fe²⁺）比例，结合添加不同种类和浓度的螯合剂和表面活性剂，获得修复的最佳条件，并比较分析不同类型PAHs的降解特征.结果表明：Na₂S₂O₈和Fe²⁺的配比显著影响土壤PAHs的降解效果，当Na₂S₂O₈用量为5mmol/g，Fe²⁺用量为0.5mmol/g，二者比例为10：1时，培养24h，PAHs总去除率最高，为29.32%；在此基础上添加螯合剂柠檬酸0.5mmol/g时，PAHs总去除率可提高至49.9%；继续添加0.27mg/g表面活性剂IGEPAL CA-720，PAHs总去除率最大，为80.8%.分析不同条件下SR-AOPs对PAHs的降解效果，得到总体上SR-AOPs对四环PAHs去除效果最好.添加柠檬酸和IGEPAL CA-720可以进一步强化对土壤中3环、6环PAHs的去除.柠檬酸和IGEPAL CA-720的添加可以更有效去除污染土壤中PAHs，尤其是针对高环PAHs.

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	徐源洲
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	李辉信
	胡锋
	徐莉

关键词 ：硫酸根自由基, 多环芳烃, 污染场地, 降解效率, 修复

Abstract：

Sulfate radical-based advanced oxidation processes (SR-AOPs)was used to remediate PAHs contaminated soils near a steel mill in Nanjing. The ratio of sodium persulfate (Na₂S₂O₈) and ferrous ion (Fe²⁺) used in the SR-AOPs was adjusted, combined with various types and concentrations of chelating agents and surfactants, to reach the best PAHs removal efficiency. Meanwhile, the degradation characteristics of different types of PAHs were analyzed. The results showed that the ratio of Na₂S₂O₈ and Fe²⁺ significantly influenced the PAHs degradation efficiencies. The highest removal rate of PAHs was 29.32% at the condition of 24hours incubation when the ratio of Na₂S₂O₈ and Fe²⁺ was 10:1, i.e. the dose of Na₂S₂O₈ was 5mmol/g and the Fe²⁺ dosage was 0.5mmol/g. Base on this, 0.5mmol/g citric acid was added as the best chelating agent which could further improve the PAHs removal rate to 49.9%. In addition, 0.27mg/g surfactant IGEPAL CA-720 could also increase the PAHs removal rate to 80.8%. In general, the tetracyclic PAHs showed the highest removal rate by SR-AOPs. The addition of citric acid and IGEPAL CA-720 could further promote the removal of tricyclic PAHs and pentacyclic PAHs in soil. In conclusion, the citric acid and IGEPAL CA-720 addition could help to facilitate the removal of PAHs in soils, especially for the high-ring PAHs.

Key words： sulfate free radical PAHs contaminated site degradation efficiency remediation

收稿日期: 2019-08-29

PACS:

X53

基金资助:

中央高校基本科研业务费专项资金资助项目（KYZ201626）；国家自然科学基金资助项目（41101292）

通讯作者: 徐莉,教授,xuli602@njau.edu.cn E-mail: xuli602@njau.edu.cn

作者简介: 徐源洲(1993-),男,山东潍坊人,南京农业大学博士研究生,从事土壤污染修复研究.发表论文2篇.

引用本文:

徐源洲, 张力浩, 方成, 代子文, 魏志敏, 李辉信, 胡锋, 徐莉. 优化SO₄^-_·高级氧化技术修复PAHs复合污染土壤[J]. 中国环境科学, 2020, 40(3): 1183-1190. XU Yuan-zhou, ZHANG Li-hao, FANG Cheng, DAI Zi-wen, WEI Zhi-min, LI Hui-xin, HU Feng, XU Li. Optimization of sulfate radical advanced oxidation technology on PAHs remediation in contaminated sites. CHINA ENVIRONMENTAL SCIENCECE, 2020, 40(3): 1183-1190.

