PDF(1007 KB)
PDF(1007 KB)
PDF(1007 KB)
硫化纳米铁反应带修复硝基苯污染地下水
Remediation of nitrobenzene contaminated groundwater by S-NZVI reaction zone
采用前置硫化合成法制备硫化纳米铁（S-NZVI）并进行表征，采用模拟砂柱创建S-NZVI原位反应带，研究其对硝基苯（NB）污染地下水的修复效能.X射线衍射（XRD）、X射线光电子能谱（XPS）、透射电子显微镜（TEM）表征结果表明，S-NZVI是以Fe（0）为核心，硫铁化合物为外壳的颗粒，可以有效抑制S-NZVI颗粒的团聚，具有较好的分散性.与NZVI相比，S-NZVI对NB的去除效率更高，最高去除率可达99.65%，在砂柱中具有更强的穿透能力.S-NZVI对NB的去除过程符合准一级动力学模式.S-NZVI对NB的去除机理是先将NB快速吸附于表面，然后再进一步通过化学还原降解，因此NB去除较快而苯胺生成较慢.S-NZVI反应带对NB泄露区的削减幅度较大，增加单井S-NZVI注入量和增加注入井均可提高修复效果，7d内NB累计去除率最高达87.43%，但前2d出水NB浓度仍然较高；S-NZVI反应带对NB传输区具有较好的修复效果，增加注入井比增加单井S-NZVI注入量具有更好的持续性和更高的NB去除率，7d内NB累计去除率最高达99.90%.
Sulfidated-nanoscale zerovalent iron (S-NZVI) was prepared by pre-sulfide synthesis and characterized. The S-NZVI reaction zone was established in sand columns to study the remediation efficiency of nitrobenzene contaminated groundwater. X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and transmission electron microscopy (TEM) characterization tests showed that ferrous sulfide coating on the surface of Fe(0), which could inhibit the aggregation of S-NZVI particles, thus showed better dispersibility. Compared with NZVI, S-NZVI has higher degradation efficiency for NB, and the highest degradation efficiency was 99.65%. The degradation process of NB by S-NZVI conformed pseudo-first-order kinetics. It has stronger penetrating ability in sand column. The removal mechanism of S-NZVI on NB was that NB was quickly adsorbed on the surface and then further degraded by chemical reduction, so NB removal was faster and aniline formatioon was slower. The S-NZVI reaction zone had a large reduction of NB in the leakage zone. Increasing the single-well S-NZVI injection volume and adding injection well both improved the remediation efficiency. The cumulative removal efficiency of NB in the 7days was up to 87.43%, but the NB concentration in the first 2d was still high. The S-NZVI reaction zone showed better remediation effect in the transmission zone. Adding injection well showed better persistence and NB removal rate than increasing S-NZVI injection volume in the single well, and the cumulative removal efficiency of NB in the 7days was up to 99.90%.
地下水 / 反应带 / 硫化纳米铁 / 硝基苯 / 原位修复
groundwater / in-site remediation / nitrobenzene / reaction zone / sulfidated-nanoscale zerovalent iron
[1] Yin W, Wu J, Ping L, et al. Experimental study of zero-valent iron induced nitrobenzene reduction in groundwater:The effects of pH, iron dosage, oxygen and common dissolved anions[J]. Chemical Engineering Journal, 2012,184(3):198-204.
[2] Zhang Y, Ke Z, Dai C, et al. Performance and mechanism of pyrite for nitrobenzene removal in aqueous solution[J]. Chemical Engineering Science, 2014,111(111):135-141.
[3] Bhatkhande D S, Pangarkar V G, Beenackers A a C M. Photocatalytic degradation of nitrobenzene using titanium dioxide and concentrated solar radiation:chemical effects and scaleup[J]. Water Research, 2003,37(6):1223-1230.
[4] Yin W, Wu J, Huang W, et al. Enhanced nitrobenzene removal and column longevity by coupled abiotic and biotic processes in zero-valent iron column[J]. Chemical Engineering Journal, 2015, 259:417-423.
[5] Zhang Y, Xu X, Pan Y, et al. Pre-magnetized Fe0 activated persulphate for the degradation of nitrobenzene in groundwater[J]. Separation and Purification Technology, 2019,212:555-562.
