Removal of nitrobenzene by ball-milled pyrite as permeable reactive barrier active medium
LIAO Ya-ping1, ZHANG Shan-shan1, WU Chao1, YUAN Qian1, WANG Ming-xin1,2
1. School of Environmental & Safety Engineering, Changzhou University, Changzhou 213164, China; 2. Jiangsu Petrochemical Industry Safety and Environmental Protection Engineering Research Center, Changzhou 213164, China
Abstract：Ball-milled pyrite (BMP) was prepared by mechanochemical method, and the reduction performance of BMP to nitrobenzene (NB) was studied by batch experiments. The sand column experiment was used to investigate the feasibility of using BMP to fill a permeable reaction barrier (PRB) to remediate nitrobenzene-contaminated groundwater. The morphology, crystal structure and elemental composition of BMP before and after reaction were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), Fourier transform infrared spectroscopy (FT-IR) and X-ray photoelectron spectroscopy (XPS). The results showed that BMP can effectively remove NB, the removal rate of NB was 98.8%. The main reduction product of NB was aniline. The pseudo-first-order kinetic model fitted the degradation process of NB well, and the degradation kinetic constant was 59.03×10-3min-1. No contaminants other than aniline were detected by GC-MS analysis. The results of the sand column experiment showed that BMP-PRB can continuously and efficiently remove nitrobenzene from groundwater. The groundwater composition kept stable, and the acute toxicity was significantly reduced. Characterization analysis showed that BMP has a certain adsorption capacity on NB and the reduced product. On the surface of BMP, active substances such as Fe2+ and S2- with reducibility were continuously produced, which could react with the strong electron-withdrawing nitro group of NB to generate AN and Fe3+. The pyrite can be oxidized by Fe3+ to produce Fe2+ and promote the Fe2+-Fe3+ cycle.
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 Environmental Science, 2015, 35(11):3352-3358.
[2]
张丹,张旭,李广贺.Fenton试剂快速氧化处理事故场地地下水中的硝基苯[J].环境工程学报, 2016,10(7):3439-3444.Zhang D, Zhang X, Li G H.Fenton reagent rapidly oxidized nitrobenzene in groundwater at the accident site[J].Chinese Journal of Environmental Engineering, 2016,10(7):3439-3444.
[3]
董洋,温春宇,于锦秋,等.乳化纳米铁修复硝基苯污染含水层研究[J].中国环境科学, 2017,37(12):4541-4548.Dong Y, Wen C Y, Yu J Q, et al.Laboratory evaluation of degradation of nitrobenzene in aquifer using emulsified nanoscale zero-valent iron[J].China Environmental Science, 2017,37(12):4541-4548.
[4]
Wei W, Sun R, Cui J, et al.Removal of nitrobenzene from aqueous solution by adsorption on nanocrystalline hydroxyapatite[J].Desalination, 2010,263(1-3):89-96.
[5]
周岩梅,张琼,刁晓华,等.硝基苯和西维因在活性炭上的吸附效果及动力学研究[J].中国环境科学, 2010,30(9):1177-1182.Zhou Y M, Zhang Q, Diao X H, et al.The adsorption effect and dynamics of nitrobenzene and civiine on activated carbon[J].China Environmental Science, 2010,30(9):1177-1182.
[6]
Ren Y, Yang J, Chen S Y.The fate of a nitrobenzene-degrading bacterium in pharmaceutical wastewater treatment sludge[J].Chemosphere, 2015,141:13-18.
[7]
吴晴,刘金泉,王凯,等.高级氧化技术在难降解工业废水中的研究进展[J].水处理技术, 2015,41(11):25-29.Wu Q, Liu J Q, Wang K, et al.Research progress of advanced oxidation technology in refractory wasWaste water[J].Technology of Water Treatment, 2015,41(11):25-29.
[8]
Zhang Y L, Zhang K, Dai C M, et al.Performance and mechanism of pyrite for nitrobenzene removal in aqueous solution[J].Chemical Engineering Science, 2014,111:135-141.
[9]
Zhang S S, Zhu J Y, Zhang X W, et al.The removal mechanism of nitrobenzene by the Cu-Fe/Carbon material under different aeration conditions[J].Journal of Hazardous Materials, 2021,403:123584.
[10]
Ling X F, Li J S, Zhu W, et al.Synthesis of nanoscale zero-valent iron/ordered mesoporous carbon for adsorption and synergistic reduction of nitrobenzene[J].Chemosphere, 2012,87(6):655-660.