链接本文:

http://www.zghjkx.com.cn/CN/ 或 http://www.zghjkx.com.cn/CN/Y2020/V40/I3/1183

[1]	Rivas F J. Polycyclic aromatic hydrocarbons sorbed on soils:A short review of chemical oxidation based treatments[J]. Journal of Hazardous Materials, 2006,138(2):234-251.
[2]	Rajpara R K, Dudhagara D R, Bhatt J K, et al. Polycyclic aromatic hydrocarbons (PAHs) at the Gulf of Kutch, Gujarat, India:Occurrence, source apportionment, and toxicity of PAHs as an emerging issue[J]. Marine Pollution Bulletin, 2017,119(2):231.
[3]	刘瑞民,王学军,陶澍,等.天津表层土壤PAHs分子标志物参数的空间特征[J]. 中国环境科学, 2004,(6):45-48. Liu R M, Wang X J, Tao P, et al. Spatial characteristics of PAHs molecular marker indices in surface soil of Tianjin[J]. China Environmental Science, 2004,(6):45-48.
[4]	Mastral A M, Callén, María S. A Review on Polycyclic Aromatic Hydrocarbon (PAH) Emissions from Energy Generation[J]. Environmental Science & Technology, 2000,34(15):3051-3057.
[5]	曹文文,张振江,赵若杰,等.室内空气PM10中PAHs对老年人的致癌风险评价——以天津市某社区为例[J]. 中国环境科学, 2013, 33(2):345-350. Cao W W, Zhang Z J, Zhao R J, et al. The cancer risk assessment of the elderly population exposure to PAHs in PM10 indoor air——Case study of one community in Tianjin, China[J]. China Environmental Science, 2013,33(2):345-350.
[6]	Li J, Dong H, Zhang D, et al. Sources and ecological risk assessment of PAHs in surface sediments from Bohai Sea and northern part of the Yellow Sea, China[J]. Marine Pollution Bulletin, 2015,96(1/2):485-490.
[7]	徐文迪,郭书海,李刚,等.电芬顿-生物泥浆法联合修复芘污染土壤[J]. 中国环境科学, 2019,39(10):4247-4253. Xu W D, Guo S H, Li G, et al. Remediation of pyrene-contaminated soil by a combined process with electro-Fenton and bioremediation[J]. China Environmental Science, 2019,39(10):4247-4253.
[8]	Jonsson S, Persson Y, Frankki S, et al. Degradation of polycyclic aromatic hydrocarbons (PAHs) in contaminated soils by Fenton's reagent:A multivariate evaluation of the importance of soil characteristics and PAH properties[J]. Journal of Hazardous Materials, 2007,149(1):86-96.
[9]	Glaze W H, Kang J W, Chapin D H. The Chemistry of Water Treatment Processes Involving Ozone, Hydrogen Peroxide and Ultraviolet Radiation[J]. Ozone Science & Engineering, 1987,9(4):335-352.
[10]	And A M M, Callén M S. A Review on Polycyclic Aromatic Hydrocarbon (PAH) Emissions from Energy Generation[J]. Environmental Science & Technology, 2000,34(15):66.
[11]	纪录,张晖.原位化学氧化法在土壤和地下水修复中的研究进展[J]. 环境工程学报, 2003,4(6):37-42. Ji L, Zhang H. The progress in soil and groundwater remediation by in situ chemical oxidation[J]. Techniques and Equipment for Environmental Pollution Control, 2003,4(6):37-42.
[12]	占升,郑义,李森,等.不同氧化剂活化过硫酸钠对土壤中多环芳烃降解的影响[J]. 浙江农业学报, 2017,29(1):129-136. Zhang S, Zheng Y, Li S, et al. Degradation of PAHs in soil by different oxidants activated sodium persulfate[J]. Acta Agriculturae Zhejiangensis, 2017,29(1):129-136.
[13]	Dan Z, Liao X, Yan X, et al. Effect and mechanism of persulfate activated by different methods for PAHs removal in soil[J]. Journal of Hazardous Materials, 2013,254-255(254):228-235.