[6] Ren Y, Yang J, Chen S. The fate of a nitrobenzene-degrading bacterium in pharmaceutical wastewater treatment sludge[J]. Chemosphere, 2015,141:13-18.
[7] Duan H, Yong L, Yin X, et al. Degradation of nitrobenzene by Fenton-like reaction in a H2O2/schwertmannite system[J]. Chemical Engineering Journal, 2016,283:873-879.
[8] Kumar A, Kumar P, Paul S, et al. Visible light assisted reduction of nitrobenzenes using Fe(bpy)3+2/rGO nanocomposite as photocatalyst[J]. Applied Surface Science, 2016,386:103-114.
[9] Gu D, Shao N, Zhu Y, et al. Solar-driven thermo- and electrochemical degradation of nitrobenzene in wastewater:Adaptation and adoption of solar STEP concept[J]. Journal of Hazardous Materials, 2017,321:703-710.
[10] Wu Y, Qi H, Li B, et al. Novel hydrophobic cotton fibers adsorbent for the removal of nitrobenzene in aqueous solution[J]. Carbohydr Polym, 2017,155:294-302.
[11] 孙威.地下水中苯类有机污染的原位反应带修复技术研究[D]. 长春:吉林大学, 2012. Sun W. Study on the remediation of benzene-basedgroundwater pollution by In Situ Reaction Zone[D]. Changchun:Jilin University, 2012.
[12] Hoch L B, Mack E J, Hydutsky B W, et al. Carbothermal synthesis of carbon-supported nanoscale zero-valent iron particles for the remediation of hexavalent chromium[J]. Environmental Science & Technology, 2008,42(7):2600-2605.
[13] Kocur C M D, Line L, Boparai H K, et al. Contributions of abiotic and biotic dechlorination following carboxymethyl cellulose stabilized nanoscale zero valent iron injection[J]. Environmental Science & Technology, 2015,49(14):8648-8656.
[14] 姚静波,周杰,王明新,等.纳米零价铁和过氧化钙联合降解土壤淋洗废液的α-HCH[J]. 环境科学, 2018,39(11):304-312. Yao J B, Zhou J, Wang M X, et al. Degradation of α-HCH in soil washing solutions with nZVI and CaO2[J]. Environmental Science, 2018,39(11):304-312.
[15] 王恩泽,韦志伟,曹茜,等.天然有机质对纳米零价铁去除水中六价铬的影响[J]. 现代地质, 2016,30(4):818-824. Wang E Z, Wei Z W, Cao X, et al. Effect of natural organic matter on removal of Cr(Ⅵ) from water by nanoscale zero-valent iron[J]. Geoscience, 2016,30(4):818-824.
[16] Guan X, Sun Y, Qin H, et al. The limitations of applying zero-valent iron technology in contaminants sequestration and the corresponding countermeasures:The development in zero-valent iron technology in the last two decades (1994~2014)[J]. Water Research, 2015,75:224-248.
[17] 韩建江,李常锁,温春宇,等.乳化纳米铁浆液在含水层中的迁移特征研究[J]. 中国环境科学, 2018,38(6):2175-2181. Han J J, Li C S, Wen C Y, et al. Transport characteristics of emulsified nanoscale-zero-valent-iron in saturated porous media[J]. China Environment Science, 2018,38(6):2175-2181.
[18] Zou Y, Wang X, Khan A, et al. Environmental remediation and application of nanoscale zero-valent iron and its composites for the removal of heavy metal ions:A review[J]. Environmental Science & Technology, 2016,50(14):7290-7304.
[19] Zhang Y, Su Y, Zhou X, et al. A new insight on the core-shell structure of zerovalent iron nanoparticles and its application for Pb(II) sequestration[J]. Journal of Hazardous Materials, 2013,263(Part 2):685-693.
[20] Gong Y, Gai L, Tang J, et al. Reduction of Cr(VI) in simulated groundwater by FeS-coated iron magnetic nanoparticles[J]. Science of the Total Environment, 2017,595:743-751.
[21] Rongbing F, Yingpin Y, Zhen X, et al. The removal of chromium (VI) and lead (II) from groundwater using sepiolite-supported nanoscale zero-valent iron (S-NZVI)[J]. Chemosphere, 2015,138:726-734.
