1. Key Laboratory of Groundwater Resources and Environment, Ministry of Education, Jilin University, Changchun 130021, China; 2. National and Local Joint Engineering Laboratory for Petrochemical Contaminated Site Control and Remediation Technology, Jilin University, Changchun 130021, China; 3. Jilin Provincial Key Laboratory of Water Resources and Environment, Jilin University, Changchun 130021, China
Abstract:In this study, GCW was coupled with the advanced oxidation system based on Fe2+ activated O2 to achieve efficient transmission and uniform distribution of chemical agents while continuously replenishment of oxygen to groundwater, so as to enhance the remediation effect of the Fe2+/O2/ligand was advanced oxidation system. The variation law of groundwater flow field and enhanced transport effect of solute under the enhancement of GCW were clarified using two-dimensional simulation tank experiment combined with visualization methods such as tracer dyeing. In addition, sodium tripolyphosphate (STPP) was selected as the ligand, and the effect of advanced oxidation system on the remediation of p-nitrophenol (PNP) polluted aquifer was investigated by injection of chemicals into the well. The results show that GCW had achieved efficient transmission of chemical agents and provided sufficient O2 for advanced oxidation reactions. Under the enhancement of GCW, PNP was degraded throughout the simulated tank, with an average degradation rate of 62% in 15h. The results provide a new insight for efficient remediation of organic contaminated groundwater.
[1] 高志婷.低价铁活化分子氧降解典型有机污染物的研究 [D]. 武汉:华中师范大学, 2013.Gao Z T. Activation of molecular oxygen over low valent iron for degradation of typical organic pollutants [D]. Wuhan: Central China Normal University, 2013. [2] Liao P, Yu K, Lu Y, et al. Extensive dark production of hydroxyl radicals from oxygenation of polluted river sediments [J]. Chemical Engineering Journal, 2019,368:700-709. [3] 穆 毅,贾法龙,艾智慧,等.纳米零价铁活化分子氧原理及降解有机污染物性能增强策略 [J]. 化学学报, 2017,75(6):538-543.Mu Y, Jia F L, Ai Z H, et al. Molecular oxygen activation with nano zero-valent iron for aerobic degradation of organic contaminants and the performance enhancement [J]. Acta Chimica Sinica, 2017,75(6): 538-543. [4] Page S E, Kling G W, Sander M, et al. Dark formation of hydroxyl radical in arctic soil and surface waters [J]. Environmental Science & Technology, 2013,47(22):12860-12867. [5] Tong M, Yuan S, Ma S, et al. Production of abundant hydroxyl radicals from oxygenation of subsurface sediments [J]. Environmental Science & Technology, 2016,50(1):214-221. [6] Wang L, Wang F, Li P, et al. Ferrous-tetrapolyphosphate complex induced dioxygen activation for toxic organic pollutants degradation [J]. Separation and Purification Technology, 2013,120:148-155. [7] Keenan C R, Sedlak D L. Factors affecting the yield of oxidants from the reaction of nanonarticulate zero-valent iron and oxygen [J]. Environmental Science & Technology, 2008,42(4):1262-1267. [8] Welch K D, Davis T Z, Aust S D. Iron autoxidation and free radical generation: effects of buffers, ligands, and chelators [J]. Archives of Biochemistry and Biophysics, 2002,397(2):360-369. [9] Pang S Y, Jiang J, Ma J. Oxidation of sulfoxides and arsenic(Ⅲ) in corrosion of nanoscale zero valent iron by oxygen: evidence against ferryl ions (Fe(IV)) as