[14]	张海欧,郭书海,李凤梅,等.焦化场地PAHs污染土壤的电动-化学氧化联合修复[J]. 农业环境科学学报, 2014,33(10):1904-1911. Zhang H O, Guo S H, Li F M, et al. Remediation of PAHs contaminated soil at coking site by integrated electrokinetics and chemical oxidation[J]. Journal of Agro-Environment Science, 2014,33(10):1904-1911.
[15]	张成,万金泉,马邕文,等.pH及络合剂对亚铁活化S2O82-氧化去除活性艳蓝的影响研究[J]. 环境科学, 2012,33(3):871-878. Zhang C, Wan J Q, Ma Y W, et al. Influences of pH and complexing agents on degradation of reactive brilliant blue KN-R by ferrous activated persulfate[J]. Environmental Science, 2012,33(3):871-878.
[16]	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, et al. Tween 80 enhanced-activated sodium persulfate oxidation of PAHs contaminated soil[J]. CIESC Journal, 2016,67(9):3879-3887.
[17]	高彦征,朱利中,凌婉婷,等.土壤和植物样品的多环芳烃分析方法研究[J]. 农业环境科学学报, 2005,24(5):1003-1006. Gao Y Z, Zhu L Z, Ling W T, et al. Analysis method for polycyclic aromatic hydrocarbons (PAHs) in plant and soil samples[J]. Journal of Agro-Environment Science, 2005,24(5):1003-1006.
[18]	付文怡.多环芳烃污染土壤的化学氧化修复及微生物群落多样性研究[D]. 上海:华东师范大学, 2018. Fu W Y. Chemical Oxidation remediation and microbial community research of PAHs contaminated soil[D]. Shanghai:East China Normal University, 2018.
[19]	Ling W T, Zeng Y C, Gao Y Z, et al. Availability of polycyclic aromatic hydrocarbons in aging soils.[J]. Journal of Soils & Sediments Jss, 2010,10(5):799-807.
[20]	Ranc B, Faure P, Croze V, et al. Selection of oxidant doses for in situ chemical oxidation of soils contaminated by polycyclic aromatic hydrocarbons (PAHs):A review[J]. Journal of Hazardous Materials, 2016,312:280-297.
[21]	赵丹,阎秀兰,廖晓勇,等.不同化学氧化剂对焦化污染场地苯系物的修复效果[J]. 环境科学, 2011,32(3):849-856. Zhao D, Yan X L, Liao X Y, et al. Chemical oxidants for remediation of BTEX-contaminated soils at coking sites[J]. Environmental Science, 2011,32(3):849-856.
[22]	Andreottola G, Ferrarese E. Application of advanced oxidation processes and electrooxidation for the remediation of river sediments contaminated by PAHs[J]. Environmental Letters, 2008,43(12):1361-1372.
[23]	Liao X, Liu Q, Li Y, et al. Removal of polycyclic aromatic hydrocarbons from different soil fractions by persulfate oxidation[J]. Journal of Environmental Sciences, 2019,78(4):241-248.
[24]	Sra K S, Thomson N R, Barker J F. Stability of Activated Persulfate in the Presence of Aquifer Solids[J]. Soil and Sediment Contamination:An International Journal, 2014,23(8):820-837.
[25]	张玉秀,黄智博,柴团耀.螯合剂强化重金属污染土壤植物修复的机制和应用研究进展[J]. 自然科学进展, 2009,19(11):1149-1158. Zhang Y X, Huang Z B, Chai T Y, et al. Mechanism and application of chelators in strengthening phytoremediation of heavy metal contaminated soil[J]. Progress in Natural Science, 2009,19(11):1149-1158.
[26]	Nadim F, Huang K C, Dahmani A M. Remediation of soil and ground water contaminated with PAH using heat and Fe(II)-EDTA catalyzed persulfate oxidation[J]. Water Air & Soil Pollution Focus, 2006,6(1/2):227-232.
