EK/Fe0-PRB联合修复实际砷污染土壤的协同机制

doi:10.11949/j.issn.0438-1157.20180787

化工学报 ›› 2018, Vol. 69 ›› Issue (12): 5276-5282.DOI: 10.11949/j.issn.0438-1157.20180787

EK/Fe⁰-PRB联合修复实际砷污染土壤的协同机制

纪冬丽¹, 张竞², 孟凡生³, 王业耀⁴

1. 天津城建大学环境与市政工程学院, 天津 300384;
2. 天津地质调查中心, 天津 300170;
3. 中国环境科学研究院环境基准与风险评估国家重点实验室水污染控制技术研究中心, 北京 100012;
4. 中国环境监测总站, 北京 100012

收稿日期:2018-07-12 修回日期:2018-09-04 出版日期:2018-12-05 发布日期:2018-12-05
通讯作者: 纪冬丽
基金资助:
天津市教委科研计划（2018KJ170）。

Synergistic effects of electrokinetics process coupled with zero-valent iron permeable reaction barrier in remediation of arsenic-contaminated soil

JI Dongli¹, ZHANG Jing², MENG Fansheng³, WANG Yeyao⁴

1. School of Environmental and Municipal Engineering, Tianjin Urban Construction College, Tianjin 300384, China;
2. Tianjin Geological Survey Center, Tianjin 300170, China;
3. State Key Laboratory of Environmental Criteria and Risk Assessment, Chinese Research Academy of Environmental Sciences, Beijing 100012, China;
4. China National Environmental Monitoring Station, Beijing 100012, China

Received:2018-07-12 Revised:2018-09-04 Online:2018-12-05 Published:2018-12-05
Supported by:
supported by the Education Commission Scientific Research Project in Tianjin(2018KJ170).

摘要/Abstract

摘要：

以我国某矿区砷污染土壤为研究对象，采用EK/Fe⁰-PRB联合修复工艺去除土壤中的砷，考察了土壤含水率及增强试剂对砷去除的影响，分析了修复前后土壤中砷的迁移分布及砷价态分布变化，并借助X射线光电子能谱（XPS）对修复前后PRB填料Fe⁰进行了表征分析，探讨了EK/PRB修复砷污染的协同机制。结果表明，在EK/PRB联合修复过程中，EK去除作用所占比例为22%～43%，而PRB的去除作用所占比例为52%～71%，以PRB的去除作用为主；未添加增强试剂时，阳极液砷收集含量明显高于阴极液砷收集含量，电动去除机制主要为电迁移作用，添加增强试剂后，阴极液砷收集含量所占比例明显升高；EK/PRB修复后，As（Ⅴ）和As（Ⅲ）在土壤、电极液、PRB中的含量比例基本没有变化，As（Ⅴ）含量比例略微升高，即处理之后土壤中的五价砷并不会经氧化还原作用而转变成毒性较高的三价砷；反应后Fe⁰表面存在As（Ⅲ）和As（Ⅴ），未发现As（0）的存在，因此砷在PRB中仅通过铁表面氧化物的吸附作用而去除。

关键词: 砷, 污染土壤, 电动修复, PRB, 协同机制

Abstract:

The remediation of arsenic polluted soil from a mining area in China using the electrokinetics process coupled with zero-valent iron permeable reaction barrier was researched. The influence of soil moisture content and enhancement reagents on arsenic removal was investigated. The changes of distribution and valence state of arsenic before and after the remediation were analyzed. In addition, surface features of the fresh and used zero-valent iron were characterized by X-ray photoelectron spectroscopy (XPS). Then synergistic effects of EK/PRB in the remediation of arsenic-contaminated soil was discussed. The results showed that in the EK/PRB remediation process, fraction of the EK removal mechanism was 22% to 43%, while fraction of the PRB removal mechanism was 52% to 71%, so the PRB process was dominate. When the enhancement reagents was absent, arsenic mainly tends to move toward the anolyte, which indicated the mainly removal mechanisms was electromigration. However, when the enhancement reagents was added, the proportion of arsenic collected from the cathode solution was significantly increased. After EK/PRB remediation, the percentage content of As(Ⅴ) and As (Ⅲ) in soil, electrode liquid and PRB had no substantial changes, only the content ratio of As(Ⅴ) raised slightly. Pentavalent arsenic will not be reduced into trivalent arsenic with higher toxicity. There were no As(0) but As(Ⅲ) and As(Ⅴ) on the surface of the used Fe⁰. Therefore, arsenic was removed in PRB only through adsorption of the iron surface oxides.