active intermediates in fenton reaction [J]. Environmental Science & Technology, 2011,45(1):307-312. [10] Hou X, Shen W, Huang X, et al. Ascorbic acid enhanced activation of oxygen by ferrous iron: a case of aerobic degradation of rhodamine b [J]. Journal of Hazardous Materials, 2016,308:67-74. [11] Zhou H, Sun Q, Wang X, et al. Removal of 2,4-Dichlorophenol from contaminated soil by a heterogeneous ZVI/EDTA/Air fenton-like system [J]. Separation and Purification Technology, 2014,132:346-353. [12] Belanzoni P, Bernasconi L, Baerends E J. O2activation in a dinuclear Fe(Ⅱ)/EDTA complex: Spin surface crossing as a route to highly reactive Fe(IV) oxo species [J]. Journal of Physical Chemistry A, 2009, 113(43):11926-11937. [13] Keenan C R, Sedlak D L. Ligand-enhanced reactive oxidant generation by nanoparticulate zero-valent iron and oxygen [J]. Environmental Science and Technology, 2008,42(18):6936-6941. [14] Cao M, Wang L, Ai Z, et al. Efficient remediation of pentachlorophenol contaminated soil with tetrapolyphosphate washing and subsequent ZVI/Air treatment [J]. Journal of Hazardous Materials, 2015,292:27-33. [15] Biaglow J E, Kachur A V. The generation of hydroxyl radicals in the reaction of molecular oxygen with polyphosphate complexes of ferrous ion [J]. Radiation Research, 1997,148(2):181-187. [16] Zong Y, Mao Y, Xu L, et al. Non-selective degradation of organic pollutants via dioxygen activation induced by Fe(Ⅱ)-tetrapolyphosphate complexes: Identification of reactive oxidant and kinetic modeling [J]. Chemical Engineering Journal, 2020,398: 125603. [17] Xie W, Zhang P, Liao W, et al. Ligand-enhanced electron utilization for trichloroethylene degradation by ·OH during sediment oxygenation [J]. Environmental Science & Technology, 2021,55(10):7044-7051. [18] Wang L, Cao M, Ai Z, et al. Design of a highly efficient and wide pH electro-fenton oxidation system with molecular oxygen activated by ferrous-tetrapolyphosphate complex [J]. Environmental Science & Technology, 2015,49(5):3032-3039. [19] Zhang C, Kong C, Tratnyek P G, et al. Generation of reactive oxygen species and degradation of pollutants in the Fe2+/O2/Tripolyphosphate system: regulated by the concentration ratio of Fe2+ and tripolyphosphate [J]. Environmental Science & Technology, 2022,56 (7):4367-4376. [20] 张成武.配体调控Fe(Ⅱ)/O2反应体系原位修复对硝基酚污染地下水的效果及机制 [D]. 长春:吉林大学, 2023.Zhang C W. Effect and mechanism of in-situ remediation of nitrophenol contaminated groundwater through ligand modulation of Fe(Ⅱ)/O2 reaction system [D]. Changchun: Jinlin University, 2023. [21] 刘 洋,袁松虎,张耀强,等.电化学循环井耦合氧化-还原降解地下水中三氯乙烯 [J]. 水文地质工程地质, 2020,47(3):44-51.Liu Y, Yuan S H, Zhang Y Q, et al.. Electrolytic circulation well coupled with oxidation and reduction for trichloroethylene degradation in groundwater [J]. Hydrogelogy & Engineering Geology, 2020,47(3): 44-51. [22] 顾 维.循环井技术修复地下水氯苯污染的效果分析 [J]. 资源节约与环保, 2020,(11):45-46.Gu W. Analysis of effect of recirculating well technique in remediation of chlorobenzene pollution in groundwater [J]. Resource Conservation and Environmental Protection., 2020,(11):45-46. [23] 宋 刚,岳豪康,李恒超,等.地下水循环井技术研究进展 [J]. 地下水, 2022,44(1):9-13,108.Song G, Yue H K, Li H C. et al. Research progress of groundwater circulation well technology [J]. Ground Water, 2022,44(1):9-13,108. [24] 鲁 亮,蒲生彦,李博文.热强化循环井驱动热量传输及苯胺修复效果 [J]. 