[11]
Yin W Z, Wu J H, Li P, 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, 2012,184:198-204.
[12]
Khataee A, Fathinia S, Fathinia M.Production of pyrite nanoparticles using high energy planetary ball milling for sonocatalytic degradation of sulfasalazine[J].Ultrasonics Sonochemistry, 2017,34:904-915.
[13]
Sun Y, Lv D, Zhou, J S, et al.Adsorption of mercury (II) from aqueous solutions using FeS and pyrite:A comparative study[J].Chemosphere, 2017,185:452-461.
[14]
杨世迎,杨鑫,梁婷,等.零价铁还原和过硫酸盐氧化联合降解水中硝基苯[J].环境化学, 2012,31(5):682-686.Yang S Y, Yang X, Liang T, et al.Combination of zero-valent iron reduction and persulfate oxidation to degrade nitrobenzene in water[J].Environmental Chemistry, 2012,31(5):682-686.
[15]
Yang Z, Ma X W, Shan C, et al.Enhanced nitrobenzene reduction by zero valent iron pretreated with H2O2/HCl[J].Chemosphere, 2018,197:494-501.
[16]
Zhang Y, Zhang K, Dai C M, et al.An enhanced Fenton reaction catalyzed by natural heterogeneous pyrite for nitrobenzene degradation in an aqueous solution[J].Chemical Engineering Journal, 2014,244:438-445.
[17]
Pourghahramani P, Akhgar B N.Characterization of structural changes of mechanically activated natural pyrite using XRD line profile analysis[J].International Journal of Mineral Processing, 2015,134:23-28.
[18]
朱颖一,王城晨,王明新,等.硫化纳米铁反应带修复硝基苯污染地下水[J].中国环境科学, 2020,40(2):670-680.Zhu Y Y, Wang C C, Wang M X, et al.Remediation of nitrobenzene contaminated groundwater by S-NZVI reaction zone[J].China Environmental Science, 2020,40(2):670-680.
[19]
Zingaretti D, Verginelli I, Luisetto I, et al.Horizontal permeable reactive barriers with zero-valent iron for preventing upward diffusion of chlorinated solvent vapors in the unsaturated zone[J].Journal of Contaminant Hydrology, 2020,234:103687.
[20]
Dong J, Zhao Y S, Zhao R, et al.Effects of pH and particle size on kinetics of nitrobenzene reduction by zero-valent iron[J].Journal of Environmental Sciences, 2010,22(11):1741-1747.
[21]
Wen Z, Nan S, Ying, B, et al.The innovative application of agriculture straw in in situ field permeable reactive barrier for remediating nitrate-contaminated groundwater in grain-production areas[J].Biochemical Engineering Journal, 2020,164:107755.
[22]
Huang Y J, Zeng Q, Hu L, et al.Column study of enhanced Cr(Ⅵ) removal and removal mechanisms by Sporosarcina saromensis W5assisted bio-permeable reactive barrier[J].Journal of Hazardous Materials, 2021,405:124115.
[23]
Gong Y Y, Gai L S, Tang J C, 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.
[24]
叶倩,王城晨,王明新,等.球磨硫铁矿-过硫酸盐联合降解水中硝基苯和苯胺[J].环境工程学报, 2021,15(1):30-42.Ye Q, Wang C C, Wang M X, et al.Ball-ground pyrite-persulfate combination degrade nitroenzene and aniline in water[J].Journal of Environmental Engineering, 2021,15(1):30-42.
[25]
Du M M, Zhang Y Q, Zeng X L,et al.Enhancement of ball-miling on pyrite/zero-valent iron for arsenic removal in water:A mechanistic study[J].Chemosphere, 2020,249:126130.
[26]
Diao Z H, Liu J J, Hu Y X, et al.Comparative study of Rhodamine B degradation by the systems pyrite/H2O2and pyrite/persulfate:Reactivity, stability, products and mechanism[J].Separation and Purification Technology, 2017,184:374-383.
[27]
Han D S, Song J K, Batchelor B, et al.Removal of arsenite(As(III)) and arsenate(As(V)) by synthetic pyrite (FeS2):Synthesis, effect of contact time,and sorption/desorption envelopes[J].Journal of Colloid & Interface Science, 2013,392:311-318.
[28]
Thomas J E, Jones C F, Skinner W M, et al.The role of surface sulfur species in the inhibition of pyrrhotite dissolution in acid conditions[J].Geochimica et Cosmochimica Acta, 1998,62(9):1555-1565.