[27]	Man X, Ning X A, Zou H, et al. Removal of polycyclic aromatic hydrocarbons (PAHs) from textile dyeing sludge by ultrasound combined zero-valent iron/EDTA/Air system[J]. Chemosphere, 2017, 191:839.
[28]	Shih Y J, Binh N T, Chen C W, et al. Treatability assessment of polycyclic aromatic hydrocarbons contaminated marine sediments using permanganate, persulfate and Fenton oxidation processes[J]. Chemosphere, 2016,150:294-303.
[29]	Ling W, Ren L, Gao Y, et al. Impact of low-molecular-weight organic acids on the availability of phenanthrene and pyrene in soil[J]. Soil Biology & Biochemistry, 2009,41(10):2187-2195.
[30]	Jones D L, Dennis P G, Owen A G, et al. Organic acid behavior in soils-misconceptions and knowledge gaps[J]. Plant and Soil, 2003,248(1/2):31-41.
[31]	聂婧.低分子量有机酸及黑炭对土壤中PAHs形态及结合态残留释放的影响[D]. 南京:南京农业大学, 2015. Nie J. Effect of low-molecular-weight organicacids and black carbon on forms of PAHs and bound-PAH residue release in soils[D]. Nanjing:Nanjing Agriclutural University, 2015.
[32]	魏星媛.水溶液中溶解态多组分多环芳烃(PAHs)的生物降解[D]. 厦门:厦门大学, 2009. Wei X Y. Biodegradation of dissolved multi-component polycyclic aromatic hydrocarbons (PAHs) in aqueous solution[D]. Xiamen:Xiamen University, 2009.
[33]	Bogan B W, Trbovic V. Effect of sequestration on PAH degradability with Fenton's reagent:roles of total organic carbon, humin, and soil porosity[J]. Journal of Hazardous Materials, 2003,100(1-3):285-300.
[34]	蒋兵,赵保卫,赵兰萍,等.阴-非混合表面活性剂对菲和萘的增溶作用[J]. 兰州交通大学学报, 2007,26(1):153-157. Jiang B, Zhao B W, Zhao L P, et al. Water solubility enhancement of phenanthrene and naphthalene by anionic-nonionic surfactant solutions[J]. Journal of Lanzhou Jiaotong University (Natural S ciences), 2007,26(1):153-157.
[35]	Gómez J, Alcántara M T, Pazos M, et al. A two-stage process using electrokinetic remediation and electrochemical degradation for treating benzo[a]pyrene spiked kaolin[J]. Chemosphere, 2009,74(11):1516-1521.
[36]	刘晶蕊.单一和混合表面活性剂对多环芳烃的增溶性研究[D]. 北京:华北电力大学, 2011. Liu J R. Studies on the solubilization of polycyclic aromatic hydrocarbons by single and mixed surfactants[D]. Beijing:Power and Mechanical Engineering, 2011.
[37]	王欢,王瑶,肖鹏飞.非-阴离子表面活性剂对PAHs的增溶作用及无机盐的强化效果研究[J]. 环境科学与管理, 2014,39(10):96-100. Wang H, Wang Y, Xiao P F. Solubilization of PAHs by nonionicanionic surfactants and influence of inorganic salts[J]. Environmental Science and Management, 2014,39(10):96-100.
[38]	孙晓慧,卢瑛莹,陈曙光,等.膨润土对复合污染中表面活性剂的吸附及机理[J]. 环境科学, 2007,28(4):838-842. Sun X H, Lu Y Y, Chen S G, et al. Sorption and mechanism of surfactants on bentonite in combined pollution[J]. Environmental Science, 2007,28(4):838-842.
[39]	陈敏婷.表面活性剂强化PAHs污染土壤微生物修复的研究进展[J]. 广东化工, 2013,40(8):77-78. Chen M T. Surfactant strengthen PAHs contaminated soil microbial repair research progress[J]. Guangdong Chemical Industry, 2013, 40(8):77-78.
[40]	Ferrarese E, Andreottola G, Oprea I A. Remediation of PAHcontaminated sediments by chemical oxidation[J]. Journal of Hazardous Materials, 2008,152(1):128-139.