中国环境科学, 2023,43(9):4639-4647.Lu L, Pu S Y, Li B W. Study on heat transfer and aniline restoration effect of thermal enhanced circulation well [J]. China Environmental Science, 2023,43(9):4639-4647. [25] Elmore A C, Graff T. Best available treatment technologies applied to groundwater circulation wells [J]. Remediation Journal, 2002,12(3): 63-80. [26] Papini M P, Majone M, Arjmand F, et al. First pilot test on the integration of GCW (Groundwater Circulation Well) with ENA (Enhanced Natural Attenuation) for chlorinated solvents source remediation [J]. Chemical Engineering Transactions, 2016,49:91-96. [27] 何允玉,王 铎,郭 都.地下水中挥发性有机污染物去除新技术-循环井工艺 [J]. 资源节约与环保, 2013,(3):37-38.He Y Y, Wang D, Guo D. A new technique for removing volatile organic pollutants from groundwater -circulating well technology [J]. Resource Conservation and Environmental Protection., 2013,(3):37-38. [28] 张 莉,白 静,赵冬宇,等.基于抽注水的水动力循环井不同抽注流量对地下水流场的影响 [J]. 安全与环境工程, 2023,30(4):203-210.Zhang L, Bai J, Zhao D Y, et al. Effect of different pumping and injection flow rates on flow field of groundwater in water pumping and injection driven hydrodynamic circulation wells [J]. Safety and Environmental Engineering, 2023,30(4):203-210. [29] Wang P, Li J, An P, et al. Enhanced delivery of remedial reagents in low-permeability aquifers through coupling with groundwater circulation well [J]. Journal of Hydrology, 2023,618,129260. [30] 孙冉冉,杨再福,汪 涛,等.地下水循环井技术处理土壤和地下水中甲基叔丁基醚研究 [J]. 环境工程, 2017,35(9):186-191.Sun R R, Yang Z F, Wang T, et al. Study on MTBE remediated in soil and groundwater by GCW [J]. Environmental Engineering, 2017, 35(9):186-191. [31] Zhao Y, Qu D, Zhou R, et al. Efficacy of forming biofilms by pseudomonas migulae AN-1toward in situ bioremediation of aniline-contaminated aquifer by groundwater circulation wells [J]. Environmental Science and Pollution Research, 2016,23(12):11568-11573. [32] Yuan S, Liu Y, Zhang P, et al. Electrolytic groundwater circulation well for trichloroethylene degradation in a simulated aquifer [J]. Science China Technological Sciences, 2020,64(2):251-260. [33] Wang X, Zhang L, Han C, et al. Simulation study of oxytetracycline contamination remediation in groundwater circulation wells enhanced by nano-calcium peroxide and ozone [J]. Scientific Reports, 2023,13 (1):9136. [34] Xia H, Guo J, Yang Y, et al. Remediation of PNP-contaminated groundwater using a modified CaO2/Fe(Ⅱ) fenton system: reactive principles, degradation performance and potential pathways [J]. Journal of Environmental Chemical Engineering, 2022,10(2):107305. [35] Harvey A E, Smart J A, Amis E S. Simultaneous spectrophotometric determination of iron(Ⅱ) and total iron with 1,10-Phenanthroline [J]. Analytical chemistry (Washington), 1955,27(1):26-29. [36] GB 11893-89 水质总磷的测定钼酸铵分光光度法 [S].GB 11893-89 Water quality-determination of total phosphorus-ammonium molybdate spectrophotometric method [S]. [37] Zhang C, Kong C, Tratnyek P G, et al. Effect of interfacial action on the generation and transformation of reactive oxygen species in tripolyphosphate-enhanced heterogeneous Fe3O4/O2 systems [J]. Environmental Science & Technology, 2024,58(2):1378-1389. [38] 白 静.表面活性剂强化地下水循环井技术修复NAPL污染含水层研究 [D]. 长春:吉林大学, 2013.Bai J. Remediation of NAPL contaminated aquifer with surfactant-enhanced groundwater circulation well [D]. Changchun: Jinlin University, 2013.