机械化学法修复石油烃污染土壤及对土壤特性的影响

doi:10.16085/j.issn.1000-6613.2020-0246

摘要/Abstract

摘要：

以典型石油烃正十六烷为特征污染物，采用批次实验研究机械化学处理对模拟石油烃污染土壤的修复效果及影响因素；采用GC/MS分析土壤中正十六烷的降解产物，通过XRD、FTIR、SEM和BET对处理前后土壤样品进行表征，并分析土壤有机碳含量的变化，揭示石油烃污染土壤的机械化学法修复机理。结果表明，在球磨机转速为500r/min，球料比为35∶1，大、中、小钢球配比为2∶5∶3，正十六烷投加量为2.5μL/g时，球磨4h后正十六烷降解率达95.86%。球磨处理过后土壤颗粒表面变粗糙，助磨效果较好的石英含量显著增多。与处理前相比，球磨处理后未检出短链烷烃，表明正十六烷降解较为彻底。土壤有机碳含量和吸附能力显著提高，使得残留低浓度石油烃难以全部去除。机械化学法修复石油烃污染土壤具有快速、高效、彻底等优势，具有良好的应用前景。

关键词: 土壤, 石油烃, 机械化学修复, 理化性质

Abstract:

Batch experiments were used to study the mechanochemical method for remediation effects and influencing factors of simulated petroleum hydrocarbon-contaminated soil with the typical petroleum hydrocarbon n-hexadecane as a characteristic pollutant; GC/MS was used to analyze the degradation products of n-hexadecane in the soil. XRD, FTIR, SEM and BET were applied for the characterization of the soil samples before and after treatment and the changes in soil organic matter content were analyzed, revealing the mechanism of mechanochemical method for remediation of petroleum-contaminated soil. The results showed that the degradation rate of n-hexadecane reached 95.86% after ball milling with 4h at a ball mill speed of 500r/min, a ball-to-material ratio of 35∶1, a large, medium, and small steel ball ratio of 2∶5∶3, and a dosage of n-hexadecane of 2.5μL/g, The surface of soil particles became rough and the quartz content with better grinding aid was significantly increased after ball milling. Compared with the tested soil before pretreatment, no short chain alkane was detected after milling treatment, suggesting that n-hexadecane degradation was more thorough. It was difficult to completely remove residual low-concentration petroleum hydrocarbons due to the improvement of soil organic carbon content and adsorption capacity. The mechanochemical method shows excellent application potential due to its advantages of rapidness, efficiency and completeness in remediation of petroleum hydrocarbons contaminated soil.

Key words: soil, petroleum hydrocarbons, mechanochemical remediation, physical- chemical properties

中图分类号:

张金永, 汪林, 王明新, 肖扬, 韩莹. 机械化学法修复石油烃污染土壤及对土壤特性的影响[J]. 化工进展, 2020, 39(11): 4726-4733.

Jinyong ZHANG, Lin WANG, Mingxin WANG, Yang XIAO, Ying HAN. Mechanochemical remediation of petroleum hydrocarbons contaminated soil and its effects on soil properties[J]. Chemical Industry and Engineering Progress, 2020, 39(11): 4726-4733.

