Abstract
Chlorinated organic solvents (COSs) are extensively detected in contaminated soil and groundwater that pose long-term threats to human life and environment. In order to degrade COSs effectively, a novel catalytic composite of natural zeolite-supported nano zero valent iron (Z-nZVI) was synthesized in this study. The performance of Z-nZVI-catalyzed sodium percarbonate (SPC) in a heterogeneous Fenton-like system was investigated for the degradation of COSs such as 1,1,1-trichloroethane (1,1,1-TCA) and trichloroethylene (TCE). The surface characteristics and morphology of the Z-nZVI composite were tested using scanning electron microscopy (SEM) and transmission electron microscopy (TEM). Total pore volume, specific surface area, and pore size of the natural zeolite and the Z-nZVI composite were measured using Brunauer-Emmett-Teller (BET) method. SEM and TEM analysis showed significant elimination of aggregation and well dispersion of iron nano particles on the framework of natural zeolite. The BET N2 measurement analysis indicated that the surface area of the Z-nZVI composite was 72.3 m2/g, much larger than that of the natural zeolite (0.61 m2/g). For the contaminant analysis, the samples were extracted with n-hexane and analyzed through gas chromatograph. The degradation of 1,1,1-TCA and TCE in the Z-nZVI-catalyzed percarbonate system were 48 and 39 % respectively, while strong augmentation was observed up to 83 and 99 %, respectively, by adding the reducing agent (RA), hydroxyl amine (NH2OH•HCl). Probe tests validated the presence of OH● and O2 ●– which were responsible for 1,1,1-TCA and TCE degradation, whereas both free radicals were strengthened with the addition of RA. In conclusion, the Z-nZVI/SPC oxidation with reducing agent shows potential technique for degradation of groundwater contaminated by 1,1,1-TCA and TCE.
Similar content being viewed by others
References
Adams JA, Reddy KR, Tekola L (2011) Remediation of chlorinated solvent plumes using in situ air sparging-A 2-D laboratory study. Int J Environ Res Public Health 8:2226–2239
Ahmad A, Gu X, Li L, Lv S, Xu Y, Guo X (2015) Efficient degradation of trichloroethylene in water using persulfate activated by reduced graphene oxide-iron nanocomposite. Environ Sci Pollut Res 22:17876–17885
Akyol N, Yolcubal I (2013) Oxidation of nonaqueous phase trichloroethylene with permanganate in epikarst. Water Air Soil Pollut 224:1–19
Anipsitakis GP, Dionysiou DD (2004) Radical generation by the interaction of transition metals with common oxidants. Environ Sci Technol 38:3705–3712
Bellona C, Drewes JE (2007) Viability of a low-pressure nanofilter in treating recycled water for water reuse applications: a pilot-scale study. Water Res 17:3948–3958
Beydoun D, Amal R (2002) Implications of heat treatment on the properties of a magnetic iron oxide titanium dioxide photo catalyst. Mater Sci Eng B 94:71–81
Bogan BW, Trbovic V, Paterek JR (2003) Inclusion of vegetable oils in Fenton’s chemistry for remediation of PAH-contaminated soils. Chemosphere 50:15–21
Burbano AA, Dionysiou DD, Suidan MT, Richardson TL (2005) Oxidation kinetics and effect of pH on the degradation of MTBE with Fenton reagent. Water Res 39:107–118
Che H, Lee W (2011) Selective redox degradation of chlorinated aliphatic compounds by Fenton reaction in pyrite suspension. Chemosphere 82:1103–1108
Chen L, Ma J, Li X, Zhang J, Fang J, Guan Y, Xie P (2011) Strong enhancement on Fenton oxidation by addition of hydroxylamine to accelerate the ferric and ferrous iron cycles. Environ Sci Technol 45:3925–3930
Christina RK, Sedlak DL (2008) Factors affecting the yield of oxidants from the reaction of nanoparticulate zero-valent iron and oxygen. Environ Sci Technol 42:1262–1267
Clewell H, Gentry P, Gearhart J, Allen B, Andersen M (1995) Considering pharmacokinetic and mechanistic information in cancer risk assessments for environmental contaminants: examples with vinyl chloride and trichloroethylene. Chemosphere 31:2561–2578
