H2O2、Na2FeO4去除土壤中总石油烃的反应动力学

董万涛; 王亚军; 李丽; 张兴

doi:10.13205/j.hjgc.202110025

H₂O₂、Na₂FeO₄去除土壤中总石油烃的反应动力学

doi: 10.13205/j.hjgc.202110025

董万涛¹,
王亚军^1, ,,
李丽²,
张兴²

1. 兰州理工大学土木工程学院, 兰州 730000;
2. 中铁科学研究院有限公司成都分公司, 成都 610000

基金项目:

中铁科学研究院有限公司重点项目[中铁科研院（科研）字2018-KJ003-Z003-XB]；国家自然科学基金资助项目（41967043）；甘肃省自然科学基金项目（20JR5RA461）；甘肃省高等学校产业支撑引导项目（2020C-40）。

详细信息

作者简介:
董万涛(1988-),男,硕士研究生,主要研究方向为水土污染与修复。d316284531@163.com

通讯作者:
王亚军(1979-),男,博士,副教授,主要研究方向为水土污染与修复。wyj79626@163.com

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出版历程
- 收稿日期: 2020-08-24
- 网络出版日期: 2022-01-26

REACTION KINETICS STUDY ON H₂O₂ AND Na₂FeO₄ REMOVING TOTAL PETROLEUM HYDROCARBON FROM SOIL

1. School of Civil Engineering, Lanzhou University of Technology, Lanzhou 730000, China;
2. Chengdu Branch of China Railway Research Institute Co., Ltd, Chengdu 610000, China

摘要

摘要: 利用H₂O₂、Na₂FeO₄ 2种氧化剂对土壤中TPH进行去除实验，根据反应条件和反应速率的关系建立反应动力学模型，并对反应过程中反应速率变化、半衰期、TPH去除率等因素进行讨论和对比，寻找其反应规律。结果表明：H₂O₂去除TPH过程符合一级反应动力学模型。Na₂FeO₄去除TPH过程符合二级反应动力学模型，H₂O₂浓度增大导致反应动力学常数增加，Na₂FeO₄浓度增大导致反应动力学常数减小。采用0.078，0.156，0.234 mol/L 3种浓度H₂O₂溶液与TPH的初始反应速率分别为0.61×10^-3，1.38×10^-3，2.09×10^-3 mol/（L·min），浓度为0.070，0.140，0.210 mol/L的Na₂FeO₄溶液与TPH的初始反应速率分别为13.30×10^-3，20.47×10^-3，12.86×10^-3 mol/（L·min）。2种氧化剂与TPH的反应速率大小为：Na₂FeO₄>H₂O₂。H₂O₂、NaFeO₄与TPH反应半衰期分别为40.40~66.50，4.10~7.14 min。H₂O₂的半衰期约为Na₂FeO₄的10倍。2种氧化剂对土壤中TPH去除率均可达到60%以上，但利用率较低。总结了2种氧化剂在去除TPH过程中反应速率、半衰期和去除率的特点，最终筛选并优化反应条件，为黄土高原土壤修复提供参考。
- 总石油烃 /
- 土壤有机质 /
- 反应速率 /
- H₂O₂ /
- Na₂FeO₄
Abstract: Two oxidants, H₂O₂ and Na₂FeO₄, were used to remove TPH from soil. The reaction kinetic model was established according to the relationship between reaction conditions and reaction rate. The factors such as reaction rate change, half-life and TPH removal rate in the reaction process were discussed and compared, and their reaction laws were also found out. The results showed that the process of removing TPH by H₂O₂ conformed to the first-order reaction kinetic model. The process of removing TPH by Na₂FeO₄ conformed to the second-order reaction kinetic model. The increase of H₂O₂ concentration led to the increase of reaction kinetic constant, and the increase of Na₂FeO₄ concentration led to the decrease of reaction kinetic constant. The initial reaction rates of H₂O₂ solution with TPH at concentrations of 0.078, 0.156, 0.234 mol/L TPH were 0.61×10^-3, 1.38×10^-3, 2.09×10^-3 mol/(L·min). The initial reaction rates of Na₂FeO₄ solution with TPH at three concentrations of 0.070, 0.140 and 0.210 mol/L were 13.30×10^-3, 20.47×10^-3, 12.86×10^-3 mol/(L·min). The reaction rates of the two oxidants with TPH were in the order of Na₂FeO₄>H₂O₂. The half-life of H₂O₂ reacted with TPH was 40.40~66.50 min, and the half-life of Na₂FeO₄ reacted with TPH was 4.10~7.14 min. The half-life of H₂O₂ was about 10 times of that of Na₂FeO₄. The removal rate of TPH in the soil by the two oxidants could reach more than 60%, which would not cause residue in the soil, but the utilization rate was low. The characteristics of the reaction rate, half-life and removal rate of the two oxidants in the process of removing TPH were summarized. Finally, the paper screened and optimized the reaction conditions to provide a theoretical basis for soil remediation in the Loess Plateau.
- total petroleum hydrocarbons (TPH) /
- soil organic matter (SOM) /
- reaction rate /
- H₂O₂ /
- Na₂FeO₄