Key words: arsenic, polluted soil, electrokinetics, PRB, synergistic effects

中图分类号:

纪冬丽, 张竞, 孟凡生, 王业耀. EK/Fe⁰-PRB联合修复实际砷污染土壤的协同机制[J]. 化工学报, 2018, 69(12): 5276-5282.

JI Dongli, ZHANG Jing, MENG Fansheng, WANG Yeyao. Synergistic effects of electrokinetics process coupled with zero-valent iron permeable reaction barrier in remediation of arsenic-contaminated soil[J]. CIESC Journal, 2018, 69(12): 5276-5282.

参考文献 30

[1]	RUÍZ-HUERTA E A, DELG V A, GÓMEZ-BERNAL J M, et al. Arsenic contamination in irrigation water, agricultural soil and maize crop from an abandoned smelter site in Matehuala, Mexico[J]. Journal of Hazardous Materials, 2017, 339:330.
[2]	GARCÍA-CARMONA M, ROMERO-FREIRE A, ARAGÓN M S, et al. Evaluation of remediation techniques in soils affected by residual contamination with heavy metals and arsenic[J]. Journal of Environmental Management, 2017, 191:228-236.
[3]	赵婉雨, 杨雨寒. 土壤重金属污染修复技术分析[J]. 高科技与产业化, 2015, 11(9):64-69. ZHAO W Y, YANG Y H. Analysis on soil heavy metal pollution repair technology[J]. High-Technology & Industrialization, 2015, 11(9):64-69.
[4]	RODRÍGUEZLADO L, SUN G, BERG M, et al. Groundwater arsenic contamination throughout China[J]. Science, 2013, 341(6148):866.
[5]	陈寻峰. 砷污染土壤淋洗修复技术研究[D]. 长沙:湖南大学, 2016. CHEN X F. Research on leaching repair technology of arsenic-contaminated soil[D]. Changsha:Hunan University, 2016.
[6]	PATRICIA M, ALICIA F C. Remediation of arsenic-contaminated soils by iron amendments:a review[J]. Critical Reviews in Environmental Science & Technology, 2010, 40(2):93-115.
[7]	MAHESWARI S, MURUGESAN A G. Remediation of arsenic in soil by Aspergillus nidulans isolated from an arsenic-contaminated site[J]. Environmental Technology, 2009, 30(9):921-926.
[8]	MA J, LEI E, LEI M, et al. Remediation of arsenic contaminated soil using malposed intercropping of Pteris vittata L. and maize[J]. Chemosphere, 2017, 194:737-744.
[9]	SHIN S Y, PARK S M, BAEK K. Soil moisture could enhance electrokinetic remediation of arsenic-contaminated soil[J]. Environ. Sci. Pollut. Res. Int., 2017, 24(10):9820-9825.
[10]	LIMA A T, HOFMANN A, REYNOLDS D, et al. Environmental electrokinetics for a sustainable subsurface[J]. Chemosphere, 2017, 181:122-133.
[11]	VOCCIANTE M, BAGATIN R, FERRO S. Enhancements in electrokinetic remediation technology:focus on water management and wastewater recovery[J]. Chemical Engineering Journal, 2016, 309:708-716.
[12]	LÓPEZ-VIZCAÍNO R, NAVARRO V, LEÓN M J, et al. Scale-up on electrokinetic remediation:engineering and technological parameters[J]. Journal of Hazardous Materials, 2016, 315:135-143.
[13]	DONG Z Y, HUANG W H, XING D F, et al. Remediation of soil co-contaminated with petroleum and heavy metals by the integration of electrokinetics and biostimulation[J]. Journal of Hazardous Materials, 2013, 260:399.
[14]	VIGNOLA R, BAGATIN R, D'AURIS A D F, et al. Zeolites in a permeable reactive barrier (PRB):one year of field experience in a refinery groundwater(Part 1):The performances[J]. Chemical Engineering Journal, 2011, 178(140):204-209.