Crane RA, Scott TB (2012) Nanoscale zero-valent iron: future prospects for an emerging water treatment technology. J Hazard Mater 211:112–125
de la Calle RG, Gimeno O, Rivas J (2012) Percarbonate as a hydrogen peroxide carrier in soil remediation processes. Environ Eng Sci 29:951–955
Devi LG, Kumar SG, Reddy KM, Munikrishnappa C (2009) Photo degradation of methyl orange an azodye by advanced Fenton process using zero valent metallic iron: influence of various reaction parameters and its degradation mechanism. J Hazard Mater 164:459–467
Du Y, Zhou M, Lei L (2006) Role of the intermediates in the degradation of phenolic compounds by Fenton-like process. J Hazard Mater 136:859–865
Fukuchi S, Miura A, Okabe R, Fukushima M, Sasaki M, Tsutomu S (2010) Spectroscopic investigations of humic-like acids formed via poly condensation reactions between glycine, catechol and glucose in the presence of natural zeolites. J Mol Struct 982:181–186
Fukuchi S, Nishimoto R, Fukushima M, Zhu Q (2013) Effects of reducing agents on the degradation of 2, 4, 6-tribromophenol in a heterogeneous Fenton-like system with an iron-loaded natural zeolite. Appl Catal B 147:411–419
Fukushima M, Tatsumi K, Morimoto K (2000) Influence of iron (III) and humic acid on the photodegradation of pentachlorophenol. Environ Toxicol Chem 19:1711–1716
Gu X, Lu S, Qiu Z, Sui Q, Miao Z, Lin K, Liu Y, Luo Q (2012) Comparison of photodegradation performance of 1, 1, 1-trichloroethane in aqueous solution with the addition of H2O2 or S2O8 2−oxidants. Ind Eng Chem Res 51:7196–7204
Han Y, Yang MD, Zhang W, Yan W (2015) Optimizing synthesis conditions of nanoscale zero-valent iron (nZVI) through aqueous reactivity assessment. Front Environ Sci Eng 9:813–822
He F, Zhao D, Liu J, Roberts CB (2007) Stabilization of Fe–Pd nanoparticles with sodium carboxymethyl cellulose for enhanced transport and dechlorination of trichloroethylene in soil and groundwater. Ind Eng Chem Res 46:29–34
Hoigne J, Bader H (1976) The role of hydroxyl radical reactions in ozonation processes in aqueous solutions. Water Res 10:377–386
Huang KC, Hoag GE, Chheda P, Woody BA, Dobbs GM (2001) Oxidation of chlorinated ethenes by potassium permanganate: a kinetics study. J Hazard Mater 87:155–169
Kim JS, Zhang L, Keane MA (2001) Removal of iron from aqueous solutions by ion exchange with Na-Y zeolite. Sep Purif Technol 36:1509–1525
Kim SA, Kamala-Kannan S, Lee KJ, Park YJ, Shea PJ, Lee WH, Kim HM, Oh BT (2013) Removal of Pb (II) from aqueous solution by a zeolite–nanoscale zero-valent iron composite. Chem Eng J 217:54–60
Klamerth N, Rizzo LL, Malato L, Maldonado MI, Agüera A, Fernández-Alba AR (2010) Degradation of fifteen emerging contaminants at μgL−1 initial concentrations by mild solar photo-Fenton in MWTP effluents. Water Res 44:545–554
Li R, Jin X, Megharaj M, Naidu R, Chen Z (2015) Heterogeneous Fenton oxidation of 2, 4-dichlorophenol using iron-based nanoparticles and persulfate system. Chem Eng J 264:587–594
Liang C, Su HW (2009) Identification of sulfate and hydroxyl radicals in thermally activated persulfate. Ind Eng Chem Res 48:5558–5562
Liang CJ, Bruell CJ, Marley MC, Sperry KL (2004) Persulfate oxidation for in situ remediation of TCE. I. Activated by ferrous ion with and without a persulfate thiosulfate redox couple. Chemosphere 55:1213–1223
Lim H, Lee J, Jin S, Kim J, Yoon J, Hyeon T (2006) Highly active heterogeneous Fenton catalyst using iron oxide nanoparticles immobilized in alumina coated mesoporous silica. Chem Commun 4:463–465
Liou RM, Chen SH, Hung MY, Hsu CS (2004) Catalytic oxidation of pentachlorophenol in contaminated soil suspensions by Fe+3 resin/H2O2. Chemosphere 55:1271–1280
Liou RM, Chen SH, Hung MY, Hsu CS, Lai JY (2005) Fe (III) supported on resin as effective catalyst for the heterogeneous oxidation of phenol in aqueous solution. Chemosphere 59:117–125