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参考文献(40)

[1]	张晓曦, 张玲玲, 雷航宇, 等. 草本凋落物与尿素联合修复对油污土壤生物化学性质的影响[J]. 生态学报, 2020, 40(8):2715-2725.
[2]	纪学雁. 土壤中石油污染物迁移规律实验模拟研究[D]. 大庆:大庆石油学院, 2005.
[3]	冯程程. 松嫩石油污染及重度盐碱化草地土壤酶动力学及热力学特征的比较研究[D]. 哈尔滨:哈尔滨师范大学, 2019.
[4]	张辉, 宋琳, 陈晓琳, 等. 土壤退化的原因与修复作用研究[J]. 海洋科学,2020,44(8):147-161.
[5]	魏样. 石油污染对土壤性状的影响及植物修复效应研究[D]. 咸阳:西北农林科技大学, 2019.
[6]	李丽, 董万涛, 张兴, 等. 石油污染土壤修复技术研究进展[J]. 四川环境, 2020, 39(4):200-205.
[7]	CHEN Y, ZHAO R, XUE J, et al. Generation and distribution of PAHs in the process of medical waste incineration[J].Waste Management, 2013,33(5):1165-1173.
[8]	耿坤宇. 管式涡流强化石油烃污染土壤洗脱技术的研究[D]. 上海:华东理工大学, 2019.
[9]	李小康. 深层土壤原油污染的微生物修复[D]. 西安:西安石油大学,2020.
[10]	徐佰青, 李平平, 王山榕, 等. 植物修复石油污染土壤的研究进展[J]. 当代化工, 2020, 49(7):1527-1531.
[11]	GLAZE W H, KANG J, CHAPIN D H. Chemistry of water treatment processesinvolving ozone, hydrogen peroxide and ultraviolet radiation[J]. Ozone:Science andEngineering, 1987, 9:335-352.
[12]	赖冬麟, 张奇, 陈亭亭, 等.张家口市某机械厂原址电镀污染场地土壤修复工程实践[J].环境工程,2020,38(6):75-80.
[13]	HASELOW J S, SIEGRIST R L, CRIMI M, et al. Estimating the total oxidant demand for in situ chemical oxidation design[J]. Remediation, 2003, 13(4):5-16.
[14]	ZAPPI Y B. Infrastructural needs in waste containment and environmental restoration[J]. Journal of Infrastructure Systems, 1995, 1(2):82-91.
[15]	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.
[16]	阳杰, 杜保森. 活化过硫酸钠修复多环芳烃污染土壤效果研究[J]. 广州化工, 2020, 48(14):88-90.
[17]	OURIACHE H, ARRAR J, NAMANE A, et al. Treatment of petroleum hydrocarbons contaminated soil by Fenton like oxidation[J]. Chemosphere, 2019, 232:377-386.
[18]	罗玉虎, 卢楠. 芬顿法修复石油污染土壤使用条件优化的研究[J].西部大开发(土地开发工程研究), 2019, 4(4):33-37.
[19]	徐正国, 唐秋萍, 王颖. 不同氧化剂对某煤制气厂多环芳烃污染土壤的修复效果研究[J]. 环境工程, 2016,34(增刊1):988-992.
[20]	贾恒义.黄土丘陵草地土壤营养元素含量迁移及分布[J].水土保持研究,1998, 5(1):3-5.
[21]	刘柏玲, 蔡强国, 史志华, 等.黄土土质对溅蚀特征的影响[J]. 水土保持研究, 2016, 23(5):1-6.
[22]	LEMAIRE J, LAURENT F, LEYVAL C, et al. PAH oxidation in aged and spiked soils investigated by column experiments[J]. Chemosphere, 2013, 91(3):406-414.
[23]	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.
[24]	张耀亭,白世基,张维. 改进的水中痕量过氧化氢的分光光度测定法[J]. 环境与健康杂志, 2006,23(3):258-261.
[25]	贾汉东,杨新玲,杨勇,等. 高铁酸盐的直接分光光度法测定[J].分析化学, 1999, 27(5):617.
[26]	WANG W, LIU Y, LI T L, et al. Heterogeneous Fenton catalytic degradation of phenol based on controlled release of magnetic nanoparticles[J]. Chemical Engineering Journal, 2014,242:1-9.