参考文献

1	王金南, 董战峰, 蒋洪强, 等. 中国环境保护战略政策70年历史变迁与改革方向[J]. 环境科学研究, 2019. 32(10): 1636-1644.
1	WANG J N, DONG Z F, JIANG H Q, et al. Historical evolution and reform of China’s environmental strategy and policy during the past seventy years (1949—2019)[J]. Research of Environmental Sciencs, 2019, 32(10): 1636-1644.
2	PEPPER L. The soil health-human health nexus[J]. Critical Reviews in Environmental Science and Technology, 2013, 43(24): 2617-2652.
3	FRANCESCO D. Mechanochemical behavior of surface radicals in ground quartz[J]. The Journal of Physical Chemistry C, 2011, 115(43): 21230-21235.
4	KHAN M A I, NAIDU R, MEGHARAJ M, et al. Toxicity assessment of fresh and weathered petroleum hydrocarbons in contaminated soil—A review[J]. Chemosphere, 2018, 212: 755-767.
5	WANG Y, LIANG J, WANG J, et al. Combining stable carbon isotope analysis and petroleum-fingerprinting to evaluate petroleum contamination in the Yanchang oilfield located on loess plateau in China[J]. Environmental Science & Pollution Research, 2018, 25(3): 2830-2841.
6	RAMADASS K, MEGHARAJ M, VENKATESWARLU R, et al. Ecological implications of motor oil pollution: earthworm survival and soil health[J]. Soil Biology and Biochemistry, 2015, 85: 72-81.
7	CHENG M, ZENG G, HUANG D, et al. Advantages and challenges of Tween 80 surfactant-enhanced technologies for the remediation of soils contaminated with hydrophobic organic compounds[J]. Chemical Engineering Journal, 2017, 314: 98-113.
8	LU M, LV T, LI Y, et al. Formation of brominated and chlorinated dioxins and its prevention during a pilot test of mechanochemical treatment of PCB and PBDE contaminated soil[J]. Environmental Science and Pollution Research International, 2017, 24(6): 1-10.
9	杨茜, 吴蔓莉, 聂麦茜, 等. 石油污染土壤的生物修复技术及微生物生态效应[J]. 环境科学, 2015, 36(5): 1856-1863.
9	YANG Q, WU M L, NIE M Q, et al. Effects and biological response on bioremediation of petroleum contaminated soil[J]. Environmental Science, 2015, 36(5): 1856-1863.
10	YANG H J, ZHANG Y P, LIU P, et al. Different responses to soil petroleum contamination in monocultured and mixed plant systems[J]. Ecotoxicology and Environmental Safety, 2018, 161: 763-768.
11	YUAN W Y, XU W T, ZHANG Z W, et al. Rapid Cr(Ⅵ) reduction and immobilization in contaminated soil by mechanochemical treatment with calcium polysulfide[J]. Chemosphere, 2019, 227: 657-661.
12	CAGNETTA G, HUANG J, YU G. A mini-review on mechanochemical treatment of contaminated soil: from laboratory to large-scale[J]. Critical Reviews in Environmental Science and Technology, 2018, 48: 1-49.
13	PETER B, MARCELA A, MATEJ B, et al. Hallmarks of mechanochemistry: from nanoparticles to technology[J]. Chemical Society Reviews, 2013, 42(18): 7571.
14	CAGNETTA G, ROBERTSON J, HUANG J, et al. Mechanochemical destruction of halogenated organic pollutants: a critical review[J]. Journal of Hazardous Materials, 2016, 313: 85-102.
15	LI D C, XU W F, MU Y, et al. Remediation of petroleum-contaminated soil and simultaneous recovery of oil by fast pyrolysis[J]. Environmental Science & Technology, 2018, 52: 5330-5338.
16	ZHANG J, DAI J L, DU X M, et al. Distribution and sources of petroleumhydrocarbon in soil profiles of the Hunpu wastewater-irrigated area, China's northeast[J]. Geoderma, 2012, 173/174: 215-223.
17	王玉功, 马亮, 李玉泽, 等. ASE-气相色谱法测定油田区土壤中多种石油烃[J].环境监测管理与技术, 2019, 31(5): 43-45, 49.