[15]	BAIN J, SPINK L, BLOWES D, et al. The removal of arsenic from groundwater using permeable reactive materials[C]//The 9th International Conference on Tailings and Mine Waste. Fort Colling, Colorado, 2002:213-216.
[16]	CHIANG T H. Study of the effect of permeable reactive barriers (PRB) on the electrokinetic remediation of arsenic contaminated soil[D]. Taiwan:National Sun Yat-Sen University, 2005.
[17]	石荣, 贾永锋, 王承智. 土壤矿物质吸附砷的研究进展[J]. 土壤通报, 2007, 38(3):584-589. SHI R, JIA Y F, WANG C Z. Research progress of soil mineral adsorption of arsenic[J]. Chinese Journal of Soil Science, 2007, 38(3):584-589.
[18]	ZHOU T, LI Y, JI J, et al. Oxidation of 4-chlorophenol in a heterogeneous zero valent iron/H2O2, Fenton-like system:kinetic, pathway and effect factors[J]. Separation & Purification Technology, 2008, 62(3):551-558.
[19]	GIASUDDIN A B M, KANEL S R, CHOI H. Adsorption of humic acid onto nanoscale zerovalent iron and its effect on arsenic removal[J]. Environmental Science & Technology, 2007, 41(6):2022-7.
[20]	YOON I H, KIM K W, BANG S, et al. Reduction and adsorption mechanisms of selenate by zero-valent iron and related iron corrosion[J]. Applied Catalysis B Environmental, 2011, 104(1):185-192.
[21]	BANG S, JOHNSON M D, KORFIATIS G P, et al. Chemical reactions between arsenic and zero-valent iron in water[J]. Water Research, 2005, 39(5):763-770.
[22]	LI S S, JIANG M, JIANG T J, et al. Competitive adsorption behavior toward metal ions on nano-Fe/Mg/Ni ternary layered double hydroxide proved by XPS:evidence of selective and sensitive detection of Pb(Ⅱ)[J]. Journal of Hazardous Materials, 2017, 338:1-10.
[23]	YU H, CHU Y, ZHANG T, et al. Recovery of tellurium from aqueous solutions by adsorption with magnetic nanoscale zero-valent iron (NZVFe)[J]. Hydrometallurgy, 2018, 177:1-8.
[24]	YAMASHITA T, HAYES P. Analysis of XPS spectra of Fe2+, and Fe3+ ions in oxide materials[J]. Applied Surface Science, 2008, 254(8):2441-2449.
[25]	MULLET M, KHARE V, RUBY C. XPS study of Fe(Ⅱ)?Fe(Ⅲ) (oxy)hydroxycarbonate green rust compounds[J]. Surface & Interface Analysis, 2010, 40(3/4):323-328.
[26]	ABASS O K, MA T, KONG S, et al. A novel MD-ZVI integrated approach for high arsenic groundwater decontamination and effluent immobilization[J]. Process Safety & Environmental Protection, 2016, 102:190-203.
[27]	KOLOBOV A V, BADYAL J P S, LAMBERT R M. Novel photoinduced surface oxidation of an amorphous semiconductor:an XPS study of vitreous arsenic sulphide[J]. Surface Science Letters, 1989, 222(2/3):L819-L824.
[28]	JONES R A, NESBITT H W. XPS evidence for Fe and As oxidation states and electronic states in loellingite (FeAs2)[J]. American Mineralogist, 2002, 87(11/12):1692-1698.
[29]	BAKSHI S, BANIK C, RATHKE S J, et al. Arsenic sorption on zero-valent iron-biochar complexes[J]. Water Research, 2018, 137:153.
[30]	SUN F, OSSEO-ASARE K A, CHEN Y, et al. Reduction of As(Ⅴ) to As(Ⅲ) by commercial ZVI or As(0) with acid-treated ZVI[J]. Journal of Hazardous Materials, 2011, 196(12):311-317.