[27]	USMAN M, FAURE P, HANNA K, et al. Application of magnetite catalyzed chemical oxidation (Fenton-like and persulfate) for the remediation of oil hydrocarbon contamination[J]. Fuel, 2012, 96(1):270-276.
[28]	BEN W W, QIANG Z M, PAN X, et al. Removal of veterinary antibiotics from sequencing batch reactor (SBR) pretreated swine wastewater by Fenton's reagent[J].Water research, 2009, 43(17):4392-4402.
[29]	PIGNATELLO J J, OLIVEROS E, MACKAY A. Advanced oxidation processes for organic contaminant destruction based on the Fenton reaction and related chemistry[J]. Critical Reviews in Environmental Science and Technology, 2006, 36(1):1-84.
[30]	徐金兰, 郭玉琴, 郭阳. 低浓度双氧水提高原油污染土壤氧化效果的实验研究[J]. 西安建筑科技大学学报(自然科学版), 2019, 51(5):743-750.
[31]	燕启社,高镜清,孙红文,等. Fenton氧化处理对土壤中芘的生物可利用性的影响[J].生态环境, 2008, 17(6):2215-2220.
[32]	贺泓, 李俊华, 上官文峰, 等.环境催化原理及应用[M]. 北京:科技出版社, 2008.
[33]	VENN Y, GAN S Y. Current status and prospects of Fenton oxidation for the decontamination of persistent organic pollutants (POPs) in soils[J]. Chemical Engineering Journal, 2012, 213(12):295-317.
[34]	VENN Y, GAN S Y. Inorganic chelated modified-Fenton treatment of polycyclic aromatic hydrocarbon (PAH)-contaminated soils[J]. Inhalation Toxicology, 2012, 180(7):1-8.
[35]	SHARMA V K, ZBORIL R, VARMA R S. Ferrates:greener oxidants with multimodal action in water treatment technologies[J].Accounts of Chemical Research, 2015, 48(2):182-191.
[36]	GOFF H, MURMANN R K. Mechanism of Isotopic Oxygen Exchange and Reduction of Ferrate(Ⅵ) ion (FeO₄^2-)[J]. Journal of the American Chemical Society, 1971, 93(23):6058-6065.
[37]	LEE Y, KISSNER R, GUNTEN U. Reaction of ferrate(Ⅵ) with ABTS and self-decay of ferrate(Ⅵ):kinetics and mechanisms[J]. Environmental Science & Technology, 2014,48(9):5154-5162.
[38]	SARMA R, ANGELES A M,BRINKLEY D W, et al. Studies of the di-iron(Ⅵ) intermediate in ferrate-dependent oxygen evolution from water[J]. Journal of the American Chemical Society, 2012,134(37):15371-15386.
[39]	RUSH J D, ZHAO Z, BIELSKI B H J. Reaction of ferrate(Ⅵ)/ferrate(Ⅴ) with hydrogen peroxide and superoxide anion-a stopped-flow and premix pulse radiolysis study[J]. Free Radical Research, 1996, 24(3):187-198.
[40]	KAMACHI T, KOUNO T, YOSHIZAWA K. Participation of multioxidants in the pH dependence of the reactivity of ferrate(Ⅵ)[J]. The Journal of Organic Chemistry, 2005, 70(11):4380-4388.