Liu Y, Phenrat T, Lowry GV (2007) Effect of TCE concentration and dissolved groundwater solutes on NZVI-promoted TCE dechlorination and H2 evolution. Environ Sci Technol 41:7881–7887
McCarty, Perry L (2010) Groundwater contamination by chlorinated solvents: history, remediation technologies and strategies. In: Ward CH (ed) In situ remediation of chlorinated solvent plumes. Springer, New York, pp 1–28
Miao Z, Gu X, Lu S, Dionysiou DD, Al-Abed SR, Zang X, Wu X, Qiu Z, Sui Q, Danish M (2015a) Mechanism of PCE oxidation by percarbonate in a chelated Fe (II)-based catalyzed system. Chem Eng J 275:53–62
Miao Z, Gu X, Lu S, Zang X, Wu X, Xu M, Ndong LBB, Qiu Z, Sui Q, Fu YG (2015b) Perchloroethylene (PCE) oxidation by percarbonate in Fe2+-catalyzed aqueous solution: PCE performance and its removal mechanism. Chemosphere 119:1120–1125
Miao Z, Gu X, Lu S, Brusseau ML, Zhang X, Fu X, Danish M, Qiu Z, Sui Q (2015c) Enhancement effects of chelating agents on the degradation of tetrachloroethene in Fe (III) catalyzed percarbonate system. Chem Eng J 281:286–294
Miura A, Okabe R, Izumo K, Fukushima M (2009) Influence of the physicochemical properties of clay minerals on the degree of darkening via polycondensation reactions between catechol and glycine. Appl Clay Sci 46:277–282
Navarro S, Fenoll J, Vela N, Ruiz E, Navarro G (2009) Photocatalytic degradation of eight pesticides in leaching water by use of ZnO under natural sunlight. J Hazard Mater 172:1303–1310
Neamtu M, Zaharia C, Catrinescu C, Yediler A, Macoveanu M, Kettrup (2004) A Fe-exchanged Y zeolite as catalyst for wet peroxide oxidation of reactive azo dye Procion Marine H-EXL. Appl Catal B 48:287–294
Neyens E, Baeyens J (2003) A review of classic Fenton’s peroxidation as an advanced oxidation technique. J Hazard Mater 98:33–50
Nishimoto R, Zhu Q, Miyamoto T, Sato T, Tu X, Aneksampant A, Fukushima M (2015) Monopersulfate oxidation of Acid Orange 7 with an iron (III)-tetrakis (N-methylpyridinium-4yl) porphyrin intercalated into the layers of montmorillonite and pillared clay. J Mol Catal A 396:84–89
Northup A, Cassidy D (2008) Calcium peroxide (CaO2) for use in modified Fenton chemistry. J Hazard Mater 152:1164–1170
Oller I, Malato S, Sánchez-Pérez JA (2011) Combination of advanced oxidation processes and biological treatments for wastewater decontamination a review. Sci Tot Environ 409:4141–4166
Oturan MA (2000) An ecologically effective water treatment technique using electrochemically generated hydroxyl radicals for in situ destruction of organic pollutants: application to herbicide 2, 4-D. J Appl Electrochem 30:475–482
Qu X, Alvarez PJJ, Li Q (2013) Applications of nanotechnology in water and wastewater treatment. Water Res 47:3931–3946
Ramirez JH, Costa CA, Madeira LM, Mata G, Vicente MA, Rojas-Cervantes ML, López-Peinado AJ, Martín-Aranda RM (2007) Fenton-like oxidation of orange II solutions using heterogeneous catalysts based on saponite clay. Appl Catal B 71:44–56
Savant MM, Pansuriya AM, Bhuva CV, Kapuriya N, Patel AS, Audichya VB, Pipaliya PV, Naliapara YT (2009) Water mediated construction of trisubstituted pyrazoles/isoxazoles library using ketene dithioacetals. J Comb Chem 12:176–180
Seol AK, Seralathan KK, Kui-Jae L, Yool-Jin P, Shea PJ, Lee WH, Kim HM, Oh BT (2013) Removal of Pb (II) from aqueous solution by a zeolite nanoscale zero-valent iron composite. Chem Eng J 217:54–60
Shin S, Yoon H, Jang J (2008) Polymer-encapsulated iron oxide nanoparticles as highly efficient Fenton catalysts. Catal Commun 10:178–182
Sun H, Zhou G, Liu S, Ha MA, Tade MO, Shaobin W (2012) Nano-Fe0 encapsulated in micro carbon spheres: synthesis, characterization, and environmental applications. ACS Appl Mater Inter 4:6235–6241
Sunder M, Hempel DC (1997) Oxidation of tri- and perchloroethene in aqueous solution with ozone and hydrogen peroxide in a tube reactor. Water Res 31:33–40
