气动力循环井强化Fe2+/O2/配体高级氧化体系修复对硝基酚污染地下水

赵薇; 张成武; 张慧; 姚禹; 辛思怡; 秦传玉

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中国环境科学 ›› 2025, Vol. 45 ›› Issue (2) : 820-828.

水污染与控制

气动力循环井强化Fe²⁺/O₂/配体高级氧化体系修复对硝基酚污染地下水

赵薇^1,2,3, 张成武^1,2,3, 张慧^1,2,3, 姚禹^1,2,3, 辛思怡^1,2,3, 秦传玉^1,2,3

作者信息 +

Remediation of p-nitrophenol contaminated groundwater using Fe²⁺/O₂/ligand advanced oxidation system enhanced by groundwater circulation well

ZHAO Wei^1,2,3, ZHANG Cheng-wu^1,2,3, ZHANG Hui^1,2,3, YAO Yu^1,2,3, XIN Si-yi^1,2,3, QIN Chuan-yu^1,2,3

Author information +

文章历史 +

摘要

本研究将气动力循环井(GCW)与Fe²⁺活化O₂的高级氧化体系耦合,在持续补充地下水含氧量的同时实现修复药剂的高效传输和均匀分布,以强化Fe²⁺/O₂/配体高级氧化体系的修复效果.通过二维模拟槽实验,结合示踪染色等可视化手段,明确了GCW作用下地下水流场的变化规律和溶质传输强化效果.在此基础上,选取三聚磷酸钠(STPP)为配体,通过井内注入药剂的方式,考察了高级氧化体系修复对硝基酚(PNP)污染含水层的效果.结果表明,GCW实现了对药剂的高效传输、为高级氧化反应提供充足的O₂,在GCW强化作用下,整个模拟槽内PNP均有降解,15h平均降解率达62%,成果为有机污染地下水的高效修复提供了新的思路.

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.

导出引用

赵薇, 张成武, 张慧, 姚禹, 辛思怡, 秦传玉. 气动力循环井强化Fe²⁺/O₂/配体高级氧化体系修复对硝基酚污染地下水[J]. 中国环境科学. 2025, 45(2): 820-828

ZHAO Wei, ZHANG Cheng-wu, ZHANG Hui, YAO Yu, XIN Si-yi, QIN Chuan-yu. Remediation of p-nitrophenol contaminated groundwater using Fe²⁺/O₂/ligand advanced oxidation system enhanced by groundwater circulation well[J]. China Environmental Science. 2025, 45(2): 820-828

中图分类号： X703 X523

参考文献

[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.