[29]
Zheng X F, Cao S T, Nie Z Y, et al.Impact of mechanical activation on bioleaching of pyrite:A DFT study[J].Minerals Engineering, 2020, 148:106209.
[30]
邓靖,徐盼琦,倪永炯,等.黄铁矿活化过硫酸钠降解水中卡马西平[J].水处理技术, 2016,42(4):34-38.Deng J, Xu P Q, Ni Y J, et al.Pyrite activates sodium persulfate to degrade carbamazepine in water[J].Technology of Water Treatment, 2016,42(4):34-38.
[31]
Wu D L, Chen Y F, Zhang Y L, et al.Ferric iron enhanced chloramphenicol oxidation in pyrite (FeS2) induced Fenton-like reactions[J].Separation and Purification Technology, 2015,154:60-67.
[32]
Che H, Bae S, Lee W.Degradation of trichloroethylene by Fenton reaction in pyrite suspension[J].Journal of Hazardous Materials, 2011,185(2/3):1355-1361.
[33]
Yin W Z, Wu J H, Li P, 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, 2012,184:198-204.
[34]
Furukawa Y, Kim J W, Watkins J, et al.Formation of ferrihydrite and associated iron corrosion products in permeable reactive barriers of zero-valent iron[J].Environmental Science & Technology, 2002, 36(24):5469-5475.
[35]
Kakavandi B, Jafari A J, Kalantary R R, et al.Synthesis and properties of Fe3O4-activated carbon magnetic nanoparticles for removal of aniline from aqueous solution:equilibrium, kinetic and thermodynamic studies[J].Iranian Journal of Environmental Health Science & Engineering, 2013,10:19.
[36]
蒋柱武,廖薇,刘涛.3种氧化铁矿物/亚铁体系还原转化芳香硝基化合物的比较[J].环境工程学报, 2016,10(8):4266-4270.Jiang Z W, Liao W, Liu T.Comparison of reduced-transformed aromatic nitroso compounds in three iron oxide mineral/ferrous systems[J].Chinese Journal of Environmental Engineering, 2016, 10(8):4266-4270.
[37]
Ling X F, Li J S, Zhu W, et al.Synthesis of nanoscale zero-valent iron/ordered mesoporous carbon for adsorption and synergistic reduction of nitrobenzene[J].Chemosphere, 2012,87(6):655-660.
[38]
Huang Y H, Zhang T C.Effects of low pH on nitrate reduction by iron powder[J].Water Research, 2004,38(11):2631-2642.
[39]
Lin Y T, Huang C P.Reduction of chromium(VI) by pyrite in dilute aqueous solutions[J].Separation and Purification Technology, 2008, 63(1):191-199.
[40]
Bonnissel-Gissinger P, Alnot M, Ehrhardt J J, et al.Surface oxidation of pyrite as a function of pH[J].Environmental Science & Technology, 1998,32(19):2839-2845.
[41]
Rabieh A, Albijanic B, Eksteen J J.Influence of balling media and water quality on flotation performance of gold bearing pyrite[J].Minerals Engineering, 2017,112:68-76.
[42]
Cai H Y, Wang P, Chen X T, et al.Sulfide ions-induced release of biocides from a metal-phenolic supramolecular film fabricated on aluminum for inhibition of microbially influenced corrosion[J].Corrosion Science, 2020,167:108534.
[43]
Wu B C, Gu G H,Deng S, et al.Efficient natural pyrrhotite activating persulfate for the degradation of O-isopropyl-N-ethyl thionocarbamate:Iron recycle mechanism and degradation pathway[J].Chemosphere, 2019,224:120-127.
[44]
黄涛,张胜男,黄菲,等.红透山黄铁矿的红外光谱研究[J].地学前缘, 2013,20(3):104-109.Huang T, Zhang S N, Huang F, et al.Infra-red spectroscopic study of Hongtoushan pyrite[J].Earth Science Frontiers, 2013,20(3):104-109.
[45]
Mikhaylova Y, Adam G, Haussler, L, et al.Temperature-dependent FTIR spectroscopic and thermoanalytic studies of hydrogen bonding of hydroxyl (phenolic group) terminated hyperbranched aromatic polyesters[J].Journal of Molecular Structure, 2006,788(1-3):80-88.
[46]
Pan J J, Guan B H.Adsorption of nitrobenzene from aqueous solution on activated sludge modified by cetyltrimethylammonium bromide[J].Journal of Hazardous Materials, 2010,183(1-3):341-346.