17	WANG Y G, MA L, LI Y Z, et al. Determination of petroleum hydrocarbons in oilfield soil by accelerated solvent extraction and gas chromatography[J]. The Administration and Technique of Environmental Monitoring, 2019, 31(5): 43-45, 49.
18	吴鹏. 机械化学法处理高浓度滴滴涕污染土壤的初步研究[D]. 天津: 天津大学, 2014.
18	WU P. Preliminary study on mechanochemical treatment of soil heavily contaminated with DDT[D]. Tianjin: Tianjin University, 2014.
19	李同清. 球磨机矿磨介质动力学行为研究[D]. 徐州: 中国矿业大学, 2018.
19	LI T Q. Study on charge dynamic behaviour of ball mills[D].Xuzhou: China University of Mining and Technology, 2018.
20	JIA X Q, HE Y, HUANG L, et al. n-Hexadecane and pyrene biodegradation and metabolization by Rhodococcus sp. T1 isolated from oil contaminated soil[J]. Chinese Journal of Chemical Engineering, 2019, 27(2): 411-417.
21	LI Y T, LI D, LAI L J, et al. Remediation of petroleum hydrocarbon contaminated soil by using activated persulfate with ultrasound and ultrasound/Fe[J]. Chemosphere, 2020, 23: s124657.
22	GUO X, XIANG D, DUAN G, et al. A review of mechanochemistry applications in waste management[J]. Waste Management, 2010, 30(1): 4-10.
23	WANG H, HWANG J, HUANG J, et al. Mechanochemical remediation of PCB contaminated soil[J]. Chemosphere, 2017, 168: 333-340.
24	ZHANG K L, HUANG J,WANG H Z, et al. Mechanochemical degradation of hexabromocyclododecane and approaches for the remediation of its contaminated soil[J]. Chemosphere, 2014, 116: 40-45.
25	王玉, 张一平, 陈思根. 中国6种地带性土壤红外光谱特征研究[J]. 西北农林科技大学学报(自然科学版), 2003, 31(1): 57-61.
25	WANG Y, ZHANG Y P, CHEN S G. The characteristics of infrared spectrum of 6 typical zonal soils in China[J]. Journal of Northwest Sci-Tech University of Agriculture and Forestry(Natural Science Edition), 2003, 31(1): 57-61.
26	ECKHARDT C J. Mechanochemistry: the last energetic frontier[J]. Molecular Crystals & Liquid Crystals, 2006, 456(1): 1-14.
27	RYBKIN V V. Franck-Condon theory of quantum mechanochemistry[J]. The Journal of Physical Chemistry A, 2017, 121(30): 5758-5762.
28	赵帅群, 刘刚, 欧全宏, 等. 不同类型土壤的FTIR和ICP-MS分析[J]. 光谱学与光谱分析, 2014, 34(12): 3401-3405.
28	ZHAO S Q, LIU G, OU Q H, et al. Analysis of different types of soil by FTIR and ICP-MS[J]. Spectroscopy and Spectral Analysis, 2014, 34(12): 3401-3405.
29	罗松英, 陈东平, 陈碧珊, 等. 红树林湿地土壤矿物的分析[J]. 分析测试学报, 2019, 38(7): 823-829.
29	LUO S Y, CHEN D P, CHEN B S, et al. Application of mineral analysis in mangrove wetland soils[J]. Journal of Instrumental Analysis, 2019, 38(7): 823-829.
30	TRITTSCHACK R, GROBETY B, KOCHMULLER M. The lizardite phase transformation followed by in situ high-temperature Raman and FTIR spectroscopy[J]. American Mineralogist, 2012, 14(97): 4354.
31	郝翔翔, 韩晓增, 邹文秀. 示差红外光谱在土壤有机质组成研究中的应用[J]. 分析化学, 2018. 46(4): 616-622.
31	HAO X X, HAN X Z, ZOU W X. Studies on composition of soil organic matter by fourier transform infrared spectroscopy differential analysis[J]. Chinese Journal of Analytical Chemistry, 2018. 46(4): 616-622.
32	许维通, 苑文仪, 李培中, 等. 机械球磨固化修复六价铬污染土壤[J]. 环境科学与技术, 2019, 42(4): 155-160.
32	XU W T, YUAN W Y, LI P Z, et al. Solidification and remediation of hexavalent chromium spiked soil using mechanical ball milling treatment[J]. Environmental Science & Technology, 2019, 42(4): 155-160.
33	ANCONA V, DI LEO P, PIZZIGALLO M D R. Sequestration of catechol and pentachlorophenol by mechanochemically treated kaolinite[J]. Clays and Clay Minerals, 2016, 64(5): 513-522.
34	WU S, LIU X, LIU M, et al. Sources, influencing factors and environmental indications of PAH pollution in urban soil columns of Shanghai, China[J]. Ecological Indicators, 2018, 85: 1170-1180.