[22] Bae S, Gim S, Kim H, et al. Effect of NaBH 4on properties of nanoscale zero-valent iron and its catalytic activity for reduction of p-nitrophenol[J]. Applied Catalysis B Environmental, 2016,182:541-549.
[23] Li D, Mao Z, Zhong Y, et al. Reductive transformation of tetrabromobisphenol A by sulfidated nano zerovalent iron[J]. Water Research, 2016,103:1-9.
[24] Xu C, Zhang B, Wang Y, et al. Effects of Sulfidation, Magnetization, and Oxygenation on Azo Dye Reduction by Zerovalent Iron[J]. Environmental Science & Technology, 2016,50(21):11879-11887.
[25] Tang J, Tang L, Feng H, et al. pH-Dependent degradation of p-nitrophenol by sulfidated nanoscale zerovalent iron under aerobic or anoxic conditions[J]. Journal of Hazardous Materials, 2016,320:581-590.
[26] Gao J, Han D Q, Xu Y, et al. Persulfate activation by sulfide-modified nanoscale iron supported by biochar (S-nZVI/BC) for degradation of ciprofloxacin[J]. Separation and Purification Technology, 2019, 235(2020):116202-116209.
[27] 张瑾,魏才倢,白鸽,等.多聚物吸附纳米零价铁在多孔介质中的迁移[J]. 中国环境科学, 2018,38(10):149-156. ZHANG J, WEI C J, BAI G, et al. Transport of PAA modified nanoscale zero-valent iron in water saturated porous media[J]. China Environment Science, 2018,38(10):149-156.
[28] Petosa A R, Brennan S J, Rajput F, et al. Transport of two metal oxide nanoparticles in saturated granular porous media:role of water chemistry and particle coating[J]. Water Research, 2012,46(4):1273-1285.
[29] 温春宇,王敏,董军,等.植物油改性纳米铁修复硝基苯污染地下水的研究[J]. 生态环境学报, 2013,2013(6):1048-1052. Wen C Y, Wang M, Dong J, et al. Degradation of nitrobenzene in groundwater using vegetable oil modified zero-valent-iron[J]. Ecology and Environment, 2013,(6):1048-1052.
[30] 张立国,罗燕群,张树喜,等.零价铁还原体系硝基苯初始浓度对还原过程的影响[J]. 广东化工, 2011,38(8):247-248. Zhang L G, Luo Y Q, Zhang S X, et al. Effect of Initial Nitrobenzene Concentrations on Nitrobenzene Reduction by Zero-valent Iron[J]. Guangdong Chemical Industry, 2011,38(8):247-248.
[31] 李卉,赵勇胜,韩占涛,等.蔗糖改性纳米铁原位反应带对硝基苯污染的模拟修复研究[J]. 中国环境科学, 2015,35(11):3352-3358. Li H, Zhao Y S, Han Z T, et al. Simulated remediation for nitrobenzene pollution with in-situ reactive zone of sucrose-modified nanoscale zero valent iron[J]. China Environment Science, 2015, 35(11):3352-3358.
[32] Park S W, Kim S K, Kim J B, et al. Particle Surface Hydrophobicity and the Dechlorination of Chloro-Compounds by Iron Sulfides[J]. Water Air & Soil Pollution Focus, 2006,6(1/2):97-110.
[33] Rajajayavel S R C, Ghoshal S. Enhanced reductive dechlorination of trichloroethylene by sulfidated nanoscale zerovalent iron[J]. Water Research, 2015,78:144-153.
[34] Lim T T, Zhu B W. Practical applications of bimetallic nanoiron particles for reductive dehalogenation of haloorganics:Prospects and challenges[J]. Acs Symposium, 2009,2009:245-261.
[35] 李卉.蔗糖改性纳米铁原位反应带修复硝基苯污染地下水研究[D]. 长春:吉林大学, 2014. Li H. Study on remediation of nitrobenzene contaminated groundwaterwith in situ reactive zone of sucrose-modified nano-iron[D]. Changchun:Jilin University, 2012.
国家自然科学基金项目（41772240，21906009）
京公网安备 11010802030352号 /
| 〈 |
|
〉 |