Tamura H, Goto K, Yotsuyanagi T, Nagayama M (1974) Spectrophotometric determination of iron (II) with 1,10-phenanthroline in the presence of large amounts of iron (III). Talanta 21:314–318
Tong L, Wu F, Yan S, Ji T, Lin B (1996) Paramagnetic behavior in NiNaY zeolites. Solid State Commun 97:1043–1046
Vogan JL, Focht RM, Clark DK, Graham SL (1999) Performance evaluation of a permeable reactive barrier for remediation of dissolved chlorinated solvents in groundwater. J Hazard Mater 68:97–108
Wang W, Zhou M, Mao Q, Yue J, Wang X (2010) Novel NaY zeolite-supported nano scale zero-valent iron as an efficient heterogeneous Fenton catalyst. Catal Commun 11:937–941
Watts RJ, Teel AL (2005) Chemistry of modified Fenton’s reagent (catalyzed H2O2 propagations–CHP) for in situ soil and groundwater remediation. J Environ Eng 131:612–622
Watts RJ, Teel AL (2006) Treatment of contaminated soils and groundwater using ISCO. Pract Period Hazard Toxic Radioact Waste Manage 10:2–9
Watts RJ, Foget MK, Kong SH, Teel AL (1999) Hydrogen peroxide decomposition in model subsurface systems. J Hazard Mater 69:229–243
Wei X, Guo S, Wu B, Li F, Li G (2015) Effects of reducing agent and approaching anodes on chromium removal in electro kinetic soil remediation. Front Environ Sci Eng 10:253–261, 1-9
Wigle DT, Arbuckle TE, Walker M, Wade MG, Liu S, Krewski D (2007) Environmental hazards: evidence for effects on child health. J Toxicol Environ Health Part B 10:3–39
Wu C, Maurer C, Wang Y, Xue S, Davis DL (1999) Water pollution and human health in China. Environ Health Perspect 107:251–256
Xu L, Wang J (2012) Magnetic nano scaled Fe3O4/CeO2 composite as an efficient Fenton-like heterogeneous catalyst for degradation of 4-chlorophenol. Environ Sci Technol 46:10145–10153
Xu M, Gu X, Lu S, Miao Z, Zang X, Wu X, Qiu Z, Sui Q (2015) Degradation of carbon tetrachloride in thermally activated persulfate system in the presence of formic acid. Front Environ Sci Eng 1–9
Yang Y, Zhang G, Yu S, Shen X (2010) Efficient removal of organic contaminants by a visible light driven photo catalyst Sr6Bi2O9. Chem Eng J 162:171–177
Zhang X, Gu X, Lu S, Miao Z, Xu M, Fu X, Qiu Z, Sui Q (2015) Degradation of trichloroethylene in aqueous solution by calcium peroxide activated with ferrous ion. J Hazard Mater 284:253–260
Zhao F, Yin J, Zhang XX, Chen Y, Zhang Y, Wu B, Li M (2015) Reduction in health risk induced by semi-volatile organic compounds and metals in a drinking water treatment plant. Int J Environ Sci Technol 12:527–536
Zied A, Bahaa M, Schwieger W, Unger A (2008) Nitrous oxide decomposition over transition metal exchanged ZSM-5 zeolites prepared by the solid-state ion-exchange method. Appl Catal B 84:277–288
Acknowledgments
This study was financially supported by the grant from the National Natural Science Foundation of China (Nos. 41373094 and 51208199), China Postdoctoral Science Foundation (2015M570341), and the Fundamental Research Funds for the Central Universities (22A201514057). One of the authors would like to thank KKS—The Knowledge Foundation of Sweden—and industrial partners (Mälarenergi and Eskilstuna Energi och Miljö) for their funding.
Author information
Authors and Affiliations
Corresponding author
Ethics declarations
Conflict of interest
The authors declare that they have no conflict of interest.
Additional information
Responsible editor: Santiago V. Luis
Electronic supplementary material
Below is the link to the electronic supplementary material.
ESM 1
(DOCX 412 kb)
Rights and permissions
About this article
Cite this article
Danish, M., Gu, X., Lu, S. et al. Degradation of chlorinated organic solvents in aqueous percarbonate system using zeolite supported nano zero valent iron (Z-nZVI) composite. Environ Sci Pollut Res 23, 13298–13307 (2016). https://doi.org/10.1007/s11356-016-6488-5
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s11356-016-6488-5