[1]	刘柏成, 李法云, 赵琦慧, 吝美霞. 禾本科植物修复多环芳烃污染土壤研究进展[J]. 化工进展, 2023, 42(7): 3736-3748.
[2]	李若琳, 何少林, 苑宏英, 刘伯约, 纪冬丽, 宋阳, 刘博, 余绩庆, 徐英俊. 原位热解对油页岩物性及地下水水质影响探索[J]. 化工进展, 2023, 42(6): 3309-3318.
[3]	吴中杰, 谢连科, 王晶辉, 黄仁亮. 多级结构羟基硝酸铜纳米酶的制备及其对酚类污染物的降解[J]. 化工进展, 2023, 42(1): 497-505.
[4]	颜子涵, 陈群云, 李卓, 付融冰, 李彦伟, 吴志根. 改进型土壤破碎混拌结构的性能数值分析与优化[J]. 化工进展, 2022, 41(S1): 72-80.
[5]	郑瑾, 韩瑞瑞, 李丹丹, 王馨妤, 高春阳, 杜显元, 张晓飞, 邹德勋. 过氧化尿素与微生物联合修复石油污染土壤[J]. 化工进展, 2022, 41(9): 5085-5093.
[6]	吕莹, 胡学武, 陈素素, 刘兴宇, 陈勃伟, 张明江. 多环芳烃污染土壤的微生物修复技术研究进展[J]. 化工进展, 2022, 41(6): 3249-3262.
[7]	汪林, 蒲思淇, 王明新, 薛金娟, 韩莹. 过碳酸钠修复石油污染土壤及其环境效应[J]. 化工进展, 2022, 41(4): 2171-2179.
[8]	潘云飞, 唐正, 彭欣怡, 高品. 石油烃污染土壤微生物修复技术研究现状及进展[J]. 化工进展, 2021, 40(8): 4562-4572.
[9]	唐垂云, 钟娟, 吕莹, 张明江, 孙娟, 刘兴宇. 土壤中铀污染修复技术研究进展[J]. 化工进展, 2021, 40(8): 4587-4599.
[10]	李薇, 王信粉, 时利香, 宋瑶, 张杰, 杜显元. 表面活性剂复配体系修复芘污染土壤实验[J]. 化工进展, 2021, 40(6): 3526-3535.
[11]	李松旌, 樊向阳, 崔二苹, 胡超, 崔丙健, 刘源, 李中阳, 景若瑶, 李胜曙. PPCPs在土壤-作物系统行为特征及环境风险的研究进展[J]. 化工进展, 2021, 40(5): 2827-2838.
[12]	幸艳, 张雪凯, 周康根, 彭长宏. CaCl₂回收液赤泥碱性调控[J]. 化工进展, 2021, 40(5): 2909-2916.
[13]	刘贤力, 侯昭胤. 重金属污染土壤回转窑协同处置和资源化利用[J]. 化工进展, 2020, 39(S1): 287-291.
[14]	王龙, 刘会娥, 于云飞, 王娩, 刘宇童, 陈爽, 王彬. 槐糖脂用于含油砂质土壤处理及石油资源回收[J]. 化工进展, 2020, 39(5): 1930-1937.
[15]	王哲,骆逸飞,郑春丽,张雪峰,王维大,姜庆宏. 淋溶条件下生物炭对矿区土壤中重金属迁移的影响[J]. 化工进展, 2020, 39(2): 738-746.