EK/Fe⁰-PRB联合修复实际砷污染土壤的协同机制

Synergistic effects of electrokinetics process coupled with zero-valent iron permeable reaction barrier in remediation of arsenic-contaminated soil

PDF (PC)

可视化

摘要/Abstract

引用本文

使用本文

参考文献 30

相关文章 15

编辑推荐

Metrics

本文评价

[1]	李锦潼, 邱顺, 孙文寿. 煤浆法烟气脱硫中草酸和紫外线强化煤砷浸出过程[J]. 化工学报, 2023, 74(8): 3522-3532.
[2]	王永良, 杨晓玲, 董永霞, 杜英超, 刘翔, 韩培伟, 叶树峰. pH调整剂对含砷酸性废水中氧化Fe（Ⅱ）共沉淀固砷行为的影响[J]. 化工学报, 2019, 70(9): 3511-3516.
[3]	孙燕, 蓝际荣, 郭莉, 孙朋, 叶恒朋, 杜冬云, 占伟. 利用电解锰渣制备As(Ⅲ)吸附材料及其性能研究[J]. 化工学报, 2019, 70(6): 2377-2385.
[4]	任新林, 梅毅, 冯梦黎, 李柏扬, 吕武华, 问亚玲, 王驰, 何德东. SK静态混合器对工业磷酸脱砷的过程强化研究[J]. 化工学报, 2018, 69(S2): 218-225.
[5]	朱文会, 李志涛, 王夏晖, 王兴润. 不同异位修复工艺对高浓度铬渣污染土壤中Cr的去除特性[J]. 化工学报, 2018, 69(6): 2730-2736.
[6]	邹潺, 王春波, 郭辉, 王贺飞. 燃煤过程中砷的赋存形态及其挥发特性[J]. 化工学报, 2018, 69(4): 1670-1677.
[7]	芮泽宝, 杨晓庆, 陈俊妃, 纪红兵. 光热协同催化净化挥发性有机物的研究进展及展望[J]. 化工学报, 2018, 69(12): 4947-4958.
[8]	王倩, 郭莉, 陈绍华, 薛余化, 杜冬云. 辉光放电等离子体辅助碱浸铜冶炼烟灰中铜砷分离[J]. 化工学报, 2017, 68(5): 1932-1939.
[9]	赵斌, 刘安琪, 刁法林, 谭赟, 张朝晖, 王亮. 道南渗析除砷过程影响因素分析[J]. 化工学报, 2016, 67(6): 2456-2461.
[10]	刘慧敏, 王春波, 郭永成, 张月, 黄星智, 王家伟. 高砷褐煤与低砷烟煤混燃砷的挥发特性及模型[J]. 化工学报, 2016, 67(10): 4477-4484.
[11]	赵雅光, 万俊锋, 王杰, 余飞, 王岩. 零价铁(ZVI)去除水中的As(Ⅲ)[J]. 化工学报, 2015, 66(2): 730-737.
[12]	刘慧敏, 王春波, 黄星智, 张月, 孙鑫. 富氧燃烧方式下煤中砷的挥发行为[J]. 化工学报, 2015, 66(12): 5079-5087.
[13]	刘慧敏, 王春波, 张月, 孙喆, 邵欢. 温度和赋存形态对燃煤过程中砷迁移和释放的影响[J]. 化工学报, 2015, 66(11): 4643-4651.
[14]	彭昌军, 姜秀丽, 计红芳, 王远鹏, 欧阳通, 李清彪. 铁锰复合氧化物对As(Ⅲ)、As(Ⅴ)的吸附研究及其在沼液中的应用[J]. 化工学报, 2014, 65(5): 1848-1855.
[15]	刁潘1，刘静2，张永奎3，刘瑾1，姚太平2. 阴离子/非离子表面活性剂体系洗涤含油污泥[J]. 化工进展, 2014, 33(10): 2753-2757.